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Encyclopedia of Sustainability Science

and Technology Series


Editor-in-Chief: Robert A. Meyers

Michael Evan Goodsite


Matthew Stanley Johnson
Ole Hertel  Editors

Air Pollution
Sources,
Statistics and
Health Effects
A Volume in the Encyclopedia of
Sustainability Science and Technology,
Second Edition
Encyclopedia of Sustainability Science
and Technology Series

Editor-in-Chief
Robert A. Meyers
The Encyclopedia of Sustainability Science and Technology series (ESST)
addresses the grand challenges for science and engineering today. It provides
unprecedented, peer-reviewed coverage in more than 600 separate articles
comprising 20 topical volumes, incorporating many updates from the first
edition as well as new articles. ESST establishes a foundation for the many
sustainability and policy evaluations being performed in institutions
worldwide.
An indispensable resource for scientists and engineers in developing new
technologies and for applying existing technologies to sustainability, the
Encyclopedia of Sustainability Science and Technology series is presented at
the university and professional level needed for scientists, engineers, and their
students to support real progress in sustainability science and technology.
Although the emphasis is on science and technology rather than policy, the
Encyclopedia of Sustainability Science and Technology series is also a com-
prehensive and authoritative resource for policy makers who want to under-
stand the scope of research and development and how these bottom-up
innovations map on to the sustainability challenge.

More information about this series at http://www.springer.com/series/15436


Michael Evan Goodsite
Matthew Stanley Johnson
Ole Hertel
Editors

Air Pollution Sources,


Statistics and Health
Effects
A Volume in the Encyclopedia of Sustainability
Science and Technology, Second Edition

With 188 Figures and 63 Tables


Editors
Michael Evan Goodsite Matthew Stanley Johnson
School of Civil, Environmental and Department of Chemistry
Mining Engineering University of Copenhagen
The Australian School of Petroleum Copenhagen, Denmark
The University of Adelaide
Adelaide, SA, Australia Airlabs, Copenhagen, Denmark

Ole Hertel
Department of Environmental Sciences
Aarhus University
Roskilde, Denmark

ISBN 978-1-0716-0595-0 ISBN 978-1-0716-0596-7 (eBook)


ISBN 978-1-0716-0597-4 (print and electronic bundle)
https://doi.org/10.1007/978-1-0716-0596-7
© Springer Science+Business Media, LLC, part of Springer Nature 2021
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Series Preface

Our nearly 1000-member team recognizes that all elements of sustainability


science and technology continue to advance as does our understanding of the
needs for energy, water, clean air, food, mobility, and health and the relation of
every single aspect of this vast and interconnected body of knowledge to
climate change. Our Encyclopedia content is at a level for university students,
professors, engineers, and other practicing professionals. It is gratifying for our
team to note that our online First Edition has been heavily utilized as evidenced
by over 500,000 downloads, which of course is in addition to scientists’
utilization of the Encyclopedia and individual “spin-off” volumes in print.
Now we are pleased to have a Living Reference online which assures the
sustainability community that we are providing the latest peer-reviewed con-
tent covering the science and technology of the sustainability of the Earth. We
are also publishing the content as a Series of individual topical books for ease
of use by those with an interest in particular subjects, and with expert oversight
in each field to ensure that the Second Edition presents the state-of-the-science
today. Our team covers the physical, chemical, and biological processes that
underlie the Earth system including pollution and remediation and climate
change, and we comprehensively cover every energy and environment tech-
nology as well as all types of food production, water, transportation, and the
sustainable built environment.
Our team of 15 board members includes two Nobel Prize winners (Kroto
and Fischlin), two former Directors of the NSF (Colwell and Killeen), the
former President of the Royal Society (Lord May), and the Chief Scientist of
the Rocky Mountain Institute (Amory Lovins). And our more than 40 eminent
section editors and now book editors assure the quality of our selected authors
and their review presentations.
The extent of our coverage clearly sets our project apart from other publi-
cations which now exist, both in extent and depth. In fact, current compendia
of the science and technology of several of these topics do not presently exist
and yet the content is crucial to any evaluation and planning for the sustain-
ability of the Earth. It is important to note that the emphasis of our project is on
science and technology and not on policy and positions. Rather, policy makers
will use our presentations to evaluate sustainability options.
Vital scientific issues include: human and animal ecological support sys-
tems; energy supply and effects; the planet’s climate system; systems of
agriculture, industry, forestry, and fisheries and the ocean; fresh water and

v
vi Series Preface

human communities; waste disposal; transportation and the built environment


in general and the various systems on which they depend, and the balance of all
of these with sustainability. In this context, sustainability is a characteristic of a
process or state that can be maintained at a certain level indefinitely even as
global population increases toward 9 billion by 2050. The population growth,
and the hope for increase in wealth, implies something like a 50% increase in
food demand by as early as 2030. At the same time, the proportion of the
109 population that lives in an urban environment will go up from about 47%
to 60%. Global economic activity is expected to grow 500%, and global
energy and materials use is expected to increase by 300% over this period.
That means there are going to be some real problems for energy, agriculture,
and water, and it is increasingly clear that conflicting demands among biofuels,
food crops, and environmental protection will be difficult to reconcile. The
“green revolution” was heavily dependent on fertilizers which are
manufactured using increasingly expensive and diminishing reserves of fossil
fuels. In addition, about 70% of available freshwater is used for agriculture.
Clearly, many natural resources will either become depleted or scarce relative
to population.

Larkspur, CA, USA Robert A. Meyers, Ph.D.


July 2020 Editor-in-Chief
Volume Preface

Air pollution causes illness and death regardless of political boundaries. As of


the date of writing (May 2020), our world continues to face the coronavirus
(COVID-19) pandemic. There have been some preliminary observations that
emission and air pollution levels are falling, not unexpectedly, as society
restricts its activities via recommended measures to mitigate the spread of
the virus.
All of this is happening though at great human and societal costs. There is
therefore a pressing need to better understand the interplay of air pollution
sources, statistical analysis, and health effects. More than ever, it is critical to
have and deploy technologies that will help keep the air we breathe clean, both
through technologies that reduce harmful emissions as well as technologies
that keep the air that we breathe in enclosed spaces clean.
We are grateful for the contributions of the authors of this volume: those
who contributed foundational knowledge in the first edition and those who
have expanded the knowledge base for this volume with new or updated
contributions in the second edition. We appreciate the experts at all stages of
their careers who have shared their knowledge so that anyone may advance
their understanding of globally important issues.
We encourage the use of the Encyclopedia of Sustainability Science and
Technology and its Part Air Pollution Sources, Statistics and Health Effects for
teaching or for obtaining a foundational oversight of the important concepts
and technologies in the section. There is a wealth of knowledge relevant not
only in this volume but more broadly across the Encyclopedia, and we encour-
age those who found this part to browse other topics in the Encyclopedia.
This volume is suitable for a spectrum of readers: students in advanced
courses, academics and scholars of all experience levels, and practitioners and
policymakers in air pollution or public health science, engineering, or policy
making or related fields.
We are all very proud to be associated with the Encyclopedia of Sustain-
ability Science and Technology. The benefits of the Encyclopedia are many,
and at a time when several scientists and engineers may focus their efforts on
other types of scientific writing and many citizens may turn their reading to
sources on the Internet, the utility of this Encyclopedia should be commended.
The possibility to update the articles whenever research warrants and without
having to wait for a new edition to be published is both unique and important.

vii
viii Volume Preface

We stand committed to support this effort through a high-quality continu-


ous peer-review process as updates are warranted. We welcome contact from
those wishing to update articles, improve upon entries, or submit new entries to
this volume. This is important knowledge to maintain and improve and it can
only be done so through the efforts of those generous enough with their time
and expertise.
We are humbled and honored to have taken further the work started by the
editors and authors of the first edition. Thanks to the efforts of the authors and
the professional support of the editorial team, we are confident that this
updated edition will be beneficial to readers. We encourage readers to reach
out to authors to pursue more information.
While it was not our intention to promote the field per se, the current
epidemic underlines how important clean air is for life on our planet. We
encourage potential authors to start developing entries now, or reach out with
updates to the entries already part of this volume. It is our hope that the next
edition will bring an even greater number of updates and a renewed focus on
statistical analysis – including the fall in pollution levels due to global events
such as being currently experienced.
In addition to the authors we would like to thank the referees for their
contributions in improving the entries. We would also like to express our
gratitude and appreciation to the editorial team: Ms. Nanna Rahbek Jørgensen
of the University of Southern Denmark whose contribution to this effort was
nothing short of outstanding; the incredible team at Springer Nature:
Ms. Sunali Mull and Ms. Neha Thepa whose professionalism, assistance,
and patience to help make this a success cannot be understated. We would
also like to thank Professor Robert A. Meyers, the editorial team, and the
publisher for inviting us as the editors of this volume and for their assistance,
patience, and inspiration. Lastly, we would like to acknowledge our employers
and colleagues, students, and families for their support in working on this
section all of whom continue to provide helpful support and inspiration.

Adelaide, Australia Michael Evan Goodsite


Copenhagen, Denmark Matthew Stanley Johnson
Roskilde, Denmark Ole Hertel
September 2020
Contents

Air Pollution Sources, Statistics, and Health Effects:


Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
Ole Hertel, Matthew Stanley Johnson and Michael Evan Goodsite

Part I Ground Level Localized Air Quality . . . . . . . . . . . . . . . . . . . 5

Air Quality Guidelines and Standards . . . . . . . . . . . . . . . . . . . . . . . 7


Roger O. McClellan
Air Quality, Surface Transportation Impacts on . . . . . . . . . . . . . . . 47
Paul Boulter
Airborne Nanoparticles: Control and Detection . . . . . . . . . . . . . . . 85
Mohsen Rezaei and Matthew Stanley Johnson
Indoor Air Quality: Status and Standards . . . . . . . . . . . . . . . . . . . 135
Freja Hasager, Joachim Dithmer Bjerregaard, James Bonomaully,
Hasse Knap, Alireza Afshari and Matthew Stanley Johnson
Urban Air Quality: Meteorological Processes . . . . . . . . . . . . . . . . . 163
David Carruthers, Silvana Di Sabatino and Julian Hunt
Urban Air Quality: Sources and Concentrations . . . . . . . . . . . . . . 193
Michael Evan Goodsite, Ole Hertel, Matthew Stanley Johnson and
Nana Rahbek Jørgensen
Urban Atmospheric Composition Processes . . . . . . . . . . . . . . . . . . 215
William Bloss
Urban Drainage Modelling for Management of Urban
Surface Water . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 229
Birgitte Lilholt Sørensen

Part II Regional and Global Air Quality and Effects . . . . . . . . . . 237

Aerosol in Global Atmosphere . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 239


Colin O’Dowd

ix
x Contents

Air Pollution and Climate Change: Sustainability,


Restoration, and Ethical Implications . . . . . . . . . . . . . . . . . . . . . . . 279
Jiaying Chen, Mie Jul Dahlin, Linnea Luuppala, David Bickford,
Lina Boljka, Vanessa Burns and Matthew Stanley Johnson
Aviation and Atmosphere . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 327
Hartmut Grassl
Regional Air Quality . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 347
Erika von Schneidemesser and Paul S. Monks
Stratospheric Pollution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 373
Martyn P. Chipperfield

Part III Sensors, Measurement, and Control . . . . . . . . . . . . . . . . . 383

Air Pollution Monitoring and Sustainability . . . . . . . . . . . . . . . . . . 385


Andrew Knox, Greg J. Evans, Colin J. Lee and Jeffrey R. Brook
Low-Cost Sensors for Indoor and Outdoor Pollution . . . . . . . . . . . 423
Louise Bøge Frederickson, Emma Amalie Petersen-Sonn,
Yuwei Shen, Ole Hertel, Youwei Hong, Johan Schmidt and
Matthew Stanley Johnson
Measuring Heatwaves and Their Impacts . . . . . . . . . . . . . . . . . . . . 455
Benjamin Disher, Brandon Edwards, Thomas Lawler and
Douglas Radford
Industrial Emissions Control Technologies: Introduction . . . . . . . 477
Szymon Kwiatkowski, Merve Polat, Weijia Yu and
Matthew Stanley Johnson
Index . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 513
About the Editor-in-Chief

Robert A. Meyers
President: RAMTECH Limited
Manger, Chemical Process Technology, TRW Inc.
Post-doctoral Fellow: California Institute of Technology
Ph.D. Chemistry, University of California at Los Angeles
B.A., Chemistry, California State University, San Diego

Biography

Dr. Meyers has worked with more than 20 Nobel laureates during his career
and is the originator and serves as Editor in Chief of both the Springer Nature
Encyclopedia of Sustainability Science and Technology and the related and
supportive Springer Nature Encyclopedia of Complexity and Systems Science.

Education

Postdoctoral Fellow: California Institute of Technology


Ph.D. in Organic Chemistry, University of California at Los Angeles
B.A., Chemistry with minor in Mathematics, California State University,
San Diego

Dr. Meyers holds more than 20 patents and is the author or Editor in Chief of
12 technical books including the Handbook of Chemical Production Pro-
cesses, Handbook of Synfuels Technology, and Handbook of Petroleum

xi
xii About the Editor-in-Chief

Refining Processes now in 4th Edition, and the Handbook of Petrochemical


Production Processes, now in its second edition, (McGraw-Hill) and the
Handbook of Energy Technology and Economics, published by John Wiley
& Sons; Coal Structure, published by Academic Press; and Coal Desulfuri-
zation as well as the Coal Handbook published by Marcel Dekker. He served
as chairman of the Advisory Board for A Guide to Nuclear Power Technology,
published by John Wiley & Sons, which won the Association of American
Publishers Award as the best book in technology and engineering.
About the Editors

Michael Evan Goodsite, B.Sc.C.E., M.Sc.Env.E., MBA, Ph.D., FIEAust,


FIUPAC, MAusIMM, MAICD, is Full Professor of Civil and Environmental
Engineering, Interim Director of The Institute for Mineral and Energy
Resources (IMER), and the Director of the UoA Industry Engagement Priority
for Energy, Mining and Resources (reporting to the Provost in this role).
Professor Goodsite is Seconded from his role as Head of the School of Civil,
Environmental and Mining Engineering. He was Professor of Atmospheric
Chemistry, Climate and Global Processes at the University of Southern Den-
mark and formerly the Region of Southern Denmark’s Chief Operating Officer
with responsibility for Regional Development. A portfolio that included
Regional business development, environment, and natural resources. His
international university service includes Special Advisor to the Peking Uni-
versity Centre for Natural Resource Economics, China, Adjunct Professor at
the University of Iceland, and Honorary Senior Research Fellow to the Insti-
tute for Security and Development Policy (ISDP) in Stockholm, Sweden.
School of Civil, Environmental and Mining Engineering, The Australian
School of Petroleum, The University of Adelaide, Adelaide, SA, Australia

xiii
xiv About the Editors

Matthew Stanley Johnson, Ph.D., B.A., is Professor of Chemistry at the


University of Copenhagen and Chief Science Officer at Airlabs. His research is
in atmospheric chemistry, clean technology, and innovation. This work
includes the kinetics and spectroscopy of pollution and the development of
new pollution control systems. Professor Johnson has published more than
110 peer-reviewed journal articles, 8 patents, and the book Chemistry and the
Environment. He has received the Environmental Prize from the Aase og Ejnar
Danielsen Fond, the Innovation Prize from the University of Copenhagen, and
was voted Best Teacher by the students in the Department of Chemistry.
Professor Johnson has served as an Advisor for NASA and sits on the board
of the Villum (High Arctic) Research Station and Infuser, a successful spin-off
company from the University of Copenhagen.
Department of Chemistry, University of Copenhagen, https://scholar.goo
gle.se/citations?user¼CVtvNmQAAAAJ&hl¼en

Ole Hertel, D.Sc., Ph.D., M.Sc., B.Sc., is Deputy Head of Department, Head
of PhD Program, and Full Professor in the Department of Environmental
Science at Aarhus University. His research is air pollution modelling and
assessment of human exposure to air pollution. In recent years he has worked
with low-cost air pollution sensors for pollution mapping and personal expo-
sure monitoring. Professor Hertel has published more than 110 peer-reviewed
journal articles, more than 100 technical reports, almost 30 textbook contri-
butions, and he has contributed more than 200 conference presentations. He
has been involved in numerous national and international research projects
regarding assessment of air pollution impacts on human health, nature, and
climate. Professor Hertel is former Vice Chair of the Scientific Committee at
About the Editors xv

the European Environment Agency (EEA) and has served in several commit-
tees of the International Union for Pure and Applied Chemistry (IUPAC) and
for the Nordic Council of Ministers. He is Advisor to the Danish Ministry of
Environment, the Danish Ministry of Health, and Copenhagen Municipality.
Professor Hertel is member of editorial committees of several international
peer-reviewed journals. He is Adjunct Professor at the University of Roskilde,
Denmark.
Department of Environmental Science, Faculty of Science and Technology,
Aarhus University, Roskilde, Denmark
Contributors

Alireza Afshari Danish Building Research Institute, Aalborg University


Copenhagen, Copenhagen, Denmark
David Bickford Biology Department, University of La Verne, La Verne, CA,
USA
Joachim Dithmer Bjerregaard Department of Chemistry, University of
Copenhagen, Copenhagen, Denmark
William Bloss School of Geography, Earth and Environmental Sciences,
University of Birmingham, Birmingham, UK
Lina Boljka Department of Atmospheric Science, Colorado State University,
Fort Collins, CO, USA
James Bonomaully Airlabs, Copenhagen, Denmark
Paul Boulter PAEHolmes, Sydney, Australia
Jeffrey R. Brook Department of Chemical Engineering and Applied Chem-
istry, University of Toronto, Toronto, ON, Canada
Air Quality Research Division, Atmospheric Science and Technology Direc-
torate, Environment Canada, Toronto, ON, Canada
Vanessa Burns School of Geography and the Environment, University of
Oxford, Oxford, UK
David Carruthers Cambridge Environmental Research Consultants, Cam-
bridge, UK
Jiaying Chen Department of Chemistry, University of Copenhagen, Copen-
hagen, Denmark
Martyn P. Chipperfield Institute for Climate and Atmospheric Science,
School of Earth and Environment, University of Leeds, Leeds, UK
Mie Jul Dahlin Department of Chemistry, University of Copenhagen,
Copenhagen, Denmark
Silvana Di Sabatino Dipartimento di Scienza dei Materiali, Università del
Salento, Lecce, Italy

xvii
xviii Contributors

Benjamin Disher The School of Civil, Environmental and Mining Engineer-


ing, The University of Adelaide, Adelaide, SA, Australia
Brandon Edwards The School of Civil, Environmental and Mining Engi-
neering, The University of Adelaide, Adelaide, SA, Australia
Greg J. Evans Department of Chemical Engineering and Applied Chemistry,
University of Toronto, Toronto, ON, Canada
Louise Bøge Frederickson Department of Chemistry, University of Copen-
hagen, Copenhagen, Denmark
Airlabs, Copenhagen, Denmark
Michael Evan Goodsite School of Civil, Environmental and Mining Engi-
neering, The Australian School of Petroleum, The University of Adelaide,
Adelaide, SA, Australia
Hartmut Grassl Max Planck Institute for Meteorology, Hamburg, Germany
Freja Hasager Department of Chemistry, University of Copenhagen, Copen-
hagen, Denmark
Ole Hertel Department of Environmental Science, Aarhus University,
Roskilde, Denmark
Youwei Hong Institute of Urban Environment, Chinese Academy of Science,
Xiamen, China
Julian Hunt University College London, London, UK
Matthew Stanley Johnson Department of Chemistry, University of Copen-
hagen, Copenhagen, Denmark
Airlabs, Copenhagen, Denmark
Nana Rahbek Jørgensen Faculty of Engineering, University of Southern
Denmark, Odense M, Denmark
Hasse Knap Airlabs, Copenhagen, Denmark
Andrew Knox Department of Chemical Engineering and Applied Chemistry,
University of Toronto, Toronto, ON, Canada
Szymon Kwiatkowski Department of Chemistry, University of Copenhagen,
Copenhagen, Denmark
Thomas Lawler The School of Civil, Environmental and Mining Engineer-
ing, The University of Adelaide, Adelaide, SA, Australia
Colin J. Lee Department of Chemical Engineering and Applied Chemistry,
University of Toronto, Toronto, ON, Canada
Linnea Luuppala Social and Moral Philosophy, Department of Political and
Economic Studies, University of Helsinki, Helsinki, Finland
Roger O. McClellan Toxicology and Health Risk Analysis, Albuquerque,
NM, USA
Contributors xix

Paul S. Monks Department of Chemistry, University of Leicester, Leicester,


UK
Colin O’Dowd School of Physics and Centre for Climate and Air Pollution
Studies, Ryan Institute, National University of Ireland Galway, Galway,
Ireland
Emma Amalie Petersen-Sonn Department of Chemistry, University of
Copenhagen, Copenhagen, Denmark
Merve Polat Department of Chemistry, University of Copenhagen, Copen-
hagen, Denmark
Douglas Radford The School of Civil, Environmental and Mining Engineer-
ing, The University of Adelaide, Adelaide, SA, Australia
Mohsen Rezaei Department of Chemistry, University of Copenhagen,
Copenhagen, Denmark
Johan Schmidt Airlabs, Copenhagen, Denmark
Yuwei Shen Department of Chemistry, University of Copenhagen, Copen-
hagen, Denmark
Birgitte Lilholt Sørensen Institute of Chemical Engineering, Biotechnology
and Environmental Technology, SDU Life Cycle Engineering, University of
Southern Denmark, Odense M, Denmark
Erika von Schneidemesser Department of Chemistry, University of Leices-
ter, Leicester, UK
Weijia Yu Department of Chemistry, University of Copenhagen, Copenha-
gen, Denmark
air pollution levels have decreased substantially
Air Pollution Sources, Statistics, and in urban areas around the world because of reduced
Health Effects: Introduction travel and industrial activity. These improvements
in air quality have made real some of the improve-
Ole Hertel1, Matthew Stanley Johnson2,3 and ments that can be obtained from, e.g., moving
Michael Evan Goodsite4 towards a society less dependent on fossil fuels.
1
Department of Environmental Science, Aarhus Improved cleaning technologies are the result of
University, Roskilde, Denmark both pull and push strategies. This can be seen in
2
Department of Chemistry, University of the vehicle industry where strict emission stan-
Copenhagen, Copenhagen, Denmark dards have forced manufacturers to develop new
3
Airlabs, Copenhagen, Denmark technologies. These developments have been
4
School of Civil, Environmental and Mining important for improving air quality in many parts
Engineering, The Australian School of Petroleum, of the world over the past two to three decades.
The University of Adelaide, Adelaide, SA, Our knowledge about air pollution is based on
Australia data obtained from field measurements, labora-
tory studies, and air pollution modeling. It is
often through the combination of information
from these very different types of studies and
activities that new and deeper understanding is
Air pollution threatens our health, environment, and established. One example is our understanding
climate. The sources of air pollution are numerous of the pollution distribution inside urban street
anthropogenic and natural emissions; some are pol- canyons, achieved through painstaking analyses
lution in their own right, and some trigger the for- of data from monitoring stations in busy streets,
mation of secondary pollution. Detailed knowledge wind tunnel experiments, and models of traffic
of the sources of pollution and the transformations emissions, photochemistry, and air flow. Air pol-
of pollution in the atmosphere is the best possible lution assessments are often based on combina-
basis for effective and cost-effective management tions of measurements and model calculations. In
strategies. While this knowledge is the basis of reporting air quality levels in the scientific com-
environmental management as regards emissions munity, for industry and environmental agencies,
standards and best-practice pollution control sys- it is becoming standard practice to include indic-
tems, it is also critically important to society as it ative data from air pollution modeling. Indicative
seeks to adopt policies and behaviors to reduce air measurements are sometimes also included in
pollution and its associated impacts and direct such reporting based, e.g., on passive samplers
resources toward research and technological devel- with coarse temporal resolution. More recently a
opment to achieve sustainability. In fact, reducing variety of new low-cost sensor-based measure-
air pollution emissions and thereby improving air ment devices have been designed and deployed.
quality will help us to meet a series of United Electrochemical and metal-oxide sensors can pro-
Nations Sustainable Development Goals. Environ- vide high temporal and spatial resolution and may
mental pollution contributes to poverty, low crop be able to substantially extend the abilities of
yields, and disease, and the fight for resources established monitoring stations to investigate
leads to political instability. Thus, reducing air pol- local air pollution sources and remediation strate-
lution helps us achieve sustainability by reducing gies. It should be noted that such devices are not
poverty and inequality, providing jobs in the clean intended to replace high-quality monitors and
technology sector, and reducing and overcoming measurement stations since their precision
climate change. During the 2020 Corona crises, and accuracy are not sufficient for monitoring
© Springer Science+Business Media, LLC, part of Springer Nature 2021 1
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_911
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2020, https://doi.org/10.1007/978-1-4939-2493-6_911-3
2 Air Pollution Sources, Statistics, and Health Effects: Introduction

compliance with guideline values. The require- pollution with a variation on local spatial scales
ments for using such devices are that the measure- and typically with a shorter lifetime. This section is
ment range matches the range of ambient levels, of particular interest in pollution exposure, as obvi-
that their accuracy and precision are sufficiently ously, this is where people spend their time.
high, and that proper calibration and validation are The article ▶ “Air Quality Guidelines and
conducted. Standards” by McClellan details the regulatory
Since the Dockery and Pope studies in the US in framework used in air quality management.
the 1990s, it has been known that exposure to air There is growing recognition of the impacts of
pollution poses not only short-term (acute) but also shipping and railways on emissions and air qual-
long-term (chronic) health effects in the popula- ity, and Boulter’s entry ▶ “Air Quality, Surface
tion. Recent research by the Max Planck Institute Transportation Impacts on” seeks to quantify the
of Chemistry has established that the impact of air issues and place them in context.
pollution is on the scale of a global pandemic, Rezaei and Johnson’s ▶ “Airborne Nano-
causing the loss of 8.8 million lives annually. particles: Control and Detection” discusses the
Despite substantial improvements in many parts state of the art for the control and detection of
of the world, globally, air pollution is still the airborne nanoparticles. Unfortunately, given the
most hazardous environmental threat. The increas- increased attention they are receiving, the chemi-
ing quality of exposure assessments, access to new cal and physical properties of nanoparticles make
and better statistical methods, and more complete them a challenge to detect and control.
and precise health data have led to stronger associ- ▶ “Indoor Air Quality: Status and Standards”
ations between air pollution exposure and health (Hasager et al.) is an essential entry in terms of air
effects. More health endpoints have been added to pollution exposure, as people spend nearly 90% of
the list in recent years and health effects are seen at their time indoors.
lower pollutant levels that were previously known The meteorological processes leading to the
or even expected. During the 2020 Corona crises, it vertical mixing of pollutants after emission and
was even speculated, that the death risk related to their horizontal transport by the wind are
Corona infection may be strongly affected by described in the entry ▶ “Urban Air Quality:
simultaneous exposure to high air pollution levels. Meteorological Processes” by Carruthers, Di
Air pollution exposure-effect relationships have Sabatino, and Hunt. Computational models used
now been established for a wide variety of health to describe these processes are also included.
outcomes, and well documented through parallel ▶ “Urban Air Quality: Sources and Concentra-
studies in many countries around the world using a tions” by Goodsite, Hertel, Johnson, and
variety of approaches and methodologies. Assess- Jørgensen was updated to reflect the latest devel-
ments of the health effects in the population are opments with particular attention given recent
now performed on a routine basis in many coun- technological advances, as well as the latest
tries and by many agencies, and often these also research from around the world.
include calculation of externalities associated with The complementary entry ▶ “Urban Atmo-
the negative health effects. Again, such knowledge spheric Composition Processes” (Bloss) describes
is essential for pushing development towards a the key chemical reactions which serve both to
more sustainable society. limit the concentrations of toxic pollutants and
This book has been divided into three sections: control concentrations of secondary pollutants
such as ozone and airborne particles, important
• Ground-Level Localized Air Quality to human health and regional pollution.
• Regional and Global Air Quality and Effects Surface water links climate change and sus-
• Sensors, Measurement, and Control tainability with the human environment. Poor
management of urban surface water can have seri-
There are eight chapters in the section Ground- ous effects. The article by Sørensen, ▶ “Urban
Level Localized Air Quality that focus on Drainage Modelling for Management of Urban
Air Pollution Sources, Statistics, and Health Effects: Introduction 3

Surface Water” demonstrates how combining Release of long-lived pollutants at ground-level


technologies that have previously been taken sep- as well as aircraft emissions lead to ▶ “Strato-
arately can assist planners in the management of spheric Pollution” (entry by Chipperfield) with
urban surface water, an important climate adapta- consequences for stratospheric ozone concentra-
tion issue. tions, penetration of UV radiation to ground-level,
The next section, “Regional and Global Air and global climate.
Quality and Effects,” comprises five chapters The last section is titled “Sensors, Measure-
discussing the effects of air pollution in terms of ment, and Control” and comprises four chapters
global climate. that primarily focus on monitoring and controlling
Air pollutants comprise both gases and parti- air pollution.
cles. The latter are tiny airborne liquid or solid The entry ▶ “Air Pollution Monitoring and
droplets ranging from nanometers to tens or even Sustainability” (Knox, Evans, Lee and Brook)
hundreds of micrometers in size. The entry by discusses the design of monitoring networks and
O’Dowd ▶ “Aerosol in Global Atmosphere” how monitoring data can inform urban design and
details the impact of aerosol on climate. The air quality management policy. In addition to
impacts are numerous and complex, and aerosol monitoring networks, the monitoring of emissions
in the global atmosphere may have both warming sources and remote sensing of the atmosphere on
and cooling effects upon climate. regional scales from space play important roles.
Johnson et al.’s entry ▶ “Air Pollution and Frederickson et al.’s ▶ “Low-Cost Sensors for
Climate Change: Sustainability, Restoration, and Indoor and Outdoor Pollution” introduces low-
Ethical Implications” describes air pollution and cost methods for sensing indoor and outdoor pol-
its links to climate change, and in addition the lution. Sensing pollution is the key to monitoring,
profound philosophical and ethical quandaries mitigating and controlling it. The lower the cost,
created by our current dilemma. the greater the potential deployment, especially in
Aviation is a significant source of pollutant developing markets and as a way to increase the
emissions. Because of the altitude at which most spatial resolution of current measurement stations.
of these emissions occur, its effects on ground- Edwards, Lawler, Disher, and Radford’s article
level air quality are modest. The main conse- on ▶ “Measuring Heatwaves and their Impacts”
quences are due to aviation’s climate impacts, details heatwave events that are forecast to
arising from emissions of greenhouse gases and become more frequent and severe. Heatwaves
water vapor, described in Grassl’s entry ▶ “Avia- contribute to air pollution.
tion and Atmosphere.” Kwiatkowski, Polat, Yu, W, and Johnson, in their
As air pollutants are advected from urban entry ▶ “Industrial Emissions Control Technolo-
areas, they are subject to atmospheric transport gies: Introduction” explain novel and innovative
leading to impacts on ▶ “Regional Air Quality” technologies for controlling industrial emissions.
which have important human health and ecosys- The ‘solution to pollution’ is no longer dilution, it
tem effects, described in the entry of this name by is clean technology, applying basic science in anal-
von Schneidemesser and Monks. ogy to natural processes to industrial-scale issues.
Part I
Ground Level Localized Air Quality
guidance to the public and government on
Air Quality Guidelines and levels of air pollutant that will improve air
Standards quality.
Air quality monitoring Measurement of the
Roger O. McClellan concentration of various pollutants in air for
Toxicology and Health Risk Analysis, regulatory compliance or research purposes.
Albuquerque, NM, USA Ambient air Air found out of doors, which is a
mixture of gases and suspended particles and
droplets.
Article Outline Ambient concentration-response function A
mathematical description of the relationship
Glossary between ambient air concentrations and asso-
Definition of the Subject ciated morbidity or mortality indicators, usu-
Introduction ally expressed as increased risk for a defined
Air Quality Management Framework increment of increased pollutant.
Context for Air Quality Impacts Anthropogenic Causal by humans, man-made.
The US Legal Framework for Air Quality Background levels The concentration of a pol-
Standards lutant in the air after accounting for all local or
National Ambient Air Quality Standards regional emissions.
US Process for Setting National Ambient Air Biogenic Produced by biological processes.
Quality Standards Carbon monoxide The chemical, CO, that is a
Paradigm Shift product of incomplete combustion. It is regu-
WHO Process for Setting Air Quality Guidelines lated as a Criteria Air Pollutant or Common Air
Assessing Hazards and Risks Pollutant.
Sources of Information for Setting Standards and Emissions The quantities of pollutants emitted
Guidelines by a particular source or multiple sources.
Particulate Matter as an Example Excess risk Risk associated with exposure to an
Ozone agent over and above the baseline risk.
Current Air Quality Standards and Guidelines Exposure Taking materials into the body via
Future Directions inhalation, ingestion, or absorption through
Bibliography the skin.
Guidelines Guidance provided for use by the
Glossary public or government officials.
Hazardous The property of having the potential
Adverse health effect Alteration in the health to cause adverse health effects with sufficient
status of individuals or populations. duration and concentration of exposure.
Aerodynamic diameter The diameter of a Lead Pb, an element that occurs naturally and
spherical particle of unity density with a termi- found many uses including as a paint additive
nal velocity equal to the particle being and as tetraethyl Lead added to gasoline to
sampled. enhance engine performance. Regulated as a
Aerosol Relatively stable suspension of particles Criteria Air Pollutant or Hazardous Air
or droplets in a gaseous media. Pollutant.
Air quality guidelines AQG, established by Mobile sources Mobile sources, such as vehi-
World Health Organization to provide cles, of air pollution emissions.

© Springer Science+Business Media, LLC 2012 7


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_553
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_553
8 Air Quality Guidelines and Standards

Morbidity A statistical measure of number of Definition of the Subject


fractions of indicators of illness.
Mortality A statistical measure of number or Air quality is the state of the atmosphere in which
fraction of deaths. humankind lives and works. The air consists of a
National Ambient Air Quality Stand- complex mixture of gases and suspended droplets
ards NAAQS, established under the US and particles. Some of the gases, such as oxygen
Clean Air Act to protect health and welfare. and carbon dioxide, within rather tight concentra-
Nitrogen oxides NOx, a mixture of NO and NO2 tion limits, are essential for sustaining the life of all
produced in high-temperature combustion pro- living things. Some of the gases and aerosol parti-
cesses. Regulated as a Criteria Air Pollutant or cles and droplets, when certain concentrations are
Common Air Pollutant. exceeded and with sufficient duration of exposure,
Ozone O3, a molecule with three atoms of oxy- may have adverse effects on humans and other
gen. It is highly reactive with other chemicals living things, including vegetation. Various gov-
and biological systems. It is regulated as a ernmental agencies around the world have devel-
Criteria Air Pollutant or Common Air Pollutant. oped air quality guidelines and standards for
Particulate matter Airborne solid material, ambient or outdoor air quality. These guidelines
unspecified as to chemical composition, regu- or standards, when achieved or attained, are
lated as a Criteria Pollutant or Common Air intended to be protective of human health and
Pollutant. minimize the potential for other effects such as
Particulate matter, 10 mm PM10, airborne partic- impacts on visibility or plants. Some government
ulate material included in sampled air size frac- entities and statutes characterize the guidelines as
tion with aerodynamic size of 10 mm and less. goals to be attained, while other government enti-
Particulate matter, 2.5 mm PM2.5, particulate ties and statutes treat them as rigid standards which
material included in sampled air size fraction are legally enforced. Guidelines or standards, when
with an aerodynamic size of 2.5 mm or less. attained, are intended to improve the quality and
Primary standards or guidelines Air Quality sustainability of human life.
Standards or Guidelines for Criteria or Com-
mon Pollutants set to protect public health.
Risk The probability of an adverse health out- Introduction
come associated with exposure to a hazardous
material for a defined period of time and expo- The quality of the air that people live in and
sure level. Usually expressed as a level of breathe has no doubt been of concern to people
adverse effect, morbidity, or mortality, over since early in the evolution of humans. This con-
and above background. cern, which must have preceded recorded history,
Risk assessment The analytical process of eval- likely coincided with man’s use of purposeful
uating exposure and the hazard potential of a combustion, fire, for cooking and heating and
material to estimate risk. ultimately, for manufacturing and other activities,
Secondary standards or guidelines Air Quality including transportation. There is abundant evi-
Standards or Guidelines for Criteria or Com- dence that early humans found it convenient to
mon Air Pollutants set to protect public welfare live in caves both for shelter and safety. The poor
such as visibility or effects on plants. quality of the air is apparent from the residual soot
Standards Regulations that are legally binding. coating the interior of caves used as dwellings.
Stationary sources Fixed sources of air pollu- Indeed, pictographs of the interior of the caves
tion emissions such as power plants. provide documentation of aspects of the life of
Sulfur dioxide SO2, released from combustion those early cave dwellers. As community life
of sulfur-containing fossil fuels. It is regulated evolved, people continued to live and use fire for
as a Criteria Air Pollutant or Common Air both cooking and heating in poorly ventilated
Pollutant. dwellings.
Air Quality Guidelines and Standards 9

Domestication of both plants and animals reputed to have given rise to the term smog, a
played a critical role in the development of contraction of smoke and fog.
agriculture-based societies and the growth of The development of steam engines soon led to
communities. The agricultural base influenced their use in sea-going vessels that initially
the size of communities and their proximity to depended heavily on coal as a fuel. Later, coal
one another. The ability to transport essential would be replaced by oil as a fuel. Emissions from
foodstuffs by ship or overland by horses, camels, ships did not attract major attention until the late
and oxen allowed cities to emerge. With larger twentieth century when concern developed for air
communities came increased air pollution and emissions when the ships were near land and
the impact of an individual family’s pollution on especially when in harbor.
their neighbors and vice versa. With the discovery of electricity a revolution
Coal apparently was first used as a fuel in the occurred in the generation and use of energy.
Far East. The introduction of coal as an energy More appropriately, it is the conversion of energy
source in the Western world followed Marco from one form to another, for example, from coal
Polo’s return to the west from his trip to the to thermal energy to electric energy that could be
more advanced societies of the Far East. As easily transmitted. It was now possible to generate
early as the thirteenth century, there was concern electricity with coal as an energy source at one
over coal smoke and odor in London, and the location and transport it over long distances for
Queen of England reportedly moved from use at multiple locations. Over the course of the
London to Nottingham because of the insufferable twentieth century the generation of electricity
smoke. In 1661, John Evelyn published from the combustion of fossil fuels in large
Fumifugium: Or the Inconvenience of the Air power plants continuously grew, first in heavily
and Smoke of London Dissipated, which drew industrialized countries and, ultimately, around
attention to the problem for air pollution. the world.
The industrial revolution in the early years was In the 1900s, a series of incidents drew atten-
dependent on wood as a fuel, and therefore, indus- tion to air pollution as a serious and even acute
try was located near forests. This restriction health problem. In December 1930, static atmo-
served as a throttle on industrial development. spheric conditions in the Meuse Valley of Bel-
The development of effective steam engines in gium resulted in pollution that caused over
the eighteenth century provided a major impetus 60 deaths and hundreds of illnesses. In December
for the use of coal as a fuel. With coal, the pace of 1952, smog in London resulted in about 4,000
industrial activity increased, and factories devel- deaths, principally among the infirm, the old,
oped near sources of coal and along the waterways and those with respiratory diseases. The effects
that served to efficiently transport the coal. The were not restricted to humans. Acute respiratory
smoke and ash from coal-fired boilers in factories, symptoms were also reported in cattle at the
power plants, and locomotives increasingly Smithfield Club livestock show. The effects may
became of concern. Interestingly, this concern have been most severe in the heavy-weight prize
about air pollution was stimulated by impairment cattle, who were well cared for and had their litter
of visibility and soiling as well as effects on and excreta promptly removed. Other cattle that
health. In addition, the damage to vegetation were not as well cared for apparently fared better,
from emissions produced in the smelting of sul- perhaps because of some benefits of ammonia
fide ores gave clear evidence of yet another effect from the excreta neutralizing the effects of sulfur
of air pollution. Air pollution problems were rec- oxides and sulfuric acid. Another major smog
ognized in many industrial countries in the late episode in London during December 1962
nineteenth century, but the problem was probably resulted in 340 deaths.
nowhere as apparent as in London. The high In October 1948, a particularly calm and stable
levels of pollutants combined with the notorious meteorology in Donora, Pennsylvania, about
London fog created a serious problem and is 30 km from Pittsburgh, PA, resulted in a 4-day
10 Air Quality Guidelines and Standards

buildup in levels of oxides and inorganic sulfates many of the basic concepts of aerosol science
from the local steel and zinc smelters. More than and inhalation toxicology trace their roots to
20 individuals died and 6,000 people developed those research efforts.
respiratory problems. The official government The post-World War II era brought with it an
report [57] on the Donora episode noted that the increased awareness of air pollution arising from
health effects were likely related to a combination another source – motor vehicles. Perhaps nowhere
of contaminants and identified sulfur dioxide as a was this more the case than in the Los Angeles
chief culprit. The word smoke did not appear in basin with its marked increase in population,
the report. The attention previously focused on industry, and cars. As concern increased for the
smoke was now broadening to include other air- Los Angeles smog in the late 1940s and 1950s, the
borne materials and, indeed, more broadly to air name “Bay of Smokers,” which was coined in
quality. 1542 by Juan Rodrigues Cabrillo for San Pedro
Despite early concerns about whether airborne Bay, took on a contemporary tone. Haagen-Smit
materials could cause disease, relatively little [25] of the California Institute of Technology
research was conducted prior to World War I to reported the scientific basis for photochemical
improve our knowledge of the relationship smog – reactions among oxides of nitrogen and
between the air pollution and disease. The unfor- hydrocarbons from vehicle exhaust in the pres-
tunate use of poisonous gases in World War ence of sunlight produced ozone and other photo-
I provided a stimulus for developing a better chemical oxidants that were the key components
understanding of how these specific agents pro- of Los Angeles smog. It is noteworthy that his
duced disease. Unfortunately, the meager litera- early research was motivated by understanding
ture generated indicates that research in this area the effects of smog on citrus fruit production.
was not substantial or very long-lasting. In retro- Haagen-Smith’s findings were another key factor
spect, the lack of research related to airborne in broadening the concern for air quality from
toxicants is probably not surprising considering smoke to ozone and other air contaminants.
the generally low level of biomedical research Post WWII then was a major and continuing
activity in the first third of the twentieth century. increase in the use of airplanes both to transport
The strong preventive medicine orientation that people and goods. Indeed, transport of goods by
exists today toward diseases of both occupational aircraft is a central element of the global economy
and environmental origin had not yet developed. that emerged in the latter part of the twentieth
Between World War I and World War II, con- century. As with ships, aircraft as sources of air
cern for airborne materials impacting on human pollution did not attract much attention in the late
health centered primarily on occupational expo- twentieth century when attention began to focus
sures. World War II brought with it renewed con- on air quality in the vicinity of major airports. In
cern for purposeful exposures of people to toxic the case of some areas, such as the Los Angeles
gases and biological agents. In both the United International Airport and a nearby harbor, concern
Kingdom and the United States, major research has developed for the contribution of multiple
efforts were conducted to better understand the sources: aircraft, cargo ships, locomotives, trucks,
effects of these agents thereby providing and passenger cars.
improved approaches to defending against their So far the discussion has centered on air pollu-
use and effects. World War II also brought with it tion from combustion of hydrocarbons, from
major research efforts focusing on the potential recently fixed carbon in wood and other plant
toxic effects of uranium and newly discovered materials to the fossil fuel energy sources, coal,
radionuclides such as plutonium and fission prod- oil, and natural gas, created in earlier geologic
uct related to the manufacture and use of nuclear eras. With each of these fuel sources hydrocar-
weapons and, later, the development of nuclear bons are combusted releasing thermal energy, CO,
reactors as energy sources to generate electrical CO2, H2O, variable amounts of Nitrogen Oxides,
power. These activities are noteworthy since and traces of other elements.
Air Quality Guidelines and Standards 11

There are non-hydrocarbon-based energy sys- everywhere. These common air pollutants are iden-
tems that do not depend on combustion of hydro- tified as criteria pollutants in the Clean Air Act, the
carbons that deserve mention. This includes wind, principal statute governing air quality in the United
hydro, nuclear, and solar power. Some of these States [14]. Some of these same pollutants have
such as wind and water have been in use for been identified by the World Health Organization
centuries to provide power. Nuclear power had (WHO) as common air pollutants [94].
its advent post-WWII. Solar power with its cur-
rent focus on photovoltaic conversion is relatively
new. All of these systems have the advantage of Air Quality Management Framework
not creating airborne emissions related to combus-
tion. However, each of these energy sources has Air quality guidelines and standards are a key
its own disadvantages related to potential impacts element of air quality management as practiced
on human health and ecosystems. around the world. Bachmann [7] provides an infor-
It is important to recognize that there are a mative historical review of the evolution of air
multitude of other industrial and personal activi- quality management in the United States with par-
ties beyond combustion of hydrocarbons that ticular emphasis on the National Ambient Air
result in air emissions that may be harmful to Quality Standards (NAAQS). A conceptual frame-
human health and ecosystems. These range from work for Air Quality Management is depicted in
mining and extraction of minerals to processes Fig. 1. Air quality goals, which may be expressed
producing specialized products such as paper, as air quality guidelines or standards, are the
fabric, silicon chips, and chemicals to the manu- drivers for all the other elements of the framework.
facture of vehicles and other commercial goods. Emissions from various sources are considered
Agricultural activities also have unique airborne within the context of the guidelines or standards.
emissions. Each of these activities require variable Are specific sources or kinds of sources significant
amounts of energy and, thus, contribute to the contributors based on estimates of emissions? If so,
potential for local emissions of combustion prod- what strategies can be used to reduce their emis-
ucts or emissions at a remote location such as a sions? Do source permits have a role in setting
central facility producing electrical power. In emission limits? Ambient monitoring can be used
addition, each of these activities has airborne to provide an overall assessment of air.
emissions unique to the processes being used. Quality and, perhaps, over time monitoring can
The focus of this entry is on the pollutants that establish whether the intended improvements in air
arise from multiple sources and, thus, are found quality are being achieved. The total air quality

Air Quality Guidelines


and Standards, Establish Air
Quality Goals Determine Emissions
Fig. 1 Conceptual
Monitoring Inventories
framework for air quality
Standard Analysis and Modeling
management
Guidelines
Scientific
Research and Develop Programs to
Track and Technological Reduce
Evaluate Development Emissions and Achieve
Results Goals

Monitoring
Implement and Identify Sources
(emissions and
Enforce Control Allocate Reductions
ambient Air)
Strategies Create Plans to
Receptor
Achieve Reductions
Modeling
Source Permits Compliance
12 Air Quality Guidelines and Standards

management cycle shown should be viewed as an standards and guidelines is the treatment of spe-
integrated system. The system is dynamic with cific concentrations of agents in ambient air as
new sources being introduced, old sources surrogates for human health. Air quality can be
retrofitted with controls, and some sources readily characterized with an appropriately
removed. In addition, as I will discuss later, the designed monitoring scheme for multiple air pol-
guidelines and standards are periodically reviewed lutants. In contrast, it is challenging to attempt to
and the concentration levels reduced. As some determine the association between specific risk
would say, the goal posts are constantly being factors, such as air pollution, and the health
moved to lower concentrations making it more response of an individual. This is especially the
challenging to achieve success and declare victory. case for current ambient concentrations of air
As will be discussed later, how low is low enough? pollutants in industrialized countries, concentra-
Another key concept embedded within the air tions substantially reduced from those observed
quality management system is the linkage from only a few decades ago. Even when the focus of
sources to health responses illustrated in Fig. 2. research investigations shifts from individuals to
The schematic rendering in the figure is a general large populations, it is a challenge to characterize
concept not exclusively linked to air pollution. an association between a specific air pollutant and
The goal of air quality management is to have a increased probability of a specific kind of
positive impact on human health responses, the response compared to a baseline. It is rarely pos-
endpoint at the right of the figure. As illustrated in sible to establish a causal relationship.
Fig. 3, multiple factors, not just air quality, influ- The complexity of relationships between sources
ence human health. Thus, in a specific sense, the of air pollution and health responses can be readily
goal is to minimize the health impacts of air pol- grasped by considering Fig. 4. In this figure, the
lution relative to all the other factors that influence concept of outdoor versus indoor exposures is intro-
human health while achieving an overall improve- duced. The situation with regard to indoor exposures
ment in health. Implicit in the setting of air quality is even more complicated than may initially appear.

RISK COMMUNICATION
Effectively communicate the total risk process and risk characterization to all
stakeholders

RISK RESEARCH RISK ASSESSMENT RISK MANAGEMENT


Understanding the 1. Hazard Identification Risk management
mechanistic linkages 2. Exposure, Dose, and decisions incorporate
between sources of Response Assessment the results of risk
toxicants, exposure, 3. Exposure Assessment characterizations and
dose, and response 4. Risk Characterization public health, economic
5. Identification of social and political
Research Needs considerations

Action
Identification of Research Needs

Air Quality Guidelines and Standards, Fig. 2 The risk paradigm


Air Quality Guidelines and Standards 13

Workplace As noted earlier (Fig. 3) multiple factors influence


the health of each individual and, in turn, the health
Personal Health of populations. Each individual has its own unique
Lifestyle Care
Choices genetic background inherited from its parents. That
genetic background can have a profound influence
on the individual’s potential health status through-
Personal Public out their life. Each of the other factors shown in the
Environment Environment diagram can have a significant influence on the
health status of an individual. Income and, more
Genetics broadly, socioeconomic status are important fac-
tors influencing health.
Air Quality Guidelines and Standards, Fig. 3 Multiple
factors influencing the health status of individuals and
The role of income and environmental factors
populations are intertwined. This is readily apparent from con-
sidering Table 1 [31]. This table reports an analy-
sis of the health impact of various risk factors in
This is the case because most individuals, during the
low- and middle-income countries versus high-
course of their daily lives, spend variable amounts of
income countries [31]. Urban air pollution and
time in multiple indoor environments: home (their
indoor smoke from household use of solid fuels
bedroom, kitchen, living room, etc.), workplace,
are identified as risk factors. Taken together these
school, automobile, etc. Each of these micro-
two air pollution risk factors account for 5.2% of
environments may have a different mix of air pol-
deaths in low- and middle-income countries ver-
lutants, both as to kind and concentration, arising
sus 1.0% of deaths in high-income countries, the
from multiple sources. Some variable portion of the
latter related exclusively to urban air pollution.
indoor pollution may also arise from outdoors, the
It is important to recognize that the role of
ambient environment.
socioeconomic status influencing health is a com-
The outdoor air pollution arises from multiple
plex issue. Steenland et al. [59] have analyzed this
sources, some local, some regional, and some
issue for the US population and their findings are
quite remote. Indeed, it is increasingly apparent
summarized in Table 2. Several points can be made
that emissions arising in one continent such as
using these findings. First, even for a country like
Asia soon reach North America and then Europe.
the United States, typically identified as high-
The air trajectory of emissions from coal-fired
income, there are gradients in socioeconomic sta-
power plants in the Midwest extending to the
tus and these have associated substantial gradients
Northeastern United States is well known. Dust
in health outcomes. Keep in mind the relative risks
originating from deserts in China regularly
on the order of 2.0 when the relative risks of
reaches the United States and Europe. Dust orig-
particulate matter and ozone are discussed. It is
inating from the Sahara Desert also regularly cir-
obvious that the national good will be served by
culates around the globe.
improving the socioeconomic status of the total
population. Second, a multitude of factors have a
role in influencing the health status of the individ-
Context for Air Quality Impacts uals in the lower quartile. Poor air quality to the
extent it is experienced more by individuals in the
Although the focus of this entry is on air quality lower quartile than in the upper quartile may be one
and its influence on human health, it is important of those factors. The substantial influence of socio-
that context be provided for considering the role of economic status on health emphasizes the impor-
air pollution on human health. The introductory tance of attempting to control for it as a variable in
chapter by Ayres et al. [5] in the textbook on epidemiological studies of air pollution and to
Environmental Medicine [6] provides a useful report findings on it to provide perspective for the
review of the multiple factors influencing health. reported effects of air pollution.
14 Air Quality Guidelines and Standards

Industrial Cooking & combustion


Commercial Particle re-suspension
Urban Hobbies
Outdoor Indoor
Mobile Work activities
Sources Sources
Regional Indoor activation
Agricultural Consumer products
Natural Building materials
Heating

Infiltration
Dispersion
Exfiltration
Transformation
Deposition
Deposition
Chemical Reactions

Outdoor Indoor
Concentrations Concentrations

Microenvironmental
Concentrations

Time-Activity
Data

Personal
Exposures

Dose

Internal Dose

Biologically
Effective Dose

Health
Responses

Air Quality Guidelines and Standards, Fig. 4 Schematic rendering of the relationship between outdoor and indoor
sources, personal exposure, biologically effective dose and health responses. (Adapted from Özkaynak [50])
Air Quality Guidelines and Standards 15

Air Quality Guidelines and Standards, Table 1 Deaths by cause: low- and middle-income countries, high-income
countries, and world, 2001
Low- and middle-income High-income World
deaths deaths deaths
Total number (thousands) 48,351 7,891 56,242
Rate per 1,000 population 9.3 8.5 9.1
Age-standardizeda rate per 1,000 11.4 5.0 10.0
Risk factor Number in thousands (percent)
Childhood and maternal undernutrition
Childhood underweight 3,630 (7.5) 0 (0.0) 3,630 (6.5)
Iron-deficiency anemia 613 (1.3) 8 (0.1) 621 (1.1)
Vitamin A deficiency 800 (1.7) 0 (0.0) 800 (1.4)
Zinc deficiency 849 (1.8) 0 (0.0) 849 (1.5)
Other nutrition-related risk factors and Physical activity
High blood pressure 6,223 (12.9) 1,392 (17.6) 7,615
(13.5)
High cholesterol 3,038 (6.3) 842 (10.7) 3,880 (6.9)
Overweight and obesity 1,747 (3.6) 614 (7.8) 2,361 (4.2)
Low fruit and vegetable intake 2,308 (4.8) 333 (4.2) 2,641 (4.7)
Physical inactivity 1,559 (3.2) 376 (4.8) 1,935 (3.4)
Addictive substances
Smoking 3,340 (6.9) 1,462 (18.5) 4,802 (8.5)
Alcohol use 1,869 (3.9) 24 (0.3) 1,893 (3.4)
Illicit drug use 189 (0.4) 37 (0.5) 226 (0.4)
Sexual and reproductive health
Unsafe sex 2,819 (5.8) 32 (0.4) 2,851 (5.1)
Nonuse and use of ineffective methods of 162 (0.3) 0 (0.0) 62 (0.3)
contraception
Environmental risks
Unsafe water, sanitation, and hygiene 1,563 (3.2) 4 (<0.1) 1,567 (2.8)
Urban air pollution 735 (1.5) 76 (1.0) 811 (1.4)
Indoor smoke from household use of solid fuels 1,791 (3.7) 0 (0.0) 1,791 (3.2)
Other selected risks
Contaminated injections in health care setting 407 (0.8) 4 (<0.1) 412 (0.7)
Child sexual abuse 65 (0.1) 6 (<0.1) 71 (0.1)
All selected risk factors together 22,014 (45.6) 3,473 (44.0) 25,488
(45.3)
Source: Adapted from [31]
a
Age-standardized using the WHO World Standard Population

Figure 5 provides a related perspective by ischemic heart disease, and lung cancer. The first
contrasting environmental with non-environ- three of these conditions account for about 4% of
mental contributions to specific categories of the total global burden disease in disability-
disease using disability-adjusted life years as an adjusted life years while lung cancer accounts
endpoint [55]. The merits of monetizing risks and for about 1%. Air pollution is generally viewed
benefits as statistical life-years versus lives have as a contributor to global disease burden. How-
been reviewed by Sunstein [61]. Of special note ever, its contribution needs to be placed in
are four diseases: lower respiratory infections, perspective relative to other major contributors
chronic obstructive pulmonary disease (COPD), to ill health.
16 Air Quality Guidelines and Standards

Air Quality Guidelines


Mortality rate ratio ¼ highest
lowest quartile
quartile of socioeconomical status
and Standards,
Table 2 The impact of Mortality Men Women
socioeconomic status on All cause 2.02 (1.95–2.09)a 1.29 (1.25–1.32)
mortality
Heart disease 1.88 (1.83–1.93) 1.84 (1.76–1.93)
Stroke 2.25 (2.14–2.37) 1.53 (1.44–1.62)
Diabetes 2.19 (2.07–2.32) 1.85 (1.72–2.00)
COPD 3.59 (3.35–3.83) 2.09 (1.91–2.30)
Lung cancer 2.15 (2.07–2.23) 1.31 (1.25–1.39)
Breast cancer – 0.76 (0.73–0.79)
Colorectal cancer 1.21 (1.16–1.27) 0.91 (0.86–0.96)
External causes 2.67 (2.58–2.78) 1.41 (1.35–1.48)
Source: Steenland et al. [59]
a
95% confidence interval

Diarrhoea
Lower respiratory infections
Other unintentional injuries
Malaria
Road traffic injuries
COPD
Perinatal conditions
Ischaemic heart disease
Childhood cluster disease
Lead-caused mental retardation*
Drownings
HIV/AIDS
Malnutrition
Cerebrovascular disease
Asthma
Tuberculosis
Suicide
Depression
Poisonings
Falls
Hearing loss
Violence
Lymphatic filariasis
Lung cancer
0% 1% 2% 3% 4% 5% 6% 7%

Fraction of total global burden of disease in DALYs

Environmental fraction Non-environmental fraction

COPD, Chronic obstructive pulmonary disease.


* Lead-caused mental retardation is defined in the World Health Organization list of diseases for 2002,
accessed at: www.who.int/evidence.
DALYs represent a weighted measure of death, illness and disability.
For each disease, the fraction attributable to environmental risks is shown in black,
Grey plus black represents the total burden of disease.

Air Quality Guidelines and Standards, disability-adjusted life-year, HIV human immunodefi-
Fig. 5 Diseases with the largest environmental contribu- ciency virus. (Adapted from Pruss-Ustun and Corvalan,
tion. AIDS acquired immune deficiency syndrome, DALY with permission)
Air Quality Guidelines and Standards 17

In this entry, there is a focus on the development United States concerned with air quality [14]. The
of air quality standards in the United States since, to original CAA [14] directed the then Department of
a large degree, these activities have served as a Health, Education and Welfare (HEW) to “compile
template for other countries. For comparative pur- and publish criteria on the effects of air pollutants,”
poses, the World Health Organization’s Air Quality hence the identification of “criteria pollutants” and
Guidelines have also been summarized. Reference “criteria documents” summarizing the scientific
will be made at several junctures to the distinction knowledge on certain air pollutants arising from
between guidelines providing guidance for multiple sources and found across the United
policymakers versus standards that are legally bind- States. The National Air Pollution Control Admin-
ing and, in turn, may mandate certain actions. The istration (NAPCA) within HEW was initially
omission of detailed discussions of guidelines and assigned responsibility of administering the CAA.
standards as developed and used in other countries The role of NAPCA was strengthened with the
around the globe is not intended as a judgment of CAA Amendments of 1967. However, in the
their quality or utility. absence of a specific time schedule progress
remained slow. A single document on SO2 was
developed [32]. When the US Environmental Pro-
The US Legal Framework for Air Quality tection Agency (EPA) was created in 1970 by
Standards consolidating numerous existing federal agencies,
responsibility for administering the CAA was
As concern mounted for the poor quality of air, effectively transferred from NAPCA to the EPA.
citizens increasingly turned to the government to In 1970, almost coincident with creation of the
enact laws to restrict emissions and improve air US Environmental Protection Agency, major
quality [7, 60]. Bachmann’s perspective is of special amendments to the CAA were passed that opened
interest since as a US EPA employee for more than a new era in managing air quality in the United
three decades, he had a central role in the setting of States [15]. The Clean Air Act as amended is a
NAAQS. Readers interested in legal details of the very broad piece of legislation. The sections deal-
Clean Air Act and NAAQS will find the summary ing with the establishment of National Ambient
of Martineau and Novello [33] useful. Initially, these Air Quality Standards are a key part of the Act and
air quality initiatives were focused at the local level are viewed by many individuals as the core of the
in major cities around the world. In the United Act. Other sections of the Act provide authority
States, heavily industrialized cities, such as Pitts- for implementing processes to achieve attainment
burgh, Chicago, Philadelphia, and Detroit, enacted of the NAAQS and otherwise in improving air
legislation setting local standards. In most cases, quality. This includes a delegation of responsibil-
these early standards focused on smoke. ity to the individual States for taking steps to attain
By the mid-twentieth century in the United the NAAQS. This includes the development of
States, it had become apparent that local efforts State Implementation Plans if the States have
on air pollution control were not sufficient, and areas that are not in attainment with regard to
complementary efforts were needed at the state or any specific NAAQS as evaluated by the concen-
national level. At the national level in the United tration and statistical form of the Standard.
States post-WWII, the lead agency for air quality Other sections of the Act address both Station-
was the Division of Air Pollution of the Public ary and Mobile Sources and the control of their
Health Service within the Department of Health, emissions. This includes specific emission stan-
Education and Welfare. The Air Pollution Control dards for vehicles and provision for issuance of
Act of 1955 [60] provided funding to the PHS for fuel efficiency goals that in the course of being
air pollution control research and to support the achieved impact on air quality. The rigid “com-
state’s efforts. However, the impact of this Act on mand and control” and standard-setting approach
progress in managing air quality was limited. of the United States contrasts sharply with the
In 1963, the Clean Air Act (CAA) was passed, guidance approach taken by the World Health
which became the principal national statute in the Organization (WHO).
18 Air Quality Guidelines and Standards

National Ambient Air Quality Standards particular, Congress noted that the Standards
should protect “particularly sensitive citizens
Section 108 of the amended CAA specifies the such as bronchial asthmatics and those with
development of scientific criteria for certain air emphysema who in the normal course of daily
pollutants. It specifies that the Administrator pub- activity are exposed to the ambient environment.”
lish a list for pollutants: (a) which have an adverse This has been interpreted to exclude individuals
effect on public health or welfare, and (b) which who are not performing normal activities, such as
are derived from numerous or diverse mobile or individuals who are hospitalized. Further guid-
stationary sources. It explicitly states – “the ance was given noting that the Standard is statu-
criteria shall accurately reflect the latest scientific torily sufficient whenever there is “an absence of
knowledge on the kind and extent of all identifi- adverse effect on the health of a statistically
able effects on public health and welfare which related sample of persons in sensitive groups
may be expected from the presence of the pollut- from exposure to the ambient air.”
ant in ambient air, in varying quantities” [15]. The challenge of interpreting the “adequate
Section 109 of the CAA [15] directs the margin of safety” language of the CAA was noted
Administrator to propose and promulgate “pri- in an editorial by Donald Kennedy on Risk versus
mary” and “secondary” NAAQSs for criteria pol- Risk published when he served as Editor-in-Chief
lutants identified under Section 108. The primary of Science [27]. He wrote – “In the United States
Standards are to be set to protect public health; and some other industrial democracies, where peo-
secondary Standards are to be set to protect the ple and their governments tend to be risk averse,
public welfare such as effects on soils, water, legislatures, courts, and administrative entities usu-
crops, visibility, and deterioration of property. In ally create a presumption favoring more safety
this entry, I focus on the setting of the primary rather than less. The definitions of risk in law are
Standards and on the specific NAAQS. However, often vague (‘reasonable certainty of no harm’ or
the issues discussed are also broadly applicable to ‘adequate margin of safety’) and are likely to
the setting of secondary Standards. encourage an unrealistic belief that risks can be
Section 109(b)(1) defines a primary NAAQS minimized or even eliminated altogether.” I think
as one that “the attainment and maintenance of Kennedy has captured the conundrum posed by the
which in the judgment of the Administrator, based language of the CAA, a conundrum that has been
on the criteria and allowing an adequate margin of addressed by US Supreme Court Justice Stephen
safety, is requisite to protect the public health.” Breyer as I will relate later.
The margin of safety, as interpreted by the EPA, is In 1977, several key amendments were made
intended to address uncertainties associated with to the CAA [16]. Concern about slow action of the
inconclusive scientific and technical information EPA in preparing criteria documents and
at the time the Standard is set and to account for reassessing NAAQSs prompted a legislated
hazards that research has not yet identified. requirement that the NAAQSs be reevaluated not
The primary Standards are intended to protect later than January 1, 1980, and at 5-year intervals
against “adverse effects, not necessarily against thereafter. Reevaluation was not intended to auto-
all identifiable effects of changes produced by a matically result in changes in the NAAQSs for a
pollutant.” Although the US Congress did not pollutant; rather, reevaluation was intended to
rigorously define an adverse effect, it did provide ensure that the scientific database was reviewed
general guidance in the legislative history of the and that the NAAQSs were consistent with cur-
debate on the CAA [30]. Congress was concerned rent knowledge. To my knowledge, this require-
with effects ranging from cancer, metabolic and ment for mandatory review every 5 years is
respiratory disease, and impairment of mental unique to the setting of the NAAQS in the United
processes to headaches, dizziness, and nausea. States. Indeed, I know of no other statute calling
Congress also noted concern for sensitive pop- for an updating of the science and reconsideration
ulation groups in setting the NAAQSs. In of the Standard every 5 years.
Air Quality Guidelines and Standards 19

Peer review of the earliest criteria documents and non-methane hydrocarbons (later dropped as
prepared by the EPA was carried out by various a criteria pollutant). The EPA [64] established
committees of the agency’s Science Advisory NAAQS for these pollutants soon after the
Board. The 1977 amendments to the CAA insti- Agency was created using existing scientific doc-
tutionalized the peer-review process for the umentation, that is, criteria. The original NAAQS
NAAQS [16]. The amendment requires the EPA set in 1971 are shown in Table 3. As I will discuss
Administrator to appoint an independent scientific below, the EPA later added Lead as a criteria
committee, composed of seven members, includ- pollutant with legal prodding from the National
ing at least one member of the National Academy Resources Defense Council [49, 72].
of Sciences, one physician, and one person
representing state air pollution control agencies
to advise the Administrator on the science US Process for Setting National Ambient
informing the policy judgments made in setting Air Quality Standards
the NAAQS. The EPA has implemented this pro-
vision of the CAA by appointing a Committee, The process for developing and issuing NAAQS
which designated itself as the Clean Air Scientific after the initial NAAQS were set is quite complex
Advisory Committee (CASAC). The CASAC is as discussed by Bachmann [7] and McClellan [36,
directly responsible to the EPA Administrator, 37, 39, 41]. Key elements of the process, as used
although it functions administratively as one of until quite recently, include preparation and
the standing committees of the EPA Science Advi- review of (a) criteria document, (b) staff paper,
sory Board. Traditionally, the requirement for one (c) more recently a risk assessment, and (d) a
CASAC member to be a member of the National regulatory decision package leading to the
Academy of Sciences has been broadly Administrator’s policy judgment decisions as to
interpreted to also include membership in either the proposed and final NAAQS which are
the National Academy of Engineering or the Insti- published in the Federal Register. Traditionally,
tute of Medicine. To complement the expertise of CASAC focused its attention on reviewing the
regular members of the CASAC, a number of Criteria Documents and Staff Papers and, more
consultants, sometimes as many as a dozen, with recently, a formal Risk Assessment. As an aside,
specialized expertise usually have been added to the process was changed at the end of 2006 [51]
the review panels for specific pollutants. with an Integrated Science Assessment and Policy
The CAA was amended again in 1990 Assessment Document replacing the Criteria Doc-
[17]. Although major changes were made in the ument and Staff Paper. Time will tell if these
CAA with these amendments, especially with changes really improve the overall process.
regard to the regulation of hazardous air pollut- In addition to the documents noted above, the
ants, there were no changes in the fundamental Agency now prepares a Regulatory Impact Anal-
approach to dealing with the setting of NAAQS ysis which is required under Executive Order
for criteria pollutants. However, there were 12866 issued by President Clinton [18] that
changes in the CAA that have had major impact applies to economically significant rules that
on the regulation of emissions of PM and pre- have “an annual effect on the economy of
cursors especially from large power plants. $100 million or more or adversely effect in a
The pollutants originally designated as material way the economy, a sector of the econ-
“criteria pollutants” because of their ubiquitous omy, productivity, competition, jobs, the environ-
distribution and potential to endanger health ment, public health or safety or site, local, or tribal
were photochemical oxidants (later regulated as governments or communities.” The results of the
ozone), particulate matter (later regulated as Total Regulatory Impact Analysis are not considered
Suspended Particulates, then PM10, and PM2.5), during the NAAQS rulemaking process given
carbon monoxide, sulfur oxides (regulated as sul- the prohibition of consideration of cost in the
fur dioxide), nitrogen oxides (regulated as NO2), setting of the NAAQS [93].
20 Air Quality Guidelines and Standards

Air Quality Guidelines and Standards, Table 3 Primary and secondary National Ambient Air Quality Standards
initially set by the US Environmental Protection Agency in 1971a
Averaging
Pollutant (indicator)b Level time Formb
PM (total suspended 75 mg/m3 Annual Geometric mean
particulates) 260 mg/m3 24 h Not to be exceeded more than once per
year
TSP secondary standard 150 mg/m3 24 h Not to be exceeded more than once per
year
SO2 0.03 ppm Annual Arithmetic mean
0.14 ppm 24 h Not to be exceeded more than once per
year
SO2 secondary standards 60 mg/m3 (0.02 ppm) Annual Arithmetic mean
1,300 mg/m3 3h Not to be exceeded more than once per
(0.5 ppm) year
CO 10 mg/m3 (9 ppm) 8h Not to be exceeded more than once per
year
40 mg/m3 (35 ppm) 1h Not to be exceeded more than once per
year
Photochemical oxidants 200 mg/m3 1h Not to be exceeded more than once per
(as O3) (0.08 ppm) year
HC 160 mg/m3 3 h, 6–9 a.m. Not to be exceeded more than once per
(0.24 ppm) year
NO2 100 mg/m3 Annual Arithmetic mean
(0.053 ppm)
a
With the exception of PM and SO2, secondary NAAQS set identical to the primary standards
b
The terms “indicator” and “form” were not used in the 1971 notice

It is important to recognize that the NAAQS time it issues its final rule; and (4) all of the
process in the United States started as an informal above documents, analyses, preambles, and
rulemaking process [7, 41, 52]. The DC Court of responses constituted the record that the court
Appeals found that the informal process was not would examine in reviewing the final standard
sufficiently well documented with regard to the decision. Objections not raised in the record
four key elements (indicator, averaging time, con- could not be raised in court. The halcyon days of
centration, and statistical form) that the Court a speedy NAAQS process were over.” I agree that
could perform a judicial review of the rules that the speed of the process was reduced, however,
were promulgated. This resulted in a judicial deci- I would add that transparency of the process was
sion to overturn the secondary SO2 NAAQS in also substantially improved. Congress apparently
1973 [10]. This in turn led the US Environmental agreed and these provisions were substantially
Protection Agency to develop more rigorous pro- codified by the CAA Amendments of 1977 [16].
cedures including formal documentation [52]. EPA’s implementation of the CAA, especially
Bachmann [7] summarized the adoption of its setting of NAAQS even with improved docu-
these procedures in the late 1970s noting the fol- mentation, has been a matter of continuing con-
lowing points: “(1) EPA was to make available to troversy and litigation. Some persons might note
the public the information and technical method- that controversy and litigation were enhanced by
ologies it relied upon by the time of proposal; improved documentation. Bachmann [7] summa-
(2) the preambles to proposal and final rules rizes many of the key legal cases in his review. In
were to provide a detailed explanation of EPA’s this entry, I will only highlight several key legal
decision; (3) EPA was required to respond to all cases. The 1997 revisions of the Ozone NAAQS
“significant” comments on the proposal by the [65] and Particulate Matter NAAQS [66] proved
Air Quality Guidelines and Standards 21

to be very contentious including within CASAC. PM and Ozone standards in 1997 effected “an
For example, the members of the CASAC PM unconstitutional delegation of legislative author-
Panel, chaired by George Wolff, had a range of ity.” The Panel found that “the factors EPA uses in
views on the PM2.5 standard that was being set for determining the degree of public health concern
the first time replacing, in part, the PM10 standard. associated with different levels of ozone and par-
This range of views was clearly articulated in the ticulate matter are reasonable.” However, it
CASAC Chair’s letter [97] to the Administrator remanded the rule to EPA. The Judicial Panel
by including a Table showing the views of each stated that when the Agency considers these fac-
individual member of the CASAC Panel. This tors for potential non-threshold pollutants “what
approach stands in stark contrast to the approach EPA lacks is any determinate criterion for drawing
of more recent CASAC Panels that have empha- lines” to determine the level at which the stan-
sized consensus advice. dards should be set. The Panel also found that the
The contentious nature of the debate over these Administrator, under the CAA, is not permitted to
revised NAAQS prompted Administrator consider the cost of implementing these standards
Browner to involve President Clinton. Bachmann in setting them.
[7] recounts that Administrator Browner had a 1-h Not surprisingly, the nature of the Circuit Court
meeting on these standards with the President – opinion resulted in cross appeals being filed on the
“she reported that the President quickly accepted several issues and the involvement of the US
her decision and spent much of the time Supreme Court. The Supreme Court in February
discussing how to reduce unnecessary burdens in 2001 issued a unanimous opinion upholding
the implementation process. This resulted in some EPA’s position on both the constitutional and
of us writing the first draft of a letter that was later cost issues [93]. On the constitutional issue, the
sent by President Clinton [19] to EPA directing Supreme Court held that the statutory requirement
implementation be carried out so as to “maximize that the NAAQS be “requisite” to protect public
common sense, flexibility, and cost effective- health with an adequate margin of safety suffi-
ness.” Not surprisingly, President Clinton [46] ciently guided EPA’s discretion, affirming EPA’s
had a role in announcing the tighter standards approach of setting standards that are neither more
which included for the first time a separate nor less stringent than necessary.
PM2.5 standard to complement the PM10 standard Supreme Court Justice Breyer, who partici-
and a shift from a 1-h averaging time to an 8-h pated in the Whitman v. American Trucking Asso-
averaging time standard for Ozone. ciations case, is well known and highly regarded
The issuance of a revised PM NAAQS triggered for his opinions and writings on risk assessment
the legal case of American Trucking Associations [11, 12]. Thus, it is not surprising that he took the
v. EPA [4]. The Court found “the growing empiri- opportunity in Whitman v. American Trucking
cal evidence demonstrating a relationship between Associations [93] to offer comments on the
fine particle pollution and adverse health effects standard-setting process and, specifically, the
amply justifies establishment of new fine particu- identification of the level of the NAAQS and
late standards.” The Court went on to find “ample the associated level of health risk. While concur-
support” for EPA’s decision to regulate coarse par- ring that EPA cannot consider the costs of
ticulate pollution, but vacated the 1997 PM10 stan- implementing the Standards, he went on to
dards, concluding in part that PM10 is a “poorly note – “this interpretation of §109 does not require
matched indicator for coarse particulate pollution” the EPA to eliminate every health risk, however
because it includes fine particulates. Subsequently, slight, at any economic cost, however great, to the
EPA removed the vacated 1997 PM10 standard point of “hurtling” industry over “the brink of
allowing the 1987 PM10 standard to remain in ruin,” or even forcing “deindustrialization.”
place along with the new PM2.5 issued in 1997. (Id. At 494) (Breyer, J., concurring in part and
In addition, the three-judge panel held, two to concurring in judgment) (citations omitted).
one, that EPA’s approach to setting the level of the Rather, as Justice Breyer explained:
22 Air Quality Guidelines and Standards

The statute, by its express terms, does not compel very healthy society; hence a standard demanding
the elimination of all risk; and it grants the Admin- the return of the Stone Age would not prove “req-
istrator sufficient flexibility to avoid setting ambient uisite to protect the public health.”
air quality standards ruinous to industry. Although I rely more heavily than does the
Section 109(b)(1) directs the Administrator to set Court upon legislative history and alternative
standards that are “requisite to protect the public sources of statutory flexibility. I reach the same
health” with “an adequate margin of safety.” But ultimate conclusion, Section 109 does not delegate
these words do not describe a world that is free of to the EPA authority to base the National Ambient
all risk – an impossible and undesirable objective Air Quality Standards, in whole or in part, upon the
(citation omitted). Nor are the words “requisite” and economic costs of compliance.
“public health” to be understood independent of con-
text. We consider football equipment “safe” even if its
The case of Whitman v. American Trucking Asso-
use entails a level of risk that would make drinking
water “unsafe” for consumption. And what counts as ciations [93] is widely cited for the conclusion
“requisite” to protecting the public health will simi- that EPA cannot consider the economic costs of
larly vary with background circumstances, such as the compliance in the setting of NAAQS. Unfortu-
public’s ordinary tolerance of the particular health risk
nately, in my opinion, insufficient attention is
in the particular context at issue. The Administrator
can consider such background circumstances when given to the thoughtful guidance of Justice Breyer
“deciding what risks are acceptable in the world in on exercising policy judgment informed by sci-
which we live.” (Citation omitted). ence in deciding on an acceptable level of health
The statute also permits the Administrator to take risk, a judgment that in turn determines the level
account of comparative health risks. That is to say,
and statistical form of each NAAQS. It is interest-
she may consider whether a proposed rule promotes
safety overall. A rule likely to cause more harm to ing that Justice Breyer’s opinion appeared in
health than it prevents is not a rule that is “requisite to Administrator Johnson’s notice of the Ozone
protect the public health.” For example, as the Court NAAQS [81], but did not appear in Administrator
of Appeals held and the parties do not contest, the
Jackson’s “reconsideration” proposal for Ozone
Administrator has the authority to determine to what
extent possible health risks stemming from reduc- [85] that will be discussed later.
tions in tropospheric ozone (which, it is claimed,
helps prevent cataracts and skin cancer) should be
taken into account in setting the ambient air quality
standard for ozone. (Citation omitted).
Paradigm Shift
The statute ultimately specifies that the standard
set must be “requisite to protect the public health”
“in the judgment of the Administrator,” §109(b)(1), At this juncture, it is appropriate to note that it is
84 Stat. 1680 (emphasis added), a phrase that grants my view that a paradigm shift has taken place in
the Administrator considerable discretionary the selection of the level of each NAAQS over the
standardsetting authority.
past four decades. In my opinion, the paradigm
The statute’s words, then, authorize the Admin-
istrator to consider the severity of a pollutant’s shift has been driven in part by the changing
potential adverse health effects, the number of nature of the scientific evidence of pollution
those likely to be affected, the distribution of the effects. In the 1970s, most scientists and regula-
adverse effects, and the uncertainties surrounding tions viewed the criteria pollutants as having a
each estimate (citation omitted). They permit the
Administrator to take account of comparative health threshold in their ambient concentration- response
consequences. They allow her to take account of relationship, sometimes referred to as a hockey
context when determining the acceptability of small stick function [36, 39]. In contrast cancer-causing
risks to health. And they give her considerable agents have been assumed to have linear, non-
discretion when she does so.
The discretion would seem sufficient to avoid threshold, concentration-response relationships.
the extreme results that some of the industry parties In the late 1960s and early 1970s, the available
fear. After all, the EPA, in setting standards that data on each criteria pollutant were quite modest,
“protect the public health” with “an adequate mar- with attention focusing on only a few epidemio-
gin of safety,” retains discretionary authority to
avoid regulating risks that it reasonably concludes logical studies. For those few studies, attention
are trivial in context. Nor need regulation lead to often focused on whether a relative risk on the
deindustrialization. Preindustrial society was not a order of 2.0 was statistically significant or not. For
Air Quality Guidelines and Standards 23

a given pollutant there were few, if any, controlled correlates. There’s nothing sinful about checking
human exposure studies. The data from laboratory for confounding variables. The sin comes in believ-
animal studies with specific pollutants had fre- ing a casual hypothesis is true because your study
quently been acquired in studies with exposure came up with a positive result, or believing the
concentrations much higher than ambient concen- opposite because your study was negative.”
trations of the pollutants. The results of these It is interesting to note that CASAC discus-
studies raised questions about extrapolation both sions of criteria pollutant effects have frequently
from laboratory animals to humans and high to focused initially on the level of the standard some-
low exposure concentrations. The general times devoid of any consideration of the statistical
approach taken was to identify the lowest levels form of the level. This approach was in keeping
where effects were statistically significant and with traditional practice in the setting of standards
assume this was the inflection point in the such as Threshold Limit Values for occupational
concentration-response relationship. It could be exposures to chemicals based on scientific judg-
argued that setting the Standard at a lower con- ments [34–36, 40]. That approach has involved a
centration satisfied the requirement for “an ade- review of the available human data on a toxic
quate margin of safety.” chemical to determine a no-observed effect level,
In contrast, the most recent reviews have or the lowest observed effect level, and then using
involved thousands of papers with observations safety factors to arrive at an acceptable exposure
ranging from human population level to studies level set at a lower level. In the absence of ade-
of intact laboratory animals to studies of effects quate human data, laboratory animal data are used
of air pollutants on cells and molecules. Despite and an additional safety factor used to account for
the huge number of published studies, attention has the potential that the animal observations might
ultimately focused on the results of a few studies not adequately predict human effects. This
where attention turns to the critical issue of how approach was routinely used for a wide range of
they inform the setting of the level and statistical health responses that were assumed to have an
form of the standard. In the epidemiological stud- exposure-response relationship that exhibited
ies, the debate often focuses on whether relative either a true or practical threshold, an excess of
risks of less than 1.1 for excess morbidity and effects above some level and an absence of effects
mortality are significant. Of course, the specific below that level. A review of the earliest Criteria
relative number is dependent on the denominator Documents and, indeed, also the Staff Papers,
being used, for example, per 10 ppb of ozone (24-h documents that a similar line of reasoning was
average). For controlled exposure clinical studies, used in the setting of the NAAQS.
attention has focused on the lowest levels with The implementation of standards set with this
statistically significant changes, which in turn, trig- approach soon revealed that if the standard was to
gers debate over whether the changes are adverse. be rigorously enforced, that is, no exceedances of
A news report [63] in Science that I view as a the specific level of the standard, the practical
classic report highlighted the issues involved in the effect would be to cause average levels of the
search for subtle links between diet, lifestyle, or pollutant to be reduced to levels far below the
environmental factors and disease, especially using standard so as to avoid the occasional high value
retrospective observational studies. I especially exceeding the standard. Fortunately, common
liked the quote at the end attributed to Sander sense prevailed and the EPA, over time, moved
Greenland, a well-known epidemiologist, in offer- to the practice of routinely linking the specific
ing advice to his “most sensible, level-headed, level of the standard with a statistical form such
estimatable colleagues.” Remember, he says – as the 98th percentile 24-h concentration averaged
“there is nothing sinful about going out and getting over 3 years or the fourth highest 8-h average
evidence, like asking people how much do you concentration during a 3-year period. In my opin-
drink and checking breast cancer records. There’s ion, most of the attention of the CASAC in the
nothing sinful about seeing if that evidence NAAQS setting process has focused on the level
24 Air Quality Guidelines and Standards

of the standard with limited discussion of the for particulate matter [69], ozone [77, 78, 79] and
statistical form of the Standard. In doing so, sulfur dioxide [83]. Guidance has also been pro-
there has been a failure to recognize that the vided by the US National Research Council
stringency of the standard and the degree of health [48]. First and foremost, conduct of a risk assess-
protection provided depends on both the level and ment requires some knowledge of the nature of the
statistical form of the standard for a particular ambient concentration-response relationships for
indicator and averaging time. various temporal metrics for the pollutant in ques-
The challenges of selecting appropriate averag- tion. Typically, the response term is expressed as
ing times and statistical forms for the NAAQS are excess risk per unit of increased concentration over
substantial. The original epidemiological and toxi- some range of ambient concentrations. The question
cological studies that provide the scientific informa- then becomes one of whether the relationship is
tion that should inform the setting of the NAAQS do linear and whether there is a threshold level below
not always report results with an averaging time that which the coefficient for excess risk holds or does
is the same as that ultimately selected for the Stan- not hold. The issue of whether there are or are not
dard. Hence, the need to make extrapolations from thresholds for noncancer health endpoints from
results reported based on one metric, such as aver- exposure to many agents is very contentious [56,
age daily exposure to a second metric such as an 8-h 92]. It is well recognized that the use of linear
averaging time. The setting of standards at extreme no-threshold exposure-response relationships for
values, the 98th percentile for NO2 [86] or, even the cancer-causing agents is closely linked to experience
99th percentile form as done with the 1-h averaging with radiation [47]. An additional issue becomes the
time standard for SO2 [87], results in extremely selection of suitable reference baseline statistics for
stringent standards that at best are only very loosely the particular health effects to use along with a given
related to the underlying data. In my view, selection ambient concentration-response coefficient. Yet
of the specific level and statistical form for a specific another question becomes the appropriate popula-
averaging time is clearly policy judgments beyond tion to be evaluated, a single city, multiple cities, or
the dominion of the science. It is my opinion that the population of the United States. It is obvious that
decisions on the selection of specific averaging there are substantial uncertainties associated with
times are ultimately policy judgments reserved to each component of the analysis of benefits of poten-
the Administrator by the language of the CAA. tial reductions in a given pollutant.
In the 1990s, concurrent with the increasingly With the use of linear, no-threshold, ambient
widespread use of formal risk analysis procedures concentration-response models, the EPA has, on
across society [35, 40], EPA moved to quantify the some occasions, calculated estimated excess mor-
health benefits associated with setting the NAAQS bidity and mortality effects attributable to the spe-
at various levels, with an associated statistical cific pollutant down to background concentrations.
form. I must admit to being an early advocate of The Health Risk Assessment [77] and the Regula-
formal quantification of health benefits. I viewed tory Impact Analysis [82] for the 2008 Ozone
the approach then and I still do today, as providing NAAQS [81] serve as examples. Further, dependent
useful guidance for making policy decisions. I did on the assumptions made with regard to how ambi-
not envision that some enthusiastic advocates of ent concentrations of the pollutant would change in
quantitative risk analysis would actually view the response to various levels and forms of the standard,
results of the analyses as being highly accurate substantial health effects avoided, that is, health
projections of potential health benefits expressed benefits can be calculated. Expressing the benefits
to two or more significant figures, sometimes with- in monetary units raises some critical issues. Typi-
out any indication of uncertainty. cally, mortality effects drive the monetized benefits
The quantification of health effects potentially calculations because of the substantial value placed
associated with various levels and forms of the on deaths avoided. Sunstein [61] has addressed this
Standards requires several kinds of input. Examples contentious issue and has argued that years of life
are the risk assessments conducted by the USEPA loss is a more appropriate metric than is the use of
Air Quality Guidelines and Standards 25

lives lost as is the typical approach used by the Agency of the United Nations to be the directing
USEPA. and coordinating authority for international health
A key consideration as to whether these benefits matters and public health. WHO develops air qual-
can be realized relates to whether the roll-back in ity guidelines (AQG) designed to offer guidance in
air concentrations that is assumed in the analysis as reducing the health impacts of air pollution. The
a result of the new standard can actually be real- first AQG were produced in 1987 [94]. Updates
ized. In part, this relates to how realistic the were published in 2000 and 2005 [95, 96]. The
assumptions have been with regard to background AQG are intended to inform policymakers and to
levels. The analysis of benefits of reducing a given provide appropriate targets for a broad range of
pollutant, say Ozone, becomes even more convo- policy options for air quality management in dif-
luted when the analysis includes postulated reduc- ferent parts of the world, despite the more recent
tions in a second pollutant, such as particulate documents being titled AQG for Europe.
matter, associated with achieving the Ozone Stan- The WHO AQGs are developed by working
dard. A discussion of this issue for Ozone can be groups of scientific experts [95, 96]. In addition to
found in McClellan et al. [43]. Indeed, as the levels preparing AQG for the classical air pollutants
of the standards are ratchetted down toward back- (Particulate matter, Ozone, Nitrogen dioxide, and
ground levels, there is increasing uncertainty as to Sulfur dioxide) the WHO also developed AQG for
whether there are any health effects attributable to (a) inorganic air pollutants, (b) certain indoor air
single pollutants and even greater uncertainty as pollutants, (c) polychlorinated biphenyls, dioxins,
to the magnitude of the health benefits associated and furans, and (d) volatile organic compounds. The
with any new lower standard. The use of single WHO AQG process does not include any opportu-
pollutant models for estimating benefits raises the nity for the involvement of interested parties such as
issue of double-counting of benefits as the benefits the public, national governments, nongovernmental
of the individual pollutants are aggregated. organizations, or industry. They represent expert
Hence, the paradigm shift. It is apparent that in judgment exercised by scientists knowledgeable of
setting the earliest NAAQS some individuals, the subject material. This approach contrasts
including CASAC members, envisioned that the sharply with the more formal and complex approach
standards were being set at levels protective of pub- followed by the US Environmental Protection
lic health with an adequate margin of safety based on Agency in developing NAAQS.
threshold ambient concentration-response models. The primary aim [95] of the AQG is “to pro-
In short, if there were health effects at the level and vide a uniform basis for the protection of public
form of the NAAQS, they were de minimis. It is health and ecosystems from adverse effects of air
useful to recall the Editorial by Kennedy [27]. In pollution and to eliminate or reduce to a minimum
contrast, more recent NAAQS have been set at exposure to those pollutants that are known or
levels which both the CASAC and EPA characterize likely to be hazardous.” “They have the character
as having residual health effects even if the standard of recommendations, and it is not intended or
were to be attained. The central question remains – recommended that they simply be adopted as
how low is low enough? I view the answer as a standards.” The WHO [95] report notes:
policy judgment informed by science that can only In the process of moving from a “guideline” or a
be made by the EPA Administrator [41]. “guideline value” to a “standard,” a number of
factors beyond the exposure-response relationship
need to be taken into account. These factors include
current concentrations of pollutants and exposure
WHO Process for Setting Air Quality levels of a population, the specific mixture of air
Guidelines pollutants, and the specific social, economic and
cultural conditions encountered. In addition, the
standard-setting procedure may be influenced by
The approach taken by the World Health Organi- the likelihood of implementing the standard.
zation (WHO) contrasts with the USEPA approach. These considerations may lead to a standard above
WHO was established in 1948 as a specialized or below the respective guideline value.
26 Air Quality Guidelines and Standards

Assessing Hazards and Risks Sources of Information for Setting


Standards and Guidelines
The risk approach used around the world today
(Fig. 2) developed within the USEPA in parallel The multiple sources of information for evaluat-
with the process for setting NAAQS [35, 36, 38, ing the potential health effects of any air pollutant
39]. The setting of air quality standards and guide- are illustrated in Fig. 6 [35–39, 41]. In the case of
lines may be viewed as a specialized use of the risk all the criteria air pollutants, the dominant sources
characterization paradigm illustrated in Fig. 2 of information are those based on the study of
[35]. In particular, the establishment of air quality humans, the left side arm of the figure. However,
standards and guidelines draws on the schematic all of the common air pollutants have been viewed
rendering in the box labeled “risk assessment.” An as being sufficiently innocuous, and with effects
initial step in that process is to determine the hazard that are readily reversible when exposures are
potential of the agent, in short, to determinewhether discontinued, that controlled human exposure
the specific agent has the potential for causing studies can be conducted with the pollutant.
adverse health effects in humans. In the case of the Such studies have provided very useful informa-
criteria or common air pollutants discussed in this tion on short-term exposures, typically a few
entry, there is sufficient evidence to establish that hours in duration as will be discussed later for
with exposure of sufficient duration and concentra- ozone. A limitation of such studies is the appro-
tion the agent is capable of causing disease in peo- priate requirement for the conduct of such studies
ple, based on epidemiological evidence. The key only in healthy adults or individuals with modest
issue then becomes the nature of the relationship preexisting disease. Controlled exposure studies
between ambient concentrations and duration of in individuals with serious preexisting disease
exposure and increased disease. The specific char- would not be ethical. The paramount advantage
acteristics of that complex relationship are crucial to of controlled human exposure studies is that the
determining for a particular ambient concentration exposures can be well characterized unlike the
the estimated health impacts including the ambient situation for field studies or epidemiological
concentration level. Moreover, the same informa- studies.
tion is required if one is to estimate the health For some of the common air pollutants, valu-
benefits associated with a postulated improvement able data on shorter-term exposures have been
in air quality, that is, reductions in ambient acquired from field studies of individuals exposed
concentrations. to ambient concentrations of pollutants. In these

Characterization of Hazard and Estimation


of Potency

Extrapolation Across Extrapolation Required Across


Species Not Required Species
Clinical Case Studies in Laboratory Animals
Observations in
Species of Interest
Extrapolation to Intact Organism,
Controlled Exposure May Require Cross Species Extrapolation
Studies in Species Studies with Cells and Tissues From
of Interest Species of Interest and Other Species

Multiple Extrapolations
Epidemiological of
Epizootological Studies
in Species of Interest Structure-Activity Analyses

Air Quality Guidelines and Standards, Fig. 6 Sources of information for evaluating potential health effects
Air Quality Guidelines and Standards 27

studies, the investigators can obviously only study studies seek to characterize the relationship
air concentrations that are present and the extent between ambient concentrations on a given day
they can be characterized and then relate the ambi- or series of days and excess morbidity or mortality
ent concentrations to one or more health indices occurring concurrently or on subsequent days. An
such as changes in lung function. example is the study of Bell et al. [8, 9] and Smith
The predominant source of information on the et al. [58] that will be discussed later. An advan-
health effects of the common air pollutants has tage is that it is assumed that many other risk
been from epidemiological studies. It is beyond factors that may be influencing the health of the
the scope of this entry to discuss the conduct and population is not varying on a day-to-day basis,
results of those studies in detail. The reader inter- for example, socioeconomic status. Other factors
ested in more detail will find the textbook on such as temperature may vary along with pollu-
Environmental Medicine edited by Ayres et al. tion levels.
[6] useful. Suffice it to note that most epidemio- In the next section, information on the health
logical studies of air pollution are a kind of cohort effects of particulate matter and ozone will be
study or a time-series study. None of the studies briefly reviewed as examples of the kind of infor-
are strict cohort studies in which a population is mation used in setting NAAQS. In this section
randomly assigned to one or more treatment I draw heavily on a previous review of risk assess-
groups. This is rarely possible in studying air ment/risk management [40].
pollution. Investigators are constrained to study-
ing populations under natural conditions of ambi-
ent exposure and other risk factors associated with
the natural course of life. The study that may come Particulate Matter as an Example
closest to the ideal cohort study is the Six-City
Study [20, 23] which will be discussed later. In The Particulate Matter (PM) NAAQS was initially
such a study, the investigators may use regulatory set in 1971 using Total Suspended Particulate
compliance monitoring data supplemented by (TSP) Matter as an indicator [36, 37, 39, 42,
research monitoring to characterize ambient air 64]. Later, the standard was revised with the TSP
concentrations of the various pollutants. Health indicator replaced by PM10. PM10 is defined as
outcomes information may be obtained by contact the size fraction collected using a device that
with the enrollees supplemented by information includes 50% of the particle with an aerodynamic
acquired from Administrative databases such as diameter of 10 mm. A progressively smaller frac-
records of deaths. Other studies such as those tion of PM mass is collected as the particle size
using the ACS populations, for example, Pope increases above 10 pm and a progressively larger
et al. [54] are totally dependent upon regulatory fraction of PM mass is sampled as particle size
compliance modeling and administrative data- decreases below 10 mm. Later, the standard was
bases for health outcomes. As might be expected, again changed with PM2.5 introduced as an indi-
the quality of these studies is dependent upon the cator to complement the PM10 indicator. PM2.5,
quantity and quality of the monitoring data, the the fine particle fraction indicator is defined as for
availability of data on other risk factors, the dura- PM10 indicator with a 50% cut point at 2.5 mm
tion of follow-up, the quality of the health out- aerodynamic diameter. To state the obvious, the
come data, and the rigor of the analyses. PM2.5 fraction is contained within the PM10 frac-
A second type of study design is that used in tion which is contained within the TSP sample. In
the time-series studies as pioneered by the Johns recent years, increased attention has been focused
Hopkins University investigators in the National on the ultrafine particle number which is
Morbidity and Mortality Air Pollution Studies contained within the PM2.5 size range. There has
(NMMAPS). These studies utilize regulatory also been interest in characterizing health effects
compliance monitoring data to characterize ambi- of the PM10–2.5 fraction which has been called the
ent concentrations of pollutants and administra- course particle fraction. Consideration is given to
tive databases for morbidity and mortality. These regulating this fraction with a separate NAAQS.
28 Air Quality Guidelines and Standards

A detailed review of the evidence for health not surprising. When this is done it is necessary to
effects of PM is beyond the scope of this entry. normalize the smoking history to pack-years, for
Suffice it to say, abundant data are available on the example, 1 pack/day for 25 years or 2 packs/ day
health effects of PM, characterized using different for 12.5 years equals 25 pack-years. The relative
PM indicators, from epidemiological and labora- risks for an average current smoker (men and
tory animal studies using a range of indicators of women combined, 22 cigarettes per day for
morbidity and mortality [65, 68, 84]. In setting the 33.5 years with smoking initiated before age
PM standards, the greatest weight, appropriately, 18 years) (equivalent to 37 pack-years) were
has been given to the epidemiological evidence equal to 2.58, 2.89, and 14.80 for all-cause, car-
and, specifically, to those studies which can pro- diopulmonary, and lung cancer mortality, respec-
vide quantitative exposure-response information. tively. The magnitude of these relative risks is
Two large studies have yielded especially valu- substantially greater than that of PM2.5 and
able information that has played a key role in the emphasizes the critical importance of considering
setting of the PM NAAQS using the PM10 and cigarette smoking in any study of air pollution.
PM2.5 indicators. The first of these is the Harvard Moreover, it is important that investigators follow
Six Cities study designed by Ferris and colleagues the lead of the ACS investigators and report the
[20, 23] to specifically evaluate the health effects results of the analyses done for cigarette smoking
of criteria air pollutants. In my opinion, this is one at the same time they report relative risks for
of the best studies ever conducted of the influence various air pollutants. These results on cigarette
of air quality on health. It involves a 14–16-year smoking provide valuable perspective for consid-
follow-up of 8,000 subjects living in six commu- ering the results of analyses for the various air
nities in the United States selected to provide a pollution indicators. A comparison of the relative
gradient in several indices of air quality. Extensive risk estimates they obtain for smokers with those
efforts were made to characterize air quality. of other investigators serves as a “reality check”
A second air quality study made opportunistic on their analyses.
use of data from a population of 500,000 individ- The results from the Six Cities study and ACS-
uals who self-enrolled in 1982–1989 in an Amer- based studies are generally similar [28, 53]. Sum-
ican Cancer Society Study [54]. A subgroup of mary information from the two studies is given in
240,000 of these individuals lived in 50 metropol- Table 4 with a comparison made of the risk ratios
itan areas in which PM2.5 measurements were for the most polluted versus least polluted cities.
made for regulatory compliance purposes. For comparison, results are also shown for typical
The vast amount of information available from smokers. Note that in this case the typical smoker
the Six Cities and ACS studies has been reviewed has been defined as about a 25 pack-year smoker,
by the EPA [68, 70, 84]. Selected data will be about two thirds that of the current smoker
presented here to illustrate some of the key results discussed earlier for the ACS study. Interestingly,
that have influenced the setting of the PM the relative risk, for example, for lung cancer
NAAQS. Figure 7 summarizes an impressive mortality is about two thirds of the value cited
array of information from the ACS study on all- earlier, 9.73 versus 14.80. The range of the confi-
cause mortality, cardiopulmonary mortality, lung dence intervals for the association between PM2.5
cancer mortality, and all other cause mortality and cardiopulmonary mortality, even for these
[54]. With control for smoking, education, and studies with thousands of subjects, emphasizes
national status, the controlled forward stepwise the challenges faced in teasing out small effects
inclusion of additional covariants had little influ- of air pollution in developed countries.
ence on the estimated associations between fine Laden et al. [29] extended the observations for
particulate (PM2.5 indicator) air pollution on car- the Six Cities Study Cohort by including deaths
diopulmonary and lung cancer mortality. As may for 1990–1998 and compared those observations
be noted, the inclusion of cigarette smoking atten- to the earlier time period (1974–1984) and for the
uated the estimated relative risk of PM2.5, which is entire period. The estimated city-specific average
Air Quality Guidelines and Standards 29

a All-cause mortality
1.50
1.40
1.30
RR (95% CL)

1.20
1.10
1.00
0.96
0.80

b Cardiopulmonary mortality
1.50
1.40
1.30
RR (95% CL)

1.20
1.10
1.00
0.96
0.80

c Lung cancer mortality


1.50
1.40
1.30
RR (95% CL)

1.20
1.10
1.00
0.96
0.80

d All other cause mortality


1.50
1.40
1.30
RR (95% CL)

1.20
1.10
1.00
0.96
0.80
3

10 )

(P 5 )

19 ,2.5 )

90

80

98

80

80

ar 8
98

00

ag

98

98

98

98

99

19 199

98

99

qu 99
1
M

PM

19

19

19

19

19

r
te
er
–1

–2

–1

–1

–1

–1

–1

–1

–1

1
15
(P

ird –
Av

(
79

99

80

79

82

80

82

82

82

80

82

th 82
6

3
99

98
19

19

19

19

19

19

19

19

19

19
3
–1

–1

98
87

79

–1
19

19

79

Fine particles Total suspended Sulphate Sulphur Nitrogen Carbon Ozone


19

(PM2.5) particles particles dioxide dioxide monoxide

Inhalable, coarse particles Gaseous pollutants

Air Quality Guidelines and Standards, Fig. 7 Relative PM10 particles measuring less than 10 mm in diameter,
risk (RR) ratio for adjusted mortality evaluated at subject- PM15 particles measuring less than 15 mm in diameter,
weighted mean concentrations. CI confidence interval, PM2.5–15 particles measuring between 2.5 and 15 mm in
PM2.5 particles measuring less than 2.5 mm in diameter, diameter. (Adapted from Pope et al. with permission)

PM2.5 levels were lower in the extended follow-up A critical issue in interpreting the data shown
period in the 1990s than in 1974–1989 and the in Fig. 8 is the nature of the exposure-response
mortality risk ratios were lower. relationship. It must be noted that this is the
30

Air Quality Guidelines and Standards, Table 4 Comparison of mortality risk ratios (and 95% C.I.) for smoking and air pollution from the six cities and American Chemical
Society (ACS) Prospective Cohort Studies
Current smokera Particulate air pollution (most vs least polluted city)
Cause of death Six cities ACS Six cities (PM2.5) ACS (PM2.5) ACS (504)
All 2.00 (1.51–2.65) 2.07 (1.75–2.43) 1.25 (1.08–1.47) 1.17 (1.09–1.26) 1.15 (1.09–1.22)
Cardiopulmonary 2.30 (1.56–3.41) 2.28 (1.79–2.91) 1.37 (1.11–1.68) 1.31 (1.17–1.46) 1.26 (1.16–1.37)
Lung cancer 8.00 (2.97–21.6) 9.73 (5.96–15.9) 1.37 (0.81–2.31) 1.03 (0.80–1.33) 1.36 (1.11–1.66)
All others 1.46 (0.89–2.39) 1.54 (1.19–1.99) 1.01 (0.79–1.30) 1.07 (0.92–1.24) 1.01 (0.92–1.11)
Source: Adapted from Pope and Dockery [53]
a
Risk ratios for current cigarette smokers with approximately 25 pack-years (about average at enrollment for both studies) compared with never smokers
Air Quality Guidelines and Standards
Air Quality Guidelines and Standards 31

a All-cause mortality b Cardiopulmonary mortality


0.2
0.1
Log RR (95% CI)

0
–0.1
–0.2
–0.3
–0.4

c Lung cancer mortality d All other cause mortality


0.2
0.1
Log RR (95% CI)

0
–0.1
–0.2
–0.3 10
–0.4

10 15 20 10 15 20
PM2.5 (µg/m3) PM2.5 (µg/m3)

Air Quality Guidelines and Standards, plot of mean fine particulate pollution. CI confidence interval,
Fig. 8 Nonparametric smoothed exposure-response relation- PM2.5, fine particles measuring less than 2.5 mm in diameter,
ship. Vertical lines along the x-axes indicate a rug or frequency RR relative risk. (Adapted from Pope et al. with permission)

ambient concentration for PM that is being eval- particulate pollution and total mortality, although
uated for an association, not PM exposure. The he could not rule out a small effect, particularly
PM exposure cannot be evaluated since the esti- before 1983. The 2006 EPA analysis used to revise
mated indoor PM concentrations cannot even be the PM NAAQS interpreted the available epidemi-
estimated. Pope et al. [54], using the ACS cohort ological data as not clearly supporting or refuting
data, evaluated the nonparametric smoothed the existence of a threshold. The EPA analysis did
exposure-response relationships between cause- calculate added risks down to an assumed thresh-
specific and average PM2.5 (Fig. 8) [54]. They old of 7.5 mg/m3; a level on the order of the ambient
observed that the log-relative risk for all-cause, PM2.5 concentrations found in many US cities.
cardiopulmonary, and lung cancer mortality While the estimated or excess risk for the var-
increased across the gradient of PM2.5 concentra- ious PM indicators are quite small, it is apparent
tions. Goodness-of-fit tests indicated that the asso- that when used in company with standard baseline
ciations were not significantly different from data for specific cities with populations measured
linear associations. The mean concentration of in the millions, the calculated number of excess
PM2.5 across the ACS cohort was 14 mg/m3. deaths appears large. The USEPA Administrator
Enstrom [22] evaluated the relationship can consider such quantitative risk assessment
between fine particulate air pollution and total results in making a “judgment call” in setting the
mortality among nearly 50,000 elderly standards. However, the Administrator is explic-
Californians for 1973–2002 using a subpopulation itly prohibited from considering cost when setting
of the ACS enrollees. He concluded that the results the standard. In separate regulatory impact ana-
did not support a current relationship between fine lyses, the risk assessment results are monetized in
32 Air Quality Guidelines and Standards

economic analyses used to estimate the benefits To provide context for the discussion of the
associated with achieving a revised standard com- Ozone NAAQS it is important to understand the
pared to maintaining an existing standard. The background levels of ambient ozone. A team of
regulatory impact analysis prepared for ozone investigators at Harvard University led by Daniel
and particulate matter [67] and separately for par- Jacob have made major contributions to under-
ticulate matter [76] and ozone [78] are examples. standing tropospheric ambient ozone levels
Substantial controversy developed in the final around the world using a global chemical trans-
stages of revision of the PM2.5 standard port model (GEOS-Chem). The Harvard team
announced in 2006. A majority of the EPA’s [90] reported the use of the GEOS-Chem model
Clean Air Scientific Advisory Committee’s with 1 latitude by 1 longitude spatial resolution
(CASAC) PM Panel recommended that the EPA to quantify the effects of anthropogenic emissions
Administrator reduce the PM2.5 24-h averaging from Canada, Mexico, and outside North America
time standard from the previous level of 65 mg/ to estimate daily maximum 8-h average ozone
m3 to a level in the range of 25–35 mg/m3 and that concentrations in US surface air. Their simula-
for the PM2.5 annual averaging time the standard tions for summer 2001 estimated mean North
be reduced from the previous level of 15 mg/m3 to American and US background contributions of
a level in the range of 12–14 mg/m3. I was in the 26  8 ppb and 30  8 ppb, as obtained by
minority and argued that identifying a specific eliminating anthropogenic emissions in North
bright line, upper bound such as 14 mg/m3 was America versus in the United States only. The
an issue that went beyond scientific interpretation background 8-h highest Ozone concentrations
of data and was a policy judgment as to acceptable approached 60 ppb. The frequency distribution
risk. The Administrator, ultimately, revised the of the simulated daily 8-h-maximum surface
PM2.5 NAAQS, 24-h averaging time standard, to Ozone concentrations are shown in Fig. 9. It is
35 mg/m3 and retained the annual standard at important to recognize that the statistical form of
15 mg/m3 [74, 75]. Obviously, the majority of the Ozone NAAQS is directed at minimizing the
CASAC was not happy with the Administrator’s occurrence of the highest ozone events, the right
policy judgment call. side tail of the distributions in the figure. The high
levels of background Ozone will make it challeng-
ing to achieve any Ozone NAAQS set in the range
Ozone of 60–80 ppb (8-h daily maximum).
The initial Ozone NAAQS in the United States
Ozone is an interesting air pollutant because it is was set in 1971 using photochemical oxidants as
not directly emitted from industrial sources except an indicator and with a 1-h averaging time [7,
in rare circumstances. The majority of Ozone 64]. The standard was later revised with ozone
found in the ambient environment is formed as the indicator. Later the averaging time was
from reactions of Volatile Organic Compounds changed from a 1-h maximum during a 24-h
(VOC) and Nitrogen Oxides (NOx) in the pres- period to an 8-h rolling average maximum.
ence of sunlight. The VOCs originate both from There is an abundant database on the health
natural and industrial sources and the NOx is effects of ozone from epidemiological investiga-
largely from combustion of hydrocarbon fuels. tions and toxicity studies conducted in laboratory
Ozone concentrations typically have distinct diur- animals [38, 71, 80, 81]. In addition, there is a
nal cycles with the highest levels observed at substantial amount of data acquired from studies
midday and the lowest concentrations at night in conducted with human volunteers exposed to con-
the summer. Lower concentrations are typically trolled levels of ozone for short periods of time. In
observed in the winter than in the summer. This is the setting of the Ozone NAAQS, quantitative
the case because of the manner in which ozone is exposure-response data from human studies have
formed with sunlight driving the reactions been given the greatest weight. This is especially
between NOx and VOCs. appropriate since there are well-established
Air Quality Guidelines and Standards 33

0.05
0.04
0.03

ppb−1
0.02
0.01
0.00
0 20 40 60 80 100
Ozone (ppb)

Air Quality Guidelines and Standards, dashed line), for the contiguous United States during June–
Fig. 9 Frequency distribution of the simulated daily 8-h- August 2001. The frequency distributions are constructed
maximum surface ozone (black solid line). North Ameri- from the 1  1 daily model output. (From [90])
can background (red dotted line) and US background (blue

quantitative differences between laboratory ani- was included in the final compilation of informa-
mal species and humans in the disposition of tion provided to the EPA Administrator to render a
inhaled ozone which minimize the utility of the judgment on the revision of the Ozone NAAQS.
data from laboratory animals for quantitatively A key piece of information on the health effects
estimating human risk of ozone exposures. of ozone came from the time-series study of Bell
The effects of ozone on the respiratory tract are et al. [8, 9]. Their analysis used a 24-h averaging
well known, thus it is not surprising that consid- time and, thus, was not directly applicable to
eration of these effects has had a primary influence setting the Ozone NAAQS with an 8-h averaging
on the setting of the Ozone NAAQS. In the review time. Smith et al. [58] extended the analyses of
culminating with a revised standard in March Bell et al. [8] focusing on the development of city-
2008, the information from pulmonary function specific ozone mortality estimates. The analyses
evaluations conducted on young adult volunteers of both Bell et al. [8] and Smith et al. [58] used the
undergoing moderate exercise while exposed to National Air Pollution Morbidity and Mortality
various concentrations of ozone for 6.6 h played a air pollution database assembled at Johns Hopkins
prominent role. The key parameter evaluated, University. The results for the 8-h averaging time
changes in the forced expiratory volume in 1 s are shown in Fig. 11. The degree of intercity
(FEV1), are shown in Fig. 10 [1–3, 13, 24, 26, 44, heterogeneity is noteworthy including recognition
45]. Data from individuals exposed to 0.08 ppm that only 5 cities of the 98 cities evaluated had
ozone and higher were considered in the previous statistically significant effects of ozone on acute
review of the ozone standard. In the most recent mortality.
review, data were available from the studies of Smith et al. [58] called attention to this
Adams and colleagues [3] with 0.06 and intercity heterogeneity across the United States
0.04 ppm exposures conducted to complement (Fig. 12). The ozone effects are most striking in
earlier studies conducted with 0.08 and the Northeastern United States and absent in the
0.012 ppm, Adams [3] interpreted his studies as Western United States including the Los Angeles
showing a statistically significant effect at Basin. It is not surprising that Smith et al. [58]
0.08 ppm, effectively reproducing the effects caution against the use of national estimates of
seen in earlier studies. However, he interpreted ozone concentration-response functions.
his studies at 0.06 and 0.04 ppm as not showing The EPA’s CASAC recommended to the
statistically significant changes compared to Administrator that he revise the Ozone NAAQS
exposure to clean air. The USEPA reanalyzed the with an 8-h averaging time, from 0.08 ppm to a
data of Adams and colleagues using different sta- level within the range of 0.060–0.070 ppm. Ulti-
tistical procedures [13]. The USEPA reanalysis mately, the Administrator exercised his judgment
34 Air Quality Guidelines and Standards

Air Quality Guidelines 20


and Standards, Adams (2006)81
Fig. 10 Changes in the x Adams (2002)82
lung function of young Adams (2003)83
health adults following a 15 Folinsbee et al. (1988)84 x
6.6-h exposure to ozone.

FFV1 decrement (%)


Horstman et al. (1990)85
FFV1 forced expiratory

Ozone-induced
McDonnell et al. (1991)86
volume in 1 s, ppm parts per McDonnell et al. (2007)87
million. (Adapted from
10
Brown et al. with
permission)

x
0
0.02 0.04 0.06 0.08 0.1 0.12 0.14
Ozone (ppm)

in revising the standard to 0.075 ppm. The (including an absence of excess risk) and the
CASAC Ozone Panel expressed its displeasure associated uncertainty in the estimate. However,
at the Administrator’s setting the NAAQS at a the selection of a specific level for the standard
level higher than they recommended. In my opin- goes beyond the science and represents a policy
ion, the science alone can never be sufficient for judgment or decision. The issue of the role of
establishing a specific numerical standard. The science and judgment in standard setting is
setting of the standard also involves judgment as drawn to the forefront by agents that do not have
to acceptable risk, a judgment call I viewed as clear thresholds in their exposure-response rela-
being delegated to the Administrator, not the tionships. In these cases, some level of excess risk
Advisory Committee, by the Clean Air Act. may be calculated for exposures that extend down
After the revised standard was promulgated, the to ambient levels routinely observed in developed
EPA’s statistical reanalysis [13] was published countries.
with a conclusion that the Adams [3] data demon- In March 2008, then EPA Administrator Ste-
strated a statistically significant, but small biolog- phen Johnson announced a revised Ozone
ical effect at 0.060 ppm. These published findings NAAQS (8-h averaging time) of 75 ppb, a reduc-
as well as any new data that may become available tion from the previous level of 0.08 ppm (which
from studies conducted with human volunteers by rounding convention was effectively 84 ppb)
exposed to ozone at concentrations of less than set in 1997 [81]. In setting the 75 ppb level, he
0.080 ppm will certainly be considered in the explicitly noted that he was not explicitly follow-
current review (post-2008) and potential revision ing the advice of the CASAC which advised that
of the Ozone NAAQS. he set the standard in the range of 60–70 ppb. He
The setting of both the PM and Ozone NAAQS noted that he viewed the CASAC advice as a
serves to illustrate the complex interplay between blend of science and policy judgment which he
science and policy judgment in the setting of was not compelled to follow. The previous statis-
guidelines and standards [41]. In my opinion, the tical form for the standard was not changed.
selection of any specific numerical standard for The Administrator also elected to set the Sec-
exposure to a chemical involves both science and ondary (Welfare) Standard equal to the Primary
a policy judgment as to an acceptable risk. The (Health) Standard. The 1997 Secondary Standards
scientific information can identify for a particular for Ozone [65] had been set equal to the Primary
level of exposure an associated level of risk Standard based on the view that attainment of the
Air Quality Guidelines and Standards 35

OZONE−MORTALITY COEFFICIENTS AND 95% PIs


8−HOUR OZONE

Orlando
Denver
Kansas City, KS
Jersey City Posterior Mean
Little Rock
Des Moines National Prior
Jacksonville
San Antonio
Los Angeles
Atlanta
Posterior Mean
Lexington
Fresno
Regional Prior
Tampa
Birmingham
Lafayette Raw Estimate
Boston
El Paso
Charlotte
St. Petersburg
Seattle
Sacramento
Cedar Rapids
New Orleans
Las Vegas
Indianapolis
Wichita
Coventry
Santa Ana/Anaheim
Jackson
Riverside
Austin
Buffalo
Miami
Omaha
Salt Lake City
Evansville
Stockton
Milwaukee
San Diego
Modesto
Washington
Greensboro
Akron
Columbus, OH
Muskegon
Dayton
Baton Rouge
Raleigh
Lake Charles
Albuquerque
Fort Wayne
Louisville
Oakland
Biddeford
Johnstown
Spokane
Oklahoma City
Baltimore
Pittsburgh
Phoenix
Corpus Christi
Arlington
Kansas City, MO
San Jose
Mobile
Tacoma
Nashville
Portland
Bakersfield
Grand Rapids
Columbus, GA
Tucson
Rochester
Honolulu
Toledo
Houston
Providence
Kingston
Colorado Springs
Lincoln
Memphis
Shreveport
San Bernardino
St. Louis
Tulsa
Madison
Cleveland
Worcester
Knoxville
Cincinnati
Detroit
Syracuse
Chicago
Huntsville
Philadelphia
Dallas/Fort Worth
Newark
New York

National
−1.5 −1 −0.5 0 0.5 1 1.5 2 2.5 3 3.5
% rise mort. per 10 ppb 8−hr O3

Air Quality Guidelines and Standards, Fig. 11 Ninety- are shown alongside those for the “regional prior”
five percent posterior intervals for the ozone-mortality (squares) and the raw maximum likelihood estimates
coefficients, based on 8-h ozone, all-year data. The Bayes- (triangles). (Adapted from [58])
ian posterior estimates under the “national prior” (circles)
36 Air Quality Guidelines and Standards

8H: all-year 8H: summer


1.0 1.0
0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
0.0 0.0

24H: all-year 1.0 1H: all-year 1.0


0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
0.0 0.0

Air Quality Guidelines and Standards, Fig. 12 Map of spatially dependent ozone-mortality coefficient for 8-h ozone
(all-year data), 8-h ozone (summer data), 24-h ozone (all-year data), and 1-h ozone (all-year data). (Adapted from [58])

Primary Standard would be protective of welfare Senior Agency officials of the opportunity to
impacts and effects on plants. The CASAC had review and, perhaps, revise any rules and regula-
recommended that the averaging time form of the tions that originated with the prior Administration
Secondary Standard be changed to a more com- and not yet finalized [21]. Administrator Lisa
plex form that used a weighted average of the Jackson took the bold step of announcing that
Ozone concentration over a growing season. she was going to reconsider the Ozone NAAQS
Thus, it was not as easy to compare the Primary set by Administrator Johnson in March 2008. In
and Secondary Standards. As an aside, the revi- taking this action she was in essence saying – if
sion of the Ozone NAAQS in March 2008 also set I had been in office as EPA Administrator earlier
the dates for completing the next regularly sched- I would have made a different policy decision.
uled 5-year review, March 2013. Administrator Jackson proceeded to publish a
The failure of the EPA Administrator to explic- proposal to “reconsider” the Ozone NAAQS
itly follow the advice of CASAC was greeted with using the same science used as a basis of the
outrage by the CASAC Ozone Panel. The Com- March 2008 standard [81]. The proposal indicated
mittee took the unusual step, post-final announce- Administrator Jackson intended to follow the
ment of the new Ozone NAAQS, of holding a advice of CASAC and set a primary standard
Panel meeting to discuss the new Standard and (8-h averaging time) in the range of 60–70 ppb.
writing a letter to the Administrator reminding The proposed date for release of a final standard
him of their previous advice and calling for the was announced, a target date that was revised on
Administrator to follow their advice in future multiple occasions. A Presidential Executive
revisions of the standard [41]. Order issued by President Clinton [18] requires
In January 2009, President Barak Obama took that any proposed federal rule or action that will
office and Lisa Jackson was appointed EPA result in annual costs in excess of $100 million per
Administrator. Coincident with Obama taking year must be reviewed by the Office of Informa-
office his Chief of Staff, Rahm Emanuel, took tion and Regulatory Affairs in the Office of Man-
the customary step of reminding newly designated agement and Budget. On September 2, 2011,
Air Quality Guidelines and Standards 37

President Obama announced in a press release that will be periodically reviewed and possibly revised
he had advised EPA Administrator Jackson to not as new information is required.
proceed with the “reconsideration” of the Ozone The NAAQS as of September 18, 2011 are
NAAQS [91]. At the same time, a brief summary shown in Tables 5 and 6 in summary form. The
of the conclusions of the OIRA review was reader interested in the details that support each of
released by the Director of that Office, Cass the NAAQS is referred to the US EPA’s Website
Sunstein [62]. It briefly noted that the EPA “recon- for criteria air pollutants where detailed docu-
sideration” proposal (a) was discretionary and not ments can be found on each of the Criteria Pollut-
required by the CAA 5-year review schedule, ants. This includes information on previous
(b) was not based on the best available science reviews as well as reviews that are currently in
(the record was based on scientific literature that progress.
had been published in most cases before 2006), The final rule for each of the primary (health)
and (c) was not consistent with the President’s NAAQS published in the Federal Register are as
desire for regulations that reduced uncertainty. follows: particulate matter [75], Lead [73], Ozone
Environment groups greeted the President’s [82], Nitrogen dioxide [86], Sulfur dioxide [87],
announcement with dismay, while Business and Carbon monoxide [89]. Each of these final
applauded it. A Forum (Forum.HSPH.org) held rules contains references to the Criteria Document
on September 21, 2011 at the Harvard School of (or Integrated Science Assessment), Risk and
Public Health entitled “Smog or Jobs: The Impact exposure assessment, and proposed rule that
of Tighter Ozone Control” provides insight into undergirds the final rule. In addition, the EPA
the controversial nature of President Obama’s Web site for criteria pollutants provides linkages
decision informed by the views of his advisor, to the Regulatory Impact Analyses (RIA) that has
Sunstein. The current review of the Ozone been conducted on the proposed final rule. The
NAAQS initiated in 2008 will now proceed. RIA contain information on the monetized bene-
A key initial step in the review process occurred fits of the rule and the associated costs of achiev-
with release in March 2011 of new integrated ing the NAAQS. In accordance with the US
science assessment for ozone [88]. A proposal Supreme Court ruling in American Trucking Asso-
for the Ozone Standard should be issued in 2012 ciations v. EPA [4] and Whitman v. American
for public comment and a final rule for continuing Trucking Associations [93], the costs of
or revising the Ozone NAAQS should be issued in implementing the NAAQS may not be considered
March 2013 if EPA adheres to the 5-year schedule by the EPA Administrator in the setting of the
specified in the Clean Air Act [16]. NAAQS. However, these costs can be considered
in developing a schedule for implementation of
each NAAQS.
The current WHO air quality guidelines are
Current Air Quality Standards and summarized in Tables 7, 8, 9, and 10. The basis
Guidelines for these guidelines is contained in WHO docu-
ments [95, 96].
As noted earlier, the National Ambient Air Qual-
ity Standards established by the US Environmen-
tal Protection Agency are constantly changing. Future Directions
Indeed, the Clean Air Act specifies that each
NAAQS should be reviewed every 5 years. This entry has provided an overview of Air Qual-
Although this schedule has been rarely met, the ity Guidelines and Standards focusing on the stan-
reviews continue and changes in the NAAQS dards developed by the US Environmental
have occurred. There is no specified schedule for Protection Agency and the Guidelines developed
review of the WHO Air Quality Guidelines. How- by the World Health Organization. The latter
ever, it would be reasonable to assume that they Guidelines, although stated to provide guidance
38 Air Quality Guidelines and Standards

Air Quality Guidelines and Standards, Table 5 Summary information on criteria air pollutants regulated as NAAQSa
by the USEPA
Subpopulations of
Pollutant Sources Key effects of concern concern
Ozone Photochemical oxidation of nitrogen Decreased pulmonary Children, people with
oxides (primarily from combustion) function, lung inflammation, preexisting lung disease
and volatile organic compounds (from increased respiratory hospital outdoor-exercising health
stationary and mobile sources) admissions people
Nitrogen Photochemical oxidation of nitric oxide Respiratory illness, decreased Children, people with
dioxide (primarily from combustion of fossil pulmonary function preexisting lung disease
fuels) and direct emissions (primarily
from combustion of natural gas)
Sulfur Primarily combustion of sulfur- Respiratory injury or death, Children, people with
dioxide containing fossil fuels; also smelters, decreased pulmonary function preexisting lung disease
refineries, and others (especially asthma)
Particulate Direct emission of particles during Injury and death Children, people with
matter combustion, industrial processes, gas preexisting heart and lung
reactions and condensation and disease
coagulation natural sources
Carbon Combustion of fuels, especially by Shortening of time to onset People with coronary
monoxide mobile sources angina and other heart effects artery disease
Lead Leaded gasoline (prior to phase-out in Developmental neurotoxicity Children
gasoline);point sources such as Pb
mines, smelters, and recycling
operations
a
NAAQSs are specified by indicator concentration, averaging time, and statistical form. The latter used to determine
compliance and is too complex for coverage here. However, suffice it to note that both the specific numerical level and the
statistical form determine the stringency of the standard

for use around the world, have focused on Europe. goals. In the United States, major regulations have
For Europe, the WHO Guidelines have provided mandated reductions in emissions of particulate
valuable input to national and local authorities for matter, SO2, and NO2 from stationary sources
developing legal binding air quality standards. such as power plants and from mobile sources
The Standards developed by European nations such as passenger cars and on-road trucks and,
and other nations round the world have not been more recently, from off-road equipment, rail loco-
reviewed in detail in this entry. motives, and ships. These regulations have
The section on “Air Quality Management resulted in substantial reductions in the emissions
Framework” emphasized that Air Quality Stan- of the criteria pollutants or their precursors while
dards and Guidelines were a key element of the the economy also grew until recently. A stagnant
overall scheme; however, the Standards and economy in 2011 is raising questions as to the
Guidelines are just one element of an integrated wisdom of further reductions in NAAQS and
air quality management scheme. It is noteworthy aggressive regulatory actions to further reduce
that substantial progress has been made in emissions.
improving air quality in the United States and in Since the Clean Air Act Amendments of 1970
western European countries. That progress has no were passed in the United States there has been a
doubt been facilitated by the Standards and steady increase in research on the health effects of
Guidelines. However, setting up goal posts air pollutants. The increase in research has been
(Standards and Guidelines) does not necessarily most notable since the mid-1990s when major
mean the goals will be achieved. Specific emis- controversies arose over the health effects of
sion reductions informed by the Standards and PM2.5. Indeed, what has developed might be char-
Guidelines are ultimately required to achieve the acterized as a “clean air enterprise” involving air
Air Quality Guidelines and Standards 39

Air Quality Guidelines and Standards, Table 6 National Ambient Air Quality Standards for criteria pollutants
Primary standards Secondary standards
Pollutant Level Averaging time Level Averaging time
Carbon monoxide 9 ppm (10 mg/m3) 8-ha None
35 ppm (40 mg/m3) 1-ha
Lead 0.15 mg/m3 b Rolling 3-month average Same as primary
Nitrogen dioxide 53 ppbc Annual (arithmetic average) Same as primary
100 ppb 1-hd Nonel
Particulate matter (PM10) 150 mg/m3 24-he Same as primary
Particulate matter (PM2.5) 15.0 mg/m3 Annualf (arithmetic average) Same as primary
35 mg/m3 24-hg
Ozone 0.075 ppm (2008 std) 8-hh Same as primary
0.08 ppm (1997 std) 8-hi
0.12 ppm 1-hj
Sulfur dioxide 0.03 ppm Annual (arithmetic average) 0.5 ppm 3-ha
0.14 ppm 24-ha
75 ppbk 1-h Nonel
Source: Taken from US EPA Website, July 26, 2011
a
Not to be exceeded more than once per year
b
Final rule signed October 15, 2008. The 1978 lead standard (1.5 mg/m3 as a quarterly average) remains in effect until
1 year after an area is designated for the 2008 standard, except that in areas designated nonattainment for the 1978
standard, the 1978 standard remains in effect until implementation plans to attain or maintain the 2008 standard are
approved
c
The official level of the annual NO2 standard is 0.053 ppm, equal to 53 ppb, which is shown here for the purpose of
clearer comparison to the 1-h standard
d
To attain this standard, the 3-year average of the 98th percentile of the daily maximum 1-h average at each monitor within
an area must not exceed 100 ppb (effective January 22, 2010)
e
Not to be exceeded more than once per year on average over 3 years
f
To attain this standard, the 3-year average of the weighted annual mean PM2.5 concentrations from single or multiple
community-oriented monitors must not exceed 15.0 mg/m3
g
To attain this standard, the 3-year average of the 98th percentile of 24-h concentrations at each population-oriented
monitor within an area must not exceed 35 mg/m3 (effective December 17, 2006)
h
To attain this standard, the 3-year average of the fourth-highest daily maximum 8-h average ozone concentrations
measured at each monitor within an area over each year must not exceed 0.075 ppm (effective May 27, 2008)
i
(a) To attain this standard, the 3-year average of the fourth-highest daily maximum 8-h average ozone concentrations
measured at each monitor within an area over each year must not exceed 0.08 ppm(b) The 1997 standard – and the
implementation rules for that standard – will remain in place for implementation purposes as EPA undertakes rule making
to address the transition from the 1997 ozone standard to the 2008 ozone standard(c) EPA is in the process of
reconsidering these standards (set in March 2008)
j
(a) EPA revoked the 1-h ozone standard in all areas, although some areas have continuing obligations under that standard
(“antibacksliding”)(b) The standard is attained when the expected number of days per calendar year with maximum hourly
average concentrations above 0.12 ppm is 1
k
Final rule signed June 2, 2010. To attain this standard, the 3-year average of the 99th percentile of the daily maximum 1-h
average at each monitor within an area must not exceed 75 ppb
l
On July 12, 2011, the EPA Administrator proposed to set Secondary NAAQS for NO2 and SO2 for a 1-h averaging time at
concentrations equal to the Primary Standards, NO2 – 100 ppb and SO2 – 75 ppb (Note: This footnote was added by Roger
O. McClellan)

quality regulators, the academic research commu- or “dirty air.” This polarized approach has fre-
nity, and nongovernmental organization advocacy quently resulted in the focus being on a single
groups. Some individuals would quickly note that risk factor, air quality, rather than the overall
this enterprise is counterbalanced by corporations well-being of the health of societies around the
and industrial groups advocating for the status quo world.
40 Air Quality Guidelines and Standards

Air Quality Guidelines and Standards, Table 7 WHO air quality guidelines and interim targets for particulate mattera
Annual mean concentration
PM10 PM2.5
(mg/m3) (mg/m3) Basis for the selected level
Interim Target-1 70 35 These levels are associated with about a 15% high long-term mortality
(IT-1) risk relative to the AQG level
Interim Target-2 50 25 In addition to other health benefits, these levels lower the risk of
(IT-2) premature mortality by approximately 6% (2–11%) relative to the IT-1
level
Interim Target-3 30 15 In addition to other health benefits, these levels reduce the mortality risk
(IT-3) by approximately 6% (2–11%) relative to the IT-2 level
Air Quality 20 10 These are the lowest levels at which total, cardiopulmonary and lung
Guideline (AQG) cancer mortality have been shown to increase with more than 95%
confidence in response to long-term exposure to PM2.5
24-h concentrations [99th percentile (3 days/year)]
PM10 PM2.5 Basis for the selected level
(mg/m3) (mg/m3)
Interim Target-1 150 75 Based on published risk coefficient from multi-center studies and meta-
(IT-1) analyses (about 5% increase of short-term mortality over the AQG value)
Interim Target-2 100 50 Based on published risk coefficients from multiple-center studies and
(IT-2) meta-analyses (about 2.5% increase of short-term mortality over the
AQG value)
Interim Target-3 75 37.5 Based on published risk coefficients from multi-center studies and meta-
(IT-3)a analyses (about 1.2% increase in short-term mortality over the AQG
value)
Air quality 50 25 Based on relationship between 24-h and annual PM levels been shown to
increase with more than 95%
Source: WHO [96]
a
The use of PM2.5 guideline value is preferred

The earlier section on “Context for Air Quality commonplace around the world centuries ago. It is
Impacts” noted the multitude of risk factors that clear that in the future a major challenge exists to
impact on health. That section contrasted the burden improve the income of families in low- and middle-
of disease attributed to the various risk factors income countries so they can move away from
including urban air pollution and indoor smoke uncontrolled combustion of solid fuels indoors. It
from household use of solid fuels. The contrast is well recognized that improving the economy of a
between the burden of disease for low- and country or region inevitably requires increases in
middle-income countries versus high-income coun- energy usage and the availability of clean water
tries was striking. In the former, 3.7% of deaths were and adequate foodstuffs. A major challenge exists
associated with indoor smoke and 1.5% from urban in providing adequate energy, in the form of distrib-
air pollutions. In contrast, in the high-income coun- uted electricity and liquid fuels for transportation
tries urban air pollution was estimated to be associ- and also avoiding negative impacts on air quality.
ated with 1.0% of the deaths and no deaths were Major progress has been made in the highest income
estimated to be associated with indoor smoke. The countries in the world in developing low-emission
health hazards associated with indoor smoke from stationary sources for generating electrical power
use of solid fuels for cooking and heating has not and low emission internal combustion [both spark
been reviewed in this entry. It is sufficient to note ignition and compression ignition (diesel)] engines
here that the greatest hazards from indoor cooking for on- and off-road use. The challenge is to facili-
are those related to burning of wood, agricultural tate the transfer of those low emission technologies
residue, and coal in the same manner as was to the rest of the world.
Air Quality Guidelines and Standards 41

Air Quality Guidelines and Standards, Table 8 WHO air quality guideline and interim target for ozone: 8-h
concentrations
Daily maximum 8-h
mean (mg/m3) Basis for selected level
High levels 240 Significant health effects; substantial proportion of vulnerable
populations affected
Interim Target-1 160 Important health effects; does not provide adequate protection of public
(IT-1) health
Exposure to this level of ozone is associated with:
Physiological and inflammatory lung effects in healthy exercising
young adults exposed for periods of 6.6 h
Health effects in children (based on various summer camp studies in
which children were exposed to ambient ozone levels)
An estimated 3–5% increase in daily mortalitya (based on findings of
daily time-studies)
Air Quality 100 Provides adequate protection of public health, though some health effects
Guideline (AQG) may occur below this level. Exposure to this level of ozone is associated
with:
An estimated 1–2% increase in daily mortalitya (based on findings of
daily time-series studies)
Extrapolation from chamber and field studies based on the likelihood
that real-life exposure tends to be repetitive and chamber studies exclude
highly sensitive or clinically compromised subjects, or children
Likelihood that ambient ozone is a marker for related oxidants
a
Deaths attributable to ozone. Time-series studies indicate an increase in daily mortality in the range of 0.3–0.5% for every
10 mg/m3 increment in 8-h ozone concentrations above an estimated baseline level of 70 mg/m3

Air Quality Guidelines and Standards, Table 9 WHO air quality guidelines and interim targets for SOx: 24-h and
10-min concentrations
24-h
average 10-min average
(mg/m3) (mg/m3) Basis for selected level
Interim 125 –
Target-1 (IT-1)a
Interim Intermediate goal based on controlling either motor vehicle
Target-2 (IT-2) emissions, industrial emissions, and/or emissions from power
production. This would be a reasonable and feasible goal for
some developing countries (it could be achieved within a few
years) which would lead to significant health improvements that,
in turn, would justify further improvements (such as aiming for
the AQG value)
Air Quality 20 500
Guideline
(AQG)
a
Formerly the WHO Air Quality Guideline [95]

With the above as background, it is appro- a science based on the health effects of air
priate to return to the central focus of this pollutants and the use of that science to inform
entry – air quality standards and guidelines the development of air quality standards and
and their role in the future. The past 40 years guidelines and to inform the development and
have been a period of major activity in creating implementation of strategies and technologies
42 Air Quality Guidelines and Standards

Air Quality Guidelines and Standards, Irrespective of the specifics of the science
Table 10 WHO (European) guideline values for carbon available, it can be anticipated that increasing
monoxide
attention will focus on how science is used to
100 mg/m3a 15 min decide on the level and statistical form of air
60 mg/m3 a 30 min quality standards and guidelines. The issue is rel-
30 mg/m3 a 1h
evant to both the setting of Standards and Guide-
10 mg/m3 8h
a
lines, however, it is especially critical as it relates
Exposure at these levels should be no longer than the
to standards which are legally binding. A review
indicated times and should not be repeated within 8 h
Source: WHO [95] of all the existing Guidelines and Standards for
criteria or common air pollutants suggests they
have been based on judgment. In some cases,
to improve air quality. The field is at an inter- those judgments were made exclusively by scien-
esting juncture that may be framed with the tists, that is, the WHO Air Quality Guidelines. In
question – “how low is low enough for air other cases, as in the setting of National Ambient
quality standards and guidance?” Air Quality Standards by the US EPA, the deci-
Science should have an important role in sions were made by appointed government offi-
addressing that question, however, scientific cials and informed by the science reviewed by the
knowledge alone will not be sufficient to answer Clean Air Scientific Advisory Committee. As best
the question. Epidemiological studies with it can be determined none of the Guidelines or
improved design and execution may give us Standards were set at a specific defined level of
some marginal improvement in estimates of the risk. This is remarkable since each level (and its
health risks associated with exposure to low ambi- associated statistical form) for a Guideline or
ent concentrations of various air constituents. It Standard reflects a level of acceptable risk:
will be especially challenging to demonstrate the above this level and statistical form the health
shape of the ambient concentration-response rela- risks are not acceptable and below this level and
tionship at concentrations that include back- statistical form the health risks of exposure are
ground levels. Rather than a singular focus on deemed acceptable. If scientists argue that there
health effects attributable to air pollution as in is a linear, nothreshold relationship between ambi-
the past, future epidemiological studies will better ent concentrations of an air pollutant and associ-
serve the needs of Society when they consider ated health responses down to background
more broadly the multiple factors that influence concentrations, then no concentration is free of
disease outcomes. A finding of relative risks of 1.1 some level of calculated excess risk.
or less for a specific air pollutant begs the question In this author’s view, decisions on acceptable
of what are the dominant risk factors driving the health risks for the public should be informed by
baseline health risks. the best science available. However, scientists
It has become commonplace for scientists alone are not in a position to make broad policy
using cellular and molecular approaches to argue decisions on acceptable risk. Indeed, pronounce-
for more research using their tools to investigate ments by individual scientists or scientific com-
the mechanisms of action of various air pollutants. mittees need to be recognized as a statement of the
Based on the evidence that air pollution in the individual preference for a particular policy out-
highest income countries of the world is not a come or the collective view of the Committee. The
major influence on the health of the population it current worldwide economic crisis results in every
is appropriate to ask whether a more detailed major financial investment made by either public
understanding of this specific risk factor, air pol- or private entities being considered in the context
lutants, will be of value in guiding critical societal of the future return on the investment in terms of
decisions. An alternative would be to focus on the the public or private good that will result. The
broader range of risk factors that influence the focus increasingly is on choices that must be
baseline risk. made between alternative uses of funds,
Air Quality Guidelines and Standards 43

irrespective of whether the funding is from the 11. Breyer S (1982) Regulation and reform. Harvard Uni-
public or private sector. Clean air is universally versity Press, Cambridge
12. Breyer S (1993) Breaking the vicious circle: toward
viewed as a right. The question increasingly for effective risk regulation. Harvard University Press,
policy makers, as representatives of the public, is Cambridge, MA . (Based on 1992 Oliver Wendell
how clean is clean enough? This question cannot Holmes lectures at Harvard Law School)
be addressed in isolation; it should be addressed in 13. Brown JS, Bateson TF, McDonnell WF (2008) Effects
of exposure to 0.06 ppm ozone in FEV1 in humans: a
the context of all the risk factors influencing secondary analysis of existing data. Environ Health
human health. The question for scientists is how Persp 116:1023–1026
to create the scientific knowledge on air pollutants 14. CAA (1963) The Clean Air Act of 1963
and other risk factors that affect human health to 15. CAA (1970) The Clean Air Act Amendments of 1970-
P.L. 91–04 (December 31, 1970), Plus Technical
inform these important societal decisions. Amendments Made by P.L. 92–157 (November
18, 1971)
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exposure to high concentrations of NO2 causes
Air Quality, Surface adverse health effects, and levels regularly
Transportation Impacts on exceed air quality standards.
O3 Ground-level ozone, a secondary pollutant
Paul Boulter produced by reactions between NO2, hydrocar-
PAEHolmes, Sydney, Australia bons, and sunlight. High levels of ozone are
generally observed during hot, sunny weather,
and concentrations tend to be higher in rural
Article Outline areas than in urban areas.
PM10 Mass concentration of particles with an aero-
Glossary dynamic diameter of less than 10 mm. Particles
Definition of the Subject smaller than 10 mm (also known as “thoracic”
Introduction particles) can settle in the bronchi and lungs.
Historical Trends PM2.5 Mass concentration of particles with an
Air Pollution Pathways aerodynamic diameter of less than 2.5 mm,
Emission Processes sometimes referred to as “fine” or “respirable”
Modelling Transport Emissions particles. Particles in this size range can pene-
Pollutant Dispersion and Transformation trate deep into the lungs.
Modelling Air Pollution from Transport Primary particles Particles emitted directly to
Reducing Air Pollution from Transport the atmosphere, typically as a result of com-
Future Directions bustion or abrasion processes.
Bibliography SCR Selective catalytic reduction, an exhaust
aftertreatment method that is used to reduce
Glossary emissions of nitrogen oxides. It will be the
main technology for enabling compliance
DPF Diesel particulate filter, the preferred and with future emission standards.
most effective technology for removing partic- Secondary particles Particles formed within the
ulate matter from diesel exhaust. DPFs can be atmosphere from gas-phase precursors. These
broadly divided into two types: “full flow” and include particles originating from atmospheric
“partial flow.” The latter are more permeable oxidation of sulfur and nitrogen oxides, and
and are less effective, but need no maintenance. their reaction products with ammonia, and
DPFs physically capture particles and can fill up from the oxidation of organic compounds.
rapidly. They must therefore be periodically Ultrafine particles Particles with a diameter of
“regenerated,” and several passive and active less than 0.1 mm. These can pass through cell
systems have been developed for this purpose. membranes and migrate from the lungs into
Emission standard A value that specifies the other organs. There is evidence to indicate
maximum amount of a pollutant that can be that they may be more damaging to the cardio-
released into the environment per unit activity vascular system than PM10 and PM2.5.
(e.g., g/km or g/kWh).
NO2 Nitrogen dioxide, a gaseous air pollutant
produced as a result of combustion. NO2 is Definition of the Subject
also a precursor for a number of harmful sec-
ondary air pollutants such as ozone, and plays a Until the middle of the twentieth century poor air
role in the formation of acid rain. Long-term quality in populated areas was usually associated

© Springer Science+Business Media, LLC 2012 47


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_554
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_554
48 Air Quality, Surface Transportation Impacts on

with domestic and industrial combustion, with direct and indirect detrimental impacts on amenity,
coal burning leading to high concentrations of health, ecosystems, and cultural heritage over dif-
smoke and sulfur dioxide. A recent retrospective ferent time periods and on different geographical
analysis has indicated that the most famous exam- scales. The effects of transport pollution can be
ple of this type of pollution – the great London very local and immediate, such as the nuisance
smog of 1952 – was responsible for 12,000 deaths caused by a plume of black smoke from the
[1]. However, during the 1940s and 1950s an exhaust pipe of a car or a diesel train. More seri-
altogether different type of pollution was observed ously, repeated exposure to exhaust gases and
in the United States. Haagen-Smit identified a particles is linked to aggravated respiratory and
mechanism by which air pollutants reacted with cardiovascular disease, changes to lung tissue,
the Los Angeles sunlight to produce a noxious changes in the function of the nervous system,
photochemical smog [2], and it became clear that and premature mortality [3, 4]. Threats to cultural
the pollution originated not from the use of coal heritage posed by atmospheric pollutants include
but from road vehicles. the soiling of historical buildings – a common
In the subsequent decades urban air pollution sight alongside busy urban roads – and indoor
has become synonymous with road transport, the damage to works of art and museum exhibits.
link being attributable primarily to the growth in Transport emissions also contribute to the regional
the ownership and use of private cars. Photochem- degradation of air quality, to eutrophication, and to
ical smog has remained a problem in some of the acidification (see Chapter, ▶ “Regional Air Qual-
largest cities in the world, and many people are ity”). Moreover, stable pollutants, including the
exposed to pollutant concentrations which exceed greenhouse gases carbon dioxide (CO2), methane,
health-based air quality standards. It has also and nitrous oxide can contribute to environmental
become evident that some transport-derived pol- problems on a global scale for decades and even
lutants can travel thousands of kilometers before centuries.
deposition and damage occur and, in the case of The pollutants that are currently causing the
greenhouse gases, can have a global effect over greatest concern in terms of air quality, primarily
long timescales. If transport systems are to become because of their impact on human health, are air-
environmentally sustainable, then the scale of such borne particulate matter (PM), nitrogen dioxide
adverse effects will have to be greatly reduced. (NO2), and ground-level ozone (O3). Surface
The aim of this entry is to provide an overview transport is an important contributor to all three
of the impacts of surface transport (road, rail, and [5], but road transport is the main culprit, espe-
shipping) on emissions and air quality. Different cially in population centers, and it presents some of
regions of the world have different air pollution the greatest challenges in terms of sustainability.
problems, and not all countries and issues can be The importance of road transport as a source of
covered here. The entry refers mainly, but not pollution can be illustrated by reference to sectoral
exclusively, to the European Union (EU), and emissions in Europe. Figure 1 shows emission
the emphasis is on local air pollution in populated data for the EU-27 countries, based on submis-
areas. Inevitably, the entry deals predominantly sions to the UNECE Convention on Long-range
with road transport, but some consideration is Transboundary Air Pollution (CLRTAP). In 2008,
also given to the other modes. road transport was the largest contributor to NOx
emissions in Europe (41%), and was also a major
contributor to PM10 emissions. By comparison,
Introduction non-road transport was responsible for just 7% of
total NOx emissions and only 2% of total PM10
Surface transport is an important, and in many emissions. However, it is important to observe
respects, the most important source of air pollu- that the totals in Fig. 1 are based on national
tion. The pollutants released from road, rail, and reporting, and do not include international avia-
waterborne traffic are implicated in a variety of tion or international maritime shipping. The latter
Air Quality, Surface Transportation Impacts on 49

NOx Commercial, PM10


institutional and
households Industrial
Non-road 14% processes
transport Solvent and
2% product use
7%
1%
Industrial
Solvent and
processes
product use Waste
17% Agriculture
0% 2%
12%
Road transport Agriculture Commercial, Other
41% 2% institutional and 0%
Energy households
Waste 35%
production and 0% Energy
distribution Energy use in production and
Other
20% industry distribution
Energy use in 0%
10% 7%
industry Road transport
14% 14%

Non-road
transport
2%
Total = 10.4 million tonnes Total = 2.1 million tonnes

Air Quality, Surface Transportation Impacts on, Fig. 1 NOx and PM10 emissions in 2008 by sector, based on data
submitted by EU-27 countries to CLRTAP [8]

is an important source of NOx and sulfur oxides directly affect a large population [13]. Ships at
(SOx). Recent studies have indicated that around berth are the main source of shipping emissions
15% of global NOx emissions and 5–8% of global in ports; the time spent at berth is typically 1 or
SOx emissions are attributable to oceangoing more days, whereas the time spent maneuvering is
ships [6, 7]. typically only a few hours [14]. Moreover, almost
At the local level, the impacts of road transport 70% of maritime ship emissions occur within
are exacerbated by the proximity of vehicles (and 400 km of land, and ships therefore have the
their emissions) to the population, although the potential to contribute significantly to pollution
other surface transport modes can contribute sig- in coastal communities [13]. On the global scale,
nificantly to poor air quality at specific sites such PM emissions from marine shipping are thought
as busy railway stations, underground systems, to be responsible for around 60,000 deaths annu-
and large ports. ally, with impacts concentrated in coastal regions
Rail transport only contributes a small propor- on major trade routes. Most mortality effects are
tion to total emissions from the transport sector, seen in Asia and Europe where high populations
but individual diesel locomotives have large and high shipping-related PM concentrations
engines, and exhaust aftertreatment equipment is coincide [13].
not currently used on traction units. Elevated pol- The literature on transport-related air pollu-
lutant concentrations have therefore been tion is very extensive, and it is not possible to
observed where diesel locomotives are running cover every aspect in depth in this entry. The
with the engine at idle in enclosed stations emphasis is therefore on key areas such as his-
[9]. Several studies have addressed the exposure torical trends in transport activity and emissions,
of passengers to air pollution in underground rail the processes of pollutant formation, and model-
systems, where pollutant concentrations appear to ling approaches. Importantly, given the context
be considerably higher than those above ground. of this encyclopedia, a substantial part of the
For example, consistently high concentrations of entry is devoted to policies and measures which
PM10 and PM2.5 have been reported [10–12]. can be implemented to reduce the impacts of
Many major ports are also major cities, and so surface transport on air quality, and thus contrib-
emissions from seagoing ships in such ports can ute to sustainability.
50 Air Quality, Surface Transportation Impacts on

Historical Trends transport by air increased by 62% (see Chapter,


▶ “Aviation and Atmosphere”). Road freight in
The general trend in motorized transport has been the EU-27 increased by almost 50% between
one of unremitting growth, driven primarily by the 1995 and 2008, and there was also substantial
association of personal mobility with quality of life growth in the transport of freight by rail (15%),
[15] and its consequence in terms of passenger car inland waterways (19%) and shipping (30%).
ownership. In the United States the number of cars In response to similar trends in all industrialized
grew from 140,000 in 1907 to more than 20 million countries and their implications for air quality,
in 1927 [15]. A similar pattern occurred in Europe legislation and strategies have been put in place
several decades later – Fig. 2 shows car ownership to combat transport-related emissions. Calcula-
in some European countries since 1970 – and is tions have established that emissions from road
being repeated again now in parts of Asia. transport in the EU peaked in the early 1990s [18]
The recent evolution of transport activity in the but have been reducing since then as controls on
EU-27 countries is shown in Fig. 3. The top graph fuel and emissions have tightened (Fig. 4). Emis-
shows passenger transport by mode in passenger- sions of regulated pollutants are likely to continue
kilometers (pkm) (note the different scales), and to decrease in the future as new vehicles, locomo-
the bottom graph shows freight transport in tonne- tives, and vessels, which comply with more strin-
kilometers (tkm). Between 1995 and 2008, passen- gent emission limits, replace older ones, although
ger transport by car increased by 21%. The growth the reductions will be offset to some extent by
in passenger transport was lower for buses/coaches growth in transport activity.
(9%) and rail (17%), and there was a net reduction There have been some notable successes. In spite
of 8% in passenger transport by sea. Although it is of the continued growth in traffic in Europe, the
not of direct relevance to this entry, it should be emissions and atmospheric concentrations of some
recognized that during the same period passenger pollutants – such as lead, carbon monoxide and

Air Quality, Surface


Transportation 700
Impacts on, Belgium
Fig. 2 Passenger car
ownership in selected Denmark
600
European countries. Greece
(Adapted from [16, 17])
Italy
500
Romania
cars per 1,000 people

400

300

200

100

0
1965 1970 1975 1980 1985 1990 1995 2000 2005 2010
Year
Air Quality, Surface Transportation Impacts on 51

5,000 1,000
Passenger cars (billion pkm)

Other modes (billion pkm)


4,000 800
Passenger cars
3,000 600 Bus and coach
Two-wheel veh.
2,000 400
Railway

1,000 200 Sea

0 0
1995
1996
1997
1998
1999
2000
2001
2002
2003
2004
2005
2006
2007
2008
2,500
Freight transport (billion tkm)

2,000
Road
1,500 Rail
Inland waterway
1,000 Sea

500

0
1995
1996
1997
1998
1999
2000
2001
2002
2003
2004
2005
2006
2007
2008

Air Quality, Surface Transportation Impacts on, Fig. 3 Passenger and freight transport in the EU-27 countries by
mode between 1995 and 2008. (Adapted from [17])

benzene – have decreased so dramatically that they currently increasing in line with traffic growth
are no longer considered to be a major threat to (bottom graph in Fig. 4).
human health. However, in many urban areas the
concentrations of NO2 and PM10 still frequently
exceed health-based limit values. According to the Air Pollution Pathways
European Environment Agency, in 2004, more than
20% of the European urban population were The links between transport, emissions, air pollu-
exposed to ambient NO2 concentrations above the tion, and adverse impacts are not straightforward.
annual mean limit value (40 mg/m3) [19]. Further- To illustrate this, the complex pathway from emis-
more, NO2 and PM10 concentrations at many road- sions to one specific type of impact – the health
side monitoring sites are not decreasing [19–21]. outcomes of road transport pollution – is summa-
The problem is not confined to Europe; for exam- rized in Fig. 5.
ple, a similar problem has been observed in Japan Many different pollutants are emitted by road
[22]. Some possible reasons for this are explored traffic, and the strength of the source depends on
later in this entry. A further concern is that emis- the emission factors for the vehicles and the char-
sions of non-exhaust particles – especially those acteristics of the traffic (e.g., volume, speed and
arising from road vehicle tire and brake wear – are composition). The emitted (primary) pollutants
not subject to legislation or control, and are are then dispersed in the ambient air according
52 Air Quality, Surface Transportation Impacts on

40,000
CO emissions (1,000 tonnes)

Road: Passenger cars


30,000 Road: Light duty vehicles
Road: Heavy-duty vehicles
20,000
Road: Two-wheel vehicles
Railways
10,000
International inland waterways
National navigation (shipping)
0
1990
1991
1992
1993
1994
1995
1996
1997
1998
1999
2000
2001
2002
2003
2004
2005
2006
2007
2008
8,000
NOx emissions (1,000 tonnes)

Road: Passenger cars


6,000 Road: Light duty vehicles
Road: Heavy-duty vehicles
4,000
Road: Two-wheel vehicles
Railways
2,000
International inland waterways
National navigation (shipping)
0
1990
1991
1992
1993
1994
1995
1996
1997
1998
1999
2000
2001
2002
2003
2004
2005
2006
2007
2008
PM10 emissions (1,000 tonnes)

450
Road: Passenger cars
400
350 Road: Light duty vehicles
300 Road: Heavy-duty vehicles
250 Road: Two-wheel vehicles
200
Road: tyre & brake wear
150
100 Road: road abrasion
50 Railways
0
International inland waterways
1990
1991
1992
1993
1994
1995
1996
1997
1998
1999
2000
2001
2002
2003
2004
2005
2006
2007
2008

National navigation (shipping)

Air Quality, Surface Transportation Impacts on, Fig. 4 CO, NOx, and PM10 emissions by transport mode (excluding
aviation) between 1990 and 2008, submitted by EU-27 countries to CLRTAP [8]

to the local topography and meteorology. The which they are engaged, the locations of those
main direct impacts of primary pollutants are activities, and the pollutant concentrations in
near to the point of emission; further away, con- those locations. One way of determining “inte-
centration decreases rapidly as a result of disper- grated” personal exposure is through the use of a
sion and dilution. However, many of the primary “microenvironment” model [24]. The term micro-
pollutants react together, and with pollutants from environment describes a location with a distinct
other sources, to form secondary pollutants. level of pollution, such as outdoors in the street,
Because of the time required for their formation, indoors at home, in transit, at the workplace,
the concentrations of secondary pollutants are not etc. The fraction of time spent in each microenvi-
always highest near the emission source. ronment allows the calculation of integrated expo-
The overall exposure of individuals to air pol- sure. However, the calculation of such an integral
lutants is dependent upon the types of activity in is often not possible because the pollutant
Air Quality, Surface Transportation Impacts on 53

Emission factors
vehicles powered by electricity drawn from an
Emissions
external grid (as in the case of rail locomotives),
from on-board batteries (as in the case of road
Activity data
vehicles and waterborne vessels) or, more
recently, from in situ generation involving fuel
Atmospheric conditions
cells.
The principles of ICEs apply equally to road
Ambient
concentrations
vehicles, rail locomotives, and waterborne ves-
sels, the main differences being the size of the
Human activity engine and the type of fuel used. In an ICE energy
is derived from the burning of hydrocarbon fuel in
Exposure
air, with the main products being CO2 and water
vapor. Incomplete combustion results in the pro-
Respiratory conditions
duction of CO, PM (especially in the case of diesel
Dose engines), and many different organic compounds.
In addition, at the high temperatures and pressures
Physiological conditions found in the combustion chamber, some of the
nitrogen in the air is oxidized, forming mainly
Health effects
nitric oxide (NO) with some NO2. By convention,
the sum total of oxides of nitrogen (i.e., NO +
Air Quality, Surface Transportation Impacts on, NO2) is termed NOx.
Fig. 5 Simplified pathway from transport emission to NO formation proceeds via two main mecha-
health effect. (Adapted from [23])
nisms: the “thermal” (Zel’dovich) and “prompt”
mechanisms [26], with the former being respon-
concentrations in the different microenvironments
sible for more than 90% of emissions [27]. NO2 is
are not known. The term “average exposure” is
predominantly a secondary pollutant, its major
therefore commonly used, and this is normally
source being the atmospheric oxidation of
taken to mean the pollutant concentration over a
combustion-derived NO. The NO2 emitted
specified period (e.g., annual mean) at an outdoor
directly from vehicles is referred to as “primary
location which is broadly representative of where
NO2,” and its importance will be described later.
people are likely to spend time. This approach is
Particles in diesel exhaust cover a range of
used in the regulation of ambient air quality.
sizes, and the shape of the size distribution
Once the pollutant has crossed a physical
depends on whether the weighting is by number
boundary (e.g., alveolar epithelial cells), the con-
or mass (Fig. 6). There are three distinct size
cept of “dose” is used [25]. The dose is the mass of
modes: the nucleation mode (sometimes referred
material absorbed or deposited in the body during
to as nuclei or nanoparticles), the accumulation
an interval of time, and depends on the respiratory
mode, and the coarse mode. The nucleation mode
activity of the individuals concerned. Responses
has traditionally been defined as particles with a
to doses – the actual health effects – can also vary
diameter of less than 50 nm. Accumulation mode
from person to person, depending on physiologi-
particles range in size from around 50 nm to
cal conditions.
around 1 mm, with particles smaller than 0.1 mm
being referred to as ultrafine particles. When a
nucleation mode is observed (this is not always
Emission Processes the case in engine exhaust), it contains many more
particles than the accumulation mode, although
Combustion because each particle is so small the total mass
Most vehicles are powered by internal combus- will not increase substantially. The coarse mode
tion engines (ICEs). Notable exceptions include consists of particles larger than around 1 mm.
54 Air Quality, Surface Transportation Impacts on

0.20
Number Nanoparticles
0.18 (Dp < 50 nm)
weighted
0.16 Mass
weighted Ultrafine particles
0.14
(Dp < 100 nm)
0.12 Fine particles
dlogDp

(Dp < 2.5 µm)


0.10

0.08

0.06

0.04
Nucleation Accumulation Coarse
0.02 mode mode mode
0.00
0.001 0.01 0.1 1 10
Diameter (mm)

Air Quality, Surface Transportation Impacts on, Fig. 6 Typical particle size distributions in vehicle exhaust. The
y-axis is a normalized log scale. (Adapted from [28])

The processes of particle formation during The main factors that govern exhaust emis-
diesel combustion have been described in sions are the vehicle type, the fuel used, the vehi-
detail [26]. Carbonaceous spherules (soot) are cle technology, and the driving conditions. The
initially created in the cylinder. A phase of particle term “vehicle technology” can be used to refer to
growth then follows, involving the adsorption of either a specific type of engine or exhaust aftert-
gas-phase components, as well as coagulation and reatment, or more generally compliance with a
agglomeration. Almost all the particles found in particular emission standard. Some examples of
the exhaust prior to dilution are present as these these effects are shown for road vehicles in Fig. 7.
carbonaceous agglomerates (hence, accumulation Other factors include vehicle weight, road gradi-
mode), with a small amount of metallic ash. The ent, vehicle load, and the use of auxiliary equip-
processes leading to the presence of nucleation ment such as air-conditioning. Another important
mode particles in the exhaust during measurement consideration is the so-called dynamics of driving
are quite complex. Most nucleation mode parti- (see section “Modelling Transport Emissions”).
cles are thought to originate from the condensa- The thermal state of the engine and exhaust
tion of volatile material (hydrocarbons, hydrated emission-control system also has a strong influ-
sulfuric acid and salts) in the exhaust gas during ence on emissions from road vehicles. Most emis-
dilution, rather than during combustion itself, and sions occur under what are known as thermally
their formation is a function of measurement stable or “hot” engine and exhaust conditions. The
parameters such as temperature, dilution ratio, temperature of engine coolant during normal
residence time, and humidity [28–30], as well as operation is typically between around 70  C and
fuel sulfur content [31, 32]. Particles in the coarse 90  C, whereas the temperature of the exhaust
mode are formed by re-entrainment of material system reaches several hundred degrees centi-
previously deposited on engine cylinder and grade. During the warm-up period following an
exhaust system surfaces. Some of the pollutants engine start, emissions and fuel consumption are
emitted by fuel combustion (sulfur oxides and elevated as a result of incomplete combustion, the
nitrogen oxides) are also precursors of secondary low conversion rate of pollutants in the catalyst,
particles in the atmosphere. and increased viscous friction due to the low
Air Quality, Surface Transportation Impacts on 55

lubricant temperature in the engine and transmis- are mainly of light hydrocarbons (C4–C6)
sion. These “cold-start” emissions can constitute a [36]. Evaporative emissions from diesel-fuelled
significant proportion of total road transport emis- vehicles are considered to be negligible due to
sions, particularly in urban areas. Cold-start emis- the low volatility of diesel fuel.
sions and fuel consumption are higher for lower There are several different mechanisms of
engine starting temperatures which will, in turn, evaporation. “Diurnal losses” are due to the ther-
depend upon factors such as the length of time the mal expansion and emission of vapor, mainly in
vehicle has been parked and the prevailing ambi- the fuel tank, as a result of changes in ambient
ent temperature. temperature during the day. “Hot-soak losses”
Rail locomotives are mainly powered by either occur when a warm engine is turned off and heat
diesel or electricity. The nature of the pollution is dissipated into the fuel system. Whilst a vehicle
emitted from rail transport is dependent upon the is being driven, the engine provides a continuous
type of traction. In the case of diesel locomotives, input of heat to the fuel system, resulting in “run-
pollutants are emitted directly into the local envi- ning losses.” In addition, “refueling losses” occur
ronment as result of combustion, whereas for while the tank is being filled and the saturated
electric locomotives the emission is effectively vapors are displaced and vented into the atmo-
transposed to the power stations which are respon- sphere, but these are usually attributed to the fuel
sible for producing the electricity. Emissions from handling chain.
electric trains are therefore normally allocated to Evaporative emissions are dependent upon
the power generation sector. Compared with road four major factors: the vehicle design, the ambient
vehicles, trains generally have low emissions per temperature, the volatility of the petrol, and the
passenger-kilometer although this depends, of driving conditions. Emissions have decreased sig-
course, on the passenger load factors. nificantly in recent years as a result of new cars
Shipping is responsible for a significant frac- being equipped with sealed fuel injection systems
tion of NOx and primary PM emissions in some and activated carbon canisters in fuel tank
countries. Many ships have old engines or old vents [5].
technology, and compared with road transport
few exhaust aftertreatment devices are in use. Abrasion
The quality of the fuel is also poor relative to As noted earlier, particles are also generated as a
that used for road vehicles. In particular, the resid- result of various unregulated abrasion processes,
ual fuel oil used in ship engines contains very high including tire wear, brake wear, and road surface
levels of sulfur (up to 4.5% by mass), which leads wear. These sources are becoming increasingly
to high PM emissions [34]. To put this in perspec- important (Fig. 4), but the understanding of emis-
tive, the PM emission factor for ship engines is sions of abrasion particles is relatively poor and
typically around 1.25 g/kWh [35], compared with their health effects are not well documented.
the legislative limit value of 0.02 g/kWh for a There is little information on the composition
modern Euro V truck. There is little information of tire wear particles. Components that have been
on the size distribution of PM emissions from suggested as environmental tracers of tire wear
ships, although some recent data indicate that a include styrene butadiene rubber [38],
large fraction of the emitted particles can be clas- benzothiazole [39], and organic zinc [40]. Studies
sified as PM2.5 [34]. NOx and sulfur dioxide (SO2) conducted in the 1970s revealed that wear parti-
emissions from shipping also contribute signifi- cles had a bimodal distribution, with mass in the
cantly to secondary particle formation. both the fine (<2.5 mm) and coarse (2.5–10 mm)
modes [38, 41–43]. Several laboratory and field
Evaporation investigations have demonstrated that most parti-
Volatile organic compounds (VOCs) are emitted cles are present in the coarse fraction [38, 44, 45],
from the fuel systems of petrol vehicles as a result or are larger still [46], whereas others have indi-
of evaporation. The compounds that are emitted cated substantial mass in both the PM2.5 and PM1
56 Air Quality, Surface Transportation Impacts on

Effect of vehicle type and fuel (all vehicles Euro 3/III)


10
NOx emission factor (g/km)

0
Car Car LDV LDV HGV Bus Coach Moped M/C
a Petrol Diesel Petrol Diesel Diesel Diesel Diesel Petrol Petrol

Effect of technology (rigid HGV >32 t)


14
NOx emission factor (g/km)

12
10
8
6
4
2
0
b Pre-Euro I Euro I Euro II Euro III Euro IV Euro V Euro VI

Effect of average speed (Euro 4 diesel car)


1.2 0.06
NOx emission factor (g/km)

NOx (g/km)

HC/PM emission factor


1.0 0.05
HC (g/km)
0.8 PM (g/km) 0.04

(g/km)
0.6 0.03
0.4 0.02
0.2 0.01
0.0 0.00
0 20 40 60 80 100 120 140
c Average speed (km/h)

Air Quality, Surface Transportation Impacts on, Fig. 7 Factors influencing emissions: (a) vehicle and fuel type, (b)
technology, and (c) average speed. (Adapted from [33])

fractions [40, 47, 48]. In one early study, it was depends on the severity of the braking and the
observed that mean particle diameter decreases design of the vehicle [49]. The remaining debris
with increasing speed, and this may be one factor either falls on the road or is retained on the vehicle.
contributing to the differences in the reported It appears that most airborne brake wear particles
findings [42]. can be classified as PM10, although a substantial
Airborne brake particles are composed of proportion has a diameter of less than 2.5 mm [49–
metals (iron, copper, lead, etc.), organic material, 52]. The highest proportions of PM2.5 have been
and silicon compounds, which are used as binders found under urban driving conditions [52].
in brake pads, but composition varies greatly Very little information is available on the size
[37]. Test track and wind tunnel measurements distribution of road surface wear particles. The
have revealed that typically 50% of the brake data that are available suggest that airborne bitu-
wear debris escapes the vehicle and enters the men particles range in size between 0.35 mm and
atmosphere, although the actual proportion 2.8 mm [40].
Air Quality, Surface Transportation Impacts on 57

Particle measurements conducted near a busy transport modes. Most emission models are
electrified railway line in Zurich showed that the empirical in nature, being based on data from
main elements abraded by railway traffic were laboratory or real-world tests. However, it is
iron and manganese originating from the wheel– worth noting that such tests are not always
track interface, as well as copper from the over- designed to deliver emission factors for model-
head catenary system [53]. More than half of the ling, and simulate only a small fraction of all
iron and manganese particles resulting from wheel possible operational conditions [5].
and track abrasion were in the coarse range. The
abrasion particles provided a small but
Road Transport Models
measureable contribution to local PM10 concen-
Combustion In the simplest terms, the total
trations [54]. However, the contribution of rail
emission of a given pollutant during a given time
transport on lines with a larger diesel share of
period is calculated as the sum product of specific
the traction could be much higher.
emission factors and quantities of activity:
Resuspension X
v¼n
Another source of PM – the resuspension of mate- Ep ¼ ep,v  T v ð1Þ
rial previously deposited on the road surface – v¼1
occurs as a result of tire shear, vehicle-generated
turbulence, and the action of the wind. Studies in where
the United States have indicated that resuspension
is responsible for between 30% and 70% of total Ep ¼ total emission (e.g., in grams) of pollutant
PM10 in urban areas [55–57]. Large contributions p during the period
of resuspension have also been observed in Ger- v ¼ vehicle category (with n different categories)
many [44, 58, 59] and the UK [60], albeit with a ep,v ¼ emission factor (e.g., in grams per kilometer
large variation between locations. or liter of fuel burnt) of pollutant p from vehicle
Resuspension is a major concern in Scandina- category v
vian countries, especially in relation to the use of Tv ¼ activity (e.g., in kilometers or liters of fuel)
studded tires and “road sanding.” Indeed, it can of vehicle category v
provide a much larger contribution to PM10 than
exhaust emissions, and also form a significant The definition of emission factors that repre-
fraction of PM2.5 [61, 62]. An investigation in sent different aspects of vehicles and their opera-
Sweden revealed that PM10 resuspension is highly tion forms a substantial area of research. Emission
dependent on vehicle speed [63]. models are generally classified in terms of how
they take vehicle operation into account. Here, the
term “vehicle operation” is used in a general
Modelling Transport Emissions sense, and refers to a wide range of parameters
which describe the way in which a driver controls
Estimates of emissions from transport are required a vehicle (e.g., average speed, maximum speed,
for various purposes. National inventories cover- acceleration pattern, gear-change pattern), as well
ing all sectors are part of the reporting obligations as the way in which the vehicle responds (e.g.,
of CLRTAP, the United Nations Framework Con- engine speed, engine load). The main types of
vention on Climate Change and, in the European approach are aggregated emission factors,
Union, Directive 2001/81/EC on National Emis- average-speed models, traffic situation models,
sion Ceilings. At a more local level, emission multiple-regression models, modal models, and
estimates are required for assessing the impacts instantaneous models.
of policies and measures, and for input into air Aggregated emission factors operate on the
quality modelling studies. Separate modelling simplest level, with a single emission factor
approaches have been developed for the different representing a general type of driving; the
58 Air Quality, Surface Transportation Impacts on

traditional distinction is between urban roads, vehicles in the laboratory. The results from the
rural roads, and motorways. Vehicle operation is laboratory tests on vehicles in the same category
therefore only taken into account at a very rudi- (e.g., small petrol cars complying with the Euro
mentary level. However, they are generally the 4 legislation) are then plotted as a function of
only way of estimating emissions of unregulated average speed, and a regression curve is fitted to
pollutants, for which there is often insufficient the date to give an emission function. Given that
information to define a more detailed relationship exhaust emissions are inherently variable, there is
with vehicle operation. usually a considerable amount of scatter in the
Average-speed models are based upon the prin- emission data.
ciple that the emission factor varies according to Average-speed models are widely used in
the average speed during a trip. The general pro- emission inventories and local air pollution
cess of model development is shown in Fig. 8. models. In Europe, the most widely used example
Firstly, vehicle operation in the real world is mea- is COPERT [33]. A number of factors have con-
sured using on-board instruments, with the vehi- tributed to their popularity. The modelling
cles being driven under a wide range of road and approach is one of the oldest, it is comparatively
traffic conditions. The numerous resulting driving easy to use, several models are available free of
patterns are then condensed, using statistical charge, and there is a reasonably close correspon-
methods, into a much smaller number of represen- dence between the required inputs and the data
tative driving cycles which can be used to test available to users. However, trips having very

Real-world driving patterns Laboratory measurements

Record of vehicle
operation via
OBD, GPS, etc.

Driving cycles Emission function


Speed (km/h) ARTEMIS Urban, part 2
NOx (g/km)
80 0.6
60
Laboratory measurements Emission function
40 0.5
20
0 0.4
0 20 40 60 80 100 120 140 160 180 200
Time (s)
0.3
Speed (km/h) ARTEMIS Rural, part 4
120 0.2

80
0.1
40
0
0 0 40 80 120 160
0 20 40 60 80 100 120 140 160 180
Time (s) Speed (km/h)

Air Quality, Surface Transportation Impacts on, Smith, Tim Barlow of TRL in the UK, and TNO Automo-
Fig. 8 Process of development for average-speed models. tive in the Netherlands)
(Photographs reproduced by kind permission of Alistair
Air Quality, Surface Transportation Impacts on 59

different vehicle operation (and different emission parameters for the various driving cycles, giving
levels) can have the same average speed. Clearly, the descriptive variables which are the best pre-
all the types of operation associated with a given dictors of emissions (the group of descriptors
average speed are not accounted for by the use of a being different for each type of vehicle and
single emission factor. This is a particular problem each pollutant). The model requires a driving
at low-medium average speeds, for which the pattern (speed-time profile) as the input, from
range of possible operational conditions associ- which it calculates the same range of descriptive
ated with a given average speed is great. In addi- variables and estimates emissions based on the
tion, for modern vehicles a large proportion of the regression results.
total emission during a trip can be emitted as very In modal models emission factors are allo-
short, sharp peaks, often occurring during gear cated to the specific modes of vehicle operation
changes and periods of high acceleration, and encountered during a trip. In the simplest type,
this detail is lost when only average speed is vehicle operation is defined in terms of a rela-
considered. The concept of “driving dynamics” tively small number of modes – typically idle,
has therefore been developed to enable model acceleration, deceleration, and cruise. For each
developers to describe vehicle operation using of the modes the emission rate is fixed, and the
additional parameters [64]. In qualitative terms, total emission during a trip, or on a section of
dynamics can, perhaps, be thought of as the road, is calculated by weighting each modal
“aggressiveness” of driving. Quantitatively, the emission rate by the time spent in the mode
term refers to the variation in various properties [68, 69]. This approach has usually been used
or statistical descriptors of a driving pattern. One to determine the impacts of traffic control mea-
of the more useful parameters appears to be rela- sures and signal improvements [70].
tive positive acceleration (RPA) [65]. However, Some more detailed modal models aim to give
most model users have no straightforward means a precise description of vehicle emission behavior
of quantifying such parameters. during a series of short time steps (often 1 s).
In “traffic situation” models, emission factors These are commonly referred to as “instanta-
are referenced to specific traffic situations that are neous” models, although several alternative
known by the model user. A typical example is the terms can be found in the literature, including
Handbook of Emission Factors [66]. The traffic “microscale,” “continuous,” and “online”
situations are characterized by the features of the [71]. In the simplest type of instantaneous
sections of road concerned (e.g., “motorway with model, emission rates are defined for different
120 km/h limit,” “main road outside built-up combinations of speed and acceleration, usually
area”). The driving dynamics are not quantified in the form of a matrix [72, 73]. Theoretically, the
by the user, but are defined through a textual finer the resolution of the emission factor matrix
description (e.g., “free flow,” “stop and go”). the higher the model accuracy, but as the resolu-
However, requiring the user to define the traffic tion improves the complexity of the calculations
situation using a textual description of dynamics increases. Some models use the product of speed
may lead to inconsistencies in interpretation. and acceleration instead of the acceleration alone
Multiple-regression models are another com- [74]. A more flexible approach relies upon emis-
paratively recent development, and the most sion maps that relate to engine power [75,
prominent example is the Dutch VERSIT+ 76]. This allows all relevant factors to be taken
model [67]. The model contains test data for a into account, including rolling resistance, aerody-
large number of cars over a range of different namic resistance, acceleration, gradient, transmis-
driving cycles. Within the model, each driving sion losses, and the use of auxiliaries.
cycle is characterized by various descriptive Instantaneous models should have a number of
parameters (e.g., average speed, RPA, number advantages. Firstly, emissions can be calculated
of stops per km, etc.). A regression model is fitted for any operational profile, and thus new emission
to the average emission factors and cycle factors can be generated without the need for
60 Air Quality, Surface Transportation Impacts on

further vehicle testing. Secondly, the models associated with obtaining data on the temporal
inherently take into account dynamics. Thirdly, and spatial allocation of cold-start operation.
emissions can be resolved spatially, and this
ought to lead to improvements in the prediction Evaporation The earliest studies of evaporative
of air pollution. However, detailed and precise emissions were carried out in the United States in
data on vehicle operation and location are the 1960s [82], but the first European studies were
required, or any potential benefits may be lost. only conducted 20 years later [36]. The models
Such data are difficult to obtain for many model that were developed from the resulting data were
users. Moreover, it is extremely difficult to mea- not updated for many years. However, modelling
sure emissions on a continuous basis with a high improvements have recently been possible fol-
degree of precision, and then it is not straightfor- lowing a number of new investigations [83–85].
ward to allocate those emission values to the cor-
rect operating conditions. During measurement in Abrasion and Resuspension One non-exhaust
the laboratory, an emission signal is dynamically PM model in common use is that presented in
delayed and smoothed, and this makes it difficult the European Environment Agency’s Air Pollut-
to align the emissions signal with the vehicle ant Emissions Inventory Guidebook [33]. The
operating conditions [77]. Such distortions have method uses reference emission factors (in g/km)
not been fully taken into account in instantaneous and incorporates corrections for both speed and,
models until relatively recently. in the case of HDVs, vehicle load and number of
Once the basic modeling approach has been axles. However, the use of average brake wear
identified a number of other effects may need to emission factors (in g/km) means that differences
be considered, depending on the type of model in the extent of braking for different traffic situa-
being used. These effects include potential future tions cannot be taken into account. Such emission
improvements to fuels and technologies, the dete- factors are likely to overestimate brake emissions
rioration of vehicle exhaust emissions with age, in areas of low brake use, and underestimate
the presence and use of auxiliary devices (e.g., air emissions in areas of high brake use.
conditioning, windscreen wipers, radios), road The calculation method presented in the US
gradient, and vehicle load/occupancy. Such Environmental Protection Agency’s AP-42
effects may be taken into account via separate document [86] is one of the more widely used
models [78] or through adjustments to the basic for predicting resuspension on paved roads,
emission factors, with assumptions concerning although some shortcomings have been identi-
levels of uptake and effectiveness in future years. fied [87]. There is no widely accepted Euro-
Separate models also exist for the estimation of pean method for calculating emissions due to
cold-start emissions. In some cases, the hot emis- resuspension.
sion factor is multiplied by a ratio of cold-start to
hot emissions for the fraction of kilometers driven Rail Transport Models
with a cold engine [33]. In others, a reference Emissions from electric trains occur at the power
cold-start excess emission value is adjusted to stations which are responsible for generating the
take account of, for example, the ambient temper- electricity. The actual emissions will therefore be
ature, the average speed, the parking duration, and a simple function of power consumption and
the distance travelled (some trips are shorter than emission factors for power generation. However,
the distance needed to fully warm the engine) [79, power losses between the power station and the
80]. Specific models have also been developed to train, and within the train itself, also need to be
determine the effects of different parking scenar- taken into account where possible.
ios [81]. Cold-start emissions are usually included Emissions from diesel locomotives are typi-
in regional and national emission inventories, but cally estimated using fuel consumption data and
are often excluded from local air pollution studies. fuel-specific emission factors. The types of train
One of the main reasons for this is the difficulty which are typically included in models include
Air Quality, Surface Transportation Impacts on 61

highspeed passenger trains, intercity passenger modelled by analogy to marine shipping. How-
trains, regional passenger trains, urban passenger ever, the operational characteristics of inland
trains, and goods trains. Early models were based ships are rather different from those of their sea-
on empirical correlations between emissions, train going counterparts. Firstly, they sail at lower
type, operating speed, and other simple variables speeds and in restricted waterways. The lower
such as the distance between stops, and average speeds reduce energy consumption and emis-
emission factors for train types [88, 89]. More sions, whereas shallower depths increase sailing
recent models allow the user to specify an opera- resistance and hence fuel consumption and emis-
tional matrix for a journey, from which energy sions. In order to make the most of the limited
consumption and emissions can be calculated space on inland waterways, vessels tend to be
[90, 91]. This approach is a broadly analogous to squarer in shape than seagoing ships. This also
that used in modal models for road transport. As causes the sailing resistance to differ from that of
with road vehicles, passenger trains consume seagoing ships [94]. Recent models are therefore
energy for loads other than propulsion. These more specific to inland vessels and their operating
include the heating and cooling loads, and electri- conditions. For example, in the ARTEMIS pro-
cal power to operate lights, instruments, and other ject, a model was developed and validated for nine
electrical accessories. However, the energy con- types of vessel based on size and type of waterway
sumption for auxiliary power is fairly low com- [94]. The model calculates the energy consump-
pared with that required for propulsion. The tion and emissions under different service condi-
effects of regenerative braking on energy con- tions (speed, waterway dimensions, load, etc.).
sumption may also be important.
Activity Data
Shipping Models For all transport modes the accurate characteriza-
For shipping, both simple and detailed methods tion of traffic activity (such as numbers vehicles,
have been developed for calculating emissions trip distances, and modes of operation) and the
[33, 92, 93]. The simple methods are essentially fleet composition is vital to the estimation of
similar to that for road transport (see Eq. 1), and emissions. Although models and emission factors
combine fuel use (in tonnes) with fuel-specific are continually improving, poor activity data
emission factors. Detailed calculation approaches remains one of the main sources of uncertainty
firstly involve obtaining ship movement data, in the calculation of emissions [95]. For many
including sailing routes and distances between years, the direct measurement of road traffic has
ports. Different ship operating modes may also been the primary source of activity data. The
be considered, such as cruising, in-port operation collection of accurate information on important
(hotelling, loading and unloading), and maneu- parameters such as traffic speed, road gradient,
vering. Each vessel also needs to be characterized. or vehicle load can often be difficult and time-
National and international shipping covers a wide consuming, rendering it impractical for large geo-
range of vessels, from recreational craft to large graphic areas. However, the quality and availabil-
oceangoing cargo ships that are driven primarily ity of activity data has increased substantially in
by large, low-, and medium-speed diesel engines. recent years as a result of improved data collection
In addition, marine engines can be further classi- technologies (e.g., tag-and-beacon systems, cam-
fied according to their principal fuel: bunker fuel eras, in-vehicle data collection, and satellite tech-
oil, marine diesel oil, or marine gas oil. Again, nology) and online dissemination. Furthermore,
auxiliary engines are used to provide power and there have been significant advances in micro-
services when berthed [33]. In Europe, a widely simulation traffic models, the outputs from
used set of emission factors was determined in a which are well suited to integration with instanta-
study for the European Commission [92]. neous emission data. Some workers have linked
The fuel consumption and emissions of vessels microscale traffic and emission models for practi-
operating on inland waterways were initially cal applications [96].
62 Air Quality, Surface Transportation Impacts on

In the case of passenger rail transport the activ- a need for data that give a better description of the
ity data are available from timetables. Rail freight fleet, the traffic, and the waterways.
movements are more complicated, and data are
generally more difficult to obtain. There are essen-
tially three types of freight movement: long-term Pollutant Dispersion and
scheduled, short-term scheduled, and “on Transformation
demand.” Clearly, it would be difficult to incor-
porate on-demand movements in any emission Once pollutants have been released into the atmo-
calculations. Encouragingly, an increasing num- sphere, they are subject to various processes of
ber of operators are adopting “black box” technol- dispersion and physical or chemical transforma-
ogies, which can provide useful journey and fleet tion. Emissions from transport are also super-
information. For example, in Germany, the rail imposed on emissions from other sources.
company Deutsche Bahn has installed equipment Figure 9 shows a simplified representation of pol-
to monitor the real-time location and energy con- lutant concentrations in and around an urban area
sumption of its locomotives [97]. However, at the with tall commercial buildings in the urban center
moment, it appears that access to the data from and low residential buildings in the surrounding
train event recorders is rather limited. districts. The regional background pollution orig-
The primary source of information on ship inates from a range of sources, extends over a
movements is the database provided by Lloyd’s wide area, and is relatively invariant outside the
Maritime Information Service. The database urban area. Within the built-up area there is an
includes ship size, destination, approximate time additional “urban background” component. This
of arrival and departure, engine type and number, results from combined emission sources located
but only for ships greater than 500 gross tons. within the urban area, including transport, power
Ferries, fishing vessels, and operations at smaller plant, industry, and domestic heating. Alongside
ports are not included. Port calling statistics are heavily trafficked roads there is also likely to be a
also available from national sources. In the future, significant local contribution to the concentration.
the availability and accuracy of activity data and
emissions data should improve further due to Dispersion
onboard GPS technology, continuous emission The dispersion of pollutants is influenced to a
monitoring systems (CEMS) and the development large extent by the local weather conditions (see
of a universal Automatic Identification System Chapter, ▶ “Urban Air Quality: Meteorological
(AIS) [98]. For inland shipping there is currently Processes”). In particular, the temperature

Air Quality, Surface


Transportation
Pollutant concentration

Impacts on, Local traffic sources


Fig. 9 Simplified
representation of urban
structure and pollution Urban background
levels. (Adapted from [18])

Regional background

Urban structure (km)


Air Quality, Surface Transportation Impacts on 63

inversions and low wind speeds associated with several of which are emitted by transport. For
stable high-pressure systems can restrict disper- example, particles can be produced by the oxida-
sion and lead to high pollutant concentrations. tion of precursor gases such as SO2 and NOx to
Dispersion is also influenced by the local topog- acids followed by neutralization with ammonia
raphy, and is reduced by the presence of local (NH3), or by the partial oxidation of organic
obstacles such as buildings. The effect is most compounds. The formation of secondary parti-
pronounced in the case of so-called street can- cles is relatively slow. Their persistence in the
yons. Moreover, vehicle-induced turbulence atmosphere is therefore prolonged, and they are
needs to be taken into account. distributed more evenly throughout the air than
primary particles. They can also travel large dis-
Transformation tances, resulting in the transport across national
Some of the transformation processes that influ- boundaries.
ence the concentrations of PM, NO2 and ozone are
summarized below. Meteorological factors, Nitrogen Dioxide The ambient concentration of
including solar radiation, precipitation, and NO2 is dictated by various complex processes and
humidity, also play important roles in these factors. Under the majority of atmospheric condi-
processes. tions the following reaction is the dominant path-
way by which NO is converted to NO2:
Particulate Matter The emission of primary
particles from combustion sources was described NO þ O3 ! NO2 þ O2 ð2Þ
earlier. Nucleation mode particles have a rela-
tively short existence in the atmosphere since At polluted locations comparatively close to
they readily transform into larger particles and sources of NOx (such as road vehicles), NO is in
deposit quite efficiently to surfaces because of large excess and the reaction proceeds quickly
their highly diffusive nature. Accumulation (seconds), with the availability of O3 limiting the
mode particles are too large to be subject to quantity of NO2 that can be produced. Primary
rapid diffusion and too small to settle from the NO2 emissions are therefore important at such
air rapidly under gravity. Their further growth is locations. At unpolluted locations, when O3 is
inhibited because they do not coagulate quickly present in excess, the timescale for conversion of
and there are diffusion barriers to their growth by NO to NO2 is longer (minutes). When neither NO
condensation. Particles in the accumulation nor O3 is in large excess, the reaction progres-
mode can therefore have a long atmospheric life- sively depletes both reagents, and can become
time (typically 7–30 days), although incorpora- very slow [20].
tion into rain can shorten it significantly. Within Under normal ambient daytime conditions, the
the coarse particle size range, gravitational set- reverse process also occurs – the destruction of
tling velocities become appreciable and therefore NO2 by photolysis to form NO and ozone, as
atmospheric lifetimes are much shorter than for shown in reactions (3) and (4):
accumulation mode particles. Particles larger
than ~100 mm in diameter rapidly settle out of NO2 þ sunlight ! NO þ O ð3Þ
the air and are of minor health significance
because, although they can be inhaled, they do O þ O2 ðþMÞ ! O3 ðþMÞ ð4Þ
not generally penetrate beyond the nose and
mouth [99]. where M is a third body, most commonly
A substantial fraction of the fine PM mass, nitrogen.
especially at background locations, is secondary The mean daylight lifetime of NO2 with
in nature [99–101]. Secondary particles are respect to photolysis is around 3 min. In winter,
formed by atmospheric reactions involving both it is typically a factor of 2 or 3 longer. Under
inorganic and organic gaseous precursors, conditions when photolysis is sufficiently rapid,
64 Air Quality, Surface Transportation Impacts on

NO, NO2, and O3 are potentially in chemical vehicles which involve in situ generation
equilibrium, a condition usually referred to as of NO2, such as catalytically regenerative
the “photostationary state.” DPFs [106].
Other chemical processes that can convert NO The changes in f-NO2 for traffic emis-
to NO2 involve the formation of free radicals, sions have not had a large impact on NO2
which can catalyze the oxidation of emitted concentrations away from the roadside,
hydrocarbons [20], but these reactions tend to be where the dominant contribution is from
comparatively slow [102]. secondary NO2.
A third-order reaction, involving the oxidation 2. The possibility that real-world NOx emissions
of NO by oxygen, is of minor importance under from road vehicles are not decreasing as rap-
normal atmospheric conditions: idly as models are predicting [110].
3. Increasing background ozone concentrations
2NO þ O2 ! 2NO2 ð5Þ [111]. As the O3 concentration increases, the
amount of NO converted to NO2 increases.
However, this reaction is rapid at low temper-
atures and high NO concentrations, such that it is Ozone Ground-level O3 is implicated in summer
much more rapid at the elevated levels typical of smog, such as the one that affected large areas of
those close to points of emission. Under winter- Europe in the summer of 2003, and high concen-
time pollution episode conditions, when a shallow trations lead to increases in the frequency of respi-
inversion layer can lead to a combination of high ratory symptoms and in deaths [112]. It is not
NOx levels and stagnant air for periods of a day or produced directly from emission sources but is
more, reaction (5) can potentially make a substan- created by photochemical reactions such as those
tial contribution to NO2 concentrations, as during described above. It can be transported over long
an episode in London in December 1991 [20]. distances, and is therefore regarded as a regional air
Given that model predictions show a decrease pollution problem. High concentrations are typi-
in NOx emissions, the absence of a downward cally observed downwind of large cities in the
trend in NO2 concentrations (see earlier section summer when photochemical formation is
on “Historical Trends”) is not completely under- enhanced. Because road transport is a major source
stood. Three contributing factors have often been of ozone precursors (e.g., NOx and hydrocarbons),
cited: it is an important contributor to ground-level con-
centrations. Globally, road transport is responsible
1. The likelihood that the average proportion of for 5–15% of tropospheric O3 [113, 114].
NO2 in NOx (termed f-NO2) in diesel exhaust is
increasing. Analyses of NO2 concentrations in
urban areas have indicated that a significant Modelling Air Pollution from Transport
proportion of NO2 must be emitted directly
from the exhaust, and that the f-NO2 value Predictions from air quality models are used in a
has increased in recent years [104–108]. This diverse range of applications. A common one is
has two causes: air quality management (AQM), which includes
• The increasing market share for diesel vehi- the identification of high-pollution areas (“hot
cles in many European countries. For exam- spots”), the development of plans and programs
ple, the share of first registrations of diesel for improving air quality, the checking of progress
passenger cars in Finland increased from toward targets, and the provision of information to
17% in 2005 to 52% in 2008 [109]. Petrol the public. Applications that are closely linked to
cars emit less NOx than diesel vehicles, and AQM are transport planning and land-use plan-
with a smaller proportion of NO2. ning. Air quality predictions are also an important
• The increase in the use of specific aftert- element of environmental impact assessment
reatment technologies in modern diesel (EIA).
Air Quality, Surface Transportation Impacts on 65

Modelling methodologies can be categorized distributions in the horizontal and vertical direc-
according to two general types: empirical/statistical tions. Two other types of model – Eulerian and
models and deterministic models. Empirical models Lagrangian – take as their basis the principle of
are based largely on correlations between pollutant conservation of mass of a pollutant as it spreads in
concentrations and other variables, such as meteo- the air. In Eulerian models, the calculations are
rological parameters. Although empirical models undertaken simultaneously for all the grid points
can be used for short-term predictions, they are in the model domain, whereas in the Lagrangian
most reliable for longer term averages. The assump- approach the calculations relate to a parcel of air
tions that correlations represent cause and effect, and which follows a defined trajectory. Several thou-
that regression parameters remain constant into the sand trajectories are usually required to generate
future, are their main weaknesses [20]. Deterministic statistically significant results. CFD models use
models predict concentrations downwind of an numerical methods to predict air flows. They
emission source using mathematical formulae focus on the detailed modelling of complex struc-
which describe the physical and chemical processes tures on the local scale (e.g., street canyons), and
operating within the atmosphere [20]. They include are not appropriate for calculating areawide
Gaussian plume models, Eulerian grid models, concentrations [20].
Lagrangian trajectory models, and computational The most commonly used street canyon model
fluid dynamics (CFD) models. For transport is the Operational Street Pollution Model (OSPM)
sources, emissions are typically entered as a line [115]. The OSPM approach involves an idealized
source (such as a road or railway line), or as an representation of a street as a long road enclosed
area/volume source (such as a car park). along its length on both sides by buildings of
Models vary enormously in sophistication. The equal height (Fig. 10). The wind passing across
simplest and most common deterministic models the street induces a recirculation vortex in the
are based on Gaussian dispersion theory. This street, and this leads to elevated pollutant concen-
assumes that a pollutant emission develops into a trations on the leeward side of the canyon.
plume under the influence of the wind, and that Some models include a preprocessor module
the concentrations in the plume have Gaussian for the input of meteorological data. Allowances

Roof-level wind
Background
pollution

Recirculating
Leeward air Windward
side side

Direct vehicle
exhaust

Air Quality, Surface Transportation Impacts on, Fig. 10 Schematic illustration of street canyon modelling in
OSPM. (Adapted from [115])
66 Air Quality, Surface Transportation Impacts on

97
94
91
88
85
83
79
76
73
70
67
64
61
58
55
52
49
46
43 Limit Value
40
37
34
31
28
25
22
19
16
13

Air Quality, Surface Transportation Impacts on, Fig. 11 Modelled annual mean NO2 concentrations (mg/m3) in
London in 2008 [116]. (Photograph reproduced by kind permission of Greater London Authority)

can also be made for concentration changes pro- important to consider ways in which this might
duced by chemical reactions in the air. Again, the be achieved. The emphasis here is on road trans-
chemical reaction schemes vary greatly in port, but some measures for rail transport and
sophistication. shipping are also mentioned. It has been noted
Dispersion model outputs are often expressed that if no aggressive emission-reduction strategies
as contour or surface maps in order to show the are introduced, global CO2 and SO2 emissions
spatial variation in pollutant concentrations over a from ships could double from present-day values
wide area. Such plots can enable spatial relation- by 2050, and NOx emissions could exceed the
ships between air pollution and other variables to current value for road transport [117]. Shipping
be established, and sensitive locations to be iden- has therefore been recognized as a growing prob-
tified. Appropriate pollution-reduction measures lem by policymakers and scientists.
can then be developed. The example provided in This entry considers two philosophies: “preven-
Fig. 11 shows NO2 concentrations in London. The tion” and “mitigation.” Of course, other distinctions
area with high NO2 concentrations to the west of are possible (e.g., “technical,” “systematic,” “behav-
London is Heathrow Airport. ioral,” etc.), but in any case these tend to be artificial;
interactions are often so strong that few strategies
are based on a single measure of policy. In the
Reducing Air Pollution from Transport context of the entry, prevention measures are
designed to reduce or eliminate emissions at source,
If transport systems are to become environmen- whereas mitigation measures are designed to
tally sustainable their impacts on air pollution will remove pollutants which have already been emitted,
have to be greatly reduced, and it is therefore or to convert them to more benign compounds.
Air Quality, Surface Transportation Impacts on 67

An important tool is air quality legislation (see Emission Legislation In Europe, emission tests
Chapter, ▶ “Air Quality Guidelines and Stan- are required at type approval for all new light-duty
dards”), but it does not fall conveniently into the vehicle models and for the engines used in heavy-
prevention or mitigation categories. Although air duty vehicles. Light-duty vehicles are tested using
quality legislation acts as a driver for the develop- a power-absorbing chassis dynamometer, as
ment of pollution-reduction policies and technol- shown in Fig. 8, whereas heavy-duty engines are
ogies, and can thus be considered as “prevention,” operated on a test bench. The sampling of exhaust
compliance with the legislation can only be deter- emissions is then performed as the vehicle or
mined from historical data, usually for the calen- engine progresses through a predefined driving
dar year, such as the annual mean or the number of cycle.
days on which pollutant concentrations were Limit values are usually defined for CO, HC,
above a certain value. Neither does the legislation NOx, and PM in exhaust, as well as evaporative
specifically target transport. emissions of VOCs. In the regulation of exhaust
Compliance with air quality standards for particles, practically all worldwide emission stan-
PM10 requires control of both fine and coarse dards are expressed in terms of the mass of total
particles. As the two modes tend to have different particulate matter with no differentiation by parti-
sources and formation mechanisms, different cle size. Particle number emissions are included in
types of control are required. The compounds the latest European legislation.
that are precursors to secondary particles also The most advanced regulations are to be
need to be controlled. Primary fine particles from found in the EU, the United States, and Japan.
combustion sources are subject to regulation. The The specific differences between the legislation
control of coarse particles is less straightforward in different countries are too numerous to men-
[118], as such particles arise from diverse natural tion here, but the principles involved are broadly
and anthropogenic disruption and attrition pro- similar and there is a general move toward har-
cesses which are difficult to characterize (e.g., monization. Moreover, the technology being
non-exhaust emissions, resuspension, dust from built into cars and trucks to comply with the
industrial processes, quarrying). European, US, and Japanese standards is very
As a result of reaction (2), O3 levels near to similar.
roads tend to be low. Thus, the limitation of local Over the course of several decades the limit
traffic emissions would tend to lead to increased values for the pollutants in vehicle exhaust have
O3 concentrations at roadside locations. The con- decreased (Fig. 12), and changes have been made
trol of O3 depends ultimately on the control of to the test method to make it more realistic. As a
emissions of NOx and HC on a larger scale. result, manufacturers have been required to
develop increasingly effective emission-control
technologies (some effects of this were shown in
Prevention Measures Fig. 4b). For example, the latest EU emission
Some examples of prevention (i.e., emission- standards for cars and heavy-duty vehicles require
reduction) measures are listed in Table 1. The large reductions in PM and NOx emissions, and
list is not comprehensive, but provides an indica- these will be achieved through the use of DPFs
tion of the types of action which are currently and SCR.
being considered. Two general approaches are Some examples of the progressive reduction in
noted here: reducing emissions per vehicle and the exhaust emission limits in several countries
reducing travel/transport activity, and several spe- (in terms of equivalence to the EU legislation)
cific measures are available in each case. The are illustrated in Fig. 13. Most developing
applicability of each measure to road transport, countries lag behind the EU, although the gap is
rail transport, and shipping is also shown. Several narrowing and in some places it has been possible
prevention measures are described in more detail to “leapfrog” standards. However, a prerequisite
in the following paragraphs. for the introduction of advanced engine and
68 Air Quality, Surface Transportation Impacts on

Air Quality, Surface Transportation Impacts on, Table 1 Prevention measures for surface transport
Applicability
General approach Type of measure Measure Road Rail Shipping
Reducing emissions per vehicle, vessel Emission Vehicle/engine type ✓ ✓ ✓
or train legislation approval
In-service inspection ✓ – –
Roadside checks ✓ – –
Fuel legislation Improved fuel quality ✓ ✓ ✓
Exhaust DPF ✓ ✓ ✓
aftertreatment
SCR ✓ ✓ ✓
Scrubber – – ✓
Alternative fuels CNG/LPG ✓ ✓ ✓
Biofuels (biodiesel, ✓ ✓ ✓
ethanol)
Vehicle/engine Improved combustion ✓ ✓ ✓
technology Improved aerodynamics ✓ ✓ ✓
Hybrid ✓ ✓ ✓
Fuel cell ✓ ✓ ✓
Humid air motors – – ✓
Eco-driving Training ✓ ✓ ✓
Engine switch-off ✓ ✓ ✓
Cleaning Road sweeping ✓ – –
Road washing ✓ – –
Vehicle cleaning ✓ – –
Dust suppressants Chloride salts, CMA ✓ – –
Traffic Speed control ✓ – –
management
Reducing travel/ transport activity Traffic Access restrictions ✓ – –
management
Environmental zones ✓ – –
Parking restrictions ✓ – –
Economic Congestion charges ✓ – –
measures
Tolls ✓ – –
Road user charging ✓ – –
Incentives and taxes ✓ ✓ ✓

aftertreatment technologies is the availability of operations of the vehicle (usually in a repair cen-
appropriate fuel, and in many developing coun- ter), and make use of equipment that is less precise
tries this has presented something of a barrier. and less expensive than that used in the laboratory.
Periodic in-service inspection and mainte- Moreover, the tests for petrol vehicles typically
nance represents a further (and crucial) level of only involve the measurement of CO and HC
legislative control, as it is designed to ensure that whilst the vehicle’s engine is running at idle or at
vehicles maintain low emission levels during real- fast-idle, and those for diesel vehicles tend to
world operation. However, whilst type approval cover only smoke emissions. Therefore, the tests
checks are relatively detailed and involve the use do not address the most important pollutants and
of specialist and expensive laboratory equipment, operational conditions. In some countries,
in-service checks are based on shorter, simplified attempts have been made to address these issues.
Air Quality, Surface Transportation Impacts on 69

Euro I
10.0 (1992)

9.0 Euro II
(1996)
8.0

7.0
Euro III
NOx (g/kWh)

6.0
(2000)
5.0

4.0

3.0

2.0
Euro IV (2013)
1.0 Euro VI (2013)
Euro VI (2013)
0.0
0 0.1 0.2 0.3 0.4
PM (g/kWh)

Air Quality, Surface Transportation Impacts on, Fig. 12 Evolution of EU NOx and PM emission limits for engines
used in heavy-duty vehicles
1992

1993

1994

1995

1996

1997

1998

1999

2000

2001

2002

2003

2004

2005

2006

2007

2008

2009

2010

2011

2012

2013

2014

2015

EU Euro 1 Euro 2 Euro 3 Euro 4 Euro 5 Euro 6


Thailand Euro 1 Euro 2 Euro 3 Euro 4
Singapore Euro 1 Euro 2
Hong Kong Euro 1 Euro 2 Euro 3 Euro 4 Euro 5
Australia Euro 1 Euro 2 Euro 3 Euro 4
Malaysia Euro 1 Euro 2 Euro 4
Vietnam Euro 1 Euro 2
Russia Euro 1 Euro 2 Euro 3 Euro 4 Euro 5
Argentina Euro 1 Euro 2 Euro 3 Euro 4
China (national) Euro 1 Euro 2 Euro 3 Euro 4 Euro 5
India (national) Euro 1 Euro 2 Euro 3
Indonesia Euro 1 Euro 2 Euro 4
Philippines Euro 1 Euro 2 Euro 4
Pakistan Euro 1

Air Quality, Surface Transportation Impacts on, Fig. 13 Introduction dates for emission standards in different
countries. (Adapted from [119])
70 Air Quality, Surface Transportation Impacts on

For example, in the United States, a loaded test and SO2 emissions and partly because fuel sulfur
(IM240) has been developed to simulate condi- has an adverse effect on certain types of engine and
tions under which high NOx emissions may occur. exhaust aftertreatment technology [122]. In Europe,
Some authorities may also conduct random road- the controls on fuel sulfur content have been peri-
side checks, or use remote sensing devices to odically tightened, and in the latest step Directive
screen for high emitters. In addition, onboard 2003/17/EC required a full transition to “sulfur-
diagnostics of emission-control systems are free” petrol and diesel (having less than 10 ppm of
increasingly used to alert drivers to failures. sulfur) by 2009. This should enable advanced tech-
In Europe emissions from ships and railway nologies – such as lean-burn engines, particle traps,
locomotives are governed by the legislation for and regenerative NOx storage systems – to meet
non-road mobile machinery (Stages III and IV of stringent exhaust emission limits.
Directive 2004/26/EC). The Stage III standards Because of the contribution of shipping to pol-
are further divided into two substages: Stage III lution at large ports, EU Directive 2005/33/EC
A and Stage III B. The Stage III B standards limits the fuel sulfur content to 0.1% in marine
introduce PM limit of 0.025 g/kWh, representing fuels for harbor regions in 2010.
a 90% emission reduction relative to Stage II. To
meet this limit value it is anticipated that engines Improved Combustion and Exhaust Aftert-
will have to be equipped with DPFs. Stage IV also reatment It is expected that petrol and diesel
introduces a stringent NOx limit of 0.4 g/kWh, will power road transport for the foreseeable
which is expected to require NOx after treatment. future, and considerable reductions in emissions
Given the long working lives of the engines in might still be realized in the short term through
question, these regulations will not have any con- improved engine design, fuel injection systems,
siderable effect on emission levels for another electronic timing, etc. Developments in ship
couple of decades [94]. Again, a process of world- engine technology include direct water injection
wide harmonization of regulations has begun. and humid air motors (in which water vapor is
Emission standards for diesel engines used in used to cool the charge air and reduce the NOx
railway locomotives have also been established formation during combustion) [96].
by the International Union of Railways (UIC), The main exhaust aftertreatment technologies
an association of European railway companies that enable vehicle and engine manufacturers to
[120]. The standards apply to all new engines comply with the exhaust emission legislation are
used in new vehicles or for repowering of existing three-way catalysts, oxidation catalysts, exhaust
locomotives, and are binding to UIC members. gas recirculation (EGR), DPFs, and SCR. Whilst
Emission standards for marine engines are such technologies are generally fitted during man-
defined by the International Maritime Organiza- ufacture, retrofitting is a common pollution-
tion (IMO). The standards – for NOx and SOx – reduction strategy. For example, DPFs have been
are contained in the International Convention on fitted to all of London’s 8,000 buses.
the Prevention of Pollution from Ships, known as In EGR the recirculation of the exhaust air into
MARPOL 73/78 [121]. In addition, the first sulfur the combustion chamber reduces the amount of
emission-control area (SECA, with a maximum oxygen available for NOx formation. It has been
fuel sulfur content of only 1.5% sulfur content) in fitted to light-duty diesel road vehicles in Europe
the Baltic Sea entered into force in 2006, and for some years. For trains, EGR can give signifi-
further SECAs in the North Sea and English cant reduction in emissions but can be relatively
Channel entered into force in 2007. expensive to retrofit. It may also not be possible to
fit EGR to many classes of train due to space
Fuel Legislation Engine and vehicle technologies restrictions [123]. EGR is also applicable to
normally achieve their best emissions performance ships but is not yet in regular use.
with high-quality fuels [122]. One property on DPFs physically capture particles in the
which a great deal of attention has focused is the exhaust stream. They can be broadly divided
sulfur content, partly due to the need to reduce PM into two types: “full flow” and “partial flow.”
Air Quality, Surface Transportation Impacts on 71

The former lead to a reduction in PM emissions of through water. This is effective at reducing emis-
more than 95%, whereas the latter are more per- sions of SO2 and probably has benefits for other
meable and less effective, but need no mainte- pollutants.
nance. In order to prevent the filter from
blocking the particles captured by the filter must Alternative Fuel and Vehicle and Techno-
be periodically removed (a process referred to as logies The development of technology in the
“regeneration”). The regeneration may be induced longer term will undoubtedly be driven more by
using, for example, a heater, fuel burner, or a the need to reduce CO2 emissions than by the need
reactant (such as NO2) generated in situ. DPF to improve air quality. In many cases, a “win-win”
technologies are also suitable for use on rail and outcome is possible, although there can be some
marine engines [124]. However, they can be very conflicts. For example, some studies have indi-
bulky and for rail locomotives there are questions cated that NOx emissions can increase as a result
concerning the feasibility of retrofitting. More- of biofuel use [125].
over, they appear to be a less cost-effective mea- Alternative fuels include liquefied petroleum
sure than re-engining [123]. gas (LPG), compressed natural gas (CNG), and
SCR will be the main technology for enabling various biofuels (biomethane, ethanol, esterified
compliance with future NOx emission standards. vegetable oils, etc.). For road transport, limited
The method works by injecting ammonia or urea supplies mean that LPG could never fully replace
into an exhaust stream to chemically reduce NOx petrol or diesel, and the scale of uptake of CNG
to nitrogen. Again, SCR systems are very bulky; has been impaired by the cost of converting car
the catalyst itself can be considerably larger than engines [126]. The availability of suitable engines
the engine. Space is also required for oxidation for rail applications is uncertain; available natural
catalysts and the tank for storing urea or ammonia. gas engines can also only cover the lower end of
This puts severe restrictions on its potential for the power range needed for railway applications,
use as a retrofit item to rail vehicles – where spare and there appears to be no use of LPG
space and weight availability is limited – and [123]. Around 50 seagoing ships are currently
again re-engining appears to be a more cost- powered by natural gas, with a reduction in emis-
effective option [123]. SCR is in use in a few sions of PM and NOx of at least 70%
ships and is still being developed. As well as [127]. Biofuels can be used in low concentration
being an effective NOx-reduction measure, one blends (5–10%) with petrol or diesel without
study has also shown that SCR can reduce ship engine modification, and in high concentrations
PM emissions by around 50% [35]. No limitations (85–100%) with specially adapted vehicles. The
are thought to have been encountered regarding main benefit of biofuels is their contribution to the
the fitting of SCR to different types of ship, and it reduction of CO2 emissions; its effects on NOx
can be integrated with other aftertreatment and PM are less clear. Barriers to increased biofuel
devices [96]. However, sufficiently high tempera- use include higher costs, compatibility with con-
tures in the exhaust are required for the SCR ventional fuels, and availability of technology for
process to function efficiently. Consequently, more advanced biofuels [15]. In addition, there
large NOx reductions are mainly achieved at have been warnings of hidden costs and adverse
higher engine loads. Other drawbacks include impacts on the environment and society, which
the space and additional weight requirements, could arise from the large-scale production of
and the potential for “ammonia slip.” This occurs biofuels [128]. It has also been noted that the use
when excess urea or ammonia is injected into the of alternative fuels is context-specific; a fuel that
exhaust stream, and any unused reagent is emitted is appropriate to one location may not be appro-
from the exhaust. The risk of ammonia slip is priate to another [23].
higher for transient load changes (i.e., Automobile propulsion technologies that are
maneuvering) [96]. currently under development include “mild” and
Another shipping technology is seawater “full” hybrid vehicles, “plug-in” hybrid vehicles,
scrubbing, in which the exhaust gas is passed battery electric vehicles, hydrogen ICE vehicles,
72 Air Quality, Surface Transportation Impacts on

and fuel cell vehicles. Vehicle technologies are emission is water vapor (though a small amount
currently available that can reduce CO2 emissions of NOx is produced by hydrogen ICEs). If the
per car by 30%, but demand-side and supply-side hydrogen is made from low-CO2 energy sources,
barriers are delaying their deployment [126]. Cars very low life-cycle emissions are possible. Some
that emit 50% less CO2 per kilometer than the of the main obstacles to the wider use of hydrogen
equivalent current models could be on the road for transport are the lack of an adequate infrastruc-
by 2030, subject to advances in hybrid and battery ture for storage/ distribution and the high cost of
technologies and industry overcoming cost bar- implementation [15].
riers [126]. In the longer term, a 90% reduction in
emissions is possible based on battery-electric Eco-Driving “Eco-driving” has been widely
propulsion systems [126]. publicized as a means of reducing the fuel con-
In the rail sector, hybrid systems have been sumption and emissions of road vehicles. It is
shown to result in reductions in exhaust NOx and aimed at both private motorists and fleet opera-
PM of up to 90% [123]. Hybrid propulsion has tors, and typically involves either a simple set of
been used in shipping for many years, where the rules to be followed or a program of training. The
mechanical drive for the propellers has been advice or training varies considerably in terms of
replaced by electrical connections to electric the level of detail, but it generally features a num-
motors, which in turn drive the propellers [129]. ber of common actions, including keeping the
Electricity results in zero emissions at the point tires at the correct pressure, reducing the vehicle
of use, giving it major local air quality benefits. weight, avoiding sharp acceleration and heavy
Moreover, if it is produced from renewable energy braking, driving in the highest gear, and avoiding
it can have low or even effectively zero CO2 unnecessary engine idling. Average overall reduc-
emissions over its life cycle. The main drawbacks tions in fuel consumption of around 5–10% are
with electric road vehicles include a relatively low typically reported for eco-driving, and some spe-
maximum speed, a short range, the lengthy cific examples are shown in Table 2. However, it
recharging times and the cost [126]. However, should be noted that some adverse effects of eco-
there are continual improvements in the perfor- driving have been observed, such as an increase in
mance and marketability of electric vehicles. NOx emissions from diesel cars during urban
In hydrogen vehicles the power is derived from driving [133].
either combustion or electrochemical conversion It is possible that the principles associated with
in a fuel cell. In hydrogen ICEs the combustion eco-driving on the road are transferable, with
process is fundamentally the same as that in petrol modification to the actual actions involved, to
ICEs. In a fuel cell the hydrogen reacts with oxy- rail transport and shipping.
gen to produce water and electricity, and the latter Leaving diesel engines in idle operation is a
is used to power the vehicle. When hydrogen is widespread practice at many rail termini. Reasons
used to generate power the only significant for this include keeping the engines warm and

Air Quality, Surface Transportation Impacts on, Table 2 Effects of eco-driving measures on fuel consumption
Action Change in fuel consumption References
Correction of low tire pressure –2% [130]
Removal of 100 kg load from a medium-size van 7% [130]
Removal of roof rack 20% [130]
Not driving with windows open 10% [131]
Not using air-conditioning 18% [131]
Eco-driving gear-change strategy 18% [132]
Use of a gear-change indicator 1% to 11% [133, 134]
Eco-driving training +2% to 16% [133, 135–137]
Air Quality, Surface Transportation Impacts on 73

providing power brakes, heating/cooling, lights, Road Sweeping and Washing Sweeping
catering facilities, and other auxiliaries. Whilst (or vacuuming) and washing have been applied in
pollutant emissions per train at stations are rela- several countries as means of decreasing the silt
tively low compared with those during a trip, loading of roads, the premise being that this will
where several trains are running at idle and the reduce PM resuspension. Purpose-built vehicles are
station is enclosed there may be an issue regarding usually employed, and the cleaning process can
population exposure. There may therefore be sig- involve mechanical (broom) sweeping, vacuuming,
nificant potential to reduce emissions at stations spraying with water, or a combination of these. Some
simply through enforcing maximum idle running vehicles are specifically designed to reduce PM10
times [123]. concentrations. A simpler approach is the spraying
When at berth, ships also need electrical power of water directly onto the road surface (Fig. 14) in an
for emergency equipment, refrigeration, cooling, attempt to reduce resuspension on dry days.
heating, lighting, loading/unloading equipment, Studies in the 1980s showed promising results
etc. This power is normally provided by the aux- in terms of the removal of particles from the road
iliary engines. However, such engines result in air surface [139, 140]. However, the majority of later
pollutant emissions at the port, and these are often studies have indicated only limited effects on
close to centers of population. An alternative PM10 concentrations [141–145], and in some
approach is to obtain power from shore, a process cases increases [146]. Where reductions in PM
known as “cold ironing.” The port of Gothenburg concentrations have been observed, these have
in Sweden was the first in the world to provide a generally been small and short-lived (a few
high-voltage onshore power supply for cargo ves- hours) [147, 148]. Possible explanations for such
sels. Two local wind turbines are used to generate limited effectiveness include the silt loading being
the electricity, and it is claimed that the system rapidly replaced after sweeping, the frequency of
cuts emissions by 94–97% for ships at berth and sweeping/ washing being too low, and the
has led to dramatic reductions in pollutant con- removal of only particles which are larger than
centrations. Systems are also available for opti- PM10 [145]. The spatial distribution of material on
mizing the energy efficiency of a vessel by roadways is also highly variable [149].
advising the crew on the optimal speed for the However, some investigations have indicated
prevailing water conditions [138]. effects that are large enough to warrant the

Air Quality, Surface


Transportation
Impacts on,
Fig. 14 Spraying the road
with water in Nijmegen, the
Netherlands. (Photograph
reproduced by kind
permission of the
Municipality of Nijmegen,
the Netherlands)
74 Air Quality, Surface Transportation Impacts on

consideration of sweeping or washing for reduc- restriction. Entry to a LEZ is usually conditional
ing roadside PM10 concentrations [150, 151], and on a vehicle meeting specified standards. These
if sweeping or washing can remove particles that standards can be set in various different ways,
could evolve into PM10, then sweeping may have such as emission legislation, the use of specific
a delayed beneficial effect on air quality [144]. It exhaust aftertreatment (e.g., DPF), or vehicle age.
should be technically undemanding, and rela- The potential beneficial effects of such mea-
tively low cost. Clearly, both sweeping and wash- sures can be illustrated by reference to a trial road
ing programs would have to be conducted during charging scheme introduced in Stockholm City
periods when traffic flows are low, so that any Centre in 2006. It was estimated that the scheme
disruption to the traffic is minimized. resulted in a 15% reduction in total road use
within the charging zone. Emissions of NOx and
Dust Suppressants Dust suppressants (or binders) PM10 from road traffic in the zone fell by 8.5%
appear to be an obvious choice for the reduction of and 13%, respectively. Air quality dispersion
resuspension due to road vehicles. Suppressants modelling was applied to assess the effects of the
are chemicals applied to surfaces to maintain the emission reductions on ambient concentrations. It
moisture levels or to actually chemically bind the was found that the annual average NOx concen-
surface material to reduce fugitive dust emissions. trations would decrease by up to 12% along the
The main suppressants in use are water (the oldest, most densely trafficked streets and PM10 concen-
and undoubtedly the cheapest) and solutions of trations would decrease by up to 7% [153].
salts such as calcium chloride (CaCl2), magne- Other types of traffic management are designed
sium chloride (MgCl2) and calcium magnesium to impose low-emission driving styles, including
acetate (CMA). Little quantitative information variable speed limits and synchronized traffic sig-
exists on their effects on airborne particulate mat- nals (so-called green waves).
ter, although with the need to control PM10 the
interest in suppressants is growing. There is rea-
Mitigation Measures
sonably convincing evidence from recent pilot
The possibilities for mitigation are less diverse
studies in Scandinavia that the use of dust sup-
than those for prevention. Mitigation measures
pressants could make a significant difference to
typically involve the use of physical barriers, veg-
roadside PM concentrations on timescales of
etation, or some form of air treatment.
hours to days [144, 145, 152]. However, more
information is needed on potential adverse effects
of using dust suppressants on paved roads. Physical Barriers On open roads the emissions
A notable concern is road safety, as road surface from traffic are subject to the normal processes of
friction is reduced when large amounts of sup- atmospheric dilution and dispersion. Barriers are
pressants are used. common features alongside roads with high levels
of traffic, particularly those which run through
Traffic Management Numerous forms of traffic populated areas. These features are usually intro-
management offer the possibility of reducing duced to attenuate noise, but can also block pol-
emissions from traffic. Local restrictions to the lutant dispersion, increase turbulence and initial
access and/or circulation of traffic have been mixing, or modify deposition. Any air flow per-
introduced in many cities to reduce pollutant con- pendicular to the barrier can be deflected upward
centrations. Such restrictions can take a range of by the structure, and this can increase the apparent
forms, including tolls, congestion charges, alter- release height of the pollutant and increase verti-
nate number plate schemes, and weight restric- cal mixing due to the flow separation at the top of
tions. Cities that have implemented these types the barrier. A recirculation cavity forms in the lee
of schemes include London, Stockholm, Athens, of the structure, and this can also reduce pollutant
Budapest, and Prague. Low emission zones concentrations relative to an open area with no
(LEZs) are one of the more effective types of barrier [155]. However, plume reattachment – and
Air Quality, Surface Transportation Impacts on 75

increased pollutant concentrations – can take reducing air pollution. These materials are often
place further downwind [155]. reliant upon photocatalysis, most commonly
Inside a road tunnel the dilution and dispersion involving the compound titanium dioxide
of pollution is restricted, and unless there is the (TiO2). Titanium dioxide acts as a catalyst to
injection of fresh air, the concentration of pollut- oxidize NO and NO2 into nitrate (NO3) in the
ants will increase from the entrance to the exit, and presence of oxygen and ultraviolet radiation. The
the emissions will be concentrated at the portals or nitrate is subsequently washed away by rainfall.
ventilation points. Therefore, the road traffic The effectiveness of TiO2 coatings has been suc-
source of pollution is effectively removed along cessfully demonstrated in laboratory trials [161],
the length of the tunnel and the exterior air quality but field trials have been less convincing. This is
ought to improve. However, pollutant concentra- partly because it is difficult to distinguish the
tions can be particularly high in the vicinity of the impact of chemical conversion on the catalyst
exit portals. The air quality at the portals or ven- surface from fluctuations in concentrations due
tilation points will depend upon the level of traffic to, for example, meteorology.
and whether or not the polluted air is treated in Several air treatment technologies have been
some way before release. When considering the developed for use in tunnels. For example, a num-
potential for tunnels for improving ambient con- ber of denitrification systems are available; most
centrations, it should be borne in mind that vehicle work by either a chemical absorption or catalytic
occupants and tunnel workers may be exposed to process. Tests in Norwegian and Japanese tunnels
increased concentrations, which could be detri- have indicated that removal rates for NO2 of up to
mental in public health terms. 90% are possible [162, 163]. The application of
denitrification systems at open roadside locations
Vegetation The planting of vegetation can have a does not appear to have been reported, and
positive impact on air quality in the vicinity of appears to be impractical at present. Electrostatic
roads [156–158]. A number of mechanisms are precipitators (ESPs) have been demonstrated as
involved, but the main effects are dry deposition at being effective in removing particles from tunnel
the leaf surface and the modification of dispersion. air with varying efficiency. Some electrostatic
The height, width, type, and porosity (leaf den- systems have also been developed for exterior
sity) of the vegetation appear to be important, and environments and tunnels [164], but further inves-
greater deposition can occur on coniferous plants tigation into their effectiveness is required.
than on broadleaf plants due to the larger leaf
surface area per unit ground area [159]. However,
the results of trials have been mixed, and there are Future Directions
likely to be several practical difficulties associated
with the use of vegetative barriers in built-up Outlook
areas, including available space, soiling by traffic, The future global outlook for transport-related
and the general hostility of the roadside environ- pollution currently looks rather bleak. In develop-
ment to plant life. In addition, analyses carried out ing countries, the rise in car ownership and travel
for a busy arterial road show that very large veg- is predicted to be even more dramatic than it has
etation areas (in excess of 10,000 m2) would be been in industrialized nations. For example, the
needed to compensate for the local emissions rate of car ownership in Brazil is predicted to
from vehicles [160]. overtake that in the country that has historically
been the world leader – the United States – before
Air Treatment Various air treatment approaches the middle of the century. Car ownership in China
have been devised with the aim of reducing air has doubled in the last 5 years, and it already has
pollution. In recent years considerable efforts the third highest car sales in the world [126].
have been made to develop construction materials However, at the time of writing there appear to
and coatings, which have the potential for be some signs of change, but probably not as a
76 Air Quality, Surface Transportation Impacts on

result of environmental pressures. Certain Member Shipping is currently one of the least regulated
States of the EU reported rather large decreases in emission sources, with a high reduction potential
emissions from road transport between 2007 and through technological improvements, alternative
2008, reflecting at least in part the lower amount of fuels, and ship modifications. It has been observed
freight transport by road in the second half of 2008 that if the sulfur content of fuel oil remains at
as a result of the economic recession [8]. In addi- present-day levels, a doubling in the emissions
tion, the recession has had a significant effect on of some pollutants from shipping can be expected
car sales. Several governments have introduced by 2050. However, given the increasing concern
scrappage schemes to maintain or stimulate about shipping-related air quality, further reduc-
demand for new cars, but these schemes should tions of NOx and SO2 emissions seem likely.
also result in the replacement of older polluting Using aggressive NOx emission reduction tech-
vehicles with new and more efficient ones. Data nologies, a decrease up to 85% in NOx emissions
sets from other regions also show the impact of the could be reached through technological improve-
economic climate. In 2008, in the United States, ments by 2050, in spite of a growing fleet [166].
the number of vehicles per 1,000 people decreased
for the first time since 1997. Similarly, total
Research Needs
vehicle-miles travelled decreased slightly from
Emissions from transport, and the resulting ambi-
2007 to 2008 – the first decline since 1980 [165].
ent air pollution, have been studied intensively,
Nevertheless, governments around the world
although there are still a number of areas where
are acknowledging that action is required to con-
the understanding is poor or incomplete. Some of
trol the rate of traffic growth, to improve the
these areas are summarized below.
environmental performance of vehicles, and to
increase public awareness about the impacts of
Testing Methods for New Technologies In leg-
pollutant emissions from transport. As noted ear-
islative terms, the emphasis at present is on the
lier, it is likely that the future shape of transport
definition of appropriate procedures for the type
will be influenced more by the need to reduce
approval of hybrid-electric, full-electric vehicles
greenhouse gas emissions than the need to
and hydrogen ICE vehicles. In some cases, certifi-
improve local and regional air quality. The devel-
cation will be problematic. For example, the current
opment of a sustainable transport system will
heavy-duty engine test procedure cannot be applied
involve a large number of interventions that are
meaningfully to hybrid vehicles, as the instanta-
beyond the scope of this entry, but will probably
neous behavior of the engine is decoupled from the
include reducing dependence on cars, effective
instantaneous road load. Vehicle-based tests may
land-use planning to reduce journey distances,
therefore become the norm in the future, although
improving the quality of public transport,
this in itself introduces certain challenges given the
etc. Preventative measures will also need to be
large number of possible vehicle configurations and
accompanied by mitigation measures which
differences in real-world operation. Such challenges
reduce human exposure to air pollution.
might be overcome by the modelling of powertrains.
For the control of local air pollution, it is likely
that emission legislation will still be the main
instrument for governments in the future. How- Understanding PM Emissions In recent years
ever, the future of European emission legislation evidence has accumulated indicating that airborne
post-Euro 6/VI is somewhat uncertain. There is a particles exert a range of adverse health effects.
drive toward the global harmonization of legisla- These effects are diverse in scope, severity, and
tion, but given that the threat of climate change is duration [4]. More work is needed in the future to
increasing the pressure on manufacturers to accurately characterize particle emissions from
develop low-carbon power sources as alternatives surface transport modes and to uncover the mech-
to fossil fuels (batteries, fuel cells, etc.), it is anisms by which health impacts occur.
therefore unlikely that the current test procedures It has already been noted in this entry that a
will remain relevant. better understanding of non-exhaust PM is
Air Quality, Surface Transportation Impacts on 77

required, including characterization of the emitted modelling approaches to be reevaluated, and for
particles, investigation of health impacts, and the improvements to be made. This requires a better
development of methods of prevention and miti- understanding of the circumstances under which
gation. The importance of brake wear may dimin- emission models provide inaccurate predictions.
ish in the future as regenerative braking systems in For example, some modellers believe that the
hybrid and electric vehicles partially or fully exhaust emission factors for road vehicles are
replace traditional mechanical ones. However, unsuitable for certain road types and traffic con-
this is not currently taken into account in emission ditions. Particular concerns have been expressed
calculations and projections. about the validity of the emission factors for
More detailed information on PM emissions so-called congested traffic. The term “congestion”
from rail and shipping (especially inland ship- also needs to be defined in a manner that is mean-
ping) is also required, including emission factors ingful in terms of emissions.
for different engines and fuel type combinations,
in terms of size distribution, particle numbers, and Improving Activity Data While obtaining pri-
chemical speciation [34]. Few studies have exam- mary activity data for road transport by direct
ined PM levels in the ambient air alongside rail- measurement remains the main approach for
way lines. These often run very close to housing, short-term modelling exercises, it tends to be a
and may contribute to local air quality problems, rather expensive activity, and would be unfeasible
especially where large numbers of diesel trains are where an emission estimate is required for a large
in use. PM concentrations could also be elevated geographical area. Traffic assignment models and
near shunting yards and depots. In addition, there microsimulation tools are increasingly being used
is little information on PM concentrations in sta- to provide the relevant data, and communications
tions where diesel trains are left running at idle technology such as Intelligent Transport Systems
and the dispersion of pollution is restricted. and Advanced Transport Telematics enable trans-
port networks to be monitored in real time. It
Understanding NOx Emissions In order to could well be possible to adapt a number of
understand atmospheric NO2 it is important to models and new technologies to contribute appro-
understand NOx emissions, and it is possible that priate information on fleets and traffic activity.
the latter are being underestimated by models. For In shipping the use of data from AIS and
example, there is evidence to suggest that NOx CEMS has a great deal of potential, and even
emissions from Euro V heavy-duty vehicles are more so if it can also be extended to cover inland
significantly higher than the limit at type approval shipping. Data from AIS have already been incor-
[110]. Vehicles equipped with SCR have very low porated into at least one model [167]. However,
emission levels during rural and motorway driv- some work is required to validate emission esti-
ing, but not under the low engine loads associated mates obtained using AIS data [34]. Research is
with urban or driving. The reason for this is that also required on the movements of empty ships, as
the SCR system needs to attain a certain temper- these are often excluded from emission
ature for efficient NOx reduction. The real-world estimates [34].
performance of SCR should therefore be investi-
gated. Furthermore, more extensive information Model Validation Model validation is an impor-
on f-NO2 values for a wider range of vehicles is tant area for improvement. The literature on the
required. validation of transport emission models is quite
limited, and validation studies are often only par-
Improving Emission Models Accuracy, reli- tial in the sense that they address just one type of
ability, consistency, and credibility are prerequi- road, type of vehicle, or time period. The under-
sites of emission estimates. However, standing of the uncertainties in emission models
comparisons between the results from different and the main factors affecting prediction errors is
emission models have highlighted substantial dif- therefore poor [168]. Emission models should
ferences. There is therefore a need for emission quantify prediction errors. The models in common
78 Air Quality, Surface Transportation Impacts on

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veillance de la Qualité de l’Air en Ile-de-France,
would allow for a better assessment of the relative Laboratoire d’Hygiène de la Ville de Paris, Mairie
performance of different model types. de Paris, DASES, Laboratoire Central de la Préfec-
ture de Police
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Hurley JF, Tran CL (2005) The London under-
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Prague underground transport system. Atmos Envi-
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0-19-850375-X
or plant life or property or unreasonably inter-
Airborne Nanoparticles: fere with the enjoyment of life or property,
Control and Detection outdoor recreation” [1].
Aerosol is a solid or liquid particle suspended in
Mohsen Rezaei1 and Matthew Stanley Johnson1,2 a gas. Such particles may be produced directly,
1
Department of Chemistry, University of for example, from combustion or indirectly
Copenhagen, Copenhagen, Denmark from gas-to-particle conversion. The former is
2
Airlabs, Copenhagen, Denmark primary aerosol and the latter secondary aero-
sol [2]. There are multiple processing mecha-
nisms in the atmospheric including exchange
Article Outline with the gas phase and coagulation.
Nanoparticle is a size category of aerosol parti-
Glossary cles with diameter between 1 and 100 nm [2].
Definition Anthropogenic emissions include man-made
Introduction pollution from activities such as transportation,
Source and Health Effect of Nanoparticles cooking and heating, industry, and energy pro-
Nanoparticle Control Technologies duction, involving combustion of fossil fuel
Nanoparticle Filtration and biomass. Human activities can be the
Electrospun Nanofibers main primary source of airborne nanoparticles
Electrospinning Process both indoors and outdoors [3].
Performance of Electrospun Nanofibers Filtration efficiency characterizes the perfor-
Carbon Nanotubes (CNTs) mance of a filter or any process that can trap
Electrostatic Precipitation particles passing through it. It can be determined
ESP Performance by measuring mass or number density of parti-
Thermophoresis cles before and after filtration, for a specific
Particle Coagulation source or as a function of particle size [4].
Nanoparticle Detection Particle coagulation when there is a large num-
Aerosol Particle Mass Analyzer (APM) ber of concentrations of airborne particles, they
Impaction move by Brownian or turbulent diffusion;
Optical Measurement thereby their collisions increase with each
Condensation Particle Counter (CPC) other, resulting in sometimes aggregate clus-
Particle Electrical Mobility ters or a single new larger particle [1].
Particle Diffusion Mobility Nanoparticle characterization is a subfield of
Measurements of Nanoparticle Composition and atmospheric science and technology that uses
Morphology determinations of the physical and chemical
Future Prospects properties of nanoparticles to characterize
Bibliography their behavior and impacts [5].
Impaction when a particle is large and dense, its
Glossary inertia will cause it to remain in the streamlines
to be collided with the object. This is called
Air pollution “is the presence in the outdoor impaction [1].
atmosphere of any one or more substances in Light scattering scattering of light as a result of
quantities which are or may be harmful or collisions with particles called light
injurious to human health or welfare, animal scattering [5].

© Springer Science+Business Media, LLC, part of Springer Nature 2021 85


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_1099
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2020, https://doi.org/10.1007/978-1-4939-2493-6_1099-1
86 Airborne Nanoparticles: Control and Detection

Electrical mobility “when a charged particle is fine (PM2.5), and ultrafine (PM0.1) fractions. The
exposed to an electric field, it will migrate at a subscripted number is a cutoff size, for example,
velocity that is determined by a balance PM2.5 is the total mass density of all aerosol
between the resulting electrostatic force and particles with an aerodynamic diameter less than
aerodynamic drag that resists its motion. This 2.5 mm. Airborne nano-sized particles, i.e., nano-
characteristic migration velocity is described particles, belong to the ultrafine class of particles;
as the electrical mobility of the particle” [5]. they are often solid phase and have a dimension
less than 100 nm. Nanoparticles are commonly
emitted during combustion and are formed
Definition through gas-to-particle conversion.

This chapter will review the properties and behav-


ior of nanoparticles suspended in air and measure- Introduction
ment technologies for monitoring, characterizing,
and controlling them, to reduce their adverse There is a growing interest in airborne nano-
effects on the environment and human health. particles (NPs) because of their unique properties
A huge variety of particles is found in the atmo- for health and climate and the increasing devel-
sphere and built environment. Many environ- opment of nanomaterials. NPs can easily enter
ments include unwanted gases and particles that the body and be distributed due to their small
can originate from primary emissions or from size. In addition NPs cause serious environmen-
secondary transformations in the atmosphere. In tal problems including changing the dynamics of
addition there is significant processing within the cloud formation, thereby contributing to drought
atmosphere including condensation and evapora- and global warming and impacting the radiation
tion, multiple cycles of activation into a droplet balance of the Earth, as reported in the literature
followed by dehydration, coagulation, photolysis, [6]. Recent studies have reported the harmful
and chemical reaction. Research has shown that effects of NPs on human health including
aerosol particles in the indoor and outdoor envi- mortality [7–9] and their association with pulmo-
ronments have significant detrimental impacts on nary disease, cancer, incident wheezing, asthma,
health. The word aerosol was introduced in lower spirometric values, and increased asthma-
ca. 1920, in analogy to “hydrosol,” a liquid col- related emergency in children [10, 11]. Toxico-
loidal suspension of solid particles. Aerosols are logical studies show that NPs possess unique
particulate matter, either liquid or solid or a com- physicochemical impacts due to their high
bination, suspended in a gaseous medium. “Aero- number concentration, ultrahigh reactivity, and
sol particle” refers to the suspended particles high surface area to mass ratio relative to other
themselves and can be divided into two groups, particle size classes [7], resulting in elevated
primary and secondary, depending on their origin. bioavailability and toxicity [12]. Because of
The former is generated by a source at the surface, their small size, nanoparticles can enter into the
for example, abrasion or combustion. The latter is bloodstream from the alveolar region of the
often produced from gas-to-particle conversion or respiratory tract or through the skin. Conse-
agglomeration of primary aerosols. Primary and quences include cardiopulmonary effects, oxida-
secondary aerosol particles are characterized by tive stress, and cancer [13].
their shape, size, and chemical composition. Because of their weak light scattering ability
A spherical shape is often assumed, to simplify and extremely small size, NPs are often not visi-
calculations. Aerosol particles are commonly ble. In addition they follow the streamlines of the
classified by their “aerodynamic diameter,” that carrier gas making them more difficult to control
is, the diameter of a spherical particle with the and measure than fine and coarse particles. Some
same aerodynamic behavior. These classifications common and effective technologies for removing
divide particulate matter (PM) into coarse (PM10), coarse particles, such as centrifugation or settling,
Airborne Nanoparticles: Control and Detection 87

are only marginally effective for nanoparticles. nanoparticles, as well as the principals of each
The choice of controlling technology is limited technology, and the effects of operational and
to only a few methods. Filtration and electrical structural parameters on removal efficiency.
precipitation are widely taken to be the best These parameters are discussed by comparing
options available. Fibrous filtration can filter and reviewing significant studies. In addition,
NPs close to 99.999%, and a carbon wall mem- measurement techniques for nanoparticles along
brane filter would be able to meet filtration effi- with their principal and comparative perspective
ciency up to 99.9999%. Newer technologies are presented.
include phoretic and nanomaterial approaches,
but their use in achieving clean air goals is
untested. Source and Health Effect of
Monitoring is one of the greatest challenges Nanoparticles
facing organizations that deal with indoor and
outdoor air quality. It is clear that ultrafine parti- Concern about exposure to NPs has increased
cles possess quite different physicochemical prop- dramatically due to awareness of and increase in
erties, such as ultrahigh reactivity, high number anthropogenic sources involving transportation,
concentration, and high surface area to mass ratio, industry, and energy production. Specific exam-
relative to other size classes [7]. However, data ples include soot from diesel engines, abrasion
concerning the composition and spatial/temporal from tires and brake pads, smoke, and urban
distributions of NPs are limited, making it difficult smog. The developing field of nanotechnology,
to study their health effects [12]. There is great producing new electronic, magnetic, optoelec-
interest in developing new methods for monitor- tronic, biomedical, pharmaceutical, cosmetic,
ing NPs; key parameters include sensitivity, energy, environmental, and catalytic products
range, size resolution, and cost. Instruments for and processes, is another source of human expo-
measuring NPs can be grouped into impaction, sure to engineered NPs. Some of the natural and
optical, diffusion, gravimetric, and electrical anthropogenic sources of NPs are summarized in
mobility techniques. Sometimes the techniques Table 1 [3]. In nature, NPs are produced by many
are combined. The micro-orifice uniform deposit sources such as in situ photochemical reactions,
impactor (MOUDI, TSI Nano-MOUDI 125R), forest fires, volcanic eruptions, sea-salt spray,
laser aerosol spectrometer (LAS, TSI 3340A), microorganisms, biogenic magnetite, and so
condensation particle counter (CPC TSI CPC on. Graphitic soot is produced by wildfires. Due
3750), and scanning mobility particle sizer to their light scattering properties, NPs impact the
(SMPS, TSI 3938 E57 with 3082, 1 nm electrical radiation balance of the Earth directly and indi-
classifier and CPC 3750) are commercialized rectly and are central to the mechanisms of climate
examples of systems measuring ultrafine/fine change [14]. Many kinds of NPs are known within
aerosol particles. organisms. Natural production of NPs can occur
Nanoparticle aerosol science and technology is through intracellular and extracellular mecha-
a rapidly growing field. Many research papers nisms including within human brain cells. Many
describe nanoparticle control and characterization organisms produce nanomaterials through intra-
techniques in detail. It would therefore be useful cellular and extracellular processes. For example,
to review the field’s current status and future biogenic magnetite is a kind of nanomaterial that
vision. In this review, first, the source and health has been found in many microbial species includ-
effect of nanoparticles are summarized. This is ing microorganisms (from bacteria to protozoa)
followed by a presentation of control technologies and in animals (e.g., human brain) and which has
for nanoparticles, including filtration methods, been associated with neurodegenerative
electrostatic precipitators, thermophoretic and diseases [15].
diffusiophoretic methods, and grouping technol- Anthropogenic sources are estimated to
ogy, with a focus on removal mechanisms for account for about 10% of total NPs. NP sources
88 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, documented the association of ambient NPs with
Table 1 Natural and anthropogenic sources of NPs adverse cardiovascular and respiratory effects in
Category Source humans [17–19]; however, not all studies have not
Natural Fire (forest) seen these associations [20, 21]. Intensive depo-
Volcanoes sition of laboratory-engineered NPs in the respi-
Microorganisms
Sea spray (e.g., salt) ratory tract, even greater with asthma or chronic
Biogenic magnetite obstructive pulmonary disease, has been seen in
Ferritin (12.5 nm) controlled clinical studies. On the other hand,
Anthropogenic Condensation and nucleation controlled exposure to carbonaceous NPs has
Car exhaust and brakes been seen to cause many symptoms in the cardio-
Road
Power generation vascular system including systemic inflammation
Mines and changes in pulmonary diffusion capacity and
Factories (e.g., cement) the appearance of coagulation markers in the
Incinerators (e.g., waste) blood. In vivo tests by Brown et al. [22] have
Jet engines
Fumes, e.g., polymer and metal fume shown an increased inflammatory response after
Stove (cooking) the introduction of 64 nm polystyrene particles
Smoking into the rat lung, and they have observed a pro-
Laboratories engineered nanoparticle inflammatory effect after in vitro cell culture with
(e.g., catalysts)
the model NPs. In addition, an oxidative stress-
related cellular response with ambient NPs has
been reported by Li et al. [18].
can be divided into industrial and urban. Industrial The main deposition mechanism for inhaled
activities release NPs into the atmosphere inside NPs in the respiratory tract is diffusion; other
factories working with metallurgy, power and deposition mechanisms including inertial impac-
cement production, mining, incineration, and tion, gravitational settling, and electrostatic force
any industrial product that uses fossil fuels as an are not significant. Figure 1 shows three exposure
energy source for power generation. In urban regions for inhaled aerosol particles in the human
areas, vehicles are a common source of NP out- respiratory tract including the nasopharyngeal,
doors, being produced by internal combustion tracheobronchial, and the alveolar region. The
engines, road dust and wear on brakes and tires. figures on the right (Fig. 1) show which sizes of
Important indoor sources of NP include cooking, PM can deposit in each region of the respiratory
cleaning and smoking. Of course, the chemical tract. With an increase in size from 1 to 100 nm,
and physical nature of NPs emitted in industrial high percentages of inhaled NPs are deposited on
and urban areas can be quite different. Indoor the upper regions of the respiratory tract. For
emissions can be most important for determining example, ~90% and ~10% of 1 nm particles are
health impacts because humans normally spend deposited in the nasopharyngeal and the tracheo-
>80% of their time in the indoor environment bronchial regions, respectively, while no particles
[16]. Engineered nanoparticles are commonly are deposited in the alveolar region. In contrast,
used in stain-resistant clothing, sporting goods, 50% of 20 nm particles are deposited only in the
tires, sunscreens, cosmetics, and toothpaste and alveolar region [15]. Manigrasso et al. [19] esti-
as food additives, etc. and are specifically mated a respiratory deposition of 6.6  1010 par-
engineered in the laboratory to form nano- ticles of 5.6–560-nm-diameter particles per hour
structures such as nanotubes, nanofibers, and for persons close to traffic, in short-term peak
nanowires [15, 16]. exposure events. It has been seen that deposited
Epidemiological and clinical studies on NPs are transported to extrapulmonary organs to a
humans and rodents, and also in vitro cell cultures, greater extent and by a larger variety of transfer
have shown the health effects of laboratory- routes than for larger-sized particles. One is the
generated and ambient NPs. Researchers have conduction of NPs into blood by transcytotic
Airborne Nanoparticles: Control and Detection 89

Airborne Nanoparticles: Control and Detection, region of the human respiratory tract during nose breath-
Fig. 1 Predicted fractional deposition of inhaled particles ing. (Reprinted with permission [15])
in the nasopharyngeal, tracheobronchial, and alveolar

transport across epithelia of the respiratory tract used in recent years. It should be noted that air
and subsequently into the interstitium or by lym- quality regulatory organizations are imposing
phatics which can distribute throughout the body. increasingly strict rules as knowledge of the
Another is axonal translocation of NPs to gangli- health effects of nanoparticles has grown. In par-
onic and CNS structures by their uptake by the allel with increased knowledge, it has become
sensory nerve endings of airway epithelia. Nano- increasingly urgent to implement suitable particle
toxicological studies have demonstrated that control systems. The most effective and important
inhaled NPs can deposit in the nasal cavity, technologies for capturing nanoscale particles will
being absorbed by the olfactory epithelium and be examined, based on their physical properties,
translocated into the brain through the blood-brain the required degree of control, cost, etc. [23].
barrier [17].

Nanoparticle Filtration
Nanoparticle Control Technologies
Filtration is the most commonly used method for
One of the most important concerns for air pollu- trapping airborne particles. Different types of fil-
tion control is the removal of nanoparticles from ters are used to target a wide range of airborne
airstreams. A variety of technologies have been particles. The most common forms are fibrous,
90 Airborne Nanoparticles: Control and Detection

porous membrane, capillary pore membrane, fab- the filter material. The material comprising the
ric, and granular bed [24]. Fibrous filters are the filter has a cross-sectional area reducing the area
simplest and most economical filters and are capa- through which air can flow. If Q is conserved and
ble of efficiently removing nanoscale particles A decreases, U will increase. The velocity through
from gas streams [25]. the filter (Uf) is further defined as:
It is important to quantify filtration perfor-
mance in order to document and compare the Q
Uf ¼ ð6Þ
abilities of particle filters. Filter efficiency and A ð 1  aÞ
pressure drop are the most crucial parameters in
this regard [26]. Equations (1) and (2) define filter where a is the packing solidity or density of the
efficiency in terms of mass concentration and filter, which can be obtained from Eq. (7):
particle number, respectively:
Vf
a¼ ¼1∅ ð7Þ
C C VT
E¼ 0 ð1Þ
C0
where Vf is the fiber volume; VT, the total filter
N N volume; and ∅, the porosity [24].
E¼ 0 ð2Þ
N0 The goal is to create a filter that combines a
high filtration efficiency (E) with a low pressure
where C0 and C are the mass concentrations drop (Dp), thereby cleaning air while minimizing,
(typically as mg/m3) of particulate matter before e.g., power and noise. However, in most particu-
and after filtration and N0 and N are the number late filter systems, an increase of the filtration
concentration (usually as number per m3) before efficiency also increases pressure drop. The resis-
and after filtration. tance to airflow across the filter is characterized by
The efficiency of pollution control equipment the pressure drop and arises from the combined
is often characterized in terms of the fraction drag force of the fibers. Assuming laminar flow,
entering versus exiting the filter. This metric is pressure drop will increase with the face velocity;
known as particle penetration (P): to a first approximation, this relation is linear.
Pressure drop is proportional to filter thickness
C and the packing density of fibers and is inversely
P¼ ¼1E ð3Þ
C0 proportional to the square of the fiber diameter
[27]. Despite this, for many installations, it is
N
P¼ ¼1E ð4Þ desirable that the pressure drop of the filter should
N0
be less than ~150 Pa which is often difficult to
In addition to performance against particles, achieve while maintaining high filtration effi-
ciency. The quality factor is one criterion used to
HVAC system engineers require some additional
information to design filtration systems and judge judge the performance of a filter, as defined by
their efficiency: The volumetric airflow passing Chen [28]:
the filter (Q) and its velocity at the face of the filter
(normal to the filter, “U”) impact P and E. They  ln ð1  EÞ
Quality factor ¼ ð8Þ
are related as shown in Eq. (5): Dp

Q The QF shows the correlation between filtra-


U0 ¼ ð5Þ tion efficiency and pressure drop. A filter with a
A
greater filtration efficiency and lower pressure
A is the area of the filter. However, the air drop will have a high quality factor.
velocity inside the filter is higher than the face In recent years, nanoscale fiber filters have
velocity because of the air resistance caused by received increasing attention for air filtration
Airborne Nanoparticles: Control and Detection 91

because of favorable properties including small The diffusion constant increases as the size of
pore size and high specific surface area. These particles decreases. For particles smaller than
properties enable the slip effect of airflow through ca. 100 nm, diffusional separation of particles from
the fibers, reducing the drag force on the airstream the continuum flow streamline can be the dominant
as it passes nanofibers and subsequently strength- mechanism leading to impaction. Every filter has a
ening the different filtration mechanisms on the minimum in efficiency for a characteristic particle
filter [26]. Normally the surface of a fiber blocks size called the most penetrating particle size
the airflow, diverting airstreams, triggering turbu- (MPPS), which typically falls between 100 and
lence and viscosity, and necessitating power and 300 nm. The removal efficiency of filters at the
pressure drop for the air to flow past. However, MPPS determines the filter grade. In addition there
when the fiber diameter similar to or below the are two criteria, surface chemistry and the electro-
size of the mean free path of air molecules (just static potential of fibers, which play significant roles
under 70 nm), normal continuum flow behavior in determining filtration efficiency. For example,
no longer applies. Molecules can fly past the fiber polar functional groups at the filter surface may
without interrupting the momentum of the flow; lead to strong adsorption of nanoparticles.
this is called “slip flow.” As detailed below, The relative roles of the mechanisms depend
because of slip flow, nanofiber filters hold the on the Knudsen number (Kn) as [26]:
promise of yielding high QF filtration for
nanoparticles. 2l
Kn ¼ ð9Þ
Air filtration using fibrous filters is a promising df
method for separating nanoparticles from an air-
stream while allowing air molecules to pass where df is the diameter of fiber and l is the mean
[29]. Filters manufactured with materials includ- free path of gas molecules. The mean free path is
ing plastic, cellulose, glass, and carbon are the ca. 66 nm at the standard state of air, obtained as:
most common [24]. The fibers are made into a
soft flexible mat, with fiber orientations primarily l ¼ pffiffiffi
RT
ð10Þ
perpendicular to the streamline [30]. These mats 2N a p d2m p
provide a high filtration efficiency for ultrafine
particles along with minimal aerodynamic resis- where R is the gas constant, T temperature, Na
tance and thus find many applications such as Avogadro’s number, dm the collision diameter of
industrial and indoor cleaning purification, respi- an air molecule (3.7  1010 m), and p the air
rators, and car cabins [23, 30]. pressure [31].
A few mechanisms are important for trapping There is a relationship between the airflow
nanoparticles from their air: interception, inertial regime, as defined by the Reynolds number,
impact, diffusion, and electrostatic deposition. across the filter and the fiber diameter in all the
Their relative importance will vary depending on airborne particle filtration systems. Particles can
gas velocity, particle and fiber size, particle charg- be removed from an airstream in the continuum
ing, surface static charge, and so on. The total flow regime (Kn < 0.001, generally for milli-
filtration efficiency for nanoparticles is the sum scale fibers), the slip flow regime
of the filtration efficiencies of particles by each (0.001 < Kn < 0.25, generally for microscale
mechanism (Table 2). Sound classical descrip- fibers), the transition flow regime
tions of fibrous filter performance can be found (0.25 < Kn < 10, for nanoscale fibers), and the
in many sources (see, e.g., [23, 24, 30]). free molecular regime (Kn > 10, for ultrafine
Particles larger than around 300 nm are subject scale fibers), as shown in Fig. 2a, b [32]. In the
to inertial separation from a curved flow stream- continuum flow regime, the mean free path of the
line, leading to impact with an obstruction. Such gas molecules is much smaller than the diameter
particles are unable to adjust to an abruptly chang- of the fiber. Most filtration systems use fibers
ing streamline in the vicinity of a fiber. operating in the continuum flow regime. The
92 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, Table 2 The filtration mechanisms and their filtration efficiency
Filtration mechanism Single-fiber filtration efficiency Definition Point
Interception ER ¼ ð1aÞR2 ER: filtration Only a deposition
K u ð1þRÞ or,
 
ÞR2   efficiency by mechanism does not
Fiber ER ¼ 0:6 Kð1au ð1þRÞ
1 þ kRn the result from a particle
d
R ¼ dpf interception departing from its
2
dp: particle original streamline
K u ¼  Ln2 a  34 þ a  a4 diameter
df: fiber
diameter
Ku: Kuwabara
hydrodynamic
factor
a: packing
density
(solidity)
Inertial impaction EI ¼ ðSTK ÞJ EI: filtration The most important
2K 2 u
rp d2p Cc U 0
efficiency by deposition mechanism
Fiber STK ¼ 18mdf the impaction for large particles
J ¼ (29.6  28a0.62)R2  27.5R2.8 STK: Stokes
number
J:
dimensionless
Cc:
Cunningham
coefficient
rp: particle
density
m: air dynamic
viscosity
Diffusion (Brownian  1=3 ED: filtration Only the deposition
1a 2=3
ED ¼ 1:6 2Pe
motion) Ku efficiency by mechanism that
d U
Pe ¼ fD 0 the diffusion increases as the
Fiber
D ¼ 3pmD
kb TCs Pe: Peclet particle diameter
p
   number increases
Cs ¼ 1 þ K n 1:027 þ 0:44 exp 0:78=Kn D: particle
diffusion
coefficient
kb: Boltzmann
constant
T: absolute
temperature
Cs:
Cunningham
slip correction
Electrostatic deposition Difficult to quantify because it requires – This mechanism is
knowing the charge on the particles and often neglected unless
Fiber
_ on the fibers the particles and/or
fibers have been
charged in some
quantifiable way

slip airflow regime is characterized by an regime in which the diameter of fibers is much
increase in the Knudsen number, resulting in an smaller than the mean free path of the gas mole-
increased filtration efficiency via the slip effect. cules. In general, nanoparticle-capturing fibers,
The free molecular flow regime is a dominant including electrospun fibrous filters and carbon
Airborne Nanoparticles: Control and Detection 93

Airborne Nanoparticles: Control and Detection, with permission [32]). SEM images (c) of PUR electrospun
Fig. 2 (a) Flow pattern around fibers of different diameter. nanofibers and (d) carbon nanotubes. (Reprinted with per-
(b) The surface areas of the nanofibrous filters. (Reprinted mission [31])

nanotubes, have higher surface areas for nano- air is said to slip past, as described in terms of the
particle deposition than microfibers that operate Reynold’s number above.
under the transition airflow (electrospun filters The filtration efficiency for a clean fibrous filter
(Fig. 2c)) and free molecular airflow regimes can be determined using Eq. (11):
(carbon nanotubes (Fig. 2d)). It should be noted
that it is not possible for other fibers to achieve 
4aEf Z
the free molecular regime by increasing l by E ¼ 1  exp ð11Þ
pð1  aÞdf
reducing the pressure [26]. The slip flow effect
can be understood by considering the interplay
between viscosity length and fiber diameter. where, a, Z, Ef, and df are fiber packing density,
A large fiber blocks the airflow, so the momen- filter thickness, single-fiber efficiency, and mean
tum of the air is zero in the vicinity of the surface. fiber diameter, respectively. For nanofiber filters,
As fiber size decreases, the height of the surface interception and diffusion are the most important
layer, called the quasi-laminar layer, decreases, trapping mechanisms, and thus the sum of the
becoming zero. A nanofiber is not able to signif- mechanisms can be used to approximate the the-
icantly impact the momentum of the flow and the oretical single-fiber efficiency, as follows [24]:
94 Airborne Nanoparticles: Control and Detection

Ef ¼ E R þ ED ð12Þ high potential with a voltage of kV applied


between a fiber collector and the syringe needle.
The combined forces of surface tension and elec-
Electrospun Nanofibers trostatic repulsion result in the formation of the
Taylor cone at the needle tip. The electric field
A series of studies have found that electrospinning overcomes the surface tension and a stable jet is
is capable of producing a felt or mat of high formed at the needle tip. The combined result is
porosity electrospun nanofibers which efficiently that an elongating-and-whipping process is con-
and effectively remove ultrafine PM from an air tinuously generated by electrostatic repulsion
stream. The diameter of the electrospun nano- resulting in a thin string. These fibers accumulate
fibers can be from <2 nm (microporous) to on the collector forming a mat of nanofibers.
50 nm (mesoporous) and are a thousand times Finally, the nanofiber mat is removed from the
smaller than microfibers [33]. Figure 3 shows collector, after evaporation of the solvent. It
the most common electrospinning equipment. should be noted that the solution electrospinning
method, compared to melt electrospinning, is able
to generate fibers with a smaller diameter. The
diameter of the fibers can be controlled by chang-
Electrospinning Process
ing solution parameters, such as the concentra-
tions of the components, and operating
Electrospinning is a technique that uses an elec-
parameters such as the electrospinning voltage.
trostatic force on a polymer fluid to produce nano-
Additionally, a variety of fiber structures, includ-
fibers. After Formhals, Taylor developed the
ing hollow, core/shell, secondary growth, porous,
method mathematically, describing the effect of
and helical, can be generated by controlling the
the electrostatic charge on the polymer droplet to
electrospinning procedure, solution components,
form a conical structure, called a Taylor cone [33].
and calcination parameters. In addition the nano-
As can be seen in Fig. 3, polymer solutions or
fibers can be modified after spinning using
melts are loaded into a syringe which is held at a

Airborne Nanoparticles: Control and Detection, Fig. 3 Schematic of the electrospinning technique
Airborne Nanoparticles: Control and Detection 95

thermal or chemical treatment to improve features was recently reported that nanofiber diameters
that include pore size, conductivity, and mechan- less than 100 nm enhance the slip flow effect,
ical strength. Thermal posttreatment can be used decreasing drag and pressure drop and subse-
to control the diameter of nanofibers. Metal oxides quently increasing particle capture [37]. One
or salts in the nanofibers can be used to make the study used keratin-based nanofibers to demon-
fibers bactericidal, and graphitization of carbon strate the effect [39]. Polymeric nanofiber felts
onto the nanofibers will enhance their specific made of PU nanofibers [31], cellulose [40], and
area surface. Chemical modification may add PVP [41] have been produced by electrospinning
properties similar to thermal treatment. Nano- and also show improved filter performance due to
fibers generated by electrospinning can make use their reduced fiber diameter. In sum, electro-
of a wide range of inorganic, organic, and organ- spinning provides greatly improved filtration effi-
ometallic materials. Almost any soluble polymer ciency due in part to smaller fiber diameter that is
can be incorporated into nanofibers with the able to capture ultrafine particles; the smaller the
electrospinning method with the constraint that fiber, the greater the filtration efficiency.
their molecular weight should be sufficiently The surface area and pore size of nanofibers are
high. Examples include polyvinylpyrrolidone affected by the fiber structure and the composition
(PVP), polyethylene oxide (PEO), polyvinyl ace- of the blended solution. Liu et al. [42] prepared an
tate (PVAc), and polyvinyl alcohol (PVA), which electrospun PAN/polyacrylic acid (PAA) compos-
are water-soluble polymers, and non-water- ite nanofiber felt to study the effects of PAN/PAA
soluble polymers such as polyimide (PI), polyac- ratios on filtration performance. Blending PAA
rylonitrile (PAN), polyvinylidene fluoride with PAN allowed creation of a composite with
(PVDF), polylactic acid (PLA), polymethacrylate features that could be controlled. The tensile
(PMMA), polystyrene (PS), polypyrrole (PPy), strength of the nanofibers greatly improved,
and polyvinylchloride (PVC) [34]. going from 3.8 to 6.6 MPa as the PAA content
increased, creating robust mechanical strength in
pure PAN nanofibers. The smallest pore size in the
Performance of Electrospun Nanofibers membranes resulted in a very high filtration effi-
ciency, over 99.99%, with minimal pressure drop,
Nanofiber filters have attracted a great deal of 160 Pa. A porous bead-on-string polylactic acid
interest since they have a high filtration efficiency (PLA) membrane for capturing nanoparticles was
due to interception and a low pressure drop created by Wang et al. [43]. The large surface area,
because of the slip flow effect. Many parameters coupled with microporous beads, showed
impact filtration performance including the phys- enhanced filtration efficiency. A smaller pore
ical properties of the filter (such as nanofiber size polyvinyl alcohol (PVA) nanofiber filter fab-
diameter, surface area, pore size, packing density, ricated by Li et al. [44] has shown a high filtration
basis weight, and thickness) and the conditions of efficiency for nanoparticles. Wang et al. [45]
the installation such as face velocity. Particulate found that adding SiO2 nanoparticles to multi-
matter builds up on the filter in dendrimers which layer PAN structures created bimodal distribu-
can enhance particle filtration [25]. tions of fiber sizes that increased filtration
Nanofiber diameter is an important parameter performance, with a removal efficiency of
affecting filtration performance. Mao et al. [4] 99.99% at a pressure drop of Dp ¼ 116 Pa, for
evaluated the relationship between fiber diameter nanoparticles relative to single-layer fibers. This
and filtration efficiency and pressure drop, using was said to be due to the roughness of the surface
an yttria-stabilized zirconia (YSZ) nanofiber. fibers arising from the noncircular structure and
They found a decrease in the filtration efficiency also from the greater specific surface area of the
with an increase in nanofiber diameter. At the multilayer fibers, as a result of adding SiO2. Two
same time, smaller fiber diameter decreased pres- membrane fibers, PA6 and PMIA, arranged in
sure drop, regardless of particle size (Fig. 4a, b). It sequence by Zhang et al. [46] showed high
96 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, and filtration efficiency. (Reprinted with permission [36]). (e)
Fig. 4 (a) The effect of the fiber diameter of yttria-stabilized Pressure drop and (f) filtration efficiency for PSU/TiO2-0 and
zirconia (YSZ) on filtration efficiency and pressure drop. PSU/TiO2-5 as a function of face velocity. (Reprinted with
(Reprinted with permission [4]). (b) Schematic landscape of permission [37]). Relationship between the particle diameter
the relationship between fiber diameter and particle capture. and the MPPS. (Reprinted with permission [38]). (h) The
(c) The effect of packing density on MPPS. (Reprinted with captured particle diameter increases with air velocity.
permission [35]). (d) Relationship between fiber basis weight (Reprinted with permission [31])
Airborne Nanoparticles: Control and Detection 97

filtration efficiency (99.995%) for nanoparticles at to a single thick layer nanofiber. Leung et al. [35]
a low pressure drop (100 Pa). The hybrid mem- concluded that the effect of fibers’ thickness on
brane has high porosity, small pore size, and a the MPPS is less than the effect of fiber packing
large specific surface. Generally, microporous density. The work of Yun et al. [52] demonstrated
fibrous filters, despite their higher filtration effi- that the pressure drop across an electrospun PAN
ciencies, have a higher particle retention ratio and filter (270 nm) increased linearly from 63 to
show a higher tendency for clogging [47]. Also, 220 Pa as the fiber thickness increased from
the smaller fiber diameter is associated with a 0.004 to 0.02 mm. However, they reported that
smaller pore size due to the decrease in pore all fibrous filters for a given particle size had the
aperture with fiber diameter, improving the same single-fiber efficiency values, indicating
interception-collision of nanoparticles with the thickness-independent quality factors.
nanofiber and increasing capture efficiency [48]. Hung et al. [53] found that larger fiber basis
The nanofiber packing density (a) depends on weights enhanced filtration efficiency nonlinearly.
fiber density and filter thickness. High a values However, the increased basis weights decreased
correlate with effective particle capture. Some the quality factor due to an increased pressure
workers have investigated the effect of a on the drop (Fig. 4d). Also, this study found that the
filtration efficiency of nanofilters. Leung et al. multi-structure nanofiber membrane produced in
[35] found a good relationship between the pack- the electrospinning process with low basis weight
ing density and the filtration efficiency for PEO showed better performance than a single-structure
fibers. By increasing a from 3.9  103 to nanofiber membrane with a high basis weight.
36  103, filtration efficiency increased from Besides the filter structure, there are many fil-
15% to 90%. At the same time, the most penetrat- tration parameters capable of significantly chang-
ing particle size (MPPS) decreased from 140 to ing filter performance. The air velocity across the
90 nm (Fig. 4c). Choi et al. [38] found that a filter and particle size distributions play a key role
laminated nanofiber with high packing density in this regard [35]. Many studies find that a higher
has a lower quality factor owing to its high pres- face velocity results in a lower filtration efficiency.
sure drop when compared to a mixed fiber Wan et al. [37] found the filtration efficiency of a
(nanofiber 780 nm/microfiber 11.4 mm). Further- polysulfone (PSU) membrane fibrous filter with-
more, reducing the fraction of nanofiber in a out TiO2 decreased from ~100% to 94% as the
microfiber filter enhanced the quality factor at a face velocity increased from 15 to 90 L/min, while
low packing density. Therefore they suggested filtration did not decrease significantly for a filter
that an optimal ratio would be to have a nanofiber coated with TiO2 nanoparticles at 5% by weight
mixing fraction of 5% in mass in order to decrease (Fig. 4e). In the fibrous filters, the pressure drop is
pressure drop and increase the quality factor for proportional to the face velocity in accordance
nanoparticle capture. with the experimental results of this study
According to Eq. (10), a larger fiber thickness (Fig. 4f). Thus, the results suggested low quality
can be useful for improving the performance of factors at higher face velocity. Similarly, Wang
nanofiber filters. By increasing the fiber thickness, et al. [54] have tested a polyvinylidene fluoride
the basis weight and the pore size of fibers are also (PVF)/polytetrafluoroethylene (PTFE) nanoparti-
increased, elevating filtration efficiency. How- cle filter for face velocities of 2–16 cm/s. They
ever, Kim et al. [49] noted that if the fibers are found the filtration efficiency dropped from
too thick, the filtration efficiency is reduced due to ~100% to 95% for pure PVF and a slight decrease
the increased pressure drop. Wang et al. [50] to 98% for PVF with 5 weight percent PTFE.
found that a thick filter contributed to higher The relationship between particle size and fil-
energy consumption and larger pressure drop. tration efficiency is well established. Many stud-
Research by Zhang at al [51] showed that a mul- ies have shown that filtration efficiency is very
tilayer PAN fibrous membrane can be more effec- dependent of the particle size because of its effect
tive for obtaining a high quality factor compared on the efficacy of the capture mechanisms. For
98 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, Table 3 The filtration performance in recent studies
Fiber Filtration Quality
Nanoparticle diameter efficiency Pressure factor
Nanofiber diameter (nm) (nm) (%) drop (pa) (pa1) Study
PAN <100 200 96 133 0.024 [56]
PU (polyurethane) 20–400 120 99.6 96–190 0.06–0.03 [31]
Nylon-6 300 150 99.5 500 0.01 [57]
Nylon-6 <20 15–450 99–98.5 57–283 0.01–0.018 [58]
PAN/PA 300 272 99.99 100 0.11 [59]
(PA: polyamide)
PSU/TiO2 (5%wt) 300–500 76–1590 99.997 43.5 0.17 [37]
PAN/PU-FPU (FPU: 300–500 175 99.98 120 0.07 [45]
fluorinated polyurethane)
PLA 260 144 99.997 165 0.06 [43]
PVDF/PTFE NPs (0.05% 197 250–570 99.997 57 0.14 [54]
wt)

example, for particle sizes larger than the fiber ultrahigh specific surface areas, and robust
diameter, the single-fiber efficiency derived mechanical properties. The limitation of a trade-
using interception is not correct. The relationship off between filtration efficiency and pressure drop
between particle size and filtration efficiency can inherent to fibrous filtration can likely be over-
be quantified using the MPPS. Many studies come with CNT-based filtration [26]. However, it
found that a particle size of around 100–300 nm is very difficult or perhaps impossible to fabricate
is usually the MPPS [38, 55] (Fig. 4g). It has been a CNT that can balance many design constraints
also found that the MPPS changes when the face and trade-offs involving fiber properties such as
velocity changes. Sambaer et al. have shown that air velocity, packing density, and basis weight.
with an increase of the face velocity, the MPPS The important characteristics of the CNT nano-
decreases (Fig. 4h) [31]. fibers are similar to those discussed for electro-
Table 3 shows the filtration efficiency, pressure spun nanofibers. Key features of the performance
drop, and quality factor for different polymeric of the CNTs are discussed below.
membrane nanofibers. Viswanathan et al. [27] coated a continuous
layer of MWNT (df ¼ 20–50 nm, thick-
ness ¼ 1–2 nm, porosity ¼ 93.58%) film onto
Carbon Nanotubes (CNTs) cellulose fibers (Fig. 5a, b). The diameter and
thickness of the MWNT were three and two orders
CNTs were fabricated the first time by Iijima et al. of magnitude smaller than the diameters and
[60] and have now received considerable attention thickness of the cellulose fibers, respectively.
regarding their use in filters for airborne particles. Table 4 shows that with an increase in the
CNTs are classified as single-walled CNTs MWNT/cellulose ratio, the pressure drop sharply
(SWNTs) (normally df < 10 nm) and multi-walled increased. The pressure drop of cellulose filter II,
CNTs (MWNTs) (normally df > 10 nm) [60]. The consisting of five cellulose layers, was similar to
very small diameter of fibers indicates that flow that of the MWNT I, but the filtration efficiency
around the CNTs will be in the free pass flow and thus quality factor of the MWNT I were much
regime, where the disturbance of the flow by higher. It can be seen that MWNT II–IV with a
CNTs is not significant [47]. In comparison with filtration efficiency higher than 99.97% could be
electrospun nanofibers, CNTs provide high filtra- used in HEPA class filters, which require filtration
tion efficiency because of their ultrathin fibers, of 99.975% particles at the MPPS.
Airborne Nanoparticles: Control and Detection 99

Airborne Nanoparticles: Control and Detection, continuous MWNT film (1–2 mm thick, as seen in (c)) on
Fig. 5 SEM images of MWNT-coated filters. (a) Fibrous top of the cellulose layer. (Reprinted with permission [27])
filter morphology. (b) The cross-sectional view shows a

Airborne Nanoparticles: Control and Detection, Table 4 Characteristics of cellulose filters and MWNT-coated
filters. (Reprinted with permission [27]). Note: cellulose filter II consists of five cellulose layers in series
Coverage of
MWNTs Pressure drop after Filter efficiency for Filter quality for
Sample [mg cm2] filtration [kPa] dp ¼ 300 nm [%] dp ¼ 300 nm [kPa1]
Cellulose – 0.45 66.45 2.42
filter I
MWNT I 0.07 2.10 99.96 4.12
MWNT II 0.11 3.00 99.978 3.36
MWNT III 0.14 3.77 99.9976 3.56
MWNT IV 0.22 5.42 99.9994 2.75
Cellulose – 2.11 98.76 2.65
filter II

Free-standing SWNT films (FSFs), an excel- Fig. 6a. The nanotubes have 10 mm lengths and
lent example of air-filtering CNTs, were fabri- 1.3–2 nm diameters with a few micrometer’s
cated by Nasibulin et al. [61], as shown in thickness. Figure 6b shows the filtration efficiency
100 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, filter quality factor on the particle size for commercial
Fig. 6 (a) Set of images showing a submonolayer FSF filters and a 120-nm-thick SWCNT film. The solid and
suspended over 5 mm openings in aluminum foil. (b) open symbols show results obtained by two independent
Thickness dependence of transmittance and of collection measurement techniques, namely, scanning over the entire
efficiency for 44 nm g-Fe2O3 particles. (c) Flow rate particle size range studied and at fixed particle sizes.
dependence of pressure drop for 120-nm-thick SWCNT (Reprinted with permission [61])
films and various commercial filters. (d) Dependence of the

increased linearly as the nanotube was thickened. and are durable enough to capture nanoparticles
Figure 6c shows a lower pressure drop by FSF for study. It was also found from durability tests
filters, up to ~230 Pa, as compared to commercial that the filter was able to operate for more than
filters (500–4000 Pa) in various airflow rates, a month without a drop in the filtration efficiency
illustrating the high quality factor of the FSFs; at a flow rate of 300 cm3/min. The high surface
more than one order of magnitude is higher than area of the free-standing SWNT films can reason-
that of commercial filters (Fig. 6d). They noted ably explain their high filtration efficiency beca-
that the FSF have robust mechanical properties use of the related improvement of the filtering
Airborne Nanoparticles: Control and Detection 101

Airborne Nanoparticles: Control and Detection, as a function of pressure drop at 0.3 mm particle size and
Fig. 7 (a) SEM and (b) photographic images of the 10 cm/s face velocity. (d) Quality factor as a function of
three-layer CNT filter structure with a cross-ply geometry. particle size, ranging from 0.01 to 0.3 mm, at 10 cm/s face
(c) Particle penetration fraction of the different structures velocity. (Reprinted with permission [62])

mechanisms in the FMF regime. The low pressure CNT cross-ply filter met the HEPA filtration stan-
drop results from the high porosity and low thick- dard with a filtration efficiency of 99.98% for a
ness of the films. 300 nm particle size at 10 cm/s face velocity and
Yildiz et al. [62] prepared aligned CNT sheets also had the highest quality factor (Fig. 7d). They
by embedding them between polypropylene melt- noted that the performance of novel CNT filters is
blown fabrics. The diameters of the CNTs were comparable to electrospun fabrics, making them a
25–40 nm with lengths of ~1 mm and thicknesses viable option for future filtration applications.
of 20–25 mm (Fig. 7a, b). The test particles were After the development of CNT filters for air
10–300 nm. They found, as shown in Fig. 7c, that filtration applications, researchers have observed
the filtration efficiency of the fabricated filters dra- that the filters can become clogged by nanoparticles
matically increased with the number of CNT due to the smaller space between CNT films than
layers, while the pressure drop also increased. particle aggregates. To overcome the capacity-
They observed that while the pressure drop of the related issues, a hierarchical structure for CNT filters
seven-layer filter was very high, the filtration per- has been proposed. In a typical procedure, the CNT
formance should meet high-efficiency particulate films grow on a porous material. This structure not
air (HEPA) filter standards with an acceptable pres- only provides a macroporous structure and high
sure drop. Therefore, they laid the CNTs in a cross- mechanical strength, but also the specific surface
plied structure within the filter. The three-layer area of the filter structure increased.
102 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, particles after filtration testing. The inset shows NaCl par-
Fig. 8 (a) Penetration of particles with different sizes in ticles deposited on a single CNT (the black arrow shows a
the QF filter and the CNT/QF filter; (b) quality factor NaCl particle larger than 100 nm; white arrows show NaCl
versus particle size of the QF filter and the CNT/QF filter. particles smaller than 100 nm). (Reprinted with permission
(c) SEM images of the CNT/QF filter with deposited NaCl [63])

Li et al. [63] fabricated CNT/quartz fiber amount relative to that of the pristine QF, while
(QF) filter as a depth-type hierarchical structure the filtration efficiency increased significantly,
through in situ growth of CNTs on quartz fiber resulting in an overall increase of the quality fac-
(QF) filters using a floating catalyst chemical tor for the CNT/QF filters. Scanning electron
vapor deposition (CVD) method. They observed microscope images reveal that CNTs are very
the CNT/QF filter met the standard of high- efficient at capturing submicron aerosols (Fig. 8c).
efficiency particulate air (HEPA) filters (Fig. 8a, To prevent clogging and thus increase the
b). The specific surface area of the hybrid filter service life of the filters, Li et al. [63] created
was more than 12 times higher than that of the hierarchical CNT/quartz-fiber (QF) filters with
pristine QF filters. The pore size of the CNT/QF gradient structures where the content of CNTs
filter only has a small change. The pressure drop decreases exponentially along the thickness direc-
through the CNT/QF filter changed only a small tion of the filters. They observed that by using
Airborne Nanoparticles: Control and Detection 103

(a) 3.5 (b)


Aerosol pollutants 100
3.0
99.98

Efficiency at MPPS (%)


2.5
ΔPt/ΔP0

2.0 99.96

1.5
99.94
1.0
QF filter 99.92 QF filter
0.5 CNT/QF filter; CNT-rich side upstream CNT/QF filter; CNT-rich side upstream
CNT/QF filter; CNT-rich side downstream CNT/QF filter; CNT-rich side downstream
0.0 99.9
0 5 10 15 20 25 0 4 8 12
Time (min) Time (min)
Aerosol flow
(c)

a: CNT/QF filter with CNT-rich b: CNT/QF filter with CNT-rich


c: QF filter
side upstream side downstrem
QF fiber CNTs Aerosol particle

Airborne Nanoparticles: Control and Detection, versus filtration test time for the CNT/QF filter with differ-
Fig. 9 (a) The rate of pressure drop increase versus filtra- ent placement positions and the QF filter under continuous
tion test time for the CNT/QF filter with different place- aerosol loading. (c) An illustration of aerosols accumulat-
ment positions and the QF filter under continuous aerosol ing in the CNT/QF filter with different placement positions
loading; (b) the decrease in rate of efficiency at MPPS and the QF filter. Reprinted with permission [63]

only 1.17 wt % CNT, penetration through the while the service life of the composite oriented
gradient filter reduced the MPPS by one order of with the CNT-rich side upstream was only 41.7%
magnitude, where the pressure drop was only 6% longer.
higher than that of the pristine QF filter, resulting Zhao et al. [64] fabricated a novel multi-
in a higher quality factor for the gradient structure functional Ag@MWCNTs/Al2O3 hybrid filter
(Fig. 9a, b). As shown in Fig. 9c, they also tested with a depth-type hierarchical structure. This fil-
different placements of CNT inside the quartz ter achieved 99.9999% filtration for particles at
filter to investigate clogging and service life of 300 nm particle diameter. Ag@MWCNTs/Al2O3
the gradient filter. The service life of a composite had only 35.60% of the pressure drop of the
with the CNT-rich side downstream was up to pristine Al2O3 filter, leading to a high quality
64% longer compared to the pristine QF filter, factor.
104 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, and the CNTs/ACF. Coordinates in parentheses represent
Fig. 10 (a) SEM images of the CNTs/ACF. (b) PM filtra- the MPPS and associated filtration efficiency. (Reprinted
tion efficiencies and (c) quality factors of the pristine ACF with permission [65])

Yang et al. [65] have proposed growing CNTs devices in industry. A corona discharge was first
on an activated carbon fiber (ACF) filter support used to remove particles from an aerosol in 1824
using chemical vapor deposition in a form of by Hohlfeld; in 1907 Professor F. G. Cottrell
hierarchical structure. The design goal is to of the University of California Berkeley filed a
achieve high removal efficiencies with low pres- patent (US Patent 895729) for a device to charge
sure drop and thus a superior quality factor. particles and then collect them using electrostatic
Indeed, compared with recent CNT-based filter attraction. ESPs function by using electrop-
media, CNTs grown on ACF achieved high parti- horesis to separate charged particles from an
cle filtration performance with a very low pressure airstream.
drop, leading to a high quality factor. The results A Boltzmann distribution of charged particles
are shown in Fig. 10. exists in any gas, for example, charged particles
Nonetheless, in general, while CNT-based air and gas molecules and transient free electrons. At
filters have been used with successful results, high electric fields, the ions and free electrons can
in-depth knowledge, including their behavior in be accelerated to collide with gas molecules, lead-
industrial-scale applications is lacking (Table 5). ing to the ejection of additional electrons and
further ionization. The process creates a plasma
containing a large number of positive ions and
Electrostatic Precipitation free electrons in the gas. In a typical ESP, a corona
discharge is created at an electrode with a high
Electrostatic precipitators (ESPs), along with fib- positive potential which accelerates free electrons
rous filters, are the most common particle-control from the surrounding air. The role of the plasma is
Airborne Nanoparticles: Control and Detection 105

Airborne Nanoparticles: Control and Detection, Table 5 The filtration performance of CNTs
Air Filtration Quality
Particle velocity Pressure efficiency factor
Structure type Material size (nm) (cm/s) drop (kPa) (%) (Pa1) Study
CNT coating Cellulose fiber 300 11.5 2.99 99.9976 0.0035 [27]
Free-standing – 44 1.97 0.071 99.997 0.147 [61]
SWNT film
Aligned sheet Polypropylene 300 10 0.147 99.98 0.043 [62]
fabric
Hierarchical Glass fiber 100 20 0.080 33.3 0.13 [66]
Hierarchical Metal filter 300 20 0.7 80 0.002–0.004 [67]
Hierarchical Quartz fiber 100/300 6.21 0.840 99.9979/ 0.0129/ [63]
99.9974 0.0098
Gradient Quartz fiber 63.8 5.31 0.435 99.9959 0.02321 [68]
Agglomerate – 300 1.57 0.167 99.988 0.05406 [69]
structure
Hierarchical Al2O3 filter 300 0.5 4.65 99.9999 0.0029 [64]
Hierarchical ACF 100/300 6.21 0.01–0.6 96.35/97.40 0.1068/ [65]
0.1166

to increase charging of aerosol particles so they because their stability leads to better performance
can be removed using electrostatic force. ESPs (e.g., less arcing) and lower cost.
can also be operated in negative mode. The elec- In a negative mode operation, negative ions fill
trode is given a large negative charge and emits the space outside the corona and then collide with
electrons that attach to particles. Two main types particles, charging them negatively (Fig. 11d).
of collection electrodes are used in ESPs: flat The charged particles are driven onto the positive
plates and tubes (Fig. 11b). The typical space collector plates by an electrical field. Electrostatic
between the electrodes and the plates is charging of particles occurs via two mechanisms,
10–15 cm. Particles are separated from the gas bombardment charging (important for micron-
stream as it passes between them (Fig. 11a) sized particles) and diffusion charging
resulting in the formation of a particulate cake (important for submicron particles). When the
on the plates. Some systems include shakers or initial distribution has relaxed to equilibrium, the
hammers to clean the plates. In the tubular con- charge on the particles will be proportional to
figuration, which is more common for wet ESPs, particle surface area, i.e., dp2. As submicron par-
the discharge electrode is located at the center of a ticles (<0.1 mm) have significant diffusional
tubular collector electrode. The diameter of tubes motion, they will be charged significantly by dif-
can be 8–25 cm with a 1–4 m length (Fig. 11b). In fusional charging. Thus, ESPs are widely used to
this design, the discharge electrode is parallel to control submicron particles.
the gas flow [5, 70]. Table 6 shows many advantages and disadvan-
An electrical potential of ~4 kV/cm is used to tages of ESP technologies used to control
create the corona discharge, applied between the particles.
discharge and collection electrodes. Generally, the
wires are charged at 20–100 kV below ground
potential. In most cases a negative corona ESP Performance
(Fig. 11c) is more stable than a positive corona;
however, negative corona plasmas also produce Deutsch equation is a common description of
much more ozone which can be an unwanted particle collection efficiency (E) for monodisperse
byproduct. Negative coronas are typically chosen particles:
106 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, Fig. 11 (a) Commercial plate-type ESP (General1). (b) Tube-type
electrode ESP. (c) Corona formation in a wire and plate plan. (d) Particle charging [70]



oA equation (Eq. (14)) and Matts-Ohnfeldt equation
 ¼ 1  exp ð13Þ (Eq. (15)) build on the Deutsch equation:
Q

n
where o is migration velocity, A is the collector oA
 ¼1 1þ ð14Þ
electrode area, and Q is volumetric gas flow. It has nQ
been pointed out that Eq. (13) is for particles with
x
similar drift velocities and not for mixtures of oA
 ¼ 1  exp ð15Þ
particle sizes having different drift velocities. An Q
underlying assumption in the equation is that the
particles are permanently collected. where n is an empirical constant set at 3 to 5 and
The assumption works well when the collec- x is an empirical constant set at 0.5 based on
tion efficiency is low; for high collection effic- experimental data [70, 71].
iencies (> 99%), other mechanisms besides Various studies have shown that the collection
drift velocity dominate particle collection. efficiency for nanoparticles by ESPs is largely
Re-entrainment (from rapping and scouring), dependent on structural properties including
low electrical resistivity, and uneven flow through stages of collection, combination with other
the filter can limit collection efficiency leading to methods, choice of wet vs. dry ESP, discharge
particle collection slower than predicted with electrode positioning, type of collection elec-
Eq. (13). Empirical modifications to the equations trodes and so on, and specific collection condi-
have been made, to describe the behavior of ESPs tions including cleaning gas velocity, type, size,
with ultrahigh collection efficiency. The Hazen and concentration of particles.
Airborne Nanoparticles: Control and Detection 107

Airborne Nanoparticles: Control and Detection, Kim et al. [73] used a combined electrospray/
Table 6 Advantages and disadvantages of ESPs [71] ESP to enhance the collection efficiency of mono-
Advantage Disadvantage disperse nanometer-sized particles (Fig. 13). The
Easy operation for high- High initial cost combination enhanced the collection of particles
temperature gases, such as by 21–36% depending on the particle size and in
boilers and steel furnaces
addition reduced the energy consumption of the
Low pressure drop, Large footprint
reducing energy ESP.
consumption There are a number of technical challenges
High collection efficiency Suitable for combustible associated with collecting sticky and aggregative
if operated properly particles soft nanoparticles with a conventional ESP. Dey
Effective operation over a Longer chambers are et al. [74] have designed a positive mode charged
large range of particulate required for particles with
sizes high electrical resistivity
wet electrostatic precipitation (WESP) (Fig. 14a)
(>2  1011 ohm-cm), their to address them. The goal of their system is to
buildup on collectors collect soft nanoparticles including monodisperse
limits performance polystyrene latex (PSL), polydisperse sucrose,
Low operating and Some particles are slow to and stearic acid particles directly into liquid
maintenance costs if give up their charge when
designed and constructed they reach the positive media. The collection efficiency of WESP was
properly electrode plates. They 70–90% for particles of 80–600 nm diameter, in
create an insulating layer agreement with theoretical modeling, and
on the collectors, 40–70% for small particles of 20–80 nm diameter.
generating back corona
and reducing current flow The performance for these small particles was
Particles with low significantly lower than the theoretical estimate,
electrical resistivity cannot possibly due to incomplete neutralization of neg-
be held on the collector; ative charges during air-jet atomization.
thus re-entrainment can Figure 14b shows transmission electron micros-
occur
copy (TEM) images of aggregated nanoparticles
on a collecting plate for the dry ESP and non-
aggregated nanoparticles on the collecting plate
Zhuang et al. [72] have investigated the effect of of the WESP.
various operating conditions on the collection effi- An efficient wire-to-plate wet electrostatic pre-
ciency for nanoparticles in the range of 50–500 nm cipitator (WESP) for nanoparticles was designed
in a cylindrical (tubular) ESP. The ESP was oper- by Chen et al. [75], targeting submicron- and
ated in either one- or two-stage mode. It was found micron-sized particles emitted from semiconduc-
that collection efficiencies dropped as the corona tor manufacturing. A fixed voltage of 15 kV was
current decreased due to a too small drift effect for supplied by tungsten wire discharge electrodes to
particles toward the collection electrodes at high air produce the electric field and corona ions. Water
velocities (Fig. 12a). They also found that a lower mist at room temperature was used to quench the
electrical resistivity of particles caused a decrease high-temperature exhaust gas in order to enhance
in the collection efficiency owing to decreased particle condensation growth and improve the
attractive force at collector surfaces after deposi- collection efficiency of nanoparticles. The nano-
tion. Particles of NaCl and Al2O3 showed lower particle collection efficiency was 67.9–92.9%
conductivity and ion emission, resulting in poor without fine water mist, which increased to
corona current and thus a decrease in the collection 99.2–99.7% when the water mist was used
efficiency. The two-stage ESP had a higher collec- (Fig. 15a). As shown in Fig. 15b, the results are
tion efficiency than the one-stage ESP (Fig. 21a), in good agreement with the formula  ¼ 1 – exp
and for both ESPs the collection efficiency for (a (NDe) b + g, where a, b, and g are empirical
nanoparticles in the range of 70–100 nm was better regression coefficients determined from the
than for other sizes (Fig. 12a, b). experiment and NDe is the Deutsch number.
108 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, velocities in the two-stage ESP. (b) Collection efficiency
Fig. 12 (a) Collection efficiency of Al2O3 and NaCl of Al2O3 and NaCl particles as a function of size for a
particles as a function of size for two different gas single-stage ESP. (Reprinted with permission [72])

It has been noted [76] that partial charging of ESPs for nanoparticles decreases sharply as oper-
reduces the collection efficiency for nanoparticles ation time increases, because particles deposit on
smaller than 30 nm in a traditional wire-in-plate both the collection plates and high-voltage elec-
ESP. It is also known that the collection efficiency trode, reducing the electric field [76]. Therefore,
Airborne Nanoparticles: Control and Detection 109

which have a large effect on particle collection


performance, there are some important parame-
ters related to the composition of the gas stream
that greatly contribute to the collection efficiency
of ESPs. The velocity and particle concentration
of the gas stream are the most critical operational
parameters in these processes. Oliveira et al. [79]
separately evaluated the influences of residence
time (gas velocities) and concentration of nano-
particles on the performance of a conventional
ESP. They observed a decline in collection effi-
ciency with particle concentration and particle
Airborne Nanoparticles: Control and Detection, diameter (Fig. 17a). An increase in the gas veloc-
Fig. 13 The combined effect of electrospray and ESP on ity at a fixed particulate feed rate reduced the
particle collection efficiency. (Reprinted with permission collection efficiency, which was related not only
[73])
to the residence time but also to the gas-particle
concentration (GAC). To prevent the dilution
both the discharge and collection electrodes should effect due to increased velocity, they used a par-
be rapped frequently to remove deposited particle ticle injection method called aqueous solution
cake. However, rapping may not be practical for concentration (AQC), to quantify the effect of
smaller devices such as indoor air cleaners. Further- the residence time. Figure 17b shows the
more, cleaning the wires by water spraying is diffi- decreasing trend of the collection efficiency in
cult as it can cause arcing and current bridging this test.
between the wires and the collection electrodes Table 7 shows the collection performance of
[75]. Other problems related to traditional electrodes the previously described ESPs, as a function of
include particle re-entrainment [72], reverse corona structural properties and operational conditions.
[77], and ozone generation [5]. To overcome these
issues, Li et al. [78] developed a new wire-on-plate
ESP (WOPEP). Figure 16a compares the traditional Thermophoresis
and newer ESPs. In WOPEP, discharge wires are
attached directly to the surface of a dielectric plate, The movement of a particle due to an external
leading to reduced particle deposition on the wires force is called phoresis. Examples include heat
and reduced ozone generation while maintaining a (thermophoresis) and an electrical field
high particle collection efficiency. The authors (electrophoresis).
achieved collection efficiencies of 90.9–99.7% and A temperature gradient through an aerosol
98.8–99.9% in the particle size range of leads to a thermal gradient across the aerosol
30–1870 nm, at average face velocities of 0.50 m/s particles themselves. As illustrated in Fig. 18a,
(flow rate, 30 L/min; residence time, 0.36 s) and b, collisions with gas molecules on the high-
0.25 m/s (flow rate, 15 L/min; residence time, temperature side of the particle will have more
0.72 s). The experimental collection efficiencies energy than collisions on the cooler side. As a
were seen to be in agreement with the theoretical result, particles are accelerated toward the cold
models. A key finding was that the WOP ESP, at the side. Thermophoresis is not a strong mechanism
same voltage, has one to two orders of magnitude compared to the aforementioned methods; how-
lower ozone generation, and cleaner wires and ever, it can be applied in many aerosol-related
higher collection efficiency, compared to a tradi- fields such as nanoparticle filtration. The mass of
tional ESP (Fig. 16b). a particle depends on the volume or the third
Besides the various configurations of ESP power of radius, whereas the number of collisions
structure such as operation mode and voltages, depends on the surface area, which depends on the
110 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, applied on corona wire ¼ +4.2 kV and voltage applied on
Fig. 14 (a) Cross-sectional view of fabricated wet elec- collecting plate ¼ 3.5 kV). (Reprinted with permission
trostatic precipitator (WESP). (b) TEM images of particles [74])
collected in dry ESP (left) and WESP (right) (voltage

second power of radius. Therefore, this mecha- Researchers have studied this phenomenon
nism is more important for small particles than for both theoretically and experimentally [82–
large [70, 81]. Typical temperature gradients are 84]. Tsai and Lu [85] constructed a thermo-
on the order of 20,000 K/m; for UFPs this results phoretic precipitator to collect nanoscale particles
in thermophoretic mobilities on the order of and analyzed its performance. The system built by
Brownian mobilities [70]. Gonzales et al. [86] achieved near-complete
Airborne Nanoparticles: Control and Detection 111

Airborne Nanoparticles: Control and Detection, with fine water mist between the experimental data and the
Fig. 15 (a) Collection efficiency for a WESP with and present predictions (the applied voltage is 15 kV).
without fine water mist; the applied voltage is 15 kV. (b) (Reprinted with permission [75])
Comparison of particle collection efficiency for the WESP

Airborne Nanoparticles: Control and Detection, and after the particle-loaded collection plates were cleaned,
Fig. 16 (a) Schematic of the traditional WIP-EP and with an applied voltage of 18 kV and flow velocity of
proposed WOP-EP. (b) Collection efficiency of the 0.25 m/s. (Reprinted with permission [78])
WOP-EP and the WIP-EP at the initial clean condition

deposition of NaCl and Fe nanoparticles, for dis- Boddu et al. [82] reported a near-complete
tributions with mean diameters of 50 and 3.6 nm, filtration of carbon nanoparticles with a mean
respectively, in a particle flow below 15 mL/min. size of 60 nm at a mass density of 1  103 mg/
Particle filtration was homogeneous regardless of m3. They observed that the particle filtration per-
particle size. formance decreased to near 70% for 190 nm
112 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, m3, respectively, and (b) for gas velocities of 6.6, 8.2, and
Fig. 17 Grade efficiency vs. particle diameter (a) for a 9.9 cm/s, with KCl AQCs of 4.0, 5.0, and 6.0 g/l, respec-
gas velocity of 3.3 cm/s at different KCl AQCs of 0.2, 0.4, tively. (Reprinted with permission [79])
and 2 g/L with related GACs of 7.26, 15.55, and 45.78 mg/

Airborne Nanoparticles: Control and Detection, Table 7 The collection performance of ESPs
Air
Operation Operation Particles velocity/ Collection
Process mode stage size/nm cm/s Applied voltage/kV efficiency/% Study
ESP Wire-to- Single, 50–500 0.35 7.5 to 10 >90 [72]
tube two 0.7 >70
ESP Wire-to- Single 100–300 800 19.1 95-(~100) [73]
Electrospray plate 90–260 800 EHA(4 kV/cm)/ 70–80
+ESP ESP(16.2 kV)
WESP Wire-to- Single 20–80 – +4.2 40–70 [74]
plate 80–600 70–90
ESP-fine Wire-to- Single 30–8100 62–500 15 to 34 67.9–92.9 [75]
water plate 99.2–99.7
ESP + fine
water
ESP Wire-on- Single 30–1870 0.25 18 98.8–99.9 [78]
plate 0.5 90.9–99.7
ESP Wire-to- Single 10/250 3.3 8 ~100/~90 [79]
plate
ESP Wire-to- Single 10–30 1.7–6.6 4 kV/cm 90–100 [80]
plate 30–224 ~100

particles at 1.6  104 mg/m3 in a thermophoresis and so on. Most of the time, colliding particles
cell. Based on these studies, it can be concluded form an aggregate that coalesces; the process of
that thermophoresis is an effective strategy for coagulation changes the size distribution but not
capturing nanoscale particles [87, 88]. the mass density. From the perspective of nano-
particle control, coagulation is a mechanism that
could be used to shift material into a size range
Particle Coagulation that is easier to control with standard technolo-
gies. Katoshevski et al. have described using
Particles in an aerosol collide due to their differing coagulation for nanoparticle control [89]. The
relative velocities, due to thermal Brownian attractive interaction mechanisms between parti-
motion, electro- or thermophoresis, momenta, cles such as electrostatic, Van der Waals, and
Airborne Nanoparticles: Control and Detection 113

Airborne Nanoparticles: Control and Detection, Fig. 18 Mechanisms for thermophoretic (a) and diffusiophoretic
(b) motion of particles in the gas phase

Airborne Nanoparticles:
Control and Detection,
Fig. 19 Particle
concentration at the outlet
of the original pipe and the
coagulation pipe during 30 s
of measurement at an
engine load of 200 hp. at
1900 rev/min (engine
speed). (Reprinted with
permission [90])

reduction in surface tension drive the coagulation their local concentration and thus suppressing
of nanoparticles. Soot aggregates are one example the formation of new particles by nucleation.
of the result of such interactions. Mendelevich They concluded that using a well-designed coag-
et al. [90] have tested a geometric approach for ulation pipe in the exhaust system of vehicles will
clustering nanoparticles in transportation exhaust contribute to reducing the health effects associ-
systems in which the flow velocity across a pipe is ated with exposure to nanoparticles and will help
manipulated by design. They evaluated the ability vehicles qualify within the new EURO VI regula-
of coagulation to reduce the number of nano- tion framework.
particles as a function of engine speed by compar- Acoustic agglomeration is a promising tech-
ing the particle number at the outlet of the nologies for controlling aerosols, which has been
coagulation pipe relative to the PN of the original characterized by many researchers [73, 92–95].
pipe. Their results demonstrate that the nanopar- When sound waves travel through an aerosol,
ticle number is reduced significantly by coagula- particle mutual collision probability is enhanced
tion in the coagulation pipe (Fig. 19). The authors increasing aggregation. Different particle sizes are
noted that the nanoparticles probably joined larger affected differently by the pressure wave of
particles and that it is also possible to absorb sound, leading to different velocities and colli-
gaseous molecules into the particles, reducing sion. The newly formed particles in turn continue
114 Airborne Nanoparticles: Control and Detection

to collide and grow, leading to nonlinear growth. with decreasing particle size. Therefore, they
The acoustic agglomeration can be further suggested that a higher acoustic frequency be
enhanced by orthokinetic collision [96], hydrody- used for smaller particles. They found the lower
namic interaction [92], and Brownian agglomera- limit for producing an effect via that SPL is
tion [95]. Zu et al. [95] investigated an acoustic affected by the particle concentration and size
chamber for particle agglomeration (Fig. 20a); distribution – lowest effect SPL increases with
their model agreed well with the experimental lower concentration and smaller particle size.
results. The model found that there are many Their study indicated that improved acoustic
parameters that affect the process including parti- agglomeration can be achieved for a longer resi-
cle size, acoustic frequency, and sound pressure dence time of the particles in the agglomeration
level (SPL). The work showed that the collision chamber. SEM images (Fig. 20b) of the particles
efficiency between particles is increased for large before and after the acoustic chamber showed the
particles and for higher SPLs. In addition they formation of aggregations of particles.
observed that the optimal acoustic frequency for Despite a fair number of studies of this method,
enhancing collision, around 1000 Hz, increases it seems there are two main challenges that

Airborne Nanoparticles: Control and Detection, samples at the outlet of the agglomeration chamber: in
Fig. 20 (a) Experimental setup for acoustic agglomera- the absence of sound (left) and in the presence of sound
tion of particles. (b) SEM photographs of the particle (right). (Reprinted with permission [95])
Airborne Nanoparticles: Control and Detection 115

remain. Both the high noise level and high energy was found that more than 80% of particles were
consumption inhibit use in many cases. under the nucleation and Aitken mode ranges
Another system to enhance the agglomeration [100]. Table 8 presents a summary of the instru-
of nanoparticles was recently introduced by Zhao ments used to measure nanoparticles.
et al. [91]. They developed an effective pre-
treatment agglomeration system to reduce down-
stream problems related to UFPs. As shown in
Aerosol Particle Mass Analyzer (APM)
Fig. 21a, b, Zhao et al. used a simple method to
modify the flow in ducts in which two dampers
An aerosol particle mass analyzer (APM) was
(a batch flow duct to simulate indoor stagnant air)
developed by Ehara et al.; an APM instrument is
or one damper (a continuous flow duct to simulate
now commercially available from Kanomax
a continuous airflow being treated in a down-
(Model 3602). After charging particles in a bipo-
stream cleaner device) was installed. The particle
lar charger, the aerosol passes between two rotat-
number in the batch chamber was decreased by
ing coaxial cylindrical electrodes, which rotate at
73% over 30 min. It was found that the damper
the same angular velocity. Two forces, the centrif-
movement facilitated particle collision and
ugal force and the electrostatic force, affect the
agglomeration by increasing the flow oscillations,
particles passing between the electrodes. Only
in essence, by increasing turbulence. By fitting a
those particles for which the forces balance
damper with a cycle time of 1 s, the particle
move the length of the sizer and exit through an
capture efficiency of the downstream filters
annular gap. For a given radius of cylinders (r1,
increased from 36% to 48%. The particle size
r2), angular velocity (w), particle charge (q), and
distribution was found to be larger after the
the voltage between cylinders (V), the mass to
damper demonstrating the agglomeration of the
charge ratio of particles (mc) can be obtained
particles during the process (Fig. 21c).
from [5]:

qV
Nanoparticle Detection mc ¼   ð16Þ
r 2c o2 ln r2
r1
Experimental aerosol research dates back more
than 100 years ago when John Aitken built a For electrodes with the same angular velocity,
device to count dust particles in air [5]. Today unbalanced forces may occur in the APM. For
there are many techniques for detecting and char- example, particles located near the cylinder expe-
acterizing particles that use properties such as rience a larger centrifugal force and those near the
mass, optical absorption and scattering, impac- inner, a smaller centrifugal force. This can lead to
tion, and electrostatic and diffusional behavior to deposition of the particles on the outer and inner
yield information on the mass and number con- cylinders, respectively, even at the correct mass to
centration, and size distribution, of aerosol sam- charge ratio.
ples. In some cases the methods are used in Additional complications include loss of
combination. In an urban area, as shown in mass from particles (volatilization) or gain
Fig. 22, a majority of particles by number concen- (condensation), of water or other species,
tration are typically found in the nucleation and which is also in conventional filter-based
Aitken modes. The picture changes, however, if methods. Volatilization can be encouraged by
volume or surface distributions are considered. the pressure drop across the series of impactors.
Stanier et al. [98] and Woo et al. [99] reported The method also has a relatively slow time res-
that nearly 25%, 75%, and 90% of total urban olution [5]. To obtain the desired measurement
particle number are smaller than 10, 50, and including size distribution, mass concentration,
100 nm, respectively. Similarly, in another study and chemical characteristics of the particles, a
of particle distributions in five European cities, it tandem setup including an APM with a
116 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, (b) Schematic diagrams of a partial closed damper oscilla-
Fig. 21 (a) Schematic diagrams of agglomeration cham- tion in the chamber. (c) Comparison of particle size distri-
bers, (upper) for a batch process and (bottom) for a con- butions with and without a damper. (Reprinted with
tinuous flow process with downstream filters. permission [91])
Airborne Nanoparticles: Control and Detection 117

Airborne Nanoparticles: Control and Detection, APS/SMPS data set was collected during the ClearfLo
Fig. 22 (a) Number, (b) surface, and (c) volume distribu- Project and merged by the authors. (Reprinted with per-
tion for a typical urban background aerosol in North mission [97])
Kensington, London, during 24–29 July 2012. The

differential mobility analyzer (DMA, see Impaction


section “Electrical-Based Measurement”) is
widely used. A coupled DMA/APM is capable Since the development of impactors in 1860, many
of determining the effective density [117], size- impactors have been used in aerosol research
resolved mass information [101], specific sur- [103]. Cascade impactors such as the Andersen,
face area [118], dynamic shape factor [119], and Mercer, quartz crystal microbalance (QCM), Pilat,
fractal dimension [119] of an aerosol. The Berner, low-pressure impactor (LPI) (MOUDI),
Couette centrifugal particle mass analyzer and the electric low-pressure impactor (ELPI) are
(CPMA) is a similar technology, developed by commercialized versions [122].
Olfert and Collings [120] as a mass classifier Generally, a cascade impactor consists of sev-
similar to the APM. Unlike the APM, the CPMA eral stages where each stage has a porous micro-
applies an improved transfer function to the orifice plate and an impaction plate under it. As a
classifier using a stable system of forces. The particle-laden stream passes through the stages,
system has been used recently by Liao et al. particles are impacted and thus collected on the
[117] and Johnson et al. [121] to determine the plates. Because of inertia, larger particles are not
size-resolved effective density of rural ambient able to turn with the streamlines and impact due to
and cigarette smoke nanoparticles, respectively. their forward momentum. The geometry of the
118 Airborne Nanoparticles: Control and Detection

Airborne Nanoparticles: Control and Detection, Table 8 Instruments used to characterize nanoparticles
Particle
Commercial size range
Instrument model Measures (nm) Online Notes Reference
APM/DMA Kanomax Size-resolved 30< Yes Gives only mass [101]
(Aerosol Particle APM-3602 mass information
Mass Analyzer/ concentration The measurement not
Differential dependent on particle
Mobility size or shape
Analyzer)
QCM (Quartz CMI PC-2H Size-resolved 50–10,000 Yes Ideal for medium and [102]
Crystal mass lower concentration
Microbalance) concentration measurements down
to a few mg/m3
MOUDI (Micro- TSI Nano- Size-resolved 10–10,000 No 13 stages-offline [103]
Orifice Uniform MOUDI mass characterizing
Deposit Impactor 125R concentration Collects size-
(MOUDI) fractionated particle
samples for
gravimetric and/or
chemical analysis
ELPI (Electric Dekati ELPI+ Size-resolved 6–10,000 Yes High time resolution [104]
Low-Pressure mass Able to collect
Impactor) concentration samples for offline
analysis
Spherical particle
approximation
Laser Aerosol TSI 3340A Number size 90–7500 Yes Overcomes the [105]
Spectrometer distribution limitations of classic
(LAS) optical particle
analyzers
CPC TSI CPC Number 1–10,000 Yes High sensitivity for [106]
(Condensation 3750 concentration low variation of
Particle Counter) particle number
High time resolution
EAS (Electrical Airel EAS Number size 3–10,000 Yes Spherical particle [107]
Aerosol distribution approximation
Spectrometer)
SMPS (Scanning TSI 3938 E57 Mass and 1–500 Yes Better reliability and [108]
Mobility Particle with 3082 number size reproducibility of
Sizer) 1 nm DMA distribution measurements
classifier and Spherical particle
CPC 3750 approximation
EEPS (Engine TSI 3090 Mass and 5.6–560 Yes High time resolution [109]
Exhaust Particle number size (10 times per second)
Sizer) distribution Low sensitivity EEPS
which limits these
instruments to high
concentration aerosol
measurements such as
engine exhaust
measurements
Considerably lower
size resolution
compared to SMPS
Spherical particle
approximation
(continued)
Airborne Nanoparticles: Control and Detection 119

Airborne Nanoparticles: Control and Detection, Table 8 (continued)


Particle
Commercial size range
Instrument model Measures (nm) Online Notes Reference
FMPS (Fast TSI 3091 with Mass and 5.6–560 Yes High time resolution [110]
Mobility Particle 3082 1 nm number size (one time per second)
Sizer) DMA distribution Spherical particle
classifier approximation
FIMS (Fast – Mass and ~10–600 Yes High time resolution [111]
Integrated number size Spherical particle
Mobility distribution approximation
Spectrometry)
P-Trak UPC TSI 8525 Number 20–1000 Yes Measurement is based [112]
(Ultrafine Particle concentration on condensation
Counter) particle counting
Diffusion Battery TSI 3041 Size 0.8–100 Yes Compact and simple [113]
distribution It does not need
particle charging
NSAM AEROTRAK Average 20–400 Yes An NSAM provides a [114]
(Nanoparticle 9000 (mm2/cm3) total surface area
Surface Aerosol and total concentration of
Monitor) (mm2) surface particles deposited in a
area human lung
Underestimates the
geometric surface area
of particles >100 nm
The surface area
underestimated in
comparison with APM
and TEM
ToF-AMS (Time- Aerodyne Composition 40–1000 Yes Refractory particles [115]
of-Flight Aerosol C-ToF-AMS cannot detect
Mass
spectrometer)
(T or S) EM-EDX Tecnai G2 F20 Morphology, 10–1000 No It is possible to gain [116]
(Transmission or size, and information about
Scanning electron composition morphology and size,
Microscopy- composition
Energy Dispersive (elements and
X-ray) compounds), and
crystallographic

impactor can be varied to control the cutoff size of [103]. Some workers have used oil-coated sub-
particles that will pass. In the cascade, large par- strates [123] and porous substrates [124] to over-
ticles are trapped first followed by successively come the problem of particle bounce. Also, to
smaller particles that are separated in the terminal avoid the effect of humidity, Chen et al. [125]
stages. The size resolution of the instrument is suggested controlling the relative humidity
controlled by the number of stages. Among these (RH) of the incoming aerosol of the MOUDI.
systems, the MOUDI and ELPI have been used to Another issue is particle clogging in the nozzles
obtain a smaller cutoff allowing characterization because of long-term or high particle concentra-
of nanoparticles. Problems with cascade impac- tion sampling. This problem can increase the pres-
tors include particle bounce, overloading of parti- sure drop across the plates; thus, the nozzles need
cles on the impaction plate, and interstage loss to be cleaned periodically [122].
120 Airborne Nanoparticles: Control and Detection

The MOUDI have found more widespread use sensitivity and accuracy [5]. The main drawbacks
than low-pressure impactors because they are include a high probability of particle bounce due
equipped with a lower pressure drop-inertial filter to the high frequency of the electrode, which
for classifying nanoparticles, restricting loss of increases with particle size, and saturation at low
volatile species [122]. To facilitate much longer mass levels in which case the oscillation fre-
operations, a second class of MOUDI called quency does not undergo a significant change.
MOUDI-II was developed. This model, as Researchers successfully used a QCM to monitor
shown in Fig. 23a, uses internal motors to rotate the deposition of nanoparticles [6, 103, 122].
the impaction plates [103], which makes more
uniform deposition of particles on the impaction
plates, increasing the operational lifetime and Optical Measurement
reducing the probability of particle bounce.
The ELPI is an improved low-pressure impactor Two physical phenomena, light scattering and
in which particles are charged with a unipolar light absorption by particles, are the basis of
charger and the mass aerodynamic size distribu- optical-based characterization of particles. Of the
tions, with a time response below 5 s, are obtained two, light scattering has a larger application than
by using electrometers on the stages of a cascade extinction. In a light scattering-based device, an
impactor. However, Olfert et al. [126] noted that aerosol passes across a light beam (usually a laser)
the ELPI has a poor size resolution for submicron where light is scattered by particles and received
particles and that the sensitivity of the electrome- by a photodetector (Fig. 24). The photoelectric
ters limits the ELPI to high aerosol concentrations. pulse’s frequency determines the number, and its
Use of the QCM instrument was widespread in height gives the size distribution of the particles.
the 1980s and continues to be used for many The scattering phenomena are described by Mie
applications. In a QCM, electrically charged par- scattering theory for particles with diameter about
ticles impact a mechanically oscillating quartz equal to or larger than the wavelength of light and
crystal disk and then deposit onto an electrode Rayleigh scattering theory for particles with a
attached to the center of both sides of the crystal. diameter about equal to or smaller than the wave-
The resonant frequency of the disk decreases as length of light. Also, there are two approaches for
the particles collect on it (Df ¼ CDm). The light scattering, by single particles or by an assem-
changing frequency generates a signal that is pro- bly of particles. For a high-concentration particle
portional to the collected mass. Figure 23b shows flow, the ensemble techniques are appropriate,
a typical setup. One of the advantages of the QCM while single particle counters are suitable for mea-
is that it is a direct measurement with high suring low particle concentrations [5].

Airborne Nanoparticles: Control and Detection, Fig. 23 (a) 125 nano-MOUDI II with internal motor rotation and
(b) typical schematic of a quartz crystal microbalance
Airborne Nanoparticles: Control and Detection 121

behavior, and it will change the particles them-


selves. A charged particle will have different rates
of growth and evaporation relative to a neutral
particle. A similar problem can occur in the mass
spectrometric analysis methods. In addition, Wang
et al. [130] found significant diffusional deposition
of nanoparticles at the bends or elbows of instru-
ments, which may distort results. Therefore,
recently, Bauer et al. [129] introduced a new tech-
nique called synchrotron small-angle X-ray scat-
Airborne Nanoparticles: Control and Detection, tering (SAXS) in which high-intensity X-ray
Fig. 24 Optical scattering system of a double-lens laser beams from synchrotrons make it possible to mea-
diffraction instrument. (6) The laser light, (2,4) lens, (3) the
sample cell, and (1) the forward-scattering detectors, and sure nanoparticles directly in the gas phase, over-
(5) backscattering detectors. (Reprinted with permission coming the drawback. By comparing the results
[127]) with those of a differential mobility particle sizer
(DMPS) operated in parallel, they could show that
A great deal of research and development is built the SAXS method is able to measure the primary
on using the patterns of light scattering for particle particles and the aggregates, whereas the DMPS
characterization. A partial list includes forward- measured only aggregates. They noted that in situ
scattering spectrometer probe (FSSP-100) direct nanoparticle measurement at ultralow vol-
(Knollenberg 1981) and FSSP-300 (Baumgardner ume fractions of ~1010 is feasible with SAXS
1992), 90 White Light-Scattering Analyzers under atmospheric conditions.
(Umhauer 1983), Particle Counter Sizer Velocimeter Nanoparticles have an extremely low polariz-
(PCSV) (Holve and Self 1979a), Laser Doppler ability because of their ultra-small size and are
Velocimetry (LDV) visibility based (Post 1978), therefore difficult to detect by light scattering-
Phase Doppler Particle Analyzer (PDPA) (Bachalo based techniques [127]. There are physical limits,
and Houser 1984), and Particle Dynamics Analyzer for example, when comparing the wavelength of
(PDA) (Saffman 1984). Single particle counters have visible light (ca. 500 nm) with the size of nano-
some important limitations including collection effi- particles (e.g., 20 nm). Therefore, despite
ciency and noise/poor counting statistics at low con- advances with commercial optical particle coun-
centrations, the Rayleigh effect for gas molecules, ters to maximize the collection of scattered light,
and saturation at high particle concentration due to their performance for nanoparticles is not satisfac-
coincidence and dead time. Researchers have devel- tory. Furthermore, optical devices determine par-
oped some solutions to address these limitations. It ticle size based on the scattered light intensity.
has been found that, overall, small particles scatter Although this method is faster than other tech-
light at a larger angle, while larger particles scatter at niques, variations in the refractive index of parti-
a smaller angle. Therefore, forward scattering and cles with the same size, which depends on the
side scattering are not sufficient to characterize light morphology and chemical composition of the par-
scattered from nanoparticles. Arakawa et al. [128] ticle, will always cause variations in the scattered
used a collimated light beam in a vacuum sample cell light intensity [131].
to reduce the Rayleigh effect from air molecules,
enabling the detection of smaller particles.
Bauer et al. [129] noted that the nanoparticle Condensation Particle Counter (CPC)
measurement methods all remove the nanoparticles
from their original environment, and the particles Since the size distribution that can be determined
will rapidly change in response to the new envi- from optical techniques is not reliable for particles
ronment. For example, charging particles, such as with a diameter below 100 nm, aerosol science
in the charging stage of a DMA, will change their had to find a new approach. The condensation
122 Airborne Nanoparticles: Control and Detection

particle counter (CPC) is a widely used optical Incorporated). In a common application, a CPC
instrument capable of characterizing aerosols. The is used in tandem with a differential mobility
method involves three steps: (I) generation of a analyzer (DMA) or a diffusion battery as a detec-
supersaturation of water vapor or another working tor to determine the size-resolved number
fluid, (II) growth of particles by condensation of concentration.
the vapors, and (III) the optical detection of the Operational conditions such as aerosol flow
enlarged particles, by counting individual pulses rate, saturation rate, pressure drop gradients of
of scattered light (Fig. 25). Condensation tech- the flow paths, the temperature difference
niques were used the first time by John Aitken between saturator and condenser, type of working
(1888) on atmospheric aerosols [5]. Several fluid, etc. affect the detection efficiency of com-
models of CPC designed to detect particles within mercial CPCs. A number of researches have
the range of 1 nm to 10 mm have been developed looked into some modifications of CPCs in order
and commercialized by TSI (Thermo-Systems to enhance their use for aerosols with diameters

Pressure
Across Orifice
ΔP Critical Orifice
(1.0 L/min)

External Heated
Vacuum Optics
Fitting (40°C)
Focusing Collecting Lenses
Lens

Laser
Diode

Collimating Lens Photodetector


Cooled
Condenser Pressure
(22°C) ΔP Across
Nozzle

Water Filter Liquid-soaked


Removal Wick
Pump Heated
Saturator
(39°C)
Liquid
Drain Reservoir
Bottle
Sample lnlet
(1.0 L/min)

P Ambient Pressure

Airborne Nanoparticles: Control and Detection, Fig. 25 Flow schematic of TSI Model of 3772 CPC. (Reprinted
with permission [132])
Airborne Nanoparticles: Control and Detection 123

below 2 nm. Recent studies have shown that by in section 4, when a particle charged by a corona
modifying the operating conditions of, e.g., the or gas phase ions is exposed to an electric field, it
TSI 3025A [133], TSI 3772 [134], TSI 3025 migrates at a velocity that depends on its size and
[135], and TSI 3010 [136], detection of sub-2 nm morphology. A particle’s motion is described by
particles is possible, with high detection effi- the balance between the applied electrostatic force
ciency. The studies commonly focus on modify- and aerodynamic resistance (drag). The forces on
ing the temperature difference between the nanoparticles are made sufficiently high to over-
saturator and the condenser tube [133] and work- come diffusional effects, yielding high-resolution
ing fluids [137]. These operational conditions sizing. The determination of the size distribution
strongly affect the probability of the condensa- of an aerosol using these devices requires knowl-
tional growth of the smaller nanoparticles. edge of the charge distribution of the particles,
i.e., the charge number on particles with a given
diameter [5].
Particle Electrical Mobility The differential mobility analyzer (DMA),
introduced by Knutson and Whitby [138], is the
The method of determining the size distribution of main class of electrical mobility instruments. The
an aerosol using particle’s electrical mobility was fundamental principle of this technique is shown
introduced about 120 years ago. Electrical mobil- in Fig. 26a. The DMA is a cylindrical classifier in
ity is perhaps the best and most widely used which particles are charged by colliding with a
technique for measuring ultrafine particles. As cloud of ions produced by a unipolar high voltage
mentioned above, there are significant obstacles central rod (corona electrode). Particle trajectories
toward using optical techniques for the high- then deviate radially from the airstream depending
resolution characterization of nanoparticles due on their size, toward the outer collection electrode.
to weak light scattering by small particles, smaller The applied voltage of the corona can be varied
than the wavelength of light. However impaction between 0 and 5 kV. A particle-free sheath flow
methods, e.g., MOUDI, can use pressures below passes through the cylinder. Each ring collection
atmospheric to collect such particles. Over the last electrode is connected to an electrometer for mea-
few decades, the electrostatic force has been suring the number of particles and their currents
exploited for sizing nanoparticles. As mentioned which is related to the particle size.

Airborne Nanoparticles: Control and Detection, Fig. 26 (a) Schematic of a typical DMA. (Reprinted with
permission [139] and (b) SMPS DMA [5])
124 Airborne Nanoparticles: Control and Detection

The scanning mobility particle sizer (SMPS), distribution and lower concentrations for NaCl aero-
now the most common type of mobility analyzer, sols, while for diesel soot, it showed a broader
was developed by Wang and Flagan [140] and distribution and higher concentrations, relative to
commercialized by TSI in 1993. The SMPS system the TSI instruments. The authors noted that this
has three key components: the bipolar particle difference was probably due to the different particle
charging chamber, the DMA, and the CPC. Bipolar morphologies or particle size-dependent effects. The
charging is applied in the charging chamber to SMPS recorded consistent results for both particle
create a Boltzmann distribution of charges on the sources. In addition, they found that the FMPS
particles. The charged particles then enter the underestimated the nanoparticle size distribution
DMA from near the outer electrode. Figure 26b by approximately 15% compared to the SMPS.
shows a DMA used in commercial SMPS systems. The Grimm SMPS found broader distributions and
The particles, depending on their charge, are higher concentrations than the TSI instruments. In a
attracted or repelled by the central electrode; the similar study comparing the performance of an
voltage on the electrode may be varied. Particles EEPS with a CPC and an SMPS, Johnson et al.
will thus experience a force depending on their [109] found that the particle number measured by
electrical mobility. Particles with a high mobility the EEPS was 50% higher than that measured by the
are quickly deposited on one of the electrodes CPC. For size distributions the number concentra-
(depending on polarity). Only particles within a tion measured by the EEPS was less than the SMPS
narrow, tunable range of mobility reach the extrac- for particles larger than 80 nm, in agreement with
tion port at the end of the chamber. These selected the results obtained by Asbach et al. [144]. In
“monodisperse” particles are then introduced to the another study the determinations of an FMPS and
CPC to measure their number concentration. an SMPS did not have a significant difference in
The DMA applies voltages to tune the mobility their size distributions below 200 nm, but for larger
range, and the voltages are scanned to obtain a sizes, the FMPS delivered unreliable results [145].
size-resolved number concentration. The SMPS is An important disadvantage for fast-sizing
often selected as a reference method in aerosol instruments is the low electrometer sensitivity
research. In a classic SMPS program, a scan for high particle concentrations [141]. Also, the
takes 1 min or longer, introducing a risk that the broad unipolar charge distribution used in these
particle size distribution of the source could electrometer-based analyzers means that they
change during the course of a single scan have a lower resolution than the SMPS [126].
[141]. Trostl et al. [142] have obtained a rapid The development of a new class of device called
scan time of 3 s with a precision of 3% using a fast integrated mobility spectrometry (FIMS)
newer model of SPMS (TSI 3082). However, the described by Kulkarni et al. [146] may eliminate
scan range was limited to 2.21–60.4 nm. The the need for voltage scanning and increase the time
newest model of these instruments (TSI 3839) resolution of the classic SMPS. As described by
provides the scan time of ~15 s. Kulkarni et al. [146], in a FIMS, particles are
Nano-sized particle size distributions can also be charged and electrically separated into different
measured using more rapid instruments such as the streamlines. The separated particles are introduced
Engine Exhaust Particle Sizer (EEPS, TSI 3090) into a condenser and grow into larger droplets. The
[143], which uses a design based on the electrical droplets are subsequently exposed to a pulse of
aerosol spectrometer (EAS) [107], and the Fast laser light and their image captured by a CCD
Mobility Particle Sizer (FMPS) (TSI 3091) array. The images are processed to determine the
[110]. The time resolutions for the FMPS and the number of particles and the particle distance from
EEPS are 1 and 10 Hz, respectively. While the the electric field, which directly depend on particle
EEPS has been designed for engine emissions, mobility. Counting the particles as a function of
both can be used for industrial measurements [143]. their mobility means that the FIMS is able to mea-
Asbach et al. [144] compared the performance of sure the number size distribution of particles at a
two TSI SMPS, one TSI FMPS, and one Grimm comparatively impressive time resolution, much
SMPS. The FMPS measured a more narrow faster than a classic SMPS. The ability to detect
Airborne Nanoparticles: Control and Detection 125

single particles with the FIMS allows it to measure connected to electrometers. These electrometers
distributions with a higher signal/noise ratio than quantify current signals that are proportional to
for electrometer-based instruments [146]. the number of particles collected on the plates
With the exception of a few portable detectors, [149]. The structure allows the detection of single
e.g., the NanoScan SMPS (TSI 3910), commer- particles over a wide range of mobilities.
cial mobility analyzers are heavy, large, costly, The equivalent aerodynamic diameter is only a
and complex. Some of the research goals such as good approximation for spherical particles; this
personal exposure monitoring, deployment on fact limits the performance of any mobility-
small aircraft, and spatial gradient mapping, based analysis method.
which require an array of sensors in the urban
environment, cannot be approached with current
tools. This need has driven research on newer Particle Diffusion Mobility
approaches for the particle mobility analyzer.
These instruments include the opposed migration The diffusion battery is a simple and well-
aerosol classifier (OMAC) [147], cross-flow ion characterized diffusion-based aerosol classifica-
mobility spectrometer (CIMS) [148], and a mini- tion method that is free from some of the limita-
ature electrical-mobility aerosol spectrometer tions of the techniques discussed so far. Diffusion
(MEAS) [149]. The OMAC is similar to a DMA batteries were developed to describe aerosols
in that the opposing forces of aerodynamic drag according to their diffusional mobilities
and electrostatic force are used to sort particles [150]. The diffusion battery is a versatile, com-
into size bins. Particles of too-high and too-low pact, and simple system that can be easily cleaned
mobility are deposited on the porous electrodes; after use and does not require particle charging.
only those particles with an electrostatic migration A diffusion battery comprises a stack of screens
velocity that balances the flow velocity can pass. and air is sampled at different stages of the flow.
The system uses an applied voltage of ~1 V, much The aerosol is passed through the screens, and
lower than in a conventional DMA that would use small particles with a large diffusion constant are
a potential difference of ~30 V at the same flow more likely to deposit; the particle diameter can be
rate. Also, the OMAC is much smaller than a derived from the particle size-dependent deposi-
DMA because the distance between electrodes is tion rate. The technique is one of a few methods
only 1 mm for the same operational condition. that can measure nanoparticles down to 0.8 nm,
The CIMS consists of a number of channels i.e., a cluster of just a few molecules. To achieve
between parallel plates that are 1 mm apart. The the size-resolved concentration of nanoparticles,
charging electrodes are located at the edge of the diffusion batteries are often accompanied by a
channel so that particles, after passing through CPC, but this combination limits its use as a
these electrodes, migrate across the channels personal monitor [151]. Diffusion battery systems
with the sheath flow air. While high concentra- have been made in several designs. Wire screen
tions of particles may not be suited for batteries are most commonly used to determine
electrometer-based tools (FMPS, EEPS), the size distributions. Diffusion mobility-dependent
CIMS showed a good performance for measuring size distributions have been used in countless
high-mobility gas ions and/or nanoparticles, at studies (see, e.g., [113, 151–154]).
high concentrations. The MEAS is a bipartite
rectangular chamber containing an electrostatic
precipitator and a classifier. Particles are charged Measurements of Nanoparticle
in the electrostatic section and subsequently Composition and Morphology
injected into the classifier region with a narrow-
range streamline at the desired location. The Measurements of the composition and morphology
charged particles are then separated based on of airborne nanoparticles central to determinations
their electrical mobilities and collected on plates. of pollution sources, toxicity, and atmospheric
The plates are located inside of classifier and are behavior. The most common techniques are
126 Airborne Nanoparticles: Control and Detection

aerosol mass spectrometer (AMS), scanning elec- intracavity laser vaporizer (1064 nm), along with
tron microscopy (SEM), and transmission electron a common resistively heated tungsten vaporizer.
microscopy (TEM). They showed that the laser vaporizer could mea-
An AMS designed and developed by Aero- sure both the refractory and non-refractory
dyne Research, Inc. (ARI), is used worldwide to components.
determine the size-resolved mass concentrations SEM is a microscopic method that probes a
of non-refractory aerosol. At first, the Aerodyne sample with an electron beam and can be used to
AMS was useful for measuring the ensemble characterize the morphology and to some extent
average data of the composition of the mass size the composition of nanoparticles deposited on a
distributions of fine particles with aerodynamic conductive substrate. A typical SEM includes the
diameters of ~50–1000 nm, based on a quadru- electron column, scanning system, and detectors.
pole mass spectrometer [155]. With time the sen- The electron column operates in vacuum and con-
sitivity and time resolution of the AMS were sists of an electron gun and electromagnetic
developed along with its ability to analyze single lenses. A sample is introduced into the column
particles, along with a shift to time-of-flight and is irradiated by a beam of electrons generating
(ToF)-AMS which provide higher mass resolu- secondary electrons (SEs), backscattered elec-
tion. The instrument has three main sections: the trons (BSEs), and X-rays [158]. Generally, the
aerosol inlet (particle beam generation), the parti- secondary electrons are produced by inelastic
cle size discrimination chamber, and the compo- scattering, while backscattered electrons are
sition measurement chamber. Fine particles are caused by elastic scattering of the electrons by
focused into a particle beam by an aerodynamic the sample. Normally secondary electrons have a
lens in the entrance section and then pass through low energy, ca. 50 eV. These electrons are ana-
a sizing chamber. After that, the beam enters the lyzed, for example, using an Everhart-Thornley
particle composition detection chamber where detector with a scintillator/photomultiplier sys-
particles reach a hot surface (~600  C) causing tem, yielding topographic information about the
them to vaporize. The chemical composition of sample. For SE images, the edges of the sample’s
the vapor is determined by electron impact ioni- elements are usually brighter, due to the intensity
zation (EI) and mass spectrometry [156]. of electron emission. The generation of back-
Previous studies have shown the technique can scattered electrons is related to the atomic number
be used to measure the size-resolved mass com- of the elements in the sample with higher atomic
positions of particles [115, 155–157]. Jimenez at number giving a brighter image, providing a
al. [155] used a ToF-AMS for the study of atmo- rough elemental analysis especially for heavier
spheric fine particles. This study determined the elements. Backscattered electrons are generated
size-resolved mass composition ratios and chem- at depths of 0.5–1 mm, and thus the spatial reso-
ically resolved mass distribution for atmospheric lution of the images is less than for secondary
fine particles. Also, they observed that mass con- electrons. The backscattered electrons can be
centrations of sulfate and nitrate measured with detected by scintillator and solid-state detectors.
the AMS agree with those measured by ion When secondary electrons are produced by the
chromatography-based instruments. TOF-AMS interaction of the electron beams and the sample
has been developed by Su et al. [157] to measure atoms, holes are left in the inner shells of the atom.
fine and ultrafine particles, specifically particles X-rays are emitted when outer shell electrons
measuring less than 100–300 nm in diameter. The relax into the vacancy. The frequencies of light
aerodynamic size of the particles is determined are characteristic for specific elements and even
using light scattered as the particle passes through contain information about their chemical binding.
two continuous-wave laser beams. Onasch et al. For technical reasons, these characteristic X-rays
[115] used a soot particle AMS (SP-AMS) for the are analyzed for all elements except hydrogen and
physical and chemical characterization of black helium. The X-rays are detected by either EDS or
carbon. The SP-AMS is equipped with an wavelength dispersive spectroscopy. In an SEM,
Airborne Nanoparticles: Control and Detection 127

Bremsstrahlung X-rays (continuum or back- capacity, and energy use. There is an inevitable
ground X-rays) also can be produced by the decel- trade-off between purification performance and
eration of the primary beam electrons by the economic and technical feasibility. As a conse-
electric field of the nuclei of the sample atoms. quence, there is a continual desire to develop
An FESEM (field emission SEM) is an SEM more appropriate and advanced methods. Filtra-
optimized for operation at a low energy range tion of nanofibers and nanotubes, with the lowest
(<5 kV), using an electron gun that produces a possible pressure drop, may be possible by
low- and high-energy electron beam. This kind of designing the arrangement of nanofibers or by
operation produces high resolution and also using the high-performance monolayers.
enables scanning at low potentials [159]. The most common and commercially success-
Transmission electron microscopy (TEM) can ful nanoparticle-measuring techniques have been
be used to characterize nanoparticle size, mor- reviewed. Based on the available literature, the
phology, chemical composition, crystallinity and field of nanoparticle measurement has important
structure, thermal volatility, and mixing state, gaps including development of new techniques
because of its resolution down to fractions of a better suited to different environmental conditions,
nanometer. A TEM is very similar to an SEM. In improving the sensitivity of electrometer-based
TEM, the objective lens is placed after the sample instruments and the response time of charging-
area in order to image electrons that have been based instruments and addressing inability to suc-
transmitted through the sample. These electrons cessfully use light-based and mass-based tech-
may have been scattered (elastically or niques. As always, it would be desirable to have
inelastically) or transmitted (without any interac- instruments that are smaller and more robust.
tions with the sample atoms). If the sample area is
thicker, fewer electrons are transmitted and the
images will be darker; thus, a thinner sample
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proxy for general indoor air quality including
Indoor Air Quality: Status and bioeffluents. Continued exposure to CO2 levels
Standards over 2500 ppm have been linked to drowsiness
and tiredness. Studies have shown impacts on
Freja Hasager1, Joachim Dithmer Bjerregaard1, decision making and focus from around
James Bonomaully2, Hasse Knap2, 1300 ppm [1].
Alireza Afshari3 and Matthew Stanley Johnson1,2 Carbon Monoxide (CO) CO is a product of
1
Department of Chemistry, University of incomplete combustion. Indoor sources include
Copenhagen, Copenhagen, Denmark heaters and stoves, tobacco smoke, and candles.
2
Airlabs, Copenhagen, Denmark CO is toxic to humans. Ambient air contains
3
Danish Building Research Institute, Aalborg about 1 ppm of carbon monoxide. In busy
University Copenhagen, Copenhagen, Denmark streets, the atmospheric mole fraction can be in
the range of 10–20 ppm. Indoor levels generally
follow outdoor levels except in poorly venti-
Article Outline lated houses with indoor CO sources [2].
Formaldehyde (CH2O) CH2O is a volatile
Glossary organic compound that is found in indoor air
Definition due to off-gassing from building materials
Introduction containing adhesives and polymers and objects
Biological, Physical, and Chemical Sources of like furniture and fabrics. It is also formed from
Pollution the oxidation of hydrocarbons; in the indoor
Deposition of Pollutants environment, this includes cigarettes and
Ventilation Systems in Buildings ozonolysis of aromatic hydrocarbons. Indoor
In Situ Chemistry concentrations depend on the age of the build-
Indoor Air Quality and Health ing and vary depending on season and time of
Remediation Methods day. CH2O is known to cause adverse health
Sustainable Buildings effects in humans. According to the World
Future Directions Health Organization’s guideline for formalde-
Bibliography hyde, exposure should not exceed 0.1 mg/m3
(30-min average) [3].
Glossary Ventilation Systems Ventilation can be effectu-
ated by mechanical or by natural means. In
Aerosol A suspension of particulate matter com- mechanical ventilation, fans are used to venti-
posed of solid and/or liquid material in a gas. late an enclosed space, while natural ventila-
Carbon Dioxide (CO2) CO2 is a part of the tion is dependent on the outside conditions and
atmosphere (>405 ppm), and indoor concen- is driven by natural forces.
trations in excess of ambient are mainly gener- Because modern buildings are becoming
ated by people, about a kilogram per day more well sealed (more impenetrable), ventila-
depending on metabolism. The indoor expo- tion or air exchange rates between indoor and
sure limit is commonly taken as 1000 ppm, a outdoor air have decreased. This improves ther-
level at which the negative health effects of mal efficiency, but contaminants from indoor
CO2 are not yet significant. CO2 is a useful sources will be trapped inside resulting in ele-
vated pollutant concentrations that can cause
Freja Hasager and Joachim Dithmer Bjerregaard adverse health effects in the occupants. It is
contributed equally. now recognized that an optimal balance between
© Springer Science+Business Media, LLC, part of Springer Nature 2021 135
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_1097
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2019, https://doi.org/10.1007/978-1-4939-2493-6_1097-1
136 Indoor Air Quality: Status and Standards

energy conservation and indoor air quality Ventilation Rate The flow of outdoor air into a
(IAQ) must be maintained to provide the occu- space resulting in removal or dilution of indoor
pants with a healthy indoor environment. CO2 air pollutants. Given in units of volume
can be used as general indicator of indoor air per time or air exchanges per hour.
quality (IAQ) and ventilation rate, as low ven- Volatile Organic Compound (VOC) Volatile
tilation rates will cause the accumulation of organic compounds (VOCs) are organic
CO2 as well as other pollutants. CO2 sensors chemicals that have a high vapor pressure
are often used in demand controlled ventilation (boiling point below 250  C) at room temper-
to control bioeffluents from humans. A stable ature. There are many VOCs, both natural and
level of 850 ppm of CO2 should be sufficient man-made, including most scents and odors.
for a healthy indoor environment and could be Many VOCs are regulated by law due to their
provided by a ventilation rate of 10 l/s per health impacts [4].
person.
Particulate Matter (PM) Particulate matter is a
conglomeration of molecules in the liquid and/or Definition
solid phase occurring, together with gas, in an
aerosol. PM is typically characterized according Humans have practically become an indoor spe-
to mass and aerodynamic diameter. PM10 is cies, spending up to 87% of their time in build-
defined as the total mass density (mg/m3) of all ings. The technosphere has thus become the most
particulates with an aerodynamic diame- important environment when it comes to air pol-
ter  10 mm, PM2.5 is a measure of all particu- lution exposure. Following the oil crisis in the
lates with an aerodynamic diameter  2.5 mm, 1970s, buildings have become better sealed, in
and ultrafine particles (UFP) are particles with an order to minimize energy use. This development
aerodynamic diameter  0.1 mm. led to lower ventilation rates, and accumulation of
Primary and Secondary Pollutants Primary indoor air pollution. Strategies have been
pollutants are pollutants directly emitted from implemented to ensure sufficient indoor air qual-
a source. Secondary pollutants are formed in ity for people in buildings. This chapter gives an
situ from primary pollutants. overview of indoor air pollution – its sources,
Sick Building Syndrome (SBS) A situation in sinks, health effects, and remediation methods.
which people who spend time indoors feel
unwell and suffer from symptoms including
throat irritation, difficulty breathing, runny Introduction
nose, sneezing, headache, dizziness, difficulty
concentrating, and nausea. The severity of Shelter is one of humanity’s most basic require-
symptoms often increases with the amount of ments and our species is unique in having mas-
time spent in the building. tered the use of fire for heat and cooking food. The
Technosphere The technosphere is the part of first people to discover that indoor air quality
the environment modified by technology and matters were probably the cave dwellers.
includes buildings, vehicles, and public infra- Research shows that cave dwellers addressed the
structure like the subway and highways. problem by placing their fires at the entrance, to
Humans spend the majority of their time in increase ventilation of smoke [5]. In the modern
the technosphere. world, people spend the majority of their time
Terpenes A class of hydrocarbons of biological indoors; at work or at home. According to one
origin with a skeletal structure derived from study, up to 87% of our time is spent indoors,
isoprene. Of particular concern in the indoor which makes the technosphere the key environ-
environment are monoterpenes like pinene, ment in terms of pollution exposure; modern man
limonene, linanool, and menthol, used as is basically an indoor species [6]. Even though we
scents, e.g., in cleaning agents. spend this amount of time indoors, many studies
Indoor Air Quality: Status and Standards 137

show that people rate the risk of poor air quality uniform throughout the world. In some cases
from outdoor sources higher than indoor sources. they are not enforced, or they may not exist. In
Homo sapiens evolved a particular gene in the addition, up to 90% of people in developing coun-
aryl hydrocarbon receptor that makes us less sen- tries rely on coal and biomass for their domestic
sitive to environmental pollutants including energy. These fuels are typically burned inside,
smoke from fire. This gene occurs uniquely in which means that IAQ is a much bigger concern in
humans and is not found in closely related species developing countries, as this results in high indoor
like Homo neanderthalensis. Researchers believe concentrations of pollutants [11].
that the ability to gather around a fire for cooking This state-of-the-art review article gives an
and heating gave Homo sapiens this relative overview of different types of indoor air pollutants
advantage [7]. Paradoxically, the World Health as well as their sources and sinks, in situ chemis-
Organization (WHO) has determined that nearly try, and their health impacts. Remediation strate-
four million people die each year due to indoor air gies are also assessed, as well as sustainable
pollution, largely by pollution from fires used for building practices.
cooking and heating [8].
While much research has been done on outdoor Residential Air Pollution
air pollution, indoor air pollution has not received Exposure to indoor air pollution is especially
the same attention; prior to the mid-1970s, the problematic in areas that may combine poor ven-
level of interest was very low. The oil crisis in tilation, lack of building standards and enforce-
the 1970s resulted in buildings becoming better ment, and indoor pollution sources including fires
sealed and insulated to reduce heating expenses, for cooking and heating. People in the developing
leading to accumulation of indoor air pollutants. world rely heavily on in situ generation of energy
The term sick building syndrome (SBS) was for their daily activities. In 2012, the WHO stated
coined by the WHO in 1986. At that time, the that over 1.6 million people died of causes attrib-
WHO estimated that 10–30% of new office build- utable to household air pollution in South-East
ings had poor indoor air quality. Symptoms of Asia, and around 1.6 million in the Western
SBS include headache, eye, nose, and throat irri- Pacific, and around 100,000 people in Europe.
tation, fatigue, dizziness, and nausea. There is The combustion of fuels like wood and coal in
now increasing concern regarding indoor air qual- indoor environments leads to exposure to smoke
ity [9]. In the United States, indoor air is often including particulate matter (PM) and volatile
recirculated to improve energy efficiency; outdoor organic compounds. PM is often described by
air is mixed with indoor air in air handling units the metrics PM10 and PM2.5, the total particulate
(AHUs). This reduces the energy used to adjust mass per volume of air with an aerodynamic
humidity and heat (or cool) the outside air to diameter less than 10 and 2.5 mm, respectively.
control the indoor air temperature. Consequently, PM found in the air is a combination of liquid
this leads to a decrease in the air change rates in droplets and airborne solid particles. Liquids can
buildings, which lowers the indoor air quality include an aqueous phase with dissolved salts and
(IAQ). an organic phase. Solids can include soil minerals
There are many sources of indoor air pollution. and organic material. Specific chemical compo-
The materials used in buildings, such as glues, nents include sodium, potassium, ammonium,
paint, sealants, carpets, walls, and furniture, give sulfate, nitrate, chloride, bi/carbonate, and black
off volatile organic compounds (VOCs). The con- carbon. Inhalation of PM leads to its deposition in
centrations of VOCs and other indoor pollutants the respiratory tract. Coarse particles mainly
are often higher than outdoor concentrations; deposit in the airways of the head, and fine and
indoor air can be as polluted as outdoor air with ultrafine particles penetrate deep into the lungs
the added burden of the indoor sources where they introduce foreign chemicals directly
[10]. Indoor air pollution is a complex problem; into the bloodstream. Examples of pollutants from
one example is that building standards are not combustion include soot, polycyclic aromatic
138 Indoor Air Quality: Status and Standards

hydrocarbons (PAHs), carbon monoxide (CO), maintain a safe working environment and mini-
and formaldehyde (CH2O). The composition of mize the potential of exposure to high levels of
PM is highly variable and depends on its origin polluted air in the workplace. However, there are
and processing in the atmosphere. Some PM orig- many countries where such regulations do not
inates from engines burning liquid hydrocarbons. exist or are not enforced, and many people are
This PM, commonly found in urban areas, con- unnecessarily exposed to hazardous levels of pol-
tains a mixture of black soot, fuel residues, and lutants. Poor IAQ is linked to decreased produc-
water. Indoor pollution also includes compounds tivity and personal satisfaction, while increasing
emitted from noncombustion sources, such as illness and workplace absence. Altogether,
building materials, paints, impregnated surfaces, improving IAQ provides short- and long-term
plastics, cleaning agents, batteries, plumbing, monetary benefits for companies [14].
etc. Increased attention to these pollutants has
led to decreased exposure in developed countries; Air Pollution in Offices
however, they are still an important class of pol- Office equipment is a well-known source of
lutants in developing countries. Some specific indoor air pollution. However, “office” spans a
examples include formaldehyde, radon, asbestos, wide range of types of spaces, uses, and climatic
lead, VOCs, moisture, and mold. conditions around the world. Establishing a sys-
The concentrations of PM indoors are tematic guide to office pollution is quite challeng-
influenced by indoor materials and activities, and ing. Generally, office equipment like computers
outdoor sources. A large source of indoor pollu- and printers is a source of VOCs, SVOCs (“semi-
tion is tobacco smoke [12]. A cigarette contains volatile organic compound,” which include bro-
up to 4000 different chemicals, and many deposit minated flame retardants and organophosphates),
onto particles and surfaces such as walls and fur- dust (PM), and ozone. Printers and copiers emit,
niture. Besides serious health problems, the accu- on average, more VOCs than computers; these
mulated pollution also causes discoloration and emissions may include xylene, toluene, and
aging. The deposition of environmental tobacco other alkylbenzenes. Ozone from printers easily
smoke (ETS) onto indoor surfaces results in addi- reacts with other indoor pollutants creating sec-
tional exposure beyond inhalation as deposited ondary pollutants and ultrafine aerosol particles
ETS can be absorbed through the skin. Deposited [15]. In this regard, the U.S. Environmental Pro-
ETS is reemitted over the course of hours to tection Agency (EPA) gives a simple but effective
months, and is a significant source of airborne checklist on how to keep office air healthy. People
particles in places where smoking is allowed. should be responsible for keeping airways clear
The concentration of indoor ETS can be much and unblocked, use dedicated smoking areas, tak-
higher than outdoor concentrations [13]. ing care of plants, and managing food and waste
properly. Managers, in addition, are responsible
Air Pollution in Industry and Public for maintaining a clean working environment by
Infrastructure integrating optimal HVAC systems, preventing or
People working in industries such as foundries, avoiding polluting office supplies and equipment,
chemical and food processing, and waste manage- and developing other strategies to improve the
ment can be exposed to air pollution in excess of overall IAQ (US EPA, 2014) [16].
levels typically found in residential air pollution.
For instance, workers in nuclear power plants
have a higher risk of exposure to radioactive Biological, Physical, and Chemical
materials; in the same manner, a worker in vehicle Sources of Pollution
manufacture has a higher risk of contacting sol-
vent vapors from glues or paint, or metal vapor Indoor air pollution is typically divided into that
from welding. Most industrial countries have stemming from occupancy and that from building
implemented strict regulations in order to materials; the pollution may be of biological,
Indoor Air Quality: Status and Standards 139

physical, or chemical origin. Outdoor air pollution RH can damage building materials; mold and
from whatever source enters a building by entrain- fungus can grow when RH is above ca. 50%.
ment with supply air or infiltration through the
building envelope. Biological pollutants are emis-
sions from living organisms, e.g. CO2, water
Deposition of Pollutants
vapor, bioeffluent gases, mold, bacteria, viruses,
and dandruff. Physical sources of pollutants are
Outdoor air pollutants can be removed from the
emissions from surfaces commonly found in
gas phase by deposition, where the pollutant is
households such as furniture, electronics, paints,
absorbed onto a surface or absorbed into a mate-
building materials, and household cleaning prod-
rial. There are two main processes by which
ucts (Table 1). These types of pollutants are
chemical species from the atmosphere can
named primary emissions. The most important
deposit. First, wet deposition is the washing out
physical source of air pollution is outdoor air
of chemicals by precipitation, through rain, fog, or
pollution, which enters the building through ven-
snow, which occur outdoors. The second is dry
tilation systems, doors and windows, and cracks
deposition, which is the transfer of a species from
or openings in structures. Chemical sources of air
the gas phase directly onto a surface, in the
pollution include in situ production of secondary
absence of precipitation. Dry deposition is the
pollutants, i.e., products formed from reactions
primary way that atmospheric species deposit
between primary emissions and light or reactive
indoors.
gases like ozone, NOx, and OH. It should be
The deposition velocity describes the rate at
mentioned that when designing ventilation sys-
which an atmospheric species deposits on a sur-
tems, CO2, temperature, and relative humidity
face. It depends on a number of factors:
(RH) are the central considerations. Prolonged
periods with moisture levels in excess of 75%
• The solubility of pollutant

Indoor Air Quality: Source Pollutant Type References


Status and Standards,
Building materials VOCs Physical [17]
Table 1 Sources of indoor
Biocides
air pollutants listed
Plasticizers
alphabetically
Flame retardants
Carpets VOCs Physical [16]
Computers Ozone Physical [15]
Cooking PM Chemical [17]
Formaldehyde
Soot
CO2
Furniture VOCs Physical [17]
Heating Biocides Physical [17]
VOCs
Lightning technologies Phenols Physical [17]
Cresols
Flame retardants
PM
Paint VOCs Physical [16]
People CO2 Biological [17]
NH3
H2O
Dandruff
Printers Ozone Physical [15]
140 Indoor Air Quality: Status and Standards

• Atmospheric turbulence faster for large particles (D > 1 mm) and diffusion
• Properties of the surface is faster for small particles (D < 100 nm). In
between the large “coarse” particles and the
The deposition velocity can be described by small “ultrafine” particles, the “fine” particles
the resistance model, illustrated in Fig. 1. The accumulate [18].
model uses three parameters to describe the bar- Surface resistance, the final step before uptake
riers to deposition. The deposition velocity v1
d is
at the surface, depends on the nature and proper-
given as: ties of the surface. If a particle hits a smooth inert
surface, it is more likely that it will bounce off
v1
d ¼ rt ¼ ra þ r b þ rc instead of depositing [18]. For example, more
particles will deposit on a carpet than on a wooden
where ra is the aerodynamic diameter, rb is the floor, and more VOCs will deposit on curtains
quasi-laminar, and rc is the surface resistance. than on marble countertop [19]. Furthermore,
The first step for deposition is the transport of a deposition of large particles is more likely to
chemical species from the bulk to the quasi- happen onto the floor as there is a significant
laminar layer. This is a thin layer in which flow deposition velocity that can carry the particles
is parallel to the surface; a depositing species through the quasi-laminar layer [20].
cannot get closer to the surface by flow alone.
The first parameter, the aerodynamic resistance,
depends on the rate of mixing of the bulk air by
Interaction of Humans with Indoor Air
convection, turbulence, and diffusion. To cross
Pollution
the quasi-laminar layer, a particle must leave the
Humans can act to reduce air pollutants in a num-
streamline of flow; it must somehow move per-
ber of ways. One simple way is through behaviors
pendicular to the motion of air. This can take place
such as opening a window or using a mechanical
either by gravitational settling or through diffu-
ventilation system, which removes the polluted air.
sion. By their natures, gravitational settling is
Another way is by limiting pollution sources, like

Indoor Air Quality:


Status and Standards,
Fig. 1 Resistance model
for dry deposition [18]
Indoor Air Quality: Status and Standards 141

making sure all fuel-burning appliances in the dioxide, and other gases.” [24]. The main purpose
home are working properly. The growth of mold of ventilation is to dilute indoor air pollutants and
can be discouraged by keeping humidity below to eventually get rid of them by filtration or by
50%. Old air filters can themselves be a source of releasing them outdoors. It can be achieved in two
odor and pollution. Replacing the air filters in an air general ways: mechanical or natural.
conditioning system regularly keeps appliances Mechanical ventilation relies on fans to drive
working properly and indoor air quality is ventilation. Mechanical ventilation relies on air
improved. Activities like smoking and painting handling units (AHUs) that supply outdoor air
should be done outside. Many people are surprised into a building and can also provide filtration,
to learn that candles are a large source of particulate dehumidification, and conditioning of the supply
matter indoors. Cleaning is another way to mini- air. Natural ventilation is driven by pressure differ-
mize indoor air pollution. Dust can pull SVOCs ences that occur naturally in and around buildings.
from solid materials and release them to the air, The total driving pressure depends on the wind
thus introducing pollutants to the air that would speed and direction, the temperature difference
otherwise have remained in the material. It is cru- between zones (e.g., the interior and exterior),
cial that the cleaning agent used is perfume free, as and the difference in height between inlets and
it otherwise functions as a pollution source itself. outlets. Natural ventilation takes advantage of
Limonene and a-pinene are VOCs often found in fluid behavior to channel the air through openings
household cleaning products, giving lemony and in the buildings [25, 26]. Natural ventilation is a
piney scents, respectively [21]. These and other cheap and efficient option, provided the ambient
aromatic compounds used as scents can undergo air is clean and free of pollution. However, it is not
reactions with ozone yielding oxidation products always suitable due to local climatic conditions for
harmful to humans, thus contributing to ultrafine instance in very humid, cold, or hot environments.
particles in the indoor environment. Humans also Natural ventilation can be difficult to control, since
act as sinks by inhaling the polluted air, leading to it depends on natural driving forces. Mechanical
deposition of pollutants in our tissue. Deposition ventilation techniques enable the construction of
can also occur onto skin, thus introducing pollut- airtight buildings with integrated climate control
ants directly to the bloodstream. When pollutants units (CCU), which reduce the cost of temperature
enter the human body, they can cause adverse control. Mechanical ventilation can be controlled
health effects such as eye and airway irritation, and monitored, but power or other types of failure
respiratory diseases [22], cardiovascular diseases can compromise its functionality. In contrast, nat-
[23], and cancer. ural ventilation systems are passive and efficient in
supplying un-conditioned outdoor air. They have
no need for maintenance and use no energy to drive
Ventilation Systems in Buildings ventilation. However, they can be difficult to con-
trol and the supply air is un-conditioned. In periods
As mentioned earlier, humans spend most of their with cold outdoor temperatures, occupants may
time indoors, thus mainly breathing indoor air. experience low indoor temperatures and draught.
Hence, heating, ventilation, and air conditioning Control can be improved by adding a control sys-
(HVAC) systems have been developed to tem and fitting actuators to shutters, dampers, and
recirculate air inside buildings, to provide accept- windows; however, the system will then no longer
able IAQ and thermal comfort. Ventilation is be passive or entirely maintenance-free and would
defined as the “process of exchanging or replacing be properly classified as a hybrid system, i.e., one
air in any space to provide high indoor air quality that employs both natural and mechanical elements
which involves temperature control, oxygen [25–27]. Many people like to control the environ-
replenishment, and removal of moisture, odors, ment themselves by controlling windows and
smoke, heat, dust, airborne bacteria, carbon shades.
142 Indoor Air Quality: Status and Standards

Indoor Air Quality: Status and Standards, Indoor Air Quality: Status and Standards,
Table 2 Impact of smoking on required ventilation Table 3 Lifetime of typical VOCs found in indoor
(Modified from [28]) environments
Proportion of Supply air Common indoor VOC Lifetime (days) References
occupants that (liter/ Limonene 0.02 [30]
Level of smoking smoke (%) person) a-Pinene 0.082 [30]
No smoking 0 8 Isoprene 0.32 [30]
Some smoking 25 16 Ethanol 2.8 [31]
Heavy smoking 45 24 Benzene 9.4 [32]
Very heavy smoking 75 36 Acetone 10–30 [33]

One of the key concepts of ventilation is the air @t = change in time


change rate (ACR), a ratio between the hourly V_ pol = pollutant indoor generation rate
ventilation rate divided by the volume of the
space, as shown in the following formula [25]:
However, this formula does not take other
removal processes into account, such as deposi-
Q¼kV
tion or chemical reaction (sink effect).
where:

Q = ventilation rate (units of volume/units of In Situ Chemistry


time, e.g., m3/h)
k = air change rate or exchange rate (e.g., 1/h) Indoor air contains a mix of pollutants from both
V = volume of the room (e.g., m3) outdoor and indoor sources. The outdoor and
indoor environments can be regarded as two iso-
The exchange rate expresses how often the air lated reaction chambers, where compounds emit-
inside a confined space is renewed with outdoor ted from primary sources can interact and form
(or re-circulated) air. In offices, the usual air secondary pollutants [29]. Many of the primary
change rate is about 3–4 h1, compared to VOC emissions are harmless to humans, but they
20–30 h1, for bars and nightclubs. In addition, can react with oxidizing species such as O3, OH,
tobacco smoking has a significant impact the air and NOx to yield secondary pollutants with nega-
removal required to maintain a stable healthy tive effects both on health and comfort [29]. Typ-
environment (Table 2). ically, primary pollutants are VOCs that form
The concentration of a well-mixed pollutant secondary pollutants upon reaction with ozone
inside a ventilated room can be modeled as or radicals. The lifetime of chemical species is
[25, 26]: an important factor when assessing air pollutants.
Compounds with short lifetimes will most likely
@c undergo reaction shortly after being emitted, and
V ¼ qðc0  cÞ þ V_ pol potentially form harmful secondary pollutants.
@t
Compounds with longer lifetimes will not be
where: removed by chemical reaction, but instead by
ventilation. In Table 3, the lifetimes of some com-
V = volume of room mon indoor VOCs are shown, based on reaction
c = concentration of pollutant with OH and O3. The table displays tropospheric
q = ventilation rate lifetimes, as they are determined from outdoor OH
c0 = supply air concentration and O3 concentrations, but the trend in lifetimes is
@c = change in concentration expected to reflect indoor conditions.
Indoor Air Quality: Status and Standards 143

Oxidizing species like NOx, O3, HONO, and with aromatic compounds, the reaction of HO2
OH radicals drive indoor air chemistry; they can with NO, and the photolysis of HONO
be very reactive. OH has a lifetime of less than 1 s [35]. Ozone and NO are mainly introduced to
due to its high reactivity with almost all types of the indoor environment from outdoor air, while
pollution [34]. In the indoor environment, the HONO is the product of a heterogeneous reaction
major sources of OH are the reaction of ozone between water absorbed on a surface and NO2.
with unsaturated compounds, reaction of ozone Figure 2 shows a summary of the different

Indoor Air Quality:


Status and Standards,
Fig. 2 Overview of main
reactions taking place
indoors. For further
information on the third
panel, see [36]. ‘M’ is a
molecule from the
atmosphere, a collision
partner, and O/C is the
Oxygen to Carbon ratio
144 Indoor Air Quality: Status and Standards

Indoor Air Quality: Concentration range


Status and Standards, Compound Location (mg m˗3)
Table 4 Typical indoor
HONO Living space 0.08–1.4
concentrations of reactive
species [37, 38] OH Indoor air 0.1–4
NO2 Living space 10–200
O3 Indoor air 5–300
NO2 Kitchen 300–3000

Indoor Air Quality: Status and Standards, Table 5 Possible oxidation products of common indoor compounds [37]
Reagent Products Indoor source
a-Pinene Pinene oxide, pinoaldehyde Wood
Diethylhexyl phthalate (DEHP) 2-ethyl-1-hexanol Plasticizers
Limonene Limonene oxide, carvone, formaldehyde Wood
Linoleic acid Hexanal, heptanal, 2-heptanal, octanal Food
Tris(2-chloroethyl)phosphate (TCEP) 2-Chloroethanol Flame retardants

reactions occurring in the indoor environment, secondary organic aerosols (SOAs), formalde-
mainly from the HOx, NOx,, and VOC perspec- hyde and hydroxyl radicals (OH). OH radicals
tives as these are responsible for the majority of are very reactive and can react with any organic
indoor air chemistry. compound contributing further to the formation of
Typical indoor concentrations of oxidation secondary pollutants. These are frequently more
species and common indoor air pollutants along potent irritants than their precursors [39]. An
with their reaction products are given in Tables 4 example of an ozonolysis of a common monoter-
and 5, respectively. pene is the reaction between O3 and limonene [40]
shown in Fig. 3.
The reaction scheme in Fig. 3 shows that lim-
Ozonolysis
onene ozonolysis gives many different oxidation
Pollutants can undergo reaction with other chem-
products. In many cases, the products have a
ical species present in a building, for example,
lower vapor pressures than their precursors [36],
ozone. When ozone reacts with an unsaturated
following the pattern shown in Fig. 2c, which
organic compound leading to bond cleavage, it is
leads to SOA formation. Ozonolysis can occur
called ozonolysis. For example, ozone air pollu-
both in the gas phase and when ozone is deposited
tion will deposit on indoor surfaces and oxidize
on a surface. The deposited ozone then reacts with
them, damaging fabric, paint, rubber, and adhe-
a compound in the solid material and the newly
sives releasing oxidation products. Ozone adds to
formed pollutants can be emitted [40]. For
a double bond creating an intermediate where
ozonolysis to be relevant, the reaction needs to
bond cleavage can occur at different sites,
be fast enough to compete with the air exchange
resulting in many different oxidation products.
rate. This is mostly valid in situations with high
When reaction happens, the initial compound is
ozone concentrations and low air exchange.
degraded, meaning that ozone works as a sink for
primary pollutants. However, many oxidation
products are also pollutants; hence, ozonolysis Particle Growth
removes primary pollutants but instead creates Particles in the indoor environment originate from
secondary pollutants. An example is the reaction different sources, such as ingress of outdoor air
between ozone and monoterpenes that yields and various indoor combustion processes like
Indoor Air Quality: Status and Standards 145

Indoor Air Quality: Status and Standards, Fig. 3 Reaction scheme of ozone oxidation of D-limonene [40]

smoking, cooking, burning of candles, and the use mass. The formed particles are “fine,” with diam-
of combustion apparatuses in poorly ventilated eters d < 1 mm.
areas [41]. Still, it was reported in 1990 by Smoking directly releases thousands of com-
Santanam et al. that on average 19–42% of ultra- pounds, both as gases and particulate matter, and
fine particles indoors were of unknown origin this is referred to as secondhand tobacco smoke
[42]. Since then, studies have been conducted [43]. The compounds in secondhand tobacco
suggesting that indoor ozone-terpene reactions smoke can be deposited on surfaces and then
contribute to the SOA found indoors. As previ- re-emitted, or they can undergo chemical reaction
ously mentioned, terpenes are emitted from and form secondary pollutants. The result of these
cleaning agents and air fresheners (these terpenes two pathways for secondhand smoke creates what
include limonene and a-pinene) and are readily is called thirdhand tobacco smoke [44]. The pol-
oxidized by ozone (ozone stems from outdoor air lutants in thirdhand smoke include gaseous,
or direct emissions from electronics) to form prod- sorbed, and particulate species, hereunder SOA.
ucts with low vapor pressures [41]. These prod- The SOA formed from ozonolysis of secondhand
ucts can form SOA through homogeneous tobacco smoke, including nicotine, are
nucleation, where vapor condenses to form nitrogenated ultrafine particles, which are likely
146 Indoor Air Quality: Status and Standards

to be associated with a high asthma hazard index Improving IAQ to reduce SBS can help compa-
[45]. Experiments performed by Petrick et al. indi- nies due to increased productivity. For example,
cate that SOAs (in this case ultrafine particles) are the benefits of implementing a particle filter
formed from heterogeneous reactions of surface- greatly outweigh the installation and running
sorbed nicotine with ozone, rather than through a costs [52]. This should encourage companies to
homogeneous reaction entirely in the gas phase. implement similar solutions.
This heterogeneous reaction is the major source of
SOA from ozonolysis of secondhand tobacco Asthma and Allergy
smoke. In addition, their study shows that the There has been a substantial increase in respira-
peak formation of SOA is at low humidity tory illnesses and asthma over the last generation,
levels [46]. especially in industrialized countries. Some
researchers link this trend to the indoor environ-
ment, where numerous pollutants can be found.
Indoor Air Quality and Health Variables that negatively affect the human respi-
ratory system include carbon monoxide, tobacco
Sick Building Syndrome smoke, allergens, mold, dampness, humidity, and
Sick building syndrome has been the subject of a particulate matter. Prevention of carbon monoxide
lot of research the recent years, as there seems to pollution can be affected by the correct installa-
be an increase in cases of SBS. There is no agree- tion and venting of gas appliances, while tobacco
ment on the exact definition of SBS, as it is asso- smoke can be eliminated by nonsmoking indoors.
ciated with a wide range of symptoms and Allergens from house dust mites and cats have
sources. Symptoms typically occur when people proven to exacerbate asthma in individuals
spend long periods of time in an unhealthy indoor already sensitized to the given allergen
environment, such as in an airtight office building [53]. Thus, an allergy patient will be at higher
or school [47]. SBS is mainly linked to poor IAQ risk of developing asthma when exposed to the
and the associated problem of poor ventilation. allergen. House dust mites are found in carpets,
Other contributing factors include noise, stress, a bedding, and mattresses, where the allergens are
monotonous work environment, temperature, released by, e.g., vacuuming (without a high effi-
humidity, and biological sources including mold ciency filter), general cleaning, and other indoor
and fungi. Noise in buildings has been associated activities. The amount of house dust mite aller-
with eye pain, nausea, and skin dryness. A lack of gens can be minimized by hot washing of bedding
proper lighting can cause dizziness and malaise (>55  C) [54], use of feather-filled pillows [55],
[48]. Furthermore, the risk of SBS is larger for and by encasing bedding and mattresses in imper-
smokers and for people who suffer from asthma or meable material [56], as well as having non-
allergy [47]. carpeted flooring in the home [57]. However,
Despite these many contributing factors, IAQ these measures have not shown clinical improve-
is the major contributor to SBS, and high levels of ment in patients already suffering from asthma
pollutants including NOx, PM, CO2, and VOCs [58]. The majority of pet allergens originate
have been shown to increase the risk of SBS from cats (in UK homes, there are 11.1 million
[1, 49, 50]. This is supported by the fact that an cats and 8.9 million dogs [59]), as cat allergens are
increase in ventilation rate leads to fewer cases of respirable (<5 mm), whereas 80% of dog allergens
symptoms related to SBS, such as fatigue, head- are nonrespirable due to their large size (>5 mm)
ache, and throat irritation. Another important [60]. Data shows that asthmatic individuals sensi-
aspect of SBS is the negative effect it has on tive to cat allergens will experience worsening of
productivity. This is especially relevant for work- their asthma when exposed to cats [53]. There is
ing spaces, as SBS can result in loss of work [47, insufficient evidence to determine if exposure to
50]. A study found that the most optimal temper- cat allergens will cause asthma development in
ature for work productivity is 21–22  C [51]. healthy subjects [53]. Another pollutant that has
Indoor Air Quality: Status and Standards 147

been linked with exacerbation of asthma in sensi- above 0.5 h1 in Nordic homes are associated
tized individuals is mold. Hundreds of different with lower probabilities of both asthma and
mold species can be found indoors, and the risk of allergy symptoms [64].
exposure can be difficult to diagnose as mold There are numerous negative health effects
colonies are not visible until fully grown. Mold associated with indoor air pollutants. These pol-
requires the right levels of moisture, oxygen, tem- lutants can come from products found in virtually
perature, and nutrients to grow [61]. Excess mois- every household. In Table 6, some of the impor-
ture in furnishings and condensation on surfaces is tant indoor pollutants are listed as well as their
called dampness and is caused by high humidity sources and effects on health.
giving optimal conditions for growth of mold and Ensuring a healthy indoor environment is part
dust mites. Data shows associations between of UN Sustainable and Development Goal
doctor-diagnosed asthma cases and damp condi- 3 concerning good health and well-being for peo-
tions, as well as asthma symptoms and dampness ple of all ages. This goal is to be accomplished by
[53]. Thus, there is evidence that dampness is a 2030 [69]. As humans spend the majority of their
cause and an exacerbating factor for asthma, time indoors, ensuring a healthy indoor environ-
likely related to its promotion of mold and dust ment and reducing building-related diseases is a
mites [53]. key component of the goal.
Particulate matter has adverse health effects on
humans. The effects depend on the composition CO2 as Measure for Indoor Air Quality
and size of the PM, as this is directly linked to Historically, CO2 has been used as a direct mea-
deposition in the respiratory tract and the respira- sure of overall indoor air quality. One example is
tory tree’s ability to remove the pollutants the limit of 1000 ppm CO2 in the indoor environ-
[62]. Coarse PM tends to deposit in the nasal ment set out in the ASHRAE-1989 standard [70],
and upper respiratory system, while fine PM and which is still in use today. Several studies show
UFP tend to deposit in the lower respiratory tract that CO2 levels above 1000 ppm are linked to a
and alveoli. Thus, fine particles and UFP penetrate decrease in school attendance in students [71,
deeper into the human airways. UFP have large 72]. It has been suggested that CO2 in itself is
surface areas per unit mass, which allows for the not the cause of absenteeism, but instead that an
particles to collect relatively large amounts of increase in CO2 levels is an indicator of insuffi-
toxic low-volatile compounds such as PAHs, cient ventilation (<7.5 l/s per person), which
metals, and quinones [62]. These chemicals can leads to accumulation of other pollutants. Such
generate acute inflammation of the airways, and pollutants could be bioeffluents or the scents of
sudden elevation of PM can trigger asthma flares. cleaning products, which along with their oxida-
These acute effects can be caused by exacerbation tion products cause discomfort [70]. Other pollut-
of already existing airway inflammation and ants could be any of the species implicated in sick
hyper-reactivity. In addition, there is evidence building syndrome, as described previously. CO2
that air pollution including PM and NOx changes can thus be used as an indirect measure of venti-
the structure of biofilm making it thicker and more lation rate and other odor pollutants, but only to a
porous, and thus a better substrate for infections. certain extent [73]. CO2 is also a pollutant in its
There is increasing evidence that PM induces own right. A recent study shows that indoor CO2
sensitivity to common environmental allergens, levels above 1000 ppm can cause drowsiness and
which means that long-term PM exposure may negatively affect focused activity [1]. Building
lead to increases in asthma and allergy [63]. Pol- standards for ventilation should not be based on
lutants can be removed by ventilation, and avail- indoor CO2 levels alone, as this may not be the
able data suggests that lower ventilation rates in most important indoor air pollutant [70]. A study
buildings are associated with increases in the fre- by Satish et al. finds that CO2 levels of 1000 ppm
quency of asthma and allergy symptoms, due to and 2500 ppm, relative to 600 ppm, caused a
the accumulation of pollutants. Air exchange rates statistically significant decrease in decision
148 Indoor Air Quality: Status and Standards

Indoor Air Quality: Status and Standards, Table 6 Selected pollutants, their sources, and health effects [1, 65–68]
Pollutant Source Negative health effects
Formaldehyde Building materials and consumer products Cancer, sensory irritation, irritation of the eyes
(CH2O) and upper airways
Carbon monoxide Combustion – Cooking, heating, smoking, Binds to hemoglobin and makes
(CO) candles carboxyhemoglobin, which can cause
headaches, nausea, dizziness, breathlessness,
and fatigue, and with high exposures can lead
to coma and death
Nitrogen dioxide Combustion, outdoor air Respiratory effects, may enhance asthmatic
(NO2) reactions to inhaled allergens
Carbon oxide Humans, combustion, outdoor air Drowsiness and tiredness. May have negative
(CO2) effect on decision making and focused activity
Benzene (C6H6) Building materials, cooking Cancer, drowsiness, dizziness, rapid or
irregular heartbeat, headaches, tremors,
confusion, and unconsciousness
Ozone (O3) Outdoor air, printers, electronics Respiratory effects, chest tightness, cough,
wheezing, and lung function decrement.
Acute respiratory problems in asthmatics
Particulate matter Combustion, cooking, candles, outdoor air Stroke, heart disease, lung cancer, and chronic
(PM) and acute respiratory diseases, including
asthma, reduced lung function, and mortality
Alkylphenols Detergents, disinfectants, surface cleaners May interfere with, mimic, or block hormones
Organochlorines Outdoor and indoor air, tracked-in dust, Cancer, neurotoxicity, effects on developing
disinfecting products reproductive systems, lactation
Organophosphorus Polymeric materials, fabrics, polyurethane Effects on neurodevelopment and growth in
compounds foams, electronics (cable sheathing and developing tissue, relate to respiratory disease
casings), outdoor and indoor air, dust in children through disregulation of the
autonomic nervous system
Phthalates Flexible PVC, PVC flooring, wall coverings, Effects on the development of male
electrical cables and casings, personal care reproductive tract, prenatal mortality, reduced
products growth and birth weight, may relate to asthma
and allergies in children
Polybrominated Carpet padding, wall coverings, electronics, Effects on the development of brain and nerve
diphenyl ethers furniture, cushioning, and mattresses tissues, permanent learning and memory
impairment, behavioral changes, delayed
puberty onset, fatal malformations, thyroid
hormone disruption
Polychlorinated Floor finishes, foam cushioning and Cancer, developmental neurotoxicants, effects
biphenyls mattresses, oil-filled transformers, capacitors on immune, reproductive, nervous, and
endocrine systems
Pyrethroids Outdoor and indoor air, tracked-in dust, Weak anti-androgenic, anti-estrogenic, or
cleaning products estrogenic effect
Parabens Personal care products, canned food, fabrics Weak environmental estrogens

making in human test subjects who were not use large amounts of energy, and it has been calcu-
exposed to pollutants other than CO2 [1]. lated that HVAC can increase energy consumption
and related carbon emissions up to 100%
Air Conditioners/COP [75]. Accordingly, HVAC can account for up to
One of the functions of HVAC systems is to ensure 50% of the power used in commercial buildings
thermal comfort, which in turn increases the well- (i.e., malls, offices, hospitals, hotels, etc.) [76]. It is
being of occupants including associated properties estimated that, in total, HVAC systems are respon-
like productivity [74]. Air conditioning systems sible for approximately 40% of energy demand in
Indoor Air Quality: Status and Standards 149

commercial buildings in the United States [77]. On Chillers are the usual go-to equipment for large
a global scale, taking climate change, global commercial buildings. They produce cold water
warming, and rapid population growth into consid- which in turn is used to cool the building. COP
eration, it is expected that the demand for energy values for these systems range from 2.2 to 3.2 for
use for HVAC systems will increase [74, 76]. Some small chillers. The COP generally improves as the
studies have focused on the capacity of buildings to size of the system increases with values in the
produce and retain novel pollutants due to their range of 3.7–4.1 being typical for large
tightness and indoor sources. However, many systems [77].
buildings are poorly insulated and equipped with
inefficient air conditioning systems, which lead to
increased energy consumption and maintenance Remediation Methods
costs [76, 77]. There are some easy solutions to
increase the efficiency of the AC system. For One way to decrease the level of pollution is to
instance, the system should not operate at temper- minimize or eliminate the source. This can poten-
atures lower than 24  C, and it should be able to tially take a very long time or may even be impos-
adjust the flow of inlet air according to changes sible. Another way is to apply methods that
throughout the day. In temperate climates, the use remove pollutants directly from the air, such as
of aiding systems such as free cooling coils can filter systems with implemented adsorbent mate-
reduce power consumption [75]. rials, interior plants, or ventilation.
Many strategies can be used to design better
and more efficient HVAC and AC systems. The Gas Phase Advanced Oxidation
U.S. National Institute of Building Sciences Providing good indoor air quality in a polluted
(NIBS) posits that high-performance systems can location can be a huge challenge. Increasing the
yield up to 40% monetary savings and reductions ventilation rate to bring in more air from the
in greenhouse gas emissions. In addition, design- outside would not necessarily improve indoor air
ing buildings with an “extended comfort zone” quality unless the air is thoroughly cleaned first.
can achieve savings up to 70% [77]. Most build- Any solution would have to be able to clean large
ings today could benefit from fundamental design volumes of air with low energy consumption. One
strategies to improve their overall efficiency. Most possible solution is the system being used at the
strategies aim at improving the integration, con- Danish Embassy in Beijing. The Embassy has
nectivity, and responsivity of the building and the implemented a new air cleaning technology
conditioning systems. For instance, design teams invented by the University of Copenhagen and
should consider climate control in the early stages produced by the company Infuser under a license.
of the design process, in order to ensure the right As Beijing is one of the most polluted capitals in
equipment size and distribution for the system, the world [80], the Infuser air purifying system is
consumption goals, scalability, and manage peak a good example of how to ensure IAQ when
use phases and the maintenance program [77]. natural ventilation is not an option. The method
The coefficient of performance (COP) is used is centered on the hydroxyl radical (OH) and is
to measure the performance of air conditioning inspired by air cleaning mechanism that takes
systems [78]. place in the free atmosphere. In the atmosphere,
pollutants are oxidized by OH-forming com-
Q pounds with lower volatilities than their precur-
COP ¼
W sors. The oxidation products often form particles
that deposit or are washed out of the atmosphere.
where: OH formation is initiated by the photolysis of O3.
OH will then oxidize different VOCs entering the
Q = useful heat supplied or removed by the system and the reaction products can condense
system into particles that are removed by a particle filter.
W = work required by the system The remaining ozone is removed over a catalyst.
150 Indoor Air Quality: Status and Standards

Indoor Air Quality: Status and Standards, Fig. 4 Process of gas phase advanced oxidation

Indoor Air Quality: Concentration before Concentration after Removal


Status and Standards, Species treatment treatment efficiency
Table 7 Removal
PM10 411 8 98%
efficiency of pollutants [80]
(ug/m3)
PM2.5 255 7 97%
(ug/m3)
NOx (ppm) 77 40 48%
SO2 (ppm) 17 3 83%
O3 (ppm) 19 3 82%

An advantage of this method is that it does not rely air and is mainly caused by temperature differ-
on traditional filters, which typically have a sig- ences; moisture differences can also play a role.
nificant pressure drop resulting in higher energy Buoyancy results in pressure differences between
consumption. This process is illustrated in Fig. 4. indoor and outdoor air, and can thus drive ventila-
A measurement performed for five different types tion; for example, warm air rises in a chimney. At
of atmospheric VOCs showed that the system low wind speeds, ventilation is controlled by buoy-
successfully removed a large part of contaminants ancy, and for strong wind conditions, ventilation is
in the air, as shown in Table 7. controlled by wind-induced pressure differences in
the indoor-to-outdoor environment [81]. The
Windows different ventilation strategies, based on room
As mentioned earlier, IAQ can be improved by geometry (windows and doors), are named single-
natural ventilation. The efficiency and suitability sided-, cross-, and stack ventilation. Single-sided
of natural ventilation depends on a number of fac- ventilation is the simplest and least efficient
tors. As described in the sections about Green ventilation strategy, and applies when only one
Lighthouse (see below) and Infuser (see above), opening is located in the room, typically a room
natural ventilation is only suitable when the build- with one window and closed doors. In summer, the
ing of concern is located in an environment with main driving force for single-sided ventilation is
relatively clean outdoor air. The efficiency of natu- wind turbulence. In winter, single-sided ventilation
ral ventilation depends on wind turbulence, buoy- can be driven by thermal buoyancy, with cold
ancy, and ventilation strategy. Buoyancy occurs air flowing in at the bottom of a leaky window
due to differences in density of indoor and outdoor and warm air flowing out at the top [82]. In a
Indoor Air Quality: Status and Standards 151

cross-ventilated system, openings are located at Natural ventilation operates passively, or by


opposite sides of the room and air will flow manual or automated control. WindowMaster
through one opening and exit through the other. A/S has developed an automated natural ventila-
If both openings are windows, ventilation is tion system called intelligent natural ventilation in
driven by differences in wind pressures at the which roof and façade windows open and close
surfaces where the windows are located. Stack automatically based on preset values of CO2,
ventilation occurs when air flows through a lower humidity, and temperature. Indoor temperature,
window and exits through a window placed high humidity, and CO2 levels, and outdoor tempera-
in the room, as in the Green Lighthouse (see ture, wind, and rain are monitored and used to
below). The airflow in stack ventilation is mainly control the window movements [83].
driven by thermal buoyancy, and the largest In some systems, natural ventilation is combined
effect is created by placing the two openings far with mechanical ventilation giving so-called mixed-
apart vertically [81]. Illustrations of the three mode ventilation. This may be necessary when con-
ventilation strategies are shown in Fig. 5. ditions do not allow for natural ventilation, e.g., for

Indoor Air Quality:


Status and Standards,
Fig. 5 (a) Single-sided
ventilation. (b) Cross
ventilation. (c) Stack
ventilation
152 Indoor Air Quality: Status and Standards

low wind speeds and cold outside temperatures. Photocatalysis


A mixed-mode system can be operated manually A potential drawback of using adsorbents is that
or automatically, so when the set values for temper- they do not break down pollutants, but instead the
ature, humidity, and CO2 levels are not maintained pollutants remain on the absorbent, which has a
by natural ventilation, the system will shift to limited capacity. Adsorbent capacities may be in
mechanical ventilation, where an inlet fan intro- the range of 1–10% of the mass of the filter mate-
duces outdoor air and an exhaust fan sucks out rial itself, and eventually they reach capacity and
indoor air. In colder climates, a heat recovery system must be changed. Photocatalysts, in contrast, can
can be used. Cold outdoor air is heated by the be regenerated continuously using light.
exiting indoor air, before entering the room Some photocatalysts can be driven by sunlight,
[84]. When outdoor conditions are favorable, the and therefore do not necessarily rely on an exter-
system will change back to natural ventilation. nal source of energy, typically electricity. Further-
Mixed-mode ventilation favors natural ventilation, more, they promise to transform hazardous VOCs
when possible, for optimal energy efficiency. into H2O and CO2, unlike conventional filter sys-
tems, which rely on trapping VOCs. However,
Activated Carbon research has shown that many photocatalysts do
Activated carbon (AC), also called activated char- not live up to this goal and leave many com-
coal, is a form of carbon processed to have an pounds only partially oxidized; they convert pol-
extremely high surface area. Its high surface-to- lution into byproducts that may smell worse and
mass and surface-to-volume ratio, combined with be more toxic than the precursors [87].
low price and high affinity for many kinds of pollu- TiO2, in particular, has received significant
tion, have made it a valuable material in pollution attention from researchers because of its photo-
control systems. The surface chemistry is based on catalytic activity and low cost. TiO2 has been used
graphene, but modified depending on impurities and in a wide range of applications including purifica-
modifications. AC is produced from a carbonaceous tion of wastewater and air. For purification of air,
material which could be coal, wood, or some other the material has been placed on window glass and
plant fiber. The material is heated to drive off vola- pavement or incorporated directly into materials
tile components, leaving behind a solid with a net- like paint and concrete [88]. The activity of TiO2
work of pores. The porous structure consists of long is greatly improved when using nanosized parti-
networks of channels which are termed micro- cles as opposed to microsized particles. This is
(<2 nm), meso- (2–50 nm), and macropores due to the increased surface area, which greatly
(>50 nm). Because of this porous structure, AC increases the photocatalytic activity, as there are
has a specific surface area in the range of more sites available for molecules to adsorb and
500–3000 m2/g, which is crucial for the perfor- reactions to occur. However, the use of nano-
mance of AC [85]. Many types of pollution can be particles can pose a threat to human health. One
trapped by physisorption or chemisorption. study showed that significant amounts of nano-
The surface of AC contains functional groups particles are released into the environment due to
such as epoxy bridges and carboxyl, hydroxyl, and aging of photocatalytic paints [89]. Nanoparticles
carbonyl moieties. These groups change the chem- are very toxic to humans and the environment in
ical properties of the surface and can be used to general and there is a need for improving nano-
change the hydrophilicity of the surface and the sized TiO2 materials.
affinity for specific types of species. The process of The first step is transport of the pollution to the
adsorption, including surface chemistry, is shown catalytic surface (see discussion of deposition
in Fig. 6. Even though AC has been widely used onto a surface above) followed by adsorption.
for many years, improving the adsorption proper- Different molecules will spend different amounts
ties is an active area of research. One example is the of time on the surface depending on how tightly
addition of a basic nitrogen functionality to the they are bound. Photocatalysts have a limited
surface to improve CO2 uptake [86]. ability to degrade volatile pollutants, simply
Indoor Air Quality: Status and Standards 153

Indoor Air Quality:


Status and Standards,
Fig. 6 Activated carbon
comes in many forms
including pellets, beads,
and fibers. Key features
include a high surface area
due to a fractured porous
structure, and modifications
of surface functional groups

because they may not stay on the surface long O2 is in equilibrium with HO2 and OH-; super-
enough to react. Once a molecule is on the sur- oxide has a pKa value of 4.8, so, e.g., at neutral
face, it is degraded by a heterogeneous chemical pH, most is in the superoxide form. Under suitable
reaction. In addition, because of atmospheric conditions, HO2 will react with itself to form
humidity, mineral surfaces like TiO2 will be cov- hydrogen peroxide (H2O2). The electron hole h+
ered with water. The thickness of the water layer will oxidize water, producing hydroxyl radicals:
depends on relative humidity; at low humidities, a
hydrogen-bound layer and a layer, several mono- hþ þ H2 OðadsÞ ! OH þ Hþ
layers thick, of quasi-crystalline water will be
present. At higher humidities, a layer of water The hydroxyl radicals reacts with many pollut-
with properties resembling bulk water will be ants to form products which are then desorbed and
present. First TiO2 is photoexcited, yielding an re-emitted into the ambient air [90]:
electron (e), and a corresponding hole in the
valence band (h+) OH þ VOC ! Intermediates ! Final products

TiO2 þ hv ! e þ hþ Photocatalytic paints containing TiO2 have


been shown to remove VOCs, including xylene,
The electron may react with dissolved O2, and NO2, both of which are known to have nega-
forming superoxide O2. In aqueous solution, tive health impacts. However, photocatalytic paints
154 Indoor Air Quality: Status and Standards

are also sources of VOCs such as formaldehyde, the plant [93]. Other chamber studies show that
carbonyls, and other chemical species like HONO, selected low-light requiring house plants efficiently
which in some cases are worse than their precur- remove formaldehyde [94], xylene, and ammonia
sors [89, 91]. In addition, it has been shown that [95], as well as toluene, benzene, trichloroethylene,
hydroxyl radicals react with the organic binders in octane, and a-pinene [96]. Although chamber stud-
the paint resulting in byproducts that are released ies showed that selected plants have air cleaning
from the paint [109]. A large-scale experiment properties, field experiments are needed to confirm
conducted as part of the European LIFE+ project if the plants studied will be capable of significantly
examined the effect of TiO2 coating on the concrete reducing indoor air pollution in a real-world situa-
inside the Leopold II Tunnel in Brussels; UV lamps tions. A Sydney field study tested the air cleaning
were installed along the length of the tunnel. NOx properties of two common house plants,
removal was measured before and after the TiO2 Spathiphyllum (peace lily) and Dracaena
coating was applied. In contrast to previous labo- deremensis (Janet Craig), in single-occupant
ratory experiments, no significant reduction of offices. Both naturally ventilated and air-
NOx was observed. An upper limit for NOx conditioned offices were assessed, and the air puri-
removal at 2% was identified, corresponding to fying properties were measured as total VOC
the uncertainties of the instruments used [92]. In removal. Experiments showed that offices with a
conclusion, TiO2 shows some promising air total VOC concentration larger than 100 ppb had a
cleaning properties in laboratory experiments, but significant reduction in VOC levels when either
at the same time, there are reasonable concerns, 3 or 6 Janet Craig plants were present, and that
and TiO2 products have yet to find widespread 3 plants were just as efficient at removing VOCs as
commercial success despite decades of effort. 6 plants. This was observed for both air-
conditioned and naturally ventilated offices. The
Plants as Remediation Strategy study also found that when a mix of Dracaena
In 1989, NASA conducted a study of 12 house deremensis and Spathiphyllum were present,
plants selected to tolerate low-light conditions again either 3 or 6 plants, a significant reduction
and determined their ability to remove benzene, of total VOC levels was observed, except when
formaldehyde, and trichloroethylene from indoor Spathiphyllum was in flower as it then emits
air. The study was performed as a chamber exper- VOCs. In summary, the total VOC levels were
iment at both high (15–20 ppm) and low (<1 ppm) reduced by 50–75% when the initial VOC concen-
pollutant concentrations. The plants showed poten- tration was 100 ppb or above, and 3 plants are
tial for improving IAQ in energy-efficient build- sufficient to obtain this reduction under the condi-
ings, by removing pollutants from the air. The root- tions of the study [97]. Another field study inves-
soil zone of the plant seemed to be the most effi- tigated the air cleaning abilities of Dracaena
cient at removing pollutants, possibly due to micro- deremensis (Janet Craig), Dracaena marginata
bial activity in the soil. It was also observed that (marginata), and Spathiphyllum (peace lily) in an
when the same plant and potting soil were con- urban classroom in Portugal. Six plants were
stantly exposed to a certain pollutant, their capacity placed in a 25-person classroom and air-borne
to remove that pollutant increased. Typically, pollutants were monitored over a 6-week period.
plants emit trace levels of VOCs and other metab- The study found that CO2, VOC, carbonyl, PM10,
olites. Under the temperature and light conditions organic carbon, nitrate, sulfate, ammonia, calcium,
of the experiments, the tested plants emitted negli- and carbonate levels were significantly reduced
gible amounts of metabolites. As temperature and after the introduction of the six plants [98].
light levels increased, the plants’ metabolite emis- Based on the chamber experiments and field
sions would be expected to increase, as well as studies, it can be concluded that plants can be
their air cleaning properties. Increases in O2 pro- effective air cleaning systems, and a cost-effective
duction and CO2 removal would be associated with solution for many types of buildings. Since differ-
an increase in the pollutant removal efficiency of ent plant species target different pollutants, it is
Indoor Air Quality: Status and Standards 155

most efficient to use a variety of plants for air Leadership in Energy and Environmental
cleaning purposes. Plants can also be used in Design (LEED) is a green building certificate
combination with other air cleaning methods, developed by the nonprofit organization U.S.
such as filtration systems and ventilation. Green Building Council. It consists of a point-
Table 8 shows a list of plants with air purifying based rating system with four different certifi-
properties and their target pollutants. cates. The lowest possible certification requires
(40–49 points) followed by silver (50–59 points),
gold (60–79 points), and platinum (80+ points).
Sustainable Buildings LEED focus on five different areas: water effi-
ciency, sustainable sites, materials and resources,
The need for reducing the environmental impact indoor environmental quality, and energy. For
humans have on nature has resulted in many new example, in order to obtain points, a particle filter
“green” solutions. These include a shift to sustain- could be implemented in the building to lower the
able materials, and especially in recent years, there concentration of a target pollutant under a thresh-
has been a greater focus on green buildings. The old value set by LEED. These target pollutants
process of constructing new buildings can result in include PM10 and PM2.5, with threshold values of
the loss of green areas, including forest or grass 50 mg/m3 and 10 mg/m3, respectively [101]. There
fields, and the design and choice of materials is a significant difference between the two sys-
changes a building’s environmental impact. Not tems, and if a building meets the requirements for
least of all, these choices affect building energy LEED certification, it would not automatically
efficiency; buildings use 40% of energy world- fulfill the requirements for Energy Star
wide. In particular, building heating ventilation [102]. IAQ is not included in Energy Star, and
and air conditioning (HVAC) systems are one of improving energy efficiency by sealing a building
the largest energy consumers worldwide [99]. can lead to poor IAQ if adjustments of the venti-
The U.S. Environment Protection Agency lation system are not made, as pollutants will then
defines green building: Green building is the prac- accumulate inside the building. On the other hand,
tice of creating structures and using processes that an increase in outdoor-to-indoor air exchange will
are environmentally responsible and resource- result in a less energy-efficient building. IAQ and
efficient throughout a building’s life-cycle from energy efficiency are both part of the idea about
siting to design, construction, operation, mainte- green buildings, and both aspects needs to be
nance, renovation and deconstruction. This prac- considered.
tice expands and complements the classical
building design concerns of economy, utility, dura- The University of Copenhagen Green
bility, and comfort. Green building is also known Lighthouse as an Example of Sustainable
as a sustainable or high performance building. Buildings
A number of standards have been created to The Green Lighthouse Building was built on the
define performance and help promote green build- campus of the University of Copenhagen in 2009
ings. This chapter focuses on two of the leading and is the first public CO2-neutral building in
standards and two different approaches: the certifi- Denmark. It has been designed to be as energy
cates given by Energy Star, and Leadership in efficient as possible while also creating a healthy
Energy and Environmental Design. Energy Star indoor environment. The tilted roof faces south-
was developed and is managed by the U.S. Envi- wards, resulting in maximal sun exposure. The
ronmental Protection Agency and the U.S. Depart- roof is equipped with photovoltaic cells, solar
ment of Energy with the goal of promoting energy thermal panels, and windows. The solar cells
efficiency. Energy Star certifies products (heating convert solar radiation into electrical current
and cooling systems, appliances), devices (home used by the building for cooling or heating,
electronics. lighting), and homes and industrial depending on the season. In summer, the build-
facilities [100]. ing is cooled from natural ventilation with air
156 Indoor Air Quality: Status and Standards

Indoor Air Quality: Status and Standards, Table 8 List of air purifying plants sorted alphabetically and their target
pollutants
Latin name Common name Pollutant References
Aglaonema “silver queen” Chinese evergreen Benzene [93]
Anthurium andraeanum Painter’s-palette Ammonia [95]
Formaldehyde
Xylene
Asparagus densiflorus Asparagus fern a-Pinene [96]
Benzene
Octane
Toluene
Trichloroethylene
Calathea vittata Prayer plant Ammonia [95]
Chamaedorea seifrizii Bamboo palm Benzene trichloroethylene [93]
Chrysanthemum morifolium Pot mum Ammonia [95]
Benzene [93]
Formaldehyde [95]
Trichloroethylene
Xylene
Dracaena derimensis variety Janet Craig Benzene [93]
Formaldehyde [95]
Trichloroethylene
Dracaena deremensis variety Warneckei Benzene [93]
Formaldehyde [95]
Trichloroethylene
Xylene
Dracaena marginata Marginata Benzene [93]
Formaldehyde [95]
Trichloroethylene
Xylene
Dracaena massangeana Mass cane Benzene [93]
Formaldehyde
Ficus benjamina Ficus Ammonia [93]
Benzene [95]
Formaldehyde
Xylene
Gerbera jamesonii Gerbera daisy Benzene [93]
Formaldehyde
Trichloroethylene
Hedera helix English ivy a-Pinene [96]
Benzene [93]
Formaldehyde [95]
Octane
Toluene
Trichloroethylene
Xylene
Hemigraphis alternata Purple waffle a-Pinene [96]
Benzene
Octane
Toluene
Trichloroethylene
Homalomena sp. – Ammonia [95]
Formaldehyde
Xylene
(continued)
Indoor Air Quality: Status and Standards 157

Indoor Air Quality: Status and Standards, Table 8 (continued)


Latin name Common name Pollutant References
Hoya carnosa Variegated wax plant a-Pinene [96]
Benzene
Octane
Toluene
Trichloroethylene
Liriope spicata Lilyturf Ammonia [95]
Formaldehyde
Xylene
Nephrolepis exaltata “Bostoniensis” Boston fern Formaldehyde [95]
Xylene
Nephrolepis obliterata Kimberly queen fern Formaldehyde [95]
Xylene
Phoenix roebelenii Pygmy date palm Formaldehyde [95]
Xylene
Rhapis excelsa Broadleaf lady palm Ammonia [95]
Formaldehyde
Xylene
Sansevieria laurentii Mother-in-law’s tongue Benzene trichloroethylene [93]
Scindapsus aureus Golden pothos Benzene [93]
Spathiphyllum “Clevelandii” Peace lily Ammonia [95]
Formaldehyde
Xylene
Spathiphyllum “Mauna Loa” Peace lily Benzene trichloroethylene [93]
Tradescantia pallida Purple heart plant a-Pinene [96]
Benzene
Octane
Toluene
Trichloroethylene

flowing in through low windows and out through generated by the solar thermal panels is used to
rooftop windows creating a natural stack effect heat the building’s water tank, and windows and
(cf. Fig. 5c). In winter, ventilation occurs through walls are highly insulated to avoid heat loss.
a heat exchanger to minimize heat loss [103]. The A healthy indoor environment is created by nat-
floors are made from concrete that acts as a ther- ural ventilation, as mentioned earlier, which
mal reservoir [104]. In winter, the floors are introduces outdoor air and removes indoor air
heated by energy from the solar thermal panels pollutants [103]. As the Green Lighthouse is
and from district heating. Sixty-five percent of located in Copenhagen, the ambient air is
the district heating is eco-friendly, detailed urban, but air pollution in Copenhagen is gener-
below, with a thirty-five percent share of renew- ally below threshold values [106]. Roof windows
able fuel [103]. In Copenhagen, 98% of district provide light which is distributed to all rooms
heating is provided by the public utilities com- with a minimum daylight factor (DF) of 2%
pany HOFOR, which produces heat by waste [103]. The DF is a measure of available daylight
incineration in a combined heat and power in a room compared to available outdoor daylight
(CHP) system. The CHP system generates under an overcast sky, given in percentage
energy by combustion of biomass (a renewable [107]. A room with a DF of 2% is considered
source) and gas and oil. The fossil energy is in the daylit, but still requires some artificial lighting to
process of being replaced by renewables, mainly perform visual tasks. Lamps in the Green Light-
wind [105]. In the Green Lighthouse, energy house are adjusted to compensate for variations
158 Indoor Air Quality: Status and Standards

Indoor Air Quality:


Status and Standards,
Fig. 7 Overview of Green
Lighthouse [103]

in natural light, to reduce electricity use a wider range of products will be available. As
[103]. The building is shown in Fig. 7. these technologies become more popular, they
Green buildings are an important step towards will also become more affordable and thus avail-
achieving the 11th UN Sustainable and Develop- able for developing countries.
ment Goal, of making cities resilient and sustain-
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Neighborhood scale Scale typical of groups of
Urban Air Quality: buildings or streets; hundreds of meters to a
Meteorological Processes few kilometers.
Porosity The volume fraction of air between
David Carruthers1, Silvana Di Sabatino2 and buildings and therefore a measure of building
Julian Hunt3 density.
1
Cambridge Environmental Research Urban air quality A general term representing
Consultants, Cambridge, UK concentrations of pollutants in an urban area.
2
Dipartimento di Scienza dei Materiali, Università Good air quality corresponds to low concen-
del Salento, Lecce, Italy trations of pollutants.
3
University College London, London, UK Urban meteorology Meteorology within an
urban area; the urban environment significantly
affects mean flow turbulence and temperature.

Article Outline
Definition of the Subject
Glossary
Definition of the Subject
Meteorological processes in urban areas that are
Introduction
relevant to urban air quality. Of most significance
Characteristic Regions of the Flow and Drivers
are the impacts of the urban morphology on the
Urban Data
mean flow and turbulence, which determines the
Computational Models for Meteorology and Air
transport and dispersion of pollutants and there-
Flow in Urban Areas
fore their concentration.
Examples of Output of Modelling Calculations
Future Directions
Notation and Abbreviations
Subscripts Introduction
Abbreviations
Bibliography Concentrations of pollutants within an urban area
depend on a number of different factors. These
Glossary include the emissions of pollutants within the
urban area, pollutant concentrations transported
Building and street scales Scales of buildings or into the area, and the meteorology within the urban
streets; tens to hundreds of meters. area, in particular, the mean airflow and turbulence
Fast approximate model (FAM) A model (which determines the movement and mixing of the
which uses approximations and parameteriza- emitted pollutants) and the temperature and solar
tions of the fine scale flow to speed up model insolation (which impacts on chemical transforma-
run times and reduce complexity. tion taking place). This entry discusses meteorology
Fully computational model (FCM) A model within the urban area with the focus being on the
which explicitly represents flow and turbu- mean flow and turbulence, as these may be substan-
lence around buildings. tially different from the upstream flow. Discussed
Mesoscale Scale of weather systems smaller here are the current understanding, experimental and
than synoptic scale but larger than micro- numerical simulation data, and the relative merits of
scale or urban scale; tens to hundreds of different modelling approaches. For discussions of
kilometers. dispersion within urban areas, see, for example, [1].
© Springer Science+Business Media, LLC 2012 163
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_427
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_427
164 Urban Air Quality: Meteorological Processes

Section “Characteristic Regions of the Flow the urban area on convergence/divergence and
and Drivers” presents the underlying concepts turning of the wind, and by temporal variations
and prediction methods related to the airflow and in the flow forced by diurnal and synoptic effects.
meteorology of urban areas that are particularly Where there are sharp variations in topography
relevant for understanding and modelling disper- the surface air flow may change locally (e.g., at
sion from the urban sources. It is noted how spa- the coast or edge of an urban area). However, the
tial and temporal patterns of flow and dispersion whole boundary layer flow does not adjust imme-
in urban areas greatly depend on their location diately to the change of surface conditions: this
(e.g., flat, hilly terrain, coastal, or desert), the takes place over a mesoscale distance LM which,
types of surface, prevailing meteorological condi- in the atmosphere, is typically of order 30–50 km.
tions (e.g., strong/weak geostrophic winds), and This distance is usually determined by the Rossby
on the patterns and forms of urban building/street/ length scale LRo ¼ hN/f where f is the Coriolis
open space (e.g., isolated buildings or canyons; parameter and N is the buoyancy frequency of the
high or low range of building heights, etc.). It will stable layer at or above the boundary layer of
be convenient to describe the flow in terms of height h. At midlatitudes f ~ 104 s1, and typi-
three characteristic ranges of length scale, namely, cally N ~ 103 s1, h ~ 1,000 m. In neutral
mesoscale, neighborhood scale, and building/ conditions, LM is determined dynamically by iner-
street scales, each with their own general features tia and turbulence stresses, when LM ~ Lf ¼ U/f,
and where different modelling approaches are usually a distance of greater than 30 km, while
necessary, depending on the requirements for close to large mountains of height HM,
accuracy and speed of computation. LRo ¼ HMN/f.
Section “Urban Data” presents some details of Figure 2 shows that in the zone where the
data, and sections “Computational Models for boundary layer is adjusting to the changed surface
Meteorology and Air Flow in Urban Areas” and conditions, there is an internal layer with depth
“Examples of Output of Modelling Calculations” l(x, y) above the ground, separating the air flow
provide details of modelling methods for flow in and pollutants above and below it. The depth of
urban areas and examples of model calculations. this layer tends to increase slowly over the area
where the surface conditions (temperature or sur-
face roughness) have changed; see, for example,
Characteristic Regions of the Flow and [2, 3]. Over the mesoscale LM, the internal layer
Drivers reaches the top of the boundary layer, and then the
vertical profiles of velocity and temperature over
Characteristic Regions of the Flow the whole boundary layer are changed.
In urban areas, there are usually considerable var- Over shorter horizontal scales, the internal layer
iations in the types, sizes, and layout of buildings depth is much less than h. Here the perturbed flow
and streets as illustrated in Fig. 1, and over larger has separate characteristics over the intermediate
urban areas there are often also significant varia- neighborhood scales LN (≲5 km) and over the
tions in the natural topography. Both these urban shorter building/street scales LBS (≲300 m). The
scale features and the meteorology have general former scale LN extends over groups of buildings/
characteristics over different length scales. These streets of similar size and type, and the internal layer
need to be understood and related to each other depth lN is greater than the height of the envelope or
when developing a picture of the urban airflow as canopy of the buildings HC. Note that there is sig-
illustrated in Tables 1 and 2. nificant mass, momentum and energy transfer
Over level terrain, except in very light wind between the flow in and above the canopy on this
conditions, the direction and speed of the airflow scale. Even though the neighborhood scale includes
only changes significantly over the mesoscale many buildings, the types of buildings and their
(of order 30 km) or greater scales. These changes patterns have significant effects on this exchange
are determined by Coriolis effects, by the effect of process and on the flow within the canopy.
Urban Air Quality: Meteorological Processes 165

UG
Lo

h UG
Hc′

UH Hc

LI
z = zs

UB

Change in surface z0, Fθ, θs

Urban Air Quality: Meteorological Processes, geostrophic wind, UB is the typical wind speed associated
Fig. 1 Characteristic features of the terrain, buildings, with local buoyancy effects, for example, downslope
and meteorology on the meso- (regional) scale of signifi- winds from nearby mountains. Hc is the canopy height
cance for urban dispersion. Lo and LI are the overall and and Hc0 is the standard deviation of canopy height
inner city length scales, respectively. Note that UG is the

Urban Air Quality: Meteorological Processes, Table 1 Scale ranges of urban air flow and dispersion
Relation to urban and
Range Determining factor(s) meteorological scales
1. Mesoscale Flow over buildings LM ~ LO for large urban
LM (~30 km) areas
Significant orographic/Coriolis effects lO (x ~ LM) ~ h
Surface influences and pollutants mixed through boundary
layer
2. Neighborhood Flow and dispersion above and between buildings LN < LO ≲ LM
scale Average geometrical features dominate mean flow/dispersion Typically LN ~ LI, inner city
LN (1–10 km) scale
Growing internal layer above buildings l(x ~ LN) ≲ h
3. Building/street Flow and dispersion determined by features below building 10 H ≳ LBS ≳ w, b, d
scale level (except for elevated releases)
LBS Mean geometrical and flow features on scale LBS (not smaller) l ≲ H (this defines upper
(~3–1,000 m) mainly determine dispersion scale of LBS)
Internal mixing layers below/above buildings are of order of
building/street dimensions

Mesoscale categorized in Table 2 according to the relative


In the following section, the main features of the effects of buoyancy to inertial forces produced by
flow and meteorology in the three characteristic orographic or heat island effects on the one hand and
flow regions of urban areas are discussed, beginning the effects of Coriolis forces acting over the overall
with those on the mesoscale. These are broadly scale LO of the urban area on the other. The
166 Urban Air Quality: Meteorological Processes

Urban Air Quality: Meteorological Processes, Table 2 Main types and features of urban mesoscale

Increasing effects of orography/heat island, lighter geostrophic wind →

F = UG/UB >1 ~1 <1


(typically windy (typically moderate (hilly terrain; near coast)
environment over flat wind over flat surface)
LO/LRO
plain)
←Increasing scale

(i) Roughness slow down; (iii) Weak flow (v) Slope flows in open
<1 boundary layer depth convergence, change in valleys; sea breezes; slope
~ varies. stability over urban flows and pooling in
area bounded valleys

(ii) in addition to effects (iv) Strong central (vi) Interactions between


of (i) above anticyclonic convergence and orographic and urban heat
turning of wind; weak cyclonic turning. island flows.
>1
~ convergence /divergence Significant variations in
on left/right. orographic and heat island
flow across the urban area.

Note: UG is the geostrophic wind speed,


UB = (gh|Δθ|/θ)1/2 is the buoyancy-induced local wind speed
Lf is the Coriolis advection length (= U/f)
LRo is the Rossby length scale defined by stratification and Coriolis effects (= hN/f)

buoyancy and inertial forces are essentially indi- F > 1, and Lf, LRo > LO, the scale of the urban
cated by the value of the Froude number, defined area. For case (ii), as LO increases, and if there are
as the ratio of the geostrophic wind UG to the no thermal effects, Coriolis effects begin to
average velocity UB produced by the buoyancy become significant with turning of the wind.
forces acting over the urban area, i.e., F ¼ UG/UB. Case (iii) corresponds to the case in which the
UB is driven by the horizontal temperature and urban heat island, and hence the buoyancy veloc-
hence density changes A6, which may be natural ity, increases. This will change the stability and
or caused by the urban heat island, and is defined by
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi boundary layer depth over urban areas. But if the
U B ¼ gl 0 j Dy j =y, where l0 is the internal layer area is even larger so that Lf, LRo < LO, as in case
thickness or the height of the nearby mountains if (iv), then the heat island and Coriolis effects are
these dominate the flow and g is gravitational accel- larger. In this case there is convergence with the
eration. Note that Δθ/θ depends on a number of flow toward the urban area turning cyclonically
features of the urban area, the most important (i.e., anticlockwise in the northern hemisphere), as
being the increased heat storage due to urban build- has been measured, especially at night [3].
ings, which increases temperature (urban heat Strong buoyancy forces occur in the presence
island) and the impact of vegetation inside and of mountains and sloping terrain, so that F < 1,
outside the urban area, which may reduce tempera- leading to marked diurnal variations in the wind
ture. Typically the heat island causes increases in speed and direction, over the urban area and out-
temperature of a few degrees in a small town [4, 5] side it. Such areas are associated with sudden
so that |Δθ|/θ ~ 0.01 and UB ~ 3 m/s. Larger urban changes in the airflow, internal fronts, and pooling
areas show a much higher urban heat island effect of the air in valleys, all of which greatly influence
(up to 12 C for cities in arid or semiarid environ- dispersion of air pollution.
ments, [6]) leading to larger values of UB. Coriolis Note that because of release of heat stored in
effects are significant if Lo is comparable or greater buildings at night and increased mixing due to the
than the mesoscale length scales. high surface roughness, the static stability of the
Referring to Table 2, it is seen that for typical air stream usually changes as it moves into and out
small to medium scale urban areas (case (i)), of the urban area, typically becoming less and
buoyancy and Coriolis effects are negligible, more stable, respectively.
Urban Air Quality: Meteorological Processes 167

a z ~Io

z ~ IN

z∗

Io
Hc

LA
LN

b lN

Z∗

Hc

Urban Air Quality: Meteorological Processes, buildings. lO and lN are the heights of the perturbed layers
Fig. 2 Characteristic features of building envelope and above the buildings; z* is the height of the top of the shear
zones of air flow in neighborhod scale. (Note that the layer above the buildings. LA is the adjustment distance.
definition of this scale depends partly on the level of detail (b) Non-porous canopy, where the mean flow passes over
of the computation.) (a) “Porous” canopy – with isolated the canopy

Where there are significant buoyancy forces or spaciously designed urban centers, the buildings
orographic effects, the boundary layer profiles are effectively isolated. However, in dense sub-
over the urban area and downwind may not sim- urbs and inner city areas there may be “canyons”
ply adjust toward the equilibrium states found in with long rows of buildings neighboring streets.
neutral, stable, and unstable boundary layers over The suburban areas or spacious urban centers
flat terrain. In fact there are characteristic features are essentially porous to the oncoming boundary
of the air flow on these scales, especially near layer; the airflow slows down as it passes between
hills, coasts, and urban/rural boundaries, that can the buildings, as a result of both the bulk displace-
significantly affect dispersion, such as blocked ment of the flow over and around the “envelope”
flow, unsteady slope flows, gravity currents, and or canopy of the buildings and their drag. Down-
boundary layer jets [7, 8]. wind of a characteristic adjustment distance LA
(which is of the order of H(d2/wb) or H/β where
Neighborhood Scale 1-β is the volume occupied by the buildings and β
The characteristic features of the air flow on the is the volume of air between buildings and there-
neighborhood scale are dependent on the group- fore a measure of porosity), or typically 10–30
ing of the buildings/streets (with average building building widths [9], the drag force dominates but
height H, breadth b, width w, and distance is weakened by the sheltering effect of upwind
between buildings d). In suburban areas or buildings (see Table 3). Over this adjustment
168 Urban Air Quality: Meteorological Processes

Urban Air Quality: Meteorological Processes, Table 3 Typical street/building configurations in urban areas

Increasing separation, d →

b/s
>
~2 <
~1
← Increasing width w

b/w

(i) Canyon (H/w > 2) (iv) City squares*, parksides


>
~10 Residential street (H/w <
~ 1)

(ii) Long blocks (e.g. industrial (v) Enclosed spaces (e.g. courtyards)
1–5
estates)

< (iii) Closely-packed industrial sites; (vi) Square blocks (e.g. houses), H/w <
~1
~2 ancient settlements** Office blocks, H/w ≥ 1

* Long buildings with large space are rare except for city squares/courtyards.
** Wide buildings close together are rare except on certain industrial estates.
In the above s is the distance to the nearest building.
Note:
(a) Mixed cases occur, such as office blocks as part of streets (so H/w varies).
(b) Long and square blocks are usually aligned in streets (i.e. angle between two nearest cases Δθ is 180°).

×
×
Δθ

w ×

distance the air flow above the buildings first Grimmond and Oke [10], Britter and Hanna [11],
accelerates as a result of the vertical displacement and Belcher et al. [9]. Application of Eq. 1
by the buildings, and then decelerates as slow requires knowledge of z0, zd, and u*. The estima-
moving fluid is expelled from below the level of tion of these parameters is not straightforward in
the building envelope or canopy. Downwind of urban areas. The determination of the friction
the adjustment distance (Fig. 2a), if the neighbor- velocity is also difficult because of the large var-
hood scale is large enough (i.e., LN > LA~ 30 H), iability of momentum fluxes inside the urban
the air flow (speed Uc) within the canopy is largely canopy [12].
driven by turbulent shear stresses generated in the The aerodynamic roughness length z0 is a mea-
shear layer just above buildings Hc < Z < Z* < lN(x) sure of the turbulence-generating capacity of the
(rather than by the oncoming airflow). Above this ground. The larger the roughness length, the more
shear layer, Z* > Z > lN(x), the airflow is charac- turbulent the air for a given wind speed. Gener-
teristic of a surface layer with displacement height ally, tall features such as buildings have a larger
zd, so that roughness length than short features. However a
densely built area may have a smaller roughness
 
u z  zd length than a less dense one because the interac-
U ðzÞ ffi ln , ð1Þ
k z0 tion between the air and the region beneath is
reduced. The wind speed close to a rough surface
where z0 is the aerodynamic roughness length, is reduced by friction and a velocity profile can be
and k is von Karman’s constant as discussed by plotted from the surface to the free fluid. This
Urban Air Quality: Meteorological Processes 169

reduction in wind speed as the surface is Starting from the lambda parameters zd and the
approached can be equated to a transfer of momen- aerodynamic roughness length, z0 can be com-
tum from the bulk fluid to the surface, caused by puted using the equations derived by Macdonald
the friction force. The momentum transfer et al. [18]:
(transport) is large if the roughness is large.
zd  
The displacement height zd according to ¼ 1 þ lp  1 alP , ð3Þ
Jackson [13] can be interpreted as the level of H
mean momentum absorption. According to the
(  
0:5 )
z0 zd 0:5bCD lF zd
Jackson’s formulation this can be determined by ¼ 1 exp  1 ,
H H k2 H
the following relation:
ð4Þ
Z zd  
 
ðzd  zs Þ u0 w0 s u0 w0 s  u0 w0 ðzÞ dz, ð2Þ where α ¼ 4.43, β ¼ 1.0, k ¼ 0.4, CD ~ 1.
zs Even though Eqs. (3) and (4) provide good
operational estimations for zd, as far as z0 is
where zs is the average elevation of the surface and concerned, there is a warning due to the intrinsic
u0 w0 s is the peak of the shear stress profile. Accu- difficulty linked to limited fetch, typical in urban
rate knowledge of the aerodynamic characteristics areas, which prevents the flow from being in equi-
of cities is vital to describe, model, and forecast librium with the changing surface as noted above.
the behavior of urban winds, turbulence, and the Equations (3) and (4) provide a first estimate of
dispersion of pollutants at all scales. The calcula- surface characteristics, but aerodynamic proper-
tion of zd (which is of order H) based on Eq. 2 is ties need to be evaluated on a case by case basis.
rarely feasible due to the lack of measurements. Besides, while z0 is an important parameter for the
The classical way to estimate z0 and zs in open flat above canopy flow description as expressed by
terrain is based on the measurements of wind Eq. (1), within the urban canopy its use can be
speed profiles from a tall mast or, less accurately, replaced by a combination of lambda parameters
on the inference from published aerodynamic and their variation with height [19].
roughness values for similar terrain elsewhere Going back to the discussion on the flow char-
[14, 15]. Both methods, however, are very diffi- acteristics, it is worth mentioning that despite the
cult to apply to urban areas. A promising alterna- unevenness and inhomogeneity of these boundary
tive that has become available in recent years, due layer flows, the ratios of the r.m.s. values of the
to increased computing resources and the avail- three components of turbulent velocity (su, sv, sw)
ability of high-resolution 3-D building databases, to the friction velocity u* are quite comparable
is based on the calculation of z0 and zd from the with their values over level terrain, i.e., su/u
analysis and measurement of the city geometry ffi 2.5, sv/u ffi 2.0, sw/u ffi 1.3 [20].
(urban morphometry). Morphometric methods Downwind of the “neighborhood” or urban
express the cities’ aerodynamic characteristics in area where the buildings decrease in height, the
terms of average building height (H), planar area mean air flow descends and accelerates. Typically
index (lp), frontal area index (lf), and other mea- in neutral conditions the mean velocity adjusts to
surable parameters related to the urban morphol- within 10% of its ultimate (rural) value within
ogy (e.g., [10, 16, 17]. While lp for a given about 30 lengths [21].
neighborhood is independent of wind direction, When the urban area is more densely packed
lf represents the total area of buildings projected with buildings and they are distributed in the
into the plane normal to the incoming wind direc- “canyon” form, the urban area is effectively
tion and is a function of orientation. For a given “non-porous” (Fig. 2b). An example of this case
wind direction, lf is smaller if the wind angle is is the central area of Nantes [22]. The air does not
oblique, rather than perpendicular, to the front flow continuously between the buildings but the
face of the building. mean streamlines and the cloud/plume pass above
170 Urban Air Quality: Meteorological Processes

the buildings and air flow is largely above the breadth b to separation distance d from the
canopy envelope (average height HC); the ratio nearest building, on the ratio b/w of breadth to
Uc/UH is much less than sw/UH. the width w of the building, and on the relative
Within the canopy the flow depends on the height to width ratio H/w. When there are many
particular street and building configuration at buildings, as in urban areas, these flow interac-
that scale. There are mean flows along streets at tions build up into characteristic flow patterns;
an angle to the mean flows above the buildings, this is now examined.
which results in extra lateral diffusion. Separated Buildings b/w, w/b < 2. The separa-
The flow above the canopy is essentially equiv- tion distances d are large enough that b/d  1/3
alent to airflow over a wide hill with length LN and ((vi) of Table 3 and Fig. 3a). The flow around each
height HC, but with a significant value of the building has approximately the same form as that
roughness length z0 that is of the order of the of an isolated building, with recirculating flow
thickness of the shear layer over the buildings regions, turbulent wakes, and horseshoe vortex
and the “canyons” between them [23]. The flows structures around the base of the building. In
in the inner layer above the buildings and in the slightly stable conditions the vortex structures
wake downwind of the neighborhood region are can persist far downwind but in most urban
similar to those for the porous case. cases where the flow is neutral and highly turbu-
lent they are not significant. On the other hand the
Building and Street Scale turbulent wakes from upwind buildings do impact
On the building/street scale there are also charac- on those downwind, enhancing the mixing. Iso-
teristic features of the flow corresponding to dif- lated buildings, especially in slightly stable con-
ferent categories of building street shape and ditions can produce swirling wakes far downwind
configuration. Various planning criteria and con- [25]. When there are marked variations in the
cepts have been proposed for defining these cate- height of adjacent buildings, the wake vorticity
gories, for example, rugosity (or mean canopy shed from upwind buildings can produce sharp
height HC), relative rugosity (defined by building down-flows and increased trailing vorticity in the
height variability or canopy height variability H 0C), flow direction as discussed by Lawson [26]. These
sinuosity (of canyons), the Sky View Factor effects contribute to mixing between the canopy
(SVF), which signifies the fraction of sky dome and external flow.
visible from a specific outdoor position and is For tall buildings that are not closely packed
important for estimating the amount of incoming and where H/b > 1 (Fig. 3b), there is strong
solar radiation for energy calculation, and the mixing in the horizontal plane and to a lesser
“compactness index,” which is defined as the extent in the vertical direction because of the
ratio of building surface area (excluding the plan high turbulence generated. Buildings placed suf-
area) to the surface area of a cube that has the same ficiently close to each other may result in wake
volume as the building. For microscale phenom- interaction, which tends to cause downwash [27]
ena the urban morphometry is the more important, and strong swirl around the sides of tall buildings.
but at the mesoscale both the geometry and sur- This enhances vertical mixing in the lower part
face thermal characteristics play an equal role of the downwind wakes and through lateral
[24]. These, and related concepts, have been convergence reduces their downwind extent.
used to guide the suggested categorization When b/d < 1/3, corresponding to long buildings
shown in Table 3 for building/street configura- that are sufficiently separated from each other, the
tions and the consequences for air flow features flow over an upwind building can descend into the
illustrated in Fig. 3. space between the buildings. This flow is signifi-
Fluid mechanical studies have shown how cantly sheltered and stagnation areas are larger
flows around individual buildings become sig- than for isolated buildings.
nificantly distorted in the presence of other Close Packed Buildings not Aligned. In some
buildings depending on the ratio b/d of the city centers and some types of industrial plant, the
Urban Air Quality: Meteorological Processes 171

spacing between buildings are within about two or wakes tend to be reduced in length because of
three widths (i.e., b/d ≳ 1/3), but the gaps between cancellation of vorticity.
the building do not form continuous “canyons” Where the separation distance is smaller, i.e.,
((iii) of Table 3). The air flow passes around the b/d  1, the flow is further changed because there
buildings and the streamlines move irregularly may be other complicating geometrical factors,
between the buildings, converging and diverging such as the effect of a courtyard, which further
as they do so, as sketched in Fig. 3c [28]. The slows up the flow, or open gateways, which can

a Uw Uw

w
d

f
UH

c ~
y
~
x

(xs(2), ys(2))

y ~ W
y
(xs, ys, zs) (1)
(xs , ys ) (1)
~ yc(X)
x
x b

Lse

Urban Air Quality: Meteorological Processes, Fig. 3 (continued)


172 Urban Air Quality: Meteorological Processes

UH
b
H

W d

Typical stagnation regions

w
d
Vs
f
UH

Urban Air Quality: Meteorological Processes, is yc(x); xe, ye are coordinates parallel and perpendicular to this
Fig. 3 Typical building/street configuration. (a) Normal streamline. Streamlines marked with small circles are mean
approach angle f small enough (i.e., cosf > 2w/d) for streamlines cstag passing through stagnation points where
independent wakes to be formed (approximately parallel to plumes split. The cloud/plume resulting from the source is
the approach wind). Note the complex forms of building the shaded area enclosed by heavy dashed line. LSe is the
wakes, in which swirl may persist. (b) Effects of uneven effective size of the source outside which atmospheric tur-
building heights. Note strong reverse and downdraft winds bulence determines the dispersion. (d) Enclosed spaces –
(e.g., [26, 27]). (c)nStaggered
o tall buildings (comparable Typical instantaneous streamlines of the large-scale flow in a
ðiÞ ðiÞ courtyard, where b/d ~ 1, b/w ~ 3, H/d ~ 1/3, and H/w ~ 1.
height), located at xB , yB , close to each other. Note
The shaded area indicates the region of highest concentra-
how wakes can “disappear” through converging streamlines, tion of matter released in the courtyard. (e) Normal approach
while lateral diffusion is enhanced by diverging streamlines angle f large enough (i.e., cosf ≲ 2w/d) for wakes to merge
(“topological” diffusion). Streamlines are indicated by solid and “canyon” flow to develop in streets between the
arrowed lines. The streamline through the source at (xs, ys, zs) buildings

lead to sufficiently high local winds that affect the component UC below the building height, i.e.,
overall flow pattern (Fig. 3d). Here the interaction UC/UH ≲ 0.1. However, the turbulence level is
between the vorticity layer from the top of the quite high in these recirculating flows, with
buildings and impacting on surrounding buildings su ~ sv ~ (0.5–1.0) · su(z*) ~ 1.2–2.5 u*, so that
leads to even more complex recirculating flows su ~ Vs [23].
than in street canyons. However, because of Flow Aligned with Rows of Buildings (b/w > 1,
the finite extent of these flow regions, it can gen- H/d ≳ 1/3). In this case buildings are located in
erally be assumed that (unlike elongated street rows with separation gaps d that are comparable
canyons) there is only a small mean velocity with their height H (i.e., streets). The case includes
Urban Air Quality: Meteorological Processes 173

buildings that are loosely aligned in rows or con- how the mean transport direction differs from the
tinuous canyons ((ii), (iii), and (iv) of Table 3). mean flow above the buildings, the rapid vertical
Where the downwind buildings are nearly aligned and horizontal spreading of plumes in wakes and
with the wind (Fig. 3e, cos f  w/d), they distort canyons, the more complete mixing by the
the wake’s vorticity so that the wakes tend to be interacting wakes (with lower relative levels of
aligned with the building [29]. The recirculating fluctuation compared with rural terrain), the tran-
flow in the wake of the upwind row tends to extend sition of dispersion below the buildings level to
across the “street,” and there is usually a significant above them and the variation in concentration
mean velocity Vs along the street. The mean flow downwind of sources and within the buildings.
has a component along the street and, when the In the context of urban air quality, the full use
external flow is not aligned with the “canyon,” a of models based on an up-to-date understanding
swirling motion in the perpendicular direction that of the flow as described in the previous sections is
tends to extend up to the top of the buildings. The somehow limited by the scarcity of available data.
peak mean and fluctuating velocities near the Urban flow and dispersion models require input
ground are comparable with those at the level of information and source distribution data about the
the top of the buildings. The key quantitative mean flow field, turbulence, and source distribu-
parameter for dispersion modelling is the ratio of tion. Until very recently velocity field data in
the mean wind along the street Vs to the mean wind urban areas were quite sparse and typically
UH above the buildings at the height H (in the derived from the experiments in the USA. Some
approach flow). Computation and field observa- progress has been made in recent years with some
tions [23] have suggested a large range of this field experiments performed in some European
ratio from 0.3 to 1.0. The analysis also suggests cities even though one has to accept that datasets
that the value of Vs can be quite sensitive to the from field experiments are yet not fully complete
value of Vs at the upwind end of the canyon. Thus a given the inherent difficulty and the cost of urban
major crossroad can have a large effect on the flow and dispersion experiments. This aspect has
canyon flows downwind. motivated the increase of laboratory experiments
In conclusion it has been shown that most of of flow and dispersion over simplified groups of
the usual types of building/street shape and con- buildings (building arrays) as well as over scaled
figuration found in urban areas can be categorized reproduction of real city quarters. In addition to
in geometrical terms that also correspond to the field studies, laboratory experiments allow easier
characteristic air flow patterns found in these sit- validation of physical or numerical models
uations for typical wind conditions. In particular because of carefully controlled flow conditions
there is a major distinction between, on the one and the possibility of making numerous measure-
hand, flows determined by random interactions of ments. The laboratory experiments can be either
wakes of well-separated buildings and, on the wind-tunnel experiments [30–32] or water-
other hand, flows where the interaction of wakes channel experiments [33]. Some field studies
is of less relevance, for example, highly organized have focussed on real cities, releasing a tracer
“canyon” like flows that occur when the buildings gas in selected neighborhoods, for example:
form street canyons or, if they are separated, when Copenhagen [34]; Salt Lake City, “Urban 2000”
they are positioned along streets and flows in [35]; Oklahoma City, “Urban Joint 2003” [36];
enclosed areas (e.g., courtyards) or between very Basel (BUBBLE experiment) [37]; London (the
densely packed buildings. Dispersion of Air Pollution and its Penetration
into the Local Environment known as the “Dap-
ple” experiments) [38, 39].
Urban Data The advantage of such experiments is to simu-
late flow and pollution dispersion in real condi-
Experiments and dedicated simulations have tions, but an important drawback is that the
shown features of urban dispersion at the neigh- complexity of the urban morphometry can
borhood and street buildings scale. This includes obscure the “true” impact of buildings from
174 Urban Air Quality: Meteorological Processes

other complex phenomena due to the specific in July 2003, Oklahoma City, showed that a stable
configuration of the selected city or neighbor- layer is often observed overnight, with a nocturnal
hoods. In the case of the Mock Urban Setting jet. Thus, there is no common pattern regarding
Test (MUST, [40]) it was determined that the the frequency of stable conditions; such condi-
focus would be on a simplified representation of tions are a strong function of thermal advection
a city by modelling it as a regular array of ship- due to regional scale flow processes and also
ping containers, while keeping meteorological depend on the specific materials used in the dif-
conditions real. This study has helped to clarify ferent cities.
and give scientific evidence of specific flow phe- The above are only some examples and are far
nomena as outlined in the previous sections. One from being a complete discussion of specific
important aspect for dispersion application has results obtained from the urban experiments.
been the quantification of the deflection of the
mean plume axis relative to the incoming wind
direction induced. This can be significant, being Computational Models for Meteorology
up to 23° for a wind direction of 27° relative to the and Air Flow in Urban Areas
axis of the array, as found in the MUST experi-
ment. Extrapolations to the real conditions are not This section discusses those computational
always straightforward. The full field experiments models for both meteorology and air flow in
mentioned above confirmed that, depending on urban areas that are used as input to models for
building density and morphology, transport and calculating dispersion. The numerical and physi-
dispersion may lead to complications not cal basis and operational attributes are summa-
observed in simpler building array distributions. rized in Table 4 for the three ranges of length
Near street level, for example, the dispersing scale introduced in section “Characteristic
plume may travel several blocks in a direction Regions of the Flow and Drivers”, and for the
opposing the prevailing wind and many blocks different types of model, ranging from off-line,
laterally. This topological dispersion can lead to fully computational models (FCM) to the fastest
secondary sources and significantly alter the rate approximate models (FAM) that can be run on
of lateral dispersion. A ground-level source can PCs. The choice of the model depends on their
rise several hundred meters in depth in less than a practical purpose (in relation to dispersion model-
block when caught in the updraft just downwind ling), the required level of spatial/temporal detail
of a tall building. Buildings also alter the timing of and scientific understanding involved, and on the
the transport and dispersion, generally resulting in detail and accuracy of meteorological and topo-
much longer residence times as compared to open graphical input data. For research and for off-line
terrain. Even though it is difficult to generalize the validation studies, a variety of types of model tend
time of residence of a pollutant cloud, the Bir- to be used: some studies require great detail and
mingham experiments suggested a few hours for a accuracy about particular or commonly occurring
single source. However, the Dapple experiments situations; others require simpler models for rap-
did not give a definite conclusion on this. idly calculating a wide range of meteorological
A further observation important for air quality and topographic boundary conditions. When
applications is that the experiments have shown models are analytically based, their predictions
the presence of stable stratification during the can be easily understood and may be expressed
night when consequently street level flow is less in useful formulae.
well coupled to the upper level reference. This The reason why it is necessary to have different
might be more frequent in US cities than in types of model for the different distances is
European cities. As observed by Barlow et al. because every type of model can only represent
[39], stable conditions occur in London only occa- a finite range of length scales, limited by the
sionally. The analysis by Allwine et al. [35] car- capacity and speed of the computational systems
ried out using data from the Joint Urban campaign and data input.
Urban Air Quality: Meteorological Processes 175

Urban Air Quality: Meteorological Processes, Table 4 Types of computational models for urban meteorology and
air flow
1. Mesoscale
(i) Full computational models (FCM)
Based on grid box numerical methods; full physics (fluid dynamics and thermodynamics)
Input: from synoptic (or regional) numerical weather prediction models and local surface conditions, for example,
surface fluxes for heat, Fθ, water vapor, Fv, roughness length, z0(x, y), and surface elevation, zs(x, y)
Output: mean flow, turbulence statistics from above building envelope up to tropopause as a function of space and time
over the urban area
Typical number of grid boxes for 1/3–1 km resolution on 30–100 km grid is 106–107. Takes about 3 h per 1 simulation
hour, faster for lower resolution model
(ii) Fast approximate models (FAM)
(a) Flow perturbation models (suitable where UG/UB ≳ 1) using fast/approximate numerical and analytical methods,
simple physics (for turbulence, stratification profiles), input from observational data (reduced) or NWP models and from
local surface conditions
(b) Local flow/thermal models (especially where UG/UB ≲ 1) using formula/fast approximate models for special
conditions/physics, for example, slope winds, sea breeze, and thermal convection;often adjusted for local conditions
(c) Mass consistent models to compute flow fields given data at several points in the flow domain and surface elevation
zs. (Only suitable if such data exist for all relevant cases.)
(d) Typical resolutions can be on a horizontal scale of 100 m or less
(e) These models can be run over a few minutes on PCs for each case. Current simplified models do not account for
unsteady conditions over large urban areas (where LO/Lf, Lc/LRo ≳ 1)
2. Neighborhood scale
(i) FCM using CFD methods
Grid point numerical models with approximate representation of buildings and open spaces (as porous medium;as
distributed forces;or as approximate shapes);approximate turbulence and heat transfer models;input from mesoscale
models or measured data
Output: mean and turbulence profiles within the building envelope and up to the boundary layer/inversion layer height
Typical horizontal resolution is greater than the spacing between buildings. For a “neighborhood” of 5 km (e.g., city
center) with 106–107 points, the resolution would be 100 m for an “accurate” computation
(ii) FAM
(a) Flow perturbation models (applicable where ln z0 or Fθ vary significantly) using fast/approximate numerical and
analytical methods with buildings/open spaces described by average properties and their relative fluctuations (e.g.,
average building height H, spacing d, and also typical r.m.s fluctuations in H and d); simple turbulence and heat transfer
models for canopy flows; input from mesoscale models or local data, and estimates of distributed effects of buildings
Output: mean flow within and above the canopy and turbulence above the canopy
(b) Local flow/thermal models (where ln z0 or Fθ are approximately uniform). Formulae based on local dynamical and
thermodynamic balance and estimates of distributed effects of buildings;input based on average wind, thermal flux, and
estimates of distributed effects
3. Building/street scale
(i) FCM using CFD methods
Grid box numerical models with accurate representation of buildings, approximate turbulence and heat transfer models;
input from neighborhood models or assumed data. (Very fast versions using idealized (e.g., inviscid) equations with
finite numerical diffusion and approximate boundary conditions for buildings.)
Output: mean flow and turbulence profiles around buildings of different shapes and grouping within an urban area.
Typical computational domain is greater than building length or spacing L, or d (100 m) and grid size of 1 m or less.
Note: sensitivity to inflow conditions from other buildings and atmospheric turbulence. Models better for clusters of
buildings than isolated buildings (where large-scale atmospheric turbulence has less influence). Simpler methods are
accurate/fast enough for practical use in off-line diffusion calculations
(ii) FAM
(a) Turbulent wakes of individual buildings based on perturbation methods and typical flows near buildings
(b) Closed packed buildings modelled by ideal (potential) flow
(c) Idealized models for interactions when wakes of upwind building impinge on downwind structures
(d) Canyon models (semiempirical formulae – not yet well established)
(e) Canyon/street intersection models (e.g., ideal potential flow)
176 Urban Air Quality: Meteorological Processes

Mesoscale Models wind direction in changing meteorological condi-


On the mesoscale range, the inputs to the models tions, and in complex terrain, arise from using
are the representation/parameterization of the these models with finer resolution of the order of
topography and the natural features of the surface 1 km or less. However even with finer resolution
necessary for computations down to the smallest and complex modelling, such models still cannot
scale LM/RM (which typically is of order predict some significant features of surface layer
1/3–1 km). This is therefore the scale over which turbulence, such as evening transition of upslope
the surface conditions are averaged, including flows and formation of gravity currents, or calcu-
ground surface elevation zs(x, y), roughness length late relevant statistics of the turbulence for disper-
z0(x, y), surface heat flux Fθ (x, y, t), and surface sion models, unless they are used as large eddy
temperature θs(x, y, t) (which is usually derived in simulations [47], which, because of computa-
operational mesoscale models by coupling the tional requirements, is currently only possible in
atmospheric model to a thermal model for ground research mode.
temperature, allowing for radiation from/to the As explained in Table 4, these models take
earth’s surface). In fully computational models, many hours to compute a single meteorological
FCMs, the boundary conditions at the edges of situation. Nevertheless, they are sufficiently reli-
the domain (and, in some models, above the able indicators to be used operationally. Fast
domain) have to be specified and are usually approximate models, FAMs, for air flow and
derived from larger scale regional or global meteorology over mesoscale distances are being
numerical models. These are usually updated at developed, based on recent research. These
regular intervals, for example, every 3–12 h, with models are useful as qualitative guides to the
observational data taken at all levels in the atmo- complex flow that might occur on the mesoscale,
sphere. This process of “data assimilation” is also for quantitative predictions as input to dispersion
beginning to be applied directly to mesoscale computations.
models, for example, in urban areas with many As shown in Table 4, when local buoyancy
measurement sites. effects are weak (i.e., UG/UB  1), the air flow
A critical feature of any FCM, especially in the over an urban area is generally a perturbation of
boundary layer and when the flow is influenced by the oncoming flow. Then, from semi-analytic
mountains, buildings, surface heating etc., is the models using perturbation methods, faster com-
representation of the effects on residual putational schemes have been devised, and are
(or computed) scales greater than LM or RM of being developed in a general way to allow for
the turbulence at the smaller space and timescales. orography, roughness change, and some effects
Some models, such as HOTMAC [41], contain of surface heating [8, 48]. Although these are
quite complex sub-models of the turbulence sta- perturbation methods, the changes in wind speed
tistics (with extra equations for the turbulent and direction predicted (and verified) by these
kinetic energy and turbulent dissipation rate models can be quite large (~50% or more).
(k-ε)), while others, for example, WRF [42], The perturbation modelling approach being
COAMPS [43], MM5 [44], MESONH [45], and adopted in this range of meteorological flows is
UK Met. Office unified models [46], use eddy similar to that used for sub-mesoscale/
viscosity or even simpler parameterizations (e.g., neighborhood scale orographic flows (for exam-
assuming a known form of the velocity profile). ple, in the FLOWSTAR model [49] and
The experience from field studies in the USA is RIMPUFF [50]), the main difference being that
that for urban areas located on sloping terrain over the larger scale the internal layer l reaches the
where buoyancy forces are significant (i.e., top of the boundary layer h, so that the inversion
F ≲ 1), the models with the more complex turbu- height is affected and Coriolis effects have to be
lence models are more accurate in these condi- included (which, for example, significantly influ-
tions. But the greatest improvements in accuracy, ences flows along coasts and up and down large
especially in predicting the mean wind speeds and river valleys, [51]). Typically these models are run
Urban Air Quality: Meteorological Processes 177

in the steady state. Once the time dependence over resistance. In the case of effectively porous build-
several hours is significant, a fully computational ings (Fig. 3; category (i) of Table 3), the effect of
model is necessary. the buildings is estimated by a drag coefficient
When buoyancy forces are significant, UG/ averaged over the whole volume occupied by the
UB < 1, no FAM is yet available to cover all the buildings and the space between them (typically
most significant types of air flow and meteorolog- this is of the order of the porosity β).
ical conditions that might be needed for dispersion The FCM input is the mesoscale flow field
calculations. However, models and physical esti- approaching the neighborhood region (or the
mates have been derived for some particular situ- flow leaving the adjoining neighborhood), for
ations, especially when Coriolis forces play a example, suburbs adjoining a city center as in
small role, for example, in wide valleys with low Fig. 1. FCM output will be the mean flow and
slopes, large heat island effects, and sea/lake basic turbulence statistics that depend on the par-
breezes [48, 52, 53]. Not only are the quasi-steady ticular closure model used, for example, mixing
features of these flows now quite well described, length, turbulent energy-dissipation (k-ε) closure,
but also their time/space dependence over the or Reynolds stress closure [54, 55]. All three of
diurnal cycle. In the absence of strong geostrophic these models lead to estimates of turbulent kinetic
winds (or very stable local conditions) the local energy, but only the latter also provides estimates
diurnally varying buoyancy forces may control of length scale, and the space/time dependent
the flow and therefore they are quite predictable evolution of turbulence structure, which is signif-
(e.g., a valley wind, or sea/lake breeze on a still icant where the areas of building density or height
day). Since the single most important aspect of the change sharply. The third method allows for the
air flow needed for dispersion calculations is the anisotropy of turbulence, which changes in these
direction of the wind, such physically based transition zones. Such models predict the mean
models provide vital information for estimating velocity field everywhere (spatially averaged over
the dispersion in complex terrain. the grid box) and the turbulence outside the can-
opy. Within the canopy, where large-scale inho-
Neighborhood Scale Models mogeneous turbulence is generated by the shear
On the neighborhood scale (typically 5 km), fully layer over the top and by eddying motions around
computational models, even with the latest com- buildings, the spatially averaged models are
puting systems, cannot generally resolve the flow deficient.
around every building. Typically, for computa- In the second case, an effectively non-porous
tions with 106–107 grid boxes, the horizontal neighborhood, the mean air flow passes over the
grid spacing is about 100 m or greater in the building envelope as if over a hill with elevation
horizontal direction. To resolve the velocity field zs(x, y). The roughness length z0 also changes as a
around a building in order to calculate its drag result of turbulence and recirculating flows in the
effect on the overall flow, the grid boxes would courtyards, streets, etc. between the buildings.
have to be of the order of 1 m or less. Therefore Estimating these parameters zs, z0 in terms of the
even FCMs can, at present, only calculate average building layout is only approximate, (e.g., zs ffi Hc,
features of the flow over these grid box scales by z0 ~ H/30). As with porous built-up areas, the
estimating the average effects of buildings and parameterizations for calculating average flow
streets in the model. This is expected to change properties can be estimated approximately by
in the near future with further increases in com- detailed computation of typical local areas.
putational power. These calculations can also provide estimates of
For most practical applications in urban areas, the local turbulence, needed for dispersion com-
different modelling approximations are needed putations [23]. FCMs using turbulence closure
(even with an FCM) depending on whether the models have been extensively applied to the
buildings in the neighborhood being considered kinds of recirculating flows that occur between
form effectively porous or non-porous regions of buildings in non-porous urban areas; most
178 Urban Air Quality: Meteorological Processes

validation has been for wind tunnel tests and to develop models over neighborhood scales for
engineering flows, where the kind of very-large- flow and dispersion.
scale eddies and downdrafts found in atmospheric Fully computational methods, using a variety
flows are absent. Such motions can lead to more of turbulence modelling methods, have been
rapid exchange between the upper flow above and extensively applied to computing flows around
within the canopy layer, as discussed in the review single buildings in turbulent boundary layers.
by Mestayer and Anquetin [5]. Using turbulence closure methods, many models
As shown in Table 4, and reviewed by Britter and have predicted mean velocities near the buildings
Hanna [11], most FAMs for the neighborhood scale within one or two widths; but such models (e.g.,
tend to focus on equilibrium flows within and just k-ε models) have tended to over-predict small-
above the canopy. In a “porous” canopy (Fig. 2a), scale turbulence around the structure [59] and
the mean velocity within the canopy Uc(z) is driven under-predict the large-scale atmospheric eddies.
by the turbulent shear stresses generated in the This leads to an over/under-prediction of the mean
intense shear layer just above the canopy. Here the velocity defects in the wakes downwind of 3-D/2-D
ratio of Uc/U (z*), where U(z*) is the velocity at the structures in the atmospheric boundary layer.
top of, or above, the roughness layer (Fig. 2), Only the computationally intense method of
depends on the porosity – a typical value being Large Eddy Simulation (LES), or unsteady
0.3. In a non-porous canopy, typically in the inner modelling of the fluctuating flows using turbu-
city, where flows are determined by canyon and lence closure models, can accurately represent
downdraft effects, this mean velocity ratio varies the distortion of the large-scale eddy motion
considerably over the range 0.1–0.3 [23]. around the building and its effect on downwind
The approximate average velocity profile wakes [60, 61].
(Eq. 2.1) is not applicable at the edges of “neigh- Calculations using FCM with turbulence clo-
borhoods” where the density and heights of build- sure have also been performed on flow around
ings vary, or in the interiors of such regions, such small groups of buildings using resolutions
as near parks, squares, etc. At the edges of porous down to about 0.1 H. The predictions of the tur-
canopies, where the air flow in the canopy varies bulence in these flows are more reliable than those
rapidly, an FAM approximate model has been of isolated structures because most of the turbu-
developed based on the same approach as FCM lence in this instance is generated locally between
by representing the canopy as a porous layer and the buildings and is of smaller scale (similarly,
(as for the FAM in the mesoscale range) solving wind tunnel models of dispersion around build-
perturbation equations semianalytically to pro- ings are generally more reliable when the build-
vide fast computation of the mean velocity and ings are in groups than when isolated because
shear stress [9, 56]. These have been verified wind tunnels cannot simulate the low frequency
against field and wind tunnel studies. fluctuation in wind direction). This is because the
Over non-porous canopies (typically catego- primary interactions between the wake of one
ries (i)–(v) in Table 3), the determining parameters building and its impact on adjacent buildings are
(Hc, z0(x, y)) are the same as for FCM over these not sensitive to the structure of turbulence; how-
elevation/roughness changes. The linearized ever, the wakes of isolated or well-separated
FAM approaches give very similar results to buildings are strongly affected by the form of the
those using FCMs [57, 58]. low frequency spectrum of turbulence. This is
why in some institutions, for example, the US
Modelling the Building and Street Scale Naval Laboratory [62] and more recently at Los
The purpose of detailed flow modelling in and Alamos [63], work is being undertaken on disper-
around individual buildings and the surrounding sion in dense urban areas with fast FCMs in which
streets is firstly to understand how rapidly approximate velocity fields are computed using
released matter disperses locally. Secondly, classical grid box methods of finite size (say 1 m)
detailed studies of these local scale flows are but neglecting completely any modelling of tur-
necessary, as explained in the previous section, bulent stress. This reduces the number and the
Urban Air Quality: Meteorological Processes 179

order of the equations to be solved and speeds up When d is less than dmin (Fig. 3a(ii)), it is found
the computation by a factor of 10 or more. The that the recirculating regions of the wakes of the
finite size of the grid effectively introduces upwind buildings are elongated and extend to the
numerical diffusion that simulates many of the nearest downwind building [65]. For buildings
same mean flow features developed using the designed in rows nearly parallel with the wind
more complex turbulence closures. direction, the flow structure consists of turbulent
Another simplification to speed up the compu- recirculating regions in the spaces downwind of the
tation of the mean velocity field is to represent the buildings and relatively high-speed streams in the
effects of the individual buildings as a distributed open streets between the buildings [28]. Describing
force acting on the flow (or source/sink distribu- the flow structure in this way provides the basis for
tion) and thereby only approximately representing FAM for dispersion calculations.
the shape of the building [64]. In most FCM By contrast, when the buildings are placed in a
calculations, considerable computational resource staggered pattern relative to the wind direction,
and time is spent on exactly representing the the wakes tend to disappear and the mean flow
building shape, while at the same time making between the buildings consists largely of unidi-
considerable approximations in the flow. rectional bifurcating patterns of diverging and
There are at present no general FAMs that are converging streamlines, with small regions of
capable of calculating the detailed flow around recirculating flow. Such flow can be computed
any isolated building or group of buildings, or by fast potential flow methods [28], which are
even calculating those broad features of the flow even faster if the shape of the layout of the build-
needed for modelling dispersion close to the ings is approximated [64].
building. The main reason is that the unsteady When the buildings are long enough and close
separated shear layers that control the flow are of enough (i.e., categories (i), (ii), and (iii) of
much smaller scale than the building. This means Table 3) and the wind is at any angle, or if they
that the recirculating flow region, which greatly are situated in rows and the wind is at a small
affects the magnitude and timescale of concentra- glancing angle to the row (Fig. 3a(ii)), then the
tion fluctuation, is not only highly unsteady but characteristic canyon flows are formed in the
also very sensitive to the effects of nearby build- streets between the buildings. When the buildings
ings. Nevertheless, the main features of the mean either side of the street are of comparable height, a
flow patterns and typical magnitudes of the mean strong feature of the helical canyon flow is that it
and fluctuating velocity have been classified and does not extend above the buildings. Therefore
partially quantified for many types of buildings the appropriate FAM for these flows is to assume a
and groupings. Therefore, although no practical canyon flow below the building level and a rough
FAM for the mean flow is available at present, wall boundary layer flow above it [23].
these features of the flow field are now well The final consideration is of the air flow in
enough known to derive useful quantitative typical courtyards and “squares” connected to
FAMs for the dispersion. For example, when adjoining streets (Fig. 3c). Simulations confirm
buildings are far enough apart that their near- that these are regions where fluid trajectories are
flow fields and their wakes are approximately well mixed. This provides a basis for constructing
independent, the wakes can be approximated as FAMs for dispersion in these regions using semi-
a perturbation to the approach flow, a theory by analytical diffusivity models.
Counihan et al., 1974 [21] that is used in the
“Buildings” module in ADMS [67]. The same
model can be used approximately with linear Examples of Output of Modelling
superposition when buildings are separated by at Calculations
least 3H, where H is their height. As the ratio of
breadth to height, b/H, increases from 1.0 to A series of examples of recent model calculations
10, this minimum separation distance dmin showing the impact of buildings on flow are now
increases linearly to about 10 H (Fig. 3a(i)). reported. The cases considered are a single
180 Urban Air Quality: Meteorological Processes

building, a regular building array, and a complex where Q is the emission rate, C is the measured/
urban junction. The examples mainly comprise calculated concentration, and Uref is the reference
simulations using an FCM (specifically a CFD velocity. Figure 4a shows the geometric setup and
model); one example using an FAM is also Figs. 4b–d show examples of model outputs for
presented. Cases 1 and 3 together with comparisons with
CFD models do not describe all meteorological measurements from controlled wind tunnel exper-
phenomena as described earlier; however, they are iments. In detail, Fig. 4b shows the x-velocity
useful tools for predicting flow characteristics in component (along the wind direction) contour
street canyons and within urban areas at the neigh- obtained from CFD simulations, where it can be
borhood, building, and street scale. They can also noted that the k-ε model was successful in pre-
be used to interpret wind tunnel and field data and dicting the typical vortex which develops in the
their outputs can therefore be used to improve wake zone behind the building. Figure 4c, d also
operational models. Most available general pur- show the comparison between wind tunnel and
pose CFD models currently still need to be vali- CFD data for Case 1 and Case 3. In particular, it
dated against wind tunnel or field data to obtain can be noted that in Case 1 the model under-
confidence before applying them to a particular predicts concentrations slightly. The hit rate q, a
case study [67]. Some FAM models used for cal- statistical quantitative score of the model perfor-
culating dispersion at the building and street scale mance [71], is equal to 75%. It is recalled that the
are reviewed in [68]. Hit Rate validation test is performed using a frac-
tional deviation RD ¼ 0.25 and an absolute devi-
Single Building ation W ¼ 0.06 (q > 66% is typically requested for
Table 5 summarizes cases investigated by means the comparison with wind tunnel data). Nowa-
of both wind tunnel and CFD simulations by days, statistical metrics are typically used to
Wang and McNamara [69]. The Launder and assess model performance during the model eval-
Spalding’s standard k-ε model [70] for turbulence uation process. Usually k-ε models give a satis-
and the advection-diffusion model for dispersion factory performance for wind profiles according
was used for the computation with a computa- to the q tests. For this study, the Case 2 and Case
tional grid comprising 500,000 cells and smallest 3 model predictions are in general agreement with
dimensions equal to 0.005 m. The cases com- observations from wind tunnel measurements,
prised a cube (1), a tall building (4), a wide build- with hit rate test scores of q ¼ 82% and
ing (5), and intermediate cases (2 and 3). q ¼ 77%, respectively. Finally, Case 4 and Case
Mean concentrations are expressed as dimen- 5 model predictions are also in general agreement
sionless values K which are defined as: with observations from wind tunnel measure-
ments with hit rate test scores of q ¼ 78% and
CU ref H 2 q ¼ 68%, respectively.
K¼ ,
Q

Urban Air Quality: Meteorological Processes, Table 5 Summary of the single building case. H, W, and L are the
building height, width, and length, respectively. H ¼ 0.3 m for case 4 and H ¼ 0.1 m for all other cases
Case Model details Source details
1 Isolated rectangular Cube The stack, 0.5 H high, is installed at an upwind distance of
2 building W/H ¼ 2, L/H ¼ 1 2 H from the building
3 W/H ¼ 1, L/H ¼ 2
4 W/H ¼ 1/3, L/
H ¼ 1/3
5 W/H ¼ 6, L/H ¼ 1
a b 5.1
Wind VERTICAL PROFILE
4.5
L
3.9
LATERAL PROFILE
W 3.3
0.5 Href
2.8

2.2
H 0.5 Href 1.6
0.5 Href LONGITUDINAL PROFILE
1.1
Urban Air Quality: Meteorological Processes

2 Href 0.48
z
y −0.094 Z

Y X
x −0.67

c LATERAL LONGITUDINAL Vertical d LATERAL LONGITUDINAL VERTICAL


3.5 1 0.8 3.5
Wind Tunnel Wind Tunnel
1.2 1.2 3 CFD 0.7 3 CFD
0.8
1 1 2.5 0.6
2.5
0.6 0.5
0.8 0.8 2 2

K
K
K

0.4

Z/H
Z/H

0.6 0.6 1.5 1.5


0.4 0.3
0.4 0.4 1 1
0.2
0.2
0.2 0.2 0.5 0.1 0.5

0 0 0 0 0 0
−2 0 2 0 5 0 0.5 1 −2 0 2 0 2 4 6 0 0.5 1
y/H K x/H y/H x/H K

Urban Air Quality: Meteorological Processes, Fig. 4 (a) Sketch of the single of the building from CFD simulations. (c) Concentration profiles for Case 1. (d)
building with indication of the upstream source position and profiles where wind tunnel Concentration profiles for Case 3
and CFD results are compared. (b) Contour of the x-velocity component in the middle
181
182 Urban Air Quality: Meteorological Processes

Isolated Street Canyons height H in the undisturbed approaching flow, and


Recent interest has risen in employing LES models Q/l the tracer gas source strength per unit length.
[72, 73] to overcome the shortcomings of RANS in Figure 5 shows normalized concentration con-
its inability to capture the unsteady and inherent tours at wall A (leeward) and wall B (windward)
fluctuations of the flow field within the street canyon of the street canyons.
on which the dispersion of pollutants depends. It is observed that amongst the two RANS
RANS, which is the most widely used approach in models, RSM performed better than standard k-ε,
industry for the modelling of turbulent flows, however, LES proved better than RANS in pre-
assumes that non-convective transport in a turbulent dicting the concentration distribution because it
flow is governed by stochastic three-dimensional was able to capture the unsteady and intermittent
turbulence possessing a broadband spectrum with fluctuations of the flow field, and hence, resolve the
no distinct frequencies and, therefore, models the transient mixing process within the street canyon.
entire range of the eddy length scales. This approach
has obvious weaknesses and poses serious uncer-
tainties in flows for which large-scale organized Regular Building Arrays
structures dominate, such as flows around buildings. Wind tunnel experiments have demonstrated that
In addition, RANS models assume gradient trans- street ventilation is reduced in the presence of
port, which may not be the case for pollutant upstream buildings. This seems to be because of
exchange at the roof level of a street canyon. LES, the upward displacement of the flow and the con-
although computationally more expensive, has an sequent perturbed momentum exchange between
advantage over RANS in that it explicitly resolves the street canyon and the outer region of the flow.
the majority of the energy carrying large-scale orga- Also, numerical results have indicated that the
nized structures and the internally or externally surrounding building configuration affects pollut-
induced periodicity involved, whereas only the uni- ant dispersion in a street canyon, therefore it should
versal small-scale eddies are modelled. be taken into account in numerical dispersion
As an example, an illustration is provided of the modelling (see, for example, [76]). Two examples
flow structure and pollutant dispersion within an of flow and pollutant dispersion distributions for
urban street canyon of width to height ratio W/ regular building geometries are shown in Fig. 6,
H ¼ 1 using the standard k-ε model, the Reynolds investigated by means of wind tunnel experiments
Stress Model (RSM), and LES, coupled with the and numerical simulations as previously described.
advection-diffusion method for species transport The experiment is set up in a boundary layer
[74] (Fig. 5). In the case shown, the computational wind tunnel to simulate the case of dispersion of
domain was built by using about one million cells pollutants from naturally ventilated underground
with smallest dimensions equal to 0.077 H. Numer- parking garages [77]. A finite array of idealized
ical results, which include the statistical properties building blocks with 0.1 m by 0.15 m base dimen-
of pollutant dispersion, for example, the mean con- sions and 0.125 m height (three buildings cross-
centration distributions, three-dimensional spreads wind and seven buildings along wind direction)
of the pollutant, etc., are then compared to wind- are considered, as shown in Fig. 6a. The aspect
tunnel measurements from the online database ratio of the street canyons resulting from the
[75]. Integrated into the model street, four tracer building arrangement is W/H ¼ 0.8. Four
gas emitting line sources were used for simulating ground-level emission sources were mounted
the release of traffic exhausts. Mean concentrations close to the building. RANS type simulations
are normalized according to: [78] were performed by employing the standard
k-ε model and the advection-diffusion model. The
CU ref H computational grid was built by using 500,000
cþ ¼ ,
Q=l cells, with smallest dimensions equal to 0.005 m.
Flow and dispersion were measured within the
where C is the measured/calculated concentration, street canyon positioned downwind of the build-
H the building height, Uref the flow velocity at ing equipped with the sources.
Urban Air Quality: Meteorological Processes 183

a Street Canyon

linesources

0.23 H 0.35 H

W=H

Line Sources

b WALL A WALL B
1 1
8 24 16 8
0.5 16 24 32 WT 0.5
32
0 0
a −5 −4 −3 −2 −1 0 1 2 3 4 5 −5 −4 −3 −2 −1 0 1 2 3 4 5

1 1
0.5 k-e 0.5
0 0
b −5 −4 −3 −2 −1
Z/H

0 1 2 3 4 5 −5 −4 −3 −2 −1 0 1 2 3 4 5
1 1
0.5 RSM 0.5
0 0
c −5 −4 −3 −2 −1 0 1 2 3 4 5 −5 −4 −3 −2 −1 0 1 2 3 4 5
1 1
0.5 LES 0.5
0 0
d −5 −4 −3 −2 −1 0 1 2 3 4 5 −5 −4 −3 −2 −1 0 1 2 3 4 5
y/H Normalized Concentration, c +

Urban Air Quality: Meteorological Processes, concentrations at wall A (leeward) and wall
Fig. 5 (a) Sketch of the street canyon with indication of B (windward) showing comparison between WT data
the position of line source, grid, and wind tunnel model. (available from CODASC) and numerical results
(From [74] CODASC, 2008). (b) Mean normalized performed with k-ε, RSM, and LES simulation

Wind tunnel experiments and CFD simula- As outlined in [79, 80], it should be noted that
tions show that a recirculation flow region typical CFD codes predict dispersion spread that
forms within a street canyon exposed to a per- is smaller than that predicted by the well-validated
pendicular flow. Both wind tunnel measurements integral model ADMS-Urban [81]. From a sensi-
and CFD predictions show that for aspect ratio tivity test on the turbulent Schmidt number value
W/H ¼ 0.8 a single vortex forms inside the can- (the standard value is 0.7), the value of 0.4 was
yon. In particular, Fig. 6 shows velocity vectors found to be the most appropriate in order to arti-
on the vertical plane in the middle of the street ficially increase plume dispersion, even though
canyon obtained from wind tunnel experiments such tuning should be avoided. Figure 6d (top)
(Fig. 6b) and CFD simulations (Fig. 6c). The shows the dimensionless coordinate y/H versus
figure shows that the shape and dimension of the dimensionless concentration K near the floor
the vortex predicted by the CFD simulations is (z/H ¼ 0.06) within the street canyon downwind
very similar to that observed by CEDVAL exper- the source building and dimensionless concentra-
iments [77] compiled at the University of Ham- tion K versus dimensionless coordinate x/H on the
burg. The ability to capture the right dimension same vertical plane (bottom). The horizontal
of the vortex is very important as the vortex velocity near the floor is negative because the
drives the distribution of pollutants within the vortex in the canyon is clockwise. Thus, pollut-
street canyon. ants are carried toward the leeward side and mixed
184

a b
top view
wind direction 2d flow measurements, y = 0H
2 m/s

all dimensions in mm (model scale) 100


1.5

325
100
1

z [H]
0.5

750
850 source building

0
side wall of the tunnel −0.5 0 0.5 1 1.5 2
x [H]

c d leeward middle winward


0 0 0
−0.1 −0.1 −0.1
−0.2 −0.2 −0.2
−0.3 −0.3 −0.3

y/H
y/H
y/H

−0.4 −0.4 −0.4


−0.5 −0.5 −0.5
−0.6 −0.6 −0.6
0 200 400 0 10 20 0 10 20
Dimensionless concentration K Dimensionless concentration K Dimensionless concentration K
y/H=0 y/H=−0.16 y/H=−0.32
200 200 200
CEDVAL
150 150 150
CFD Sct=0.7

100 100 100 CFD Sct=0.4

50 50 50
Dimensionless concentration K
Dimensionless concentration K
Dimensionless concentration K

0 0 0
0.4 0.6 0.8 1 0.4 0.6 0.8 1 0.4 0.6 0.8 1
x/H x/H x/H
Urban Air Quality: Meteorological Processes

Urban Air Quality: Meteorological Processes, Fig. 6 (a) Sketch of the regular building. (c) Velocity vectors obtained from CFD simulations. (d) Concentration pro-
building array with indication of the source building. (b) Velocity vectors obtained from files at different positions within the same street canyon with a sensitivity to the Schmidt
wind tunnel experiments showing the vortex inside the canyon downwind of the source number value
Urban Air Quality: Meteorological Processes 185

in the street canyon. CFD results agree well with input into the developed three-dimensional
wind tunnel measurements. Eulerian dispersion model for the dispersion
It is known that FCM type of models still simulation of a pollutant released from a point
suffers from their high computational cost which source. Results were then compared with CFD
prevents them from being largely employed in predictions.
operational applications. This has pushed the Figure 8 shows concentration contours for the
development of FAM models yet incorporating case lp ¼ lf ¼ 0.16. The pollutant source was
new understanding of flow and dispersion pro- placed along the x direction at a distance from the
cesses within the urban canopy layer. Recently, inlet of approximately 1/3–1/4 of the domain
di Sabatino et al. [82] have proposed a new model- length and equidistant from both boundaries in
ling approach for the computation of the spatially- the y direction. The domain height was 6 H,
averaged flow field, where the average is defined where H is the building height. The figure refers
at the neighborhood scale, i.e., from 0.2 km up to to a source height Zs ¼ 0.5 H and shows the
10 km. The underlying idea is the description of comparison at three horizontal sections at
the drag forces in terms of height-dependent mor- z ¼ 0.05 H, z ¼ H, and z ¼ 2 H.
phological parameters based on detailed knowl- Inside the canopy, CFD concentrations tend to
edge of building geometry such as the planar area show some periodicity, due to the presence of
index lp and lf (introduced in section “Character- cubic buildings. This specific behavior cannot be
istic Regions of the Flow and Drivers”) and the reproduced by the simplified Eulerian model.
reduction of the complete three-dimensional flow However, by using spatially-averaged
field to a one-dimensional quantity, given by the one-dimensional profiles, the model is able to
mean wind direction, and the three-dimensional reproduce the order of magnitude of fully compu-
spatial dependence to a much more simple depen- tational CFD concentration predictions, even if
dence from the height z. As a consequence, only contour shapes may differ qualitatively. The qual-
mean profiles are needed as input to the model. ity of the comparison is not homogeneous over the
There are examples in the literature [83] showing domain. As expected, the comparison is quite
the possibility of extending this modelling poor close to the source and improves down-
approach to an Eulerian dispersion model for the stream. Large differences are also found near the
computation of the concentration field. Figure 7 top boundary, but this is most probably an effect
shows the spatially-averaged profiles of wind related to the boundary condition. Overall, the
velocity and diffusivity coefficient resulting from plume width predicted by the FAM type model
full CFD simulations. is comparable to the CFD model. Similar results
This reduced description of the wind field were obtained in the case of small packing density
and the diffusivity coefficient was used as (lp ¼ lf ¼ 0.0625), not shown here.

a 6 b 6
λp = 0.0625 λp = 0.0625
5 5
λp = 0.16 λp = 0.16
4 4
z/H

z/H

3 3

2 2

1 1

0 0
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1 1.1 0 0.005 0.01 0.015 0.02 0.025 0.03
U/Uref D/(Uref H)

Urban Air Quality: Meteorological Processes, Fig. 7 Spatially-averaged profiles of wind velocity (a) and diffusivity
coefficient (b). H is the building (cube) height and Uref the average velocity at the top
186 Urban Air Quality: Meteorological Processes

CFD Fast model


20 20

y/H 15 15

10 10
1.5 10 20 30 10 20 30
1 x/H
z=0.05H
0.5 20 20
0.25
0.125
15 15
0.05
0.01
0.005 10 10
0 g/m3
10 20 30 10 20 30
z=H
20 20

15 15

10 10
10 20 30 10 20 30
z=2H

Urban Air Quality: Meteorological Processes, Fig. 8 Intermediate canopy (lp ¼ lf ¼ 0.16), Zs ¼ 0.5 H: concen-
tration (g/m3) contours from the CFD model (left) and the fast model (right) at several horizontal planes

Results highlight the potential of the approach in a neighborhood in the city of Bari in southern
based on the parameterization of one-dimensional Italy. The real geometry comprises both step-up
wind and diffusivity profiles in terms of routinely and step-down street canyons and consists of two
available meteorological parameters and morpho- asymmetric streets as shown in Fig. 9a. The
logical parameters such as lp and lf, which syn- wider street canyon is characterized by an aver-
thesize the main geometric characteristics of the age aspect ratio W/H ~ 1.8 and it is perpendicular
urban canopy. to the wind direction. The other street canyon is
characterized by an average aspect ratio W/
Complex Urban Junction H ~ 0.5 and is parallel to the wind direction.
The geometry of idealized building arrays is far The tallest building is ~ 46 m. The two canyons
less complicated than the morphology of real intersect orthogonally forming four major blocks
urban areas, where urban neighborhoods are of buildings and a junction. For the sake of com-
characterized by street intersections, asymmetric putational convenience the real geometry was
street canyons, and staggered arrays of buildings slightly simplified, yet maintaining the main geo-
of irregular and/or highly variable shapes. These metrical details of the street canyons. A fine
local features significantly alter the flow and mesh close to the ground (up to a height of 4 m)
dispersion patterns, as experimental and numerical was used (Fig. 9b), with cell dimensions
studies have concluded (see for example [32, 84, δxmin ¼ δymin ¼ 1 m, δzmin ¼ 0.3 m. The number
85]). Reported here are some results of a modelling of computational cells was approximately three
study performed with a CFD code by employing and a half million. Vectors of velocity magnitude
the RSM [86], and the advection-diffusion scheme (m/s) and turbulent kinetic energy (m2/s2) at
Urban Air Quality: Meteorological Processes 187

a b

WIND

z z
y y
x x

c 6 d 2

5.4 1.8

4.8 1.6

4.2 1.4

3.6 1.2

3 WIND 1

2.4 0.8

1.8 0.6

1.2 0.4

0.6 y 0.2
y
0.0032
z 0.00029 z
x x

Urban Air Quality: Meteorological Processes, Fig. 9 (a) Sketch of the urban junction. (b) Grid refinement close to
the ground. (c) Flow pattern at z ¼ 2 m developed within the urban junction. (d) Turbulent kinetic energy at z ¼ 2 m

z ¼ 2 m are shown in Fig. 9c, d, respectively. Due response and cheaper instrumentation, the continu-
to the interaction of the wind with buildings, the ing improvements in computer speeds, and the
resulting flow is channelled along the wider current strong interest in this topic, it is certain
street canyon (which is that perpendicular to the that more detailed data and more advanced models
wind direction), predominately blowing along of urban meteorology will increasingly become
the negative y direction. Obviously, the distribu- available, resulting in huge data resources. Under-
tion of the turbulent kinetic energy is highly standing of such data will continue to rely on the
asymmetric, showing large values in the wind- general concepts and categorizations described in
ward region. This example shows that flow pat- this entry. Also of great relevance to future devel-
tern and turbulent kinetic energy are strongly opments is both the impact of climate change on
affected by the geometry. urban meteorology and the response of the urban
environment to climate change. These issues are
discussed in [87].
Future Directions

The entry has described the impacts of urban areas Notation and Abbreviations
on urban meteorology at the mesoscale, neighbor-
hood, and building street scale. While our general
understanding of the processes is good and this b Building breadth
enables us to construct approximate models, it is C Measured/calculated
clear that at this time there is a paucity of detailed concentration
field data and the most detailed numerical models CD Drag coefficient
are still not able to resolve all the features of the c+ Normalized mean concentration
flow in good time. With the availability of faster for a line source
188 Urban Air Quality: Meteorological Processes

d Gap or separation distance UG Geostrophic wind


between buildings UH Mean wind above the buildings
f Coriolis frequency (at height H)
F Froude number Uref Reference velocity
Fv Surface water vapor flux Uc Mean wind along the street
Fθ Fθ canyon
g Gravitational acceleration VS Mean wind along street
h Boundary layer height w Building length or width
H Building height W Absolute deviation, Building
Hc Canopy height width
Hc0 Standard deviation of canopy x 5 (x, y, z) Coordinates of a point
height, Hc xB(i), yB(i) Coordinates of staggered building i
HM Mountain height xs, ys, zs Coordinates of source
K Normalized mean concentration yc(x) Streamline through source
for a point source at xs, ys, zs
k-ε Kinetic energy and energy- z0(x, y) Roughness length for wind
dissipation model of turbulence profile
l Vertical length scale of internal zd Displacement height for
layer logarithmic wind profile
l O, l N Vertical length scales of internal zS(x, y) Surface elevation of the ground
layers over the urban area, Zs Source height
neighborhood scale Z Height of top of shear layer above
La Adjustment length for mean flow buildings
to adjust as it enters the porous β “Porosity” of an urban canopy
canopy [β ~ bw/d2]
L Building length θ Mean temperature
Lf Coriolis advection length θs Surface temperature
LI Inner city length scale k Von Karman’s constant
LM, LN, LBS Length scales of the (sub-) lp Planar area index
regions M, N, BS lf Frontal area index
LO Overall city length scale su, sv, sw R.m.s velocity components (of the
LRo Rossby length scale order of u)
LSe Effective source size f Angle between wind direction and
N Buoyancy frequency normal direction to a street (Figs. 3
q Hit rate test score and 6), i.e., f ¼ 90° if wind is
Q Emission rate along the street.
RD Fractional deviation
RM Ratio of the length of the Subscripts
sub-regionLM to the smallest
scales resolved in that region
s Distance to the nearest building B Buoyancy
u Friction velocity of the turbulent BS Building/Street scale
velocity profile of the atmosphere c Canopy
U Mean velocity, with subscripts C Cloud concentration
denoting location/physical process f Coriolis
UB Typical wind speed associated G Geostrophic
with local buoyancy effects H At top of buildings/canyon
UC Wind speed within the canopy M Mesoscale
Urban Air Quality: Meteorological Processes 189

N Neighborhood scale 9. Belcher SE, Jerram N, Hunt JCR (2003) Adjustment


O Overall urban area of a turbulent boundary layer to a canopy of roughness
elements. J Fluid Mech 488:369–398
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s Surface, street erties of urban areas derived from analysis of surface
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Polycyclic Aromatic Hydrocarbons (PAH) and
Urban Air Quality: Sources Urban Air Quality
and Concentrations Sources and Emissions of PAHs
Sampling Artifacts in Measuring PAHs
Michael Evan Goodsite1, Ole Hertel2, Long-Range Transport of PAH
Matthew Stanley Johnson3,5 and Nana Rahbek Trace Elements to Include Heavy Metals in Urban
Jørgensen4 Areas
1
School of Civil, Environmental and Heavy Metals in the Urban Atmosphere
Mining Engineering, The Australian Trace Elements in the Urban Atmosphere
School of Petroleum, The University of Adelaide, Conclusions
Adelaide, SA, Australia Future Directions
2
Department of Environmental Science, Aarhus Bibliography
University, Roskilde, Denmark
3
Department of Chemistry, University of Glossary
Copenhagen, Copenhagen, Denmark
4
Faculty of Engineering, University Aerodynamic diameter Particles in ambient air
of Southern Denmark, Odense M, Denmark have irregular shapes. The aerodynamic diam-
5
Airlabs, Copenhagen, Denmark eter is the idealized spherical diameter with the
same aerodynamic behavior as the irregular
real-world particle.
Air pollutants Anything in the air around us,
Article Outline man-made or natural, which contaminates the
natural steady state of and constituents in the air
Glossary as required for life categorized as gaseous or
Definition of the Subject and Its Importance particulate pollutants.
Introduction Air pollution The state of pollutants contaminat-
Origins of Air Quality: Sources and Formation of ing the air/atmosphere around us.
Urban Air Pollution Air quality index (AQI) A numerical index for
Air Quality and Health Effects air pollution, for example, in the UK, it is from
Urban Air Pollution Concentrations in General 1 to 10 and related to the air quality bands of
Urban Air Quality Concentrations and Indices “low,” “moderate,” “high,” or “very high”
Sources in Urban Airsheds (https://uk-air.defra.gov.uk/air-pollution/daqi?vi
Impact of Physical Parameters: Geography, ew=more-info, accessed May 1st, 2019).
Topography, and Meteorology Another example is the AQI from the US EPA
Impact of Geography with a scale from 0 “good” to 500 “hazardous”
Impact of Topography https://airnow.gov/index.cfm?action=aqibasics.
Impact of Meteorology aqi (accessed May 1st, 2019).
Pollutant Dispersion in Urban Streets Air quality A subjective, often locally or nation-
Nitrogen Dioxide Pollution in Urban Areas ally, determined state of the amount of pollut-
The Impact of Particle Pollution ants in the air around us. The best air quality is
Particle Mass Concentrations when there are very low pollutant levels.
Particle Number Concentrations Ambient air Air outside of structures at any
Air Quality Measurement Locations given time. The “outdoor air” as opposed to
Natural Sources the “air indoors.”

© Springer Science+Business Media, LLC, part of Springer Nature 2021 193


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_321
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2019, https://doi.org/10.1007/978-1-4939-2493-6_321-3
194 Urban Air Quality: Sources and Concentrations

Atmosphere The envelope of gases surrounding often sharp, unpleasant, and soot pertaining
the Earth. haze that is occurring during periods when air
Coarse particles The coarse particle mass frac- pollutants are trapped at ground level. There
tion is defined as the difference between mea- are two processes producing smog: photo-
sured PM10 and PM2.5 (see definitions of chemical and physical processes, respectively,
these). referred to as photochemical smog and
Diffuse sources of air pollutants Sources for urban smog.
which the release cannot easily be traced, e.g., Ultrafine particles Particles in the size fraction
that are not geocoded like gases and particle below 0.1 micrometer in diameter. These par-
emissions from smaller industry and domestic ticles are also often termed nanoparticles.
heating, ammonia from grassing cattle, etc. Urban air pollution Ambient air in urban envi-
Emissions The discharge of man-made or natu- ronments or areas that is (expectedly) polluted
ral compounds into the environment. when compared with ambient air in pristine
Fine particles The PM2.5 fraction of particles regions. There is generally a suite of pollutants
(see definition of PM2.5). that are measured/monitored to describe the
Particulates Fine as well as coarse liquid and resulting decrease in urban air quality.
solid particles of organic or inorganic sub- Urban air quality Refers to how “clean” the
stances present in the atmosphere/suspended ambient air is inside of cities with a density,
(floating) in the air. Particulate matter consists population, and level of activity that generally
of very small liquid and solid particles floating are recognized as “urban.”
in the air. Urban smog Smog where air pollutants particu-
Photochemical smog The resulting haze and larly smoke and sulfur dioxide are trapped at
reduced visibility from pollutants formed in ground level, usually occurring on cold, wind-
reactions induced by sunlight (photochemical still winter days. The Great London Smog epi-
reactions) and involving nitrogen oxides sode of 1952 is a historical example still seen in
(NOx) and hydrocarbons (HC). Photochemical developing countries in today. In western
smog including elevated ozone (O3) levels countries photochemical smog consisting of
occurs generally on warm sunny days, which nitrogen oxides, ozone, and PAN is contempo-
promotes photochemical reactions. rarily more common.
PM10 The mass concentration of particles with less Urban An area with a large population, i.e., town
than 10 microns (mm) in aerodynamic diameter. or city, generally with a high density and large
(PM10) is generally used as an indicator for amount of population.
suspended particulate matter (e.g., regulated in Winter smog Winter smog episodes including
EU directives) and routinely measured at many elevated levels of nitrogen oxides (NOx)
locations throughout the world. occur on cold calm days when air pollutants
PM2.5 The mass concentration of particles in the are trapped in urban areas by an inversion
air with less than 2.5 microns (mm) in aerody- layer, i.e., a layer of warmer air above the
namic diameter. This fraction is often termed wind-still cold air.
fine particles and capable of penetrating into
the deepest parts of the lungs and thus causing
great health concern. Definition of the Subject and Its
Point (stationary) sources of air Importance
pollutants Sources that emit pollutants from
one given fixed location; this can, for example, Urban air quality refers to how “clean” the ambi-
be a power plant or an industrial plant. ent air is inside of cities with a density, population,
Smog A word combining “smoke” and “fog,” and level of activity that generally are recognized
first used by Dr. HA Des Voeux in 1905. as “urban.” Urban air quality generally differs
Smog is describing the poor visibility and from rural air quality since there are usually
Urban Air Quality: Sources and Concentrations 195

more concentrated sources, and the ability for the UNEP in a 2019 report, “Air pollution measures
pollutants in the air to be dispersed is limited by for Asia and the Pacific 25 science-based solutions
the physical constraints of the urban environment. to bring clean, safe air to 1 billion people” (http://
Urban air quality varies significantly in between www.ccacoalition.org/en/content/air-pollution-mea
urban cities around the world generally because of sures-asia-and-pacific, accessed May 1, 2019, or
the differences in control on pollution sources but the report itself http://www.ccacoalition.org/en/
also due to differences in meteorology and, e.g., file/5802/download?token=dBM5KOkC accessed
the domestic use of open fires and wood stoves in May 1, 2019), states that “2.3 billion people in the
the urban areas. Nevertheless, across the world, region are exposed to levels of air pollution several
illness, deaths, and damage to the environment are times the WHO guideline for safe air” and that
still attributed to air pollution. “some of the highest recorded levels of air pollution
Worldwide, the United Nations Environment are in Asia Pacific countries” with “92% of the Asia
Programme (UNEP) (http://www.unep.org/urban_ and the Pacific’s population, about 4 billion people,
environment/issues/urban_air.asp, accessed February exposed to levels of air pollution that pose a signif-
13, 2010) reported in 2010 that an estimated more icant risk to their health” – many of these are in
than 1 billion people annually are exposed to ou urban areas that will likely continue to grow and,
tdoor air pollution as seen further below; the nu unless the 25 recommended solutions from the
mbers in the Asian and Pacific Region have report followed, continue to pose a health risk to
more than doubled to the present time. There the people as well as miss an opportunity to signif-
fore since 2010, it can be expected that over one icantly benefit other UN sustainable development
million premature deaths each year are linked to goals, climate, food, and water security of the
urban air pollution in the ambient environment. regions.
Given primarily these deaths and other health Air quality as a term is subjectively defined
costs and loss of productivity, urban air pollu generally through laws regulating the maximum
tion is estimated to cost approximately 2% of concentrations of pollutants in the atmosphere via
GDP in developed countries and 5% in deve the maximum allowable emissions from sources.
loping countries. The quality of the ambient (outside) air is moni-
UNEP further reported that rapid urbanization tored, in some urban environments, continuously
has resulted in increasing urban air pollution in with advanced equipment and generally reported
major cities, especially in developing countries in some type of index by local or national author-
with over 90% of air pollution in major cities in ities, a so-called air quality index.
developing countries attributed to vehicle emis- Despite relatively unchanged levels of pollut-
sions brought about by high numbers of older ants, the air quality can be improved or degraded
vehicles coupled with poor vehicle maintenance, based on the weather and topography of the urban
inadequate infrastructure, and poor fuel quality environment. It is therefore a very complicated
with high amounts of sulfur in the fuel. issue to manage and predict. Many municipalities
Most developed countries have put in measures therefore have air quality management (AQM)
to reduce vehicle emissions, in terms of fuel qual- offices and/or plans.
ity, by, for example, regulating the amount of sul- There are specific mathematical models devel-
fur, benzene, and additives like lead in vehicle fuel oped to predict air quality and support the air
and vehicle emission reduction technologies such quality policies that naturally must be aligned
as catalytic converters; these measures are yet to be with policies affecting the other environmental
adopted in most cities in developing countries, and compartments.
there are recent cases where vehicle manufactures In cities in the industrialized world, air quality
save costs by not utilizing such technologies while, has generally improved after controls and policies
at the same time, lowering overall vehicle prices, on pollution and emittants were emplaced during
thus enhancing the number of vehicles on the road the past decades. The policies have been the result
with all of the subsequent effects on air quality. of international treaties, as well as national and
196 Urban Air Quality: Sources and Concentrations

local legislation. The United Nations Environment function of vehicular traffic and the emissions
Programme (UNEP) maintains a Register of Inter- arising from vehicles. Both petrol (gasoline)-
national Treaties and Other Agreements in the Field and diesel-driven vehicles emit vast amounts of
of the Environment for the interested reader (http:// pollutants. These include carbon monoxide (CO),
www.unep.org/law/PDF/register_Int_treaties_con the oxides of nitrogen (NOx), and volatile organic
tents.pdf). Specifically, the 1979 Convention on the compounds (VOCs). Particulates (PM10) and
Long-Range Transboundary Air Pollution and its finer-sized particles (PM2.5) are emitted not just
eight associated protocols, generally named after from the combustion processes in the motor but
the cities in which they were signed (such as Aar- also and more predominantly from physical pro-
hus, Denmark), are relevant for air quality as with cesses, such as resuspension of road dust and wear
the signing of the convention air pollution is recog- of tires, brakes, and road material.
nized as a transboundary issue. There is likewise an
international agreement regarding transboundary
haze pollution. Introduction
Air quality issues are generally on a long-term
scale; however, in urban areas, municipal authorities Air pollution is estimated by WHO to cause about
need to be prepared for acute events such as those two million premature deaths (half of this is asso-
that may be arising from an industrial accident such ciated with outdoor and the other half with indoor
as what occurred at a pesticide plant in Bhopal, air pollution) worldwide annually [2], and this is in
India, in December 1984 or from elevated levels of addition to a variety of other adverse health effects
air pollution such as experienced in London during like asthma and other airway diseases, cardiovas-
the “Great London Smog” of 1952. It has been cular disease, different types of cancer, as well as
estimated that just in this single event, about adverse pregnancy outcome. The most hazardous
12,000 deaths could be directly attributed to the of the ambient pollutants are generally believed to
incident [1]. be related to the particulate matter (PM), although
As point sources such as those responsible for the mechanisms behind these health effects are not
the acute incidents above are addressed by poli- yet fully understood. It is therefore still very uncer-
cies, other man-made sources, generally the tain what it is about the particles that cause these
“mobile sources” (i.e., vehicular traffic), are negative health effects. Despite the uncertainties
becoming the new primary contributor to related to the mechanism behind these effects, it
degraded air quality in urban areas. has, e.g., been estimated by WHO that reducing
Natural sources are also an important contrib- ambient air concentrations of PM10 from 70 to
utor depending on the locality with dust, sea 20 mg/m3 would lower the number of air quality-
spray, and other types of particulate matter such related deaths by approximately 15% [2].
as pollen as well as volatile organic compounds People are generally most at risk in the urban
emitted from plants and trees being those that areas with respect to health effects related to air
contribute often to degraded air quality. pollution. More than half of the world’s popula-
Historically in urban areas across the world, tion reside in cities, and it is here that the highest
high levels of smoke and sulfur dioxide from air pollution exposure [3] and thus also most of
domestic burning of coal in people’s homes and the associated negative health impact take place.
later combustion of fossil fuels in coal-fired power The projections for the next 50 years furthermore
plants have been the major point source of air indicate that the worldwide urban population will
pollutants, and this has led to major episodes of be increasing by two thirds [3]. As a result of rapid
air pollution with resultant degraded air quality urbanization, urban air pollution has been increas-
and associated health effects, including deaths ing in many major cities, especially those found in
directly attributed to the poor air quality. developing countries (such as in Brazil, Russia,
Air quality in urban environments, especially India, Indonesia, and China). The cost to society
in developed countries, is nearly always a of the associated health effects is very significant
Urban Air Quality: Sources and Concentrations 197

and has been estimated to be approximately 2% of the temporal pattern in the local releases. However,
the gross domestic product (GDP) in developed the extent of the urban area and the spatial distribu-
countries, whereas it is even 5% of the GDP in tion in the local emission density also play central
developing countries (www.unep.org/urban_envi roles for the local contribution to air pollution levels
ronment/issues/-urban_air.asp). There may also in the urban environments. The local contribution to
be significant associated losses in productivity [5]. pollution levels also varies heavily from one pollut-
ant to another. In addition, the meteorological con-
ditions greatly affect the actual pollution levels in a
Origins of Air Quality: Sources and Formation given situation as they govern the dispersion condi-
of Urban Air Pollution tions and the pollutant transport in and out of the city
Urban ambient air pollution concentrations arise area. In this context, the presence of the building
from the continuous competition between the emis- obstacles plays a crucial role in causing generally
sion processes that increase pollutant concentrations high pollutant levels in the urban environment. This
and the dispersion, advection, and deposition pro- is especially true inside the “street canyons” formed
cesses that reduce and remove them. Pollutant dif- with buildings on both sides of the street and where
ferences between different urban areas are naturally the canyon vortex flow governs the pollution
reflecting differences in emission densities and pat- distribution.
tern but also in the dispersion and removal pro-
cesses. The local meteorological conditions are
governing the impact on pollution levels of these Air Quality and Health Effects
dispersion and removal processes, and these meteo- Air quality and health effects have been shown to
rological conditions vary heavily with the physical be linked. Particulate matter (PM) is generally
location of the city. Air pollution concentrations in believed to be the most hazardous of ambient
an urban environment are naturally the result of the pollutants. Reducing ambient air concentrations
contribution from local emissions, but also contri- of PM10 from 70 to 20 mg m3 would lower the
butions arising from pollution from more remote number of air quality-related deaths by approxi-
sources may play a very important role (Fig. 1). mately 15% [1].
The size of the city domain together with the density Greater than half of the world’s population
of pollutant emissions governs the local contribution reside in cities, and the number is expected to
to urban air pollution [6]. Naturally, the temporal grow [2]. Cities and especially their urban centers
pattern in urban air pollution levels is a function of are where air quality is generally the poorest, and

Street increment
Concentration

City increment

Regional

Distance

Urban Air Quality: Sources and Concentrations, street. The relative magnitude of the various contributions
Fig. 1 A schematic illustration of the air pollutant contri- depends on the considered pollutant and the actual disper-
bution from the regional transport, the city area, and the sion conditions (governed by the meteorology)
198 Urban Air Quality: Sources and Concentrations

the highest air pollution exposure [4, 5] and asso- technologically up-to-date smoke stacks. This is
ciated negative health impact therefore take place. because air pollution emitted from a high release
With projections for the next 50 years indicat- height will in many cases be transported out of the
ing that the worldwide urban population will urban area before being dispersed down to ground
increase by two thirds [2], urban air quality will level, although this is of course depending on the
continue to deteriorate as air pollution continues size of the urban domain. This is the principle that
to increase in major cities, especially those in the “solution to pollution is dilution” when often
developing countries (such as in Brazil, Russia, the pollution and subsequent air quality issues are
India, Indonesia, and China). just moved from one jurisdiction to another.
Urban industries, power plants, and other
Urban Air Pollution Concentrations in General sources for which the releases come from tall chim-
Urban air pollution arises from the competition neys therefore only rarely contribute to the local
between emission processes which increase pol- ground level air pollutant concentrations inside the
lutant concentrations and dispersion, advection, urban area, and instead they are usually contribut-
and deposition processes that reduce and remove ing primarily to the regional air pollution.
them. Differences in pollution levels reflect dif- Pollutant emissions related to vehicular trans-
ferences in emission densities and emission pat- port, local domestic heating, and smaller indus-
terns. They also reflect processes of pollutant tries have low release heights [less than 10 m
dispersion and removal. Pollution is dispersed by above ground level (a.g.l.)]. Consequently, the
the flow of wind. It is removed generally via releases are not diluted as efficiently before
chemical conversion to other compounds and/or reaching ground level as in the case for emissions
by being deposited either through wet or dry from tall (more than 20 m a.g.l.) release heights.
deposition processes. The contribution from “low” sources, both
The dispersion and removal processes are point and mobile, therefore often dominates the
governed by the local meteorological conditions, pollutant concentrations at ground levels inside
which also vary heavily with the physical location the urban area.
of the city. Therefore, air pollution concentrations A steady growth in vehicular transport and
in an urban environment are naturally the result of centralization of domestic heating have made
local emissions as well as contributions from pol- road traffic the most important source of urban
lution transport from more remote sources air pollution in many countries including most of
(Fig. 1). the industrialized nations [7].
Also of importance to the local contribution to There are usually significant differences between
urban air pollution are demographic/geographic developed and developing countries when compar-
factors such as the size of the city domain and ing emissions from different industrial sectors. With
the density of pollutant emissions inside the respect to the local contribution from the various
domain [5]. sectors, a comparison of two so-called megacities
The temporal pattern in urban air pollution (Beijing and Paris) showed that aerosol particles and
levels varies as a function of the local releases. volatile organic compounds (VOCs) have a com-
However, it is the variations in the meteorological plex and multi-combustion source in Beijing,
parameters that govern the dispersion and the whereas a single traffic pollution source completely
pollutant transport into and out of the city from dominates the urban atmospheric environment in
surrounding rural areas. Paris [8].
The temporal variations in emissions and mete- Both municipalities recognize the above and
orology are not the only contributors; the emission are taking steps to improve air quality.
release height also plays an important role with Although ambient air quality is that which is
respect to how quickly the air pollution is dis- often the subject of research and the type of pol-
persed and deposited, with air quality generally lution which is heard about (and the subject of this
improving with areas with very tall and entry), indoor air quality cannot be forgotten.
Urban Air Quality: Sources and Concentrations 199

Since many of us spend most of our time indoors, especially in China where the pollution load in
indoor air quality is a major health concern and megacities like Beijing, Shanghai, Guangzhou,
may be worsened by the location of the office or Shenzhen, and Hong Kong is substantial and air
home in the urban environment. quality can be greatly affected (Photo 1).
The issue, as with case of ambient air quality, is In these cities, between 10% and 30% of days
generally worse in the developing countries. exceed the so-called grade II national air quality
Emissions from household use of fossil fuels in standards [11] by a factor of three to five times that
the year 2000 were estimated to account for of the WHO AQG (air quality grade). These cities
1.6 million deaths, mainly among women and experienced a 10% growth in traffic each year over
children in the poorest countries [9] that are the last 5 to 6 years. Therefore, even with enhanced
being exposed to elevated pollutant levels in the emission controls, NO2 and CO concentrations have
indoor environment. remained almost constant over the same period
The actual ambient air pollutant load and there- of time.
fore average air quality greatly vary from one city Air quality indices (AQIs) are commonly used
to another, but, generally, major urban areas as tools in air quality management. A description
throughout the world have poor air quality, and, of widely used indices and how they are expressed
among these, the cities in the developing countries mathematically is given in Gurjar et al. [12]. AQIs
face the greatest challenges. may be designed to handle single or a multitude of
WHO has compiled a survey on typical ranges pollutants, and they may also be used for compar-
in ambient air concentrations of four indicator ing the loads in different municipalities or describ-
pollutants, summarized in Table 1. ing the current load in relation to average loads or
air quality standards and target values.
Urban Air Quality Concentrations and Indices In an example of a multicomponent AQI (the
The greatest levels of pollutants like PM10 and SO2 authors applied the term MPI), a comparison over
are presently found in urban air concentrations in megacities throughout the world showed that the
Africa, Asia, and Latin America, whereas the highest MPI values were found for Dhaka, Beijing,
highest levels of secondary pollutants Cairo, and Karachi with values about double those
(i.e., produced via reaction in the atmosphere with of Delhi, Shanghai, and Moscow [12] (Fig. 2).
primary pollutants) like O3, PAN, and NO2 are
observed in Latin America and in some of the larger
cities and urban areas in the developed countries. Sources in Urban Airsheds
The environmental and human health impacts
are particularly severe in megacities which are Urban airsheds are the areas in and around the
cities of about ten million or more inhabitants [10]. urban areas where air mass generally reaches a
Urban air pollution has thus become one of the steady state given that they are facing stable,
main environmental concerns in Asia and normal meteorological conditions.

Urban Air Quality: Sources and Concentrations, average maximum concentrations of O3 for different
Table 1 Ranges in annual average urban ambient air regions, based on a selection of urban data. (Reproduced
concentrations (mg m3) of PM10, NO2, SO2, and 1 h from [65])
Annual average concentrations 1 h max concentration
Region PM10 NO2 SO2 O3
Africa 40–150 35–65 10–100 120–300
Asia 35–220 20–75 6–65 100–250
Australia/New Zealand 28–127 11–28 3–17 120–310
Canada/United States 20–60 35–70 9–35 150–380
Europe 20–70 18–57 8–36 150–350
Latin America 30–129 30–82 40–70 200–600
200 Urban Air Quality: Sources and Concentrations

Urban Air Quality: Sources and Concentrations, Photo 1 Photo from a Beijing Hotel, October 2008, showing
reduced visibility due to the poor air quality. (Photo by M. Goodsite)

Tokyo
New York
São Paulo
Mumbai
Kolkata
Shanghai
Buenos Aires
Delhi
Los Angeles
Osaka-Kobe
Jakarta
Beijing
Rio de Janeiro
Cairo
Dhaka
Moscow
Karachi
−2.5 −1.5 −0.5 0.5 1.5 2.5

Urban Air Quality: Sources and Concentrations, The plot is reproduced from Gurjar et al. [12]. 30% of the
Fig. 2 Megacities pollution indices (MPI) based on mea- local NOx contribution is related to aircraft, whereas the
surements of the classical air pollutants and aggregated remaining 95% to 70% is from road traffic [15]
into an index for total pollution level (multi pollutant).

There are many potential sources in urban Airports are usually located in the vicinity of
areas that are generally located physically away larger cities and often mentioned as potential
from the urban center but still have to be consid- sources of high pollution loads in the urban areas
ered as a part of the urban airshed. Airports are (note: the haze in Photo 2a at the Delhi airport is
one of these. probably not from the airport activities alone but
Urban Air Quality: Sources and Concentrations 201

Urban Air Quality: Sources and Concentrations, rainfall from the Delhi University Main Campus, showing
Photo 2 (a) and (b) Delhi in July 2010, immediately the effectiveness of wet deposition in improving air quality.
prior to rainfall at the Delhi airport and immediately after (Photos: M. Goodsite)

from the dust-producing construction activities contribution from the harbor had very limited
and traffic around the airport). impact on the local air quality in comparison
Several studies have thus been carried out to with the emissions taking place in the urban
determine the potential impact of emissions from environment.
airport activities. These studies generally point at the Wood combustion in households is a concern
main influence on air quality that is coming from the in areas with many wood stoves. These areas have
road traffic going to and from the airport, whereas relatively high local emissions of PM in compar-
the impact of aircraft emissions has been found to be ison with other anthropogenic pollution sources
very limited. A study carried out in Frankfurt Air- generally in the airshed. Investigations of wood
port showed that aircraft-specific emissions gener- combustion and air quality in developed countries
ally could not be identified, whereas emissions from like New Zealand [18], Sweden [19], the USA
vehicle traffic on surrounding motorways had mea- [20, 21], and Denmark [22] have documented
surable impact on the air quality [13]. A study from that residential wood combustion likely signifi-
Munich Airport had similar findings [14], as did a cantly elevates the local PM concentrations in
study inside Heathrow Airport [15]. outdoor air. Emission inventories for Denmark,
Ship traffic has been estimated to be responsi- where wood-burning stoves are generally second-
ble for about 60,000 lung cancer and cardiopul- ary sources of domestic heating, point at wood
monary deaths annually [16], but this outcome is combustion as the largest anthropogenic source of
linked to the contribution from ship emissions to primary particle emissions in the country, being
the background particulate matter load and not responsible for about 60% of the countrywide
directly related to contribution from ship emis- primary particle emissions.
sions to the urban air quality.
Harbors may never the less be a local source
contributing to urban pollution as they are often Impact of Physical Parameters:
part of the urban airshed in coastal areas, but Geography, Topography, and
studies indicate that as with airports, that local Meteorology
road traffic often dominates the contribution
from harbors. For example, a study in the harbor Impact of Geography
of Aberdeen thus showed a gradient of increasing The location of the city has a great impact on the
NO2 and soot concentrations from the harbor dispersion conditions and thus air quality as it
toward the city center [17], indicating that the affects the local meteorological conditions. Los
202 Urban Air Quality: Sources and Concentrations

Angeles, for example, is situated in a valley with Katabatic winds may lead, for example, to high
stagnant conditions during temperature inver- levels of local dust with resulting air quality
sions. The stagnant conditions lead to very low issues, though their occurrence is highly location
wind speeds, and this results in little air exchange specific. The warm and dry foehn wind formed on
between the valley and the surrounding areas. The the backside of a mountain chain, for example, on
hot and sunny climate and high emissions from the north side of the European Alps, is another
traffic, industry, and other sources make the valley example. As the wind flows over the mountain,
act like a large pollutant reaction chamber, and the air mass is cooled and releases moisture. The
this is ultimately leading to high concentrations of air is subsequently warmed as the air mass flows
photochemical products like ozone, nitrogen downhill. This system may then form an inversion
dioxide, and peroxyacetyl nitrate (PAN) with the with the effect of reducing the dispersion of local
resultant degradation of air quality. air pollutants.
Wind speed through a city plays an important
role. For example, nitrogen oxide (NOx) levels in Impact of Meteorology
the street Via Senato in Milan, Italy, compared Ambient temperature in the urban atmosphere of
with the street Jagtvej in Copenhagen, Denmark, larger cities is usually a couple of degrees Celsius
show similar concentrations at the two sites higher than that found in the surrounding rural
despite the much higher traffic load in the street areas due to the so-called urban heat island effect
of Copenhagen [23]. This is directly the result of [24]. The phenomenon is due to the much smaller
generally higher wind speeds in Copenhagen reflection or albedo of the city as compared with
compared with Milan. High wind speeds and neu- its surrounding area and therefore absorbs more
tral conditions prevail in Copenhagen, whereas energy, to release it later in the form of heat.
low wind speeds and stable or near stable condi- There is in addition a high consumption of
tions are frequent in Milan. Copenhagen has a energy inside the city, as a result of domestic
cold coastal climate, whereas Milan has a warm heating and intense road traffic, which further
subtropical climate, and the local wind conditions contributes to the higher releases of heat than
are furthermore affected by the location inside the rural surroundings. Buildings act as heat reser-
Po Valley. Air quality planners must take their voirs, so the city has a less pronounced diurnal
own geography into consideration. temperature variation compared with the rural
area. Lastly, buildings and other urban construc-
tions form a physical barrier for the wind flow.
Impact of Topography This shielding leads to less cooling of the surfaces
Most cities have characteristic wind systems as a inside the city.
result of local topography. An example is the In calm weather, an urban circulation cell,
rising air over a warm mountain side during day- so-called heat island circulation, may be formed
time often leading to local formation of clouds and by warm air rising from the city. As it moves away
the subsequent release of precipitation. from the city, the heated air may sink and then, in
During the night the system reverses, and the another circulation, be returned to the city at a low
cooling of the air in the mountain valley leads to altitude. A similar phenomenon is known in
stable conditions which may lead to local air pol- coastal regions, where a sea breeze may be formed
lution problems. The impact of katabatic winds is as a result of the temperature difference between
another example affecting cities along the Norwe- the sea and land surfaces.
gian coast. Katabatic winds are formed when cold A study in London showed that due to the heat
air masses move downslope (katabatic is Greek island circulation over the city, the wind speed is
for moving downhill) and meeting the colder never below about 1 m s1 [25]. Therefore, the
snow and glacier covered areas, which then cool heat island effect is very important during low
the air mass further as it continues flowing wind speed conditions in urban areas where it
downhill. may dominate the dispersion and thereby be the
Urban Air Quality: Sources and Concentrations 203

limiting factor for the highest local air pollution in the urban area (typically this will be the traffic
concentrations and therefore local air quality. The in surrounding streets) and (2) the regional
urban heat island effect may thus be the limiting (sources within a distance of a few hundred km)
factor for the highest pollution concentrations and and long-range transport (sources placed up to
thereby air quality parameters in the urban thousands of km away) of air pollution.
environment. The pollutant levels in the urban streets are
strongly affected by the emissions from traffic
taking place on the street itself. The concentration
Pollutant Dispersion in Urban Streets level and the distribution of air pollution inside the
street canyon (the street “boxed in” by buildings
Pollution “hot spots” are areas where large con- on each side) are largely governed by the sur-
centrations of pollution are emitted or concen- rounding physical conditions. These physical
trate. In urban areas, trafficked streets are air conditions heavily affect the wind speed and the
pollution hot spots (Fig. 1). The concentration wind direction inside the street, with residence
inside the urban street is generally the result of time for an air packet in the vicinity of an urban
two contributions, one from emissions from the street usually on the order of seconds to a few
local traffic in the street itself and one from back- minutes depending on the street topography. This
ground pollution entering the street canyon from means that only very fast chemical conversions of
above roof level [26]: pollutants have time to take place [26].
C ¼ cb þ cs The airflow generated inside the streets and
around building obstacles may result in very different
where c is the concentration in the street, cb the concentration levels at different places in the street.
urban background contribution, and cs the contri- The street canyon vortex flow (Fig. 3) physically
bution from traffic inside the street itself. The governs the pollutant distribution inside the street
background contribution arises from two contri- canyon. The street canyon is characterized by the
butions: (1) the contribution from nearby sources presence of tall buildings on both sides of the street.

Wind
Background pollution

Recirculated pollution

Leeward Windward
Direct emission

Urban Air Quality: Sources and Concentrations, Pronounced differences – up to a factor of 10 in air pollu-
Fig. 3 Illustration of the flow and dispersion inside a tion concentrations on the two pavements – are the result of
street canyon. The wind above roof level blows perpendic- these flows. Air quality on one side of the street might thus
ular to the street in the above figure, thus creating a vortex be poorer than on the opposite side of the street, if there are
inside the street canyon with the wind direction at street prevailing winds
level opposite to the wind direction above roof level.
204 Urban Air Quality: Sources and Concentrations

Within the vortex relatively clean air flows from NO2 in the exhaust, this value may in some
rooftop height and down the windward face of the regions be now up to as much as 40% [29]. This
street, across the road at street level, in the reverse of extremely simple chemical mechanism of two
the wind direction at roof top, thus transporting the reactions and a direct emission describes very
pollutants from the road level traffic to the leeward well the concentrations of NO2 inside urban
face of the canyon. The result is that pollution streets [27]; for many cities it may also be applied
concentrations are up to ten times higher on the for describing NO2 concentrations in urban back-
leeward side compared with the windward side of ground air (see [6] documenting this the case for
the street. This means that air quality depending on many Northern European cities).
prevailing wind conditions may often be much The use of catalytic converters in automobiles
poorer on one side of the street than another. has in recent years led to a major reduction in NOx
concentrations in the urban streets of many indus-
trialized countries.
Nitrogen Dioxide Pollution in Urban For several reasons NO2 levels have not
Areas followed the same trends (Fig. 4). Part of the
explanation is the chemical conversion of NO to
For example, the chemistry of nitrogen oxides NO2 in the reaction with O3, but the other expla-
[NOx: the sum of nitrogen monoxide (NO) and nation is, as mentioned above, the increased frac-
nitrogen dioxide (NO2)] in urban streets may be tion of NO2 in the NOx emission from vehicles
described by only two reactions: the reaction with catalytic converters.
between ozone (O3) and NO forming NO2 and Despite the overall reduction in NOx emis-
the photodissociation of NO2 [27]: sions, this is contributing to elevated NO2
concentrations.
NO þ O3 ! NO2 (1)

 The Impact of Particle Pollution


NO2 þ hv ! NO þ O 3 P (2)
 Ambient urban air contains a complex mixture of
O 3 P þ O2 ! O3 (3) particles from natural and anthropogenic sources
of varying sizes and chemical composition
where O(3P) is ground state atomic oxygen. Reac- [30–34]. The particle size is crucial for the atmo-
tion (3) is very fast, and therefore for most practi- spheric fate [35] and the human health impact as
cal applications, it may be disregarded. The both the particles’ atmospheric behavior and their
products of reaction (2) may thus be considered deposition in the human respiratory system is
to be NO and O3. governed in part by its size [36]. Particles in
NOx is therefore mainly emitted as NO and, to ambient air generally appear in two rather distinct
a lesser extent, NO2. size classes (referred to as “modes”) usually
Long-term exposure to elevated NO2 levels is a termed fine particles (diameter: 0.l–2.5 mm) and
health hazard and may decrease lung function and coarse particles (diameter: >2.5 mm). In addition,
increase the risk of respiratory symptoms such as it is common to talk about the ultrafine particles
acute bronchitis, cough, and phlegm, particularly (diameter: 0.01–0.1 mm or 10–100 nm) that usu-
in children [28], whereas NO at current ambient ally dominate the number concentrations (Fig. 5).
air concentrations is (considered to be) harmless.
The fraction of NOx directly emitted as NO2 Particle Mass Concentrations
used to be only about 5 to 10% in countries with a Mass concentration of particles <10 mm
small fraction of diesel engines. However, due to and <2.5 mm in aerodynamic diameter (PM10
the use of catalytic converters and an increasing and PM2.5) is generally used as an indicator for
number of diesel engines with high fraction of suspended particulate matter (e.g., regulated in
Urban Air Quality: Sources and Concentrations 205

Jagtvej, Copenhagen H.C.A. Boulevard, Cph


Banegaarsgade, Aarhus Albanigade, Odense
Vesterbro, Aalborg
300
250
µg(NO2)/m3
200
150
100
50
0

70
60
50
µg(NO2)/m3

40
30
20
10
0

Urban Air Quality: Sources and Concentrations, the time period 1982 to 2005 and illustrate a decrease in
Fig. 4 The measured trend in annual mean concentrations NO concentrations resulting from increasing number of
of NOx and NO2 (both shown in mg (NO2)/m3) at the street vehicles with catalytic converters in Danish vehicle parc
stations in the largest Danish cities: Copenhagen, Aarhus, but also illustrate that this decrease is not reflected in the
Odense, and Aalborg. The upper plot shows NOx and NO2 concentrations that have remained more or less con-
lower plot NO2. The plots include measurements from stant during this time period [63]

EU directives) and routinely measured at many particles in terms of the number concentration.
locations throughout the world. Particle mass is Most studies to this point of the health effects air
dominated by particles >0.1 mm in diameter. Par- particles have been related to particle mass. Neither
ticles in traffic exhaust are mainly in the ultrafine of the mechanisms are yet fully understood, and the
fraction and include elemental carbon (EC) as need for more studies has been called for [39].
well as organic carbon (OC) [37]. The ultrafine With respect to streets with a high level of
mode particles from traffic sources contribute vehicular traffic, a significant fraction of the par-
considerably to the PM number concentrations ticle pollution originates from this traffic [40]. The
but only little to the PM mass. direct emissions from car exhaust contain parti-
While some health studies have demonstrated a cles formed inside the engine as well as in the air
relationship between both acute and long-term just after leaving the exhaust pipe. The latter
health effects and the ultrafine particle mode depend on the sulfur content in the fuel.
(particle diameters <0.1 mm) [38], other studies Studies have shown that reducing the sulfur
are less conclusive concerning the health effects content in diesel significantly reduces the particle
of the ultrafine mode particles. Even though ultra- number concentrations in urban streets, and this
fine particles are a minor contribution to total par- parameter is therefore important for air quality
ticle mass concentration, they represent most of the planning and management.
206 Urban Air Quality: Sources and Concentrations

Number Mass

Coarse
Condensates and Secondary particles
(wear of tires, road
other primary (long range transport)
construction work and
particles (mainly
natural sources)
traffic)

Soot (traffic) Dust from brakes


(traffic)

0.001 0.01 0.1 1 10 100 µm

Nano particles
Ultrafine particles
PM2.5 (fine particles)
PM10

Urban Air Quality: Sources and Concentrations, particles. The dashed line is the number distribution, dom-
Fig. 5 Typical size distribution of particles in urban air: inated by ultrafine particles. Note that one particle with a
both as mass and number concentration. The horizontal diameter of 10 mm has the same weight as 1 billion parti-
axis is the particle diameter in mm. The black line is mass cles with a diameter of 0.01 mm [64]
distribution, dominated by the coarse and secondary

Directly emitted particles are mainly found in high NOx emitters such as diesel vehicles
the ultrafine particle fraction of the total particle (especially heavy-duty vehicles) are also the
concentration. Traffic, however, also contributes to high particle emitters (when these are expressed
the mechanically formed particles in the fine and in particle number concentrations) [41].
especially the coarse fraction, typically produced The Danish Operational Street Pollution
from wear of tires and brakes, wear from road Model (OSPM) [42] is an example of a numerical
surface material, as well as resuspended dust. model that, through its calculations, has been
For the particle mass (PM10), long-range trans- shown to reproduce well the observed particle
port is usually the dominating source for regional number, when treating particles as inert tracers
background levels. Studies have shown that less (i.e., by disregarding transformation and loss pro-
than 10% of the urban PM10 originate from local cesses) [43]. The particle emission factors depend
urban sources [40]. For NOx as well as particle on ambient temperature with higher emissions at
numbers, a larger difference between the urban, lower temperatures, which is accounted for in the
rural, and curb side levels has been observed, simulations reported in [44] and other refined
indicative of a large contribution from local traffic numerical models.
sources (Fig. 6). Long-range transport, however, is a significant
contributor to fine fraction particles and leads to
Particle Number Concentrations the main part of particulate sulfate and ammonium
A high correlation (one study [40] found R > 0.9) and a large part of particulate nitrate. These sec-
between concentrations of NOx and total particle ondary particles are formed from anthropogenic
number indicating that both components of air sulfur dioxide (SO2), ammonia (NH3), and NOx
pollution originate from the same (traffic) source. emissions [45] and often constitute more than
The correlation is seen as the components are 30% of the PM10. A separate fraction of particu-
emitted in a similar ratio (particle number: NOx) late nitrate appears in the coarse mode, which also
from different traffic categories; in other words, contains contributions from sea spray and
Urban Air Quality: Sources and Concentrations 207

Concentration relative to urban background (=100)


600
Curb side
500 Urban background
Near-city location
400 Rural background
300

200

100

80

60

40

20

0
ToN PM10 NOx

Urban Air Quality: Sources and Concentrations, Copenhagen, Denmark. The concentration bars are
Fig. 6 Comparison of average concentrations of total stacked, so only the additional contributions are marked
particle number (ToN), particle mass (PM10), and NOx at with the pattern shown in the legend. Note that the scale of
rural, near-city, urban, and curb side measurement stations the vertical axis changes at 100. (Adapted from Ketzel et al.
relative to urban background levels in the area of [40])

resuspended dust [46, 47] with relatively large station in the urban center and one on the out-
mass and thus quickly deposits by gravitational skirts. There is a real risk of comparing sites in the
settling, such as road dust. vicinity of large pollution sources with sites at
Due to the quick deposition, coarse particles, some distance from local sources. The location
therefore, generally have a relatively short life- of measurement stations must be very carefully
time in the atmosphere when compared with fine considered, and it is not generally good enough to
particles. just replicate what another town is doing. For all
Particles of low-temperature combustion pro- the physical and anthropogenic factors previously
cesses from wood-burning stoves and other discussed, locating stations is critical and must be
poorly controlled burning processes may be soot done in conjunctions with city planners. Recently
particles which often have high contents of poly- in the Danish press, scientists speculated if air
cyclic aromatic hydrocarbons (PAH) and other quality levels improved as a result of newly laid
carcinogens or just generally degrade the air qual- road tar thus keeping down the dust at a roadway
ity in the urban environment, despite the “charm” at the measurement station.
or, in developing countries, necessity, for burning In addition to the ambient measurements, mod-
with these methods. ern air quality management is starting to consider
locating measurement stations where many peo-
Air Quality Measurement Locations ple spend most of their time: indoors. Exposure to
When comparing observed levels of particulate air pollution in the home is an important fraction
matter or air quality in different cities, aside of a person’s overall exposure. A Danish study in
from assuring that the indices are the same, the an uninhabited apartment in central Copenhagen
location of the monitoring stations must be con- revealed that particle pollution inside the apart-
sidered, as they may be very different. An index ment was to some extent linked to the activity
that reports the “average” might consist of a level of the neighboring apartments [48]
208

Annual average PM10 concentrations in selected cities worldwide

Interim target-1 Interim target-2 Interim target-3 Air quality guidelines


240
Asia Latin America Africa Europe
200

160

120

80

40

0
Oslo

Lima
Turin

Quito
Cairo
Milan
Erfurt
Basel

Seoul
Berlin

Tokyo

Taipei
Rome
Leeds
Dallas

Zurich

Busan

Dhaka
Seville

Manila

Beijing
La Paz
Vienna
Athens
Seattle

Bogotá
Praque
Munich
London

Cracow

Karachi
Calcuta
Havana
Pittburg

Geneva

Helsinki
Warsaw

Mumbai
Bologna

Palermo
Cologne
Houston

St. Louis

Brussels

Bangkok
Florence

Santiago
Knoxville

Colombo
Arequipa
Meddelin
Memphis

Hamburg
New York

Fortaleza
San Juan

Shanghai
Budapest

Bucharest
Barcelona

New Delhi
Katmandu
Sáo Paulo

Gangzhou
Stockholm
San Diego

Cape Town

Hong Kong
Amsterdam

Mexico City
Vereeniging
Los Angeles

Copenhagen

Cochabamba
San Salvador
Johannesburg

Rio de Janeiro
Belo Horizonte
Oklahoma City

Guatemala City

Ho Chi Min City


Washington DC

Urban Air Quality: Sources and Concentrations, Fig. 7 PM10 concentrations is defined at the lowest level at which total, cardiopulmonary and lung cancer mortality
(mg m3) in selected large cities throughout the world. The plot has been derived on has been shown to increase with more than 95% confidence in response to long-term
basis of WHO (2006) [1]. The WHO Air Quality Guideline (AQG) (shown in the figure) exposure. Shown also are the WHO interim target values 1 to 3
Urban Air Quality: Sources and Concentrations
Urban Air Quality: Sources and Concentrations 209

indicating that sources in the neighboring envi- previously commonly employed measurement
ronment must also be considered in the analysis of techniques produced artifacts. Despite the toxico-
overall exposure. Measuring air quality is there- logical profile of PAHs, no country has mandatory
fore not a simple matter of purchasing machines. guidelines with respect to their ambient air quality
They need to be carefully located, and the mea- standards [54].
surements are best coupled with other data such as
meteorology and with numerical models that help Sampling Artifacts in Measuring PAHs
provide additional value with the measured In order to reduce the risk of sampling artifacts [52]
numbers. in the spring of 2003, the Mexico City Metropolitan
Area (MCMA) air quality campaign employed three
Natural Sources independent methods to measure particle bound
A 2006 WHO study (Fig. 7) indicates that PM10 PAHs [57, 58]. Peak concentrations of PAHs on
concentrations in Asia and Latin America are the order of 120 ng m3 during the morning rush
higher than are observed in Europe and North hour were observed in excellent agreement that 20%
America [1]. The highest particle levels are of the vehicles account for 50% of the PAH emis-
observed in Asia and are attributed to forest sions [59]. Like other atmospheric gaseous and
fires, poor fuel quality, and aeolian (windblown) particulate constituents, PAHs are removed from
dust. Wind erosion originating especially in the the atmosphere by wet or dry deposition and may
deserts of Mongolia and China contributes to the also be converted or degraded in heterogeneous
general level of PM in the region. processes. Despite the systematic approach, there
may have been significant concentrations of very
toxic and very reactive PAHs in the MCMA atmo-
Polycyclic Aromatic Hydrocarbons (PAH) sphere that were missed due to filter reaction arti-
and Urban Air Quality facts [58], thus attesting to how complicated
measuring PAHs is as a part of air monitoring pro-
Sources and Emissions of PAHs grams and the need for further development.
Polycyclic aromatic hydrocarbons are a group of
chemicals that are formed during incomplete Long-Range Transport of PAH
burning of coal, oil, gas, wood, garbage, or other Together with the local emission, the long-range
organic substances, such as tobacco and transport of PAHs is of a concern. PAHs are desig-
charbroiled meat. There are more than 100 differ- nated as one of the persistent toxic substances in
ent PAHs. PAHs generally occur as complex mix- central and northeast Asia under the Stockholm
tures normally as part of combustion products Convention (UNEP, 2002). It has been demonstrated
such as soot, not as single compounds. that transformation processes can lead to PAHs
PAHs can also be found in materials such as which are more toxic than their precursors [57].
crude oil, coal, coal tar pitch, creosote, and roofing The source apportionment of particulate PAHs
tar. There are numerous other sources [49, 50]. at Seoul, Korea, during a measurement campaign
In the air they are either attached to dust parti- between August 2002 and December 2003 was
cles or as solids in airborne soil or sediment. This is analyzed [60] by applying the US EPA
of great concern due to the mutagenic [51] and (2004) chemical mass balance (CMB) model.
carcinogenic [52] properties of PAHs; the US Seoul is in the atmospheric footprint of major
Agency for Toxic Substances and Disease Registry coal-burning industries and power plants of China
[50] has listed 17 PAHs as of priority concern with and Japan, as well as contributing itself to the
respect to their toxicological profile. Northeast Asia particle footprint. In Seoul, just
PAHs that have been studied in urban and other as in the MCMA, gasoline and diesel vehicles
areas appear to represent only a fraction of a accounted for 31% of the measured PAHs and
percent of the ambient particle mass [53]. How- thus were the major sources. Daily and seasonal
ever, there are compelling arguments that the variations were noted and attributed to differences
210 Urban Air Quality: Sources and Concentrations

in biomass burning and coal (heating) with a 19% distribution and relate these to the potential adverse
difference in the total concentrations observed health effects in the urban population [62].
between fall (63%) and winter (82%). The sources Humans are exposed to metals via ambient air
showed an inverse profile when moving away inhalation and consuming contaminated food or
from the city. The study authors used source anal- water, as well as, in the case of lead and children,
ysis to attribute this to the long-range transport of chewing on lead painted toys and exposure from
atmospheric pollutant (LRTAP) of PAHs and their walls or furniture. Metals were of great concern in
precursors from sources in China or North Korea western cities prior to lead being banned as an
thus demonstrating that for certain urban environ- anti-knock agent in gasoline in the mid-1970s, as
ments, in footprints of major industrial areas, well as other regulations regarding the use of lead
PAHs from local and long-range transport must in, for example, house paints.
be taken into greater consideration as air quality The US Environmental Protection Agency
management plans are updated. (US EPA) lists many trace metals as among the
worst urban air toxics (www.epa.gov/ttn/atw/nata/
34poll.html, November 28, 2008), and several
Trace Elements to Include Heavy Metals metals aside from mercury and lead are classified
in Urban Areas by the US Clean Air Act as HAPs: chromium,
manganese, nickel, and cadmium. There is no
Trace elements including heavy metals (HM) are reason that other countries should not also endorse
ubiquitous in the atmosphere of urban areas, and this classification in their air quality plans.
many are classified by authorities as hazardous air
pollutants (HAP). Trace Elements in the Urban Atmosphere
These represent serious environmental and Trace elements (and metals) and the observed
health risks and are especially of concern in urban high levels of them in the urban environment
and industrial climates, with megacities in devel- have led to extensive monitoring with consequen-
oping nations being the obvious sites of concern tial regulations and international agreements that
for populations at risk for trace element exposure. have greatly reduced the concentrations.
Air quality can be affected and trends in urban The sources of emission into the urban atmo-
areas have been noted. One study has provided sphere of commonly measured trace elements, Be,
trends and levels of trace metals in three Danish Co, Hg, Mo, Ni, Sb, Se, Sn, and V, with smaller
cities as well as at background sites [61]. The concentrations of As, Cr, Cu, Mn, and Zn, are
levels reported are less than literature values for primarily human activities, especially the com-
megacities, as expected, but in many cases, the bustion of fossil fuels and biomass, industrial
trends are similar, though the numbers of studies processes, and waste incineration [62].
are very limited. As with PAHs, there are seasonal variations of
trace metals in PM10 and PM2.5 observed in cam-
Heavy Metals in the Urban Atmosphere paigns conducted seasonally. Higher winter values
Heavy metals are still a problem for ambient and of nearly all trace elements are observed suggesting
indoor air quality, especially in general in urban a significant source of particles from domestic
and industrial areas despite that many nations have heating in most temperate urban areas and/or less
tightened and continue to restrict emissions of such efficient dispersion of emissions in winter.
trace elements as mercury. Even with history of Many trace elements are primarily observed
progressive regulation of trace metals, they still from natural sources and have local, regional, and
represent a real and pressing health and environ- global effects. Sources include sea spray near coast-
mental hazard in the USA (US EPA 2006) and lines, dust from aeolian processes and weathering
most certainly in other western nations and other (especially noted in Asia), and volcanoes.
countries as well. Trace metals have been measured The main source of trace elements in most urban
in nearly all aerosol size fractions, so it is of para- environments is never the less, anthropogenic
mount importance to characterize the particle size activities, and national regulations, especially
Urban Air Quality: Sources and Concentrations 211

regarding limits in gasoline, and emissions from particularly severe in the megacities, where qual-
coal-fired power plants, as well as other industrial ity of life is lessened due to air pollution. The
control, are in most cases effective in mitigating interaction of poor air quality with other lifestyle
their emissions. Thus, developing nations gener- decisions such as smoking generally results in a
ally have higher levels in general than industrial- synergistic effect. The negative health effects of
ized nations. poor ambient air quality are likely enhanced by
exposure to tobacco smoke, indoor particulate,
and gaseous sources from cooking, candles,
Conclusions stoves, etc. but also by exposures to the non-
airborne agents in textiles, food, etc. The possibil-
Urban air quality is subjectively determined based ity of reduced productivity from toxics and their
on levels or concentrations measured, monitored, associated costs should be investigated, and valu-
and mandated generally by law. Urban air quality ation models should be further developed [5].
is the resulting state of a function of a complex Even though the health effects of poor urban air
and dynamic mixture of gaseous and particulate quality have been documented in numerous stud-
pollutants emitted from natural and human envi- ies, there are still many unknowns, and through
ronments and their interaction with the natural and their investigation, there is a possibility for improv-
built environment. The concentration of pollut- ing health, environment, and the climate. The
ants both produced in photochemical reactions reader is referred to Hertel and Goodsite, 2009
and suspended in the air of the urban environment [65] – from which this entry was based and
and therefore air quality is weather dependent and updated, as well as the supplemental literature list
thus exhibits daily and seasonal variation due to where we have included recent reviews across
both anthropogenic and biologic activity levels various aspects of the field of urban air quality.
and weather conditions.
The actual pollution load in a given urban area
is the result of both local conditions and emissions
and transport from nearby and remote sources. Future Directions
The location of the city is very important for the
local dispersion conditions, which are governed Given the progress documented through 25 specific
by meteorology but are also heavily affected by solutions in “Air pollution measures for Asia and the
natural topographical conditions (e.g., effects of Pacific 25 science-based solutions to bring clean,
coastline, mountains, valleys, etc.). safe air to 1 billion people” http://www.ccacoalition.
Studies of the impact of transportation hubs org/en/content/air-pollution-measures-asia-and-paci
such as local harbors and airports on urban air fic, it is important to follow the recommendations
quality have generally pointed at a limited influ- made in the report. Investigating to what extent
ence, with the impact on the air quality mainly deploying the solutions will continue to improve
related to the road traffic that these facilities are urban air quality and in which context, in the studied
generating. regions and other urban regions, given increasing
The highest urban air pollutant concentrations urbanization, is needed as soon as feasible. The
of the pollutants PM10 and SO2 are generally general understanding of urban air quality within
found in developing urban environments such as the broader political, economic, social technologi-
those in Africa, Asia, and Latin America. cal, environmental, and security (PESTLES) frame-
The highest levels of photochemical pollutants work needs to be developed. Ye et al. [66]
such as O3 and NO2 are observed in Latin Amer- documented that there are cultural aspects that
ica and certain developed countries – topograph- must be taken into consideration. The understanding
ical conditions and weather conditions are very of culture and communications toward changing
important factors in this respect. practice is important to continue to understand effec-
The negative health effects of urban air pollu- tive deployment of mitigative measures and political
tion are well documented and are found to be or technological solutions in urban areas.
212 Urban Air Quality: Sources and Concentrations

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Primary pollutants Those emitted directly to
Urban Atmospheric the atmosphere, typically from mechanical or
Composition Processes combustion processes.
Secondary pollutants Those formed within the
William Bloss atmosphere by chemical reactions.
School of Geography, Earth and Environmental Street canyon The semi-isolated atmospheric
Sciences, University of Birmingham, compartment formed by adjacent rows of
Birmingham, UK multi-story buildings.
Temperature inversion An increase in temper-
ature with increasing altitude, which usually
Article Outline isolates ground-level air from the overlying
atmosphere, resulting in increased (primary)
Glossary pollutant concentrations.
Definition of the Subject Transboundary pollution The transport of
Introduction long-lived chemical species, such as O3 and
Historical Perspective CO, across national boundaries.
Meteorology, Dynamics, and Mixing VOC Volatile Organic Compound, one com-
Basic Composition and Key Pollutants monly found overwhelmingly in the gas phase.
Key Emission Characteristics VOC limited The ozone production regime
Urban Atmospheric Composition Processes where NOx is plentiful, and ozone production
Trends in Urban Atmospheric Composition is limited by the availability of hydrocarbons.
Future Directions
Bibliography
Definition of the Subject
Glossary
The majority of the population now live in cities
Boundary layer The lowermost layer of the (the 50% point was passed during 2007 [1]) and are
atmosphere, in contact with the surface and exposed to the urban atmosphere every day of their
well mixed. Extending from 100 to 200 m at lives. As global population has also doubled over
night, up to 1–2 km during the day. the past 50 years, urban air quality is a major factor
Mixing ratio The fraction of the air which a in pollutant exposure for billions of individuals.
given species comprises, typically parts per The urban atmospheric environment is unique,
million (106), billion (109) or trillion (1012), with the city landscape defining particular meteo-
by volume. rological characteristics, and a wide range and high
NOx The sum of nitric oxide (NO) and nitrogen density of emission (or pollution) sources, which
dioxide (NO2). combine to determine local air quality. Air pollut-
NOx limited The ozone production regime in ants, ranging from gases such as carbon monoxide,
which VOCs are (relatively) plentiful, and ozone ozone and nitrogen dioxide, to suspended particles
production is limited by the availability of NOx. of varying size and composition, have been shown
Photostationary steady state The rapid chemical/ to be linked to respiratory and cardiovascular
photochemical balance between a number of health issues. Urban atmospheric composition pro-
reactants, usually applied to NO, NO2 and O3. cesses affect the abundance of primary pollutants,
PM10 Suspended airborne particulate matter, and are wholly responsible for the formation of
with an aerodynamic diameter of 10 mm or less. secondary species such as ozone. In this article,

© Springer Science+Business Media, LLC 2012 215


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_493
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_493
216 Urban Atmospheric Composition Processes

the principle urban atmospheric components and Historical Perspective


their sources are introduced, followed by an
account of the predominant atmospheric composi- The history of urban atmospheric composition and
tion (chemistry) processes which affect urban air air pollution reflects developments in fuel usage for
quality. The article concludes with a brief consid- domestic heating, cooking, emerging industrial
eration of the potential impacts of future changes in activities and power generation, and the spread of
emissions, physical and political climates upon the internal combustion engine. The earliest reports
urban atmospheric composition. of atmospheric pollution issues, associated with the
combustion of coal for domestic heating and
cooking, and for industrial operations such as lime
production, are noted in historical documents dating
Introduction to at least the thirteenth century, when a Commis-
sion was established to address the problems asso-
Increasing population density implies an increasing ciated with coal smoke in London. By the sixteenth
human exposure to urban atmospheric pollutants. or seventeenth century, some of the earliest pro-
Countering this basic trend, growing scientific posals for “emission control legislation” such as
understanding of atmospheric composition pro- John Evelyn’s Fumifugium of 1661 were drafted
cesses, coupled with technological developments for (unsuccessful) presentation to Parliament
in emissions control and policy measures to limit [4]. Increasing domestic and industrial coal combus-
pollution, have led to improved urban air quality tion led to the London smogs of the nineteenth and
over the past several decades in many cities, twentieth centuries, in which the major pollutants
although this conclusion is dependent upon the spe- were highly acidic particulates and fog droplets
cies measured and metric chosen. The predominant arising from use of high-sulfur fuels. Another prom-
air quality conditions are therefore a strong function inent atmospheric pollution event of the time was
of the level of development of a city (Fig. 1), and the Donora Valley episode of 1948, in which local
have changed substantially over the past few industrial emissions of sulfur dioxide, carbon mon-
decades, with (in many cases) the removal of oxide and heavy metal particles were trapped in a
heavy industry from urban regions, while traffic week-long temperature inversion leading to tens of
has become the dominant emission source; the con- deaths and thousands suffering from respiratory ill-
cept of urban atmospheric pollution thus varies in ness. These events primarily concerned primary
time, and between different cities across the world. pollutants, those emitted directly to the atmosphere

First emission
controls

Start of Stabilisation Improvment Air quality


industrialisation of air quality of air quality standard
Air pollution level

High technology
applied

Extent of development (Time)

Urban Atmospheric Composition Processes, Fig. 1 Schematic representation of the evolution of air pollution
vs. development. (Adapted from Fenger [2]/Mage et al. [3])
Urban Atmospheric Composition Processes 217

(although strictly speaking sulfuric acid is formed multiple street canyons at rooftop level. Above the
within the atmosphere following the release of sul- canopy layer, the overlying boundary layer is
fur dioxide). Subsequent legislation, mandating the sometimes divided into the roughness sub-layer,
use of tall chimneys to aid dispersion, use of low- where building wake-induced turbulence effects
sulfur and smokeless fuels in populated areas, the predominate and atmospheric composition (as far
migration of heavy industry away from cities and as it relates to urban emissions) is highly variable,
the introduction of emissions control technologies and the higher inertial sub-layer which exhibits a
and policies (including emissions trading schemes more homogeneous composition [5].
on the case of SO2), have greatly reduced these Local wind speed and direction critically affect
pollution phenomena in many nations. Over the local pollutant levels – on a street canyon scale,
past 50 years, motor vehicle emissions have come winds perpendicular to the canyon may lead to the
to dominate urban atmospheric composition in most establishment of within-canyon vortices, leading
developed nations, as the global vehicle fleet has to the upwind side of the canyon, at ground level,
increased by an order of magnitude over this experiencing higher levels of primary pollutants
timeframe. (those from local traffic at least) – Fig. 2. Con-
In developing nations, combustion of biofuels versely, along-canyon wind effectively ventilates
(primarily wood) and coal for domestic cooking the ground-level emissions into the overlying
and heating remain major urban pollutant sources. boundary layer. While most pollutant levels fall
Alongside the reduction in some of the traditional with increasing windspeed as a consequence of
primary pollutants (sulfur dioxide, carbon monox- increased dilution, re-suspension of coarse partic-
ide), levels of secondary components formed in the ulate matter (dust, sand, tyre, and brake debris) is
atmosphere, such as ozone and (much of) nitrogen found to increase atmospheric PM (particulate
dioxide and particulate matter, have in many cases matter) levels at elevated windspeeds [6].
been rising, and have become the focus of concern. The ventilation of the urban airshed as a whole
affects the pollutant levels experienced for a
given emission source. Certain cities (notable
Meteorology, Dynamics, and Mixing examples include Mexico City, Santiago, Los
Angeles) are partially to almost entirely
The urban atmosphere may be defined horizon- surrounded by mountain ranges, leading to
tally by the extent of the particular city in question build-up of emissions within the (urban)
(see comments below regarding export of urban
atmospheric pollutants), and vertically as
encompassing the boundary layer, the first few Cb Mean wind, u-
100 m to kilometer or so of the atmosphere, Leeward side Windward side
which is regarded as well mixed. The urban C
boundary layer height determines the size of the
Building height

atmospheric compartment into which emissions


are mixed – a lower boundary layer height
(as commonly found at night) results in higher
concentrations for an equivalent emission E

strength, all other things being equal. The urban


boundary layer may be further divided into verti-
cal regions determined by the interaction between Street width
the city topography and airflow: At the street
scale, urban canyons, formed between rows of Urban Atmospheric Composition Processes,
Fig. 2 Typical within-canyon vortex circulation, driven
buildings, represent semi-isolated environments by overlying perpendicular airflow, increases primary pol-
into which traffic-related emissions are initially lutant levels on the upwind (leeward) side of the street at
discharged. The urban canopy layer encompasses ground level
218 Urban Atmospheric Composition Processes

boundary layer (e.g., Molina and Molina [7]). In Urban air pollution issues primarily relate to local
other locations, regional weather patterns lead to emissions and the chemical processing of pollutants
persistent patterns of pollutant exposure, for and natural atmospheric species which occurs on
example, the daily sea breeze circulation affect- timescales of a few hours to a few days. This can
ing Hong Kong and the Pearl River Delta be distinguished from the wider, regional impacts of
[8]. Local circulation patterns and topography air pollution (such as increasing background ozone
can therefore exacerbate, or ameliorate, the levels, and the abundance of sulfate aerosol),
atmospheric composition resulting from a given although these also impact on the urban environ-
emissions situation [9]; and the combined effects ment and are considered here. Global air pollution
of local and regional scale dynamics, mixing and issues related to long-lived species such as CFC,
chemical transformations must be considered in HCFC and halon compounds contributing to strato-
the development of urban air quality manage- spheric ozone depletion, and the climate-related
ment policies. issues associated with the global abundance of
longer-lived greenhouse gases such as carbon diox-
ide and methane, are not discussed further here –
Basic Composition and Key Pollutants although some urban air pollutants are also impor-
tant greenhouse gases, for example, ozone. Table 1
The bulk atmospheric composition is essentially gives typical abundances for key urban air compo-
constant throughout the troposphere, comprising nents which would be found in the remote boundary
gases such as nitrogen, oxygen, argon, helium, layer, away from anthropogenic emission sources,
carbon dioxide and a variable amount of water and compares these with those observed in selected
vapor. Most concern over urban atmospheric urban atmospheres. It should be noted that point
composition and air pollution arises from the measurements such as these may be representative
trace components – gaseous constituents such as of a local microenvironment only, rather than the
ozone, nitrogen oxides and volatile organic com- wider city-scale environment – if cities do not have
pounds, and suspended particulate material representative networks for air quality monitoring,
(PM) commonly referred to as aerosol (although this concern persists into reported pollution levels.
strictly the term denotes both the condensed phase As understanding of the impact of air pollut-
material and the gas it is suspended within). ants upon health has developed, various national

Urban Atmospheric Composition Processes, Table 1 Comparison of typical unpolluted boundary layer abundance
of selected pollutants, and their equivalent levels in various urban centers. All concentrations expressed in mg m3
Species Remote MBL London: MR London: NK Beijing Lagos
NO2 0.04 98 37 66 95
O3 58 18 34 109b 64
SO2 0.2 7.7 1.9 53 186
CO 140 650 280 2,100 6,700
Benzene 0.01 1.3 – 13.4a –
1.3-butadiene <0.01 0.57 – – –
PM10 – 27 17 161 228
PM2.5 – 18 11 130b –
Notes: Remote MBL (Marine Boundary Layer) data taken from the Cape Verde Atmospheric Observatory in the tropical
Atlantic Ocean [10, 11] except SO2, benzene, 1-3-butadiene from Mace Head. London NK (North Kensington) is an urban
background site while London MR (Marylebone Road) is a roadside monitoring station on a congested major road.
London data are annual averages (for 2010) taken from the UK Air Quality Archive (www.airquality.co.uk). PM data are
TEOM FDMS measurements. Beijing data are averages across the city for 2006, as given by [12] except (a): [13] and
(b) [14]. Lagos data are averages of several sites taken from [15] except O3 from [16]
Urban Atmospheric Composition Processes 219

Urban Atmospheric Composition Processes, Table 2 (Selected) EU air quality limit values and WHO air quality
guidelines. Values in mg m3
Species EU WHO
NO2 40 (annual mean) 40 (annual mean)
O3 120 (target, <25 times/year) 100 (8 h mean)
SO2 124 (24 h mean, <3 times/year) 20 (24 h mean)
CO 10,000 (running 8 h mean) 10,000 (8 h mean)
Benzene 5 (annual mean) –
1.3-butadiene 2.25 (UK, annual mean) –
PM10 40 (annual mean) 20 (annual mean)
PM2.5 25 (2020 target) 10 (annual mean)
EU limits are those in force as of 2010; target values not legally binding. Additional limit values/future reductions also
apply for some pollutants. WHO guidelines from 2005 update [17] except CO (1997 update)

and international air quality standards and targets Key Emission Characteristics
have been established, by national governments,
the European Union (EU), and the World Health Ambient urban air pollutant emissions in most
Organization (WHO). Selected current standards developed regions are primarily associated with
for key urban pollutants are summarized in vehicle traffic – direct exhaust emissions from
Table 2. These species – the gases nitrogen diox- petrol (spark) and diesel (compression) powered
ide NO2, ozone (O3), carbon monoxide (CO), vehicles, and mechanical sources such as brake
sulfur dioxide (SO2), benzene (C6H6), and tyre erosion and road surface material and
1,3-butadiene (C4H6), and polycyclic aromatic dust re-suspension from all vehicles. Fugitive
hydrocarbons (PAH), plus the integrated particu- emissions of fuel vapor from filling station opera-
late matter (PM) measures PM10 and PM2.5 (see tions are a further significant vehicle-related source
below for definitions) are the focus of this chapter. of gaseous organic (hydrocarbon) air pollutants.
An issue in comparing pollution levels is the Other significant sources include emissions from
differing units commonly used – measurements local point sources such as domestic and office
of trace gases for scientific purposes are fre- heating, cooking, and industrial processes, in par-
quently presented in terms of (volume) mixing ticular the use of solvents, paints and lubricants
ratio (vmr), in parts-per-million, billion or trillion which may have a significant vapor pressure, and
(106, 109, and 1012, respectively) while for PM, combustion processes. Large-scale industrial emis-
and for legislative purposes, concentration values sions associated with heavy industry (power gen-
(usually expressed as mg m3) are used. Conver- eration, steel making, etc.) are not major
sion between these is straightforward but is also contributors to general urban air quality issues in
dependent upon the local temperature and pres- most developed nations, as the plants responsible
sure; care is needed as different standard condi- have largely been removed from the city centers,
tions for the conversion are mandated by, for and as readily identifiable point sources in most
example, the EU (20  C) and the WHO (25  C). cases have their direct emissions scrubbed at
While mixing ratio units are commonly preferred source, for example, in the case of sulfur dioxide
for atmospheric chemistry research where gas- from coal-fired power stations. In urban regions
eous species are concerned, as they are invariant within developing nations, which incorporate
to changes in temperature and pressure (i.e., air many of the fastest-growing megacities on the
parcel transport), and preserve the stoichiometry planet, a different picture of emission sources is
of the chemical reactions (i.e., the relationship observed; again vehicle emissions are a major con-
between reactants and products), here mass con- tributor, although the fleet composition differs with
centration units are used for consistency and ease typically older vehicles (i.e., conforming to less
of comparison with air quality standards. stringent, if any, emission regulations), reduced
220 Urban Atmospheric Composition Processes

diesel prevalence and a greater contribution from (notably, South America) has been associated with
small two-stroke (oil burning) powered two increased emissions of aldehydes such as formalde-
wheelers. Domestic heating and cooking, where hyde and acetaldehyde [20] which are toxic, and
this is primarily through wood burning, is a major also potent radical precursors leading to photochem-
contributor to urban atmospheric composition (and ical smog formation (see below). Biofuel (wood and
indeed to overall pollutant exposure, through charcoal) combustion for domestic heating and
indoor effects within the home). cooking is a substantial source of pollutants within
many homes in developing nations, leading to
Characteristics of Motor Vehicle and Domestic indoor air pollutant exposure, and forming a major
Fuel Emissions emission source within urban regions. The relatively
Within internal combustion engine vehicles, emis- low temperatures commonly found lead to substan-
sions of a range of pollutants reflect the composition tial emissions of carbon monoxide, black carbon
of the fuel and oil burnt, and the high-temperature (soot) and a range of trace compounds VOCs, oxy-
decomposition of atmospheric oxygen and nitrogen genated compounds and acids, including toxic sub-
leading to the production of nitrogen oxides. NOx stances such as polycyclic aromatic hydrocarbons
(NO + NO2) at the tailpipe is conventionally (PAHs), particularly within the organic component
assumed be partitioned (on average) into 95% NO of the emitted particulate matter [21].
and 5% NO2, although there is some evidence that
the direct fraction of NO2 may be greater than this,
and increasing across the fleet on average – in Urban Atmospheric Composition
particular, for diesel-engined HGVs (heavy goods Processes
vehicles) [18]. Incomplete combustion leads to the
production of carbon monoxide (CO), a vast range Gas-Phase Composition Processes
of hydrocarbons which may be gases (if they are Gas-phase processes in urban environments are
sufficiently small and volatile) or may condense to dominated by the oxides of nitrogen, (primarily)
form the organic component of exhaust particulates, NO and NO2, emitted directly from the exhausts of
as the exhaust gases cool. The introduction of cata- high-temperature (i.e., internal combustion engine)
lytic converters has greatly reduced emissions of vehicles. Following emission, a number of gas-phase
NO, CO and hydrocarbons (which are converted processes follow. In close proximity (within a few
to N2, CO2 and H2O) for petrol-engined vehicles, meters) to the tailpipe, NO levels may be sufficiently
while diesel oxidation catalysts have reduced CO high before mixing and dilution that the NO-self-
and hydrocarbon emissions from diesel engines. reaction, converting NO into NO2, may occur:
Increasingly stringent emissions regulations, such
as the EURO-1 to EURO-5 EU series of emissions NO þ NO þ O2 ! 2NO2 ð1Þ
standards for various vehicle classes, have substan-
tially reduced emissions per unit activity (at least However the dominant chemistry of NOx in the
within the parameters of the defined driving cycles), urban environment is the interaction between NO,
and (disregarding CO2) the principal emission con- NO2, and ozone. In daylight, these three species
cerns from modern vehicles are NOx and particulate are very closely coupled by the NO + O3 reaction,
matter, for which in both cases diesel engine emis- and the solar decomposition (photolysis) of NO2:
sions tend to be higher emitters. Exhaust PM in
particular is known to incorporate toxic and carci- NO þ O3 ! NO2 þ O2 ð2Þ
nogenic components such as PAH and heavy
metals, and (as new particles are formed through NO2 þ hv ! NO þ O ð3Þ
condensation/nucleation) to contribute substantially
to the population of the smallest particles particu- The O atoms formed through NO2 photolysis
larly associated with adverse health effects [19]. The rapidly and near-exclusively recombine with molec-
introduction of biofuels (ethanol) in some markets ular oxygen (O2) to form ozone (reaction 4), where
Urban Atmospheric Composition Processes 221

M denotes the involvement of a third body, nitrogen ½NO2  k2 ½O3 


¼
or oxygen, which removes some of the excess ½NO j3
energy from the nascent ozone molecule.

O þ O2 þ M ! O3 þ M ð4Þ where k2 is the rate constant for the NO + O3


reaction, and j3 is the (solar radiation intensity-
As these reactions dominate the NO/NO2/O3 dependent) rate of photolysis of NO2. It follows
interconversion, it is possible to define two further that for a given abundance of NOx and O3, in the
quantities, NOx (¼ NO + NO2), and total oxidant Ox absence of other processes, NOx will exist primar-
(¼ NO2 + O3), which, in the absence of further ily as NO2 when light levels are lower (i.e., at
processes, are conserved. NOx and Ox provide useful dawn and dusk), while the NO fraction will max-
metrics for assessing variations in the sum of NO and imize at midday. In practice the values of k2 and j3
NO2, and of NO2 and O3, without need to consider are such that the NO2:NO ratio is typically in the
the partitioning between these species. The reaction range 2–5 during the day – see Fig. 3.
of fresh, vehicle-emitted NO with O3 reduces ozone NOx is removed from the atmospheric system
levels in many urban areas compared with the sur- through chemical conversion to more stable spe-
rounding regions, leading to an urban decrement in cies, which in turn are removed by deposition and
ozone (compare O3 concentrations for the MR and by their uptake or incorporation into aerosol par-
NK sites in Table 1) – discussed further below. ticles. During the day, NO2 reacts with the OH
The timescales of reactions 2 and 3 in the bound- radical, the gaseous oxidant which dominates the
ary layer under sunlit conditions is of the order of removal of many pollutants on a global scale,
1–2 min, while reaction 4 proceeds in milliseconds; forming nitric acid, HNO3. Nitric acid is then
consequently away from direct emission sources lost through dry deposition (i.e., contact with sur-
NO, NO2 and O3 are found in equilibrium defined faces), wet deposition/rainout, and through uptake
by the Leighton Relationship [22]: into aerosol particles (see below).

40
NO2
O3
NO
30 Ox
Volume mixing ratio /ppb

20

10

0
0 12 0 12 0 12 0 12 0
Time of day (local)

Urban Atmospheric Composition Processes, Fig. 3 Diurnal variation in NO, NO2, O3, and Ox over a 4-day period
for Birmingham City Centre. (From Bloss [23])
222 Urban Atmospheric Composition Processes

OH þ NO2 þ M ! HNO3 þ M ð5Þ O3 + sunlight + H2O

The OH radical is formed primarily through


sunlight-driven photolysis processes, so has a
HNO3
very low abundance at night; in the absence of
NO2
sunlight, the NO2 photolysis reaction also ceases,
and a separate chain of reactions dominate NOx: NO2
OH

NO þ O3 ! NO2 þ O2 ð2Þ VOC

NO
NO2 þ O3 ! NO3 þ O2 ð6Þ
CO
RO2 HO2
NO2 þ NO3 þ M , N2 O5 þ M ð7Þ

The nitrate radical, NO3, is rapidly photolysed


NO2
during the day, effectively suppressing reactions 6
and 7. At night however NO and NO2 may be O2
converted into N2O5 on a timescale of hours; NO
N2O5 is then removed from the urban atmosphere
through wet and dry deposition, and uptake into Urban Atmospheric Composition Processes,
aerosol particles (it is also photolysed slowly dur- Fig. 4 Some important steps in the gas-phase oxidation
of volatile organic compounds (VOCs) in the presence of
ing the day). In both cases, following removal NOx. The photolysis of NO2 regenerates NO and leads to
from the gas phase HNO3 and N2O5 contribute net ozone production
to the nitrate (NO3) content of aerosol particles
(see below), and to the acidity of precipitation. NO reaction therefore leads to the conversion of
The combination of reactions 5 and 7 determine a NO to NO2 without the consumption of O3
chemical lifetime for NOx (strictly, time for con- (cf. reaction 2), and the subsequent photolysis of
centrations to fall to 1/e of their initial value) of NO2 and reaction of the O atom formed with
the order of 12–24 h in urban environments. molecular oxygen (reactions 3 and 4) results in
A further major air pollution consequence of ozone formation. While initiation of the process
the interaction of NOx and VOCs in sunlight is the consumes ozone, the cyclical nature of the reac-
photochemical production of ozone, a major sec- tions leads to net ozone production overall.
ondary pollutant. Figure 4, below, summarizes the The timescale of ozone production ranges from
major reaction processes responsible (after hours to days, but is complex to determine directly.
Wayne, [24]). The process is initiated by the pro- In the boundary layer, ozone removal is dominated
duction of an oxidant radical, OH, shown in Fig. 4 by deposition, however as the atmospheric life-
from the photolysis of ozone in the presence of time of ozone is several days to weeks, advection
water vapor (although other indirect sources also (of ozone-rich or ozone-poor air from upwind
occur, e.g., aldehyde photolysis). OH radicals locations) and atmospheric mixing also have a
react with organic compounds (VOCs and CO) substantial influence upon measured ozone levels.
which leads to the formation of organic and hydro Observed ozone pollution episodes vary in extent
peroxy radicals, RO2 and HO2. In the absence of from hours in highly polluted conditions to a few
NO2, these undergo self-reaction to form perox- days, and are closely associated with the pre-
ides (not shown); however in the urban environ- vailing weather conditions. In the case of Western
ment substantial levels of NO are usually present, Europe, ozone pollution events commonly
and the peroxy radicals react with NO, converting correspond to summertime anticyclonic periods
it to NO2, and regenerating the radical species in which air masses have looped over Europe
HO2 and subsequently OH. The peroxy radical– accumulating pollutants. Ozone is chemically
Urban Atmospheric Composition Processes 223

formed along the airmass trajectory at rates of the with VOCs for OH, reduction in NOx leads to a
order of 20–30 ppb per day (daytime chemical reduction in the ozone production rate, by reduc-
production, part of which is offset by night-time ing the rate of the peroxy reaction (or strictly, by
chemistry and deposition [25]). If a typical episode allowing other competing processes, not shown
is characterized by ozone levels of the order of on Fig. 3, to occur – [24]). Two overall regimes for
90 ppb compared with the rural background of ozone production can be identified: VOC-limited,
around 30–40 ppb, several days are clearly where NOx levels are high, and ozone production
required to achieve this level. In more extreme rates will rise or fall with increase/decreases in
conditions, ozone production proceeds more rap- VOC levels respectively, and NOx-limited, where
idly: during the 2003 Western Europe heatwave VOCs are relatively more abundant, NOx levels
event, a photochemical model constrained by in low, and ozone levels rise and fall with increases/
situ observations of long-lived species from decreases in NOx. Reduction of NOx in a VOC-
suburban North-East London determined the limited regime may lead to increased ozone pro-
peak ozone production to be 17 ppb h1, with an duction. Many urban environments correspond to
average production rate during midsummer at VOC-limited conditions (i.e., higher NOx levels);
midday of 7.2 ppb h1 [26]. Observations in Mex- as air is advected from the urban centre to sur-
ico City have led to calculated ozone production rounding rural regions, with reduced emission
rates of up to 50 ppb h1 [27] during stagnant sources, NOx levels fall and the ozone production
meteorological conditions. regime undergoes a transition to a NOx-limited
Exposure to ozone has substantial human state. The complex dependence of the ozone pro-
health consequences, being associated with irrita- duction rate upon the abundance of primary pol-
tion to eyes and nose, inflammatory reactions and lutants between urban and rural areas, which is
reduced lung function. Ozone is also harmful to compounded by the reduction in ozone levels on
vegetation and ecosystems, and certain materials the street canyon scale within urban areas by the
(erosion of polymers through reaction with com- titration of O3 to NO2 by fresh vehicle NO emis-
ponent double bonds), and is an important green- sions, presents a major challenge to the develop-
house gas in its own right; consequently reduction ment of effective policy for mitigation of ozone
in ozone levels is a major goal of air quality pollution – see below.
policy. The long lifetime of ozone limits the Different organic compounds have differing
impact that local/national air quality legislation potentials for ozone production (reflecting their
can have upon boundary layer ozone levels, and chemical identity/size, and the rates of their reac-
dictates that ozone is treated as a transboundary tions with oxidants such as OH), and of course are
pollutant. emitted in varying quantities. Metrics to rank spe-
The secondary nature of ozone further compli- cies in terms of their contribution to ozone levels
cates attempts to reduce its abundance: The pre- (such as Photochemical Ozone Creation Potentials,
cursor species, NOx and VOCs, must be POCP values) have been developed to account for
controlled; however the response of the chemical the integrated effect of these factors; in the case of
ozone production rate to the level of, for example, the UK, the highest POCP values are assigned to
NOx and CO is not straightforward: As can be tri-methylbenzene, however considering the mass-
seen from inspection of Fig. 3, at high NOx levels, weighted emissions, the largest contributors to the
the reaction of OH with NO2, forming HNO3, can ozone levels experienced are toluene and n-butane
compete with the reaction of OH with VOCs. In [28]. These values are specific to the UK case, that
this instance, reducing NOx levels (e.g., through is, to the emissions, and in particular NOx levels,
emission controls) would have the effect of typically experienced by an air parcel advected
increasing the abundance of OH, and the rate of from continental Europe to southern Britain.
the OH+VOC reactions, and hence would lead to Peroxy acetyl nitrate (PAN, CH3C(O)OONO2)
an increase in ozone production. At lower NOx is the simplest example of a range of acetyl nitrate
levels, where NO2 is not competing effectively compounds, secondary pollutants which are the
224 Urban Atmospheric Composition Processes

principal lachrymator (tear inducing) component Levels of particulate matter or aerosol are usu-
of photochemical smog. PAN is formed from the ally expressed as a mass concentration below a
reaction between peroxy acetyl radicals, CH3C certain size; the size ranges commonly selected
(O)OO, and NO2, and in terms of the chemical relating loosely to the extent to which particles
cycling acts as a temporary reservoir for the HOx penetrate the human respiratory system. PM10 and
and NOx radicals involved in ozone production. PM2.5 define the fractions of suspended particu-
A key feature of the equilibrium between PAN late matter with (aerodynamic) diameters below
and its precursor species is the strong temperature 10 and 2.5 mm respectively (the aerodynamic
dependence, with lower temperatures favoring diameter is a concept used to allow for the varying
PAN stability. A scenario which arises then is morphology or shape of particles; a particle with
that PAN is formed in a polluted urban area, an aerodynamic diameter of 1 mm will exhibit the
transported aloft (where temperatures are lower same inertial properties as a sphere with a diame-
and PAN is stable) over long distances, before ter of 1 mm and a density of 1 g cm3 –
airmass descent and warming leads to PAN irrespective of the actual size, shape or density
decomposition and release of the component of the particle). PM10 and PM2.5 correspond
NOx in otherwise unpolluted regions. approximately to size ranges which may be
Sulfur dioxide (SO2) is possibly the classic air inhaled into the thoracic cavity (lungs) and into
pollutant formed from the combustion of sulfur- the alveolar regions respectively. The size distri-
containing fuels. SO2 emissions have been suc- bution of urban particles typically exhibits several
cessfully reduced in many regions, through a modes, reflecting the varying dominance of dif-
combination of the use of low sulfur fuels, and ferent processes responsible for particle formation
application of flue gas desulphurization technolo- and growth: The nucleation mode, below approx-
gies on major plants (e.g., power stations). Within imately 0.1 mm in diameter, where secondary
the atmosphere, SO2 is processed to H2SO4 on a particles are formed from the condensation of
timescale of days, both in the gas phase, initiated low-volatility gases (or, more commonly, con-
by reaction with the OH radical, and in the con- denses onto pre-existing particles); the accumula-
densed phase, within water droplets, where the tion mode (0.1–2.5 mm), where particles grow by
oxidation reactions are driven predominantly by condensation and coagulation (collisions), but
hydrogen peroxide, H2O2. Gas phase sulfuric acid within which the mass is too small for gravita-
has a very low vapor pressure, and is readily tional setting to be a major sink (hence the size
incorporated into aerosol and condensation, rais- range where particles accumulate, until removal
ing PM acidity. More widely, co-condensation of primarily by precipitation) and the coarse mode,
H2SO4 with water vapor and/or ammonia leads to which incorporates most mechanically generated
the production of new particles in the atmosphere. particles, and within which gravitation settling
begins to be a significant loss process. As simple
Condensed Phase Composition Processes geometric considerations show, the largest num-
Particulate matter is an important component of ber of particles is found in the nucleation mode,
urban atmospheric composition, in particular while the mass is dominated by the coarse and
where health effects are concerned. Sources of par- accumulation modes. It is perhaps unfortunate
ticulate matter include the local primary emissions then that most current air quality metrics focus
from vehicles and combustion described above, upon particle mass concentration (PM10 or
including mechanical sources related to vehicle PM2.5), while scientific evidence suggests that
brake pad/disc, tyre and road surface wear, wider many human health impacts are related to expo-
atmospheric inputs such as wind-blown dust and sure to the fine-mode particles which can pene-
crustal material, and secondary contributions arising trate most deeply into the alveolar structure.
from the condensation of low-volatility gases to Measurements of the composition of urban par-
form new or (predominantly) contribute to the ticulate matter are less common than total mass
growth of existing particles. concentration, but a number of composition
Urban Atmospheric Composition Processes 225

measurements are now performed routinely at a VOCs (e.g., benzene, toluene), which in turn are
small number of sites in various countries. Within sourced primarily from vehicle emissions. As in
the sphere of such semi-routine monitoring, the the case of ozone, the substantial secondary com-
(mass) contributions from sulfate, nitrate, ammo- ponent of urban particulate matter complicates air
nium, chloride and other elemental components quality management and control. A component of
may be determined, alongside the elemental and particulate matter worth of further consideration is
organic carbon fractions. Figure 5, below, shows polycyclic aromatic hydrocarbons (PAH). Formed
the composition of PM2.5 and PM10 in Birming- from two or more aromatic rings fused together,
ham city centre. Components which are apparent and produced from the incomplete combustion of
include iron and calcium components from crustal coil, oil, petrol and wood, in particular domestic
erosion, salt (sea-salt derived, possibly with some fuel usage, PAH are persistent bio-accumulative
contribution from winter road salting), elemental organic compounds; human exposure leads to a
carbon (essentially soot, from incomplete combus- range of toxic and carcinogenic effects. One spe-
tion; in these measurements, likely to arise almost cific PAH, benzo-a-pyrene, is commonly used as a
entirely from diesel vehicles), organic compounds, marker for the abundance of this family of com-
ammonium bisulphate, ammonium nitrate and pounds; the EU has established a target concen-
sodium nitrate. Of these, the ammonium, sulfate tration of 1 ng m3 for B[a]P by end of 2010,
and nitrate components are likely to be largely which may be compared with current (UK) levels
secondary, arising from agricultural emissions, of 0.16 ng m3 (mean across all sites for 2006).
combustion of sulfur-containing fuels and the
atmospheric processing of NOx respectively (see
above), while within the organic (carbon) fraction
Trends in Urban Atmospheric
comprises elemental carbon (soot, likely primarily
Composition
from diesel vehicles) and a substantial contribution
from organic compounds.
This section concerns trends in the key urban
Research-focused field measurements can dis-
atmospheric components over the forthcoming
aggregate the organic fraction in more detail, and
few decades. The trends observed reflect the inte-
typically find that this is primarily secondary in
gration of a number of independent effects: back-
origin (up to 64% in urban regions [30]), arising
ground levels of atmospheric components on a
(in urban environments) largely from aromatic
regional and global basis; changes in emissions

Other Iron-rich
3.7% Other Dusts Calcium
Iron-rich Dusts 5.9% Salts
13.4% 5.2%
2.5% NaCl
NH4NO3
/NaNO3 4.0%
NH4NO3
18.5% Calcium Salts /NaNO3
7.4% 21.2% EC
11.2%
PM10-Overall
(BCCS) PM2.5-Overall
NaCl (BCCS)
9.3%

(NH4)2SO4
16.0%
EC
8.0%
(NH4)2SO4 Organics
24.0% 26.1%
Organics
23.7%

Urban Atmospheric Composition Processes, Fig. 5 Chemical composition of particulate matter (PM10 and PM2.5)
from Birmingham City Centre. (Data from Yin and Harrison [29])
226 Urban Atmospheric Composition Processes

of primary pollutants per unit activity (i.e., from [31]. The equivalent values for the past decade
improvements in vehicle technology and penetra- from background locations are much higher – for
tion of exhaust treatments such as catalytic con- example, ca. 80 mg m3 for background air at
verters through the vehicle fleet); and changes in Mace Head, Ireland (value for 2006 from Derwent
the overall activity level, that is, increasing eco- et al. [32]); background levels have increased over
nomic prosperity and population levels, particu- the past 2–3 decades at up to 10 mg m3 per
larly in many megacities in developing nations. decade (5 ppb per decade) [33]. On top of this
A further external driver which may affect future hemispheric trend, urban ozone levels respond to
urban composition is the interaction between regional pollution events, and to the extent of
atmospheric composition processes and global local titration of O3 to NO2 through NOx
climate. (strictly, NO) emissions. Emissions controls have
For the gaseous pollutants, the species of par- reduced the prevalence and extent of ozone epi-
ticular concern on an ongoing basis are nitrogen sodes over the past 1–2 decades, reducing this
oxides (specifically NO2 as this is the NOx com- contributor to urban ozone; however reductions
ponent against which legislation is commonly in NOx emissions have offset some of this change,
framed) and ozone. Of the other regulated pollut- reducing the ozone urban decrement. These
ants (Table 2), sulfur dioxide levels are falling as effects are clearly seen in the UK over the period
the intensive sources (power and heavy industry) 1990–2006 (e.g., AQEG [34]), where the maxi-
have emissions controlled at source and carbon mum hourly mean values (associated with
monoxide levels have greatly reduced with the regional ozone pollution episodes) have
advent of catalytic converters. decreased substantially due to European controls
Urban NOx levels show a downward trend in on emissions of VOCs and NOx, while at inter-
most developed cities when viewed on a 2–3 mediate percentiles, urban sites show a positive
decade timescale, driven by improved emission trend in ozone with time due to the reduced urban
control technologies in the vehicle fleet; for exam- decrement. The lowest hourly mean ozone levels
ple, across a range of UK urban sites, annual mean show no change as these essentially correspond to
NOx levels have fallen by 40% over the period total titration of O3 to NO, consequently ozone
1993–2005, from 135 to 80 mg m3 [18]. Within levels are zero across the time period considered.
this overall trend, there are some significant local Primary sources (vehicle exhaust) of PM have
variations, for example, data from London sug- been substantially reduced in may developed
gests that the fraction of NOx emitted as NO2 has nations, and PM levels (measured as PM10) have
risen in recent years, possibly due to the introduc- fallen substantially over the past few decades.
tion of diesel particulate filters, while traffic con- Recently however, the downward trend appears
trol measures such as the London Congestion to have been arrested, at least for PM10 in Europe,
Zone have altered the average fleet composition and the sulfate and nitrate components of this
in central London to favor diesel vehicles with PM10 [35]. It is unclear if this is a temporary
increased NOx emissions, thought to be responsi- departure from the general trend or reflects an
ble for the 7% increase in NO2 observed in central ongoing leveling off, possibly reflecting non-
London over the period 2003–2008. More widely exhaust sources, changing meteorology, and the
however, NOx levels in most developed cities interaction between sulfate and nitrate via ammo-
have fallen dramatically over the past 2–3 nia availability to form ammonium nitrate.
decades [18].
Globally, background ozone levels have risen
over the past century – the earliest instrumental Future Directions
data thought to be reliable, the Montsouris mea-
surements recorded on the outskirts of Paris from In many developing megacities, the outcome of
1876, indicate average background ozone levels the opposing effects of increasing population den-
of 22 mg m3 over the period 1876–1910 sity and economic activity, and adoption of
Urban Atmospheric Composition Processes 227

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doi.org/10.1029/2007GL029979
Surface runoff The water which runs off the
Urban Drainage Modelling for surface and does not drain into the ground is
Management of Urban termed surface runoff
Surface Water

Birgitte Lilholt Sørensen


Institute of Chemical Engineering, Biotechnology Definition of the Subject
and Environmental Technology, SDU Life Cycle
Engineering, University of Southern Denmark, Management of urban surface water frames the
Odense M, Denmark challenge of managing surface water in different
contexts for the benefit of people and the environ-
ment. Water is part of the global circle of life
Article Outline (hydrological cycle) and is imperative for sur-
vival. However, excess water in developed areas
Glossary presents a challenge to people and the environ-
Definition of the Subject ment. Managing water resources requires an
Introduction understanding of the hydrological cycle and its
Development of Challenges in Urban Surface fluctuations [1]. The knowledge of the water
Water cycle base on how the water moves through the
Designing Sewer Systems soil, underground, or via stream, river, sea and air.
Modelling Flow on the Surface Water originating from rain, streams, snow-
Modelling of Water Transport in the Sewer melt, ground, sea, etc. and flowing into areas of
System human activity requires sensible management to
Future Directions the extent possible and should not result in dam-
References age to people, infrastructure, animals, and envi-
ronment. For example, it may be the aim to design
Glossary sewer systems to contain surface water generated
during severe rain events or dikes constructed for
Catchment The area where all the rainwater nat- protecting people, environment, and infrastruc-
urally drains toward the same point (outlet) ture from rising sea level. Water management,
Drainage Surface water coming from rain either when applied to the benefit of humans and nature,
drains (percolates) into the (permeable) ground is an exciting challenge for urban surface water
or runs off to the location in the area with the management. Water, when appropriately man-
lowest point of elevation. The water which does aged, can create areas of high value along its
not drain requires transporting away from the shores and add to recreation and biodiversity.
catchment premises. The task of designing Urban drainage modelling is one approach to
sewer systems for that purpose is called drainage analyzing the water transport and flow of surface
Percent imperviousness The average percent of water from severe rain events, snowmelt, rising
an area considered impervious for drainage of sea level, etc. Urban drainage modelling allows
rain assessing and thereby helping determine the best
Sewage Wastewater from households or industry approach to managing the water flow for the ben-
transported in sewer pipes efit of people and the environment [2].

© Springer Science+Business Media, LLC, part of Springer Nature 2021 229


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_1075
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2019, https://doi.org/10.1007/978-1-4939-2493-6_1075-1
230 Urban Drainage Modelling for Management of Urban Surface Water

Introduction more and more significant rain events as well as


more severe rain events [5], while others suffer
The United Nations Sustainable Development from more intense and more prolonged droughts.
Goals [3] (SDG) aim to provide a framework for In urban areas such as in Denmark, which
the challenges that need collaborative and joint follows European Union Water Management
focus from governments, the private sector, civil guidelines and directives, rainwater is led out of
society, and people. These challenges include the city through sewer systems into local rivers or
some important global environmental factors. streams, often passing through a wastewater treat-
One of the challenges mentioned is to take ment plant. In Europe, though there was signifi-
urgent action to combat climate change and its cant post-World War II modernization, there
impacts, partly because of emissions of carbon remain substantial portions of the sewer system
dioxide (CO2) and other greenhouse gases in urban areas established in the eighteenth and
resulting from the use of fossil fuels [4]. Climate nineteenth century [6]. The networks have since
change is related to urban water management expanded and many of them renovated to accom-
since a changing climate impacts weather, with modate urban growth. The primary purpose of the
the intensity of rain events, rising sea levels, i.e., sewer system has been and is today to store and
in many areas and others, perhaps the opposite transport wastewater as well as runoff from
effects occur. The challenge is not only urban as rainwater.
water management affects land-use management. Designing a sewer system to be able to handle
The problem of managing the impacts of severe the water which runs off and does not percolate
amounts of water is, therefore, becoming more into the ground during rain is a challenge by itself.
complex. There is a need to be able to assess Engineers have been managing the problem by
systems of systems across a catchment. developing methodologies for dimensioning and
This entry introduces the main concepts used designing sewer systems to drain the surface dur-
in modelling urban surface water runoff and, as an ing rain and ensure that they understand and build
example, presents a model of the Amager district into codes the effects of not only subsurface sys-
of Copenhagen, Denmark. It is intended as an tems but also surface (asphalt) and supra surface
introduction for those interested in urban drainage (roof) drainage systems.
modelling. The approach used in the example An example of how engineering societies take
presented for inspiration aims to illustrate the responsibility for the development of the design
opportunities in urban drainage modelling and is, approach is the Engineering Society in Denmark
in principle, independent of location. [7]. They have since 1949 published general
There are several inherent difficulties in man- guidelines and advice to the engineering commu-
aging the overall challenge of a severe rain event. nity [7] as do many other authorities or experts in
Water engineers and hydrologists have developed other jurisdictions around the world [8]. When it
advanced modelling tools for analysis given the is found relevant, they update or publish new
increased complexity of observed phenomena. guidelines – generally based on advances in
research or observational evidence demonstrating
the need for design updates.
Development of Challenges in Urban When rain events become more (or much less)
Surface Water severe, the capacity and the design of the sewer
systems do not match the future needs as the flow
The effects of the changing weather on the envi- conditions of the systems change. In the case of
ronment, infrastructure, and people vary with the more intense water flow, the direct approach may
weather and climate ranging from droughts to be to aim for expanding the network to accommo-
elevated water levels in rivers and rising sea levels date higher capacity. However, expanding net-
from increased freshwater runoff. In many places works by increasing the size is expensive and
around the world, the change in weather results in thus often not an option. Therefore, both the
Urban Drainage Modelling for Management of Urban Surface Water 231

amount of water in severe rain events and the Modelling Surface Runoff
intensity of the flow call for changing the The approach on designing of sewer systems for
approach to water management and sewer reno- effective and efficient surface water management
vation and design. requires advanced tools for analysis. Develop-
ments of advanced computer models for analyzing
water transport and flow on surfaces as well as in
the sewers have been very relevant. MIKE
Designing Sewer Systems URBAN is such a tool [11]. MIKE URBAN can
model an urban drainage system (urban drainage
Rain modelling) as well as water transport on the surface
As a basis for modelling, it is essential to have data of a city. The model is an advanced model using
on how much rainwater or other (waste) water comprehensive dynamic hydraulic modelling [12].
needs handling. There are different approaches to Primary data for a model is information on
collect or obtain relevant information on rainwater. catchment areas size, slope, shape, and impervi-
In Denmark, rainfall is registered via rain gauges in ousness shape. The model uses the data as char-
a national grid since the 1970s [9]. Rain gauges acteristic values or input information for the
measure the rain event volume, intensity, and dura- modelling of water flows from ground to sewer
tion of the rain at any given location. Long-term system. The data are necessary parameterizations
monitoring of rain events by measuring the dura- to the dynamic modelling of water flow.
tion, intensity, and volume has generated a histor- The development in urban areas has been
ical knowledge base of so-called rain events. toward restricting percolation of surface water
The amount of rain expected to precipitate and into the ground and thus increases flow over the
drain to the sewer system needs to be known. It ground. The decreased imperviousness of the sur-
also needs to be assessed whether the runoff from face cover is due to extended coverage of urban
the rain will be handled through a separate net- terrain. The decreasing imperviousness poten-
work or together with wastewater. Determining tially results in urban areas becoming more vul-
the amount of rainfall is generally via utilizing nerable to flooding from severe rain both due to
historical rain event data collected from local the change in weather and changes in impervious-
rain gauges or climates/geographies that closely ness and percentage non-percolating surface area.
match the catchment. Data on the frequency of For effective modelling, it is therefore essential
intensity and volume of the rain is the basis for for urban surface water management to be able to
choosing relevant rain events for input data for the estimate and map impervious surfaces in catch-
modelling [10]. ments efficiently. Data on impervious surfaces
Recent developments on measuring frequency and by association, runoff, is an indicator. The
and intensity of rain use information from radar data on imperviousness is an essential input factor
[2]. Radar measurements make it possible to mea- in hydrological models and urban drainage
sure the movement and extent of the rainfall over modelling. To obtain imperviousness data for
an area and thus provide more information than a urban drainage modelling, a comprehensive col-
rainfall measurement in a single point. When lection of information and data, as well as charac-
modelling the impact of the rainfall in a specific terization of the examined urban area, must be
area, the understanding of the movement across done. Traditionally, data from digital or other
the area may be of significance since this might maps are the basis for the calculation.
increase the effect of the rainfall on the water Conventional mapping techniques in complex
runoff systems. The usage of this type of data urban areas are often expensive and time-
enhances the ability to forecast certain events consuming, particularly when the area in question
and their impact and thus the ability of water is large. Therefore, the development of more auto-
managers and engineers to best manage and con- mated analysis and classification based on, e.g.,
trol flow into the sewer system [2]. aerial photos or satellite images, i.e., remote
232 Urban Drainage Modelling for Management of Urban Surface Water

sensing (RS), has been the subject of engineering minimum spatial resolution of 0.25–0.5 m [13,
efforts. This approach offers an alternative for 14]. For lower spatial resolutions, GIS data can
mapping urban areas, which not saves time and be integrated with satellite or airborne images to
reduces costs but also reduces the dependency on minimize misclassifications and improve
manual visual interpretation. accuracy [15].
The use of RS for classification and thereby Many different image classification methods
calculation of the percent imperviousness based can be used to automatically categorize the pixels
on same started at the beginning of the twenty-first of the RS images into land use types [16]. The
century [13], and the technology has steadily approach used to classify an urban land cover
advanced since with the development of new depends on the nature of the analyzed data, the
sensors. available computational resources, and the
The RS of urban impervious surfaces demands intended application of the data classified [17].
a high spatial and multispectral resolution to be Figure 1 shows the result of transforming infor-
able to discern features in such complex environ- mation from airborne imaging to digital maps on
ments [13]. The minimum spatial resolution the imperviousness of an area. As an example,
required for urban environments is half the diam- [18] use the airborne images of the area Amager
eter of the smallest object of interest [13, Øst, an Island East of Copenhagen, Denmark,
14]. Impervious features such as buildings utilizing remote sensing for classification of the
(perimeter, area, height, and property line) and different types of surfaces in the area. It classifies
roads (width) are generally detectable with a the areas of impervious area types such as roads,

Urban Drainage Modelling for Management of Urban Surface Water, Fig. 1 Result of transforming a digital
image to a classified map which then can be used for calculating percent imperviousness of a catchment
Urban Drainage Modelling for Management of Urban Surface Water 233

buildings/roofs, and impervious surface feature thereby generate runoff. Vegetation is considered
types such as grass, trees (vegetation), etc. and not to generate any runoff. From observations and
finally a surface type named other which can assumptions based on these, a simple calculation
correspond to different types of pavement. Build- is made to calculate an average percent impervi-
ings and roads are considered impervious and do ousness (PIMP) for a sub-catchment.

PIMP ¼ ðroad_area  100% þ building_area  100% þ vegetation_area  0%other_area  0%Þ


=total area of sub  catchement
(1)

In the study [18] the strengths and weaknesses Figure 2 is a visual comparison of the differ-
of using a remote sensing technique to calculate ences in the classification between the mapping
the percent imperviousness are investigated. approach and the RS approach.

Urban Drainage Modelling for Management of traditional GIS map (left), and finally the results of remote
Urban Surface Water, Fig. 2 Three different visual pre- sensing (RS) (right). The GIS map and RS results are used
sentations of the classification data. Firstly, a photo, then a for imperrviousness classification
234 Urban Drainage Modelling for Management of Urban Surface Water

Figure 3 shows a closeup of the result of the not only depends on the rain data and percent
classification from the RS technique compared to imperviousness. It also depends on the way the
using a traditional map as the basis of classification model represents the area. Figure 4 shows an
(electronic GIS map). The classification of trees and example of the different approaches for
garden areas is different, resulting in different esti- representing the area used for modelling. It
mated PIMP. Vazquez et al. [18] shows that the shows the urban area of Amager Øst (East) in
estiamtion of per cent imperviousness can be done Copenhagen, Denmark, was used as the analysis
based on remote sensing though this may be refined location [18]. It shows three different versions of
and adjusted manually before the classification. Sec- the MIKE URBAN model and the description of
ondly, [18] also found the classification of sandy the catchment areas. MOUSE layout is an older
areas to be difficult unless manual input of soil types model type where the areas are all considered
aligned with their imperviousness was known. squared. The GIS layout is based on a geograph-
These resulted in artifacts, classifying sandy areas ical map and the shapes accordingly. The
as impervious as asphalt-paved areas. Thiessen polygon layout version the form of the
area is based on Thiessen polygons.
The study [18] uses MIKE URBAN software
Modelling Flow on the Surface to model and compare the results on percent
imperviousness and the final modelling of surface
Firstly calculation for PIMP then follows model- runoff using a traditional approach and RS. The
ling of surface runoff. Modelling of surface runoff MIKE URBAN modelling software [11] can

Urban Drainage Modelling for Management of Urban Surface Water, Fig. 3 Visual presentation of the difference
in classification using GIS map or RS

Urban Drainage Modelling for Management of Urban Surface Water, Fig. 4 Catchment layouts for modelling,
GIS catchment layout, MOUSE catchment layout, and Thiessen polygons catchment layout
Urban Drainage Modelling for Management of Urban Surface Water 235

model runoff from numerous sub-catchments with remote sensing as [18] demonstrated was possible.
individual percent imperviousness and sewage The technique may be an option for a simpler and
transport in a sewage network. This software can faster approach to setting up a model for the anal-
simulate flow from catchments to the sewer based ysis of water transport and drainage in, e.g., urban
on their actual spatial geometry and the areas. However, more case studies are needed and
corresponding hydrological parameters. an understanding as to when it is economical to use
According to [18] the volumes and peaks of such technology for efficient classification and cal-
runoff are comparable to the ones using the tradi- culation of percent imperviousness and other run-
tional approach. The specific result from surface off and surface data characteristics.
runoff modelling is the primary input data for
modelling sewer flow and overflow. Therefore
the method described is promising and useful
References
already. However, even though the first trial
using remote sensing technique results in similar 1. Ferrier RC, Jenkins A (2010) The catchment manage-
peak flow and runoff volume, some refinements ment concept. In: Ferrier RC, Jenkins A (eds) Hand-
are desirable [18]. The classifications based on the book of catchment management, vol 1. Blackwell,
remote sensing technique can and should be Oxford
2. Thorndahl S et al (2017) Weather radar rainfall data in
adjusted, e.g., to adjust for shadowing from trees urban hydrology. Hydrol Earth Syst Sci 21:1359–1380
and more precise classification of some specific 3. United Nations, SDG (2015) Sustainable development
soils, e.g., sandy areas [18]. goals, 17 goals to transform our world. [Online].
https://www.un.org/sustainabledevelopment/sustaina
ble-development-goals/
4. United Nations, Goal 13 (2015) Take urgent action to
Modelling of Water Transport in the combat climate change and its impacts. [Online].
Sewer System https://www.un.org/sustainabledevelopment/climate-
change-2/
5. Intergovernmental Panel on Climate Change
The last step in the modelling approach is the (2014) Climate change 2014 synthesis report summary
transport of water into the sewer system. At this for policymakers
point in the process of modelling, any significant 6. Garnier J et al (2013) Modeling historical changes in
differences in the modelling approaches in [18] nutrient delivery and water quality of the Zenne River
(1790s–2010): the role of land use, waterscape and
should not be apparent. The uncertainties urban wastewater management. J Mar Syst 128:62–76
connected to using airborne images as input for 7. Spildevandskomiteen (2018) Skrifter. [Online].
analyzing overflow and sewage transport are sim- https://universe.ida.dk/spildevandskomiteen/skrifter/
ilar to using the traditional approach, as observed 8. American, Society of Civil Engineers (ASCE)
(2013) Standard guidelines for the design, installation,
in the specific case of the comparison made at and operation and maintenance of urban subsurface
Amager Øst. drainage. American Society of Civil Engineers, Pro-
Quest Ebook Central, Reston. https://ebookcentral.pro
quest.com/lib/sdub/detail.action?docID=3115658
9. Spildevandskomiteen. Spildevandskomiteens
Future Directions regnmålersystem. SVK bestilling . [Online] Danmarks
Meteorologiske Institut. http://svk.dmi.dk/
The example of the modelling tools and remote 10. Spildevandskomiteen (2014) Skrift nr. 30. Opdaterede
sensing technique mentioned in this chapter for klimafaktorer og dimensionsgivende regnintensiteter.
[Online]. [Cited: 05 07 2018.] https://ida.dk/sites/
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MIKE_Urban.htm gressing from object-based to object-oriented image
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Part II
Regional and Global Air Quality and
Effects
precursors through a phase transition, without
Aerosol in Global Atmosphere need of a particle nucleus.
Hygroscopicity The ability to absorb water from
Colin O’Dowd the atmosphere.
School of Physics and Centre for Climate and Air Radiative forcing The radiative forcing of the
Pollution Studies, Ryan Institute, National surface-troposphere system due to the pertur-
University of Ireland Galway, Galway, Ireland bation in or the introduction of an agent (say, a
change in greenhouse gas concentration) is
defined as the change in net (down minus up)
Article Outline irradiance (solar plus longwave in Wm2) at
the tropopause.
Glossary
Definition of the Subject
Introduction: The Nature and Impacts of Definition of the Subject
Atmospheric Aerosols
Aerosol Formation, Dimensions, and Removal Atmospheric aerosols are airborne liquid or solid
Global Aerosol Budgets, Burdens, and Spatial particles, varying in size from nanometers to hun-
Distributions dreds of microns. Atmospheric aerosols are formed
Water Uptake by Aerosols from both natural and anthropogenic sources and
Aerosols, Global Radiative Budget, Precipitation, can have complex chemical speciation and shape.
and Climate They are formed from mechanical breakup of a
Aerosols and Air Pollution parent material, such as dust or sea spray
Future Directions: Interactions Between Aerosol (so-called primary aerosol formation), or from
Air Pollution and Climate gas-to-particle conversion processes, such as con-
Bibliography densation of semivolatile organic compounds
(VOCS) or chemical reactions in the aerosol
Glossary phase such as oxidation of SO2 to SO4 (so-called
secondary aerosol formation). These tiny airborne
Aerosol optical depth Quantitative measure of particles can form haze and cloud layers that influ-
the extinction of solar radiation by aerosol ence the Earth’s climate: aerosols directly reflect
scattering and absorption between the point of incoming solar radiation back out to space, provid-
observation and the top of the atmosphere. ing a direct radiative effect on climate, some of
Aerosol A suspension of liquid or solid particles which act as cloud condensation nuclei in the
in a fluid (in this context air). Also referred to cloud formation process where they determine
as particulate matter (PM). cloud microphysical and radiative properties, ulti-
Climate Mean values of meteorological param- mately determining cloud reflectance providing an
eters in a given region over relatively long indirect radiative effect. The net climatic impact of
periods of time. atmospheric aerosols is to provide a cooling effect
Cloud droplet activation Spontaneous conden- that partially offsets greenhouse gas-induced
sation growth of a wettable aerosol particle into global warming. Aerosols also contribute to poor
a cloud droplet. air quality and adverse health effects, typically
Homogeneous nucleation Spontaneous forma- resulting in reduced life span and increased mor-
tion of an aerosol particle from vapor phase tality rates in the most polluted environments.

© Springer Science+Business Media, LLC 2012 239


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_322
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_322
240 Aerosol in Global Atmosphere

Introduction: The Nature and Impacts of aerosol haze and cloud layers play an important
Atmospheric Aerosols role in the global radiative budget through con-
tributing to 50% or more of the Earth’s albedo.
Atmospheric aerosols are tiny airborne liquid or The significant contribution to global albedo
solid droplets or particles, ranging from nanome- necessitates an important role in climate, and in
ters to tens or even hundreds of microns in size. terms of a changing global aerosol population, a
They are diverse in shape and chemical composi- role in climate change also exists. Aerosols are
tion and can posses varying optical properties and both natural and anthropogenic, the former pro-
hygroscopic (water uptake) properties. Particle duced by the biosphere (sulfate and organics) and
shape ranges from the most simple to characterize, wind interaction at the Earth’s surface (sea spray
that is, spherical, to complex fractal agglomerates and dust production), the latter produced by
with similar diversity in aerosol density. Chemical industrial, transport, and combustion emissions
composition ranges from relatively simple inor- (sulfate, nitrate, soot, and organics). Biosphere
ganic composition to very complex organic matter emissions are connected to climate change feed-
composition and mixtures thereof. The vast backs and virtually impossible to control while
majority of organic chemical species have not, to anthropogenic emissions can be controlled to a
date, even been identified. The aerosol population certain extent. Although some aerosol species
is a dynamic physical and chemical evolving sys- absorb solar radiation, partially contributing to
tem with fresh aerosol plumes often being exter- global warming, the predominant climate effect
nally mixed in terms of chemical composition, is one of net global cooling. Since the start of the
evolving with time into more complex internal industrial era, aerosol-related air pollution has, to
mixtures. Primary aerosol production is the a significant degree, been masking the global
breakup of a parent material or incomplete com- warming impact of greenhouse gases and has
bustion and results in the direct injection of aero- been slowing the rate of global warming. The
sol particles into the atmosphere. Secondary effect on climate can be considered as a welcome
aerosol production is the formation of aerosol impact of atmospheric aerosols; however, micron-
phase products from nucleation, condensation, sized and submicron-sized aerosol also have a
and multiphase chemical reactions resulting in high penetration efficiency through the human
aerosol production in the atmosphere itself as respiratory system leading to increased respira-
opposed to injection into the atmosphere. Aerosol tory and cardiovascular health impacts. The
particles in the size range from 100 nm to 1 mm are adverse health impacts lead to increased mortality
particularly efficient at scattering, and depending rates and reduced life span. For example, the
on the chemical composition, absorption of solar London black smoke pollution events in the
radiation. Sea-salt, sulfate, and nitrate are all effi- 1950s resulted in thousands of excess deaths
cient scatters, while soot or black carbon and dust over periods lasting the order of several days. To
are efficient absorbers. These important optical counteract the adverse health impacts of atmo-
properties lead to a reduction of visibility from spheric aerosols, various clean air acts have been
aerosol haze layers under conditions of high aero- introduced in various continents, particularly
sol concentrations and such haze layers are developed industrial continents. Such legislation,
responsible for a number of atmospheric optical while having the required successful impact on air
phenomena such as beautiful sunsets often seen quality and public health, has had a negative
under clear sky conditions. Aerosol particles also impact on global warming in that the reflective
act as condensation nuclei for cloud droplets to haze and cloud layers have become less reflective
form on. Without condensation nuclei, it would be with the effect of reducing the masking effect on
virtually impossible for clouds to form, therefore global warming. Particularly over the last two to
aerosols also play an important role in the hydro- three decades, cleaner air has resulted in a remark-
logical cycle. Cloud drops are also efficient scat- able increase in the rate of global temperature
ters of solar radiation and consequently, both increase as greenhouse gas concentrations in the
Aerosol in Global Atmosphere 241

atmosphere continue to rise. The coupling condensation of low-volatility gases onto existing
between air pollution, air quality, and climate aerosol, homogeneous nucleation (phase-
change has led to the synergetic development of transition) producing new aerosol particles, aque-
air pollution and climate change policy to achieve ous phase reactions of dissolved gases producing
optimal effect in attempting to mitigate and abate stable aerosol phase species, or chemical reactions
climate change while simultaneously striving for on aerosol surfaces leading to an increase in the
clean air. condensed aerosol mass. In contrast to direct ejec-
The challenge, however, is great in terms of tion of primary aerosols into the atmosphere,
producing accurate assessments of aerosol which necessitates a surface source for primary
impacts, particularly those relating to climate aerosol (excluding aviation emissions), secondary
change because the atmospheric aerosol system aerosols are formed in situ in the atmosphere,
is incredibly complex and this complex system although many of their precursors are likely to
needs to be incorporated into large-scale and originate at the surface. The formation of second-
global climate assessment and prediction models. ary aerosols can occur at all levels in the atmo-
From the emission and formation stage of the sphere, from the boundary layer in the lower
aerosol life cycle, through its evolution, interac- troposphere to above the stratosphere.
tion with clouds and radiation, to its removal from Once formed, an aerosol particle may undergo
the atmosphere is a highly complex non-linear physical and chemical transformation, but gener-
system spanning spatial and temporal scales ally there are only two main sinks – that is through
from nanometers and seconds (in terms of nucle- dry deposition at the surface, or wet deposition
ation of new particles, to global and decadal involving washout by precipitation. Dry deposi-
scales, respectively, in terms of climatic impacts. tion is the transport of aerosol particles from the
The complexity is further compounded by the atmosphere to the surface in the absence of pre-
diverse and even incomplete quantification of cipitation. The level of turbulence in the atmo-
the chemical speciation of atmospheric aerosol sphere, particularly that close to the ground,
particles. This chapter summarizes the nature, for- determines the rate at which particles are depos-
mation, transformation, distribution and impacts ited [1]. The deposition rate depends on surface
of aerosols in the global atmosphere and docu- type (i.e., roughness) and particle size since there
ments the recent advances in the knowledge relat- also is a gravitational settling component to dry
ing to atmospheric aerosols and their impacts. deposition. Combining both wet and dry deposi-
tion removal processes, on average, submicron
particles reside in the boundary layer for up to
Aerosol Formation, Dimensions, and ~4–8 days [2] depending on precipitation, while
Removal supermicron particles, depending on the size,
have lifetimes from an hour to 1–2 days. For
Aerosols are produced via two generic mecha- example, a 100-nm particle takes approximately
nisms: (1) primary aerosol formation and (2) sec- 36 years to fall 1 km whereas a 10-mm particle
ondary aerosol formation. Primary aerosols are takes 3.6 days. Clearly, if particles are vertically
formed from the mechanical breakup of a parent transported to the free troposphere or the strato-
material, with the resultant aerosol inheriting the sphere, their lifetime in the atmosphere is greatly
chemical properties of the parent bulk material. In increased even to timescales of a year or more in
addition, primary aerosol production can result the stratosphere. Removal in the atmospheric
from incomplete combustion processes. These boundary layer is increased due to turbulent
processes result in the direct emission of aerosols effects. In terms of aerosol-related air pollution,
into the atmosphere. Secondary aerosols, on the effects are more so on a local-to-regional scale
other hand, are formed via gas-to-particle conver- rather than on a global scale due to removal time-
sion processes such as oxidation or other means of scales; however, as it will be seen later, in a
chemical reduction of volatile precursor gases, climate context, a small amount of aerosol
242 Aerosol in Global Atmosphere

pollution transported to very remote regions can smaller particles (in the nucleation and Aitken
have a notable impact, despite relatively short modes) and larger (supermicron mode) particles
atmospheric residence timescales. Physical trans- have notably shorter lifetimes than that associated
formations include condensation growth and with accumulation mode particles but for different
coagulation (collisions of two particles resulting reasons. Smaller particles are highly diffusive and
in one larger particle), while chemical transforma- either self-coagulate to form a larger particle, or
tions include changes in chemical composition they coagulate with larger particles (with a high
from chemical reactions (e.g., oxidation), along surface area) where they are effectively removed
with condensation of different vapors to that from the size distribution. Their mass is so small
already in the aerosol phase. These transforma- that gravitational settling is negligible. In contrast,
tions result in the aerosol population becoming larger particles have a negligible diffusion coeffi-
“internally mixed” at long distances from source cient, but significant mass so that gravitational
regions as opposed to “externally mixed” near settling determines their lifetime. Also shown in
source regions. Fig. 1 are scanning electron micrographs of vari-
Primary production results typically in larger- ous aerosol types such as soot (black) carbon,
micron- or supermicron-sized particles, while sec- marine organic, sulfate, and bioaerosol particles.
ondary production results in nanometer- to These images demonstrate the complexity of
submicron-sized particles, leading to size distri- atmospheric aerosols in terms of shape, chemistry,
butions spanning many orders of magnitudes. In and resultant density, and this complexity is prop-
Fig. 1, a typical number size distribution is agated through measurement and modeling chal-
displayed. The peak in the number frequency lenges associated with quantification of aerosol
distribution is in submicron sizes; however, for properties and effects.
the same distribution, the volume or mass distri-
bution is more often than not in supermicron sizes, Primary Aerosol Formation
even though the contribution of supermicron par- In the atmosphere, the most important natural
ticles generally only comprises less than 1% of the primary aerosol types result from the interaction
total number concentration. Similarly, the mass of of wind with terrestrial or oceanic surfaces. For
particles where the peak concentration occurs terrestrial primary aerosols, wind interaction with
contribute less than 1% of the total mass. The agricultural and desert soils lifts loose fragments
peak in aerosol surface area (not shown) usually of the parent material through saltation and sus-
lies between the number concentration and vol- pension processes resulting in airborne dust parti-
ume peaks. The size distribution comprises a cles [4]. These primary dust particles are typically
number of “log-normal” modes reflecting differ- supermicron in size, comprising low number con-
ent formation and transformation processes. At centration, but high surface area and mass con-
the smallest sizes is the nucleation mode where centrations. The most dramatic example of this is
new particles, nanometers in size, are formed from the vertical uplifting of large amounts of desert
nucleation of condensable vapors. As the nucle- dust into aerosol plumes that can extend for thou-
ation mode grows through further condensation, sands of kilometers (Fig. 2). These plumes often
an Aitken mode (called after the Scottish Scientist are transported and deposited into oceanic regions
John Aitken) of a few tens of nanometers is where they can provide an important source of
formed. Through further transformations and nutrients for the marine biota [5].
growth processes, the Aitken mode grows into Wind interaction with terrestrial vegetation can
an accumulation mode of between about 100 and also trigger the release and dispersion of
200 nm. Generally, the coarse or supermicron bioaerosol such as pollen and seeds as well as
mode arises from the direct injection of primary waxlike and leaf-fragment debris. Humic matter,
particles. The accumulation mode is termed so as plant decomposition products, fungi, and
removal processes are least efficient at these sizes microbes are also released from plants. Fungi, in
and particles tend to accumulate there. Both turn, release spores through a variety of ejection
Aerosol in Global Atmosphere 243

Aerosol in Global
Atmosphere, Fig. 1 A Soot Dust
typical aerosol size 100 nm

distribution covering
4 orders of magnitude in
size. Two moments of the
Ammonium Sulfate
size distribution are shown: 1 μm
number and volume. Also
Sulfuric Acid Marine Organic
shown is a variety of
different aerosol types from
scanning electron
microscope images.
(Copyright Springer.
Modified from [3]) Sea Salt
Crystal Bio-Organic

Biomass Smoke

1 μm Pollen
Nucleation Aitken Accumulation Coarse

Number Volume
1 10 100 1000 1000
Particle Diameter, nm

processes [6]. Primary bioaerosols also include water jet which fragments into a few jet droplets,
entire organisms such as bacteria, fungi, and typically 1–10 mm in size, of similar composition
viruses as well as debris [7, 8]. to film drops [11]. Film and jet drops are produced
Over oceanic water surfaces, wind stress at the at wind speeds greater than 3–4 m s1 which is
air–sea interface leads to breaking waves and the observed to be the threshold for the onset of
entrainment of air into the water column, produc- whitecaps. At wind speeds of 8–10 m s1, the
ing whitecaps [9, 10]. Whitecaps are ensembles of wind stress is sufficient to tear off the crests of
bubbles of entrained air rising to the surface where waves and produce spume droplets, typically
they burst due to the pressure differential inside 10–100 mm in size. The flux of sea spray follows
and outside of the bubble. When the bubble film a power-law dependency on wind speed [12]. In
bursts, it breaks up into hundreds of individual biologically active waters, organic matter tends to
seawater drops that rapidly equilibrate to ambient become concentrated at the ocean surface and at
humidity leaving behind sea-salt “film” droplets, the bubble–water interface. This organic matter
0.01–1 mm in size and comprising a concentrated displaces seawater in the bubble film, ultimately
solution of the ionic compounds found in sea-salt displacing the ionic sea-salt in the film and jet
and water. After the film bursts, the cavity drops produced, leading to the enrichment of
remaining collapses through instabilities leading organic matter in sea-spray aerosol [13]. The
to the formation of an upward movement of a enrichment is observed to increase with
244 Aerosol in Global Atmosphere

Atlantic
Ocean
Argentina

100 km
N

Aerosol in Global Atmosphere, Fig. 2 Patagonian dust over the Atlantic Ocean. (Courtesy of NASA-MODIS)

decreasing particle size. The vast bulk of the results in predominantly submicron carbonaceous
organic matter enriched in sea-spray aerosol is aerosols comprising soot carbon and organic
water-insoluble organic matter. The chemical material [16]. In addition to primary emissions,
composition of marine aerosol is shown in Fig. 3 secondary aerosol precursors such as SO2, NOx,
for periods of low and high biological activity and hydrocarbons are also emitted from combus-
over the North Atlantic as illustrated by oceanic tion sources.
chlorophyll-a concentrations. Supermicron sizes
contain predominantly sea-salt, while for submi- Secondary Aerosol Formation via Nucleation
cron sizes, the enrichment of water-insoluble Homogeneous nucleation is the term used for the
organic matter is linked to biological activity in spontaneous formation of an aerosol particle from
the ocean (the water-soluble organic matter in the vapor phase precursors through a phase transition.
figure is also thought to be marine biogenic in Homogeneous-homomolecular nucleation is the
origin but formed from secondary processes). self-nucleation of a single species, while
In terms of anthropogenic sources of primary homogeneous-heteromolecular nucleation is the
aerosol, incomplete combustion (mainly from fos- self-nucleation of two or more species. Homoge-
sil fuel, but also from biomass burning and neous nucleation occurs in a supersaturated vapor
cooking) results in pyrogenic aerosols in the phase where the saturation ratio (S) of a species in
form of primary organic matter and soot (black) air is the ratio of the species’ partial pressure to the
carbon particles. Fossil fuel emissions result from saturation vapor pressure in equilibrium with its
industrial, power plant, transport, and residential liquid phase at a given temperature. The Classical
heating sources and the resulting aerosol chemical Theory of nucleation is based on rate equations
composition varies according to the fuel type and relating to the random formation of vapor clusters
the combustion technology used [14, 15]. Coal of more than one vapor molecule and the evapo-
combustion results in the emission of supermicron ration of these clusters [1]. The majority of these
fly-ash particles, while petroleum combustion clusters evaporate as quickly as they form since
Aerosol in Global Atmosphere 245

Sea salt NH4 nss SO4 NO3 WSOC WIOC BC


a c 100 10
90 9
80 8
70 7
60 6

Not detectable
50 5
Mace Head
40 4
30 3

Mass fraction (%)


20 2

Mass (μg m–3)


10 1
b d 100 10
90 9
80 8
70 7
60 6
50 5
40 4
30 3
20 2
Chlorophyll concentration (mg m−3) 10 1
0 0
0.01 0.03 0.1 0.3 1 3 10 30 60 0.06 0.125 0.25 0.5 1 2 4 8
D (μm)

Aerosol in Global Atmosphere, Fig. 3 Left: Organic the Arctic and northwest Atlantic. Right: Chemical com-
matter in sea-surface waters. SeaWiFS-derived seasonal position of marine aerosols. Shown are average size-
average sea-surface chlorophyll-a concentrations in winter segregated chemical compositions and absolute mass con-
(a) and spring (b), illustrating low biological activity in centrations for North Atlantic marine aerosols sampled
North Atlantic waters during low and high biologically with a Berner Impactor, for low biologically active periods
active periods. (Courtesy of SeaWiFS Project, NASA/ (c) and high biologically active periods (d). The concen-
Goddard Space Flight Center and ORBIMAGE). The loca- trations of water-soluble organic carbon, water-insoluble
tion of Mace Head is shown in (a). Marine air masses arrive organic carbon, and black carbon are reported as mass of
at Mace Head after at least 96 h transit over the ocean from organic matter. (Reprinted from [13])

they are generally thermodynamically unstable. If higher vapor pressure is required to maintain equi-
a sufficient number of the right low-vapor pres- librium for a smaller droplet (i.e., higher curvature
sure molecules collide, the cluster can achieve a effect). The change in Gibb’s free energy DG
critical radius and achieve thermodynamic equi- associated with the formation of a single drop of
librium (i.e., where the evaporation rate is zero). a pure substance or radius Rp is given by:
The nucleation rate is the net number of clusters
per unit time that will grow past the critical size. DG ¼ DGdroplet  DGpure vapor
In addition to the kinetic aspect of forming
clusters, the thermodynamics of the phase change which after expanding and rearranging, the right-
has to be considered. In a thermodynamic process, hand side terms become:
such as a phase change resulting in chemical
potential equilibrium of the molecular compo- 4 kT
DG ¼  pR3p ln S þ 4pR2p s
nents, the change in the Gibbs free energy (G) 3 vl
must be zero or negative. This condition must
also hold for a curved surface of an aerosol parti- The second term on the right-hand side is the
cle or droplet. The curved surface will affect the free energy associated with an interface with
equilibrium vapor pressure in a manner that a radius of curvature Rp, vl is the volume occupied
246 Aerosol in Global Atmosphere

Aerosol in Global

DG
Atmosphere,
Fig. 4 Gibbs free energy S<1
change for formation of a
droplet of radius Rp from a ΔG = − 4 pRp3 kT
vl In S + 4pRp s
2
3
vapor with saturation ratio S
>0 >0

DG*

S>1
0 ΔG = − 4 pRp3 kT
vl In S + 4pRp s
2
3

<0 >0
Rp* Rp

by a molecule in the liquid phase, S is the super- equilibrium vapor pressure of a vapor over a
saturation, T is the temperature, and s is the sur- droplet relative to that over a flat surface:
face tension. The first term is a function of the
change in free energy for a molecule going from    
2su1 2sM
the gas phase to the liquid phase (ultimately a S ¼ exp PA ¼ P0A exp
function of the saturation ratio, S) and the particle kTRp RT r1 Rp
volume. It is seen, in Fig. 4, that if S < 1, both
terms are positive and DG increases monotoni- where M is the molecular weight of the substances
cally. However, if S > 1, DG contains both posi- and rl is the liquid phase density.
tive and negative terms and for small droplet radii The Kelvin equation demonstrates an exponen-
the second term dominates with DG increasing as tially increasing equilibrium vapor pressure with
for the scenario for S < 1. As the radius increases, decreasing particle size. From this equation, a sat-
the first term (providing a reduction in DG) pro- uration ratio of the order of 10 is required for the
gressively becomes more important until DG smallest water vapor clusters to be thermodynam-
reaches a maximum at DG*, corresponding to a ically stable and grow. The critical radius in this
critical radius of Rp*. Above Rp*, the first term case comprises of the order of 20 water molecules.
starts to dominate, resulting in a reduction in DG. For realistic supersaturations encountered in the
The critical radius can be determined by setting atmosphere (e.g., S ¼ 1.01%), the critical radius
the derivative of DG ¼ 0 and solving, resulting in: is 0.12 mm and contains >108 molecules. As a
result, it is seen that water vapor does not partici-
2sv1 pate in homogeneous nucleation in the atmosphere.
R¼
p ¼ kT ln S For homogeneous-homomolecular nucleation,
supersaturation with respect to the species is
DG* represents a metastable equilibrium state required. In contrast, this is not the case for hetero-
where if one molecule evaporates from the droplet molecular nucleation where nucleation can take
of critical radius, the droplet will continue to place when the individual species are subsaturated
evaporate and shrink, while if one molecule is with respect to the pure substances but supersatu-
added to the droplet, the droplet will continue to rated with respect to the resulting solution droplet
grow. DG* represents a free energy barrier that the containing these substances. Binary homogeneous
system has to overcome in order to grow and nucleation is a process typically considered to
become stable. occur in the atmosphere and the theory is an exten-
Rearranging the previous equation gives the sion of homogeneous-homomolecular nucleation
so-called Kelvin equation that describes the to account for two species.
Aerosol in Global Atmosphere 247

Air contains many rapidly moving and collid- rate and sulfuric acid concentration corresponds to
ing trace gases of varying vapor pressures. Those the number of molecules in a critical cluster:
with low saturation vapor pressures, given the
right conditions, prefer to be in the liquid solution N crit ¼ dð ln J Þ=d ð ln ½H2 SO4 Þ
phase or the solid phase from a thermodynamic
perspective. The random collisions of this soup of Atmospheric measurements of the nucleation
molecules result in the continuous formation of rate versus sulfuric acid concentration reveal a
clusters of a few to tens of molecules. Such stable slope of between 1 and 2 [19, 20] as do the most
clusters will then grow in size with each subse- recent laboratory studies of nucleation. A slope of
quent collision of a low vapor pressure molecule. 2 can be explained by collision controlled or
The size of a critical cluster is of the order of kinetic nucleation [21] while a slope of 1 can be
0.5 nm; however, at this size, the cluster has a explained by two processes: one being the require-
very high diffusion coefficient and unless it grows ment of an additional stabilizing or condensing
rapidly, it will be scavenged by diffusion to larger, vapor participating in the initial growth of the
preexisting aerosol particles. For example, if the clusters; the other being activation of clusters by a
cluster can grow to 3 nm, its diffusion coefficient supersaturated vapor [22, 23]. It is thought that the
is reduced by a factor of 10 and if it grows to 6 nm, acid clusters are activated into aerosol particles in
it is reduced further by a factor of 10 [17]. In other the presence of a supersaturated organic vapor field
words, if the cluster can grow to 6 nm, its proba- in the same way that cloud nuclei are activated into
bility of survival is increased by a factor of 100. cloud droplets in a supersaturated water vapor field
In the atmosphere, very few vapors can partic- (the theory behind activation will be discussed later
ipate in homogeneous nucleation. The best candi- in the section on aerosol–cloud interactions).
date is sulfuric acid, which in conjunction with Recently, the formation of organosulfate clusters
water vapor can participate in binary homoge- was suggested to explain the chemistry behind the
neous nucleation. It should be noted that the prob- cluster activation or kinetic mechanisms and thus
ability of stable cluster formation (or nucleation) atmospheric nucleation [24]. The aforementioned
is exponentially inversely dependent on tempera- analysis reveals a critical cluster diameter of 0.8 nm
ture, and as a result, binary nucleation of sulfuric and 1–2 sulfuric acid molecules in the cluster. The
acid and water vapor is likely to occur only in the most recent laboratory studies [25] reveal that
upper troposphere and the stratosphere where nucleation occurs at H2SO4 concentrations similar
temperatures are sufficiently low to promote to those found in the ambient atmosphere during
nucleation under atmospheric concentrations of nucleation events and that the measured particle
sulfuric acid. In the troposphere, a different mech- formation rates are proportional to the product of
anism is required for nucleation to proceed under the concentrations of H2SO4 and an organic mole-
atmospheric concentrations of sulfuric acid con- cule. This suggests that only one H2SO4 molecule
centrations (typically 106–107 molecules cm3). and one organic molecule are involved in the rate-
In the presence of ammonia, classical theory pre- limiting step of the observed nucleation process.
dicts that ternary nucleation of ammonia, sulfuric Indirect measurements of 3–10 nm particle
acid, and water can readily proceed to more read- chemical composition immediately after a natural
ily produce thermonynamically stable clusters new particle production event over forested regions
under tropospheric conditions. The presence of reveal that the chemical composition of newly
ammonia lowers the thermodynamic barrier formed particles are not sulfuric acid or aerosol
which has to be overcome to form an embryo. In sulfate [26], but comprise more so of condensed
classical theory, whether binary or ternary nucle- organic matter. Calculations also reveal that there is
ation, the number of molecules in a critical cluster insufficient sulfuric acid to nucleate new clusters
is of the order of 10 or more. and to grow these into aerosol particles larger than
According to the nucleation theorem [18], the 3 nm. Whereas sulfuric acid appears to drive the
slope of the relationship between the nucleation nucleation of new clusters, an additional species is
248 Aerosol in Global Atmosphere

required to grow the clusters into aerosol particles. of sea-salt and dust aerosol are found in super-
Under very polluted conditions, there is typically micron size ranges, it is in these size ranges where
sufficient availability of sulfuric acid to both form nitric acid can also be found. However, in polluted
stable clusters and to grow these clusters into aero- regions, and in the absence of sea-salt and dust,
sol particles tens to hundreds of nanometers in size. nitric acid is also found in significant amounts in
During particle production events in background submicron-sized aerosol. Nitric acid and sulfate
air, the aerosol population typically increases from aerosol are generally sourced from pollution
concentrations of ~1,000 to ~100,000 cm3, while sources; however, in marine regions, the oxidation
in polluted air concentrations increase from of dimethylsulfide, a waste product from plankton
~10,000 to ~100,000 cm3 [22, 23]. activity, can provide a significant source of natural
The most dramatic and intense nucleation events SO2 and methane sulfonic acid, leading to natural
occur in coastal air where background concentra- aerosol production.
tions increase from ~500 to ~1,000,000 cm3 [26, Aqueous phase reactions can occur in liquid
27]. These events occur when seaweed beds are aerosol particles but typically, the majority of
exposed during low tide conditions. The algae aqueous phase production occurs in cloud drop-
emit I2 and CH2I2 which are rapidly photolyzed lets. It is estimated that between 75% and 90% of
and oxidized by O3 resulting in the formation of aerosol sulfate (SO4– –) is produced through this
iodine oxides which readily nucleate into stable pathway. In cloud, the droplet surface area and
clusters. In addition, there is sufficient iodine oxide volume of the cloud droplets promote the disso-
produced to account for the rapid growth of the lution of SO2 into the aqueous phase where it can
clusters into aerosol particles of 100 nm [28]. be rapidly oxidized by ozone and/or hydrogen
peroxide [29]. The oxidation route by ozone is
Multiphase Secondary Aerosol Production highly pH dependent and dominant in alkaline
The vast majority of secondary aerosol mass is not drops such as those formed on sea-salt aerosol,
produced through the nucleation process but while the hydrogen peroxide route dominates at
through condensation, aqueous phase reactions, lower pH values [30]. When sea-salt is present in
and multiphase processes. Condensation typically cloud nuclei, the cloud behaves as a virtual buffer,
involves both inorganic low-volatility gases, such increasing alkalinity and accelerating ozone-
as sulfuric acid and nitric acid, and a vast range of driven aqueous phase oxidation of SO2 to produce
condensable organic species. Sulfuric acid results sulfate [30]. This sulfate formation route led to the
from the oxidation of SO2 by the OH radical, significant production of acidic sulfate aerosol in
while nitric acid results from the oxidation of polluted air and was the primary cause of the acid-
NO2 in the atmosphere. NH3 can also condense rain problem in the 1970s–1980s.
on acidic particles resulting in fully or partially Oxidation of volatile organic compounds
neutralized particles. Nitric acid is regarded as a (VOCs) leads to the production of condensable
semivolatile condensable gas that can be thermo- organic vapors, ultimately producing secondary
dynamically stable in either the gas phase or the organic aerosol (SOA). The major oxidizing spe-
aerosol phase, depending on environmental con- cies are the OH radical, ozone, and the nitrate
ditions. At lower temperatures and higher relative radical (NO3). Like in the case of nitric acid,
humidities, nitric acid is more likely to be found in some of these condensable vapors can be semi-
the condensed aerosol phase, while at warmer volatile. There are both natural VOCs (biogenic:
temperatures and lower humidities, it is more BVOCs) and anthropogenic VOCs (AVOCs),
likely to evaporate. The chemistry of the pre- although it is estimated that the BVOC emissions
existing aerosol also influences the gas phase are of the order of ten times that of AVOC emis-
partitioning of nitric acid. For example, in sions. Some modeling studies suggest that in cer-
the presence of alkaline aerosol species such as tain heavily populated regions, AVOCs can
sea-salt and dust, nitric acid will preferentially contribute significantly to total organic carbon
condense to these aerosol types. Since the bulk levels [31]; other studies using carbon isotope
Aerosol in Global Atmosphere 249

analysis suggest that BVOC oxidation products characterized by relatively high H–C and low
contributed to the majority of SOA even in urban H–C–O groups which partly overlap; however,
regions [32]; however, it should be noted that the marine samples have a significantly lower
even BSOA production is somewhat linked to aromatic content. The functional composition of
anthropogenic activity as the main VOC oxidants biogenic OA and that of rural anthropogenic OA
are associated with anthropogenic emissions. are relatively close with the rural samples having a
For BVOC emissions, terpenes and sesquiter- higher H–C–O content. Both also contain high
penes from terrestrial vegetation emissions, are fractions of aliphatic carbonyls. The biomass
thought to be the dominant precursors of BSOA, burning water-soluble OA contained the highest
and to a lesser extent isoprene (particularly under content of hydroxyls and the lowest amount of
high NOx conditions [33]), while aromatic com- alkylic groups.
pounds such as toluene, xylene, and trimethyl The formation of SOA is not always via the gas
benzene are thought to account for the majority phase formation of condensable vapors. In the
of ASOA formation. There has been considerable case of isoprene-related SOA production, its rela-
effort to identify the composition of SOA in recent tively high vapor pressure oxidation products sug-
years; however, the vast majority of compounds gest little contribution to SOA; however,
remain unidentified due to complex mixtures of alternative routes have been suggested, which
compounds often with few distinguishing fea- produce low-volatility aerosol phase products.
tures. SOA is generally oxygenated and water For example, tetrols with the same backbone as
soluble, in contrast to hydrocarbon-like water- isoprene have been observed in atmospheric aero-
insoluble POA. Various approaches have been sols [35] possibly formed by the heterogeneous
taken to speciate the organic mass found in acid-catalyzed oxidation of isoprene in the pres-
SOA. For example, 1H nuclear magnetic reso- ence of peroxides [36]. Additionally, heteroge-
nance (HNMR) techniques have been applied to neous reaction of isoprene under highly acidic
evaluate functional groups in water-soluble OA conditions was also observed to lead to the for-
for different aerosol source regimes [34]. The mation of polymeric, humic-like substances
technique readily detects four main functional [37]. Other studies showed that some high-
groups in atmospheric water-soluble OA: volatility carbonylic oxidation products can con-
unfunctionalized alkyls (H–C); aliphatic carbons tribute to SOA through the interaction with highly
bound to an unsaturated carbon atom (H–C–C¼); acidic inorganic preexisting aerosols [38], while
aliphatic alcohols, ethers, and esters (H–C–O; and polymerization of second-generation products has
aromatic rings (H–Ar). Additionally, formylic been suggested to contribute to SOA growth
(H–C¼O), acetalic (O–CH–O), and sulfonic [39]. Cloud modeling studies [40] also predict
(H–C–S¼O) groups are detected. Water-soluble that low-volatility water-soluble oxidation prod-
OA samples from the boreal forest in Finland ucts of isoprene can be oxidized in the aqueous
(terrestrial biogenic), biomass burning events in phase in clouds to produce dicarboxylic acids.
Brazil, rural UK, and the Northeast Atlantic Once SOA is formed, it contributes to a
(marine) were analyzed for functional groups dynamic thermodynamic and chemical evolution
using this approach. Figure 5 illustrates, on system. SOA species can be repartitioned to the
the vertical axis, the aliphatic carbon fraction gas phase and undergo polymerization and oxida-
(carbonylic/carboxylic, HC–C¼O groups) and, tion leading to significant changes in the chemical
on the horizontal axis, the fraction of alip- nature of SOA. The evolution of SOA is well
hatic carbon accounted for by hydroxyl groups illustrated through the examination of SOA mass
for a range of standard SOA compounds spectral properties moving from strong urban
(levoglucosan, succinic acid, adipic acid, pinonic source regions to remote continental regions.
acid, glutaric acid, and nonanoic acid) alongside Aerosol mass spectrometry (particularly using
the diverse atmospheric samples. The analysis the Aerodyne Aerosol Mass Spectrometer –
show that marine and terrestrial biogenics are AMS) delivers increased speciation capability on
250 Aerosol in Global Atmosphere

Aerosol in Global a 1
Atmosphere, Fig. 5 (a)
Functional group 0.9

HC-C=O / sum aliphatics


distributions of standards of 0.8 levoglucosan
water-soluble organic 0.7
compounds. The area succinic acid
0.6
including the composition adipic acid
of the real atmospheric 0.5
samples is also indicated. 0.4 pinonic acid
(b) Functional group
0.3 glutaric acid
distribution of WSOCs
samples characteristic of 0.2 nonanoic acid
specific aerosol sources. 0.1
Diagonal lines represent the samples
0
percentage fraction of total 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
oxygenated groups (H–C– HC-O/sum aliphatics
O + HC–C¼O). (Copyright
American Chemical Society
2007. Reprinted from [34]) b 0.60
Po Valley FA/WI

70

80
%

%
HC-C=O / sum aliphatics

0.55 Po Valley SP/SU


Mt Cimone
Aromatic/ 0.50 SOA
aliphatic Brazil semi-clean
0.45 ACE-Asia SP
0.3
Hyytiala polluted
0.2 0.40 Marine
BB Singapore
0.1 OA
0.35 UK SU urban
60
50

UK SU coastal
%

0.30
0.00 0.10 0.20 0.30 0.40
HC-O/sum aliphatics

both POA and SOA. This technology splits the remote rural locations, is shown in Fig. 6. What
organic aerosol into three generic types – an oxy- is clearly evident from the suite of measurements
genated organic aerosol (OOA), a hydrogenated is that organic matter comprises a significant
fossil-fuel-derived organic aerosol (HOA), and a fraction of the aerosol mass at all locations; how-
biomass burning organic aerosol (BBOA). OOA ever, the further from pollution sources, the more
is characterized by its highly oxidized state with oxygenated the organic aerosol is (i.e., the ratio
atomic O:C ratios between 0.25 and 1 and can be of OOA/HOA increases) and the more aged, or
further categorized into two subgroups based on distant from pollution sources, the higher frac-
volatility and O:C ratio. Low-volatility OOA tion of OOA is low-volatility OOA. This study
(~C8O5.5H10) has a high O:C ratio and is fre- also reports the evolution of the Mexico City
quently correlated to other secondary species pollution plume within which there is intense
such as sulfate aerosol and is consistent with an SOA formation. They found that near the plume
aged aerosol. Semivolatile OOA (~C8O3H10) has source region, semivolatile OOA dominated the
a lower O:C ratio and is better correlated with organic aerosol signal; however, as the plume
other semivolatile species such as nitrates and is advected and aged downwind, the fraction of
consistent with a partially photochemically aged low-volatility OOA and the O:C ratio increased.
aerosol. Laboratory studies on the evolution of biogenic
A compilation [41] of measurements of HOA SOA (from a-pinene oxidation), biomass burn-
and OOA types, along with major inorganic spe- ing smoke, and the POA surrogate squalane also
cies, at different urban, urban downwind, and exhibit similar aging patterns as in the reported
Aerosol in Global Atmosphere 251

Urban Inorganics: Sulfate Nitrate Ammonium Chloride


Urban Downwind
Remote Organics: HOA Other OA SV-OOA Total OOA LV-OOA
New York City, NY Manchester, UK Hyytiala Taunus Mainz
Pinnacle Park, NY Edinburgh, UK Chelmsford, UK
(Winter) (Summer) (Winter) (Summer) Finland Germany Germany
12.3 12.2 5.2 3.0 5.3 2.0 16.3 25.5
11.6 14.3 4.2

(Winter)
Zurich, Switzerland
14.7 9.6
Pittsburgh. PA

(Summer)
7.0 2.3

Jungfraujoch
Switzerland
Boulder, CO Storm Peak, CO Vancouver
Canada

2.1 1.0 80.0


0.8

Beijing
China
0.6

0:C
0.4
0.2
4.4 0.0 16.2

HOA

Other OA

SV-OOA

Total OOA

LV-OOA

(Winter)
Tokyo, Japan
19.1 12.8 26.8 2.8 9.5 8.5 2.9 10.7 7.9 11.0 13.2
Riverside, CA

(Summer)
Houston, TX Mexico Duke Forest Thompson Off Coast Chebogue Cheju Island Okinawa Fukue
City NC Farm, NH New England, US Canada Korea Japan Japan

Aerosol in Global Atmosphere, Fig. 6 Total mass con- FA-AMS methods identified one OOA factor, whereas in
centration (in micrograms per cubic meter) and mass frac- other locations, two types, SV-OOA and LV-OOA, were
tions of nonrefractory inorganic species and organic identified. HOA is a surrogate for urban primary OA, and
components in submicrometer aerosols measured with Other OA includes primary OAs other than HOA that have
the AMS at multiple surface locations in the Northern been identified in several studies, including BBOA.
Hemisphere (21). The organic components were obtained (Reprinted from [41])
with FA-AMS methods (3, 15–17). In some studies, the

atmospheric plumes. The laboratory results dem- The previous study developed, on the basis of
onstrate that in the early stages of SOA produc- the mentioned experimental studies, a simple 2D
tion, the OA mass spectrum resembles that basis (2D-VBS) model encapsulating the evolu-
associated with the respective source, but as oxi- tion of OA volatility (determined as saturation
dation and aging proceeds, the SOA spectra concentration C* at 298 K) and oxidation state
evolve into initially semivolatile OOA spectra (O:C ratio) to describe the evolution of OA in the
and ultimately into low-volatility OOA spectra. atmosphere [41]. These two properties can be
The combined atmospheric and laboratory stud- measured in real time and are thus used to con-
ies suggest that with atmospheric oxidation, most strain the model with experimental field data. The
types of OA converge to a final state of low- model incorporates photochemical aging using a
volatility OOA, irrespective of the original branching ratio between functionalization and
source. It should, however, be noted that primary fragmentation kernels and homogeneous and het-
and secondary marine aerosol aging was not erogeneous oxidation by OH, and where the first
evaluated and that these, potentially, could generation of oxidation is explicitly modeled
behave differently to the terrestrial biogenic and while the second generation is phenomenologi-
anthropogenic OA types. cally modeled. The conceptual framework was
252 Aerosol in Global Atmosphere

applied to SOA production from a-pinene ozone- modules along with deposition schemes and are
driven oxidation and was found to predict first- underpinned by field and laboratory studies into
generation products with 1 < C* < 107 mg m3 key processes. In addition, quantification is
and 0.1 < O:C < 0.4. Given that generally achieved by long-term observations of atmo-
organics with C* < 10 mm3 will partition into spheric composition at various point locations
the aerosol phase, it is evident that most of the around the globe. Remote sensing of aerosol
oxidation products remain as volatile gases. The parameters from surface and space-borne plat-
first-generation products can then functionalize forms also provide added information on horizon-
through OH reactions resulting in a tripling of tal and vertical distributions.
SOA mass production after second-generation
oxidation. The model is able to predict the evolu- Global Budgets
tion of SOA in the 2D volatility and O:C space, Atmospheric aerosols are derived from both nat-
remaining consistent with the production key ural and anthropogenic sources. Natural sources
products such as the first-generation cis-pinonic include sulfate and sea spray (sea-salt and primary
acid, regarded as a semivolatile OOA, and organic matter) from the oceans, dust from desert
second-generation products such as a,- regions, particulate organic matter from biogenic
a-dimethyltricarballylic acid, a low-volatility sources (both terrestrial and oceanic), and sulfate
OOA. Similar evolution was found for other and silicates from volcanoes. Anthropogenic
SOA sources like evaporated diesel and biomass sources include sulfate, black carbon and primary
burning. This 2D volatility and O:C conceptual and secondary organic matter from fossil fuel
has made considerable advances in simplifying combustion and biomass burning, dust from
the treatment of an incredibly complex system industrial sources, and nitrates mainly from trans-
and can be further developed and extended to port emissions. The best estimated emissions and
include other key processes such as oligomeriza- resulting atmospheric mass and number burdens
tion. The combined perspective to emerge from are displayed in Table 1 [42]. The largest natural
the recent mass spectral measurements and the emission is that of sea-salt with a “best guess” of
modeling framework is that most OA appears to 10,130 Tg a1, followed by dust with a best guess
be an intermediate or transition state between emission of 1,600 Tg a1. Biogenic secondary
primary emissions and highly oxidized volatile organic emissions are 25 Tg a1, compared to
gases such as CO and CO2. 3.5 Tg a1 for anthropogenic emissions. For sul-
fate aerosol, anthropogenic emissions (122 Tg
a1) dominate over natural biogenic (57 Tg a1)
Global Aerosol Budgets, Burdens, and and volcanic (21 Tg a1) emissions and for pri-
Spatial Distributions mary organic aerosol, anthropogenic emissions
amount to 95 Tg a1 while natural oceanic pri-
The diverse nature of aerosol sources from natural mary organic aerosol (not shown in Table 1) is
and anthropogenic emissions, different formation estimated to be 16 Tg a1 [56]. Black carbon
and removal processes, and different transport emissions from fossil fuel amount to 4.5 Tg a1.
mechanisms results in great inhomogeneity in
annual emission budgets, atmospheric burdens, Global Burdens
and spatial distributions of individual aerosol spe- The spatial distribution of total aerosol mass is
cies. The result is ultimately significant variability shown in Fig. 7. The distribution is a medium
in radiative forcing and air pollution on regional mass composite from 10 global atmospheric cli-
scales. To quantify budgets and distributions, gen- mate (general circulation) models and chemical
eral circulation (climate) models or chemical transport models for the year 2000. From the
transport models, are used in conjunction with model output, the global average column burden
emission inventories. These models contain aero- for all aerosol types is ~50 mg m2, with regional
sol–cloud chemistry formation and evolution loadings exceeding 500 mg m2, in places such as
Aerosol in Global Atmosphere 253

Aerosol in Global Atmosphere, Table 1 Particle emission/production and burdens estimated for the year 2000.
(Copyright Elsevier 2008. Reprinted from [42])
Mass Mass
emission burden Number prod.
Min Max
Tg Number
“Best guess” a1 Tg a–1 burden
Carbonaceous aerosols
Primary organic (0–2 mm) 95 40 150 1.2 – 3101024
Biomass burning 54 26 70 – 71027 –
Fossil fuel 4 3 9 – – –
Biogenic 35 15 70 0.2 – –
Black carbon (0–2 mm) 10 8 14 0.1 – 2701024
Open burning and 6 5 7 – – –
biofuel
Fossil fuel 4.5 3 6 – – –
Secondary organic 28 2.5 83 0.8 – –
Biogenic 25 2.5 79 0.7 – –
Anthropogenic 3.5 0.05 4.0 0.08 – –
Sulfates 200 107 374 2.8 21028 –
Biogenic 57 28 118 1.2 – –
Volcanic 21 9 48 0.2 – –
Anthropogenic 122 69 214 1.4 – –
Nitrates 18 12 27 0.49 – –
Industrial dust etc. 100 40 130 1.1 – –
Sea-salt
d < 1 pm 180 60 500 3.5 7.41026 –
d ¼ 1–16 mm 9,940 3,000 20,000 12 4.61026 –
Total 10,130 3,000 20,000 15 1.21027 271024
Mineral (soil) dust
<1 mm 165 – – 4.7 4.11025 –
1–2.5 mm 496 – – 12.5 9.61025 –
2.5–10 mm 992 – – 6 – –
Total 1,600 1,000 2,150 18  5 1.41026 111024
Range reflects estimates reported in the literature. The actual range of uncertainty may encompass values both larger and
smaller than those reported here. Values are based on the following publications: [31, 43–55])

North Africa and Asia. These plumes of high global burden is 0.36 mg m2, with values
aerosol burdens extend out into ocean regions exceeding 5 mg m2 occurring over China and
(e.g., the African plume is seen to extend out burdens of 1–2 mg m2 occurring over regions
west into the Atlantic). North America and Europe such as Africa and South America, with slightly
exhibit moderate levels of aerosol burden, while lower burdens occurring over Europe and North
somewhat higher burdens are seen over South America. Significant black carbon plumes are
America and Australia. Significant burdens are seen to advect out over the Atlantic and Indian
also seen over remote oceanic regions such as Oceans from the two aforementioned highest bur-
the south Pacific and Indian Ocean. The dominant den regions.
source regions for different species are revealed For dust, the global average burden is
when burden distribution maps are examined for ~25 mg m2, with peak burdens exceeding
individual aerosol species. For black carbon, the 500 mg m2 occurring over the Sahara desert in
254 Aerosol in Global Atmosphere

AEROCOM_MEDIAN Mean: 5.05818E+01 mg/m^2 AEROCOM_MEDIAN Mean: 3.60902E–01 mg/m^2


90 mg/m^2 90 mg/m^2
500.0000
50.0000
100.0000
45 45 10.0000
25.0000
2.5000
Latitude

Latitude
5.0000
0 0 0.5000

1.0000
0.1000

0.2500 0.0250
−45 −45

0.0500 0.0050

0.0100 0.0010
−180 −120 −60 0 60 120 180 −180 −120 −60 0 60 120 180
Longitude Longitude
Total Aerosol Black Carbon

AEROCOM_MEDIAN Mean: 2.55353E+01 mg/m^2 AEROCOM_MEDIAN Mean: 2.90209E+00 mg/m^2


90 mg/m^2 90 mg/m^2
500.0000
50.0000
100.0000
45 45 10.0000
25.0000
2.5000
Latitude

Latitude

5.0000
0 0 0.5000

1.0000
0.1000

0.2500 0.0250
−45 −45

0.0500 0.0050

0.0100 0.0010
−180 −120 −60 0 60 120 180 −180 −120 −60 0 60 120 180
Longitude Longitude
Dust Particulate Organic Matter

AEROCOM_MEDIAN Mean: 3.53260E+00 mgS/m^2 AEROCOM_MEDIAN Mean: 1.35300E+01 mg/m^2


90 mg/m^2 90 mg/m^2
500.0000
50.0000
100.0000
45 10.0000 45
25.0000
2.5000
Latitude

Latitude

5.0000
0 0.5000 0
1.0000
0.1000

0.0250 0.2500
−45 −45

0.0050 0.0500

0.0010 0.0100
−180 −120 −60 0 60 120 180 −180 −120 −60 0 60 120 180
Longitude Longitude
Non-sea-salt Sulphate Sea-Salt

Aerosol in Global Atmosphere, Fig. 7 Median global 2000. (Copyright European Geophysical Union 2006.
distribution of aerosol column mass, total and per aerosol Reprinted from [57])
species, derived from 10 AEROCOM models for the year

Northwest Africa. East Europe and Asia are also black carbon, but with a significantly higher col-
seen as significant dust source regions, and to a umn burden of 3 mg m2. Peak values approach
lesser degree, western USA and central Australia. 50 mg m2 and the main source regions are the
For Particulate Organic Matter, the spatial distri- southwestern African Continent, South America,
bution of the column burden is similar to that of Europe, India and China, northern Australia, and
Aerosol in Global Atmosphere 255

southeast USA. Significant levels of the order of such as sodium, chloride, nitrate, sulfate, and
1 mg m2 are also seen over most oceanic regions. ammonium are easily detected; however, it is
Non-sea-salt sulfate exhibits a global average bur- also possible to quantify the water-soluble and
den of ~3.5 mg m2, with peak values of the order water-insoluble organic component. It is readily
of 50 mg m2. Again, the main developed and seen that the absolute and relative contributions of
developing countries with significant population the above species varies greatly with air mass, or
densities appear as burden “hot spots” as for the source origin [58]. Peak submicron mass loadings
other anthropogenic aerosol types (e.g., black car- occur for the continental air, while peak super-
bon and particulate organic matter). In contrast to micron masses occur for marine air. In marine
other anthropogenic sources, there are notable polar air, the supmicron sizes are almost exclu-
burdens over remote oceanic regions, reflecting sively composed of sea-salt, while submicron
also its natural oceanic source. sizes are marginally dominated by nss-sulfate,
Finally, the sea-salt burden is 13.5 mg m2, with the second largest contribution derived
with peak burdens of ~50 mg m2. The peak from sea-salt. Small amounts of ammonia,
burdens occur at midlatitudes, or the “roaring water-soluble organic matter and water-insoluble
40s,” north and south of the equator, and are organic matter are also evident. By contrast, in the
associated with regions of intensive cyclonic continental air, sea-salt and nitrate are the two
activity. dominant species in supermicron sizes, with
It is interesting to note that in Table 1, sea-salt smaller amounts of organic matter visible and in
was highlighted as being the single most important the submicron sizes, nss-sulfate and water-soluble
aerosol emission type, but it had a mass burden organic matter dominate. It should be noted that
slightly lower than dust which had significantly marine aerosol can be significantly enriched in
lower emissions than sea-salt. In the AEROCOM organic matter depending on the degree to which
(http://dataipsl.ipsl.jussieu.fr/AEROCOM; [57]) air masses pass over biologically rich waters.
study, dust also has a higher burden for generally Mass is only one important parameter of an
lower emissions. The explanation is that significant aerosol size distribution. Perhaps the other most
dust plumes are vented into the Free Troposphere important parameter is the number concentration,
where removal rates are slower and residence times and in particular, the concentration in the so-called
are longer than in the marine boundary layer where accumulation mode (100–500 nm diameter). This
removal rates are likely higher due to higher pre- size range is not only important for scattering and
cipitation rates and, for the larger-sized particles, radiative effects of atmospheric aerosols, it is cru-
shorter gravitational settling timescales (i.e., sea- cially important in terms of influencing the num-
salt is not injected at as high altitudes as dust, so ber concentration of cloud condensation nuclei.
they settle out more rapidly). Figure 9 illustrates the horizontal and vertical
At any one location, the chemical composition (zonal) average concentration in the accumulation
of atmospheric can vary significantly depending mode size range [59]. It can be seen that the
on the air mass back trajectory arriving at that highest number concentration of aerosols
location. An example of the chemical variability (N ¼ 3,000–5,000 cm3) occurs over regions in
encountered is demonstrated for the Northeast Europe such as the Netherlands and Northern
Atlantic region where clean marine and polluted Italy, China, India, and Brazil.
continental air masses are frequently encountered
at the Mace Head Atmospheric Research Station, Vertical Distributions
which is representative of the region. Figure 8 The vertical distribution of aerosol particles, mea-
illustrates the absolute chemical composition and sured as aerosol backscatter using a LiDAR (Light
the relative chemical composition observed in two Detection And Ranging), typically reveals maxi-
contrasting air masses (continental polar, mari- mum particle mass and number concentrations in
time polar) of different origin over the Northeast the atmospheric boundary layer (lower
Atlantic. Typically, the main ionic compounds ~1,000–2,000 m) as shown in Fig. 10. In this figure,
256 Aerosol in Global Atmosphere

SS NO3 nssSO4 NH4 MSA non-MSA-WSOM WIOM

3.0 100%

2.5 cP
80%

Mass contribution
2.0
60%
μg m−3

1.5
40%
1.0

20%
0.5

0.0 0%
0.06–0.125

0.125–0.25

0.25–0.5

0.5–1.0

1.0–2.0

2.0–4.0

4.0–8.0

0.06–0.125

0.125–0.25

0.25–0.5

0.5–1.0

1.0–2.0

2.0–4.0

4.0–8.0
Size range [μm] Size range [μm]
7.0 100%
6.0
mP 80%
5.0
Mass contribution

4.0 60%
μg m−3

3.0
40%
2.0
20%
1.0

0.0 0%
0.06–0.125

0.125–0.25

0.25–0.5

0.5–1.0

1.0–2.0

2.0–4.0

4.0–8.0

0.06–0.125

0.125–0.25

0.25–0.5

0.5–1.0

1.0–2.0

2.0–4.0

Size range [μm] Size range [μm] 4.0–8.0


1.4 100%

1.2 mA
80%
Mass contribution

1.0
60%
μg m−3

0.8

0.6
40%
0.4
20%
0.2

0.0 0%
0.06–0.125

0.125–0.25

0.25–0.5

0.5–1.0

1.0–2.0

2.0–4.0

4.0–8.0

0.06–0.125

0.125–0.25

0.25–0.5

0.5–1.0

1.0–2.0

2.0–4.0

4.0–8.0

Size range [μm] Size range [μm]

Aerosol in Global Atmosphere, Fig. 8 Absolute (left measured at Mace Head, Northeast Atlantic, during June
panel) and relative (right panel) chemical composition of 2008. (Copyright European Geophysical Union 2009.
the aerosol samples collected in continental polar (cP), Reprinted from [58])
maritime polar (mP), and maritime Arctic (mA) air masses
Aerosol in Global Atmosphere 257

Aerosol in Global 180°W 120°W 60°W 0° 60°E 120°E 180°


Atmosphere,
Fig. 9 Climatological
annual means of simulated 60°N 60°N
accumulation mode aerosol
particle concentration
obtained from a 10-year
integration. The 0° 0°
geographical distribution is
of the lowermost model
layer, which is about 60 m
thick. (Copyright European
60°S 60°S
Geophysical Union 2006.
Reprinted from [59])
180°W 120°W 60°W 0° 60°E 120°E 180°

0 1 2 5 10 20 50 100 200 500 750 1000 1500 2500 5000


Particle concentration [cm–3 STP]

Attenuated Backscatter Coefficient x 10−3


5000 2

4500 1.8

4000 1.6

1.4
3500

1.2
Range (m)

3000

sr−1 m−1
1
2500
0.8
2000
0.6
1500
0.4
1000
0.2
500
00:00 02:24 04:48 07:12 09:36
Time (UTC)

Aerosol in Global Atmosphere, Fig. 10 LIDAR aero- Research Station on the Irish Atlantic coastline. Measure-
sol attenuated backscatter vertical profiles of the atmo- ments were taken during polluted continental air outflow
spheric boundary layer and free troposphere. from Europe into the Atlantic region
Measurements were taken at the Mace Head Atmospheric

the attenuated atmospheric aerosol backscatter pro- in the free troposphere, very clean aerosol levels are
files illustrate the vertical aerosol structure [58]. In seen.
the case shown, the main boundary layer tempera- Figure 11 displays a 10-year climatology of
ture inversion is at ~1,500 m and within the bound- accumulation mode zonal vertical distributions
ary layer there is a surface-mixed layer at 500 m. demonstrating that the Northern Hemisphere
The peak aerosol burden occurs in the surface- from 60 N to 20 into the Southern Hemisphere
mixed layer and corresponds to a European pollu- contains the highest particle number concentra-
tion plume advecting out into the tions (~700 cm3). The cleanest concentrations
Atlantic. Significant aerosol backscatter (and hence occur in and around Antarctica, while the second
aerosol loading) is seen in the residual boundary cleanest is in the upper troposphere–stratosphere
layer between 1,000 and 2,000 m. Above 2,000 m, region.
258 Aerosol in Global Atmosphere

100
200
300
pressure (hPa)

400
500
600
700
800
900
1000
90°S 60°S 30°S 0° 30°N 60°N 90°N

0 1 2 5 10 20 50 100 200 500 750 1000 1500 2500 5000


Particle concentration [cm−3 STP]

Aerosol in Global Atmosphere, Fig. 11 Climatological obtained from a 10-year integration. The concentrations are
annual means of simulated zonally averaged vertical cross- given at STP conditions. (Copyright European Geophysical
section accumulation mode aerosol particle concentration Union 2006. Reprinted from [59])

Vertical profiles of total number of concentra- source of stratospheric aerosols with injections to
tions (historically defined as condensation nuclei, the tune of 30 Tg SO2 for intense eruptions such as
or CN, typically larger than 10 nm), and size- Pinatubo, producing the main precursor for strato-
resolved concentration measurements (with spheric aerosol formation. In terms of strato-
radius > 0.15 mm to sizes greater than 2 mm) up spheric aerosol chemical composition, the
to the higher stratosphere are shown in Fig. 12 majority of stratospheric aerosol is composed of
(taken from [60]). In this figure, concentrations 75% sulfuric acid and 25% water, formed from
are shown for 1 year and 15 years after the binary homogeneous nucleation and subsequent
Mt. Pinatubo eruption. What is evident is that condensation of sulfuric acid as suggested by
total aerosol, or CN, concentration at the surface boiling point measurements of the stratospheric
is between 500 cm3 (typical of clean background aerosol [61]. Other sources of stratospheric aero-
continental air masses) and 3,000 cm3 (typical of sols include organic carbonyl sulfide, particularly
polluted continental air masses) and that free tro- above altitudes of 25 km, and meteoritic material,
posphere, or upper free tropospheric concentra- rocket exhaust, and aircraft emissions are
tions are relatively constant at a concentration of regarded as having minimal influence on the
the order of 500 cm3. Above 15 km, in the stratospheric aerosol layer [[60] and references
stratospheric layer, CN concentrations are typi- therein.].
cally 1–10 cm3, despite the volcanic eruption. A particularly interesting stratospheric aero-
However, what is evident in the difference in time sol is aerosol forming polar stratospheric clouds
lapse following the eruption is that there is a (PSCs). These aerosol haze layers, or more often
significant increase in aerosol concentration known as cloud layers, have been the subject of
(at least an order of magnitude) at sizes greater intense interest after the discovery of their role in
than 0.15 mm radius 1 year after the eruption stratospheric ozone loss through converting
compared to what is considered the background chlorine inactive to active chlorine and
stratospheric aerosol burden 15 years after the denitrifying the stratosphere. Observational, lab-
eruption. Clearly, volcanic eruptions are a major oratory, and theoretical work has since shown
Aerosol in Global Atmosphere 259

Temperature (K) Temperature (K)


180 200 220 240 260 280 180 200 220 240 260 280
40 40
r>0.15, r>0.25, r>0.50, r>0.78, r>1.08, r>1.58, r>2.0 μm

(41°N, 105°W) Laramie, Wyoming


a) 24 June 1992
35 35
b) 6 May 2006

30 30

25 25
Altitude (km)

20 CN CN 20

15 15

10 10

5 5

0 0
10−3 10−2 10−1 100 101 102 103 10−3 10−2 10−1 100 101 102 103
Concentration (cm−3) Concentration (cm−3)

Aerosol in Global Atmosphere, Fig. 12 Stratospheric top is also shown. These profiles were measured in (a) June
aerosol profiles above Laramie Wyoming (41 N, 106 W) 1992, 1 year after the Pinatubo eruption and (b) May 2006,
indicating the concentration of condensation nuclei 15 years after Pinatubo. (Copyright Elsevier 2008.
(CN) and aerosol with radii greater than 0.15, 0.25, 0.50, Reprinted from [60])
0.78, 1.08, 1.58, and 2.0 mm. Temperature with scale at the

that PSC particles above the ice point are either dehydration/denitrification, thus determining
solid nitric acid trihydrate (NAT) particles or the time frame during which chlorine will remain
liquid ternary aerosol (LTA), droplets composed active, and ultimately determining the funda-
of nitric acid, sulfuric acid, and water. The com- mental processes associated with ozone deple-
position and phase of the particles determines the tion in the polar stratosphere.
threshold temperatures at which they occur and The main open question concerning the forma-
persist – specifically, NAT will exist at tempera- tion of PSCs is the process by which NAT forms.
tures 3–5 K above LTA temperatures, while LTA LTA growth is strictly a function of gas-phase-
will begin to appear about 3 K above the ice point mixing ratios and temperature, as the vapor pres-
for polar stratospheric levels of gaseous nitric sures of sulfuric acid, nitric acid, and water adjust
acid and water [62, 63]. Particle phase also con- to environmental temperature and molecular col-
trols the development of particle size, which lisions. LTA begins to grow on the SA as soon as
plays a large role in the extent and rate of temperatures reach about 3 K above the ice point.
260 Aerosol in Global Atmosphere

At these temperatures, the concentration of NAT sea-salt or ammonium sulfate which readily dis-
particles is often at best only 0.001 of the aerosol sociates in water to form an electrolyte solution
population [64–66] indicating clearly a nucleation droplet. In subsaturated air (relative humid-
barrier which is not well understood. Laboratory ity < 100%), these solution droplets can exist
investigations suggest that LTA must be signifi- due to the lowering of the equilibrium vapor pres-
cantly supercooled for NAT nucleation. Arctic sure above the droplet surface by the presence of
PSC observations in the early 2000s suggest the the dissolved ions (known as the Roault Effect).
importance of a small population of NAT particles As a result, soluble aerosol particles, depending
and that such a population forms at temperatures on the chemical composition, readily form solu-
just a few degrees below the NAT point in both tion drops with a water fraction dependent on
leewaves [64] and synoptic situations [66]. These relative humidity. This means that the “wet” aero-
latter observations are the clearest evidence yet sol equilibrium size responds to, and is dependent
indicating that NAT forms readily on a small on, ambient relative humidity. The “wet” aerosol
fraction (104–105) of SA through heteroge- size will grow with increasing humidity and
neous nucleation. shrink with reducing humidity. Since the optical
properties (e.g., scattering) of aerosols is size
dependent (and proportional to crosssectional
Water Uptake by Aerosols area), relative humidity can significantly influence
the hazing, or optical extinction effect of aerosol
One of the most important gases in the atmo- layers. A measure of this effect is the hygroscopic
sphere is water vapor as it not only contributes growth factor, normally defined as the change in
predominantly to the natural greenhouse effect, aerosol diameter from a low relative humidity
resulting in a livable global average temperature, (e.g., 40%) corresponding to a dehydrated dry-
in its condensed liquid and ice phases, it forms size diameter to a high relative humidity
aerosol haze and cloud layers which contribute to (normally 90%) with significant hydration. Salts
approximately 50% of the planetary albedo. like ammonium sulfate and sea-salt have a growth
Many aerosol types have an affinity to water factor of 1.8 and 2.2, respectively, over this
and, under the right humidity conditions, they humidity range, while organic aerosol possesses
can become solution droplets, larger than the a growth factor typically from 1 to 1.4 depending
dry aerosol size, by uptake of water vapor from on the degree of solubility.
the air around it. Aerosol humidification has
implications for optical scattering, condensation
processes, and chemical interactions on and Cloud Droplet Activation
within aerosol particles. Liquid water clouds are In supersaturated environment, a subset of the
extensive in the atmosphere, but as was shown aerosol can grow to a critical size which becomes
above, pure water droplets cannot form under metastable, and with an infinitesimal further
atmospheric conditions. Condensation nuclei increase in humidity, the droplet will become
are required for the formation of cloud droplets. unstable and spontaneously grow to sizes of the
Cloud droplets are aerosol particles that have order of 10 mm and become a cloud droplet. This
rapidly grown to 10–100 times the size of the process is called cloud droplet activation. The
initial nucleus, corresponding to more than 1,000 description of the equilibrium size of a droplet
times increase in mass, almost solely through with water saturation ratio, founded on the early
water uptake. work of Kőhler [67], is now well established and
can be readily derived from the Clausius–
Aerosol Hygroscopicity Clapeyron equation modified to give a general
A large fraction of the atmospheric aerosol popu- equilibrium relation between an aqueous salt solu-
lation is water soluble or partially water soluble. tion droplet and water vapor (known as the Kőhler
The soluble aerosols are typically salts such as curve):
Aerosol in Global Atmosphere 261

 
2vw s unless the environmental S reduces below the
S ¼ aw exp
RTr equilibrium value of Sc at the instantaneous
value of rc. In this case, with no further change
S, is known as the saturation ratio, aw is the in S, the droplet will evaporate to its subcritical
water activity, the term within the brackets is the equilibrium size.
Kelvin factor, vw is the partial molar volume of The Kőhler expression can be envisaged as the
water, s is the surface tension of the solution at the competition between the two expressions of com-
composition of the droplet, R is the universal gas ponent properties determining activation of parti-
constant, T is the droplet temperature, and r is the cles: the curvature term and the solute term. The
particle radius. solute terms depend first on the number of solu-
This form of the Kohler equation can be sim- tion molecules and then on the dissociation of
plified to [1, 68–72] these molecules. The effect can be illustrated for
two frequently assumed cloud condensation
A B 2s vmM w
S¼1þ  A¼ B¼ nuclei types: ammonium sulfate and sodium chlo-
rc rc 3 nw KT Ms 4=3prw ride. (NH4)2SO4 has a molecular weight of 132 g
Mol1, while that of NaCl is 58.5 g Mol1. Thus,
where v is the number of dissociated ions per in the absence of dissociation, a given mass of
solute molecule, ms is the solute mass, and sub- NaCl in solution would yield 2.26 times more
scripts “s” and “w” relate to solute and water dissolved molecules than (NH4)2SO4. Assuming
properties, respectively. The term in A is denoted full dissociation (infinite dilution), (NH4)2SO4
the Kelvin or curvature term, and the term in B, is yields three ions while NaCl yields two, so the
known as the Raoult or solute term. The curvature net effect of the molecular mass and dissociation
term results in an increase in equilibrium vapor is that NaCl is 2.26/1.5 ¼ 1.5 times more active
pressure with reducing particle size, while the than (NH4)2SO4 for the same dry mass of particle
solute term results in a reduction in equilibrium (the Sc ratio for the two species is around 1.22 due
vapor pressure with increasing solute mass. to the square root dependence). This is illustrated
Figure 13 shows the contribution of the Kelvin in Fig. 13 where the peak supersaturation is plot-
and Raoult terms to equilibrium vapor pressure ted versus dry diameter for particles comprising
and equilibrium droplet size for a 200 nm dry each electrolyte. This figure directly illustrates the
diameter ammonium sulfate particle in a sub- significant differences in the critical supersatura-
saturated and supersaturated regime [73]. This tion as a function of both the chemical composi-
form of the expression shows a single character- tion and dry size of a particle (Raoult and Kelvin
istic maximum in supersaturation for a given dry effects). Additionally, in this figure is illustrated
composition and size, known as the critical super- the effect of nuclei containing an insoluble core.
saturation, Sc, associated with a unique size, The effect of an insoluble core is to increase the
denoted by the critical radius, rc, Using the sim- critical supersaturation required for activation.
plified Kőhler curve expression, the analytical Cloud nuclei can comprise more complex compo-
solutions for the critical quantities are: sition compared to the above cases which will
rffiffiffiffiffiffi  12 require modifications to the Kőhler expression.
3B 4A3 For example, nuclei can contain limited solubility
rc ¼ Sc ¼
A 27B components, immiscible liquid phases, and
surface-active components. In the latter case,
nuclei containing surface active components
For an increasing environmental value of which alter the droplet surface tension (i.e., reduce
S below Sc, there is a unique equilibrium droplet surface tension) will have a reduced contribution
size. Once the droplet grows beyond its critical from the Kelvin term in the Kőhler equation and
size (i.e., as the environmental S increases above consequently will require a lower critical super-
Sc), the droplet will exhibit unimpeded growth saturation for activation. However, critical
262 Aerosol in Global Atmosphere

0.06
Sc
Kelvin term
Raoult term
(S−1)

0.04 Total
Supersaturation % = 100

0.02

−0.02.

rc
−0.04

10−1 100 101 102


wet droplet radius, r,μm

1.005

1.004

1.003

1.002
Saturation Ratio

1.001

0.99 50 nm (NH4)2SO4
50 nm NaCl
0.98 100 nm (NH4)2SO4
100 nm NaCl
0.97 200 nm (NH4)2SO4
200 nm NaCl
200 nm (NH4)2SO4, 50% insol
0.96
200 nm NaCl, 50% insol

0.95
10−1 100 101 102
Droplet Diameter μm

Aerosol in Global Atmosphere, Fig. 13 Top: The Kőh- ((NH4)2SO4 – solid, NaCl – dashed) particles (red, green
ler equation can be envisaged as the competition between and blue curves) and for 200 nm particles containing 50%
the curvature (Kelvin) and solute (Raoult) terms. Bottom: by mass insoluble core (magenta). (Copyright European
Activation curves for a range of dry diameter of salt Geophysical Union 2006. Reprinted from [73])
Aerosol in Global Atmosphere 263

supersaturation is not always decreased since the effect where radiative forcing is defined as “The
surfactant may not dissociate into as many ions radiative forcing of the surface-troposphere sys-
and while the Kelvin term may be reduced, so may tem due to the perturbation in or the introduction
the Raoult effect to an even greater amount. This of an agent (say, a change in greenhouse gas
effect for an ammonium sulfate nuclei (which concentrations) is the change in net (down minus
dissociates into three ions) enriched with 30% up) irradiance (solar plus longwave in Wm–2) at
mass fraction by the surfactant stearic acid the tropopause after allowing for stratospheric
(single ion) is that the critical supersaturation is temperatures to readjust to radiative equilibrium,
actually increased. Supersaturations in natural but with surface and tropospheric temperatures
clouds are of the order of 0.1–0.5% for stratiform and state held fixed at the unperturbed values.”
clouds and below 1% for most convective clouds. In simple terms, it is “the rate of energy change per
This provides a lower limit to the size of particles unit area of the globe as measured at the top of the
that can act as cloud nuclei, namely, 30–50 nm, atmosphere” and often it refers to the change since
but more commonly, aerosols larger than 100 nm preindustrial conditions (year 1750). Radiative
provide the majority of cloud nuclei. Nitric acid forcing affects the climate, while alterations in
can also influence cloud nucleus activation in that aerosol availability and radiative forcing can
it can temporarily partition into the aerosol phase affect precipitation.
as a nucleus takes up water vapor in the rising
humidity field below cloud base. The uptake of Direct Effect
nitric acid into the solution droplet increases the Rayleigh scattering describes the irradiance
solute mass and, as a result, lowers the critical scattered by a sphere as small compared to the
supersaturation required for the nucleus. incident wavelength and proportional to 1/l4,
Ice nuclei are also important cloud nuclei but while Rayleigh absorption is proportional to 1/l4
produce cloud particles in a very different manner [75]. When particles are comparable to the inci-
and are comprised of very different chemical com- dent wavelength, Mie scattering must be invoked
position. Typically, they comprise non-water- where scattering is strongly dependent on particle
soluble matter such as mineral dust and certain size, shape, composition (via refractive index),
primary biogenic aerosol particles. Ice particles and orientation relative to the incident radiation.
are formed either by heterogeneous nucleation in For particles large relative to the wavelength, the
a supersaturated (with respect to ice) environment extinction efficiency converges at 2 (the extinc-
or homogeneous freezing of supercooled liquid tion paradox where twice the energy is removed
droplets [74]. Far less is known about the nature compared to that derived using geometrical
of ice nuclei than what is known about cloud optics). For particles with a complex refractive
condensation nuclei. index, some fraction of the incident radiation is
absorbed. The extinction efficiency is defined as
the sum of the scattering and absorption efficiency
Aerosols, Global Radiative Budget, and the single scattering albedo (o) is the ratio of
Precipitation, and Climate the scattering coefficient to the extinction coeffi-
cient. One parameter used to quantify scattering
Aerosols affect the global radiative budget, and extinction is the mass scattering and mass absorp-
hence the global climate, directly through the tion efficiency, which quantifies scattering and
scattering and/or absorption of incoming solar extinction in terms of the aerosol mass distribu-
radiation (and for some aerosol species generally tion function. Both the mass scattering and mass
of supermicron size, outgoing infrared radiation) absorption efficiencies as a function of particle
and indirectly through the modification of cloud size exhibit peak scattering and absorption effi-
microphysics and radiative properties. The former ciencies at sizes between 0.1 and 1 mm for typical
effect is called the direct aerosol radiative forcing atmospheric aerosol chemical compositions
effect and the latter, the indirect radiative forcing pointing to this size range as being the most
264 Aerosol in Global Atmosphere

important size range for aerosol optical properties. over Antarctica. Black carbon is seen to contribute
Efficient aerosol scattering types are sulfates and 0.0036 to the global AOD, with hot spots over
sea-salt, while efficient absorption types are black Europe and China where black carbon contributes
carbon and dust constituents such as hematite. 0.05 to AOD. Dust contributes 0.025 to global
One of the more important parameters associ- AOD with peak contributions of 0.3 arising over
ated with the direct radiative effect is aerosol Northwest Africa, and 0.2 of Asia. Particulate
optical depth (AOD) which describes the extinc- Organic Matter contributes 0.017 to global
tion of radiation as it propagates through the AOD, with hot spots in midwest Africa (from
atmosphere: biomass burning), South America, some regions
in Europe and China contributing AOD greater
I=I 0 ¼ et than 2. Sulfate contributes 0.032 to the global
AOD, with Europe, east Asia, and east USA con-
and tributing to hot spots with AOD about 0.3. Sea-
salt contributes 0.033 to the global AOD, with
t ¼ sext H, values up to 0.2 seen in some oceanic regions
were wind speeds are generally high (i.e.,
where sext is the extinction coefficient of radiation midlatitudes).
propagating through an aerosol layer of height H. The AEROCOM models predict [76] that, for
In terms of radiative forcing, an aerosol layer anthropogenic aerosols, a harmonized estimate
can either cause a negative or positive sign change for the aerosol direct radiative forcing under all-
to planetary albedo, leading to a cooling or sky conditions, on a global annual basis, is
warming effect. o is the key parameter, along 0.22 Wm2, ranging from +0.04 to
with the albedo of the underlying surface, that 0.41 Wm2, with a standard deviation of
determines whether an aerosol layer leads to 0.16 Wm2. Anthropogenic nitrate, secondary
heating or cooling. Over dark surfaces like the organic aerosol, and dust were not, however,
ocean, and regardless of the degree of absorption, included in the estimate. By comparison, the
albedo will be increased primarily due to the IPCC AR4 [100] reported a direct aerosol radia-
upscatter of incoming radiation. In contrast, over tive effect best estimate of 0.5 W m2 with an
bright surfaces such as snow and desert surfaces, uncertainty of 0.9 to 0.1 W m2. The global
an absorbing component will reduce the amount annual mean aerosol surface radiative forcing is
of surface-reflected radiation radiated back out to illustrated in Fig. 15 where it can be seen in the
space. An additional important factor related to regions with highest aerosol loadings, negative
absorbing aerosol layers is that they warm as they forcings as high as 10 W m2 are encountered.
absorb radiation, leading to increased atmospheric More recent estimates, using a combination of
stability and reduced convection. This effect, it satellite data with a global model [77] suggested
will be seen later, can have important implications a value of 0.65 W m2. The diversity in model
for cloud formation. estimates stems more from different model
The global distribution of AOD for total aero- approaches to transport processes, removal mech-
sol types and individually for black carbon, par- anisms, and microphysics treatment rather than
ticulate organic carbon, sulfate, dust, and sea-salt aerosol emission inventories.
is shown in Fig. 14. The global average AOD,
derived from the medium of the 10 AEROCOM Indirect Effect
models, is0.12 (compared to 0.137 derived from There are a number of indirect aerosol radiative
satellites and sunphotometers) [57]. Peak AOD effects whereby aerosol fields modify the cloud
values of >0.6 are encountered over Northwest microphysics, structure, or lifetime, all of which
Africa and the Asian continent, and to a lesser have albedo impacts. The first indirect effect
degree, over Europe, the USA, and South Amer- (typically associated with “warm” or water clouds
ica. The lowest AOD values of ~0.01–0.02 occur of fixed liquid water content), results from an
Aerosol in Global Atmosphere 265

AEROCOM_MEDIAN Mean: 1.18189E–01 AEROCOM_MEDIAN Mean: 3.61807E–03


90 90
0.90 0.3000
0.80
0.2000
0.70
45 45 0.1000
0.60
0.50 0.0750
0.40
Latitude

Latitude
0.0500
0 0.30 0
0.0250
0.20
0.10 0.0100
0.08 0.0050
−45 −45
0.06
0.0025
0.04
0.02 0.0010

0.00 0.0000
−180 −120 −60 0 60 120 180 −180 −120 −60 0 60 120 180
Longitude Longitude
Total Aerosol Black Carbon

AEROCOM_MEDIAN Mean: 2.45290E–02 AEROCOM_MEDIAN Mean: 1.72301E–02


90 90
0.3000 0.3000

0.2000 0.2000
45 0.1000 45 0.1000

0.0750 0.0750
Latitude

Latitude

0.0500 0.0500
0 0
0.0250 0.0250

0.0100 0.0100

0.0050 0.0050
−45 −45
0.0025 0.0025

0.0010 0.0010

0.0000 0.0000
−180 −120 −60 0 60 120 180 −180 −120 −60 0 60 120 180
Longitude Longitude
Dust Par ticulate Organic Matter

AEROCOM_MEDIAN Mean: 3.18976E–02 AEROCOM_MEDIAN Mean: 3.27001E–02


90 90
0.3000 0.3000

0.2000 0.2000
45 0.1000 45 0.1000

0.0750 0.0750
Latitude

Latitude

0.0500 0.0500
0 0
0.0250 0.0250

0.0100 0.0100

0.0050 0.0050
−45 −45
0.0025 0.0025

0.0010 0.0010

0.0000 0.0000
−180 −120 −60 0 60 120 180 −180 −120 −60 0 60 120 180
Longitude Longitude
Non-sea-salt Sulphate Sea-Salt

Aerosol in Global Atmosphere, Fig. 14 Median global (Copyright European Geophysical Union 2006. Reprinted
distribution of aerosol AOD, total and per aerosol species, from [57])
derived from 10 AEROCOM models for the year 2000.

increase in cloud condensation nuclei leading to a droplets, and the increased scattering associated
higher number of smaller cloud droplets which with smaller droplets, leads to an albedo increase
ultimately, through an increase in number of [72, 74]. Figure 16 illustrates this effect. A cloud
266 Aerosol in Global Atmosphere

90 W m−2
5.0
4.0
60 3.0
2.0
1.0
30 0.5
0.2
Latitude

0.0
0 −0.2
−0.5
−1.0
−30
−2.0
−3.0
−4.0
−60
−5.0
−10.0
−90 <
−180 −135 −90 −45 0 45 90 135 180
Longitude

Aerosol in Global Atmosphere, Fig. 15 Aerosols in the Global AtmosphereGlobal annual mean aerosol surface
radiative forcing from AEROCOM models. (Copyright European Geophysical Union 2006. Reprinted from [76])
altitude

altitude

re re

N N

clean polluted

droplet concentration droplet concentration


effective radius effective radius

Aerosol in Global Atmosphere, Fig. 16 Illustration of is thus smaller and smaller droplets are more efficient
changes in cloud microphysics resulting from low (clean) scatters of visible radiation. This, combined with an
and high (polluted) aerosol fields. Fora cloud with the same increase in the number of scattering droplets, results in a
available liquid water content. With more cloud nuclei more reflective cloud. (Courtesy L. Schuller and
available for droplets to form on, the resulting droplets J.L. Brenguier)
are necessarily smaller in size. The cloud’s effective radius
Aerosol in Global Atmosphere 267

is generally formed by rising air parcels which


eventually become supersaturated. Cloud droplets
are activated at cloud base and continue to grow as
the air parcel containing the droplets rise to the top
of cloud. Even for a fixed number of droplets,
their size and liquid water content increases with
increasing height into the cloud. A parameter used
to describe an effective radius in such a changing
field is the cloud drop effective radius defined as
the weighted mean of the size distribution of the
cloud droplets. This amounts to the ratio of the
volumetric distribution to the surface area distri-
bution – or the ratio of the third moment of the
distribution to the second moment. Take the two
cases of clouds forming under the same environ-
Aerosol in Global Atmosphere, Fig. 17 AVHRR sat-
mental conditions (and hence the same available ellite image of a stratocumulus cloud deck off the US
liquid water content), but under different aerosol Washington coast. The tracks are ship tracks produced by
fields, one clean containing a low number of cloud ship stack emissions mixing into cloud, resulting in an
nuclei, and the other polluted, containing a high increase in cloud droplet concentration and reflectance
number of cloud nuclei. The same amount of
liquid water has to be shared out to different nuclei persistent and extensive stratocumulus cloud
concentrations entering into cloud base. The result decks occur. It is in these regions that the radiative
is that the clean cloud with a low nuclei and forcing associated with the indirect effect is at its
droplet concentration (N ~ 50 cm3) leads to a maximum.
relatively large effective radius (of the order of The second indirect effect relates to the cloud
15 mm), while the polluted cloud with high nuclei lifetime effect [78], and relates to a suppression of
and droplet concentration (N ~ 300 cm3) leads to precipitation due to the smaller mean droplet
a relatively low effect radius (of the order of sizes. The smaller drops have reduced collision-
5 mm). The net effect is a higher cloud albedo coalescence efficiency and as a result the onset of
seen at cloud top. An excellent example of this precipitation can be delayed or even shut down.
effect is seen in Fig. 17, which displays a satellite Given that precipitation is one important process
image of a Pacific Ocean stratocumulus cloud in shortening the lifetime of a cloud, lack of pre-
deck off the west US coast. Seen within the cipitation can increase cloud lifetime and at times,
cloud deck are numerous tracks more visible vertical and horizontal extent. Longer lifetimes or
than the background cloud. These tracks are greater extent of clouds effectively increases the
called ship tracks and result from ship stack emis- albedo since cloud optical depth is always greater
sions, rich in cloud nuclei, rising into cloud and than aerosol optical depth.
modifying cloud microphysics as described The semi-indirect effect results from aerosol
above. These tracks are easily visible since the with a significant absorbing component, which
tracks have produced regions of increased reflec- heats the atmospheric layer in which the absorb-
tance relative to the “clean” regions of the cloud. ing aerosol resides [79]. This can inhibit cloud
While ship tracks do not necessarily have a cli- formation by reducing stability and reducing rel-
mate impact, they are excellent illustrative exam- ative humidity through increasing the layer tem-
ples of the first indirect aerosol effect. perature and reducing surface water vapor
The first indirect effect is particularly impor- evaporation. It can also lead to increased evapo-
tant over oceans (where surface albedo is low and ration rates for existing clouds. The sign of the
clouds are very susceptible to changes in aerosol effect is, however, a matter of debate. Some stud-
or nuclei availability) and in regions where ies [80] support the warming effect of absorbing
268 Aerosol in Global Atmosphere

aerosols through decreased low-level cloud cover colder temperatures (T < 0  C). Through the
and other studies found that cooling effects delay of precipitation, the additional latent heat
through increased cloud coverage [81, 82]. The release invigorates the cloud. In addition, by not
height of the absorbing layer seems to impact on raining early, the condensed water can form ice
the sign of the effect. precipitation particles that release the latent heat
Other effects include the cloud glaciation effect of freezing aloft and these reabsorb heat at lower
where an increase in anthropogenic ice nuclei can levels where they melt after falling [88]. This
lead to an increase in cloud glaciation [83], the process leads to consumption of more convective
deactivation effect where anthropogenic sulfate available potential energy (CAPE) which would
coats ice nuclei making them inactive [84], and then be converted to an equally greater amount of
the thermodynamic effect where smaller droplets released kinetic energy that could invigorate con-
freeze less efficiently than larger droplets [85]. vection and lead to a greater convective over-
From the IPCC AR4, the most recent consen- turning, more precipitation, and deeper depletion
sus on the first indirect effect of warm clouds [86] of the static instability.
estimated a range between 0.22 and The increased amount of aerosol has two com-
1.85 W m2, with a best estimate of peting effects: one radiative, which suppresses
0.7 W m2. The combined first and second convection (and consequently rainfall) through
indirect effect was estimated to have a radiative absorption and warming of atmospheric layers
forcing between 0.2 and 2.3 W m2, illustrat- relative to the surface, and the other, which can
ing the difficulties in achieving convergence of lead to invigoration of updrafts, leading to an
these models as the level of complexity increases. increase in precipitation. These two processes
have typically been treated separately leading to
Aerosol–Cloud–Precipitation Interactions opposing views on the impact of aerosols on pre-
Although the second indirect effect, through cipitation. This competing effect was elucidated
changes in cloud microphysics, has been demon- recently [89] by looking at the combined effect of
strated to reduce precipitation with increased increasing aerosol and cloud condensation nuclei
anthropogenic aerosol, this effect typically applies concentrations on both microphysical and radia-
to warm stratiform clouds and shallow cumulus tive properties. They modeled typical warm trop-
clouds. Similarly, the radiative effects generally ical convective clouds and found that the
act to suppress precipitation through decreasing microphysical invigoration effect was at a maxi-
the amount of solar radiation reaching the surface mum for moderate cloud condensation nuclei con-
thereby reducing the amount of energy available centrations, above which the impact of additional
to evaporate water and energize convective nuclei was reduced. However, as the cloud con-
clouds. The radiation not reflected back to space densation nuclei concentrations were linearly cor-
is partly absorbed in the atmosphere in the pres- related to AOD, AOD progressively increased
ence of absorbing carbonaceous aerosol leading to with increasing cloud condensation nuclei con-
a warming of the air above the surface. This centrations which reduced the solar flux which in
warming stabilizes the lower atmosphere and sup- turn energized convection reaching the surface.
presses convection and the generation of convec- As a result, with increasing aerosol loads beyond
tive clouds. the optimum, the weakening of the microphysical
Some studies have also shown [87] that invigoration is reinforced by the suppressive
increases in cloud nuclei can invigorate deep con- effect of reduced surface heating. This conceptual
vective rain clouds with warm cloud bases model is illustrated in Fig. 18 where it is seen that
(T > 15  C). In such clouds, the auto-conversion starting out with clean (low) nuclei concentrations
processes (coalescence of droplets into raindrop (N ~ 100 cm3), the addition of more nuclei has
sizes) are delayed and hence the onset of precip- the effect of increasing the released convective
itation in the cloud is also delayed. This results in energy up to a maximum point corresponding to
more water ascending to higher altitudes and a cloud condensation nuclei concentration of the
Aerosol in Global Atmosphere 269

Transmission
CAPE
AOT

1
1000
Released convective energy 0.8

Aerosol optical thickness


Aerosol transmission
500
0.6
(J kg-1)

0
0.4

−500
0.2

−1000 0
100 1000 10,000
CCN0.4 aerosol concentration (cm-3)

Aerosol in Global Atmosphere, Fig. 18 Illustration of tropopause. Note that a maximum in CAPE occurs at
the relations between the aerosol microphysical and radia- CCN0.4 1,200 cm3, which corresponds to the maxi-
tive effects. The aerosol optical (dept) thickness (AOT) is mum cloud invigoration. The AOT corresponding to the
assumed to reach 1 at CCN0.4 ¼ 104 cm3 (dashed red CCN0.4at the microphysical optimum is only 0.25. Adding
line), which corresponds to nucleation of 2,000 cloud aerosols beyond this point substantially decreases the vigor
drops cm3. The related transmission of radiation reaching of the cloud because both microphysical and radiative
the surface is shown by the solid red line. The vigor of the effects work in the same direction: smaller release of con-
convection is shown by the blue line, which provides the vective energy aloft and less radiative heating at the sur-
released convective available potential energy (CAPE) of a face. (Reprinted from [89])
cloud parcel that ascends to the cloud top near the

order of 1200 cm3. At this point, AOD is a greenhouse gases. This suggests that aerosols,
moderate 0.25. Further increases in cloud conden- perhaps, have been masking the true rate of
sation nuclei result in a reduction of released global warming, or the climate-temperature sen-
convective energy with CAPE dropping rapidly sitivity to CO2-induced global warming. Over
at concentrations over 5,000 cm3, but AOD con- the past 40 years, there has been both observed
tinues to rise, reaching 1 for extreme nuclei con- dimming and brightening trends that point to a
centrations of 10,000 cm3 (corresponding to direct aerosol influence on climate. Global dim-
2,000 cm3 cloud droplets. The slope of the ming is a term associated with a decadal decrease
CAPE curve represents the effect of aerosols on in surface solar radiation, while global brighten-
precipitation. For increasing CAPE release with ing refers to an increase in surface solar radiation.
increasing aerosol concentrations, an increase in Studies [90–92] have shown a widespread
precipitation is expected. This trend reverses for decrease in surface solar radiation at a variety
moderate levels of aerosol pollution, above which of locations worldwide between 1960 and 1990.
suppression of precipitation is associated with Increasing aerosol concentrations associated
increasing aerosol concentrations. with increased air pollution over the period are
considered responsible for the dimming
Aerosol–Climate Interactions [93]. Changes in cloud reflectance and cloud
The IPCC AR4 concluded that the combined amount contribute to the dimming [90]; however,
aerosol radiative forcing was negative and partly in a particular study over Europe [94], it was
offset the warming, or positive forcing, by concluded that cloud amount could not explain
270 Aerosol in Global Atmosphere

Mainland Europe
2.0

T diff 1961–1990 (°C)


+0.19 [+0.09 to +0.29] °C dec−1
1.0

0.0

−1.0
−0.07 [−0.29 to +0.15] +0.38 [+0.06 to +0.70]

1950 1960 1970 1980 1990 2000

Aerosol in Global Atmosphere, Fig. 19 Temperature trends with 95% confidence interval show the temperature
rise over mainland Europe since 1950. Annual temperature decline from 1950 to 1980 (green), and the temperature rise
differences for the period 1950–2005 with respect to the to be twice as large for the period 1981–2005 (blue) than
1961–1990 climatological mean for mainland Europe for the whole period 1950–2005 (red). (Copyright Ameri-
(45_–55_N; 5_–15_E). Linear regression lines and decadal can Geophysical Union 2009. Reprinted from [96])

the dimming and that the aerosol direct and indi- quality is regulated in terms of exposure to a partic-
rect effect was the predominant cause for the ular PM standard. Air pollution has been a serious
trend. The period from 1990 to the present problem since the eighteenth century with the inven-
shows a reversal of the trend into a brightening tion of the steam engine which increased the amount
trend [95]. The dimming effect appeared to have of coal burning. Prior to that, air pollution was still a
been masking, or suppressing, greenhouse problem due to wood and coal burning although not
warming with reduced or even negative trends as severe. In 1905, the term “smog” was coined and
on global temperatures over the period as green- it described the combination of smoke and fog that
house gases continued to accumulate. As the was visible in many industrialized cities. London
trend reversed from dimming to brightening, experienced the most frequent and severe smog
rapid temperature rises became evident since events resulting in many “excess” deaths. The
the mid-1980s. Since the mid-1980s, the decadal worst of these occurred in December 1952 when
rise in temperature has been +0.38  C per decade there were 4,000 excess deaths during the London-
(Fig. 19), significantly higher than any other type event. During this period, smoke mass concen-
period since the preindustrial era [96]. The trations reached 4,460 mg m3. This is to be com-
brightening has been associated with reduced pared with a current EU yearly exposure of
aerosol pollution since the 1980s as developed 25 mg m3 for PM2.5 and 50 mg m3 sustained
countries implemented policies to clean up air over 24 h 35 times in 1 year for PM10. The events
pollution. typically occur in winter and during high pressure
weather systems.
High pressure systems generally are accompa-
Aerosols and Air Pollution nied by colder temperatures resulting in increased
coal burning. In addition to the colder tempera-
Aerosol is one atmospheric constituent regarded as tures are stable atmospheric boundary layers,
an air pollutant. In Air Quality communities, aerosol which suppress the dispersion of pollution. Fur-
particles are termed particulate matter (PM). Aerosol ther exasperating the situation are very stable
air pollution is typically measured as the total mass surface-mixing layers 100–200 m deep, which
less than a particular cutoff size (e.g., 10 mm for trap the pollution and confine the pollution to a
PM10, 2.5 mm for PM2.5, and 1 mm for PM1). Air thick layer close to the ground.
Aerosol in Global Atmosphere 271

In addition to the London-type smog, there is a greenhouse gases to an equivalent amount. The
chemically produced smog known as photochemical IPCC estimate the net forcing due to anthropogenic
smog. Photochemical smog is produced through gas activities as ~+1.5 W m2. This positive forcing has
phase reactions typically involving hydrocarbons, led to a global temperature increase of the order of
NO, and ozone and is a frequent phenomenon 0.8  C. The European Union, leading the way in
encountered in many megacities such as Los climate policy development, have set a long-term
Angeles, Mexico City, Tokyo, Beijing, Johannes- (i.e., by year 2050) target of an upper limit of 2  C to
burg, and Athens. the increase in global temperature.
The main health impacts of PM relate to respi- Until recent times, climate policy has been han-
ratory and cardiovascular effects and, addition- dled separately to air pollution problems, where in
ally, some of the smoke products are considered the latter case, adverse health effects from PM and
carcinogenic, all potentially resulting in prema- ecosystem damage have been the biggest drivers of
ture mortality. The European Union’s Clean Air policies to improve air quality. What has become
for Europe Programme estimated that 348,000 evident is that the air pollution policies in recent
premature deaths occur in Europe due to expo- decades have impacted on global warming in a
sure to PM2.5. Figure 20 illustrates the estimated manner that has accelerated temperature rise as
losses in life expectancy attributable to exposure dirty air was cleaned up. The current decadal rate
to PM2.5 from anthropogenic emissions in of temperature increase is estimated to be
Europe [97]. The data are calculated for emis- 0.3–0.4  C per decade. As a result, by the year
sions for the year 2000 and for targeted emission 2030, the predicted temperature increase is
reductions by the year 2020. ~1.9  C – that is, almost reaching the long-term
While air pollution, particularly aerosol air target limit. Figure 22 illustrates the problem
pollution, has been steadily reducing in the devel- [99]. If there were only long-lived greenhouse
oped world, it has become an increasing problem gases (LLGHG), the past temperature increase
in developing countries, not only on urban mega- would have been approximately double the actual
city scales but also on regional and almost hemi- increase since the preindustrial era. Without emis-
spheric scales. Intercontinental and hemispheric sion reductions, looking into the future, tempera-
transport of pollution is now regarded as a serious ture will increase by about 0.2  C per decade.
concern, impacting on local- and regional-scale However, taking account of the presence of aero-
air quality. sols, the approximate 50% masking of temperature
increase is evident up until the 1990s and then the
current day and near future rapid rise in tempera-
ture from aerosol emission controls is evident,
Future Directions: Interactions Between rapidly approaching the increase seen by treating
Aerosol Air Pollution and Climate the system as only containing LLGHG. With both
a reduction on aerosol emissions and LLGHG,
Atmospheric aerosol has played an important role in only then can the dual target of clean air and
partly offsetting global warming due to greenhouse minimal temperature rise be achieved. Such com-
gases. The IPCC AR4 quantifies the best atmo- bined policy development, while in the near term
spheric composition component estimates of radia- will accelerate temperature rise, in the long term, a
tive forcing since 1750–2005 (Fig. 21). From this sustainable temperature rise can be expected.
assessment, the combined direct and indirect effect The development of sophisticated policy devel-
amounts to ~1.2 W m2, which effectively can be opment is underpinned by the development of
regarded as a reduction in the positive forcing by sophisticated climate and air pollution assessment
272

0 .. 1 month 0 .. 1 month
1 .. 2 1 .. 2
2 .. 4 2 .. 4
4 .. 6 4 .. 6
6 .. 9 6 .. 9
9 .. 12 9 .. 12
12 .. 12 ..

Aerosol in Global Atmosphere, Fig. 20 Estimated loss in life expectancy attributable to exposure to fine particulate matter (PM2.5) from anthropogenic emissions for the year
2000 (left) and projected reduced emissions for the year 2020 (right). (Modified from EEA Report No2/2007. Courtesy of Zbigniew Klimont and Markus Amann)
Aerosol in Global Atmosphere
Aerosol in Global Atmosphere 273

Radiative forcing of climate between 1750 and 2005


Radiative Forcing Terms

CO2
Long-lived
N2O
greenhouse gases
CH4

Halocarbons
Ozone Stratospheric Tropospheric
(−0.05)
Human activities

Stratospheric
water vapour

Surface albedo Land use Black carbon


on snow

Direct effect
Total
Aerosol Cloud albedo
effect

Linear contrails (0.01)


processes
Natural

Solar irradiance

Total net
human activities

−2 −1 0 1 2
Radiative Forcing (watts per square metre)

Aerosol in Global Atmosphere, Fig. 21 Summary of water vapor, surface albedo, aerosols, and contrails. The
the principal components of the radiative forcing of climate only increase in natural forcing of any significance
change. All these radiative forcings result from one or between 1750 and 2005 occurred in solar irradiance. Pos-
more factors that affect climate and are associated with itive forcings lead to warming of climate and negative
human activities or natural processes as discussed in the forcings lead to a cooling. The thin black line attached to
text. The values represent the forcings in 2005 relative to each colored bar represents the range of uncertainty for the
the start of the industrial era (about 1750). Human activi- respective value. (Reprinted from the Intergovernmental
ties cause significant changes in long-lived gases, ozone, Panel on Climate Change Assessment Report 4)

models. Current climate models do not possess global-scale radiative impacts and interactions
treatments of aerosol emissions, formation, trans- with clouds will remain for some time. Neverthe-
formations, and radiative effects to a high enough less, the advances in recent years have been
level of sophistication yet. This limitation results immense, most notably in the current day improved
from the aerosol life cycle being one of the understanding of the highly complex nucleation
most complex systems to model and the challenges processes and in the characterization of organic
of modeling the formation of nanoclusters to aerosols, their properties, and their life cycle.
274 Aerosol in Global Atmosphere

Imagine: only LLGHG present in the atmosphere


without LLGHG emission reductions
with LLGHG emission reductions

global mean temperature

de
ca
In reality: LLGHG and air pollutants present

/de
only aerosol reduction

°C
LLGHG and aerosol reduction

.4
–0
0.3
pre-
1940s 1980s 2030s >2100
industrial

Aerosol in Global Atmosphere, Fig. 22 The figure on global warming. Air pollutants have lifetimes of weeks
shows schematically the climate consequences of climate to months, and the climate system would realize, in about
change and air pollution abatement strategies. The only 5 years, 50% of the global warming caused by their reduc-
way to reach global temperature stabilization is through tion [98]. Air pollutant reductions are expected to acceler-
LLGHG reductions. Such stabilization would be achieved ate the increase in global mean temperature in the short
according to the timescales mainly related to the several term (<30 years), on the way to eventual long-term
decade lifetime of LLGHG in the atmosphere. Reduction (>100 years) climate stabilization. (Copyright Elsevier
of air pollution (including that resulting from LLGHG 2009. Reprinted from [99])
emission reductions) would have a more immediate impact

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Glossary
Air Pollution and Climate
Change: Sustainability, Adaptation An adaptation is an adjustment made
Restoration, and Ethical in response to an actual or expected climate that
Implications moderates or avoids harmful impacts. Adapta-
tion can be divided into incremental and trans-
Jiaying Chen1, Mie Jul Dahlin1, Linnea Luuppala2, formational actions. Incremental adaptation
David Bickford3, Lina Boljka4, Vanessa Burns5 refers to relatively small changes and actions
and Matthew Stanley Johnson1,6 that affect a system while maintaining its integ-
1
Department of Chemistry, University of rity, while transformational adaptation includes
Copenhagen, Copenhagen, Denmark changes and actions that affect the fundamental
2
Social and Moral Philosophy, Department of attributes of a system [10].
Political and Economic Studies, University of Air Pollution Air pollution is “a mix of particles
Helsinki, Helsinki, Finland and gases that can reach harmful concentra-
3
Biology Department, University of La Verne, La tions both outside and indoors” [12]. Determin-
Verne, CA, USA ing the harmfulness of substances is not always
4
Department of Atmospheric Science, Colorado straightforward. For example, some substances
State University, Fort Collins, CO, USA that are toxic have been found to have benefi-
5
School of Geography and the Environment, cial effects in low quantities [13], while for
University of Oxford, Oxford, UK others there may be no safe dose. A pertinent
6
Airlabs, Copenhagen, Denmark example is that carbon dioxide is a natural part
of the atmosphere and is exchanged with the
biosphere via photosynthesis thus fertilizing
Article Outline plants but clearly there could be too much of
a good thing, as excessive amounts of CO2
Glossary have a clear negative impact on the biosphere
Definition through climate change. Plants require fixed
Introduction nitrogen, and some is produced naturally by
Atmospheric Chemistry: The Physical Origin of lightning, depositing to the surface as nitrate
Climate Change from nitric acid, one cause of acid rain [5]. In
Observations of Climate Change small amounts it is a good thing and clearly
Sustainability and Climate Change damaging in large amounts. Thus the classifi-
Environmental Management and Climate Change cation of a given substance as pollution
Ecological Restoration depends on context.
Mitigation and Adaptation Biosphere The biosphere is the global aggregate
Mitigation of all ecological systems including all living
Carbon Capture and Storage (CCS) beings and their interrelationships with each
Adaptation other and with the atmosphere, geosphere,
Ethics and Philosophy of Climate Change hydrosphere, and lithosphere.
Conclusion Conference of the Parties (COP) The United
Future Directions Nations Framework Convention on Climate
Bibliography Change (UNFCCC) is an international treaty
signed and put into action in 1994. The con-
Jiaying Chen, Mie Jul Dahlin and Linnea Luuppala vention’s principle goal is to prevent negative
contributed equally with all other contributors. impacts to society from anthropogenic climate
© Springer Science+Business Media, LLC, part of Springer Nature 2021 279
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_1082
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2020, https://doi.org/10.1007/978-1-4939-2493-6_1082-1
280 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

change. It implements greenhouse gas emis- Preservation A conservation strategy that attempts
sion limits but has no enforcement capacity. to protect nonhuman species including their
The Conference of the Parties (COP) consists habitats.
of countries that are part of the United Nations Resilience Resilience is the capacity of social,
Framework Convention. The COP is the supreme economic, and environmental systems to
decision-making body in the Convention. respond to hazardous events, trends, or distur-
Climate Hazards According to the 2014 Intergov- bances from climate change [10].
ernmental Panel on Climate Change (IPCC) Thermohaline Circulation Ocean circulation,
report, climate hazards are “climate-related phys- and especially the deepwater formation that
ical events or trends or their physical impacts” sequesters dissolved inorganic carbon (DIC)
[3]. Climate hazards are different from natural from the surface ocean, is driven by density.
hazards, which include earthquakes, pandemics, The density of seawater is controlled by its tem-
and weather-related disasters. Weather-related perature (“thermo-”) and its salinity (“haline,”
disasters include drought, wildfires, floods, trop- which refers to mineral sodium chloride called
ical cyclones, and severe storms [10]. halite). Salinity can be defined as a mass fraction,
Ecological Restoration “Ecological restoration grams of dissolved salts per kg seawater [5]. Sea-
is the process of assisting the recovery of an water is typically around 35 g/kg, and values can
ecosystem that has been degraded, damaged, range from rainwater, ca. 20 mg/kg, to the Dead
or destroyed” [64]. Sea, >200 g/kg. The amount of salt in the oceans
Ecological Justice Considerations of justice that is fixed; thus, salinity can only be changed by
relate to human relationships with other spe- removal or addition of freshwater, such as by
cies and ecosystems. evaporation or addition of glacial meltwater [5].
Environmental Ethics A branch of philosophy Vulnerability In the context of climate change,
that studies human interaction with the natural vulnerability is the inability of social, eco-
world including the moral relationship nomic, and environmental systems to persist
between humans and natural entities including and thrive in a changed environment, including
the moral status of such entities. “sensitivity or susceptibility to harm and lack
Exposure In the context of climate change, of capacity to cope and adapt” [4]. The assess-
exposure is additional risk and is defined as ment of vulnerability is a key element of
“the presence of people, livelihoods, species describing current and future climate risks
or ecosystems, environmental functions, ser- [10]. The main goal of climate change adapta-
vices, and resources, infrastructure, or eco- tion is to reduce vulnerability [19].
nomic, social, or cultural assets in places and
settings that could be adversely affected” [10].
Global Justice Considerations of justice that Definition
take collective human actions and relationships
into account on a global level. Climate change is a profound global-scale chal-
Intergenerational Justice Considerations of lenge to the sustainability of human society and
justice that reflect the moral relationship the biosphere. This entry introduces the key
between currently living people and future scientific research on climate change and its ethi-
generations. cal implications. It begins by summarizing the key
Mitigation Climate change mitigation comprises types of anthropogenic climate forcing agents
actions that limit anthropogenic climate change. including CO2, CH4, N2O, and air pollution
It includes reducing emissions of greenhouse including particulate matter (PM) and their
gases (GHGs). In the case of CO2, this includes sources. A combination of mitigation, restoration,
renewable energy, reforestation, land use changes, and adaptation strategies currently being
carbon capture and storage (CCS), and direct air considered is introduced and compared. Global
capture (DAC). climate change intersects with many academic
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 281

disciplines, and this entry attempts to provide a climate change in ethical terms? Can and should
holistic overview of the current observations of we attempt to restore environmental damage?
climate change based on scientific and ethical Current scientific evidence combined with eth-
considerations. Our analysis includes the atmo- ical arguments can yield a strong foundation for
sphere and hydrosphere, and the impacts of cli- change and guide us toward stronger actions and
mate change on society. The aim is to provide a strategies for dealing with climate change and
fuller account of climate change from perspective environmental restoration.
of disciplines not often seen together, thus provid-
ing a more comprehensive account of the most
defining problem of our time. Atmospheric Chemistry: The Physical
Origin of Climate Change

Climate is determined by flows of energy and


Introduction material within the Earth system; key factors are
radiation, flows of air and water, and evaporation
Climate change and air pollution are closely and condensation of water. Nearly all of the
linked; climate change is caused by air pollution, planet’s energy comes from our sun at a rate of
and climate change makes air pollution worse. Air 174,600 TW, which represents 99.977% of power
pollution from human society is the key factor from all sources. In comparison, tidal energy con-
currently driving climate change. As it is a signif- tributes only 3 TW, fossil fuel combustion 14 TW,
icant existential threat to society, climate change is and geothermal energy 23 TW [5]. The Earth sys-
not only the subject of intense scientific research, tem is in a state of dynamic equilibrium between
but it is also an important ethical issue. Ethics, and “shortwave” radiation, coming from the sun, mainly
in particular environmental ethics, is an important at visible wavelengths, and “longwave” radiation
tool to analyze the ethical implications and moral emitted from surface into space – mainly at infrared
acceptability of human actions. Despite the (IR) wavelengths. Our atmosphere is largely trans-
mounting evidence of the causes of climate parent to shortwave radiation, and roughly 30% of
change, environmental pollution, and their incoming sunlight is reflected back into space by
effects, action to tackle these issues has been clouds, ice, and the surface of the planet. The rest is
nominal, slowed down by myopic economic fac- absorbed at the surface and re-emitted as longwave
tors that dominate the discussions surrounding radiation [6, 7].
climate and environmental policy. It is clear to There are many gases in the atmosphere that
many that the economy is a subset of society that absorb and re-emit thermal radiation, hindering its
can only operate within the context of the bio- escape. Absorption and emission of infrared light
sphere and that in addition to threatening human are allowed if there is a change in the molecule’s
well-being and health, climate change threatens dipole moment for a given vibrational mode. Thus
global ecosystem functioning as we know it. many gases absorb infrared (IR) light, including
This entry is mainly concerned with the prob- water vapor (H2O), carbon dioxide (CO2), meth-
lems and ethical implications of climate change ane (CH4), nitrous oxide (N2O), dichlorodifluoro-
on the sustainability of human society. The methane (CCl2F2), and ozone (O3). Oxygen (O2)
attempt is to provide a preliminary roadmap of and nitrogen (N2) do not have a dipole moment
the main scientific research and ethical issues with and therefore do not absorb IR radiation. This
climate change and air pollution. The influence of means that our planet has always had a strong
economic development on climate change and the natural greenhouse effect due to the presence of
current status of the natural environment will be water vapor and carbon dioxide. An increase in
explored, driven by a number of key questions: the concentration of any “greenhouse gas” (one
What strategies can be used to mitigate climate that traps infrared heat radiation) causes an
change? Can we contextualize anthropogenic increased warming effect.
282 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

A change in the balance between ingoing and A kilogram of CO2 released into the atmo-
outgoing radiation is called a radiative forcing sphere produces a radiative forcing; a kilogram
(RF) [8]. Different atmospheric compounds affect of CH4 produces even more as it is more efficient
climate differently. The change of global average at absorbing infrared light. The cumulative radia-
surface temperature is dependent on the changes tive forcing of a given gas relative to CO2 is called
in radiative forcing with DT ¼ l DRF; l is the the global warming potential (GWP) and is
climate sensitivity parameter. Figure 1 shows defined for a specific length of time, the time
changes in radiative forcing in 2011 relative to horizon. The IPCC is currently using standards
1750 for the most important factors [10]. of 20, 100, and 500 years with the 100-year time
There are many anthropogenic radiative forc- horizon being implemented as the preferred stan-
ing agents, including greenhouse gases, land use dard since the Kyoto Protocol [9].
change, and aerosol particles. Some anthropo- The relative GWP is calculated using the fol-
genic changes have had a cooling effect on the lowing equation [14]:
climate system (i.e., a negative radiative forcing) Ð tf
aA ½AðtÞdt
partially offsetting warming, for example, GWP ¼ Ð0tf
injecting sulfate aerosols in the stratosphere 0 aR ½RðtÞdt
cools by increasing the scattering of shortwave
solar radiation [140] and by absorbing and emit- where tf is the time horizon, aA is the radiative
ting longwave radiation [118]. forcing resulting from a 1 kg increase of

Radiative forcing estimates in 2011 relative to 1750


2.5

1.5
Radiative forcing / W m-2

1
1.68

0.5 Aerosols
0.97 and
precursors Cloud Albedo change
adjustments due to
0.18 0.17 0.23 NOx due to aerosols land use
0 0.1
CO2 CH4 Halocarbons N2O CO NMVOC -0.155 -0.15
-0.27

-0.695
-0.5

-1

-1.5

Air Pollution and Climate Change: Sustainability, change [4]. Positive RF refers to the warming effects,
Restoration, and Ethical Implications, Fig. 1 Radia- while negative RF refers to the cooling effects caused by
tive forcing estimates in 2011 relative to 1750 and different driving factors, for example non-methane volatile
aggregated uncertainties for the main drivers of climate organic compounds (NMVOC)
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 283

compound A, [A(t)] is the time decay of a pulse of being whether the material is oxidized organic
a compound A, and aR and [R(t)] are the compa- material or elemental carbon, for example, poly-
rable quantities for the reference compound, the cyclic aromatic hydrocarbon soot [14].
accepted standard being CO2 [14]. PM changes the planetary energy balance, and
The GWP incorporates the different atmo- its effects can be either direct or indirect [11]. Direct
spheric lifetimes of different gases. For example, forcing is caused by the absorption and scattering
CH4 is removed relatively rapidly by the OH of light. PM with chromophores, for example,
radical giving it a lifetime of around a decade, black carbon, absorbs light to produce heat. Parti-
whereas N2O persists for a century. Therefore cles with transparent material like salts scatter light
the GWP of methane decreases from a 20- to a giving a cooling effect. When dark particles are
100-year time horizon (specifically from 86 to deposited on snow and ice surfaces, they reduce the
34), while nitrous oxide increases (268–298). albedo and cause a positive radiative forcing.
These particles accumulate on ice surfaces as the
Particulate Matter (PM) water deliquesces, leaving behind impurities.
Particulate matter (PM) is important for climate as Indirect forcing effects are caused by particles’
it plays a key role in cloud and fog formation as ability to function as cloud condensation nuclei
well as rainfall. PM impacts climate through the (CNN). High concentrations of CCN change the
radiative balance by scattering incoming solar distribution of droplet sizes within a cloud,
radiation; by changing the albedo or reflectivity shifting it toward smaller droplets. Light scatter-
of the planet; by absorbing sunlight, e.g., “black ing occurs because of a surface, and a cloud with
carbon” soot; and by absorbing outgoing infrared many small droplets has more surface area than a
heat radiation. In addition it serves as the basis of cloud with fewer, larger droplets, even though
cloud formation thus affecting the hydrological both may have the same liquid water content.
cycle. Sources of PM can be natural or anthropo- Thus, paradoxically, clouds in a polluted atmo-
genic; sea spray is the most important natural sphere are whiter and result in additional cooling.
source. Anthropogenic PM has increased signifi- In addition smaller droplets have a smaller depo-
cantly since industrialization due to combustion sition velocity and stay in the atmosphere longer
exhaust containing, e.g., soot, fly ash, and pre- reducing rainfall and contributing to drought.
cursors of nitric and sulfuric acid.
PM is classified according to size of the par-
ticle: (i) coarse where the aerodynamic diameter Greenhouse Gases
(d) is 2.5–10 mm, (ii) fine where d is 0.1–2.5 mm, The French mathematician Joseph Fourier intro-
and (iii) ultrafine where d is <0.1 mm. Coarse duced the “greenhouse effect” property of the
particles include mold, pollen, sea spray, and atmosphere in 1824 by writing that the atmosphere,
material from the surface including minerals like a greenhouse, admits the visible light of the
and soil. The settling velocity of coarse particles sun and blocks escape of infrared heat radiation [5,
means that they do not travel far and thus only 14]. In an article from 1896, Swedish chemist and
pose a hazard as a local air pollutant. Fine par- Nobel Laureate Svante Arrhenius calculated that a
ticles are lighter and can be transported over doubling of atmospheric CO2 would result in a
long distances. They can originate from com- temperature increase of 4  C (modern climate
bustion and consist of organic carbon and models agree!) and predicted that such a change
metals; they can also form in situ from coagula- was likely as we are “evaporating the coal mines
tion. Ultrafine particles can also originate from into the air” [1]. Since that publication, scientists
combustion and condensation of oxidized have discovered other key greenhouse gases
organic gases; due to Brownian motion, they shown in Fig. 1 like methane (CH4), nitrous
undergo many collisions and build into fine oxide (N2O), particulate matter (PM), and ozone
particles. Ultrafine PM can contain so-called (O3), and the halocarbon gases, which all contrib-
“brown” and “black” carbon, the distinction ute to the greenhouse effect [14].
284 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Atmospheric CO2 has increased from a pre- Methane is one of the most important green-
industrial mixing ratio of around 280 ppm to over house gases and the most abundant hydrocarbon
410 ppm today, mainly because of fossil fuel com- in the atmosphere. It is a strong greenhouse gas,
bustion. Fossil fuel combustion has also had other and its global warming potential is 86 times that of
impacts on the climate and the environment as a carbon dioxide over a 20-year time period
whole. Unburned hydrocarbons are released into [10]. Methane sources are diffuse and both natural
the atmosphere by many sources, leaks in mines and anthropogenic. The atmospheric concentra-
and wells and distribution systems, fuel and solvent tion of methane has increased 2.5 times relative
evaporation, and other industrial processes. In to pre-industrial. Initial growth of methane over
addition, large amounts of naturally occurring vol- the last millennium was linked to agriculture and
atile organic compounds (VOCs) are released by animal husbandry. Leakage from natural gas sys-
plants. The VOCs are fuel for photochemical chain tems has also became a factor, and most recently
reactions taking place in the atmosphere. Fossil natural emissions are increasing due to climate
fuel combustion produces nitrogen oxides change. The dominant anthropogenic methane
(NO and NO2) that catalyze these reactions. The sources are livestock, loss from fossil fuel extrac-
products include CO2, ozone, acid rain, and oxi- tion and use, emissions from landfills and waste,
dized volatile organic compounds that condense rice production, and biomass burning. Natural
into secondary organic aerosol (SOA). All of sources include wetlands, termites, oceans,
these components of air pollution impact climate. marine hydrates, geological sources, wild ani-
While the stratospheric ozone layer protects us mals, melting permafrost, and wildfires.
from harmful radiation, tropospheric O3 is catego- As shown in Fig. 1, CO2 is the main driver of
rized as a pollutant since it has adverse effects on anthropogenic climate change [10]. The primary
humans and ecosystems. These five reactions source of CO2 is fossil fuel use, but it can also be
describe the core of the mechanism [5]: emitted directly from cement production, biolog-
ical respiration, and land use change [161].
NO2 þ hv ðl < 420 nmÞ➔NO þ O
Anthropocene
Nobel Laureate and atmospheric chemist Paul
O þ O2 ➔O3 Crutzen coined the term “Anthropocene” to
describe our current geological epoch, in which
NO þ HO2 ➔NO2 þ OH human activity has been the dominant influence
on climate and the environmental change [15,
CO þ OH➔CO2 þ H 162, 163]. In geological terms, an epoch is defined
by a specific layer of rock or strata [16]; it is clear
H þ O2 ➔HO2 that Homo sapiens is leaving many markers of the
current epoch in Earth’s geology. Microplastic par-
CO is the fuel, NOx (NO and NO2) is the ticles and soot can be found everywhere including
catalyst, and CO2 and O3 are the products. The ocean sediments. Enough concrete has been
underlying form is the same for VOC which is manufactured to cover every square meter of the
oxidized by OH to produce HO2, which then planet’s surface with a kilogram. No matter our
couples with NO to produce NO2 and O3. species’ fate, our society will endure in the crust.
Through atmospheric chemistry the emission of Proposals for a precise date for the beginning of the
NOx leads to an increase in tropospheric O3. NOx Anthropocene range from the beginning of the
is also harmful to humans when inhaled and to agricultural revolution (12–15,000 years ago) to
ecosystems when removed from the troposphere the Trinity nuclear bomb test of 16 July 1945.
as HNO3, contributing to rainwater acidity at a The Anthropocene Working Group of the Sub-
regional level. The main source of NOx is fossil commission on Quaternary Stratigraphy of the
fuel combustion. International Commission on Stratigraphy has
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 285

approved a formal, official “golden spike” proposal A wealth of information concerning past climate
to define the Anthropocene epoch in the geologic and atmospheric composition has been obtained
time scale. Final approval awaits a decision by the by analyzing the composition of annual ice accu-
International Geological Congress [16]. mulation layers, obtained by boring into the gla-
ciers of Greenland and Antarctica.

Observations of Climate Change Surface Temperature


The GISS Surface Temperature Analysis
There are many direct methods of observing cli- (GISTEMP) record comprises temperature data
mate change, for example, records of tempera- from 1880 to present, with the base period
ture and rainfall, tide gauges, and satellite 1951–1980 used to define “average” conditions
observations, including observations of land use (Fig. 2). From recent data (GISTEMP Team,
change and sea surface temperature. The obser- 2019), on a global scale, the smoothed land-
vational record is extended by analyzing the ocean temperature index (the combined Land-
world around us. For example, tree growth Surface Air and Sea-Surface Water Temperature
rings contain information on growing condi- Anomalies) had reached 1  C by 2016, relative to
tions; stalactites, corals, and sediments have sim- the base period [18].
ilar annual growth layers with compositions Looking at the mean annual surface air tem-
which can be analyzed to yield climate data. perature over ocean or land areas, Fig. 3 shows

Global Mean Air Temapure (1880-2018)


1.5

1
Temperature Anomaly /degC

0.5

-0.5 Annual
Lowess smoothing (5yr)

-1
1880 1890 1900 1910 1920 1930 1940 1950 1960 1970 1980 1990 2000 2010
Time / yr

Air Pollution and Climate Change: Sustainability, Scatterplot Smoothing, is a widely used statistical method
Restoration, and Ethical Implications, Fig. 2 Land- for smoothing data points in order to average out noise
ocean temperature index (1880–2018), with base period and/or high-frequency variations. The method uses a poly-
1951–1980. The solid blue line is the global annual mean, nomial regression analysis over a moving interval
and the solid orange line is the 5-year LOWESS smoothed [17]. (Dataset from GISTEMP Team, 2019 [18])
line. LOWESS, which stands for LOcally WEighted
286 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Mean Surface Air Temperature over Ocean or Land Areas


2 (1880-2018)

Land_Annual
1.5 Lowess smoothing (5yr)
Ocean_Annual
Temperature Anomaly / degC

Lowess smoothing (5yr)

0.5

-0.5

-1
1880 1890 1900 1910 1920 1930 1940 1950 1960 1970 1980 1990 2000 2010
Time / yr

Air Pollution and Climate Change: Sustainability, Earth’s land area, and sea surface temperature anomalies
Restoration, and Ethical Implications, Fig. 3 Mean averaged over the part of the ocean that is free of ice at all
surface air temperature over ocean or land areas (C). times (open ocean) [17]. (Dataset from GISTEMP Team,
Annual (thin) and 5-year LOWESS smoothed (thick) 2019 [18])
lines for the temperature anomalies averaged over the

that in the last 30 years, the rate of increase of the Greenhouse Gas Changes
land surface air temperature was faster than that Increasing anthropogenic emissions of green-
of the sea surface water temperature, leading to house gases are the key drivers of increasing
the temperature anomaly between land surface global temperatures [19]. Thus it is critical to
air temperature (1.2  C in 2018) of almost twice explore the changes in mole fraction or mixing
that of the sea surface air temperature (0.68  C in ratio of the main greenhouse gases (Fig. 4).
2018). Due to the mixing of the water column, Charles Keeling of the Scripps Institution of
the effective heat capacity of the ocean is higher Oceanography was the first person to make accu-
than that of land so that oceans are able to absorb rate repeated measurements of atmospheric car-
more heat [164]. bon dioxide. The measurements began at the
Besides recording temperature changes on Mauna Loa Observatory on Hawaii in 1958 and
global land and ocean scales, the NASA GISS have continued to the present day [20]. Figure 4a
dataset also demonstrates that temperature shows that as of February 2019, the concentration
changes in the Southern Hemisphere were of CO2 has exceeded 410 ppm, with an average
more than 0.2  C smaller than those in the increase of 1.64 ppm per year over the past
Northern Hemisphere (Dataset from GISTEMP 60 years (1958–2018).
Team, 2019 [18]). In addition, owing to shrink- While atmospheric methane increased rapidly
ing polar ice, less solar radiation is reflected at after the agricultural and industrial revolutions,
high latitudes producing temperature anomalies somewhat mysteriously, its rate of growth decreased
at polar latitudes much larger than in other in the 1990s, and it essentially stopped growing in
regions. the 2000s. A number of theories have been proposed
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 287

Carbon Dioxide Concentrations at Mauna Loa Observatory


a 420

Full record ending at February 10, 2019

400
CO2 mole fraction / ppm

380

360

340

320

300
1958 1968 1978 1988 1998 2008 2018
Time/yr

Annually Mean Methane Concentrations (1979-2017)


b 1900

1850
CH4mole fraction / ppb

1800

1750

1700

1650

1600

1550
1979 1984 1989 1994 1999 2004 2009 2014
Time / yr

Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications, Fig. 4 (continued)
288 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Annually Mean Nitrous Oxide Concentrations (1979-2017)


c 335

330

325
N2O mole fration / ppb

320

315

310

305

300

295
1979 1984 1989 1994 1999 2004 2009 2014
Time / yr

Annually Mean CFCs Concentrations (1979-2017)


d 580 HCFC-22
CFC-11
CFC-12
480 HFC-134a
CFCs mole fraction / ppt

380

280

180

80

-20
1979 1984 1989 1994 1999 2004 2009 2014
Time/yr

Air Pollution and Climate Change: Sustainability, concentrations of methane (1979–2017). (c) Global average
Restoration, and Ethical Implications, Fig. 4 Global concentrations of nitrous oxide (1979–2017). (d) Global
average changes of greenhouse gases abundances. (a) The average concentrations of CFCs and HCFCs (1979–2017).
Keeling Curve (1958–2019.02). (b) Global average ((b, c, d) Dataset from NOAA/ESRL/GMD, 2019 [165])
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 289

including changes in natural gas leaks from Russia, to 2000, the ocean absorption sink was
wetlands, and a drop in the atmospheric concentra- 1.71  0.52 Pg C per year and the terrestrial
tion of OH, the main oxidant for methane ecosystems sink was 1.41  0.66 Pg C per year,
[171]. More recently, methane growth has resumed; matching data from Manning in 2001 [26].
as of March 2019, its mole fraction was 1866.4 ppb,
compared to less than 700 ppb prior to 1700 [165]. Oceans
The concentration of nitrous oxide in the atmo- Oceans cover 71% of Earth’s surface and have a
sphere reached 330 ppb in 2017 with an average mass a million times higher than the atmosphere
rate of increase of 0.9 ppb per year over the past and are therefore able to exert a very large effect
decade. Many people have heard about the anthro- on the atmosphere [5]. Oceans stored 90% of the
pogenic ozone hole, caused by release of chloro- additional energy in the climate system between
fluorocarbons (CFCs, a type of halocarbon). What 1971 and 2010 [10], leading to ocean temperature
is not as well recognized is that the CFCs are increases. The largest observed effect is in the
powerful greenhouse gases and that the Montreal upper layer (0–700 m), where the near-surface
Protocol, created to protect the ozone layer, is also (upper 75 m) temperature increase exceeds
the most successful climate treaty in history. The 0.1  C per decade, whereas at 700 m, the increase
atmospheric concentration of the CFCs is decreas- is only 0.015  C per decade. The ocean tempera-
ing, due to international agreements. As the main ture rise is most distinct in the Northern Hemi-
substitutes of CFCs, HFCs (hydrofluorocarbons) sphere due to the concentration of landmass,
and HCFCs (hydrochlorofluorocarbons) are population, Arctic sea ice loss, and ocean circula-
increasing in concentration as they have no or tion itself. The ocean warming will spread from
small ozone depletion potential. the surface to lower ocean (depth > 1000 m), and
this, in turn, will affect ocean currents. The global
Oxygen Changes mean sea surface temperature change from 2046
The concentration of oxygen in the atmosphere has to 2065 is estimated to be in the range of 1–2  C
decreased due fossil fuel combustion (Fig. 5a). The and from 2081 to 2100 in the range of
change in the concentration of O2 is a few parts per 1–3.7  C [10].
million per year and is not a threat in itself. The Ocean warming results in sea level rise due to
measurement series is used to calculate the sizes of thermal expansion of water [10]. There is addi-
the land and oceanic sinks of global CO2 [21] due tional sea level rise due to the melting of land ice,
to the mass balance between the amount of carbon glaciers, ice caps, and the major ice sheets of
released by human activity, the amount of CO2 Antarctica and Greenland. Thermal expansion
dissolved in the ocean, and the amount taken up combined with melting land ice is responsible for
by photosynthesis [22]. By recording the atmo- 75% of observed sea level rise since 1971. Sea
spheric ratio of O2 to N2, atmospheric abundance level is also affected by water storage in terrestrial
of CO2, and emissions of CO2 from burning fossil systems, for example, irrigation removes water
fuel [23], it is possible to calculate the carbon from reservoirs on land, and dams prevent some
dioxide sequestration by terrestrial and marine sys- runoff into the ocean.
tems (Fig. 5b). The rate of global mean sea level rise between
A series of papers have explored the fate of 1901 and 2010 was 1.7 mm/year, yielding a total
CO2 released into the atmosphere [20–24]. Atmo- rise of 0.19 m in that time period. It is likely that
spheric potential oxygen (APO) is “a weighted the rate was higher between 1993 and 2010, at
sum of O2 and CO2 in an air parcel” [24] that “is 3.2 mm/year. Future projections of sea level rise
essentially the O2/N2 ratio added to 1.1 times the estimate that from 2046 to 2065, the global mean
concurrent CO2 concentration” [25]. Using the rise will be in the range of 0.24–0.30 m and from
atmospheric and fossil fuel emission records, 2081 to 2100 in the range of 0.40–0.63 m [10].
the ocean and land biotic uptake can be deduced. Melting ice introduces freshwater to oceans,
Manning and Keeling [24] found that from 1990 thus changing salinity. Salinity also depends on
290 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Oxygen Concentrations Recorded at Mauna Loa


a Observatory (1991-2018)
Time / yr
0
1991 1996 2001 2006 2011 2016

-100

-200
O2/N2 ratio / per mg

-300

-400

-500

-600

-700

b -60

1990
-80
change due to fossil fuel combustion only

-100
APO / per meg

-120
1995

-140

2000
-160
Land biotic uptake Ocean uptake
Atomospheric increase

-180
352 357 362 367 372 377 382
CO2 / ppm

Air Pollution and Climate Change: Sustainability, sinks [25] from 1990 to 2000, “the slope for the oceanic
Restoration, and Ethical Implications, Fig. 5 (a) the sink is fixed to an APO:CO2 molar ratio of 1.1, whereas the
records of O2:N2 ratio; (b) Vector diagram showing the land sink by terrestrial system is a horizontal line, having
calculation of the global oceanic and land biotic carbon no effect on APO” [25]
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 291

patterns of evaporation and precipitation. Obser- Hemisphere are warming faster than the rest of
vations from 1950 to 2008 show that very saline the planet, primarily because of the albedo feed-
waters have become even more saline and low- back [186, 187]. The albedo feedback comes from
saline waters have freshened, increasing the con- the warming of the ocean and atmosphere that
trast between low and high salinity areas. It is leads to sea ice melting, which in turn leads to
likely that this contrast is due to changes in fresh- lower albedo over the polar cap and further
water transport between ocean waters and the absorption of the sunlight and further warming
atmosphere caused by warming of the lower (white sea ice that reflects sunlight changes to
atmosphere [30] (hydrological cycle, see below). relatively much darker open water).
Ocean currents have an enormous impact on As the melting of land and sea ice in polar
climate as well. Currents are generated by forces regions accelerates (along with hydrological cycle
affecting the water such as wind, gradients in tem- changes, see below), more freshwater flows into the
perature and salinity, breaking of waves, and ocean. Due to its low salinity, this water is less
mixing of waters of different densities. Ocean cur- dense, and its introduction disrupts the normal ther-
rents form the great conveyor belt, also called mohaline circulation that drives ocean flow, for
thermohaline circulation. The thermohaline circu- example, mixing surface and deep waters. There is
lation is driven by horizontal mixing of water evidence that this meltwater has weakened the
caused by density differences. Thermohaline cir- Atlantic overturning circulation [188]. Europe
culation transports warm, saline surface waters receives about a third of a sun’s worth of energy
northward and colder, denser waters southward. from the Gulf Stream [5], and changes in the Atlan-
The warm, saline water is cooled when it reaches tic Meridional Overturning Current (AMOC) will
the high latitudes of the Northern Hemisphere and impact European weather as climate warms.
then sinks. From there waters are transported back
southward [31]. Perturbations of ocean salinity will Hydrological Cycle
affect deep ocean water circulation and will affect A simplified global hydrological cycle depicts
transport of heat from ocean to land as well [32]. ocean and land surfaces heated by the sun’s radi-
Atmospheric CO2 is in equilibrium with CO2 ation, resulting in evaporation of water that moves
dissolved in the surface ocean [5]; its uptake is with winds in the atmosphere, condenses to form
limited by mixing of surface and deep water. By clouds, and falls back to the Earth’s surface as rain
introducing more CO2 to the atmosphere, a greater or snow, flowing back to oceans via rivers
amount of CO2 will be dissolved in ocean waters. [5]. However, human-induced climate change
This will lead to a reduction of ocean pH, a pro- has a direct influence on precipitation and the
cess called “ocean acidification.” Over the last hydrological cycle, especially for extreme events.
250 years, oceans have absorbed about Increased heating leads to greater evaporation and
1.55  1014 kg of anthropogenic carbon [33], thus surface drying, increasing the intensity and
which has caused average pH of ocean surface duration of droughts. The water-holding capacity
waters to drop from 8.2 to 8.1 [34]. Ocean acidi- of air increases by about 7% per  C warming [35]
fication is problematic because it is detrimental to leading to an increase in water vapor in the atmo-
marine ecosystems, as acidic conditions nega- sphere; water vapor is also a powerful greenhouse
tively affect formation of corals and both chitin- gas. On balance, the relative humidity of the atmo-
ous and calcareous shells of arthropods and sphere has not been seen to increase with temper-
molluscs, respectively [30]. In addition, less CO2 ature as much as the holding capacity; globally the
dissolves in acidic solutions, and the solubility of increase is only about 2% per  C warming, due to
CO2 decreases as temperature increases [5]. reduced moisture over land and moisture trans-
port. The increased moisture capacity of the atmo-
Polar Amplification sphere at higher temperatures has multiple effects
It has been observed that the polar regions and [189]. Storms (tropical and extratropical cyclones,
especially the Arctic region of the Northern thunderstorms) supplied with increased moisture
292 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

produce more intense precipitation events, fluxes in these regions, while the direction and
increasing the risk of flooding. The higher amount speed of extratropical cyclones are affected by
of moisture in the air will also result in stronger the jet stream. Therefore, the distribution of pre-
moisture transport between dry and wet regions, cipitation is related to the course of the jet stream.
generally resulting in dry areas becoming drier Generally, the jet streams are predicted to move
(e.g., in subtropics – increased risk of droughts) poleward with climate change [27], moving
and wet areas becoming wetter (e.g., in tropics storms poleward from their current positions and
and extratropics – increased risk of flooding) leaving less storms where they’re currently
[189]. However, with a warming climate, atmo- located. This will result in more precipitation
spheric circulation patterns are also expected to from extratropical storms poleward from current
change (e.g., Hadley cell expansion, poleward precipitation bands and less precipitation equator-
movements of jet streams, changes in stationary ward. Changes to the meandering of the jet stream
waves) and with it regional precipitation patterns (i.e., changes to stationary waves) will further
[190] (see below). contribute to the changes in precipitation patterns.
These effects have important implications for
Hadley Cell, Jet Streams, Storms, and Rainfall water resources (via rainfall redistribution) in
Distribution these regions as a consequence of climate change;
One of the predicted atmospheric circulation one example is the drying of the Mediterranean,
changes under climate change is the expansion which largely results from drier cold season in the
of the Hadley cell [29]. Work by Hu and Fu has region [28].
shown that the Hadley cell has already expanded
significantly, between 2 and 4.5 of latitude, since Soil Carbon Content and Permafrost
1979, especially during the summer and fall. This Soils store carbon, and the rate of decomposition of
implies a poleward shift of the subtropical dry soil organic matter depends on temperature
zone, leading to less precipitation in regions pole- [37]. With climate change the flux of CO2 from
ward of the current/past subtropical zone soils will also increase, simultaneously depleting
[29]. This means that the effect of the circulation soil carbon. In Arctic and sub-Arctic regions, large
changes is that areas with currently sufficient quantities of organic carbon, twice as much carbon
amount of rainfall can become drier with global as there is the atmosphere [38], are trapped in frozen
warming and vice versa, as well as to potentially soils as permafrost. Permafrost carbon is derived
further enhance the wet-gets-wetter and dry-gets- from plants and animals that have accumulated in
drier patterns (mentioned above). permanently frozen soil over thousands of years.
With warmer atmosphere and oceans, there Human activities in northern regions cause local
will also be more energy available for storm climate warming as well. Over the last 30 years,
growth, potentially leading to intensification of the temperature has risen 0.6  C per decade in high-
tropical and extratropical cyclones and associated latitude regions [10], causing frozen ground to thaw
stronger winds, storm surges, and precipitation. [39]. When organic carbon is exposed to soil
The different distribution of heat across the microbes, it decomposes releasing methane and
Earth’s surface and upper layers of the atmosphere CO2. This positive feedback accelerates climate
will also lead to different distributions of these change, but the magnitude and timing of greenhouse
storms in a warming climate. gas emissions from these regions and their impacts
Extratropical cyclones, distinct from tropical on climate change remain uncertain.
cyclones (i.e., hurricanes and typhoons), are
formed by large mid-latitude surface temperature Consequences of Climate Change: The Sixth
gradients, for example, in the North Atlantic, Mass Extinction
North Pacific, and Southern Oceans and the Med- There have been five historical/geological mass
iterranean Sea [27]. Generally, extratropical extinction events in the history of our planet, the
cyclones contribute to rainfall, winds, and thermal last one occurring roughly 65 million years ago
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 293

[40]. Scientists concur there is a sixth ongoing fats, and oils is excessive, while the production of
mass extinction, driven by humanity’s domination fruits, vegetables, and proteins is low relative to
of the Earth system and multiple interacting fac- the Harvard Healthy Eating Plate guidelines
tors including habitat loss, emerging infectious (Table 1). The suggested servings meet require-
diseases, overexploitation, pollution, invasive ments of nutrients for humans [44].
species, and climate change. A mass extinction Increasing production of protein works
can be defined as >75% of species disappearing against the goal of keeping the global mean
within a geologically short timeframe (< two annual temperature within 1.5  C, but this
million years). The normal background rate of could be offset if production consisted mostly
extinction is 10–100 times less than the rate of of plant-based protein and fish, which only con-
species having gone extinct in last 100 years tribute 3% and 4% of total GHG emissions,
[41]. Climate changes such as higher tempera- respectively, in contrast to animal agriculture
tures, rainfall extremes, sea level dynamics, and which currently contributes 50% [44]. Earth’s
CO2 concentrations directly impact biodiversity growing human population requires food, but
in many ways (e.g., thermal threshold exceeded, there is an obvious limit to the amount of arable
inundation, phenology, etc.) [42, 166]. land available. One solution would be to
More than 40% of insect species are declining de-emphasize animal production and increase
and threatened with imminent extinction, and the plant-based protein production.
total mass of insects is falling at the calamitous In food production, fertilizer is often used to
rate of 2.5% per year [43]. Human impacts, both achieve faster growth and higher yield [5]. Fertil-
directly and indirectly, are almost entirely the cause izers contain fixed nitrogen which contributes to
due to synergies of overharvesting, habitat loss, cli- emissions of N2O. N2O has a global warming
mate change, and pollution from intensive agricul- potential 298 times that of CO2 on a 100-year
ture and consumerism. Habitat loss (a consequence time horizon [45]. Table 2 shows how agriculture
of intensive agriculture and urbanization) and pollu- impacts climate, via CO2 emissions, but also
tion from fertilizers and pesticides have massive through methane and nitrous oxide [45].
impacts on insect biodiversity. Of many proposed The United Nations’ Sustainable Development
solutions, using sustainable and less harmful fertil- Goals [167] focus attention on the primary chal-
izers and pesticides could be very effective if not lenges facing the world. The second goal is to
economically popular or feasible [43]. eliminate hunger and achieve food security
throughout the world. This could be achieved by
ending malnutrition and increasing agricultural
Sustainability and Climate Change outputs through investment, stable food produc-
tion, and dissemination of knowledge [168].
Food Security
Feeding the world’s growing human population
(currently estimated at 7.6 billion people [5]) in a Air Pollution and Climate Change: Sustainability,
sustainable way is one of the problems facing Restoration, and Ethical Implications, Table 1 Com-
society. If all people lived with a high standard parison of current and suggested production of foods [44]
of living, including a “Western” diet with more Servings Suggested
meat, fats, and processed foods, it would require Food type produced servings
an additional gigahectare of land currently not Grains 12 8
available. Food production worldwide is currently Fruit and 5 15
estimated to be 2750 kcal/person [44], but due to vegetables
waste, it is more likely to be around 2200 kcal/ Oil and fat 3 1
Protein 3 5
person. In addition to waste, overproduction con-
Milk 1 1
tributes significantly to the problem of sustainable
Sugar 4 N/A
food production. In general, production of grains,
294 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Health Consequences of Climate Change Energy and the Development of Human


Areas that are food-insecure are most likely to suffer Society
negative environmental effects due to climate change. Energy is closely related to our daily life and is an
Climate change will cause a higher probability of important driver of the development of human
illness and death due to extreme heat waves, inhala- society. Energy is fundamental to the economy
tion of pollutants, food shortages, and an increased and is easily correlated with economic output.
risk of water- and foodborne diseases [169]. Before the industrial revolution, traditional socie-
Increasing temperatures from climate change ties relied on physical labor, biofuels, and wind
will also affect human populations, directly and and water power [48]. After the discovery of the
indirectly. It is estimated that by 2100, surface steam engine, coal became the dominant fuel, and
temperatures could increase by 7  C, which will subsequently oil and natural gas, and nuclear
affect the ability to work outdoors and will affect energy [5]. The share of renewable energy (i.e.,
agriculture and crops [47]. solar, wind, tidal, hydropower) is growing quickly
but is still small relative to fossil fuel (Fig. 7).
Air Pollution and Climate Change: Sustainability, Development of human societies is only achieved
Restoration, and Ethical Implications, Table 2 Agri- with development of energy sources.
cultural emissions as fraction of total greenhouse gas
emissions [45]
The Status of Energy Consumption
Pollutant CO2 CH4 N2O
Since energy is central to our society, it is critical
Agricultural 15 49 66
emissions as to explore the relations between energy and eco-
fraction of total nomic development. Trends in energy consump-
emissions (%) tion from 1965 to 2017 show the largest increases
Expected changes Stable or From rice: Up to in developing regions such as the Asia Pacific and
by 2030 declining stable or ~60%
Africa are much higher than developed regions
declining increase
From (see Fig. 6), and in those regions, the reliability on
livestock: coal tends to be larger as well (Fig. 7).
~60% Different regions of the world rely on a differ-
increase
ent mixes of energy; Fig. 7 shows the values for

Global Primary Energy Consumption (1965-2017)


14000.0

12000.0
Million tonnes oil equivalent

10000.0

Total Asia Pacific


8000.0 Total Africa
Total Middle East
Total CIS
6000.0 Total Europe
Total S. & Cent. America
Total North America
4000.0

2000.0

-
1965 1970 1975 1980 1985 1990 1995 2000 2005 2010 2015
Time/yr

Air Pollution and Climate Change: Sustainability, dataset from BP Statistical Review of World Energy:
Restoration, and Ethical Implications, Fig. 6 The https://www.bp.com/en/global/corporate/energy-economics/
global primary energy consumption from 1965 to 2017, statistical-review-of-world-energy.html
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 295

TOTAL NORTH AMERICA TOTAL EUROPE


Renewables
Hydroelectric 4.0% Renewables
Nuclear 5.9% Hydroelectric 8.2%
Oil 6.6%
energy 7.8% 40.0% Nuclear
Coal energy 9.8% Oil
13.1% 37.1%

Coal
15.1%

Natural Gas Natural Gas


29.2% 23.2%

GLOBAL ENERGY STRUCTURE IN 2017 TOTAL S. & CENT. AMERICA


Renewables Renewables
Hydroelectric
4% Hydroelectric 4.7%
Nuclear 7%
energy 4% Oil 23.2%
34%
Nuclear
energy 0.7% Oil
45.5%
Coal
28% Coal
4.7%

Natural Gas Natural Gas


23% 21.3%

TOTAL ASIA PACIFIC TOTAL CIS


Hydroelectric
Hydroelectric Renewables Renewables
Nuclear Nuclear 5.8%
6.5% 3.0% 0.1% Oil
energy 1.9% energy 6.7%
Oil 20.8%
28.6% Coal
16.1%

Coal
48.4%

Natural Gas
11.5%

Natural Gas
50.5%

TOTAL MIDDLE EAST TOTAL AFRICA


Nuclear Hydroelectric
energy 0.2% Hydroelectric
0.5% Renewables
Renewables Nuclear 6.5%
Coal 1.2%
0.9% 0.2% energy 0.8%
Oil
46.8% Oil
Coal 43.7%
20.7%

Natural Gas Natural Gas


51.4% 27.1%

Air Pollution and Climate Change: Sustainability, Review of World Energy: https://www.bp.com/en/global/cor
Restoration, and Ethical Implications, Fig. 7 The porate/energy-economics/statistical-review-of-world-energy.
global energy structure in 2017, dataset from BP Statistical html
296 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

2017. Coal is the main fuel in the Asia Pacific countries such as China and India are relatively
region, while natural gas dominates in CIS low due to their large populations.
(Commonwealth of Independent States) and the
Middle East accounting for over 50% total fuel Hubbert’s Peak or Peak Oil Theory
use [49]. Oil is the dominant fuel in the Americas, Hubbert’s peak theory was developed by the
Europe, and Africa [49]. On a global scale, oil, American geophysicist Marion King Hubbert.
coal, and natural gas are the top three consumed He asserted that oil production from a given
fuels accounting for 34%, 28%, and 23% of the region tends to increase rapidly to a maximum
total, respectively. output level and then enters a terminal decline
until extraction becomes prohibitively expensive
The Relationship Between per Capita GDP and [35]. While the basic idea that petroleum
Energy Consumption resources are finite and will come to an end is
Economic analysis shows a clear a positive rela- not refuted, there is significant debate concerning
tionship between per capita GDP (gross domestic when the peak will be reached and what the effects
product) and energy consumption (Fig. 8). Energy will be for society [35]. Even though the growth of
consumption in 2011 in the United States, the oil consumption is driven by economic develop-
equivalent to 7032 kg of oil per capita, was much ment, oil is not limitless. Production of oil and
larger than that of China, 2029 kg per capita, linked other nonrenewable resources including natural
at least in part to a larger per capita GDP, $49,854, gas, coal, and rare metals is facing similar issues
in the United States versus $10,041 in China of extraction and production [50].
(Fig. 8). Even though total energy consumption One of the famous examples of Hubbert’s peak
across the Asia Pacific region is relatively high, theory is the production of whale oil in the nine-
energy consumption per person in developing teenth century [35]. With cheap supply and the

Correlation of energy consumption and GDP per person in 2011


20000
per capita energy consumption /kg oil equivalent

18000

16000

14000

12000

10000

8000 Canada United States

6000 Australia
Japan
New Zealand
4000

2000 India European Union

China
0
0 20000 40000 60000 80000 100000 120000 140000 160000
GDP per capita based on purchasing power parity/current international $

Air Pollution and Climate Change: Sustainability, equivalent per capita), https://data.worldbank.org/indica
Restoration, and Ethical Implications, Fig. 8 Rela- tor/EG.USE.PCAP.KG.OE; GDP per capita, PPP (current
tionship of per capita GDP and energy consumption/kg international $), https://data.worldbank.org/indicator/NY.
of oil equivalent of 132 countries and regions in 2011, GDP.PCAP.PP.CD
dataset from the World Bank: Energy use (kg of oil
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 297

ability to burn brightly, the demand for whale oil became more efficient [55]. In general, improve-
spurred the whaling industry and caused it to go ments in efficiency increase consumption rather
“through a spectacular cycle of growth and than reduce it due to subsequent increased
decline” in the nineteenth century [35]. The num- demand [56]. However, environmentalists, indus-
ber of whales and whaling ships shows a classic try, and government often disregard this paradox
predator-prey dynamic, and the output of whale when trying to reduce energy consumption by
oil follows a bell-shaped curve. increasing efficiency.
A clear modern-day example of Jevon’s para-
Relationship Between Greenhouse Gas dox is the “paperless office.” In theory, increasing
Emission and Economic Development use of computers and electronic storage of data
Economic externalities are those costs born not by should reduce paper usage eventually leading to a
the buyer or seller but by society [170]. Climate “paperless” office environment. However, con-
change and air pollution are two good examples of trary to the expectation, consumption of paper
external costs: those who create the pollution do has increased [56].
not pay, and the costs are imposed on everyone. Jevon’s paradox has important implications for
The 2006 Stern Report [51] presupposes that the sustainability of energy resources [57]. One
atmospheric greenhouse gas levels should be sta- potential solution to avoid Jevon’s paradox is
bilized between 450 and 550 ppm of CO2 equiv- governmental regulation (e.g., taxing higher con-
alent to avoid catastrophic ecological collapse and sumption, offering discounts for reducing con-
severe negative impacts for society. This concept sumption, etc.) coupled with energy efficiency.
involves converting other gases to an equivalent
amount of CO2, denoted CO2e. In 2006, the level
of CO2e was already at 430 ppm [20]. To accelerate Environmental Management and
the low-carbon energy transition from coal to Climate Change
renewable energy sources, governments and indus-
tries need to develop and distribute environment- Preservation
friendly technologies. Renewable energy sources For the past century, preservation has been the
(solar, wind, geothermal, and hydroelectric) are traditional environmental management strategy
currently the most sustainable energy sources around the world [175]. The core idea of preser-
because there are no direct emissions of carbon vation has been captured by the Wilderness Act
dioxide and resource potentials are virtually set by the US Congress in 1964 which defines
unlimited [52]. wilderness as follows:
Climate action is a major objective in the
A wilderness, in contrast with those areas where
United Nations Sustainable Development Goals man and his own works dominate the landscape, is
(SDGs) with the idea that “urgent action to com- hereby recognized as an area where the earth and its
bat climate change and its impacts” is needed community of life are untrammelled by man, where
man himself is a visitor who does not remain.
[53]. The United Nations wrote that “global (Wilderness Act of 1964) [174]
warming is causing long-lasting changes to our
climate system, which threatens irreversible con- Thus, preservation attempts to protect natural
sequences if we do not take action now” [54]. areas from human influence and places a high
value on their “naturalness” and “wildness” and
Jevon’s Paradox the independence of an area from human
Jevon’s paradox was an observation about energy impact [59].
consumption and energy efficiency made by the
English economist William Stanley Jevons in his Habitat
book The Coal Question in 1865 [55]. Jevons As human populations and consumption grow,
observed that the production and consumption of areas formerly used for animal habitats are being
coal increased at the same time as the use of coal converted into areas used for human interest such
298 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

as agriculture and city expansion [72]. The main Seeds and Plants
areas converted are forests (both tropical and tem- Food security is of major concern worldwide;
perate), savannas, and coastal marshes. This is food production is threatened by climate change.
causing a major contribution to the extinction of In addition, with the ongoing degradation of the
species. ecosystem, preservation of the plants we eat has
People around the world are trying to preserve, become a concern. Gene- and seed banks are
restore, and manage ecosystems, but with the emerging as a way of preserving seeds and plants
climate changing at a different speed in different and their respective genetics. It is estimated that
areas around the globe, these environmental man- there are currently 1750 gene banks worldwide.
agement practices are difficult to prepare. One of them is the Svalbard Global Seed Vault
Not only does the coming climate change pose located in Norway and owned by the Norwegian
a big challenge for restoration; the emissions over government. The Vault can hold up to 4.5 million
the last several decades pose a challenge as well. seed samples and is surrounded by permafrost to
In a study from 2000, scientists found that the cool and preserve samples if power systems fail.
proportion of herbaceous and woody components However with climate change and associated ris-
of the savanna are connected to CO2 in the air. As ing temperatures, the vault has experienced some
a consequence, the savanna cannot be restored as water damage due to the permafrost melting. Cur-
it was before the heavy CO2 emissions, because it rently, it holds around 5000 different kinds of
will not grow back in the same way [70]. species and far more samples. The Seed Vault is
considered a key operator in the preservation of
Species seeds and plants [74]. Another approach for pre-
Climate change is threatening global biodiversity venting the extinction of seeds and plants is to
including the numbers of species, the numbers of create more protected and monitored areas [75].
individuals, and the interrelationships between spe-
cies. Many species are struggling to adapt to rising
temperatures and changing weather. The protection Ecological Restoration
of ecological systems and biodiversity depends on
existing systems, but given the increasing losses of Human societies are putting increasingly danger-
habitat and environmental quality, and increasing ous pressure on ecosystems that support life on
losses of species and individuals, it is clear that the Earth, and the scientific studies that document
existing systems are not sustainable. their destructive impacts on the global biosphere
Changes in net photosynthetic productivity at the are mounting [60–62]. These impacts have
base of the food chain affect the entire ecosystem. become so widespread and severe that ecological
On land this is mainly plants and in the oceans, restoration has become a major form of environ-
algae. Plants are affected by, e.g., drought and mental management [58, 59] and it is currently
flooding, loss of habitat, and air pollution. Oceanic going through an exciting growth period
productivity is affected by, e.g., nutrient availability, [191]. For example, the Bonn Challenge attempts
ocean circulation, and pH. There is less space avail- to restore 150 million hectares of deforested and
able for the ecosystem due to roads, buildings, and degraded land by 2020 and 350 million hectares
agriculture, and the space that is there is changing, by 2030 [192]. At the beginning of 2019, the UN
due to flooding, drought, pollution, etc. declared 2021–2030 to be a “Decade of Ecosys-
In a review on biodiversity management from tem Restoration” [193]. Restoration projects can
2008, scientists evaluated 113 papers and their rec- vary from local small-scale projects such as with
ommendations for conservation of natural habitat the Greene Prairie, a 47-acre restoration at the
and species. A third of the papers point out that the University of Wisconsin-Madison’s Arboretum
need for ecological information is greater than the in the United States, to large-scale projects such
need for additional social or political information, as the Comprehensive Everglades Restoration
with the related conclusion that actions are more Plan in the United States which is the broadest
important than just passing on information [73]. and most expensive restoration project to date
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 299

[194]. The plan combines more than 50 projects be appropriate to attempt to return the area to the
and consists of 68 project components estimated temperate woodland which once stood there
to cost over $10.5 billion over a timeframe of [70]. Therefore, historical fidelity, which links the
more than 35 years. Ecological restoration has present to the past, might not be an attainable goal
also been recognized as an important objective in the future dictated by climate change.
in environmental policy. For instance, the Will this render ecological restoration impossible
European Union is committed to restoring 15% in the future? Philosopher Andrew Light predicts
of degraded ecosystems in Europe by 2020 that for some restoration practitioners, climate
(European Commission 2011 [63]). change will relax the obligation to follow historical
The most widely accepted definition of ecolog- reference conditions and for others, it will lead to an
ical restoration has been presented by the Society existential crisis [71]. Looking at the predictions
for Ecological Restoration (SER) [64]: “Ecologi- provided by the IPCC, some warming is inevitable,
cal restoration is the process of assisting the recov- and even the most optimistic scenarios predict
ery of an ecosystem that has been degraded, warming of at least 2  C above pre-industrial levels,
damaged, or destroyed.” which will likely lead to significant ecological con-
The definition provides important information sequences [10]. Light argues that as species and
about the contents of ecological restoration. First, entire ecosystems start moving as a consequence
the definition suggests that the act of ecological of climate change, the definition of ecological resto-
restoration is an intentional human activity. The ration will also be on the move and will likely adapt.
restoration practitioner makes an active choice to However, how ecological restoration as a practice
restore a particular area. The term assisted recovery will evolve along with the challenge of climate
highlights this active role of the restorationist in change will likely have important societal and eco-
assisting the transition to a “healthy” or intact con- logical consequences. If ecological restoration con-
dition. Second, the definition provides vital infor- tinues to hold fast to historical fidelity, it is likely that
mation about the goal of restoration projects. it will not be a viable practice in the future. At the
Restoration projects are not aimed solely at improv- other extreme, if the grip on historical fidelity is
ing the state of a particular environment, but to loosened completely, ecological restoration might
restore it to the pre-disturbance condition transform into a practice of complete human eco-
[65]. Therefore, ecological restoration takes a strong logical domination focused only on ecosystem ser-
stance on appointing value to historical legacy vices and goods aligned with utilitarian economic
(often called historical fidelity) of the system prior ends leading to a future of designer ecosystems. As
to human degradation and subsequent intervention. pointed out by Harris et al., “it is one matter to watch
Finally, the definition recognizes the destructive role change happen in ecosystems and wonder how and
that humans have played in ecosystems and the how much to intervene, and quite another to become
responsibility resulting from this destruction. a determining agent in that change” [70].

Ecological Restoration and Climate Change


Ecological restoration can play an important part in Mitigation and Adaptation
the mitigation efforts toward climate change. This
is because the restoration of vegetation and soils – Relations Between Climate-Related Risk,
especially of forest ecosystems – is considered safe Hazard, Vulnerability, and Exposure
sinks to absorb carbon dioxide [68, 69]. However, There is a close relationship between climate-
climate change also poses a threat to the practice of related risk, hazard, vulnerability, and exposure
ecological restoration by challenging its main (Fig. 9). The risks of climate-related impacts
goals: historical fidelity and ecological integrity. include the changes in the climate system and
Climate change will likely make it difficult, if not socioeconomic that result from the interactions
impossible, to return a damaged ecosystem back to between climate-related hazards, vulnerability,
its previous pre-disturbed state. For example, if an and exposure of human and natural systems
area was flooded by rising sea levels, it might not [4]. The change of climate system consists of
300 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Air Pollution and Climate


Change: Sustainability,
Restoration, and Ethical Hazards Exposure Vulnerability
Implications,
Fig. 9 Overview of the
causes, impacts, and
feedbacks of climate risk

Climate Risk

Impacts

Climate System Socioeconomic


Processes

• Governance
• Natural Variability
• Adaptation and Mitigation Actions
• Anthropogenic Climate Change
• Socioeconomic Pathways

anthropogenic climate change and natural vari- [118]. While using the land sink has positive second-
ability, while socioeconomic processes consist of ary effects for the environment, since, e.g., replanting
adaptation and mitigation actions, governance, trees leads to both ecological restoration and uptake
and socioeconomic pathways. These changes are of carbon dioxide (in contrast past land use changes,
the drivers of hazards, exposure of human and like deforestation, have contributed about 30% to
natural systems, and vulnerability [4]. global CO2 emissions [195]), the ocean sink leads
Mitigation and adaptation are two approaches for to ocean acidification (see below). Other forms of
dealing with climate change. Mitigation includes geoengineering are presented under adaptation strat-
actions that limit, stop, or reverse long-term climate egies as they do not include carbon sinks.
change, whereas adaptation focuses on adjusting to
actual or expected climate. There are many mitiga- Land Carbon Sink Enhancement
tion strategies including land use change (e.g., refor- The land-based biosphere is a large reservoir of
estation) and carbon capture and storage (from a carbon, driven by photosynthetic plants. Compared
point source or open air). Adaptation strategies to the ocean which is a large reservoir for dissolved
include flood prevention (e.g., flood barriers on inorganic carbon, the carbon lifetime is relatively
river estuaries and sea gulfs), water supplies in dry short on land because stored carbon returns to the
regions, and food security. atmosphere when plant matter decays.
The carbon content and lifetime of the main
reservoirs of carbon on land [118] are shown in
Mitigation Table 3. There are several ways of enhancing land
reservoirs including the production of biochar,
Carbon Dioxide Removal (CDR) via Land Use afforestation, and reforestation.
Changes and Ocean Sink
Carbon dioxide removal is a form of geoengineering Biochar
that comprises a number of technologies for large- Biochar is a kind of charcoal produced by pyrol-
scale removal of CO2 from the atmosphere ysis. Biochar production converts half of the car-
[132]. Two methods that are often discussed involve bon of biomass into charcoal and produces CO2
modifications to the land and ocean carbon sinks that can be removed by carbon capture and storage,
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 301

Air Pollution and Climate Change: Sustainability, It may take decades before their net carbon foot-
Restoration, and Ethical Implications, Table 3 Car- print becomes negative [195]. Further research is
bon content and lifetime of different reservoirs of land
carbon sink [118] necessary to reduce cost, improve performance,
and scale up BECCS.
Carbon Average
Reservoirs of land carbon content/ lifetime/
sink PgC years Afforestation and Reforestation
In leaf litter and detritus 90 ~2 Afforestation refers to establishing forests at for-
In global biomass (mostly 550 ~50 merly forested locations that have lost their tree
woody vegetation) cover for over half a century, while reforestation
In soil as labile organic 660 ~50 refers to establishing forests at locations that
carbon
have lost their trees within the last 50 years
In soil as recalcitrant 750 ~500
material
[118]. Afforestation and reforestation are feasi-
ble options for increasing land carbon storage in
the form of soil carbon and plant biomass includ-
ing wood [143]. A study shows that the regrowth
see below, by heating biomass in the absence of of forests on farms that were abandoned during
oxygen [118]. Sources of biochar include pyrolysis the medieval outbreak of bubonic plague in
of agricultural, forestry, and urban waste and other Europe can account for the CO2 and temperature
sources of plant waste [118]. decrease during that period [144]. Storing
Compared to crop wastes and woods, biochar 11–27 GtC by reforestation was shown to result
safely captures and stores carbon for a much lon- in decreases of atmospheric CO2 of
ger time as biochar is resistant to biological oxi- 4–10 ppm [144].
dation, in contrast to plant material including Due to its potential for storing carbon and
wood. In addition, mixing biochar with soil improving environmental resilience, several
enhances crop yield and shows a strong potential projects have been launched to address deforesta-
for reducing emissions of the greenhouse gases tion. One example is the United Nations’ Reduc-
CH4 and N2O by soil, and NH3, and improving ing Emissions from Deforestation and forest
soil structures [142]. Degradation (REDD+) project, which aims to
support reforestation in developing countries
Bioenergy with Carbon Capture and Storage [196]. Another is the Great Green Wall project to
(BECCS) re-establish a continuous band of trees across
BECCS refers to carbon sink technologies that Africa across the Sahel to reduce desertification
extract energy from biomass, for example, by [145]. The 8000 km project is already 15% com-
making ethanol or biogas, and trap and store the plete. By establishing green belts and trees, the
CO2 that is produced [195]. Photosynthetic Great Green Wall will moderate temperature,
plants and algae (e.g., crops like sugar cane, reduce wind speed, and enhance humidity of
corn, rapeseed) take up CO2 as they grow; the soil [145].
biomass is then used as food or fuel. The pro- In addition to storing carbon and providing bio-
cesses of producing biofuel, for example, fer- diversity, increasing forest cover can enhance cloud
mentation to produce ethanol, give CO2 that is cover, increasing the albedo, via evapotranspiration,
captured. The carbon in the biofuel came from and providing biogenic precursors of cloud conden-
the atmosphere and is released back into the sation nuclei, helping to counteract the lower albedo
atmosphere when the fuel is used, and in addi- of forest relative to grassland [118].
tion, the CO2 produced in fuel manufacture is
captured and stored. When optimized, BECCS Ocean Carbon Sink Enhancement
thus promises to be a carbon-negative technol- The ocean is a formidable reservoir for carbon that
ogy. However, significant amounts of energy can can absorb over a quarter of anthropogenic carbon
be used in producing and processing biomass, for dioxide [118]. There are several ways to improve
example, as fertilizer and for tractors and trucks. the carbon sink capacity of the ocean.
302 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Ocean Alkalinity Enhancement deeper in the water column or to sediment.


Carbon dioxide (CO2) is soluble in water (H2O) Often, the rate of photosynthesis is limited by
forming carbonic acid (H2CO3), bicarbonate the availability of one or a few key nutrients,
(HCO3), and carbonate (CO32) and producing such as iron, whose addition can greatly increase
acidity (H+) [5]: the net primary productivity, enhancing CO2
uptake [149]. In 2004, seven tons of iron sulfate
CO2 þ H2 O  H2 CO3  Hþ þ HCO3  was added into the Southern Ocean resulting in a
 2Hþ þ CO3 2 massive bloom of diatoms and the highest chloro-
phyll column recorded in a fertilization test. It was
There is a rapid equilibrium between these shown that at least half the resulting bloom bio-
forms, and the relative amounts are determined mass sank into the deep ocean resulting in storage
by the pH of the solution. Together, H2CO3, for centuries or longer [150].
HCO3, and CO32 are called dissolved inorganic However, this technique can have negative
carbon (DIC), and the concentration of DIC effects on marine ecosystems including the poten-
depends on acidity, increasing with pH. One tial disruption of fisheries which should be taken into
method for enhancing ocean alkalinity is to add consideration when implementing the ocean fertili-
lime into the ocean [146]. This process consists of zation (see the section on “Ecological Justice”).
three steps: firstly turning the calcination of lime-
stone (CaCO3) into lime (CaO) and CO2; secondly
the lime is hydrated to generate calcium hydroxide Carbon Capture and Storage (CCS)
(Ca(OH)2) [147]; and thirdly calcium hydroxide is
put into oceans to increase ocean pH and increase Carbon dioxide is the primary anthropogenic
the uptake of atmospheric CO2 [148]. It is shown greenhouse gas; its concentration has increased
that an increase in seawater alkalinity of 10% is rapidly (see Fig. 4a). Carbon capture and storage
enough to uptake 50% of anthropogenic-emitted (CCS) is a key strategy for mitigating climate
carbon dioxide for around half a decade [148]. change. It consists of the separation of CO2 from
Although additional CO2 is released during the a gas stream after which it is compressed and
process of calcination, the generated CO2 can be stored [103].
captured directly during production using carbon
capture and storage (CCS) [118]. Besides the need Carbon Dioxide Capture
for capturing CO2, the scale and availability of The first step of the carbon capture and storage
limestone are worth considering. A study claimed process is the capture of CO2 produced by, e.g.,
that sequestering 15 billion tons of CO2 the combustion of fossil fuels or calcination of
(approximately 2 ppmv CO2), approximately the limestone.
amount of the annual increase of atmospheric There are three main applications of carbon cap-
CO2, would require 10 km3 of limestone, and the ture including pre-combustion, post-combustion,
energy required for its calcination [147]. Although and oxyfuel combustion [104] (Fig. 10). In general,
the demand for limestone is large, it does not the choice of capture methods and capture systems
exceed the quarrying and calcination capacity, is determined by [105] the types of fuels and the
and there is abundant limestone in the crust. properties of the gas stream including the pressure
and concentration of CO2.
Ocean Fertilization
In the ocean, photosynthesis takes up DIC and Pre-combustion Capture
converts it into carbohydrate biomass: In pre-combustion capture, the fuels are combined
with the air or O2 to produce a mixture of hydro-
H2 CO3 ! 1=nðCH2 OÞn þ O2 gen, carbon monoxide, and carbon dioxide, which
is called gasification [106]. The reforming step is
When planktons die, they fall in the water followed by gasification, when water is added to
column, transporting carbon from the surface convert the CO into H2 and CO2. The H2 can
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 303

subsequently be used in power generation, and the beneath an impermeable nonporous layer. In
pure CO2 can be safely captured. some cases the CO2 is used for enhanced recovery
of oil or gas, to press more hydrocarbons out of a
Post-combustion Capture formation.
In post-combustion capture, fossil fuels are If the geology of the formation is suitable, the
burned, and then the flue gas passes through a CO2 can bind into minerals. For instance, carbon
suitable absorber which absorbs the carbon diox- dioxide can be stored in basalt in the form of
ide before it enters the atmosphere. In this way, the stable carbonate minerals. The calcium, magne-
CO2 is safely captured. Stripping carbon dioxide sium, and iron oxides in basaltic rocks are avail-
from the gas stream is the key step of the capture able to react with CO2 to generate carbonate
process. It can be achieved by several different minerals [115] such as CaCO3, MgCO3, and
methods such as solvents [107], solid sorbents FeCO3.
[108], membrane systems [109], and adsorption/
desorption processes. Silicate of Mg or CaðsÞ þ CO2 ðgÞ
One of the mature technologies is the amine ! MgCO3 ðsÞ or CaCO3 ðsÞ þ SiO2 ðsÞ
solvent absorbents. Some studies have shown that
the working fluid can break down over time This carbon capture technique has been achieved
resulting in the release of by-products [110]. The in Iceland, and “it is estimated that about
subsequent atmospheric reactions of these com- 7000 GtCO2 can be stored in offshore of Iceland
pounds would form products including carcino- within the Exclusive Economic Zone” [116].
genic nitrosamines that could potentially pose a Ocean storage can be achieved by injecting and
hazard for surrounding areas [110]. dissolving (dissolution type) or injecting liquid-
The other example of absorbers in post- like supercritical carbon dioxide (lake type) in the
combustion capture method is the use of metal- deep ocean [103]. Dependent on its lower viscos-
organic frameworks [111]. The metal-organic ity and higher density relative to and water (and
frameworks are one of the promising carbon diox- oil), the mobility of an injected lake of supercrit-
ide capture materials due to their high surface ical CO2 is determined by hydrodynamic forces
areas and adjustable pore functionality allowing [117]. In time, centuries to millennia, the CO2 lake
them to selectively adsorb a large amount of will dissolve and disperse and become part of the
CO2 [112]. global carbon cycle [103]. Ocean storage is asso-
ciated with a number of environmental impacts.
Oxyfuel Combustion First, ocean carbon storage will cause a decrease
The last key capture method is the oxyfuel pro- in ocean pH which is harmful to marine organ-
cess. The nitrogen is stripped from the oxygen isms. Second, CO2 lakes themselves are toxic to
before combustion in an air separator [113]. The marine life and will likely kill creatures that come
purified O2 is combusted with fossil fuels that into contact with them [103].
produce CO2 and water vapor. Then the water It is important to note that a significant amount
vapor is cool condensed and removed. of CO2 is stored nonpermanently in soil and bio-
mass such as in leaf litter and detritus, in the soil as
Carbon Storage labile organic carbon, in the soil as recalcitrant
The second step of CCS is to store the CO2 safely material, and in woody vegetation [118].
and permanently. Therefore, it is important to establish a sophis-
Land carbon storage (“geosequestration”) is ticated long-term monitoring system for stored
the primary carbon storage method; the sites CO2 in order to avoid leakage. In addition, storage
may be on land or under the ocean floor. Sites sites should be carefully selected to allow for
with porous rocks such as oil fields, gas fields, permanent storage of the CO2 at the site, and
saline formations, and saline-filled basalt forma- additionally, the acceptability of the site should
tions are chosen to store the compressed, liquified be taken into consideration to avoid any negative
CO2 [114]. The method requires a reservoir impacts on the ecosystem [117].
304 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Pre-combustion: Heat & Power


Air/O2 H2 Other products

CO2 Compression
Fossil fuels Gasification/reforming H2/CO2 Separation
& Transport

Post-combustion:
Air

Combustion CO2 Separation CO2 Compression


Fossil fuels
& Transport

Heat & Power

Oxy-fuel combustion:

Air Fossil fuels

Air separation O2 Combustion CO2 Compression


& Transport

Heat & Power

Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications, Fig. 10 Carbon
capture categories: pre-combustion, post-combustion, and oxyfuel combustion

Direct Air Capture scalability. Estimates of the cost range of DAC


In direct air capture (DAC), CO2 is captured from range from $30 to $1000 per ton of CO2 (/t CO2).
the ambient air. It is absorbed or adsorbed onto a In contrast, the price of CO2 as a chemical com-
solid or liquid sorbent which is regenerated yield- modity varies from $100 to $300/t CO2, depending
ing clean sorption substrate and CO2 for use, on the transport method; this price is a result of
storage, or sequestration. The air-to-CO2 ratio is current market conditions, and the price would be
currently 2500:1, so to collect enough CO2 to be expected to fall if new CO2 sources went into
meaningful, large amounts of ambient air must be production. It is estimated that at a price of $50/t
processed. This requirement limits the efficiency CO2, it would be economically feasible to make
of the process and places requirements on the fuel from algae. This process requires CO2 but is
materials that can be used. The energy and size only in play if the price of CO2 were to be signif-
requirements mean that the method is currently icantly lower.
more expensive than other approaches [119]. Another challenge for CCS is transporting CO2
Reaching the Paris targets, whose goal is to from the capture facility to the storage site. This
keep global warming below 2  C by the year transportation, whether by road or pipeline,
2100, is not possible given current trends. Achiev- requires energy and infrastructure. With DAC,
ing them would require drastic reductions in CO2 capture and storage can take place at the same site.
emissions combined with direct air capture. Authors have noted that the possibility of DAC
The feasibility of a given technology is deter- could work against efforts to reduce CO2 emis-
mined by its cost and to some extent by its sions because people may think we can just
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 305

recapture it again, someday. It’s important to note A number of research organizations have
that CO2, once emitted, becomes very dilute in the published MAC curves [2, 3, 123, 124]. The
atmosphere and is therefore much harder to cap- global greenhouse gas abatement cost curve pro-
ture than when it is highly concentrated at a point duced by the McKinsey & Company (Fig. 11) is a
source of emissions. In addition, it is not sustain- typical and well-known example. It summarizes
able to rely on the promise of a technology that is the costs of different emissions reductions ordered
not fully developed. To prevent a catastrophic from lowest to highest and provides a discussion
climate trajectory, it is important to reduce emis- about “what actions would be most effective in
sions now, by decreasing emissions of CO2 and reducing emissions” [2].
pursuing negative emissions approaches [120]. This figure shows vetted technologies for achiev-
ing a greenhouse gas abatement of 38 GtCO2e per
Methane Control year [2]. Improving the energy efficiency of indus-
As shown in Fig. 1, the radiative forcing of meth- tries, buildings, and vehicles costs little and in many
ane is quite large and has contributed over half cases saves money due to the decrease in energy
again as much radiative forcing as CO2. On a per consumptions. In addition, many abatement
gram basis, methane is 86 times more warming methods use low-carbon energy sources such as
than CO2 which means that reducing methane wind, nuclear, solar, and hydro. There are also
could potentially be very cost-effective. Also, approaches based on forestry and agriculture, such
since its atmospheric lifetime is short, about as reforestation and land use change. Finally, emerg-
10 years, reducing methane emissions would ing technologies such as CCS do not contribute
have immediate benefits in contrast to CO2 which large abatements and are expensive; these prices
stays in the climate system for centuries [5]. Unfor- are expected to drop with further development and
tunately, methane is very inert chemically. Its CH implementation.
bond is the least reactive of any hydrocarbon. It has Besides McKinsey & Company, the Wuppertal
a very high vapor pressure and does not condense Institute for Climate, Environment and Energy
or adsorb easily. Scientists discovered that zeolites has produced MAC curves for Germany [124],
may hold promise for methane capture; the next and the Bloomberg New Energy Finance has pro-
step is to test the zeolites and determine if the duced the curves for the United States [3].
theory works in practice [121]. Methane sources
include wetlands, methanogenic bacteria, garbage
dumps, cows, and termites [5]. The sources are Adaptation
diffuse making them difficult to control.
Due to legacy emissions, past decisions, and
McKinsey Marginal Abatement Cost Curve “political inertia,” humanity is already committed
Besides focusing on the mitigation target of keep- to some dangerous climate change impacts, which
ing the temperature increase below 2  C relative to means that adaptation appears to be inevitable.
pre-industrial [122], it is critical to consider the Adaptation has traditionally received less atten-
effectiveness, cost, and scale of mitigation and tion than mitigation mainly due to its limited
abatement actions when governments and organi- potential, uncertain benefits, and less straightfor-
zations put the climate change mitigation strate- ward measurements [127].
gies into wide practice.
The marginal abatement cost (MAC) is a mea- Examples of Adaptation Strategies
sure of the cost of reducing an additional unit of
pollution. The MAC for many methods can be Adaptation in Europe
summarized in a MAC curve which is defined as Countries across the globe are preparing and
“. . .a graph that indicates the cost, usually in $ or implementing adaptation strategies. Though the
another currency per ton of CO2, associated with the seriousness and speed of climate change impacts
last unit (the marginal cost) of emissions abatement are being debated, there is no doubt that it is
for varying amounts of emission reduction” [123]. happening. Given the wide range of impacts, it is
306 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

Global GHG abatement cost curve beyond business-as-usual – 2030


Gas plant CCS retrofit
Abatement cost Coal CCS retrofit
€ per tCO2e Iron and steel CCS new build
60 Low penetration wind Coal CCS new build
Cars plug-in hybrid Power plant biomass
50 Residential electronics co-firing
Degraded forest reforestation
Residential appliances Reduced intensive
40 Nuclear agriculture conversion
Retrofit residential HVAC Pastureland afforestation High penetration wind
30 Degraded land restoration
Tillage and residue mgmt Solar PV
20 Insulation retrofit (residential) 2nd generation biofuels Solar CSP
Building efficiency
Cars full hybrid new build
10
Waste recycling
0
5 10 15 20 25 30 35 38
-10 Organic soil restoration
Geothermal Abatement potential
-20 Grassland management GtCO2e per year
-30 Reduced pastureland conversion
Reduced slash and burn agriculture conversion
-40 Small hydro
1st generation biofuels
-50
Rice management
-60 Efficiency improvements other industry
Electricity from landfill gas
-70 Clinker substitution by fly ash
-80 Cropland nutrient management
Motor systems efficiency
-90 Insulation retrofit (commercial)
Lighting – switch incandescent to LED (residential)
-100
Note: The curve presents an estimate of the maximum potential of all technical GHG abatement measures below €60 per tCO2e if each
lever was pursued aggressively. It is not a forecast of what role different abatement measures and technologies will play.
Source: Global GHG Abatement Cost Curve v2.0

Air Pollution and Climate Change: Sustainability, abatement cost curve, September 2013, McKinsey & Com-
Restoration, and Ethical Implications, Fig. 11 Global pany, www.mckinsey.com. Copyright (c) 2019 McKinsey
greenhouse gas abatement cost curve beyond business-as- & Company. All rights reserved. Reprinted by permission
usual in 2030. (Source: Exhibit from Pathways to a low- [2])
carbon economy: Version 2 of the global greenhouse gas

challenging to create a comprehensive plan to deal circulation, and pH, resulting in shifts in the dis-
with climate change. tributions of plankton and fish [129].
In Europe, the key risks of climate change will The European Union (EU) requires its mem-
include rising sea level, an increase in economic bers to adopt an adaptation plan in preparation for
losses, increased pressure on water resources, and the effects of climate change. Currently, 25 of the
many more. Adaptation will require preparation 28 member countries have adopted such a plan.
for flooding, higher efficiency for water use, and The focus of the EU adaptation strategies is to
more [128]. address three main points: preparing and approv-
Besides having a negative impact on wildlife, ing a national adaptation plan, “climate proofing”
ecosystems, and nature, flooding has a major eco- key elements such as agriculture and the fishing
nomic impact. Flooding in coastal areas may industry, and promoting the use of Climate-
cause erosion and damage to buildings, which ADAPT, which is the EU’s climate adaptation
require additional insurance when located in platform, thereby promoting knowledge on adap-
flood zones. Increasing urbanization in coastal tation and climate change.
areas carries increased economic risk. In 2012 Denmark approved a National Adap-
Food security is also at risk. On land there tation Plan (NAP). The NAP requires all munici-
are obvious effects from increased variability in palities to participate with the result that they
rainfall and increased temperature. In the ocean have all implemented a local plan. Money was
there are impacts from changing temperature, set aside in the national budget to support the
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 307

municipalities with implementation. Nationwide, and carbon dioxide removal (CDR), discussed above
the adaptation focus was on transport, coastal with mitigation strategies. Mitigation and adaptation
protection, and roads. are not mutually exclusive.
Solar radiation management (SRM), also known
Adaptation in Food Security and Agriculture as solar engineering, is a category of climate engi-
Climate change is a key challenge to food secu- neering with the goal of increasing planetary albedo
rity, posing a serious threat to countries around the and thereby reducing absorption of solar radiation at
world [197]. Crop yields are negatively affected the surface [132]. There are three main types of
by climate change including extreme tempera- SRM: albedo enhancement, space reflectors, and
tures, changes in growing season and climate stratospheric aerosol injection [118].
zone, and variable rainfall [130]. Reduced pro-
duction will cause higher prices and a higher risk Cloud Albedo Enhancement
of shortages. Countries in many regions have Cloud albedo enhancement can be achieved by
taken steps toward adaptation in the areas of agri- increasing the reflectivity of low-level maritime
culture and food security. clouds. The amount of condensed water in a cloud
In North Africa, a study focusing on Morocco is determined by the total amount of water present
documented the effects of water scarcity on social and the temperature. If a cloud forms in an air
stability [131]. For agriculture that depends on parcel with relatively more cloud condensation
rainfall, planting patterns and crop types have nuclei (CCN), the same amount of liquid water
shifted in response to climate change. Strategies is distributed among more cloud droplets. While
for reducing risk may include more accurate sea- the amount of liquid water may be the same as if
sonal weather predictions and crop insurance [4]. the cloud had formed in a clean atmosphere, the
In Australia, industries have relocated due to surface area is not the same. Light scattering is
climate change. Further, individual farmers have determined by the surface area of the water, not
moved or changed activities, such as changing the amount of water, and so the effect of increas-
from grazing to cropping and changing crops, ing CNN is to make clouds “whiter” [133]. Artifi-
due to long-term changes in rainfall [4]. cially increasing CNN would cool the Earth due to
In China, there are adaptive responses to cli- increasing the albedo; oddly, air pollution has the
mate change ranging from individual farmers to same effect and has resulted in “global dimming,”
the government. China is making efforts to a reduction in the amount of sunlight reaching the
improve agricultural infrastructure, including surface. The CCN to cloud albedo interaction is
accelerating the construction of water-saving irri- known as the first indirect aerosol effect and is
gation projects, restoring degraded farmland, also called the Twomey effect [134].
planting trees to combat desertification, and One of the techniques being discussed involves
developing water storage and utilization projects spraying minute water droplets into the atmo-
in mountainous and desert areas [130]. Besides sphere from the ocean using high-volume atom-
government-level actions, individual farmers izers or generating bubbles that would burst at the
have adopted water-saving technologies and new surface, generating sea spray, by blowing air
crop varieties to reduce climate-related risks through porous pipes, concepts first proposed by
[130]. Latham [135, 136]. The sea spray particles would
be dispersed in the atmosphere by turbulent diffu-
Geoengineering with Solar Radiation sion and convection, increasing the albedo and
Management (SRM) cooling the surface. Mixing could possibly be
In the context of climate change adaptation, enhanced by space-charge repulsion of like-
geoengineering refers to technologies that are inten- charged particles. Although raw materials are
tionally used to modify synoptic or global climate. free and nonpolluting, the infrastructure would
There are two major types of climate geoengineering: need to be built [137]. While this approach
solar radiation management (SRM), discussed here, would in theory be able to counteract warming
308 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

due to excess CO2, it would not reduce ocean OCS from the troposphere and volcanic injection
acidification, and its cooling effects would be [198]. Large volcanic eruptions such as the erup-
regional due to the limited lifetime of CCN. tion of Mount Pinatubo in 1991 are known to cool
the global climate [141]. Paul Crutzen proposed
Surface Albedo Enhancement [199] that if elemental sulfur was injected into the
Increasing the surface’s reflectivity toward solar lower stratosphere using missiles, the dispersed
radiation is another method of albedo enhance- sulfur, after being oxidized in the atmosphere
ment. One method is to use reflective materials to yielding sulfate, would give a cooling effect with
cover roads and roofs. This has an immediate a lifetime of 1–2 years. The amount of cooling
local effect for the building or road and, with would thus be reversible and could be controlled
widespread use, could cool a city and region. by the rate of injection. The sulfate aerosols
There are several kinds of roofing technologies increase scattering of shortwave solar radiation
conducive to this approach including membranes, before it reaches the Earth’s surface [140] by
cool-surfaced modified asphalt systems, and absorbing and emitting longwave radiation
metal roofing panels [138]. The city of Los [118]. There are several proposed techniques of
Angeles found that streets painted with a white sulfate injection including the use of artillery
sealant were 5–15  C cooler than similar asphalt shells and putting the sulfur in aircraft fuels [140].
streets. Painting the roofs will not only reflect Compared with the space reflectors and sea
50–70% solar radiation [138] but also reduce spray generation, stratospheric aerosol injection
energy consumption for air conditioning due to is more technologically feasible and less costly.
the decreased cooling load after reflecting the However, there are unavoidable disadvantages
solar radiation. of stratospheric sulfate injection. First, it could
cause a small increase in ozone depletion by
Space Reflectors increasing the number of aerosols. Second, the
Another way to reduce the absorption of solar aerosols will cause sky whitening [140]. Finally
radiation at the surface would be to reflect parts this method would not solve the problem of ocean
of incoming solar radiation before it enters Earth’s acidification.
atmosphere. This could be accomplished by plac-
ing reflectors in space, between the sun and Earth
[118]. In 1989 Walter Seifritz proposed [139] Ethics and Philosophy of Climate
placing mirrors in a Lagrange orbit [140]. The Change
Lagrangian point is the (moving) location where
the gravitational forces of the sun and Earth cancel Scientific understanding of the issues surrounding
[140]. Placing mirrors in a Lagrange orbit is effec- climate change is a vital foundation, and in addi-
tive at deflecting sunlight for the entire planet, not tion, there are critical ethical implications which
just for a certain region(s). Putting mirrors in a should not be ignored. Environmental and climate
Lagrange orbit is very costly. A cheaper option science addresses complex and interacting sys-
would be to place reflectors in orbit around the tems, thus involving “integrating knowledge and
Earth [140]. However, mirrors in Earth orbit expertise from several disciplines” [200,
reflect less solar radiation because the reflectors 201]. One such interdisciplinary intersection
might be in the Earth’s shadow part of the orbit. occurs with the field of environmental ethics,
which is a “discipline in philosophy that studies
Stratospheric Aerosol Injection the moral relationship of human beings to, and
The third method or achieving solar radiation also the value and moral status of, the environ-
management would be to inject sulfur into the ment and its non-human contents” [202]. In fact,
lower stratosphere. The stratosphere is known to many of the arguments made in environmental
contain a layer of sulfuric acid aerosol, the ethics are often dependent on the findings of sci-
so-called Junge layer, with sulfur provided by entific research [200]. However, ethics and
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 309

science do not obviously fit together. For instance, summarized: “climate change involves the con-
the question of the appropriate role of values in vergence of a set of global, intergenerational and
science is a long-standing debate in the philoso- theoretical problems. This convergence justifies
phy of science. It is often perceived as inappropri- calling it a ʻperfect moral stormʼ” (see also [77]).
ate for values to “to intervene on the evaluation In fact, this perfect moral storm not only does
scientific hypotheses” promoting a view that sci- make answering these ethical questions difficult
entific hypothesis should be as value-free as pos- but also makes effective action to combat the
sible [200, 203, 204]. However, there is support problem harder. This is because climate change
for the idea that there is an appropriate place for complicates our ethical analyses and relationships
values within science. There is extensive support and creates suitable conditions for moral corrup-
backing the use of social, political, and ethical tion whereby those in power can effectively
values in the selection of research priorities and ignore the problems and delay action until it is
determining “which technological applications of too late. Moral corruption instantiates by “subvert
scientific knowledge to pursue” [200]. The aim of [ing] our understanding of what is at stake” ([77],
this section is to embrace the exchange between pp. 45–46) by undermining our moral language
scientists and philosophers by describing the eth- and arguments to serve the purposes of the mor-
ical implications of the global environmental ally corrupted. What is particularly problematic is
change and the ethical implications of some of that most of the victims of climate change – future
the scientific results and technologies that are generations and nonhumans – are not able to
being developed to deal with these issues. Raising participate in the discussion since they have not
the scientific and ethical discussions together will yet been born or are otherwise unable to commu-
hopefully represent the issues of climate change nicate and/or understand the problem to
more holistically, providing a more realistic rep- begin with.
resentation of these issues. Similarly to Gardiner, the seriousness of cli-
mate change as a moral problem has led philoso-
Climate Change: A Perfect Moral Storm pher Dale Jamieson to lament: “Today we face the
Scientific, political, and economic research on possibility that the global environment may be
climate change has dominated the academic and destroyed, yet no one will be responsible. This is
public discussions of climate change, despite it a new problem” [160]. Jamieson has argued that
being an inherently ethical issue [71, 72]. This climate change poses such a great moral problem
failure to evaluate climate change holistically that we need a new environmental ethic altogether
has led to a fragmented debate which in turn has to help unravel the complicated relationships of
led to one of the key aspects of climate change responsibility for climate change. For Jamieson,
being ignored: how to inspire change in individual anthropogenic climate change poses a challenge
and collective action. Philosophical analysis can to our understanding of “rational self-interest,
be invaluable in shedding light on important prob- ethics and justice among states” [160]. According
lems and potential solutions beyond the reach of to Jamieson, climate change struggles to gain
scientific and economic analyses [78–80]. traction and inspire action because of its complex
The analyses of the ethical dimensions of cli- and asymmetrical structure as a moral problem
mate change are varied but could be grouped into across different sectors of society. The reason
three broad categories: global justice, ecological why climate change is so problematic as a moral
justice, and intergenerational justice [81]. How- dilemma is because the challenges it poses range
ever, these categories are by no means exhaustive, across different dimensions – relational, temporal,
and not all the ethical issues fit neatly into one and spatial. Most ethical models of responsibility
category or into any of them. are based on clear person-to-person interactions,
The ethical problems that climate change cre- such as telling a lie to a friend or stealing a bicycle.
ates are particularly large and messy, which phi- Climate change on the other hand operates on a
losopher Steven Gardiner (2006) [84] has completely different scale as an international,
310 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

global, intergenerational, and interspecies collec- described the effect of individuals allowing their
tive action problem. According to Jamieson, our livestock to graze in the village commons. The
old theories and models of morality are not problem of the tragedy of the commons was pop-
equipped to deal with such complicated ethical ularized and recast in a modern context by ecolo-
problems. Therefore, ethics itself needs to be gist Garret Hardin in 1968 [90] (for other
advanced to develop new ethical systems discussions on the tragedy of the commons, see
equipped to handle such complex ethical prob- Johnson 2003 [91]; Soroos 1997 [92]). Even
lems. Not all philosophers feel we need to go as though Garret framed the concept to warn against
far as creating a new environmental ethic as overpopulation, it is equally valid in describing
Jamieson suggests [79]. However, there is con- the problem of climate change. In classic ethical
sensus that climate change poses a real moral problems, the consequence of an action is here
threat that demands resolution. and now, but with climate change, the impact of,
e.g., burning a lump of coal is distributed, thinly,
Global Justice over the entire globe, and it is not immediate but
Global justice issues encompass the global reach rather spread out, thinly, over generations; the
and scale of the ethical issues caused by anthropo- burner does not, in most cases cannot, meet their
genic climate change. There appears to be a wor- victim. The benefit of burning the coal, for heat or
rying disconnect in how the acts of individuals are to cook food, is immediate and local.
transformed into the huge collective action prob- The tragedy of the commons describes situa-
lems often referred to the tragedy of the commons, tions where individuals acting in their own self-
followed by the worrying political and social iner- interest overuse a shared common resource, such
tia needed to deal with such problems [83, 84]. as natural resources, fossil fuels, and natural sinks
One of the major ways that the global justice for emissions, thereby depleting or spoiling the
issues are manifested is through the unethical and resource altogether, thus acting against the com-
unfair geographical distribution of harms caused mon good of all users. The crux of the problem is
by climate change. In other words, poor people, that it is in the individual’s interest to use the
poor nations, and the ones most vulnerable are shared resource and to get there first, despite this
often the ones that suffer the most, despite the leading to its despoiling. However, tragedy can be
fact that they have often been the least responsible avoided by group action such as privatization or
for the emissions that have led to climate change. regulation. For instance, Elinor Ostrom [93]
Similar pattern of vulnerability is present with air famously argued that members of a community
pollution and pollution in general [205]. This are able to create mutually agreed governance
imbalance could be framed as the rich “taking systems and moral sanctions, thereby guiding
advantage of the poor and more vulnerable, and individual use of the common resource to a sus-
especially their vastly inferior bargaining posi- tainable level. From the perspective of climate
tion” [81]. The political branch of climate ethics change, individual emissions produce a tricky
looks into these issues, on how the burdens and collective action problem, when a set of rational
obligations between different individuals, demo- actions by individuals all over the world cause
graphics, nations, and international justice as a climate change, thereby creating a worse outcome
whole should be dealt with [85–88]. Philosophical to everyone compared to a scenario where the
discussions are also focused on climate negotiations same individuals would have cooperated by intro-
and the role of justice in these negotiations [89]. ducing restraint to their actions.

Tragedy of the Commons Individual Action


The tragedy of the commons arises when individ- Is it possible then to hold individuals morally
ual users, acting in their own self-interest, ruin a responsible for collective action problems such a
common resource by their collective action. The climate change? For example, philosopher Walter
name comes from an essay written in 1833 by Sinnott-Armstrong [94] has argued that individ-
British economist William Forster Lloyd, which uals have no obligation to reduce their emissions;
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 311

causally, individual emissions are too small to Climate Change (IPCC) Working Group II as “a
cause climate change, and thus individuals cannot human intervention to reduce the sources or enhance
be held morally responsible for such harms. The the sinks of greenhouse gases” [207]. However,
only obligation that individuals might have with what counts as a sink is not ethically straightfor-
regard to climate change, he proposes, would be ward. All the attempted descriptions of what can be
political responsibility, since only political insti- considered “as a ‘sink’ are normatively charged
tutions which produce climate policy have the because they must assume a specific answer to the
capacity to respond to the harms caused by cli- question, safe for whom?” [69]. Also, what counts
mate change. For instance, Baylor Johnson [91] as a sink can raise ethical problems. Any destination
argues that individuals only have the responsibil- other than the atmosphere can be considered as a
ity to push toward collective agreements to deal sink; however, treating the ocean sink risks
with climate change since individual actions are compromising marine ecosystems due to ocean
not sufficient to address climate change. However, acidification. Ocean acidification will have reper-
Johnson has later withdrawn this position cussions for the biosphere as a whole including
[95]. These arguments are based on the following human food systems (see also the section on “Eco-
claims: (1) individual greenhouse gas emissions logical Justice”). So, when considering sinks, the
(GHG) cause only minimal if any harm to others; emphasis should be on safe sinks such as soils and
(2) even if an individual chooses to reduce their vegetation [68, 69]. In particular, reforestation and
GHG emissions, this would not make a meaning- afforestation would not only be considered safe but
ful contribution toward reducing global GHG would also help combat deforestation [69]. Further,
emissions; and (3) the “obligation to reduce indi- the ethical issues of mitigation are relevant to the
vidual GHG emissions is overly demanding” [96]. development of sustainable mitigation policies and
There are also several philosophers who argue technologies. The ethical issues that emerge from
that individuals can be held morally responsible for mitigation policies are often related to the fairness of
climate change. For example, Marion Hourdequin global emissions trajectories [98–100]; for example,
[97] argues for the importance of individual actions the West benefitted from using fossil fuels, and it
and responsibility as they bear communicative value would not be fair to now deny similar use to the
which in turn will encourage trust in other individual East. In addition, questions arise such as who should
actors, thus making it easier to tackle climate pay for the research and development of mitigation
change. On the other hand, philosopher Trevor technologies, should the polluter pay, or should the
Hedberg [96] has argued that individuals have a bill fall to society as a whole?
prima facie duty to reduce their personal emissions It is generally assumed, ethically speaking, that
which is demanded of them by appeals to personal mitigation is preferable to adaptation. As stated by
integrity. According to Hedberg, the concept of philosopher Henry Shue, “while mitigation is like
integrity not only helps to galvanize individuals to the prevention of an affliction, adaptation is more
political action against climate change but also pro- like rehabilitation from the affliction, or in some
vides them with strong moral reasons to reduce their cases, successful adjustment to it while it persists”
individual GHG emissions [96]. [69]. Currently, many policy decisions are guided by
scientific and economic arguments; however, choos-
Ethical Implications of Mitigation, Adaptation, and ing between mitigation and adaptation based on
Geoengineering these arguments has been heavily criticized. Evalu-
Mitigation and adaptation are the two key strate- ating future risk in terms of today’s money is diffi-
gies attempting to deal with different aspects of cult and uncertain [51] and will “involve enormous
anthropogenic climate change: “mitigation deals amounts of arbitrary evaluation” [69].
with the cause of climate change, adaptation deals
with its effects” ([206], p. 24). Ethical Implications of Adaptation Adaptation
attempts to take “the ‘danger’ out of ‘dangerous
Ethical Implications of Mitigation Mitigation climate change’” ([206], p. 24). One of the main
has been defined by Intergovernmental Panel on aspects of adaptation is vulnerability. Vulnerability
312 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

is closely related to the issues of justice and fair- p. 23). Clare Heyward [206] has argued that “criteria
ness, as the individuals who have emitted the least such as ‘deliberate,’ ‘large-scale,’ or ‘unnatural’ do
are often the ones who are, or will be, most vulner- not distinguish geoengineering, (from) either CDR
able to the effects of climate change [125, or SRM, (or) from mitigation or adaptation” ([206],
126]. The complex issue of assigning responsibil- p. 24). She notes that afforestation, one of the tech-
ity is compounded by asymmetric power relation- niques of CDR, has been considered to fall under
ships, creating a severe challenge to global mitigation by the IPCC ([211], p. 10). In contrast
cooperation on these issues. It is not possible, and SRM technologies do not attempt to tackle GHG
is often even irrational, for poorer nations to fund concentrations, but instead attempt to “prevent cli-
climate adaptation strategies, not to mention miti- mate change (or at least one key part of it) by keeping
gation [69]. In addition, it can be considered unfair global temperatures stable, despite the increased
and unreasonable to expect poorer nations to sac- GHG concentration. . . Thus, SRM is distinct from
rifice necessities when no such sacrifices were adaptation” ([206], p. 26). Heyward’s analysis shows
made by richer countries, who have been reluctant that the different technologies that fall within the
to sacrifice even luxuries [87]. remit of geoengineering vary significantly. It is cru-
cial to be precise as to which type of geoengineering
Ethical Implications of Geoengineering - technology is being referred to when the feasibility,
Geoengineering as a strategy to alleviate anthro- acceptability, or desirability of such technologies is
pogenic climate change has received considerable being discussed, let alone decided. For example, the
attention from philosophers. Discussions of ethical implications surrounding afforestation or
geoengineering face definitional complications reforestation are very different compared to strato-
as it is not necessarily clear where geoengineering spheric aerosol injections. The former would not
falls within the mitigation/adaptation spectrum. In only be less risky but would help combat deforesta-
addition, the two types of geoengineering strate- tion, provide habitat for species, and thereby
gies (SRM and CDR) are very different, with very potentially contribute to biodiversity and would not
different ethical implications and unique suites of be a global intervention and could provide other
problems and advantages. values as well such as aesthetic and/or recreational.
The Royal Society defines geoengineering as In contrast stratospheric aerosol injections would
“deliberate, large-scale manipulation of the plan- involve significant uncertainty, have significant
etary environment in order to counteract anthro- justice issues surrounding who gets to decide
pogenic climate change” ([208], p. 1). A set of key whether the technology is deployed, and have diffi-
characteristics have been identified to help distin- culty determining who is liable if something goes
guish geoengineering from other practices. For wrong. SRM technologies in particular have received
instance, according to Thomas Schelling, strong criticism from environmental philosophers
geoengineering must include three features: [81, 100, 101].
“global,” “intentional,” and “unnatural” ([209], It is also necessary to consider the direct ethical
pp. 304–305; see [210] for a summary of defini- implications of geoengineering. An influential
tions of geoengineering). These debates over report by the Royal Society [208] highlights the
nomenclature matter as they have important con- importance of ethics in determining the legitimacy
sequences for how geoengineering is perceived, of geoengineering projects: “overall it is clear that
treated, and practiced. For instance, the way ethical considerations are central to decision-
geoengineering is defined affects whether it is clas- making in this field” (Shepherd et al. 2009, p. 39
sified as part of mitigation or adaptation or as a quoted in [100]). In addition, the “analysis of
completely separate practice. In addition, this cate- ethical and social issues associated with research
gorization has ethical consequences. Geoengineering and deployment” has been listed as one out of
is often presented as being complementary to miti- eight identified research priorities ([208], p. 53;
gation and adaptation, a third option for dealing with quoted in [100]). Gardiner has been one of the key
anthropogenic climate change ([208], p. 57; [206], environmental philosophers analyzing the ethical
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 313

Air Pollution and Climate Change: Sustainability, to avoid the “nightmare scenario” of uncontrolled
Restoration, and Ethical Implications, Table 4 Ethi- climate change [102]. However, according to Gar-
cal values emerging form geoengineering based on
Gardiner’s summery [182]. This list is not an exhaustive diner, this narrative can be seen as scaremonger-
list of the different values that have been raised ing and downplaying the knowledge gaps
Values identified scientists might have of the effects of using these
with Further technologies on a large scale. In addition to these
geoengineering What type of values literature misleading narratives, political inertia has pushed
Welfare Benefit/harms [212] geoengineering to the fore as a viable option to
Justice Procedural, [100, combat the emerging climate catastrophe. This
distributive, gender; 213– has forced us into a paradoxical position with
international, 216]
intergenerational, regard to geoengineering: “What should we do,
across species ethically speaking, given that we have not done,
Rights National self-defense; [217, and will not do, what we should be doing?”
sovereignty; individual 218] [227]. Consequently, Gardiner has argued that
protections
“far from being a welcome new tool for climate
Relationship Less intrusive [100,
with nature interventions 212,
action, geoengineering policy may become
219] another manifestation of the underlying problem”
Intention Doing versus allowing; [220] ([227], p. 511, italics in original).
foreseen versus
unintended
consequences
Ecological Justice
Responsibility Compensation; [100,
rectifying injustice 214, Biodiversity loss, ecological degradation, habitat
217] loss, the sixth mass extinction, and the impacts of
Precaution Catastrophe avoidance [221, climate change most seriously affect nonhuman
222] animals, plants, and ecosystems. This type of
Virtue and vice Hubris, recklessness, [81, 214, transfer of costs to other species leads to interspe-
inflicting tragic choices 217,
223]
cies injustice [81]. Ecological justice examines
Political [214,
the relationship between humans and the natural
legitimacy 224] world, taking justice beyond the human sphere
Control and [225, [154, 155]. Ecological justice should not, how-
domination 226] ever, be confused with environmental justice.
Despite sounding similar, environmental justice
focuses only on human relationships when it
implications of geoengineering and has combined comes to environmental goods and harms. How-
a summary of ethical values that have been raised ever, this section focuses on justice for the natural
(Table 4). world. The human dominance over natural
Gardiner’s list in Table 4 demonstrates the resources and space on the Earth should be con-
richness of ethical analyses of geoengineering sidered as an injustice and should be analyzed and
[227]. Gardiner argues that geoengineering con- dealt with within the framework of justice
stitutes a serious ethical problem, so much so that [82]. Appeals to justice can demand and catalyze
he frames geoengineering as a moral failure. He “extensive conservation efforts” and as such can
argues that “it constitutes the crossing of a new serve as valuable tool in combating environmental
threshold on the spectrum of environmental reck- degradation and climate change [82]. The discus-
lessness – attempting intentional manipulation of sion of nature and nonhumans in the climate
the global system – and provides fresh and further debate is relatively new, and not much reflection
evidence of just how far we are willing to go” on this issue has been done [28]. The biggest
[81]. Arguments for geoengineering have often challenge will be convincing the constituents of
focused on the necessity of using this technology the need for this dialogue.
314 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

There are two particularly challenging issues However, the goal of preservation begs the prob-
within ecological justice: (1) Who are we talking lematic question of wilderness, a pristine state
about when we discuss ecological justice? where people are absent. Thinking of nature in
(2) How and why are these entities morally rele- this way, a nonhuman wilderness, has been termed
vant? To answer the first question, “species, eco- the “received wilderness idea” [175]. This idea has
systems, nonconscious living organisms, and received a lot of attention from environmental phi-
conscious, sentient animals” are the candidates losophers [174]. An obviously related question is
for inclusion in ethical decision-making ([228], whether humans are separator or one of many parts
p. 274). The second question attempts to answer of the ecosystem.
which parts of nature should be treated as morally The perceived wilderness idea has been criti-
considerable and why [184]. Those beings that are cized in a number of areas: for failing to preserve
morally considerable should be included in our wilderness, for conflicting with attempts to pre-
ethical thinking and decision-making. There are serve biodiversity, for being “historically and eco-
several schools of thought within environmental logically naïve,” and for being a “colonial,
ethics that present arguments as to which aspects imperialistic, unjust practice which harms peo-
of the natural world qualify as being morally ple,” including the very concept of wilderness
considerable. For example, individualistic theo- being charged for being “androcentric, ethnocen-
ries often attempt to justify why specific individ- tric, Eurocentric, and racist” to name a few ([175],
ual animals are worthy of our moral attention pp. 11–12). In addition, the emergence of the
[229, 230]. Biocentric theories [185] consider all Anthropocene has been seen as making the idea
life as morally considerable, whereas ecocentric of wilderness problematic and even meaningless.
theories [177] see ecological wholes, such as eco- Despite this long list of criticisms, the preserva-
systems or even the entire biosphere, as deserving tion of wilderness has been defended by many phi-
moral consideration. losophers and environmental practitioners [175–
Climate change will likely introduce new com- 178]. For instance, philosopher Mark Woods has
plexities to the ethical analyses of environmental constructed a detailed account defending wilderness
costs and benefits, and these will in turn effect as a meaningful concept and as an important preser-
ecological justice. Completely new species and vation goal, by developing a “wilderness ethic
ecosystems are continually coming into existence, grounded in other-than-human naturalness, wildness,
and to the extent climate change is anthropogenic, and freedom” ([175], p. 266). Ecologist Reed Noss,
this creates new obligations within the human- on the other hand, has defended wilderness by urging
nature relationship [156]. Are humans, for exam- that the wilderness ideal should be incorporated into
ple, morally responsible for having introduced “a broader vision of recovered but dynamic land-
exotic species to indigenous ecosystems? If so, scapes dominated by wildland but complemented by
are humans responsible for their removal and the true civilization” [179]. According to Noss, what
restoration of native ecosystems? How should separates humans from nature is human culture,
such restoration be performed? Would killing the with its currently unsustainable lifestyles.
introduced exotic species count as an injustice?
Even though there are aspects of environmental Ethical Implications of Ecological Restoration
morality that will fall into already existing doc- Despite the goal of ecological restoration to repair
trines (e.g., utilitarianism), not all answers to the damage caused by human impact, ecological res-
moral challenges of anthropogenic climate change toration has received criticism from environmental
will be simple or easy to resolve. philosophers. The criticism has been centered on
the goals of ecological restoration projects. The
Ethical Implications of Preservation philosophical debate surrounding ecological resto-
Preservation often attempts to preserve and protect ration was introduced by philosopher Robert Elliot
a “wild” nature that is independent of humans and in the article Faking Nature [66]. In the article,
often considered the “opposite of civilization.” Elliot presents fundamental and problematic issues
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 315

surrounding ecological restoration. Elliot attacked biodiversity? Should a rare plant trump the exis-
the claim that ecological restoration is able to tence of a common plant? Should sentience be
restore the natural state of a damaged environment. held to highest regard? Is it problematic to remove
He argued that ecological restoration is incapable a perfectly good and thriving exotic species just
of restoring a particularly important value found in because they are not indigenous to the area? [67]
nature, its naturalness. The problem was that eco-
logical restoration treated natural value as some- Intergenerational Justice
thing that could easily be recreated or replaced. The issue of intergenerational justice addresses
According to Elliot, “nature is not replaceable the challenging large time lags involved in climate
without depreciation in one aspect of its value change. A common political strategy has been to
which has to do with its genesis, its history” defer the impacts of climate change into the
[66]. In other words, he emphasized that the reason future, to future generations. However, this strat-
why people value nature is that it is “natural to a egy “strongly implies that the current generation
high degree” and this value of naturalness is is taking advantage of its privileged temporal
closely related to the area’s origin and its history position with respect to its successors in indulging
[66]. This led Elliot to argue that restored nature in political inertia” [81]. This raises several
was, in fact, faking nature. The emphasis Elliot intergenerational justice issues (see Gosseries
placed on naturalness has significance for environ- and Meyer [151]; Meyer and Roser [152]; Nolt
mental policy. Elliot was particularly concerned, [153]).
along with many other environmentalists, that But who are future generations? Philosopher
environmentally destructive activities could be John Nolt [153] has defined a future person “as
legitimized by the promise of later restoration. one [at a given time] who is not alive then but will
Elliot called this line of thinking the “restoration be later.” Persons who could actually never exist
thesis” and illustrated that it is not only naïve in are not future persons. Importantly, future people
practice but dangerously undermines conservation- are individuals despite the collective terminology
ist principles. Faking Nature sparked a vibrant that is often used to describe them. Nolt has
exchange between philosophy and ecology over argued that there are several features in our
the important discussion of the normative relation- policymaking that do not take future people seri-
ship between the human and nonhuman world [65, ously. A classic example would be economic
67]. policymaking using economic tools such as social
The obvious ethical implication of ecological discount rates. For instance, the notion of accept-
restoration is the issue of death. An important able risk – which establishes spending priorities –
“side effect” of ecological restoration is that it is usually calculated by considering how much
often involves actions that directly or indirectly people who are alive now are willing to pay to
cause the death of organisms. For instance, the reduce risk by a certain amount. However, this
introduction of a predator species into an ecosys- model completely ignores the preferences of
tem will indirectly result in deaths of the species future people and focuses on less relevant factors
that are its prey. Another example is if an invasive like the “willingness to pay” of current people.
species is removed to protect the endangered The problem with simplistic economic metrics is
indigenous species. The ethical implications that they often rely on preference satisfaction
often become more troublesome when the death which does not sufficiently represent welfare.
includes a sentient species [67]. This issue also Nolt argues that considered preferences would
raises difficult questions related to trade-offs. Is be better suited, as they are more objective and
there a straightforward way of resolving the trade- better supported by rational considerations, and
off between an invasive species of goat introduced are therefore better informed. Most people would
by humans and an endangered species of plant “value such conditions as health, longevity, safety,
that the goat eats? Does the value of rarity play a wealth adequate to needs, opportunities for learn-
role in these decisions or the value of ing, and freedom from oppression” [153].
316 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

For many, future generations might feel distant problem “shows that current policy cannot be
and irrelevant to our current decisions. However, governed by reference to harms to the interests
Nolt highlights that spatiotemporal separation of future individuals, because those policies deter-
should not be morally relevant when considering mine who those individuals will be and what
future generations. Even though we might have interests they will have” [181]. This arises
special relationships with the people close to us, because new polices will inevitably affect peo-
such as family members, friends, and colleagues, ple’s behavior, leading current people to make
when it comes to future generations, “it is the different choices, leading them to meet different
absence or attenuation of such special relation- people, and, further, leading to different children
ships, not the spatiotemporal separation, that being born than would have been born under
makes the difference” [153]. This can be tested different policies. Thus, sustainable policies can
by a simple thought experiment. Imagine Steve, only create populations that are better off com-
who is alive now, planting a bomb that will reli- pared to other different populations that could
ably explode and kill a stranger. This would be have existed under different policy regulations.
considered wrong even though Steve did not have Derek Parfit himself and other philosophers
any special relationship with the poor stranger. have, however, shown either that the nonidentity
Imagine now that Steve plants another bomb, but problem is flawed or that the problem is purely
one that will detonate far in the future, equally apparent. For instance, John Nolt has argued that
reliably killing an innocent stranger. Both bomb- the nonidentity problem relies on a questionable
ing incidents are equally wrong from a moral argument: “An action can be wrong only by mak-
perspective. One could extend this thought exper- ing someone worse off than she would have been
iment to include climate change. In fact, Nolt has otherwise” [182]. He has argued that this argu-
argued that the present generations’ insatiable ment is in fact false and that it is enough for an
production of greenhouse gases results in the action to be considered as wrong if it results in
unjust domination of future generations injuring or killing a person [183].
[126]. Political theorist Steve Vanderheiden has
attempted to address this by producing two moral
principles to take future generations seriously: The Importance of the Justice Trilemma
“the moral duty to avoid causing predictable The three dimensions of justice and the examples
harm to others” and “a basic principle of equality discussed above highlight the importance of
that refuses to discount harm simply because it ethics and philosophical analysis in disentangling
accrues in the future” [78, 153]. the swarm of moral dilemmas climate change
One of the main objections or problems with creates. The trilemma emphasizes the need for a
the idea that present people have obligations to holistic analysis of climate change that incorpo-
future generations comes in the form of the non- rates not only its scientific, political, and eco-
identity problem, raised by philosopher Derek nomic dimensions but also a detailed ethical
Parfit [180]. According to the nonidentity prob- treatment. If we truly want to find sustainable
lem, future people’s interest and well-being can- solutions to climate change, we must incorporate
not be affected by changes in policy. This is morality and ethics into the climate change
because putting sustainable policies in place debate. As Gardiner writes, “we cannot get very
(e.g., emissions reductions and the development far in discussing why climate change is a problem
of sustainable technologies) in the hope that these without invoking ethical considerations” [84]. We
will lead to increased well-being for future gener- have reached a point where there is a serious need
ations will not work because these very policies for moral accountability and responsibility. Most
would result in producing different people in the importantly, ethics represents and includes in the
future than would have otherwise been generated decision-making process, the most vulnerable, the
under the current more environmentally destruc- most disenfranchised, and the most ignored
tive policies. In other words, the nonidentity within the human and nonhuman communities.
Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications 317

Conclusion Future Directions

It is perilous and paradoxical that climate As the climate and environmental crisis deepens,
change, easily the most important problem fac- understanding the ethical implications of science
ing human society, is largely ignored. Economic and human technologies will is becoming more
development and the well-being of society immediate. Here we make recommendations for
require energy, but producing energy, especially future directions in scientific and philosophical
from fossil fuel, generates air pollution and research in the areas of climate change and air
greenhouse gases; the increasing effects of air pollution.
pollution and climate change make social devel- Since technology appears to be the main factor
opment unsustainable due to the clear threat of causing environmental degradation – climate
catastrophic effects. Therefore, it is critical to change and large-scale environmental damage
rapidly transition to a sustainable economy, for would not have been possible without technol-
the human species and the ecosystem as a whole. ogy – many philosophers have turned a critical
How much time do we have? A recent study eye on technology itself. Even though “philoso-
evaluates the risk of crossing a climate threshold, phy of technology and environmental ethics may
a point of no return into an Earth system with or may not be a match made in heaven” ([231],
significant sea level rise, higher than any point p. 445), finding a common ground between these
seen during the Holocene, and global tempera- two areas, and in addition science, may yield
tures warmer than in any interglacial in the past solutions to our environmental predicament.
1.2 million years [241]. This threshold is defined Both critical and more positive analyses of tech-
by triggering strong, intrinsic, biogeophysical nology are needed. For instance, further research
feedbacks that would be difficult to influence into the ecological modernization thesis, which
by human actions, “a pathway that could not be analyzes how technology and market forces are
reversed, steered, or substantially slowed”; cru- moving toward environmental healing and resto-
cially, it may be only decades away. There is a ration, might offer an alternative way forward
narrowing window of opportunity to take action, [231–233]. Since we will most likely need to use
and the longer we wait to limit greenhouse gas technology to capture CO2 (via DAC, CCS), tech-
emissions, especially carbon dioxide, the more nology is also a necessary part of solving the cli-
rapid the decarbonization will have to be. mate crisis, but further research into the ethical
It is tempting to believe that there will be an impacts of these technologies is needed to regulate
easy technological fix, but many authors and or rule out technologies which have unacceptable
expert panels have concluded that society must ethical implications. For instance, it may be pru-
transform itself. Since anthropogenic climate dent to favor some CCS technologies/techniques
change is an existential threat to Earth’s entire (e.g., reforestation, land use changes) over others as
ecosystem, risking our only home, every busi- they entail less risk and more direct co-benefits to
ness, community, government, and individual the environment [234–236]. The acceptable tech-
should take responsibility to tackle this problem nologies should integrate with the ecological mod-
as doing nothing and continuing with business as ernization thesis. Further research into the benefits
usual lead to serious injustice. The current situ- of developing these safer technologies compared to
ation is environmentally and ethically more risky technologies is needed [237, 238].
unsustainable. However, inspiring individual Considering that energy technologies are
and collective action remains our largest chal- responsible for the “worst sources of planetary
lenge. Nevertheless, with political action, pollution,” it is interesting that environmental eth-
broader public awareness, and better dissemina- icists have not spent more energy arguing against
tion of information to all stakeholders across the these technologies ([239], p. 391). This is partly
globe, we can realize the necessary changes that because the harms are so obvious and well-known
society ought to accommodate. and partly because their attention has instead been
318 Air Pollution and Climate Change: Sustainability, Restoration, and Ethical Implications

directed toward responding to arguments research in the relatively new area of rewilding
attempting to justify the continued use of pollut- [243] and investigation of assisted migration of
ing energy technologies [239]. There are three animals and how this might be used to alleviate
important directions for future research. First, sci- the impacts of climate change on the natural
entists should continue to develop environmen- world [244].
tally beneficial energy technologies (e.g., solar,
wind, hydro energies) using life cycle analysis to Acknowledgments Lina Boljka acknowledges support
detail their environmental impact. Second, envi- from National Science Foundation (NSF) grant number
ronmental ethicist should create a strong norma- AGS-1643167.
tive framework for our energy use. Third, leaders
need to better understand how to “use ethics to
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GWP The global warming potential is a relative
Aviation and Atmosphere measure of how much heat a greenhouse gas
traps in the atmosphere. It compares the
Hartmut Grassl amount of heat trapped by a certain mass of
Max Planck Institute for Meteorology, Hamburg, the gas in question to the amount of heat
Germany trapped by the same mass of carbon dioxide.
GTP The GTP is defined as the ratio between the
global mean surface temperature change at a
Article Outline given future time horizon following an emis-
sion (pulse or sustained) of a compound rela-
Glossary tive to a reference gas.
Definition of the Subject Radiative forcing When the balance between
Introduction the radiative energy received from the sun
Emissions of Climatically Relevant Substances and radiative energy leaving the Earth-
by Aviation atmosphere system is perturbed, e.g., by a con-
Aviation-Induced Cloudiness centration change of an absorbing gas, the
Changes of Air Chemistry by Air Traffic resulting imbalance is termed radiative forcing
Transport Sector’s Contribution to Future Climate that initiates climate change.
Change
Why Did International Air Traffic So Far Escape
from an Emission Reduction Policy?
Definition of the Subject
The European Directive to Include Air Traffic into
the Emission Trading Scheme
Commercial air traffic’s peculiarity, emissions
An Airline Emission Index
into the atmosphere mainly at cruising altitude,
Conclusions and Outlook
leads to changed impacts on global climate in
Bibliography
comparison to other modes of transport. This
entry concentrates on these differences but also
Glossary looks onto measures to reduce emissions, e.g., the
emission trading scheme in the European Union,
AIC Aviation-induced cloudiness is the sum of
and presents an airline emission index comparing
all changes in cloudiness associated with avia-
commercial airlines.
tion operations hence, it combines contrails
and so-called persistent contrail cover.
Airline emission index A measure to compare
the performance of different airlines with Introduction
respect to emissions relative to an ideal one.
Aviation Here: commercial air traffic. The exhaust of commercial and also military air-
Contrails Jet engine exhaust condensation trails craft needs – in comparison to the one from power
of airplanes. plants, cars, trucks, heaters in buildings, railway,
Emission trading A market-based approach ships, and burners in industry – a special discus-
used to control pollution by providing eco- sion, because of its main injection at cruising
nomic incentives for achieving reductions in altitudes, i.e., into the upper troposphere or
the emissions of pollutants. lower stratosphere from about 9 to 12 km height.

© Springer Science+Business Media, LLC 2012 327


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_555
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_555
328 Aviation and Atmosphere

This part of the Earth’s atmosphere is nearly all in a special report [17] entitled “Aviation and the
the time colder than 40  C, often it is with about Global Atmosphere” the air traffic influence on
70  C the coldest one in mid-latitudes in the global climate. In this report not only the effects of
lowest at least 60 km. Therefore, the water vapor air traffic on atmospheric composition and on
concentration in these layers must be lower by climate were assessed but also projected into the
typically 3–4 orders of magnitude than at the future using air traffic growth scenarios. These
Earth’s surface in low- and mid-latitudes. Hence, results and new findings have entered the third
several emissions of an aircraft besides carbon and fourth full IPCC assessments [19–21];
dioxide, for example unavoidable water vapor, in hence, the hitherto known facts have been pre-
principle avoidable nitrogen oxides can lead to a sented to the political arena and have led to first
considerable disturbance of the radiation budget hesitating measures to reduce emissions, like the
of the planet. First, via the formation of rather European Union’s decision in 2009 to include air
persistent condensation trails, an ice cloud, during traffic into the European emissions trading
frequently favorable meteorological conditions, scheme, to become effective on January 1, 2012.
and second, via the formation of ozone around This entry will start with the greenhouse gas
cruising altitudes because of the nitrogen oxide emission history of air traffic in section “Emissions
emissions. of Climatically Relevant Substances by Aviation,”
In addition, the growth rate of commercial air influenced both by the above average growth rate
traffic was on average above the one for the global of this economic sector but also by the strong
gross economic product, leading to a growing increase in fuel use efficiency per passenger kilo-
relative contribution of air traffic to the changed meter, which has been stronger than for road traffic
composition of the atmosphere. Only very and much stronger than for railways. This section
recently did the growth rate no longer surmount will also include projections of future air traffic
the growth rate of world economy as strong as greenhouse gas emissions using estimates from
before. scenarios of IPCC. It continues with the knowledge
However, it was only in the late 1980s when about long-lasting contrails and their dependence
first publications dealt with air traffic’s potential on favorable meteorological conditions in section
influence on climate. Earlier, in the early 1970s, “Aviation-Induced Cloudiness.” This section will
the planned supersonic aircraft fleet in the USA also include cirrus clouds formed or transformed
had led to an assessment of the impact of such because of air traffic, existing besides the easily
aircraft on the stratospheric ozone layer. At this detectable linear contrails. Section “Changes of Air
time the consequences of the emission of the trace Chemistry by Air Traffic” is then devoted to
gas nitrogen dioxide (NO2) were the main reasons changes in air chemistry caused by air traffic emis-
for the investigations, because it is strongly sions. Section “Transport Sector’s Contribution to
involved in stratospheric ozone chemistry leading Future Climate Change” extrapolates into the
to ozone depletion at altitudes above about 20 km twenty-first century with known scenarios of
but to ozone increases in the troposphere and human behavior. It follows the section on “Why
lowest stratosphere. did International Air Traffic So Long Escape an
In 1996, the steadily growing public and sci- Emissions Trading Scheme?” The first attempt of
entific discussions on air traffic and its potential the European Union to include international air
effect on global climate have stimulated the Inter- traffic into an emissions trading scheme will be
national Civil Aviation Organization (ICAO), the described in section “The European Directive to
UN specialized agency that has global responsi- Include Air Traffic into the Emission Trading
bility for the establishment of standards, Scheme.” The second last section on “An Airline
recommended practices, and guidance on various Emission Index” will present essentials of an air-
aspects of international civil aviation, including line index that includes a ranking concerning car-
environmental protection, to ask the Intergovern- bon dioxide and nitrogen oxides emissions,
mental Panel on Climate Change (IPCC) to assess published very recently. The last section will
Aviation and Atmosphere 329

provide the conclusions and also present avenues the Emission Trading Scheme”); second, they
how to reduce or even to avoid air traffic emissions allow the assessment of trade-offs between
changing climate. changes in emissions resulting from technological
or operational developments; third, they serve for
comparisons of different environmental impacts
Emissions of Climatically Relevant caused by the different transport sectors and thus
Substances by Aviation help in traffic policy making. Usually, the CO2
emission, common to all transport sectors, is used
The estimates of climate effects of air traffic as a reference. Therefore, all other emissions have
depend totally on a reliable time-dependent emis- to be transformed into their “CO2-equivalents.”
sion inventory on global scale for the past, the Ideally, the same equivalent CO2 emissions
present, and the future. The major research project should produce the same climate effect, regardless
QUANTIFY of the European Union’s Sixth of their shares in the exhaust or after chemical
Framework Research Programme (finished very transformation in the atmosphere. This is, how-
recently) has established such a consistent global ever, only an approximation of reality, because
three-dimensional air transport emission inven- most of the non-CO2 emissions from the different
tory for greenhouse gases, particles, and precursor transport sectors, and especially aviation, are
gases of other greenhouse gases and for aerosol short-lived substances with often rather regional-
particles for the year 2000 (also for all other ized concentrations. In addition, these short-lived
modes of transport), and has developed estimates substances are all not included in the Kyoto Pro-
of future emissions for the years 2020, 2050, and tocol basket of solely long-lived greenhouse
2100. The example for air traffic is shown in Fig. 1 gases.
and Table 1, taken from [25]. The challenges in developing generally
Since different substances in the aircraft accepted metrics are strongly magnified by the
exhaust have very different concentrations and inclusion of short-lived species. One first diffi-
also very different radiative properties, a common culty concerns the choice of an appropriate struc-
scale must be created for a just assessment of the ture for the metric. Should effects of an emission
environmental burden caused by different aircraft today be integrated over 10, 20, 50, 100, or even
and flight types. The next subsection will deal 200 years? Or should the impact, e.g., the global
with it. mean surface temperature increase after a certain
time period, be used as a measure? The first
Creating a Common Scale for the Climate approach is the most frequently used one, charac-
Effects of Air Traffic Emissions terized by the global warming potential (GWP)
The entire motorized transport sector (road traffic, and the one adopted in the Kyoto Protocol. The
shipping, rail, aviation) emits a wide variety of second one, called global temperature change
gases and aerosols into the atmosphere, with dif- potential (GTP), strongly reduces the influence
ferent characteristics, which either influence cli- of short-lived emissions if the same long time
mate directly by their radiative properties or horizon is used as typically for GWP. In view of
indirectly via chemical and physical processes the lifetime (defined as the time for the decay of
influencing concentrations of other climatically the concentration of an emitted pulse of a sub-
relevant substances. We need metrics that allow stance to 1/e) in the atmosphere of an anthropo-
these emissions to be placed on a common scale in genic addition of CO2, which is well above
terms of their impact on global climate. The appli- 100 years, 100 years have been chosen for the
cations of such metrics are manifold: First, they Kyoto Protocol, although there was no specific
have served and will serve as basic information in argument put forward for this time horizon by
negotiations for international agreements and IPCC. A further challenge is the quantification
emission trading schemes (see section “The of input parameters for the metric, originating in
European Directive to Include Air Traffic into the uncertainty of atmospheric processes. For
330 Aviation and Atmosphere

Aviation Fuel Use and RPK


300 5 0.8
Fuel Use

RPK annual change (1012 RPK yr−1)


Sausen and Schumann (2000) SARS
250 IPCC Scenario Fa1 WTC attack
4 0.6
International Energy Agency (IEA) Asian crisis
Fuel Use (Tg yr−1)

200 RPK Gulf crisis

RPK (1012)
RPK annual change 3
0.4
150 Oil crisis
Oil crisis
2
100 0.2

1
50
0.0

0 0
1940 1950 1960 1970 1980 1990 2000 2010
Year

Aviation CO2 Emissions


7.0
30
Anthropogenic CO2 6.0
Aviation CO2 (x10)

Aviation CO2 fraction (%)


CO2 emission (103Tg yr−1)

25
Aviation CO2 fraction
5.0
20
4.0

15
3.0

10 2.0

5 1.0
(x10)

0 0.0
1940 1950 1960 1970 1980 1990 2000 2010
Year

Aviation and Atmosphere, Fig. 1 Upper panel: Avia- revenue passenger kilometers (RPK) (near right-hand
tion fuel usage beginning in 1940 from Sausen and Schu- axis). (Source: ICAO traffic statistics from http://www.
mann [32] and extended with data from IEA [16] and the airlines.org/economics/traffic/World/Airline/Traffic.htm.
IPCC Fa1 scenario of Henderson et al. [13]. The arrows Accessed 19 Sept 2007) and the annual change in RPK (far
indicate world events that shortly threatened global avia- right-hand axis [Note offset zero]). Lower panel: Growth in
tion use: the oil crises of the 1970s, the Gulf war crisis in CO2 emissions in Tg CO2/year for all anthropogenic activ-
the early 1990s, the Asian financial crisis in the late 1990s, ities and from aviation fuel burn (left-hand axis), and the
the World Trade Center (WTO) attack in 2001, and the fraction of total anthropogenic CO2 emissions represented
global health crisis brought about by the severe acute by aviation CO2 emissions (%) (right-hand axis). Note
respiratory syndrome (SARS). Also shown is the growth scaling of aviation CO2 emissions. (Source: Lee et al. [24])
in air passenger traffic from 1970 to 2007 in trillions of

example: How much of the nitrogen oxide emis- where for example the emission height is decisive
sion remains available for the formation of ozone for the formation of a long-lasting contrail. The
in the troposphere, a potent but short-lived green- QUANTIFY project has evaluated existing met-
house gas of the atmosphere? On top of these rics and has introduced new concepts (for details
challenges we have to face the dependence of see Fuglestvedt et al. 2009). All these metrics
the effects on the location of the emissions for have been evaluated for emissions from the trans-
all short-lived substances, severest for air traffic, port sector both in terms of integrated radiative
Aviation and Atmosphere, Table 1 Estimations of historical and current emissions from inventory models, 1990–2005
Aviation and Atmosphere

Military fuel Total fuel Distance (civil, NOxTgNO2/ EINOxg NOx/kg


Year Inventory Civil fuel Tg/a Tg/a Tg/a Total CO2Tg/a 109 km) a fuel
1990 FAST 105 n.c. 331 15.7 1.42
1992 NASA 114 25.5 139 359 n.c. 1.44 12.6 (12.0)
1992 ANCAT/ 114 17.1 131 360 n.c. 1.60 (1.81) 14.0 (13.8)
EC2
1999 NASA 128 n.c. 404 25.8 1.69 13.2
(134 inc. charter) (423 inc. charter)
2000 TRADEOFF 152 17.1a 169 480 25.1 1.95 (2.15) 12.7 (12.9)
2000 FAST 152 n.c. 480 26.9 2.03 13.4
2000 SAGE 181 n.c. 572 33.3 2.51 13.8
2001 SAGE 170 n.c. 536 31.9 2.35 13.8
2002 SAGE 171 n.c. 539 32.6 2.41 14.1
2002 AERO2K 156 19.5 176 492 (553) 33.2 2.06 (2.24) 13.2 (12.7)
2003 SAGE 176 n.c. 557 34.5 2.49 14.1
2004 SAGE 188 n.c. 594 37.0 2.69 14.3
2005 SAGE 203 n.c. 641 40.7 2.90 14.2
References: “FAST,” Lee et al. (2005); “NASA,” (Baughcum et al. [3]) and (Sutkus et al. [33]); “ANCAT/EC2,” Gardner et al. [12]; “TRADEOFF,” Gauss et al. (2006); “SAGE,”
Kim et al. [22]; “AERO2K,” Eyers et al. [10]
a
Military emissions adopted from other study; n.c. not calculated, brackets include military emissions
331
332 Aviation and Atmosphere

forcing (When the balance between the radiative temperature change that will be caused by the
energy received from the sun and radiative energy emissions of the year 2000 for all transport
leaving the Earth-atmosphere system is perturbed, modes for four chosen time horizons. In order to
e.g., by a concentration change of an absorbing calculate surface air temperature changes ideally a
gas, the resulting imbalance is termed radiative coupled Atmosphere/Ocean/Land-Model has to
forcing. It can be calculated by changing the con- be run. If this model gets as an input the three-
centration of the substance and keeping all other dimensional emission distribution of air traffic, it
parameters fixed. In the real climate system, the must not lead to the same relation of different
imbalance stimulates climate change trying to transport sectors as the radiative forcing calcula-
restore the energy balance of the planet.) (GWP) tion, because it adds the processes at the ocean air
and the net surface temperature change (GTP) of interface that are neglected in the chemical trans-
the various transport modes for several time hori- port model used for the radiative transfer calcula-
zons. For the series of tasks to be performed tions because then sea surface temperature is
starting from transport sector emissions and end- fixed. Figure 4 clearly demonstrates that emis-
ing at climate impacts, see Fig. 2 [30]. sions from road transport in 2000 are dominating
For metrics, very different approaches are pos- the traffic sector impact on surface temperature,
sible. One can look at the current radiative or with aviation as the second largest contributor to
temperature forcing relative to the preindustrial surface air temperature changes. For time hori-
era or at the temporal development of the forcing zons of 20 and 100 years, the net warming from
over several decades for a pulse emitted today, or road transport is seven and six times larger than
to the forcing for a sustained emission or a more the net warming from aviation. This is approxi-
elaborate emission scenario. Figure 3 shows the mately the same ratio as the ratio between the CO2

Transport Emissions and Scenarios


Chain of Impacts
temporal evolution, 2D/3D distribution

Regional Dilution and Processing


effective emissions

Large-scale Chemistry Effects Cloud Processes


atmospheric composition cloud cover and optical properties

Radiative Forcing
temporal evolution, 3D distribution

Metrics
Climate Change
simple measures
new climatic state
to quantify impacts

Climate Impacts
changes in health and economy

Aviation and Atmosphere, Fig. 2 From emissions to QUANTIFY science tasks are printed in blue, output in
climate change and climate impacts (a schematic). Only the black. (Source: QUANTIFY [30])
main fluxes of information are indicated by arrows.
Aviation and Atmosphere 333

4.0

Road
3.0 Ship
Air

2.0 Rail D
Rail I
dT (mK)

1.0

0.0

−0.0

−2.0
20 yr 40 yr 60 yr 100 yr

Aviation and Atmosphere, Fig. 3 Contribution from a time horizons (20, 40, 60, and 100 years), including the
1-year pulse of current (year 2000) emissions to net future uncertainties, here given by the 1-sigma level. (Source: Lee
temperature change (mK) for each transport mode for four et al. [25])

emissions from these sectors; thus, mainly CO2 emission reduction targets. Additionally, the
controls the climate response on timescales impact of the transport sector on climate is at
beyond 10 years for the GTP metric. The net least as complex as for other sectors like heating
temperature effect of shipping changes sign from of houses, because it also involves more strongly
negative for a time horizon of 20 years to positive air chemistry and modification of cloudiness than
for the longer time horizons. Both rail sectors’ the emissions from shipping, and in addition
contributions seem small, but added together direct cloud formation (contrails) by air
they reach 15–30% of the effect of aviation for traffic. Thus an assessment of the full climate
time horizons between 20 and 100 years. The effects of the transport sector and especially avia-
results in Fig. 3 show well how the relative impor- tion has to take into account more than just the list
tance of the different transport sectors changes of gases in the Kyoto Protocol. The transport
depending on the time perspective. sector can impact on climate in the following
ways:
Climate Change Contribution of Carbon
Dioxide Emissions from Air Traffic – By direct emissions of greenhouse gases,
The entire transport sector contributes about one mainly CO2, but also by nitrous oxide (N2O)
third of the total global anthropogenic CO2 emis- and some halocarbons
sions. The annual growth rate of transport-related – By emissions of precursors of ozone, such as
greenhouse gas emissions is larger than for other nitrogen oxides (NOx), carbon monoxide
mature industrial sectors. In view of the United (CO), and volatile organic compounds (VOCs)
Nations Framework Convention on Climate – By emissions of aerosol particles or their pre-
Change (UNFCCC), its Kyoto Protocol, and pos- cursor gases, in particular black carbon (soot)
sible follow-up protocols, this high rate of and sulfur dioxide (SO2), which are directly
increase creates the severest problem for the avi- and indirectly (via cloud formation and cloud
ation sector, when trying to achieve forthcoming modification) radiatively and chemically active
334 Aviation and Atmosphere

Aviation Fuel Emissions

2500
FAST (B2, A1, A1)
CONSAVE (ULS, RPP, FW, DtE)
2000 IPCC (Fe1, Fa1, Fc1)
Fuel Emissions (Mt CO2 yr−1)

ANCAT/EC2 (1992, 2015)


NASA (1992, 1999, 2015)
AERO-2K
1500
SAGE

1000

500 Sausen and Schumann (2000)


IPCC Scenario Fa1
International Energy Agency (IEA)
FAST-A1(1)
FAST-B2(t1)
0
1990 2000 2010 2020 2030 2040 2050
Year

Aviation and Atmosphere, Fig. 4 Historical and usage because all kerosene sales are included. The Sausen
present-day inventories, and future projections of civil and Schumann [32] data are also based on IEA. The solid
aviation CO2 emissions from a variety of sources: (dashed) lines for FAST-A1 (B2) scenarios (evaluated with
AERO2K [10]; ANCAT/EC2 [12]; CONSAVE [5]; FAST the t1 technology option) and the IPCC Fa1 scenario also
(Owen and Lee 2006); IPCC [17]; NASA [3, 4, 33]; SAGE account for all fuel sales in order to be consistent with the
[22]. The open symbols indicate inventory analysis and the IEA values ending in 2005. In the figure legend, the FAST,
closed symbols indicate projections. Also shown are the CONSAVE, and IPCC symbols are shown in an order that
CO2 emissions implied by IEA fuel sales statistics matches the scenario labels in the parentheses in each case.
[16]. The IEA data represent the total of civil and military (Source: Lee et al. [24])

– By directly triggering additional clouds (e.g., constraints clear information on the climatic
contrails and contrail cirrus) impact of different transport emissions is needed.
Here we concentrate on aviation, a smaller part
On the other hand, the global and economic with respect to goods and passengers transported,
system is largely dependent on an efficient trans- but with many climatically relevant facets because
port system. This dependency has grown during of its already mentioned main emission height of
recent decades not only because of an increasing about 10 km.
world population but mainly because of globali- Each kilogram of aviation fuel, overwhelm-
zation. Life style and the availability of cheaper ingly kerosene, when burned in an engine, must
transport (mainly because of lack of internaliza- lead to 3.16 kg carbon dioxide (CO2) and 1.0 kg
tion of external costs) in developed and develop- of water vapor (H2O). These unavoidable emis-
ing countries are also enhancing demand. Further sions are two major reasons of an air traffic influ-
very strong growth of the transport sector is ence on the radiative transfer in the atmosphere,
expected in developing countries. In the long but not the only ones. The first one is nearly
term, a sustainable transport system is needed completely independent of the place where the
that satisfies the demands of economy and popu- emission occurs, because of the long lifetime
lation while following the constraints of climate of anthropogenic carbon dioxide being well
change policy measures. In order to meet these above 100 years and thus resulting in a globally
Aviation and Atmosphere 335

well-mixed anthropogenic carbon dioxide con- Aviation-Induced Cloudiness


centration addition. Aviation CO2 will contribute
to the entire CO2 burden of the atmosphere like There exist two types of impact on clouds caused
all other emissions into the atmosphere close to by particle emissions from traffic. First, the parti-
the surface of the Earth. For the second major cle emissions can cause the formation of clouds
emission, H2O, the point where it is emitted is that would not form naturally. The most promi-
decisive: At the surface this addition is negligible nent example is jet exhaust condensation trails
in comparison to the natural fluxes of water, but (contrails). This cloud circumvents the lack of
not so at about 10 km height at a water vapor so-called freezing nuclei in the rather clean and
mixing ratio ranging from about 100 ppmv to as cold upper troposphere. The large emission of
low as 5 ppmv. Flying by 1 km higher or lower in water vapor (1 kg/l of kerosene burned) in the
heights around the tropopause (the interface hot exhaust plume together with the additional
between the troposphere and the stratosphere; particles, also within the exhaust plume, leads to
typically at 10 km height in mid-latitudes), how- cloud droplet formation, which rapidly freeze by
ever, can often avoid a long-lasting linear con- mixing with the ambient air. If the flight corridor
trail (for more see section “Aviation Induced of an aircraft is supersaturated with respect to an
Cloudiness”). ice surface, the contrail formed will survive and
At present the global consumption of aviation expand depositing all the supersaturated water
fuel per year is equivalent to an emission of about vapor onto the contrail ice particles.
0.2 Gigatonnes of Carbon per year (GtC/a), A second type of anthropogenic cirrus clouds,
which is about 2% of the entire anthropogenic which is much more difficult to observe, are aerody-
carbon emissions, when emissions from land use namic contrails involving a sequence of effects: The
change (deforestation being the main contribu- emitted particles first get mixed with the background
tion to it) are included. If only counting the aerosol particles and later – when the mix of anthro-
emissions originating from the burning of fossil pogenic and natural aerosol particles becomes
fuels and cement production, the percentage of involved into cloud formation processes – the parti-
aviation emissions grows to about 2.4. Figure 4 cles emitted by air traffic will affect cloud formation,
presents an estimate of the time series of global cloud evolution, cloud properties, and eventually
CO2 emissions by aviation since 1990 and precipitation. Also most so-called ship tracks belong
extrapolation attempts by different groups as to this category. A variant of this second aviation-
compiled by Lee et al. [25]. Besides an overall induced cloud type, the hypothetical soot cirrus, is of
growth of the emissions, it is evident that differ- interest here. It describes an ice cloud that is strongly
ent scenarios of future economic development affected by soot particles emitted by aircraft. To
and technological progress lead to very different estimate the effect of aerosol particles emitted by
emission paths. air traffic (often soot) on ice clouds is difficult,
It is also interesting to compare the different because of the presence of various pathways to ice
modes of transport with respect to emissions per formation. In clean unpolluted air, ice clouds form
passenger and per tonne transported. Here again via homogeneous nucleation, while in polluted air,
results from the recently finished major European like in air traffic corridors, heterogeneous nucleation
Union’s research project QUANTIFY [30], to might be dominant. Because there exist always very
which the author has contributed, are presented: many other aerosol particles, which become solution
Aviation is the strongest contributor to radiative droplets at higher relative humidity over a water
forcing by CO2 emissions per passenger kilometer surface (about 100/cm3), an ice cloud forming
in comparison to road traffic, shipping, and rail. homogeneously has a high number concentration
As clearly visible from Fig. 6, this is not the case of ice crystals. In contrast, heterogeneous ice
for freight transport, where road traffic contributes cloud formation is a very selective process: Only
similarly to radiative forcing per tonne-kilometer about every millionth particle is an appropriate ice
(Fig. 5). forming nucleus (IN). Thus, ice clouds forming
Specific Climate Impact of Freight transport modes over various time horizons
336

8.00 8.00
10–15 K GTP5 1.60 1.60 0.80 0.80
per tkm GTP20 10–15 K GTP50
7.00 7.00 per tkm
1.40 1.40 0.70 0.70

6.00 6.00
1.20 1.20 0.60 0.60
CO2 + SLCF CO2 + SLCF CO2 + SLCF
5.00 CO2 5.00 CO2 CO2
1.00 1.00 0.50 0.50
0.49
4.50
4.00 4.00 0.80 0.80 0.40 0.40

3.00 3.00 0.60 0.60 0.30 0.30


0.31

2.00 2.00 0.47 0.20 0.20


0.40 0.40
0.40

1.00 1.00 0.20 0.20 0.10 0.10


0.61 0.07
0.00 0.00 0.00 0.00 0.00 0.00

−1.00 −1.00 −0.20 −0.20 −0.10 −0.10


Aircraft LDT HDT Rail Ship Aircraft LDT HDT Rail Ship Aircraft LDT HDT Rail Ship

Specific Climate Impact of Passenger transport modes over various time horizons

1.00 1.00 0.25 0.25 0.10 0.10


GTP5 GTP20 GTP50
10–15 K 10–15 K 10–15 K
per Pkm per Pkm per Pkm
0.80 0.80 0.20 0.20 0.08 0.08
CO2 + SLCF CO2 + SLCF CO2 + SLCF
CO2 CO2 CO2
0.07
0.60 0.60 0.15 0.15 0.06 0.06

0.05
0.45
0.40 0.40 0.10 0.10 0.04 0.04
0.08
0.03
0.07
0.20 0.20 0.05 0.05 0.02 0.02 0.02
0.05 0.02

0.11
0.10 0.02
0.06 0.02
0.00 −0.03 0.00 0.00 0.00 0.00 0.00

−0.20 −0.20 −0.05 −0.05 −0.02 −0.02


Car Aircraft 2Wheel Bus Rail Car Aircraft 2Wheel Bus Rail Car Aircraft 2Wheel Bus Rail
Aviation and Atmosphere

Aviation and Atmosphere, Fig. 5 Temperature change caused by emissions in the The columns differentiate the impact when all short- and long-lived climate forcings
year 2000 after 5, 20, and 50 years: For passenger transport modes (upper panels) per (in black) are summed up and when only CO2 (in color) is considered. (Source:
passenger kilometer, for freight transport modes (lower panels) per tonne-kilometer. QUANTIFY [30])
Aviation and Atmosphere 337

Aviation and N. America, Europe, N. Atlantic, N. Pacific


Atmosphere,
Fig. 6 Averaged cirrus HIGH air traffic corridors
cloud trends over high and LOW air traffic corridors
low air traffic regions in
North America, Europe,
North Atlantic, and North

Anomalies (%)
4 (+0.6)
Pacific. (Source:
QUANTIFY [30]) 0

−4

Anomalies (%)
4
(−0.3)
0
Differences (%)

4 −4

0
(+0.9)
−4

1984 1988 1992 1996 2000 2004 2008

predominantly by heterogeneous nucleation have a vicinity, in particular when these contrails spread
small number concentration of ice crystals. IN injec- and eventually form the so-called contrail cirrus,
tion into a clean environment leads to heterogeneous because these two ice cloud types compete for the
ice crystal formation before homogeneous freezing same space and for the same supersaturated water
can occur. Thus the ice cloud changed by air traffic vapor.
has less but bigger crystals than a cloud that would Aviation-Induced Cloudiness (AIC) has been
have formed purely homogeneously. If heteroge- defined as the sum of all changes in cloudiness
neous ice formation is dominant as in a polluted air associated with aviation operations [20]; hence, it
mass, the addition of IN can lead to more but smaller combines jet exhaust condensation trails, often
ice crystals. This simplified picture has to be modi- abbreviated as contrails, and so-called persistent
fied: First, whether heterogeneous or homogeneous contrail cover. The assessment of the latter is very
freezing dominates depends not only on the relative difficult, because AIC may be indistinguishable
number of the respective aerosol particle types but from background cirrus cover. This was the rea-
also on vertical wind speed (determining adiabatic son for IPCC [20] not to give a best estimate of
cooling rates). Second, IN from various sources may AIC amounts and its associated radiative forcing.
have a spectrum of threshold supersaturations over The value given in IPCC [20] for emissions until
an ice surface. These thresholds depend on temper- 2005 and a time horizon of 100 years, namely
ature and on particle coating. Third, ice formation in 0.03 W/m, is above the radiative forcing of
supersaturated air with respect to an ice surface is 0.025 W/m for CO2 alone. Thus more than a
difficult to be represented in large-scale models, factor of 2 would be needed, if the total air traffic
because a supersaturated state is not uniquely related influence on radiative forcing has to be accounted
with a cloudiness state. Hence first model simula- for, knowing only the fuel burned and excluding
tions like those by Penner et al. [29] have therefore additions related to air chemistry. Have these
rather the value of highlighting the problems than values given by IPCC in 2007 changed during
yielding firm results. recent research? Yes, but earlier relations between
But also natural cirrus clouds can be affected the impacts by greenhouse gases and cloudiness
by contrails formed within them or in their changes (caused by contrails and contrail cirrus)
338 Aviation and Atmosphere

have not been altered significantly [25]. There is, Much better information on the statistics of opti-
however, a discussion about a new potential influ- cal thicknesses of single contrails, including the
ence of aviation on cloudiness, the so-called soot variation over their life cycle, can be obtained now
cirrus (as already discussed above), relating to from a contrail tracking algorithm that has been
effects of changed optical properties of ice clouds developed during QUANTIFY [34, 35]. The com-
into which soot from aircraft exhaust is mixed and bination of such a tracking algorithm, based on
which may act after transformations in the atmo- satellite data from a polar orbiter (MODIS on
sphere as ice nuclei. The related model estimates NASA’s Aqua and Terra satellites) and a geostation-
[26, 29] diverge so strongly (see also the values ary one (MSG operated by EUMETSAT), with a
given for soot cirrus in Table 2) and they are not numerical contrail plume model for which first
backed by observations that much more research developments have been made in the project allows
is needed before conclusions on a changed avia- to extend the observable fraction of a contrail life
tion policy could be drawn. In this context, it is too cycle in both directions, that is, from formation up to
early to ask whether aviation’s influence on radi- its end. There are, however, not yet trends available
ative forcing might even change the sign. for a larger area with intense air traffic over Europe.
Man-made changes in cirrus cloud cover can be
detected by comparing cirrus trends over adjacent
regions with dense and nearly no air traffic. Some Changes of Air Chemistry by Air Traffic
exemplary long-term trends are shown in Fig. 6,
taken from QUANTIFY [30]. It is evident that cirrus The present and future impacts of emissions from
cloud coverage increases more or decreases less in aviation are typically evaluated using several
regions with dense air traffic compared to regions global atmospheric chemistry models in order to
with little air traffic. This could be considered a obtain not only a quantification of the impact of a
signature of increasing air traffic in the past specific transport sector on global atmospheric
20 years. Such preliminary estimates from the dif- composition but also an estimate of the associated
ferences in cirrus cloud cover, however, suggest an model uncertainties. For the QUANTIFY project
effect on radiative forcing of the order of only such an assessment included chemistry transport
6 mW/m for an assumed optical thickness of 0.4 models and chemistry-climate models. For these
for the cirrus clouds with air traffic influence. simulations the global emission inventory

Aviation and Atmosphere, Table 2 Year 2000 radiative forcing (in mWm 2) for each transport sector and each
forcing mechanism relative to pre-industrial times, together with uncertainties. SWV is stratospheric water vapor
Road Ship Air Rail
CO2 131  15 34  6 20  3 23  7
Ozone 32  9 24  6 18  3 2  0.4
CH4 lifetime 74 19  2 51 1  0.4
CH4 – ozone 32 81 2  0.5 0.3  0.2
SWV methane 1  0.7 3  0.7 1  0.3 0.1  0.1
SWV direct 1  0.2
CFCs/HFCs 28  3
Stratospheric ozone 24
Sulphate aerosol 94 26  11 1  0.4 1  0.3
Black carbon aerosol 44  17 21 0.3  0.1 1  0.3
Organic carbon aerosol 21 1  0.5 0.5  0.3
Indirect aerosol effect 6  111 49  209 127  128 0.5  10
Contrails 7 ( 4, +6)
Aviation induced cirrus 21 ( 9, +17)
Aviation and Atmosphere 339

EDGAR32FT2000 was used for anthropogenic rather uncertain. Overall, aviation remains the
emissions, with the transport sectors’ emissions sector with strongest additional effects besides
replaced by improved estimates for the present the basic CO2-related radiative forcing. The line
and for the IPCC A1 and B1 scenarios (2025, named indirect aerosol effect in Table 2 needs a
2050) from the new QUANTIFY inventory. The special remark. It is to a large extent due to model
A1 scenario represents a world of very rapid eco- calculations using comparably crude parameteri-
nomic growth, especially in developing countries, zations for the aerosol influence on cloud droplet
and rapid introduction of new and more efficient number and on absorption of solar radiation by
technologies. The B1 scenario assumes rapid soot. This research is still in its infancy as shown
introduction of clean and resource-efficient tech- by the huge error bars, and one should not argue
nologies, and is considered to be far more opti- like very often lobbies would do that any climate
mistic with respect to environmental policy policy measure concerning aviation has to be
making than the A1 scenario. The results from postponed until small error bars are reached for
the scenario calculations for the impact of ship- all entries. What is needed is a flexible reaction
ping on ozone in the lower troposphere (surface to should major changes become evident.
800 hPa) point to a significantly increasing impact
on ozone from the shipping sector, if emissions
evolve according to the A1 scenario, while the B1 Transport Sector’s Contribution to
scenario leads to a much smaller increase. The Future Climate Change
results obtained for shipping are particularly inter-
esting in the sense that the impacts on the Using a coupled atmosphere/ocean/land-model
hydroxyl radical (OH) and thus on methane and the A1B scenario of IPCC as well as account-
(CH4) were larger than anticipated. The reduction ing for six different forcings (CO2, CH4, O3, and
of the global atmospheric lifetime of methane due aerosols for all sectors, CFCs and HCFCs for road
to ship emissions was about a factor of 2–3 larger traffic, and contrail formation for aircraft) Olivie
than that due to road emissions, and about a factor et al. [28] found: In the year 2100, the warming
of 4 larger than that due to air traffic emissions from all transport sectors due to the CO2 increase
[15]. This is a consequence of the more pristine reaches about 0.5 Kwith the largest contribution
chemical conditions over the oceans and the from road traffic (0.3 K). The non-CO2 impact
slightly different mix of emissions from ships. from air traffic is larger than its CO2 impact, the
As a result, the net impact on radiative forcing of latter amounting to 0.15 K at 2100. It is caused by
ozone and methane perturbations from shipping is an enhanced O3 production (compared to road and
negative, corresponding to a more or less globally ship traffic) due to the altitude of the NOx emis-
uniform cooling. This adds up to the cooling via sions, and by the positive direct radiative forcing
widespread cloud modifications caused by ship from linear contrails and contrail-induced cirrus.
emissions of sulfate aerosols [27]. In contrast, Because the total anthropogenic global tempera-
the atmospheric chemistry influence on radiative ture increase is about 3 K in 2100 with a contri-
forcing by aviation remains strongly positive. bution of about 0.65 K from the transport sector,
The radiative forcing of aviation in the year with 0.5 K due to CO2 impact and 0.15 K due to
2000 in relation to all other transport sectors is non-CO2 impact dominated by aircraft traffic, the
given in Table 1 (QUANTIFY [30]. Peculiarities transport sector contributes slightly less than its
in comparison to other modes of transport emerge: share in total energy use. This reduced impact is
First, the radiative forcing is nearly doubled by caused by both the reduction in methane lifetime
inclusion of the effect of ozone formation due to and comparably low N2O and CH4 emissions. The
the emission of nitrogen oxides at cruising alti- warming is in general more pronounced at high
tudes. Second, aviation-induced cloudiness in latitudes, but the signal there is strongly
form of contrails and contrail cirrus adds substan- influenced by the timing of the Arctic sea-ice
tially to the positive radiative forcing, however, is melting, which is quite uncertain.
340 Aviation and Atmosphere

It is clear from the above scientific findings that no progress at COP 2 in Geneva. At COP 3 in Kyoto
international air traffic cannot be excluded from at least the domestic part of aviation and shipping
climate policy making, although it managed to was integrated into national reduction targets, and
remain largely unaffected so far. for international flights the above mentioned respon-
sibility of ICAO was decided. Although SBSTA
continued to discuss methodologies to allocate
Why Did International Air Traffic So Far emissions, it was without any agreement so far.
Escape from an Emission Reduction ICAO often reported about progress in its delibera-
Policy? tions, but never presented a real proposal to SBSTA
that could have been tabled at the next COP. Already
When the Kyoto Protocol has been formulated in in 1996 ICAO had requested that IPCC should
December 1997 the following sentence in its Arti- prepare a report on the impact of aircraft engines
cle 2.2: “Parties included in Annex 1 (these are on the atmosphere. In 1999, this first report on a
the industrialized countries with emission reduc- specific industry sector named Aviation and the
tion commitments under the Kyoto Protocol) shall Global Atmosphere had been published [17] that
pursue limitation or reduction of emissions of clearly stated:
greenhouse gases not controlled by the Montreal
Protocol from aviation and marine bunker fuels, • Since 1960, aviation passenger traffic had
working through the International Civil Aviation grown rapidly by 9% per year and was esti-
Organization (ICAO) and the International Mar- mated to grow by 5% per year between 1990
itime Organization (IMO), respectively” started and 2015.
it. In other words: The reduction of emissions • Already in 1992, chosen as the base year for
from international air traffic and international the report, aviation accounted for 2% of total
shipping has to be handled by two United Nations anthropogenic CO2 emissions.
bodies often said to be closer to the respective • Including other effects of aviation on the atmo-
industries than to the responsibility for entire soci- sphere, e.g., contrails and contrail cirrus, about
ety. Hence, about 6% of global emissions from the 3.5% of the total anthropogenic radiative forc-
use of fossil fuels or up to 15% of all transport ing in the base year 1992 of the report were due
emissions factually escaped from any regulation to aviation.
by the UNFCCC and its Kyoto Protocol. Nineteen
years after the signature under UNFCCC at the Policy options were given as well including
Earth Summit in Rio de Janeiro we are still with- more stringent engine regulations, removal of sub-
out a global legal instrument for any mitigation sidies, environmental levies, and emission trading
measure to reduce aviation fuel’s climate impact. schemes. IPCC also acknowledged that ICAO had
Why is it so? The following lines use a historical already started to assess the need for aircraft emis-
account given by EFTE [9]. At the first Conference sion standards at cruising altitude in addition to the
of the Parties (COP 1) to UNFCCC in Berlin 1995 already existing standards for nitrogen oxides. To
its Subsidiary Body on Scientific and Technical make a long story short: At present, 12 years later,
Advice (SBSTA) was requested to examine the international air traffic is not included in any bind-
allocation and control of emissions from interna- ing measure for climate protection policy, i.e.,
tional bunker fuels, the term used for shipping first ICAO was unsuccessful to perform as requested
and then also for aviation. COP 1 had identified by the international community.
eight options for SBSTA to be considered prior to
COP 2. SBSTA rejected three options: first, alloca-
tion in proportion to national greenhouse gas emis- The European Directive to Include Air
sions; second, allocation according to the country of Traffic into the Emission Trading Scheme
origin of the passenger/cargo; and third, according
to the actual location of the emission. No agreement At least for the European Union the time for an
could be reached for the remaining five. There was escape of the international air traffic from an
Aviation and Atmosphere 341

emissions trading scheme will end. The directive 5. Restriction to carbon dioxide emissions, because
(Dir 2008/101/EC) to include aviation into the EU other emissions causing for instance contrails are
Emissions Trading Scheme (EU-ETS) was very similar for all airlines. There is only one
published on January 13, 2009 in the EU’s Offi- exception: Nitrogen oxides (NOx) are included
cial Journal. It is valid for all flights to, from, and via an engine-related emission factor (needed to
within the EU and starts on January 1, 2012. For assess the radiative forcing by ozone and meth-
2012, an EU-wide cap on aviation emissions is set ane, both influenced due to chemical reactions of
at 97% of the average annual emissions for the these oxides in the atmosphere, leading to higher
years 2004–2006. It will be lowered to 95% in ozone and lower methane concentrations).
2013. All airlines will have to buy 15% of their 6. Different business plans like those for net carriers
allowance under the said cap through an auction. and low cost carriers are not valued, despite the
More allowances in order to cover growth of an air traffic stimulation caused by the low cost
airline have to be purchased. The revenues from carriers through subsidies often given to them
selling, if emissions are below the cap, must not by national governments or city councils.
be put into the industry or climate protection mea- 7. All airlines are categorized into seven effi-
sures. The inclusion of aviation into EU-ETS will ciency classes from A to G, in analogy to the
be reviewed in 2014. There are exemptions for European Union efficiency classes.
very small airlines, research, military, and rescue
flights. The directive has been included into the The AAI bases on a new atmosfair methodol-
one for EU-ETS (Dir 2003/87/EC). ogy, built upon the CO2 emission calculations of
ICAO. Its main data sources are the generally
available data sets: ICAO TFS (Traffic Flight by
An Airline Emission Index Stage), IATA WATS, OAG, Piano-x, JP-Airline
Fleet. This combination leads to 103 types of
As always in any economic sector there are large aircraft and 287 engines, constituting 87% of the
differences in behavior, here emissions, between global commercial air traffic with respect to num-
different agents. In order to bring transparency ber of flights. The parameters used are: aircraft
into the aviation sector of global transport the type, engine, winglets, seating arrangement, cargo
German nongovernmental, nonprofit organization addition, and passenger number.
atmosfair has issued for the first time in spring of The comparison of airlines follows the follow-
2011 a global airline index, comparing nearly all ing procedure:
airlines with respect to their environmental stan-
dards in the field of climatically relevant emis- 1. Calculation of the CO2 emission per kilometer
sions. The atmosfair airline index (AAI) is a for a flight between a city pair, taking into
ranking of most airlines with respect to such cli- account the above parameters.
matically relevant emissions with the following 2. The CO2 emission from step 1 for a city pair is
characteristics [1]: compared with the best case (direct flight in
best heights with least fuel consumption) and
1. Inclusion of the 130 largest airlines in the the worst case with three times higher emis-
world, arranged according to passenger kilo- sions (chosen to fully embrace all airlines).
meters as well as revenue, disregarding mere 3. The airline reaching the best case for a city pair
cargo flight companies. gets 100 points (it never happened), the one
2. Data from 2009 are used for the AAI 2011. with higher emissions for the same city pair
3. Airlines are subdivided into the following clas- gets less points according to its reduced perfor-
ses: net carrier, low cost carrier, charter, and mance, reaching zero points if emitting three
regional carrier. times as much.
4. Solely climatically relevant emissions of a car- 4. All city pairs of an airline are combined by
rier are taken into account, disregarding noise summing over all points reached for all pairs
pollution and further sustainability measures. and dividing by the number of city pairs.
342 Aviation and Atmosphere

5. Categorization of all airlines into seven effi- of seats occupied leads to an astonishing result:
ciency classes, in analogy to the color codes of Charter airlines and low cost carriers have a
EU for refrigerators, houses, etc. No single lower climate impact than well-known carriers
airline has reached class A or B. and no airline has reached category A or
6. This procedure allows the following comparisons: B. However, there needs to be a discussion on
• An airline with only a few city pairs can be that: How should the stimulation of further air
compared to one servicing hundreds of city traffic by and the subsidies often given to low
pairs. cost carriers be handled? The atmosfair group
• An airline with only short distance flights has decided not to include the low cost carriers
can be compared with one offering only in its first AAI although all the data are avail-
long-distance flights. able. For the ranking of the airlines, excluding
• A low cost carrier can be compared with a low cost carriers, see Fig. 7. There are only
net carrier. three factors nearly totally determining the
• An airline offering only one city pair with- higher ranking: high numbers of seats in a
out competitors can be ranked. certain aircraft type, percentage of seats occu-
The importance of the influencing factors age pied, and age of the aircraft. Hence, an airline
of an aircraft, number of seats, and percentage flying tourists to a destination with narrow

Aviation and Atmosphere, Fig. 7 A sample from the AAI for medium distance flights. For all airlines, please see
https://www.atmosfair.de/en/air-travel-climate/airline-index/
Aviation and Atmosphere 343

seating and leased modern aircraft can reduce 7. A temperature-based climate metric leads to a
fuel consumption to about 3 l of kerosene per very different result than one based on the
passenger and 100 km, while a net carrier with radiative forcing and thus only on the green-
first and business class seats, some old aircraft house warming potential.
and rather empty airplanes on certain dates for 8. The per person and per kilometer climate
certain city pairs cannot reach higher ranks. impact of passenger transport is much lower
for railways compared to road transport and
aviation, and the per person per kilometer cli-
Conclusions and Outlook mate impact of passenger air travel approaches
that of cars on time scale of decades. Despite
Mobility has a growing share in changing climate all the progress achieved so far many open
in comparison to other human activities like questions remain [30].
industrial production and heating or cooling of
houses. Fortunately, the European Union’s major Most of the quantifications can only be given
research project named QUANTIFY was able to with partly substantial uncertainty, sometimes
compare all modes of transport and very recently even effecting the sign of an effect. In particular,
quantified the different modes’ contributions. the climate impact of indirect aerosol effects on
Taking from their conclusions and focusing here clouds is highly uncertain. We still do not know
on the contribution of aviation (see QUANTIFY whether soot cirrus really exists. The net effect of
[30] for all modes of transport) we find: NOx emission from air traffic might cause a net
negative radiative forcing, if a recently proposed
1. The impact of transport, in particular of avia- additional chemical reaction is confirmed. There-
tion and shipping, on climate grows faster than fore, it is presently difficult to include some
the impact from other sectors of human activ- non-CO2 effects in climate policies related to avi-
ity. Hence, aviation has to excel concerning ation or to develop suitable mitigation strategies
efficiency measures in comparison to all other for all non-CO2 effects caused by the transport
human activities. sector. Furthermore, many of the emitted species
2. The effects of non-CO2 emissions on climate responsible for the non-CO2 effects of air traffic
caused by aviation and shipping (e.g., through emissions also impact air quality.
nitrogen oxide emissions and induced changes By applying a hierarchy of models (from pro-
in cloudiness) are particularly large in compar- cess models, cloud resolving models to chemical
ison to other modes of transport. transport models, global general atmospheric cir-
3. A NOx molecule from aviation is responsible culation models, and coupled atmosphere/ocean/
for five times more ozone than a molecule from land-models) and by analyzing measurements
road transport. from satellites and dedicated field campaigns,
4. A NOx molecule from shipping is four times the main uncertainties with respect to short-lived
more efficient in reducing methane concentra- non-CO2 effects on the atmospheric composition
tion in the atmosphere than a NOx molecule and on climate should be reduced:
from aviation.
5. Aircraft-induced clouds warm the atmosphere. 1. The importance and magnitude of trade-offs in
Their radiative forcing (RF) is of similar mag- the NOx effect (short-term increase in ozone
nitude than RF from aviation CO2. Hence, a versus longer-term decrease in methane and
multiplication factor of at least around 2 (includ- the associated longer-term ozone decrease)
ing air chemistry effects) seems justified when should be explicitly simulated by comprehen-
dealing with climate effects of aviation. sive models covering the long response time of
6. The relative weights of the non-CO2 effects of methane.
different modes of transport strongly depend 2. The climate impact of contrail cirrus should be
on the metric chosen and on the time horizon. simulated by climate models including
344 Aviation and Atmosphere

parameterizations of contrail cirrus and evalu- 2. Balkanski Y, Myhre G, Gauss M, Rädel G,


ated by recently available tracking algorithms Highwood E, Shine KP (2010) Direct radiative effect
of aerosols emitted by transport: from road, shipping
of these clouds in satellite data. and aviation. Atmos Chem Phys Discuss
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offs between climate and air quality effects of 7. Borken-Kleefeld J, Fuglestvedt J, Berntsen T (2010)
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examined for robust policy formulations. 8. Cariolle D, Caro D, Paoli R, Hauglustaine D,
Cuenot B, Cozic A, Paugam R (2009) Parameteriza-
Because the future will not only bring – with tion of plume chemistry into large scale atmospheric
high probability – a global carbon emission trad- models: application to aircraft NOx emissions.
J Geophys Res 114:D19302
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will also approach the metric “emissions per per- ronment) (2009) Bunker fuels and the Kyoto protocol:
son per year” as the baseline of climate policy, the how ICAO and the IMO failed the climate change test,
inclusion of aviation into the European Union Brussels, June 2009, 19 pp
10. Eyers CJ, Addleton D, Atkinson K, Broomhead MJ,
emission trading scheme is just a first step on the Christou R, Elliff T, Falk R, Gee I, Lee DS, Marizy C,
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04/0113, Farnborough
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Acknowledgment I am very thankful to Dietrich Lister DH, Massé B, Morris K, Newton PJ, Owen A,
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reduction arena and especially on different metrics to for 1991/1992 and 2015. Final report. Produced by the
account for the climate effects of air traffic besides those ECAC/ANCAT and EC working group. European
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Megacity City with a population of greater than
Regional Air Quality ten million inhabitants.
Metrics A set of measurements used to quantita-
Erika von Schneidemesser and Paul S. Monks tively gauge efficiency, progress, or perfor-
Department of Chemistry, University of Leicester, mance. In this case, as applied to air quality.
Leicester, UK Mobile sources Any object that releases pollu-
tion that is not stationary, e.g., vehicles, planes,
trains, ships, etc.
Article Outline Radiative forcing A change imposed on the
Earth’s radiation balance in units of heat flux
Glossary as watts per square meter (W m2).
Definition of the Subject and Its Importance Smog A term derived from smoke and fog
Introduction applied to extensive contamination by
Air Quality Measurements aerosols.
Health Effects, Ecosystem Effects, and Air Stationary sources Any object that releases pol-
Quality lution from one set location, e.g., power plants,
Modeling industrial factories, etc.
Current Air Quality Legislation and Metrics Temperature inversion The temperature of the
Regional Context troposphere normally decreases with increas-
Future Directions ing altitude; however, a temperature inversion
Bibliography results when warm air lies above cool air,
which is an extremely stable condition, also
Glossary known as an inversion layer.
Temporal Pertaining to time.
Anthropogenic Caused by humans; man-made. Wet deposition The deposition of gaseous or
Biogenic Produced by biological processes. particulate species from the atmosphere to a
Cohort study A long-term study of the same surface during precipitation events (e.g., rain,
group of people (the cohort) over time, typi- snow, fog, dew).
cally used in medicine social science, and
ecology.
Diurnal Relating to the 24 h/day time period.
Definition of the Subject and Its
Dry deposition The deposition of gaseous or par-
Importance
ticulate species from the atmosphere to a surface
without the involvement of precipitation.
What is Regional Air Quality?
Exceedance The amount by which something
(in this case an air quality pollutant) exceeds Clean air is considered to be a basic requirement of
the permissible standard or limit value. human health and well-being. However, air pollu-
tion continues to pose a significant threat to health
Feedback An internal climate process that worldwide [1].
amplifies or dampens the climate response to
an initial forcing, e.g., the release of methane Air pollution can be defined as “when gases or
into the atmosphere due to warmer tempera- aerosol particles emitted anthropogenically build
tures, the atmospheric methane increase fur- up in concentrations sufficiently high to cause
thers warming, which causes the release of direct or indirect damage to plants, animals,
more methane into the atmosphere, etc. other life forms, ecosystems, structures, or works

© Springer Science+Business Media, LLC 2012 347


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_561
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_561
348 Regional Air Quality

of art” [2]. The state of air pollution is often have positive effects on climate change and vice
expressed as air quality (AQ). Air quality is a versa. Therefore, as we move forward with air
measure of the concentrations of gaseous pollut- quality and climate regulation, interactions and
ants and size, number or mass of particulate matter feedbacks from air quality and climate change
(PM). Air quality is typically measured using in trade-offs need to be taken into consideration.
situ monitors that monitor species such as ozone Some of these trade-offs are shown in Fig. 1.
(O3), particulate matter, nitrogen oxides, and/or The topic as a whole is addressed in section
sulfur dioxide. “Regional Context”.
Air pollution has a history far longer than the
Why is Regional Air Quality Important? development of contemporary air quality policies.
An awareness of the detrimental effects of air Ozone, a current air quality problem and signifi-
pollution came to the forefront because of the cant contributor to urban pollution, was discov-
catastrophic effects of the “London Smog” epi- ered in 1839 by a German chemist, Christian
sode of 1952 where more than 4,000 people died Fredrich Schönbein. Air pollution from copper
[3]. Shortly after this, the Clean Air Act was smelting from as far back as Roman times has
passed by the UK Parliament in 1956 to limit been detected in ice-core measurements [2]. The
smoke/sulfur dioxide emissions and improve air plentiful use of fossil fuels in industry and home
quality in the cities. Air quality legislation heating starting in the Middle Ages, latterly in
evolved from there, mainly in Europe and the trains, was the main progenitor of degraded air
USA, to what it is today. Current air quality leg- quality through to modern times. A number of
islation is discussed in more detail in section extreme air pollution events starting in the late
“Current Air Quality Legislation and Metrics”. 1800s provided the motivation for modern air
Air quality remains an important topic because quality regulation. A number of smog episodes
of its impact on human health, ecosystems, and in London from 1878 to 1962 resulted in excess
its interactions with climate change (CC). deaths of hundreds to thousands of people, with
the most extreme and well known of these events
being the “Big Smoke” of early December 1952
Introduction that killed upward of 4,000 people [2–4]. Similar
episodes were also recorded in the Meuse Valley,
The Development of Regional Air Quality Belgium in 1930, and Donora, Pennsylvania,
Monitoring and Legislation USA in 1948 where smog events resulted in tens
The state of air pollution is often expressed as air of excess deaths and the illness of thousands of
quality (AQ). Air quality is a measure of the residents [2]. Around the same time, Los Angeles
concentrations of gaseous and aerosol pollutants was suffering from a different type of smog, this
in the atmosphere. Human health, ecosystems, one photochemical in origin, that arose from the
national heritage (e.g., buildings, monuments), mixture of ozone, nitrogen oxides, and volatile
and regional climate are all impacted by air pollu- organic compounds (VOCs) produced from a
tion. The implications for human health and eco- combination of large amounts of vehicle traffic,
system impacts can range from superficial surface sunny weather, and persistent temperature
discoloration of buildings to serious adverse inversions [4].
health effects, such as loss of months to years of These “smog” events, among others, spurred
life. These effects are discussed in further detail in the development of air quality regulation in the
section “Health Effects, Ecosystem Effects, and USA and Europe. The US Air Pollution Control
Air Quality”. Air pollution and air quality control Act was first passed in 1955, identifying air pol-
measures have implications for climate change, lution as a national problem. Further air pollution
owing to feedbacks between composition and cli- legislation followed with the Clean Air Act in
mate as well as wider atmospheric interactions. 1963 which set emission standards for stationary
Policies to improve air quality may not always sources (e.g., power plants). This was followed by
Regional Air Quality 349

AQ
Good

Energy efficiency
FGD Demand management
TWC-Petrol Nuclear
DPF-Diesel wind, solar, tidal...
hybrids, L & Z EVs
CCS

CC Bad CC
Good

Uncontrolled coal and Increase in


oil fossil fuels in “uncontrolled” diesel
stationary and mobile Biofuels
sources Biomass
CHP

AQ
Bad

Regional Air Quality, Fig. 1 The synergies and trade-offs between policies to improve air quality (AQ) and to reduce
greenhouse gas emissions/improve climate change (CC) (Monks et al. [36])

a number of amendments in the 1960s that set setting controls for household and industrial emis-
standards for motor vehicle emissions. In 1970, sions of smoke. In 1968, the UK Clean Air Act
the Clean Air Act was passed, which established was passed which required tall smoke stacks for
the National Ambient Air Quality Standards industries using fossil fuels to improve dispersal
(NAAQS), set new limits on stationary and of emissions and avoid local deposition [2]. As of
mobile sources emissions, and allowed states to 1972, the UK joined the EU and the majority of
set their own stricter standards [4]. Catalytic con- air quality policy has been determined by EC
vertors for vehicles in the USA were introduced in directives applicable across Europe. In 1979, the
1975, developed in response to the 1970 Clean International Convention on Long-Range Trans-
Air Act, significantly reducing hydrocarbon boundary Pollution was adopted to limit emis-
(HC) and carbon monoxide emissions. Further sions of acidifying pollutants. The first directive
incarnations of the Clean Air Act and amend- on ambient air quality was adopted in 1980 and
ments were passed in the years since then, reduc- assigned limits to sulfur dioxide and particles
ing standards for stationary and mobile sources, [3]. Subsequent directives in 1982 and 1985 put
and mandating control technology. In the USA, limits on ambient air concentrations of lead and
California has frequently been ahead of the curve nitrogen dioxide, and in 1989 a directive required
with more stringent air quality standards and all new cars in the EU to run on unleaded fuel
tighter standards for vehicles emissions. In 2002, [3]. A 1993 directive required the use of catalytic
California passed legislation that required auto- convertors on all new petrol vehicles. In 1996, an
makers to reduce greenhouse gas emissions from EC directive was established to provide a new
vehicles [4]. framework to control levels of sulfur dioxide,
Just after the first US Air Pollution Control nitrogen dioxide, particulate matter, lead, ozone,
Act, the UK Clean Air Act was passed in 1956, benzene, carbon monoxide, and hydrocarbons.
350 Regional Air Quality

This included establishing common methods and Gaseous Pollutants


criteria for assessment of air quality, and setting There are myriad different gaseous species that are
concentration limits for the pollutants. These emitted into the atmosphere from various air pollu-
limits were then tightened by a following directive tion sources. Some of the major gaseous pollutants
in 1999. Current legislation and regulations are are carbon monoxide (CO), nitrogen compounds
outlined in more detail in section “Current Air (e.g., NO, NO2, HNO3), sulfur compounds (e.g.,
Quality Legislation and Metrics”. SO2), hydrocarbons (HCs) including methane and
nonmethane hydrocarbons (NMHCs), and photo-
chemical oxidants (e.g., O3). Other gaseous pollut-
Air Quality Pollutants ants, such as carbon dioxide (CO2) and methane
Air pollution has many different components that (CH4), will not be addressed here because they are
differ in concentration depending on the super- not a major focus for regional air quality concerns
imposition of local, regional, and global emis- because their longer lifetimes qualify them as global
sion sources. These emissions are frequently pollutants.
separated into anthropogenic (“man-made”) and Carbon monoxide’s primary source is from
biogenic (“natural”) sources. The components of incomplete combustion. In addition to being an
air pollution can be roughly separated into gas- important primary pollutant, it is also an important
eous and particulate (or aerosol) fractions. precursor compound for the formation of ozone, as
Within both gas and particulate pollution there well as a secondary pollutant itself, formed from
can be primary and secondary pollutants, organic the oxidation of methane and other NMHCs by the
and inorganic compounds. Primary pollutants are OH radical [5]. It has a lifetime of a couple months
those emitted directly into the atmosphere from a which makes it a regional and global scale pollut-
source, such as sulfur dioxide or black carbon ant that can be transported significant distances
(BC) (a significant light absorbing component of from its emission source. Carbon monoxide is pri-
soot). Secondary pollutants are those formed in marily removed from the atmosphere by reaction
the atmosphere from chemical and/ or physical with OH, a small amount being removed by depo-
transformations of primary pollutants, such as sition. Ambient levels of 0.15–10 ppmV are com-
ozone (O3) and secondary organic aerosol mon in urban areas mainly owing to road
(SOA). transport–related sources [6, 7]. In the USA,
Regional air pollution results from the combi- mobile sources (including non-road mobile
nation of emissions, which vary both spatially and sources) make up 80% of national CO emissions,
temporally and meteorological factors (that allow while in the UK 47% of CO emissions are attrib-
the pollutants to build up in an area or transport uted to road transport sources. Figure 3 shows how
pollutants into an area where they can mix with CO emissions largely follow the road network in
local emissions) causing poor regional air quality. the UK, with the highest emissions in urban areas
Figure 2 shows different emissions sources and [8]. Furthermore, the high correlation of CO with
meteorological components that have an impact population density in Asia is shown in Fig. 4
on regional air quality. In addition to wind trans- [9]. Carbon monoxide emissions have shown sig-
porting pollutants, sunlight plays an important nificant reductions over the past 2 decades
role in photochemical reactions in the atmosphere [7]. These emission reductions are largely credited
that create some of the secondary pollutants. Air to the increased use of catalytic convertors in cars.
pollutants are then removed from the atmosphere Total CO emissions in the USA have decreased
through dry deposition (e.g., settling) or wet depo- 68% since the 1990s until 2008, and currently all
sition (e.g., rain scavenging). The following two monitoring stations in the USA show that no areas
sections will discuss the two main components of are in nonattainment for the 8-h CO standard of
air pollution – gaseous pollutants and particulate 9 ppmV [10]. Similarly, CO emissions in the UK
pollutants in terms of their sources, sinks, atmo- have been reduced by 71% from 1990 to 2005 in
spheric transport, and transformations. the UK. Elevated levels of CO observed in rural/
Regional Air Quality 351

Water vapor Halocarbons Chemical


transformation
CFCs Stratosphere

O3 destruction

Aircraft emissions
(NOx, Black Carbon, Sulfate) Troposphere

Long-range Transport of Aerosols and Gases

Chemical Chemical
transformation transformation

O3 production O3 production

Natural and
anthropogenic emissions Free
from the Earth Chemical Troposphere
(CH4, CO, CO2, transformation
VOCs, Sulfate, Black and
Cities Carbon, Dust, N2O, Evaporation Boundary
CFCs, NOx, O3) and convection layer
Sulfur
Industry Deposition
of
emissions
pollutants from oceans

Forests and other


Ecosystems
Transportation

Agriculture Transportation

Cattle
Oceans
Desert
dust
Biomass
burning

Regional Air Quality, Fig. 2 Summary of emissions, emissions sources, and atmospheric processing of air pollutants

remote areas are possible because of agricultural or with negative environmental impacts which led to
biomass burning and forest fires. an international effort to reduce acidification
Sulfur dioxide emissions originate primarily [2, 3]. It was later also determined that emissions
from coal-fired power plants. Once in the atmo- other than SO2 were also contributing to the acid
sphere SO2 is oxidized to sulfuric acid (H2SO4) deposition, such as direct emissions of HCl and
both homogeneously and heterogeneously in the nitric acid formed from nitrogen oxides emission
liquid and gas phases [11]. The resultant sulfuric and chemical transformation. Efforts to reduce
acid can be deposited in the gas phase or can acid deposition spawned international agreements
condense with water vapor onto aerosol particles such as the Convention on Long-Range Trans-
or cloud drops to produce aqueous phase sulfuric boundary Air Pollution (LRTAP), which was the
acid which can then be deposited through rain or first such agreement to deal with international air
fog. Acid deposition came to the forefront of pollution issues. Measures in the USA to reduce
environmental issues in the 1950s and 1960s and monitor sulfur emissions included amend-
when the acidification of Scandinavian lakes was ments to the Clean Air Act of 1970, as well as
linked to sulfur emissions in Europe. A Swedish the creation of the National Atmospheric Deposi-
study in 1972 connected sulfur dioxide emissions tion Program of 1977 [2]. Significant reductions
352 Regional Air Quality

Regional Air Quality, UK Emissions Map of


Fig. 3 Spatially Carbon Monoxide (as C) 2005 t/1×1km
disaggregated emissions of
carbon monoxide in the UK 0 – 0.3
from 2008 (Murrells et al. [8]) 0.3 – 0.5
0.5–2
2–3
3 –16
16 –160
160 –143,550

© Crown copyright. All rights reserved defra Licence number 100018880 2007.

in SO2 emissions were achieved in North America SO2 measured in the USA declined by 59% from
and Europe, resulting in some regeneration and 1990 to 2008, and are currently well below the
recovery of many forests and water bodies in these 0.03 ppmV (~80 mg m3) national standard. The
areas. The current guideline set by the World majority of the monitoring sites in the USA report
Health Organization (WHO) for SO2 is SO2 annual average levels between approximately
20 mg m3 (24-h average). A study looking at 0.002 and 0.008 ppmV for 2008 [10].
annual average SO2 concentrations for the late Similar to SO2, power plants are a significant
1990s of various megacities (cities with emissions source for nitrogen oxides (NOx). How-
populations greater than ten million) worldwide ever, NOx has many other important emission
found that a number of cities, such as Dhaka, sources including mobile sources, which make up
Bangladesh, Beijing, China, and Shanghai, the majority of global NOx emissions, as well as
China were still above this guideline; most other biomass burning, and natural emissions from soils
cited megacities in the study had annual average and lightning [2, 5]. NOx is the collective term for
concentrations of just under 25 mg m3 [12]. Addi- NO and NO2 as the photolysis of NO2 to NO and the
tionally, SO2 emissions from megacities in Asia subsequent regeneration of NO2 via reaction of NO
accounted for 30% of the ambient concentrations with ozone is sufficiently fast, in the moderately
measured regionally, including areas hundreds of polluted environment, for these species to be in
kilometers from the urban centers [13]. Levels of dynamic equilibrium, namely,
Regional Air Quality 353

Regional Air Quality,


Fig. 4 (Top) Population
density over China and
surroundings. All cities
with more than two million
inhabitants are indicated.
(Middle) MOPITT carbon
monoxide mixing ratios at
the surface level; average
measurements from March
2000 to June 2007.
(Bottom) The EDGAR
carbon monoxide emission
inventory for the year 2000.
All data are on a 1  1 grid
(Clerbaux et al. [9])
Population density (millions inhabitants)

0 1 2 3 4 5 6

Surface CO mixing ration(ppbv)

50 100 150 200 250 300

CO emissions (Tg/year/(1deg x 1 deg))

0.05 0.1 0.15 0.2 0.25 0.3


354 Regional Air Quality

NO2 þ hv ! NO þ O ð1Þ oxygenated organics that have low boiling points


(50–260  C). Certain VOCs such as the highly
O þ O2 þ M ! O3 þ M ð2Þ reactive “BTEX” compounds (benzene, toluene,
ethylbenzene, and xylenes) and 1,3-butadiene that
O3 þ NO ! NO2 þ O2 ð3Þ are often prevalent at significant concentrations
are frequently monitored even if other VOCs are
Therefore, at suitable concentrations, ambient not [21–24]. Highly reactive aromatics, as well as
NO, NO2, and O3 can be said to be in a photo- some other VOCs, are important precursor com-
chemical steady state or photostationary state pounds to secondary organic aerosol (SOA) for-
(PSS) [14], provided that they are isolated from mation (see discussion in the “Particulate Matter/
local sources of NOx and that sunlight intensity is Aerosol Pollutants” section). Methane is also a
relatively constant. VOC, but those discussed here are limited to
The majority of NOx emissions are initially nonmethane VOCs (NMVOCs). Methane has
emitted as NO. For example, the majority of very different sources and because of its lifetime
NOx from power stations is released from the is a global pollutant; it also has very important
stack as NO. Also, a study of vehicle emissions effects on climate. A study of NMHCs in 28 US
in Europe (for Euro-II emission standards) cities reported mean mixing ratios of individual
showed that for passenger cars, only 5% of NOx HCs of 9–8,740 pptV, with Los Angeles typically
is emitted as NO2 on average [15]. Since the Euro- reporting among the highest mixing ratios [21]. A
II emission standards were introduced NOx stan- similar study measuring NMHCs in 43 cities in
dards have been reduced through the introduction China reported a range of minimum and maxi-
of Euro-III, IV, and V. This has resulted in an mum mixing ratios from 40 pptV to 58,300 pptV
increase in the fraction of NOx emitted as primary for the same set of compounds [25]. On the other
NO2, likely due in large part to particle filters fit to end of the spectrum, measurements at a remote,
diesel vehicles [16]. In urban environments, NOx high altitude observatory at Izana, Tenerife,
emissions typically show diurnal cycles, peaking reported mean values for a similar set of individ-
during rush hours, owing to the dominant source ual NMHCs ranging from 1 pptV to 501 pptV
from the transportation sector. The data in Fig. 5 [26]. A comparison ofNMHC (and CO) measure-
show typical source time profiles from Mexico ments from global cities found that, in agreement
City [17]. The adverse health effects of NOx with the small sampling of measurements
stem from NO2 which can be inhaled and passed discussed here, the highest mixing ratios were
into the pulmonary region causing tissue damage; found in Asian and Latin American cities
NO is believed to be largely nontoxic at ambient [7]. While ambient air quality standards do not
levels [18]. The greater impact, in terms of health include VOCs, many vehicular emissions stan-
effects and air quality, results from the role that dards do, such as the European emissions stan-
NOx plays in ozone formation. NOx along with dards for passenger cars or the US “Tier”
volatile organic compounds (VOCs) and CO are regulations. The standards set for VOCs are for-
the important precursor compounds for the forma- mulated to achieve ozone standards, as the many
tion of ozone (see later). of the VOCs themselves pose relatively low
The main anthropogenic sources of VOCs are health risks owing to minimal exposures. Some
from mobile sources, evaporation from liquid VOCs, such as 1,3-butadiene and benzene are
fuels, and industrial sources. VOCs such as iso- genotoxic carcinogens and have significant health
prene and mono-terpenes also have a significant risks for any amount of exposure. These com-
biogenic source from vegetation [19]. VOCs are pounds along with some semi-volatile organic
defined as nonmethane hydrocarbons plus heavy compounds, such as polycyclic aromatic hydro-
hydrocarbons plus carbonyls plus halocarbons, carbons (PAHs) frequently have specific air qual-
typically <C20 [20]. VOCs include alkanes, ity standards because of their carcinogenic
alkenes, alkynes, and aromatics, as well as properties [2, 18, 24].
Regional Air Quality 355

CO 2001 – 2007 03 2001 – 2007


4
Mon Mon
80
Tue Tue
Wed Wed
3
Thu Thu
Fri 60 Fri
Sat Sat
ppm

2 Sun Sun

ppb
40

1 20

0 0
0 3 6 9 12 15 18 21 24 0 3 6 9 12 15 18 21 24
h h
NOX 2001 – 2007 PM10 2001 – 2007

140 Mon 80 Mon


Tue Tue
120 Wed Wed
Thu Thu
Fri Fri
100 60
Sat Sat
μg/m3
ppb

Sun Sun
80

60 40

40

20 20
0 3 6 9 12 15 18 21 24 0 3 6 9 12 15 18 21 24
h h

Regional Air Quality, Fig. 5 Diurnal cycle of carbon monoxide, nitrogen oxides, ozone, and PM10 in Mexico City,
averaged for 39 monitoring stations throughout the city over the 2001–2007 period (Stephens et al. [17])

Ozone is currently a problematic regional air of ozone that is not attributed to anthropogenic
quality issue for many locations. Ozone is formed sources of local origin and is therefore resulting
in the atmosphere from the photochemically from stratospheric ozone transport to the tropo-
driven reactions of NOx, VOCs, and CO. The sphere, ozone production from natural sources of
atmospheric cycle of reactions that form ozone NOx and VOCs (e.g., lightning, biogenic emis-
are shown in Fig. 6, where RH represents the sions), or long-range transport of ozone from dis-
VOCs/hydrocarbons. High levels of ozone can tant pollutant sources [27]. The contribution of
be found in urban areas, as well as in rural areas. background ozone, specifically that from long-
Ozone is a secondary pollutant and takes time to term transport, is a concern for many locations
form in the atmosphere, during that time can be that are in exceedance of air quality standards, as
transported away from the emission source. The the background contribution can make the differ-
time necessary for ozone formation depends on ence between being in attainment and not. This is
factors such as sunlight and the availability of the of particular concern in the Western US where
precursor compounds, and is typically on the influence from Asian emissions may be making
order of hours. Modern day average background it more difficult to achieve current regulatory air
O3 mixing ratios in the Northern Hemisphere quality standards [28]. Many urban areas, beyond
range from 20 to 45 ppbV (~39–88 mg m3). those in the Western US, are often in exceedance
Background in this case is defined as the fraction of their respective air quality standards for ozone,
356 Regional Air Quality

hν penetrate deeper into the lungs than particles in


O3 NO2
the coarse mode, remain in the air longer, trans-
O2
port over longer distances, and penetrate more
easily into indoor environments [38]. The scale
NO HO2
OH
of the possible impact of adverse health effects
from particulate matter is shown in Fig. 7 which
depicts the estimated loss of life expectancy attrib-
RH O2 O2 R−HO utable to PM2.5 from anthropogenic emissions in
NO RO 2000 and 2020 in Europe [39].
RO2
Particulate matter (PM) is composed of many

different species, including carbonaceous aerosols,
O2 O3 inorganic species (sulfate, nitrate, ammonium,
NO2
chloride), trace metals, and crustal elements from
Regional Air Quality, Fig. 6 Atmospheric cycle for the dust and water [5]. The relative contribution of
production of ozone. RH are hydrocarbons/non- aerosol components to the total aerosol burden for
oxygenated volatile organic compounds (VOCs).
(Reproduced from Fowler et al. [32])
the present atmosphere, based on a model simula-
tion for 1990 using emission estimates from 1990
such as cities in the USA, Canada, Europe, and and later, is shown in Fig. 8 [40]. Aerosols techni-
China [29–34]. These exceedances often affect cally refer to the suspension of fine solid or liquid
rural areas as well [35]. Ozone has adverse particles in a gas; however, the term aerosols is
impacts on human health, as well as vegetation. more commonly used to refer to just the particu-
Surface ozone is associated with respiratory prob- late/nongaseous component, which is how it will
lems and premature human mortality. In addition, be used here [5]. There are anthropogenic and
it can damage plants, reduce photosynthesis and natural sources of particulate matter. Natural
growth, leading to reduced crop yields [36]. sources of PM include volcanic eruptions, sea
Many of the pollutants discussed above, spray, biological debris, and dust. These types of
including carbon monoxide, sulfur oxides, nitro- PM emissions tend to fall into the coarse mode
gen oxides, and ozone, as well as particulate mat- (PM10–PM2.5) and are emitted owing to mechani-
ter (see below), are classified as “criteria cal processes [5]. Anthropogenic particulate matter
pollutants” by the US EPA. These criteria pollut- is emitted primarily from combustion sources and
ants are among the most common air pollutants falls largely into the fine mode (PM2.5) [38]. In
and are used as indicators of air quality [37]. many locations the majority of these anthropogenic
emissions stem from fossil fuel combustion use by
the transportation sector [18, 41], but other sources
Particulate Matter/Aerosol Pollutants include stationary fuel combustion (e.g., power
Particulate matter is an air quality concern plants), industry, and biomass burning. The sche-
because of its adverse health effects, as well as matic representation in Fig. 9 summarizes aerosol
its contribution to reductions in visibility. Partic- sources, sinks, and transformations in the atmo-
ulate matter is currently monitored, in the air sphere, by particle size [5, 42].
quality area, based on size-resolved fractions. In addition to primary aerosols, secondary
These are typically PM10 (particles with an aero- aerosols, i.e., those formed in the atmosphere by
dynamic diameter of 10 mm or smaller) and PM2.5 gas-to-particle conversion and/or condensation of
(particles with an aerodynamic diameter of 2.5 mm gaseous compounds onto preexisting aerosol par-
or smaller). This size fractionation is also typically ticles can be a significant fraction of the
referred to as the coarse mode (the fraction PM. Secondary aerosols can be organic or inor-
between PM10 and PM2.5) and the fine mode ganic, formed primarily from (photo)chemical
(equivalent to PM2.5). Particles in the fine mode reaction of VOC precursor emissions or the oxi-
are a more significant health concern than those in dation of NOx and SO2 [43]. Secondary organic
the coarse mode because of their ability to aerosols (SOAs) are formed in a two-step process:
Regional Air Quality 357

–30 –20 –10 0 10 20 30 40 50 60 –30 –20 –10 0 10 20 30 40 50 60

60 60

60 60

50 50

50 50

40 40
40 40

0 500 1000 1500 km 0 500 1000 1500 km


10 20 30 10 20 30

Estimated losses in life expectancy attributable to exposure to fine particulate matter (PM2.5) from anthropogenic
emissions for 2000 (left) and 2020 (right)

Months No data Outside study area


0 1 2 4 6 9 12 36

Regional Air Quality, Fig. 7 Health impact of particu- (left) and for 2020 (right) for the Clean Air for Europe
late matter (PM) mass concentrations (mg m3). Loss in (CAFE) baseline scenario, which takes into account
statistical life expectancy (months) that can be attributed to changes in air quality standards and reductions in emis-
anthropogenic contributions to PM2.5 for the year 2000 sions (IIASA; EEA [39])

BC/EC
Organics
Organic & BC/EC
compounds
SO42– SO42–

Others
NO3– Others

NH4+

Regional Air Quality, Fig. 8 Relative contribution of anthropogenic sources (SOAa), secondary organic aerosol
aerosol components to the total aerosol burden (28.9 Tg) from biogenic VOC oxidation (SOAb), primary organic
for the present atmosphere, based on a model simulation aerosol (POA), black carbon (BC), and methane sulfonic
from 1990 using emission estimates from 1990 and later. acid (MSA) (Tsigaridis et al. [40])
Secondary organic aerosol (SOA) produced from

(1) the production of the organic aerosol com- photochemical reactivity (e.g., summer months),
pound from the reaction of parent organic gases, but can be significant year-round depending on
(2) the partitioning of the organic compound the location, meteorology (e.g., humidity and tem-
between the gas and particulate phases forming perature), solar radiation, the existing aerosols and
SOA [5]. Secondary organic aerosol concentra- availability, abundance, and reactivity of gas-
tions tend to be higher during periods of greater phase precursors and oxidants [44–47]. The
358 Regional Air Quality

Regional Air Quality, Chemical conversion


Fig. 9 Schematic of the Hot vapor of gases to low
distribution of atmospheric volatility vapors
aerosols, showing principal
modes, sources, and particle Condensation
Low
formation and removal volatility
mechanisms (Whitby and Primary vapor
Cantrell [79]) particles
Homogeneous
Coagulation nucleation

Chain Condensation
aggregates growth of nuclei Wind blown dust
+
Emissions
+
Droplets Sea spray
+
Volcanoes
+
Coagulation Plant particles

gulation
Coa

Rainout
& Sedi-
washout mentation

0.001 0.01 0.1 1 10 100


Particle diameter, μm

Transient nuclei or Accumulation Mechanically generated


aitken nuclei range range aerosol range
Fine particles Coarse particles

atmospheric processes undergone by aerosols contributions of different types of aerosol sources


after emission or formation in the atmosphere are to ambient particulate matter samples, including
detailed in Fig. 10 [44, 48]. factor analysis and chemical mass balance (CMB)
Concentrations of reported PM range from less modeling. More information about these types of
than 1 mg m3 (PM10) in a remote location such as models can be found in section “Modeling”.
the Antarctic to 340 mg m3 (PM10) and
194 mg m3 (PM2.5) annual average concentra-
tions for Lahore, Pakistan in 2007, which is Air Quality Measurements
extremely polluted and has some of the highest
PM concentrations recorded [49–51]. The WHO Networks of air pollution monitoring stations
annual average guideline for PM10 is 20 mg m3 have been set up across many areas of the globe,
and 10 mg m3 for PM2.5. Annual average con- especially in developed countries. In the USA, for
centrations in 2001 of PM2.5 and PM10 from three example, ambient air quality monitoring pro-
European cities ranged from 7.8 to 28.0 mg m3 to grams are required of states by the US EPA to
15.7–41.0 mg m3, respectively [52]. assess and determine compliance with the
Various types of modeling have been national ambient air quality standards. The air
established that are able to determine the quality monitors and monitoring programs must
Regional Air Quality 359

Regional Air Quality,


Fig. 10 Primary
emissions, secondary
formation, and atmospheric Secondary
processing of natural and formation
anthropogenic aerosols
(Fuzzi et al. [48]; Poeschl
[44]; Monks et al. [36]) Cloud processing

Physical & chemical

Transformation (Aging)

Natural Anthropogenic Dry Wet

Primary emission Deposition

comply with design and quality assurance require- the LRTAP Convention with qualified scientific
ments, as well as using monitoring techniques information to support the development and further
based on federal reference methods. The results evaluation of the international protocols on emis-
from these monitoring networks are then reported sion reductions negotiated within the Convention”
to the US EPA annually [18]. There are different [53]. At this point, data are collected for the fol-
levels of monitoring networks in the USA, includ- lowing areas of interest: acidification and eutrophi-
ing the National Air Monitoring Stations (NAMS), cation, ground-level ozone, persistent organic
the State and Local Air Monitoring Stations pollutants (POPs), heavy metals, and particulate
(SLAMS), and the Photochemical Assessment matter. These are monitored using air and precipi-
Monitoring Stations (PAMS). The national net- tation sampling methods. In addition to measure-
work is for long-term monitoring to provide a ments (monitoring), EMEP also collects emissions
systematic, consistent database for comparison data, and uses modeling to look at atmospheric
with other air quality data and trend analysis. The transport and deposition of air pollutants
state and local network is for determining compli- [53]. The focus here will be on the established
ance with air quality standards, while the PAMS monitoring network. There are over 300 sites in
network is designed for monitoring ozone in areas the monitoring network in 37 countries, and more
of persistently high ozone concentrations than 20 participating institutions. There are three
[18]. More information on monitoring and the fed- different levels of monitoring stations within the
eral reference methods used in the US air quality EMEP network depending on the number and type
networks is available on the US EPA Web site and of measurements being conducted, but all EMEP
in Godish (2004) [18]. stations are located in areas classified as measuring
The overarching air monitoring network for all regional or global background. Many of the EMEP
of Europe, which focuses on transboundary air stations are also part of or working in cooperation
pollution, was established as part of the Conven- with other European monitoring framework initia-
tion on Long-Range Transboundary Air Pollution tives, such as the World Meteorological
(LRTAP). Within that convention, the EMEP pro- Organization-Global Atmospheric Watch pro-
gramme (Co-operative Programme for Monitoring gramme (WMO-GAW), national monitoring net-
and Evaluation of the Long-range Transmission of works that report to the European Commission
Air Pollutants in Europe) was tasked to “regularly under the European Union Air Quality Directives,
provide governments and subsidiary bodies under and other national and local monitoring networks
360 Regional Air Quality

[54]. The European Air Quality Directives focus Health Effects, Ecosystem Effects, and
on regional air pollution. Air Quality
In addition to the EMEP network, many coun-
tries also have monitoring networks that have Air pollution was not always associated with neg-
been established in urban areas to monitor road- ative connotations. Before the Second World War,
side pollution levels, and urban background air pollution (e.g., car exhaust, plumes from
levels. For example, the UK has an extensive air smoke stacks) were associated to a certain degree
quality network, across the country with growth and prosperity [55]. Going back as
(UK Automatic Urban and Rural Network, far as 1873 London was affected by smogs, the
AURN) and in the major urban areas, such as most infamous of which was the London smog of
London (London Air Quality Network, LAQN). December 1952 [18]. The word smog originates
The UK AURN has over 100 monitoring stations from the combination of the words smoke and fog.
located across the country for NOx, PM2.5, PM10, The smogs of London were caused by extremely
SO2, CO, and/or O3. A map showing the distribu- high concentrations of smoke and sulfur dioxide
tion of monitoring stations and station types, emissions largely from coal burning. During the
given by monitoring in compliance with AQ leg- 1940s, it became clear that cities like Los Angeles
islation, is shown in Fig. 11. had severe air quality problems owing to a differ-
ent kind of smog – a photochemical smog. This
type of smog stems from high concentrations of
oxidants (e.g., ozone) and peroxide compounds
that are produced through photochemical reac-
tions. The basic reaction scheme for the formation
of ozone, the primary ingredient in photochemical
smog is

Airport
½O2 
Kerbside
VOC þ OH ! RO2 þ H2 O ð4Þ
Remote
Roadside
Rural ½O2 
Suburban CO þ OH ! HO2 þ CO2 ð5Þ
Urban background
Urban centre
½O2 
Urban industrial RO2 þ NO ! secondary VOC þ H2 O
þ NO2 ð6Þ

H2 O þ NO ! OH þ NO2 ð7Þ

NO2 þ hv ! NO þ O ð8Þ

O þ O2 þ M ! O3 þ M ð9Þ

where RO2 represents a chain organic with


an attached O2. The OH radical is formed from
photolysis of ozone, formaldehyde, and other
secondary VOCs [56]. Since these early smogs
which documented a connection between
exposure to elevated pollution levels and acute
Regional Air Quality, Fig. 11 Monitoring stations in the illness in the affected population, a number of
UK, shown by station classification (http://www.airquality.
co.uk/monitoring_networks.php?n¼aurn) epidemiological, toxicological, and occupational
Regional Air Quality 361

exposure studies have documented the associa- remains under debate. Figure 12 shows life
tion between aerosols and adverse health effects expectancies versus PM2.5 concentrations from
[18, 38, 57]. Health effects can range from eye a study looking at fine-particulate air pollution
irritation to cardiovascular system related mor- and life expectancy throughout the USA
tality. The Harvard Six Cities study was a cohort [61]. Additional studies in Canada, Germany,
study which estimated the effects of air pollution Finland, and the Czech Republic also reported
on mortality, while also controlling for other comparable results for particulate pollution and
individual risk factors, such as smoking adverse health effects, such as respiratory symp-
[58]. Over 8,000 adults in six US cities were toms and hospitalizations and mortality [38]. For
included in the study that lasted approximately more detailed information on air pollution and
15 years. Statistically significant associations health effects, a number of books and review
were found between air pollution and mortality articles are recommended in the “Further Read-
with positive associations between air pollution ing” section of the “Bibliography”.
and death from lung cancer, as well as air pollu- In addition to adverse human health effects, air
tion and cardiopulmonary disease. The air pol- pollution can damage vegetation, buildings, and
lutants most associated with the mortality were cause loss of revenue due to impaired visibility.
fine particulates and sulfate [58]. A later cohort Vegetation effects include reduction in yields, leaf
study from 1982 to 1989 using data from 151 US damage, loss of sensitive species, and subsequent
cities and over 550,000 adults found that reduction in plant diversity and sensitivity to other
increased mortality was associated with sulfate environmental stresses [62]. Buildings and other
and fine-particulate air pollution and that partic- outdoor structures can be damaged by air pollu-
ulate air pollution was linked with cardiopulmo- tion as well. The blackened walls of historical
nary and lung cancer mortality, very similar to monuments and other buildings, such as cathe-
the Six City study findings [59]. Later studies and drals, are because of high levels of aerosols depos-
reanalysis of the data found that there was no iting on the surface. Physical erosion owing to
consistent toxicological evidence to suggest that windblown dust can impact buildings, and some
long-term exposure to sulfates had significant building materials (mainly certain kinds of stone,
effects on the cardiovascular system [60]. The such as limestone or marble) can also be chemi-
association of sulfate with adverse health effects cally eroded by acid aerosols [18].

Regional Air Quality, 82


Fig. 12 Cross-sectional
life expectancies for
80
Life Expectancy, 1997–2001 (yr)

1997–2001, plotted against


PM2.5 concentrations for
1999–2000 for the USA. 78
Dots and circles labeled
with numbers represent
population-weighted mean 76
life expectancies at the
county level and the
metropolitan-area level, 74
respectively. The solid and
broken lines represent 72
regression lines with the use
of county-level and
metropolitan-area-level 70
observations, respectively 0
0 5 10 15 20 25 30
(Pope et al. [59])
PM2.5, 1999–2000 (μg/m3)
362 Regional Air Quality

Modeling taken into account in the atmospheric models


[19]. Atmospheric models can be run on different
The fate of any chemical species (Ci) in the atmo- scales from local and regional to global. The
sphere can be represented as a continuity or mass regional or local models are most applicable to
balance equation such as regional air quality and are frequently used as
predictors for possible future scenarios, includ-
dCi duCi dvCi dwCi ing prediction of air quality, cost-benefit, and
¼  
dt dx dy dz environmental impact analyses of pollutant
  ð10Þ increases or reductions. An example is shown in
dC dCi
þK z i þ Pi  Li þ Si þ Fig. 13 where the model has been used to predict
dz dt clouds
ozone concentrations for two different scenarios,
emissions from a base case scenario and then
where t is the time, u, v, and w are the components
projected emissions based on the technology
of the wind vector in x, y, and z accounting for the
and regulations that will be or are currently
horizontal and vertical large-scale transport.
being implemented (in this case for 2000 and
Small-scale turbulence can be accounted for
2010). The model data show the expected impact
using Kz, the turbulent diffusion coefficient, Pi
of various emission legislation measures, includ-
and Li are the chemical production and loss
ing legislation regarding combustion plants, the
terms, and Si are the sources owing to emissions.
Euro standards for vehicles and non-road
Cloud processes (vertical transport, washout, and
machinery, as well as International Panel on Cli-
aqueous phase chemistry) are represented in a
mate Change (IPCC) and national legislation. As
cloud processing term. The application of this
is visible in Fig. 13, the model predicts the largest
type of equation is the basis of chemical model-
impacts in ozone reduction will occur in the
ing. There are two main types of modeling that
Mediterranean region [39].
deal with air pollution and air quality objectives,
The input data for many models are based on
atmospheric (chemical) transport models and sta-
emission inventories. Emission inventories, like
tistical models [5].
models, exist for different scales, i.e., local,
regional, and global and resolutions, ranging
Atmospheric Models from 1 km  1 km to 1 1 (which is approxi-
Atmospheric (chemistry) transport models are mately 110 km  110 km at the largest, depending
based on the fundamental description of atmo- on latitude). The species included in many emis-
spheric physical and chemical properties [5]. The sion inventories are greenhouse gases, nitrogen
reason for the “chemical” term in parentheses is oxides, carbon monoxide, methane, non-methane
that there are a number of models which model volatile organic compounds, sulfur dioxide,
only transport and do not necessarily always ammonia, particulate matter, and recently black
include chemical transformations, but the gen- carbon and organic carbon [36]. Emission sources
eral principles behind the models are the same. in inventories include anthropogenic emissions
There are two basic kinds of atmospheric from fuel production, industrial and domestic
models – Lagrangian and Eulerian. Lagrangian combustion, transportation, waste disposal, indus-
models track the path of a given air parcel (and trial processes, solvent production and use, and
the concentrations of the chemical components agriculture, and biogenic emissions from vegeta-
therein) as it is advected in the atmosphere, while tion and dust, and biomass burning emissions,
Eulerian models describe the concentrations in which can be natural or anthropogenic
an array of fixed (nonmoving) computational [36]. Anthropogenic, natural, and biomass burn-
cells [5]. The concentration of any chemical spe- ing emissions are typically compiled in separate
cies in the atmosphere are controlled by four inventories. Examples of emission inventory data
types of processes, namely emissions, chemistry, are given in Fig. 3 for carbon monoxide and
transport, and deposition (see Eq. 10) that are Fig. 14 for ammonia [8].
Regional Air Quality 363

–30 –20 –10 0 10 20 30 40 50 60 70 –30 –20 –10 0 10 20 30 40 50 60 70

60 60

50 50

50 50

40

40 40

0 500 1000 1500 km 0 500 1000 1500 km


10 20 30 40 10 20 30 40

Modelled rural ozone concentrations expressed as SOM035 for the year 2000 (left) and for the year 2010 (right)

ppb/days Outside study area


1
00
00
00
00
00
00

00
10
20
30
40
50
60

70

Regional Air Quality, Fig. 13 Modeled ozone concen- (right) for the Air for Europe (CAFE) baseline scenario,
trations expressed as the sum of means over 35ppbV which takes into account changes in air quality standards
(SOMO35) for the year 2000 (left) and for the year 2010 and reductions in emissions (IIASA; EEA [39])

Statistical Models Plans to attain PM10 requirements [65]. In addi-


Statistical models are empirical or semiempirical tion, CMB can be used to assess the success of
models based on the statistical analysis of measured implemented control technologies, and which
data. Instead of following the evolution of emissions sources are potentials for reduction controls.
in the atmosphere, statistical models work back- Such applications are possible in that CMB results
ward, from measured data collected at a given loca- yield quantitative source contributions to the mea-
tion, a receptor site, and work out the responsible sured metric, i.e., PM2.5, organic carbon, or total
emission sources. These models are also frequently mass. From such results the sources with the larg-
referred to as receptor models. There are a number est contributions can be targeted for reduction, or
of different approaches that are used based on the changes in specific source contributions assessed.
understanding of source–receptor relationships Recent reviews of CMB and other receptor
including the chemical mass balance (CMB) models found that for the studies analyzed (the
model, which requires complete knowledge of majority of which were from measurements in the
sources and results in a quantitative output of source USA and Europe), fossil fuel combustion is an
contributions and uncertainties, and factor analysis important contributor to PM concentrations, with
methods, such as Principal Component Analysis the primary contributions stemming from gasoline
(PCA), which require no a priori source information. and diesel vehicle exhaust [64, 65]. Stationary
The different types of receptor models and the sources, such as power stations, have only mini-
amount of knowledge required for model use is mal source contributions when the facilities have
summarized in Fig. 15 [63, 64]. effective pollution controls in place, but can be
Chemical mass balance models are frequently large contributors without such control technolo-
used to support air quality decision-making for gies [65]. An example of the type of result pro-
policy, such as was the case for CMB studies in duced by CMB modeling where fine-particulate
Los Angeles, CA, and Las Vegas, NV which were matter organic carbon mass is apportioned is
used for the creation of State Implementation shown in Fig. 16 for West Jerusalem in 2007 [66].
364 Regional Air Quality

UK Emissions Map of In addition to receptor models, other types of


Ammonia 2005 kg /1×1km
statistical models are also frequently used in atmo-
0 – 0.05 spheric chemistry, such as simple regression anal-
0.05 – 0.1 ysis, land use regression models, and neural
0.1 – 0.5
0.5 – 1 network models. Land use regression models
1–2 have been used in atmospheric chemistry to char-
2–4 acterize air pollution exposure and health effects
4 – 2.186
for people residing in urban areas, integrating
traffic and geographic information into the models
[67]. To learn about neural network models and
their uses in the air pollution modeling field the
reader is referred to Boznar and Mlakar [68].

Current Air Quality Legislation and


Metrics

Air quality guidelines are established to protect


human health and the environment. The World
Health Organization (WHO) has established air
quality guidelines for use worldwide that are
focused on protecting human health. Air quality
guidelines in the USA and Europe are intended to
protect human health, including sensitive
populations (e.g., elderly, asthmatics), with sec-
ondary limits set for the protection of public
Regional Air Quality, Fig. 14 Spatially disaggregated
emissions of ammonia in the UK from 2008 (Murrells welfare (e.g., visibility, animals, crops, build-
et al. [8]) ings) [37]. The standards are set based on the

Receptor models
Xt = Λ ft + et
px1 pxk kx1 px1

Knowledge required about pollution sources


prior to receptor modelling

Little Complete

Multivariate Chemical
models mass
ME COPREM balance

UNMIX CMB
PCA PMF Bayesian
models Regression
models
Exploratory factor Confirmatory factor Measurement error
analysis models analysis models models

Regional Air Quality, Fig. 15 Approaches for estimating pollution source contributions using receptor models.
Specific models are shown in italics and with dotted arrows (Schauer et al. [63];Viana et al. [64])
Regional Air Quality 365

8
(a) West Jerusalem Vegetative detritus
Biomass burning
Diesel vehicles
7 Gasoline vehicles
Residual fuel oil
Soil/Dust
LT coal comb.
SOA isoprene
6 SOA pinene
SOA caryophyllene
SOA toluene
Other
Source contribution (μg C m−3)

0
JAN FEB MAR APR MAY JUN JUL AUG SEP OCT NOV DEC

Regional Air Quality, Fig. 16 Source apportionment by temperature coal combustion; SOA ¼ secondary organic
chemical mass balance (CMB) modeling of monthly aver- aerosol from the named precursor compound (e.g., iso-
aged ambient fine organic aerosol mass concentrations for prene) (von Schneidemesser et al. [66])
West Jerusalem for 2007. LT Coal Comb ¼ low-

extensive amount of research available matter of two-size fraction, ozone, and sulfur
concerning air pollution and health effects at the dioxide, similar to those pollutants for which the
time of regulation. WHO has established guidelines [37]. European
The guidelines set by the WHO exist for the Union air quality pollutants include particulate
most common air pollutants: size-resolved partic- matter, sulfur dioxide, nitrogen dioxide, lead, car-
ulate matter, ozone, nitrogen dioxide, and sulfur bon monoxide, benzene, ozone, arsenic, cad-
dioxide [1]. These were most recently updated in mium, nickel, and PAHs and are regulated under
2005. While the WHO has set guidelines for all the air quality standards which were simplified in
countries to use as a basis for regulation if they 2008 by combining all existing legislation on air
choose to do so, most national air monitoring quality under one directive known as the ambient
authorities have a list of “air quality pollutants” air quality and Clean Air for Europe (CAFE)
that are monitored and regulated. In the USA, directive [69]. As is apparent here, all air quality
these are the “criteria pollutants” that are regu- pollutant regulation tends to contain a similar set
lated under the National Ambient Air Quality of air pollutants with some countries/regulating
Standards (NAAQS) by the US Environmental bodies selecting additional species, such as trace
Protection Agency (EPA) and include carbon metals, to be included. Regulatory standards and
monoxide, lead, nitrogen dioxide, particulate WHO guidelines are listed in Table 1.
366 Regional Air Quality

Regional Air Quality, Table 1 Annual mean (unless Environmental Protection Agency (US EPA), and the
noted otherwise) air quality guidelines as established by European Union (Euro Directives)
the World Health Organization (WHO), the United States
WHO US EPA Euro directive
Particulate matter (PM10) 20 mg m3 150 mg m3 (24 h) 40 mg m3
Particulate matter (PM2.5) 10 mg m3 15.0 mg m3 25 mg m3
Nitrogen dioxide 40 mg m3 53 ppb (~100 mg m3) 40 mg m3
Sulfur dioxide 20 mg m3 (24 h) 0.03 ppm (~80 mg m3) 125 mg m3
Carbon monoxide 10 mg m3 (8 h) 10 mg m3 (8 h)
Lead 1.5 mg m3 (quarterly average) 0.5 mg m3
Benzene 5 mg m3
Arsenic 6 ng m3
Cadmium 5 ng m3
Nickel 20 ng m3
Polycyclic aromatic hydrocarbons 1 ng m3

Metrics also exist to quantify health or environ- from atmospheric processing and the transport of
mental effects of air pollutants, with different met- pollutants become much more important and pri-
rics established for human health and the mary emissions less so.
environment. For example, AOT40 is the accumu- For example, as discussed earlier, ozone is an
lated exposure over a threshold of 40 ppbV during important secondary pollutant, which because of
daylight hours for a relevant period. SOMO35 is the atmospheric processing time, has significant impli-
sum of the daily maximum of running 8-h means cations for regional air quality. Plume transport for
over 35 ppbV. Both the AOT40 and SOMO35 are urban areas into the surrounding region can have a
ozone metrics. Metrics such as AOT40 and significant influence on the air quality in the sur-
SOMO35 are frequently considered to be more rounding region [71]. In many cases, ozone con-
appropriate measures of the effects of ozone on centrations have been observed to be higher in rural
crops and vegetation than those metrics designed areas than urban areas [72, 73]. Furthermore, since
to protect human health. A sample of environmental regional air quality frequently includes rural areas,
and health metrics are given in Table 2 [70]. and thereby areas with fewer primary anthropo-
genic emissions, natural emissions can play a
more significant role. For example, biogenic
VOCs, such as isoprene, can contribute to ozone
Regional Context
and other secondary pollutant formation, and wind
erosion can add soil and/or dust to the existing
There are a variety of spatial scales that both influ-
aerosol loading. While these factors can and do
ence air quality and that air quality impact, such as
also exist on a local scale, their relative importance
the local, regional, and global. It is clear that these
on a local or regional scale varies depending on the
scales are not independent and definitions are
location and size of the areas chosen.
loose. The local scale tends to the anthropogenic
emission/human influence scale encompassing a
city or a smaller area within a city, while regional
scales are typically larger, encompassing an entire Future Directions
metropolitan region and the surrounding area or
even greater. An example of a regional scale Air Quality and Climate
could be London and southeast England, or it Air quality and climate change are important
could also be as large as all of Europe, depending issues with complex interactions (see Figs. 1 and
on how the user defines it. When considering air 17). Both are environmental issues that are and
quality on any regional scale, secondary pollutants will continue to be addressed by environmental
Regional Air Quality 367

Regional Air Quality, Table 2 A sample of ozone metrics of relevance to human health. (Reproduced from AQEG
2009)
Key influences on the values of this
Metric Relevance metric at urban locations
Annual average Basic metric used to show long-term Includes all of the hours in the year.
trends Strongly influenced by the magnitude of
local NOx emissions and by topography
through nocturnal depletion
Annual average of the daily Used as “basic metric” for many of the Strongly influenced by the magnitude of
maximum of the running 8-h health metrics. local NOx emissions
mean
Annual average of the daily Health impact, related to SOMO35 Influenced by the magnitude of local
maximum of the running 8-h NOx emissions and by photochemical
mean with a 70 mg m3 cutoff episodes
Annual average of the daily Health impact Strongly influenced by photochemical
maximum of the running 8-h episodes and to a lesser extent by the
mean with a 100 mg m3 cutoff magnitude of local NOx emissions
Maximum 1-h average (peak Used as the basis for some The metric most sensitive to the
hour in the year) epidemiological studies, although it has magnitude of regionally generated
been suggested that the 8-h metric is photochemical episodes and thus likely
more representative to show a response to reductions in
Also an indicator of short-term peaks, relevant precursor emissions
but note low statistical power, since it is
the value for one single hour
Number of days with daily Equates to the number of exceedences of Strongly influenced by photochemical
maximum of running 8-h the UK ozone standard (the Air Quality episodes and to a lesser extent by the
mean exceeding 100 mg m3 Strategy objective is no more than magnitude of local NOx emissions
10 exceedences per year)
Number of days with daily Equates to the number of exceedences of Strongly influenced by photochemical
maximum of running 8-h the EU Target Value (no more than episodes and to a lesser extent by the
mean exceeding 120 mg m3 25 days, averaged over 3 years) and magnitude of local NOx emissions
Long-Term Objective (no exceedences)
from the third Daughter Directive
SOMO35 (sum of means over Used as a metric by IIASA, for Clean Air Influenced by the magnitude of local
35 ppb) for Europe (CAFE) and NECD revision, NOx emissions and by photochemical
related to annual average of the daily episodes
maximum of the running 8-h mean with
a 70 mg m3 cutoff

policies in the coming years. Much of the current air pollutants of greatest concern for public health
focus is on trade-offs between different scenarios. [75], while being key players in climate change
While there are win-win situations where policy and feedbacks [36, 76].
will improve both air quality and reduce green- Air pollution and greenhouse gases often have
house gas emissions, many measures may not common sources of emission. In addition to the
result in such co-benefits. As stated in the IPCC common sources, there are some gases which are
Fourth Assessment Report “Future climate both air pollutants and act as greenhouse gases,
change may cause significant air quality degrada- such as ozone [77]. To best address both issues, a
tion by changing the dispersion rate of pollutants, significant effort will need to be made to under-
the chemical environment for ozone and aerosol stand the impact of a changing climate on air
generation and the strength of emissions from the quality and vice versa. Current work with global
biosphere, fires, and dust. The sign and magnitude and regional models that couple chemical trans-
of these effects are highly uncertain and will vary port and general circulation simulations have
regionally” [74]. Ozone and aerosols are the two found that climate change alone could increase
368 Regional Air Quality

Atmospheric concentrations
O3 production O3 production
O3

Carbon NOx, HNO3


oxidation lifetimes
Temperature,
(via OH) humidity, RF (UV + IR)
dynamics
CH4, VOC
Atmospheric emissions
N2O, RF Nitrogen cycle
concentrations rates
Climate emissions
CH4 environmental
VOCs RF (IR) Lightning,
concentrations
CO precipitation,
temperature
Ecosystem nutrients
Æ Biogenic emissions

Pollutant emissions
• Fossil fuel combustion
• Biomass burning
• Industrial emissions
• Emissions relating to land-use change

Regional Air Quality, Fig. 17 Schematic representation RF radiative forcing, UV ultraviolet radiation, IR infrared
of the multiple interactions between tropospheric chemical radiation (IPCC 2007; EPA [76])
processes, biogeochemical cycles, and the climate system.

summertime ozone concentrations and the sever- affects the scattering and absorption of radiation
ity of summer smogs over the coming decades, and therefore climate. Preliminary model results
with the largest effects in polluted, urban areas show a range of increases and decreases in PM
[75–77]. The potential impact of climate change concentrations for different regions in response to
on PM is much less certain. Important factors in climate change [75, 76].
changes in PM owing to climate change include While controls of CO2 emissions should
precipitation frequency and mixing depth, as well remain a priority for mitigation of global climate
as wildfire frequencies [75, 76]. In addition to the change, reductions in emissions of air pollutants
uncertainty of the impact of climate change on PM could have a faster impact on slowing warming
emissions, the uncertainty of the reverse, the trends in the short term (10–30 years). Raes and
impact of PM on climate change, is also large. Seinfeld [78] have pointed out that we maybe on a
Part of this uncertainty arises from the differences “bumpy road” to recovery with larger short-term
in aerosol types and their climate properties. Sul- increases in temperature, owing partly to the fact
fates and nitrates have an overall cooling that significant amounts of long-lived GHGs are
(negative radiative forcing) effect, whereas black already in the atmosphere but also because reduc-
carbon has an overall warming effect [36]. There- tions in atmospheric aerosols in the next decade or
fore, while the reduction of PM improves air so will add to the positive radiative forcing of the
quality, it may result in further atmospheric Earth’s climate.
warming in terms of climate change. In addition Mitigation of short-lived agents with high radi-
to direct forcing, aerosols can also act as cloud ative forcing may reduce the possibility of cata-
condensation nuclei (CCN) and exert an indirect strophic climate change in particularly sensitive
effect on climate. The abundance of CCN affects regions such as the Arctic. However, mitigation
cloud formation and cloud lifetime, which in turn decisions must be based on sound science and
Regional Air Quality 369

would benefit from a sector-based approach 10. US EPA (2010a) Our Nation’s air, status and trends
accounting for benefits for health, ecosystems, through 2008. United States Environmental Protection
Agency
climate, and mitigation costs. While the ideal 11. Finlayson-Pitts BJ, Pitts JN Jr (2000) Chemistry of the
goal is to achieve win-win solutions for air pollu- upper and lower atmosphere: theory, experiments, and
tion and climate, in some cases health improve- applications. Academic, San Diego/London
ments via reductions in pollutant emissions may 12. Gurjar BR, Butler TM, Lawrence MG, Lelieveld
J (2008) Evaluation of emissions and air quality in
greatly outweigh possible negative effects on cli- megacities. Atmos Environ 42:1593–1606
mate. This is particularly true of the developing 13. Guttikunda SK, Tang Y, Charmichael GR, Kurata G,
world where improving health and ensuring food Pan L, Streets DG, Woo J-H, Thongboonchoo N, Fried
security currently have immediate priority over A (2005) Impacts of Asian megacity emissions on
regional air quality during spring 2001. J Geophys
the benefits of slowing the rate of climate change. Res 110:D20301
Nevertheless, the development of emission reduc- 14. Leighton PA (1961) The photochemistry of air pollu-
tion strategies or cleaner energy alternatives for tion. Academic, New York
both CO2 and shortlived climate forcers (SLCFs) 15. Soltic P, Weilenmann M (2003) NO2/NO emissions of
gasoline passenger cars and light-duty trucks with
are needed. There are clearly many challenges in Euro-2 emission standard. Atmos Environ
the area of air quality and climate and a need for 37:5207–5216
sound underpinning science across the spatial and 16. Carslaw DC (2005) Evidence of an increasing
temporal scales that air quality and climate act on. NO2/NOx emissions ratio from road traffic emissions.
Atmos Environ 39:4793–4802
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Retama A, Munoz R (2008) Weekly patterns of Mexico
City’s surface concentrations of CO, NOx, PM10 and O3
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Ozone hole Popular name given to the large
Stratospheric Pollution seasonal reduction in column ozone over Ant-
arctica, which currently occurs from August to
Martyn P. Chipperfield October each year.
Institute for Climate and Atmospheric Science, Stratosphere Region of atmosphere from about
School of Earth and Environment, University of 10–18 km to 50 km altitude. Contains 90% of
Leeds, Leeds, UK atmospheric ozone in the ozone layer.
Very short-lived species (VSLS) Source gas
with an atmospheric lifetime less than about
Article Outline 6 months.

Glossary
Definition of the Subject Definition of the Subject
Introduction
Stratospheric Ozone The stratosphere is the region of the atmosphere
Ozone Depletion between 8–18 km and 50 km altitude. This region
Ozone Recovery and Chemistry–Climate contains 90% of the ozone (O3) in the atmosphere
Interactions in the so-called ozone layer. Ozone is continually
Future Directions produced naturally in the stratosphere by sunlight
Bibliography and molecular oxygen. It is destroyed by a variety
of chemical species that are present in the atmo-
Glossary sphere both naturally and through human activi-
ties. The ozone layer prevents harmful short
Chemical transport model Three-dimensional wavelength ultraviolet radiation from reaching
model of atmospheric chemistry used to simu- the Earth’s surface and also plays an important
late past and present changes. role in the atmospheric climate balance. Over the
Chlorofluorocarbon (CFC) Class of chemical past few decades, increases in atmospheric chlo-
compound containing chlorine, fluorine, and rine and bromine have occurred through human
carbon. activities (e.g., use of chlorofluorocarbons or
Coupled chemistry-climate model (CCM) Ver- CFCs), and this has led to ozone depletion. The
sion of three-dimensional atmospheric climate most dramatic reduction in the ozone layer has
model with detailed interactive chemistry. occurred over the Antarctic in springtime where
Used to simulate past ozone changes and to about 70% of the column ozone is removed,
predict the future ozone layer. corresponding to complete loss in the lower strato-
Montreal protocol International agreement to sphere. Smaller depletion has been observed in the
limit and phase out production and emission Arctic winter and spring, and in the middle lati-
of chlorine- and bromine-containing ozone- tudes. An international agreement (The Montreal
depleting substances. Protocol and Amendments) has now acted to ban
Ozone Molecule containing three oxygen atoms the production and emission of CFCs and other
(O3). major ozone-depleting substances (ODSs). Over
Ozone-depleting substance (ODS) General the timescale of next 50 years or so the ozone layer
term for compounds which, when broken should recover, though the speed and extent of this
down in the atmosphere, can release chemical recovery will depend on stratospheric climate
species that destroy ozone. change.

© Springer Science+Business Media, LLC 2012 373


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_560
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_560
374 Stratospheric Pollution

Introduction O3 þ hv ! O þ O2 ð3Þ

The presence of the Earth’s ozone layer is essential Ozone (or odd oxygen) is destroyed by con-
for life on Earth. The realization that through version to O2 via:
human activities we had started to destroy it has
been a major science and environmental issue since O þ O3 ! 2O2 ð4Þ
the late twentieth century. This chapter briefly dis-
cusses the key science and policy issues behind the The first theory for the chemistry of the ozone
issue of global stratospheric ozone depletion. layer was put forward by Chapman in 1930
Section “Stratospheric Ozone” describes the [1]. His scheme comprised of reactions (1)–(4)
chemistry of ozone layer and summarizes the nat- and was therefore based on oxygen-only chemis-
ural and man-made substances, which can lead to try. The chemical loss of odd oxygen in the Chap-
its depletion. Section “Ozone Depletion” man mechanism occurs via reaction (4), i.e., the
describes observations of past ozone depletion direct reaction of O and O3. The Chapman mech-
and the policy measures which have been intro- anism successfully and qualitatively predicts the
duced to reverse this trend. Section “Ozone occurrence of an ozone layer in the stratosphere.
Recovery and Chemistry–Climate Interactions” However, by the 1960s, when good observations
discusses the likely future evolution of the ozone of the ozone layer became available and improved
layer and how this will depend on interactions laboratory measurements gave accurate values of
with climate change. Some future directions for the relevant chemical rate constants, it became
ozone layer research are outlined in section clear that the Chapman scheme could not explain
“Future Directions”. the observations quantitatively. While the Chap-
man scheme does include the source of strato-
spheric ozone (reaction 1), the direct reaction (4)
accounts for only about 20% of the actual loss.
Stratospheric Ozone
The Chapman mechanism ignores the very impor-
tant destruction of ozone by other chemical
The Stratosphere and the Natural Ozone Layer
families.
Ozone is produced in the stratosphere naturally by
the action of short wavelength ultraviolet radia-
tion (l  242 nm) dissociating oxygen molecules: Catalytic Ozone Loss
There are a number of cycles which can catalyze
the destruction of stratospheric ozone. Many
O2 þ hv ! O þ O ð1Þ
cycles are based on:

where hv is a photon of light with sufficient XO þ O ! X þ O2


energy to break the O–O bond. The O atoms pro- X þ O3 ! XO þ O2
duced can rapidly combine with another O2 mol-
Net : O þ O3 ! 2O2
ecule to form ozone:
In this scheme, the species X (in practice X ¼
O þ O2 þ M ! O3 þ M ð2Þ OH, NO, Cl, Br) reacts with O3 to form XO. XO
then reacts with O to reform X. Therefore, X is
where M is any third body. In fact, O and O3 form acting catalytically and the net effect of these two
a tightly coupled chemical family and are nor- reactions is the same as reaction (4) of the Chap-
mally considered together as “odd oxygen.” The man mechanism. In this way a species with an
production and removal of O or O3 is equivalent; abundance much smaller than O3 can cause its
destruction of O leads to O3 loss. O3 can be destruction, i.e., species present at the part per
converted back to O via: billion (1 in 109) or part per trillion (1 in 1012)
Stratospheric Pollution 375

level can affect ozone that is present in the part per one or more source gases, reservoirs, and radicals.
million (1 in 106) level in the stratosphere. Con- Source gases are the long-lived species (lifetime
cern over stratospheric ozone depletion really many years) which can be transported from the
started in the early 1970s with the realization surface to the stratosphere. Once in the strato-
that O3 could be destroyed catalytically by NOx sphere these source gases decompose to release
(NO + NO2) [2], and that large fleets of proposed radicals. These are the species which can catalyt-
supersonic aircraft, flying near 18 km, could ically destroy ozone in cycles described in section
directly inject NOx into the stratosphere [3]. As “Catalytic Ozone Loss”. However, the radicals
it turned out, very few supersonic passenger air- can also become temporarily tied up in reservoir
craft (i.e., Concorde) were built so the impact on species; these species do not destroy ozone and,
the ozone layer was small. In 1974, attention therefore, reduce the impact of the radical-
turned to chlorine when it was proposed that this catalyzed loss. Table 1 summarizes the main
family could catalytically destroy ozone [4]. stratospheric chemical families.
Catalytic cycles can also be based on: The only natural source of chlorine which gets
to the stratosphere is methyl chloride (CH3Cl).
X þ O3 ! XO þ O2 This is emitted from oceans and contributes
Y þ O3 ! YO þ O2 ð5Þ about 600 parts per trillion (pptv) to the atmo-
spheric loading, i.e., about 20% of the current
XO þ YO ! XY þ O2
total. The majority of chlorine in the present day
XY þ hv ! X þ Y atmosphere comes from manmade sources such as
ð6Þ chlorofluorocabons (CFCs), hydrochloro-
Net : 2O3 ! 3O2
fluorocabons (HCFCs), and solvents (e.g., CCl4,
CH3CCl3). The use of these species since the
The details of steps (5) and (6) vary between
1930s (e.g., CFCs were used as aerosol propel-
different cycles (i.e., different species X and Y),
lants and refrigerants) has resulted in a significant
though all such cycles catalyze 2O3 ! 3O2. As
increase in chlorine over the natural background
these cycles do not depend on the concentration of
levels. Similarly, industrial use of methyl bromide
atomic oxygen they are more efficient in the lower
and halons (used in fire extinguishers) has
stratosphere.
increased the atmospheric bromine loading to
about 20 pptv compared to background levels of
Stratospheric Chemistry about half that. Although bromine has a much
There are a number of important chemical fami- lower abundance in the atmosphere, it is about
lies whose species can lead to stratospheric ozone 50 times more efficient at destroying ozone
destruction. For each of these families there are because a smaller proportion is tied up in its

Stratospheric Pollution, Table 1 The four main chemical families in the stratosphere along with example source
gases, reservoirs, and radicals
Family Source gases Reservoirs Radicals
Hydrogen H2O H2O2 OH, HO2
CH4
Nitrogen N2O HNO3, N2O5 NO, NO2
ClONO2
Chlorine CH3Cl HCl Cl, ClO
CFCs ClONO2
HCFCs
Solvents
Bromine CH3Br HBr Br, BrO
Halons BrONO2
Shorter-lived organics
376 Stratospheric Pollution

reservoir species. Concern about the increasing ! 3O2) was proposed to explain how ClO could
levels of chlorine in the atmosphere started in destroy ozone in the cold polar lower stratosphere
1974 when Molina and Rowland [5] suggested when sunlight returns in spring [8]. Temperatures
that the only atmospheric sink for the stable, in the Antarctic lower stratosphere in winter, when
inert CFC molecules was transport to the strato- there is 24-h darkness, can reach as low as
sphere where they would be broken down by short 185–190 K. Strong westerly winds form a polar
wavelength UV radiation to release chlorine, vortex which isolates the stratosphere over Ant-
which could catalytically destroy ozone. arctica from middle latitudes. A key step to
explaining polar ozone depletion was the discov-
ery that polar stratospheric clouds (PSCs), which
Ozone Depletion form at around 20 km in the polar regions despite
the low pressures and dry stratosphere, could ini-
Polar Ozone Loss tiate heterogeneous reactions [9], which convert
The most dramatic manifestation of human- the normally stable reservoir HCl and ClONO2 to
induced ozone depletion has occurred over the the active radical form. Thus, it is the cold isolated
Antarctic in springtime, the so-called Antarctic conditions of the Antarctic lower stratosphere in
Ozone Hole. Reductions in the stratospheric winter and spring which favor ozone loss. Figure 1
ozone column over Antarctica were first detected shows satellite observations of the Antarctic
by Farman et al. [6] in the early to mid-1980s. Ozone Hole in 2009, along with calculations
Observations of ozone loss in this region were a from a state-of-the-art 3D model. Such models
complete surprise to the scientific community as it now include the relevant chemical processes and
was believed that in the cold Antarctic lower can reproduce the observed depletion well.
stratosphere, ozone should be very stable and The same chemical and meteorological pro-
long-lived. The publication of the observed cesses which occur over the Antarctic also occur
decrease initiated an intense period of scientific over the north pole. However, due to differences
study with field campaigns to Antarctica, analysis in surface orography, i.e., the northern hemisphere
of satellite data and numerical modeling. It was is more mountainous while the southern hemi-
rapidly established that the cause of the ozone loss sphere is largely ocean, the Arctic polar vortex is
was high levels of “active chlorine” [7], i.e., chlo- weaker, more disturbed, more variable, and
rine present as ozone-destroying radicals (ClO) warmer. Therefore, there is less occurrence of
rather than in the reservoir form. A new catalytic PSCs in the north, less activation of chlorine,
cycle involving the dimer of ClO (catalyzing 2O3 and less ozone depletion [11]. In cold Arctic

OMI satellite 3D model


23/9/2009

Stratospheric Pollution, Fig. 1 Ozone Monitoring on September 23, 2009 (left), along with calculations from
Instrument (OMI) satellite observations of total column the SLIMCAT 3D chemical transport model [10] (right).
ozone (Dobson Units) showing the Antarctic Ozone Hole (Image courtesy of W. Feng, University of Leeds)
Stratospheric Pollution 377

winters ozone loss of about 50% at 20 km, as PSCs in promoting heterogeneous reactions.
corresponding to about 30% of the column is Large volcanic eruptions can significantly
observed. enhance the stratospheric sulfate aerosol layer,
and increased ozone loss was observed after the
Middle Latitudes and Tropics eruption of Mt. Pinatubo in 1991 [14].
Ozone depletion has been observed at middle No significant decrease in column ozone has
latitudes. This reduction is not as large as been observed in the tropics (Fig. 2). However, it
observed in the polar regions and amounts to a is important to note that the ozone layer is natu-
decreasing trend of about 0.6%/year during the rally thin in this region of the world – by up to a
1980s and 1990s [12] (Fig. 2). The main chemical factor two compared to high latitudes. As the sun
cause of this midlatitude decrease is also the elevation is also larger in the tropics, humans can
increases in atmospheric chlorine and bromine. experience a much larger dose of excess ultravio-
The loss at middle latitudes can be caused by let radiation naturally at low latitudes than
export of ozone-poor or chlorine-activated air through the effects of ozone depletion at middle
from the polar vortex or by chemical processes or high latitudes.
occurring at midlatitudes [13]. Sulfate aerosols in
the lower stratosphere can perform a similar role Effects of Ozone Depletion
The ozone layer prevents wavelengths shorter
Global total ozone change than about 300 nm from reaching the Earth’s
Changes from 1964 to 1980 average surface, i.e., all UV-C radiation and most UV-B
2
radiation. Decreases in stratospheric ozone will
increase the amount of UV-B radiation reaching
0
the surface. This will affect human health (skin,
Ozone change (%)

eyes, and immune system), animal health, terres-


–2
trial ecosystems, aquatic ecosystems, biogeo-
chemical cycles, air quality and materials
–4
[16]. As ozone absorbs both in the ultraviolet
Average and infrared parts of the spectrum, it is intimately
–6
Range of observations coupled to atmospheric climate balance. Past
ozone depletion has acted to cool the surface of
–8
1965 1975 1985 1995 2005 the Earth, thereby offsetting some of the warming
Year caused by GHG increases [17]. Any changes to
Changes between 1980 and 2004 stratospheric ozone also have the potential to alter
the temperature and dynamical structure of the
0
atmosphere.

Montreal Protocol
–10 The seminal paper by Rowland and Molina [5]
Average
Uncertainty range first suggested that CFCs and other halocarbons
–20
could lead to reductions in the global ozone layer.
–90 –60 –30 0 30 60 90 This discovery prompted some efforts at regula-
South Latitude North
tion of CFCs within the USA. By 1978, some
Stratospheric Pollution, Fig. 2 Observations of global unilateral action was taken – the US banned the
ozone changes. The top panel shows changes in global sale of CFCs for use in spray cans. However,
ozone (based on ground-based and satellite observations) because of other uses of CFCs the atmospheric
from 1964 to 2005 relative to the 1964–1980 mean. Annual
and solar cycle variations have been removed. The bottom
abundance of these species continued to increase.
panel shows ozone changes between 1980 and 2004 as a The atmospheric models available at the time
function of latitude. (From [15]) predicted only modest decreases in ozone due to
378 Stratospheric Pollution

CFCs; the models were wrong because they did to ozone loss emerge. Following intense scientific
not contain a description of the role of PSCs and research in the late 1980s and 1990s to determine
heterogeneous chemistry. the cause of polar and global ozone depletion,
The first significant attempt at international such unequivocal evidence was found. The Mon-
regulation was the Vienna Convention for the treal Protocol was strengthened in a series of
Protection of the Ozone Layer in March 1985. amendments: London (1990), Copenhagen
This resulted in 22 countries agreeing to reduce (1992), Montreal (1997), and Beijing (1999).
CFC emissions and to study the impact of CFCs The past trends and predicted changes in strato-
on ozone further. In September 1987, the Mon- spheric chlorine based on these strengthened
treal Protocol was signed, initially by 27 countries, amendments are shown in Figs. 3 and 4.
leading to some limits in the production of CFCs Note that CFCs and other gases controlled
and halons. There were two key elements to the under the Montreal Protocol are potent green-
Montreal Protocol which contributed to its ulti- houses gases (GHGs). For example, CFC-12
mate success. First, a Multilateral Fund was set up (CF2Cl2) has a Global Warming Potential of
to help developing countries phase out the use of about 10,000 (on a 100-year time horizon). By
ozone-depleting substances. Second, the protocol removing these species from the atmosphere, the
allowed for strengthening of the regulations Montreal Protocol has had a significant effect in
should stronger scientific evidence linking CFCs preventing further climate change [18].

Past and expected future abundances of atmospheric halogen source gases


600
Effective stratospheric chlorine
2
CFC-12
CFCs 500
Mid
latitudes Halons
HCFCs
Relative amount

400
CCl4
CH3CCl3
1980 300 CFC-11
Atmospheric abundance (parts per trillion)

1
level
200
HCFC-22

100 CFC-113
CH3Br (natural + human sources)
CH3Cl (natural sources)
0 0
Atmospheric abundance (parts per trillion)

Estimates
120 Observations 4 Halon-1211
Future projections
100 3 Halon-1301
Carbon
2
80 tetrachloride (CCl4)
Methyl chloroform 1
60 (CH3CCl3)
0 12
HCFC-141b
40
500 Methyl chloride (CH3Cl) 10
HCFC-142b
20
400 Methyl bromide (CH3Br) 8

0 300 6
1950 2000 2050 2100 1950 2000 2050 2100
Year Year

Stratospheric Pollution, Fig. 3 The observed abun- trends and the scope of the Montreal Protocol. The top left
dances of the important bromine and chlorine source panel shows the accumulated effective chlorine due to all
gases and their expected future evolution based on current source gases. (From [15])
Stratospheric Pollution 379

15000 Montreal Protocol and Amendments. The proto-


Effective col allows for some continued production of
stratospheric Montreal HCFCs until 2030.
Predicted abundance (parts per trillion)

chlorine 1987
Overall, we expect the levels of atmospheric
No protocol
halogens (chlorine and bromine) to return to values
10000
when the Antarctic Ozone hole first appeared
London
1990 (1980) by about 2050. This date therefore sets the
reference point for the disappearance of the Ant-
arctic Ozone hole if the other atmospheric condi-
5000 tions remain constant. However, because of
Copenhagen
increases in greenhouse gases (GHGs), and asso-
1992 ciated climate change, the atmosphere in 2050 will
Beijing
1999
be markedly different to 1980. The main radiative
Zero emissions impact of GHG increases is a cooling of the strato-
0
500 sphere (accompanied by the well-known warming
Excess skin Montreal of the surface). This cooling of the stratosphere will
Cases per million people per year

cancer cases 1987


400 impact the temperature-dependent ozone chemis-
No protocol London try. Colder temperatures in the lower stratosphere
1990
300 will cause more PSCs and so while the halogen
loading remains high this could lead to increased
200 ozone loss. On the other hand, colder temperatures
Copenhagen will tend to slow down the rate of the gas-phase
1992 reactions which destroy ozone (from all cycles).
100
This will lead to more stratospheric ozone. Other
0
climate change feedbacks might occur, e.g., a
1980 2000 2020 2040 2060 2080 2100 strengthening of the stratospheric meridional cir-
Year
culation [19], which will transport more ozone to
Stratospheric Pollution, Fig. 4 The top panel shows higher latitudes. State-of-the-art predictions [20]
predicted abundance of effective stratospheric chlorine for the future of the ozone layer are shown in
(which combines chlorine and bromine) based on the Mon- Fig. 5. These CCM results show that rate of
treal Protocol and its series of amendments. The bottom
panel shows the estimated excess skin cancers which
ozone layer recovery will vary with region. The
would have resulted from these different scenarios. (From model experiments also clearly show that climate
[15]) change (stratospheric cooling) acts to speed up the
future increase in ozone.
Ozone Recovery and Chemistry–Climate The gray shaded line included both changes.
Interactions The blue shaded line shows the effect of ODS
changes only. The orange shaded line shows the
Surface observations of halocarbon source gases effect of GHG increases only. The pink line shows
from global networks have confirmed the success the change in ODS concentrations in the models
of the Montreal Protocol and Amendments in (right hand axis). (From [20]).
delaying, and reversing, the increase in atmo-
spheric chlorine concentrations. The abundance
of the shorter-lived source gases (e.g., CH3CCl3, Future Directions
lifetime 6 years) has peaked and these species are
now showing a decline. Longer-lived species An important current stratospheric science topic
(e.g., CFC-12, lifetime 100 years) have shown a concerns the rate of ozone recovery and the inter-
slowing down in growth and leveling off in abun- actions between this and climate change (see sec-
dance. This is consistent with the behavior tion “Ozone Recovery and Chemistry–Climate
expected under regulations imposed by the Interactions”). While the expected decrease in
380 Stratospheric Pollution

a Tropical upper stratosphere b Tropical lower stratosphere


3.0 3.0
0.60
1.0
2.0 2.0
0.30 0.5
Ozone [ppm]

Ozone [ppm]
ESC [ppb]

ESC [ppb]
1.0 1.0
0.00 0.0
0.0 0.0 –0.30 –0.5
100% –1.0 100%
–1.0 –1.0 75% –0.60 75%
50% 50%
25% –1.5 25%
–2.0 –2.0 –0.90
1960 1980 2000 2020 2040 2060 2080 2100 1960 1980 2000 2020 2040 2060 2080 2100

c NH midlatitudes upper stratosphere d NH midlatitudes lower stratosphere


2.0 4.0 2.0
0.40
1.0 2.0 1.0
0.20
Ozone [ppm]

Ozone [ppm]
ESC [ppb]

ESC [ppb]
0.0 0.0 0.00 0.0

–0.20
–1.0 –2.0 100% –1.0 100%
75% 75%
50% 50%
25% –0.40 25%
–2.0 –4.0 –2.0
1960 1980 2000 2020 2040 2060 2080 2100 1960 1980 2000 2020 2040 2060 2080 2100

e SH midlatitudes upper stratosphere f SH midlatitudes lower stratosphere


2.0 4.0 2.0
0.60

1.0 2.0 0.30 1.0


Ozone [ppm]

Ozone [ppm]
ESC [ppb]

ESC [ppb]
0.0 0.0 0.00 0.0

–1.0 –2.0 100% –0.30 –1.0 100%


75% 75%
50% 50%
25% –0.60 25%
–2.0 –4.0 –2.0
1960 1980 2000 2020 2040 2060 2080 2100 1960 1980 2000 2020 2040 2060 2080 2100

MMT 03 REF-B2(fODS) MMT O3(fGHG)

MMT 03 fODS MMT ESC REF-B2(fODS)

MMT 03 REF-B2(fGHG)

Stratospheric Pollution, Fig. 5 Results from lines are averages of around 15 CCMs used worldwide.
chemistry-climate model (CCM) simulations for the past The models ran three experiments to separate the effect of
and future evolution of the ozone layer. The panels show changing ODS and changing greenhouse gases (GHGs)
different geographical and altitude regions. The model

halocarbon ODS is believed to be fairly well as halocarbons are now declining, N2O will be the
constrained, there are many other uncertainties. major anthropogenic ODS. To research these
The future atmospheric concentrations of the issues of chemistry–climate interactions, and to
major GHGs CO2, CH4, and N2O are uncertain, quantify these impacts, will require the develop-
especially beyond the middle of this century. N2O ment of detailed Chemistry–Climate Models
itself is the source of stratospheric odd nitrogen, (CCMs). CCMs are essentially versions of climate
which can cause ozone loss (Table 1). models with detailed interactive chemistry. In the
Ravishankara et al. [21] argued that in the future, future, these models will become part of larger
Stratospheric Pollution 381

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Part III
Sensors, Measurement, and Control
Aerodynamic diameter The diameter of a spher-
Air Pollution Monitoring and ical particle of unit density with a terminal
Sustainability velocity equal to the particle being considered.
Aerosol Liquid- or solid-phase particles suspended
Andrew Knox1, Greg J. Evans1, Colin J. Lee1 and in a gas.
Jeffrey R. Brook1,2 Aerosol optical depth Total extinction of light
1
Department of Chemical Engineering and due to scattering and absorption by particles
Applied Chemistry, University of Toronto, suspended in air between the point considered,
Toronto, ON, Canada the light’s origin, and the point of observation.
2
Air Quality Research Division, Atmospheric Air pollution monitoring The use of scientific
Science and Technology Directorate, instruments and methods to assess the concen-
Environment Canada, Toronto, ON, Canada trations or rates of emission of air pollution in
various environments.
Air pollution policy Legal guidelines governing
Article Outline allowable emissions of pollutants to air, allow-
able concentrations of pollutants in air, and air
Glossary quality remediation efforts.
Definition of the Subject Air quality monitoring Observation of features
Introduction of air that relate to the air’s quality over some
Air Pollutants time period. Said features include concentra-
Currently Recognized Air Pollution Problems tions of pollutants.
Motivations Behind Monitoring Air Pollution Air quality The degree to which air is an ideal
Current Air Pollution Monitoring Practices supporter of life.
Past and Ongoing Success in Air Pollution Background level The concentration of a sub-
Mitigation stance or pollutant that remains regardless of
Outstanding Problems and Challenges short-term, local changes in emissions pat-
Current Air Pollution Monitoring and terns. Background concentrations are not
Sustainability static, but changes in background concentra-
Future Directions: Monitoring to Promote Greater tion happen over the relatively long term.
Sustainability Best available technology (BAT) A term relat-
Conclusion ing to emissions standards set based on the
Bibliography ability of existing pollution abatement technol-
ogy to mitigate the release of pollutants.
Glossary Biogenic Produced by biological organisms or
systems.
Acid deposition Settling on land or water of Biosphere All life and ecosystems on Earth.
acidic air pollutants or air pollutants capable Chlorofluorocarbons (CFCs) A class of chlo-
of becoming acidic once settled. rine or fluorine containing organic compounds.
Acid neutralizing capacity (ANC) The ability Climate change A long-term change in regional
of a medium (e.g., soil) to neutralize acidic pH, and global meteorological mean state or the
generally indicated by concentration of base variability of that mean state.
cations. Command and control A strategy for limiting
Adaptive capacity The capacity to adjust to new emissions by assigning specific emissions maxi-
circumstances such that successful functioning mums to pollution sources or otherwise imposing
can continue. pollution limiting rules and enforcing those rules.
© Springer Science+Business Media, LLC 2012 385
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_373
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media LLC, 2012
https://doi.org/10.1007/978-1-4419-0851-3_373
386 Air Pollution Monitoring and Sustainability

Concentration-response functions (CRFs) Natural capital The natural systems that pro-
The mathematical relationships between the duce goods such as clean air and provide ser-
environmental concentration of a pollutant vices such as life support to the biosphere.
and an effect of the pollutant. Effects, or Ozone layer A lower stratospheric region of
responses, could include health effects such more concentrated ozone, which absorbs
as premature mortality. much of the ultraviolet radiation from the sun.
Consolidated sustainability metrics Summative Particulate matter Solid or liquid particles
statistics that are a function of a number of data suspended in air. PM is not a term that distin-
on different species of pollutants and atmosphe guishes particles by chemical species, and indi-
ric conditions. Consolidated metrics are based vidual PM particles can contain a variety of
on a prior judgment of the relative importance species. Particulate Matter is often written as
of all the data in their calculation. They are desi PM10 or PM2.5 with the number in subscript
gned to give an overall picture and convey a denoting the maximum aerodynamic diameter
great deal of information in a single number or i in micrometers of the particles being described.
ndex. The subscripts (e.g., “2.5”) indicate that the PM
Critical load The maximum amount of pollution considered is less than the subscript’s value in
an ecosystem can tolerate without suffering micrometers (mm). Particles smaller than about
significant harmful effects, as far as can be 10 mm are generally considered inhalable with
understood given the present understanding. smaller particles reaching deeper into the lung.
Critical natural capital Natural capital that can- Pedestrian-oriented development Construction
not be lost without irreparable terminal damage or reconstruction of the urban form designed to
to ecosystems. facilitate walking as a primary means of per-
Ecosystem A system supporting life, including sonal transportation.
living and nonliving components and the inter- Point sources Localized emitters of large
actions between its components. amounts of pollution.
Enforcement Action taken or penalties imposed Population exposure A statistic accounting for a
to correct situations in which emissions or con- population’s distribution throughout the area it
centrations of pollutants are above the legal limit. inhabits, the pollution concentration distribu-
Exposure A time-integrated concentration met- tion over that area, and the changes in those
ric reflecting the potential for intake of distributions over time to represent the macro-
pollutants. level (population-level) exposure of the popu-
Greenhouse gas Gas which, when in the atmo- lation to a pollutant or set of pollutants.
sphere, induces a climate forcing via its ability Primary pollutants Pollutants released from a
to absorb light and convert it to thermal energy. source directly into the environment in the
Hazardous air pollutants (HAPs) Individual or given form.
families of compounds that can potentially Primary standards US EPA Air pollution stan-
induce adverse health impacts, including but dards set to protect public health.
not limited to cancer, reproductive effects, or Radiative balance The net radiation to or from
adverse environmental effects. an object or system accounting for total incom-
Holism The view that systems cannot be under- ing and outgoing radiation. A positive radiative
stood in exclusion of other systems but must be balance will lead to the warming of the system
understood in relation to the larger whole that considered, while a negative radiative balance
affects all parts within itself. will lead to cooling, assuming no non-radiative
Mortality A statistical measure quantifying the energy flows are at work.
number or fraction of deaths among populations. Resilience The ability of a system to renew and
Multipollutant monitoring Monitoring with reorganize itself after a shock or major socio-
attention to the effects of pollution arising ecological shift.
from the interaction of different species of Risk-based policy Policy based on the quantifi-
pollutants. cation and understanding of the probabilities of
Air Pollution Monitoring and Sustainability 387

damages incurred. In risk-based policy, allow- where humans exposure tends to occur but can
able pollutant concentrations are set with the also include measurements at other altitudes, in
knowledge and acceptance of the damage other spheres of the atmosphere, or in
likely to be realized. unpopulated areas. Monitoring data is often an
Secondary pollutants Pollutants not released important input into air pollution research
directly from sources but formed in the envi- projects.
ronment via chemical reactions among primary
pollutants facilitated by atmospheric condi-
tions such as moisture, temperature, and Introduction
sunlight.
Secondary standards US EPA Air pollution Air pollution monitoring is concerned with
standards set to mitigate regional environmen- collecting evidence about the emissions, concen-
tal problems. trations, and effects of air pollutants. There are a
Socio-ecological justice Fairness concerning number of effects of air pollution. Those most
both the social realm (e.g., fairness among commonly recognized are negative impacts on
social classes) and the ecological realm (e.g., human health, ecosystems, and the economy. Cur-
distribution schemes, including ecosystems as rent air pollution monitoring assesses the proper-
stakeholders), and the interaction between the ties of air pollution in the atmosphere by
two realms. monitoring ambient air, monitoring emissions
Source apportionment Attributing the pollut- from pollution sources, remotely sensing air pol-
ants in a region or at a receptor site to their lution indicators via satellite, and through the use
sources, for example, quantification of the por- of numerical models. Monitoring efforts allow for
tion of ambient NOx originating from the trans- air quality warnings, tracking trends over time, air
portation sector versus the industrial sector. pollution research, and policy development,
Target load The pollution burden aimed for in including pollutant concentration and emissions
policy. The load deemed achievable once “other standards. While air pollution monitoring has led
factors (such as ethics, scientific uncertainties, to many substantial successes in the reduction of
and social and economic effects) are balanced impacts from air pollution, many air pollution
with environmental considerations.” [1] problems are still outstanding.
Transit-oriented development Construction or Air pollution monitoring is an essential activity
reconstruction of the urban form designed to in the assessment of environmental quality and
facilitate use of public transportation vehicles provides information without which acting to pro-
as a primary means of medium to long-distance mote sustainability would be impossible. How-
personal transportation. ever, air pollution monitoring must be expanded
Troposphere The layer of the atmosphere clos- in breadth and depth if societies are to progress
est to the Earth’s surface, where human expo- toward sustainability. Monitoring must extend the
sure to air pollutants occurs. information provided in service of more diverse
Urban form The physical shape and design of goals. These goals should include facilitating
cities, their structures, and their infrastructure. urban design for air quality, socio-ecological jus-
tice, methods for acceleration of air pollution
research, resilience, and preservation of natural
capital. Work that crosses intellectual disciplines
Definition of the Subject would also help, as would public involvement in
monitoring. Immediate steps the air pollution
Air pollution monitoring is the use of scientific monitoring community could take to improve its
and mathematical tools and methods to assess the routine practice include the development of multi-
concentrations or rates of emission of air pollution pollutant impact assessments, greater consider-
in various environments. Monitoring is usually ation of consolidated metrics, more and better
performed at ground level in populated areas, use of satellite-derived observations, routine use
388 Air Pollution Monitoring and Sustainability

of available design methodologies in the design of classified as “criteria” pollutants. (In the USA,
monitoring networks, adhering to suggestions in the label “criteria” is applied to common pollut-
existing literature to improve routine practice, and ants. The EPA regulates these pollutants by set-
beginning to address some of the previously neces- ting permissible levels based on human health
sary oversimplifications involved in conventional or environmental considerations [2], whereas in
monitoring. While the air pollution monitoring com- Canada, pollutants fall into the “criteria” cate-
munity has a historical record of promoting sustain- gory as a result of sharing common sources,
ability and should be applauded, a paradigm shift is mostly notably, fossil-fuel combustion [3].)
needed if it is to address these expanded goals. The second type of air pollutant, the type capa-
ble of causing problems despite relatively low
average emissions rates, have been classified by
Air Pollutants the US EPA (US Environmental Protection
Agency) as “Hazardous Air Pollutants”
Air pollution monitoring is concerned with air (HAPs) for the particular hazards they present.
pollutants, substances which have negative One hundred and eighty-nine HAPs are offi-
effects on life. Some air pollutants are prevalent cially recognized by the US EPA [4]. Criteria
in most urban areas, and their effects are wide- pollutants and HAPs are discussed below, and
spread. Other air pollutants tend to be less con- classifications by different authorities are given
centrated, or are only concentrated in specific in Table 1. Typical ranges for many non-HAP
areas, but have gained attention for being espe- pollutants in the USA are given in Table 2.
cially problematic or acutely toxic. In the USA Table 3 summarizes the sources and effects of
and in Canada, pollutants of this first type are pollutants.

Air Pollution Monitoring and Sustainability, Environment Canada and the US EPA classify “particulate
Table 1 Pollutants and their classification by different matter” in general as CACs and Criteria Pollutants, respec-
systems. Pollutants are described in detail below. The tively [3]. Certain species of dioxins and furans are classi-
more acutely hazardous pollutants given here (those clas- fied as HAPs by the EPA, but not all are covered. CAC
sified as HAPs by the US system, for example) are only stands for criteria air contaminant, AQSP stands for air
examples and not an extensive representation of the full quality strategy pollutant, POP stands for persistent
range of hazardous pollutants. PM10 and PM2.5 are classi- organic pollutant [7], HAP stands for hazardous air
fied here as CACs by the Canadian classification and pollutant
Criteria Pollutants by the US EPA classification, as
Pollutant Canadian classification [3] UK classification [8] US classification [4]
CO CAC AQSP Criteria pollutant
NOx CAC AQSP Criteria pollutant
SO2 CAC AQSP Criteria pollutant
NH3 CAC
O3 CAC AQSP Criteria pollutant
VOC CAC
PM10 CAC AQSP Criteria pollutant
PM2.5 CAC AQSP Criteria pollutant
Dioxins and Furans POP HAP
1,3-butadiene AQSP
Benzene AQSP
Lead AQSP Criteria pollutant
Arsenic HAP
Cadmium HAP
Mercury HAP
Nickel HAP
Air Pollution Monitoring and Sustainability 389

Air Pollution Monitoring and Sustainability, What Are the Criteria Pollutants?
Table 2 Typical concentrations of pollutants in the USA Criteria pollutants include carbon monoxide
[13]
(CO), nitrogen oxides (NOx), and sulfur dioxide
US typical (SO2) [2]. Tropospheric ozone (O3) and Particu-
Pollutant US average range peakc
late Matter (PM) are also criteria pollutants. Most
COa 0.1–5 ppm 20 ppm
species of harmful Volatile Organic Compounds
NO2a 0.5–50 ppb 200 ppb
(VOCs) that are not acutely toxic enough to be
NOa 0–100 ppb 200 ppb
HNO3a 0–5 ppb 10 ppb
specifically identified as HAPs are included in the
SO2a 0.1–50 ppb 150 ppb criteria air contaminants in Canada [3]. Table 3
PM2.5 0.5–5 ng/m3 150 ng/m3 shows the common sources of the criteria pollut-
Leadb ants mentioned and comments on some of their
O3a 0–125 ppb 200 ppb effects.
(VOC)b 20–100 mg/m3 250 mg/m3 Emissions of CO are the result of the incom-
PM10b 10–100 mg/m3 300 mg/m3 plete combustion of carbonaceous fuels. Any use
PM2.5b 5–50 mg/m3 100 mg/m3 of fossil fuels can result in emissions of CO, but
(mean ¼ 13.4  5.6)
vehicles are the dominant source [5]. In motor
UFPa 1,000–20,000/cm3 100,000/cm3
a
vehicles, catalytic converters are often used to
Typical hourly average concentrations reached in US mitigate CO emissions. CO’s effects include
cities
b
Typical 24 h average concentrations human health impacts and contribution to the
c
Generally not in concentrated plumes or locations of direct formation of tropospheric ozone [6].
source emission impact NOx is the sum of NO and NO2. Atmospheric
nitrogen (N2) is oxidized during combustion to
form NOx. NOx is similar to CO in that it can

Air Pollution Monitoring and Sustainability, Table 3 Criteria pollutants, HAPs, their common sources, and effects.
(VOCs are considered CACs in Canada but are not on EPA list of Criteria Pollutants)
Substance Sources Effects
Criteria pollutants
Carbon Monoxide (CO) Combustion of fossil fuels, especially in motor Health effects, smog (Ozone)
vehicles formation
Nitrogen Oxides (NO2) Combustion of fossil fuels Health effects, smog (Ozone and
PM2.5) formation, and acid
deposition
Sulfur Dioxide (SO2) Combustion of sulfur containing fossil fuels and Health effects, acid deposition, smog
industrial activities (e.g., fuel refining, metal (PM2.5) formation, changes in
production) radiative balance
Tropospheric Ozone Chemical reactions involving other pollutants in Health effects, damage to
(O3) the atmosphere vegetation, damage to materials
Volatile organic Biogenic, vehicle emissions, petroleum products, Health effects, smog (Ozone and
compounds (VOCs) biomass combustions, landfill gas, sewage PM2.5) formation
treatment, off-gassing of building materials
Particulate Matter (PM) Varies by species, includes combustion emissions Health effects, visibility, changes in
(especially of biomass in wildfires and for fuel), radiative balance
secondary chemistry involving gaseous air
pollutants
HAPs
Hazardous VOCs Varies by VOC species Health effects, including cancer,
smog (Ozone and PM2.5) formation
Hazardous Metals Industrial sources Health Effects, soil contamination
(excluding lead) and
their compounds
Lead Fuels with lead additives, industrial sources Health Effects, soil contamination
390 Air Pollution Monitoring and Sustainability

lead to health effects and the production of tropo- various chemical species of PM exist, even
spheric ozone, its main source in many locations within single particles. Size classifications are
is emissions from vehicles, and catalytic con- typically given as PM10 (particles with aerody-
verters are used to minimize these emissions. namic diameters less than 10 mm), PM2.5
Other high-temperature combustion processes (particles with aerodynamic diameters less than
also contribute. Emissions of NOx can indirectly 2.5 mm), and Ultrafine Particles (UFP, particles
lead to acid deposition (or “acid rain”). with aerodynamic diameters less than 0.1 mm).
Combustion of fossil fuels containing sulfur Particulate species include sulfate (SO42 and
leads to emissions of SO2. Refining and production containing particles), nitrate (NO3), ammo-
of fuels and minerals (e.g., lead smelting, alumi- nium (NH4+), Organic Matter (OM), and Black
num refining) also emits substantial amounts of Carbon (BC). Long-term exposure to PM2.5 is
SO2. SO2 negatively impacts human health, con- one of the major immediate human health risks
tributes to acid deposition, and can promote aerosol from air pollution [14]. Specific health effects
formation and growth. Sulfate formed from SO2 is are varied but include cardiovascular and pulmo-
a major contributor to aerosol mass in some nary complications. Other effects of PM include
regions. Aerosol produced through historic emis- the ability to alter the radiative balance of the
sions of SO2 is believed to have caused a negative Earth [15].
climate forcing that suppressed temperature rise in
the second half of the last century. Using fuels that What Are the HAPs?
contain only trace amounts of sulfur, such as natu- Specific VOCs are very hazardous to human
ral gas, or that contain less sulfur, such as low- health. These include benzene, PAHs (polycyclic
sulfur coal, results in less emission of SO2. There aromatic hydrocarbons), 1,3-butadiene, ethane,
are also downstream options such as flue-gas propene, and some aldehydes [5]. Hazardous
desulphurization [5]. VOCs share sources with the bulk of VOCs.
Tropospheric ozone (O3) is a major irritant to Dioxins and furans are chlorine containing
human health and vegetation. O3 is a secondary chemicals with similar chemical structural ele-
pollutant, meaning that O3 is rarely directly emitted ments [16]. Their health effects can be extreme
from point sources but is formed via chemical and of a wide variety, including cancer and repro-
reactions involving other air pollutants such as ductive abnormalities [16]. Dioxins and furans
NOx and VOCs. tend to accumulate in soils and sediments, but
There is a multitude of volatile organic carbon their sources include sources of air pollution
(VOC) species both biogenic and such as municipal waste incinerators [16] and
anthropogenic. Many have been identified as par- pyrotechnics [17]. They are bio-accumulative
ticular hazards, and they are discussed in the sec- [18], meaning that they remain within the bodies
tion below on HAPs. Some anthropogenic VOCs of plants and animals that absorb them.
have been associated with causing cancer in Heavy metals such as arsenic and nickel are not
humans [9]. Anthropogenic sources include vehi- very prevalent in the atmosphere, other than near
cle emissions, petroleum product manufacture their industrial sources, but even at low concen-
and use, biomass burning, landfill gas, sewage trations they can produce serious health effects
treatment [10], and off-gassing from building [5]. These metalloids, metals and their com-
materials. Biogenic VOCs can be the result of pounds are classified as HAPs. Some lighter
the natural metabolic processes of life forms [11] metals are also classified as HAPs such as beryl-
and natural decomposition. VOCs play a crucial lium and cobalt [4].
role in the formation of tropospheric ozone [12]. Lead (Pb) is a HAP [4] worthy of note for its
PM (particulate matter) is a term that covers a relative abundance. Lead emissions are the source
wide variety of liquid and solid particles of a wide range of human health problems [19,
suspended in the atmosphere. PM is classified 20]. While lead as a fuel additive has largely been
by size (according to aerodynamic diameter) and phased out in the Western world, there are many
Air Pollution Monitoring and Sustainability 391

regions where it is still in use and continues to Europe, the “EU Focus on Clean Air” [23] lists
exist in high concentrations in the atmosphere climate change and the destruction of the ozone
[5]. Lead is classified both as a HAP [4] and a layer among air pollution issues, placing global
criteria pollutant in the USA [2]. problems alongside childhood asthma and acidi-
Mercury (Hg) is a HAP [4] with a number of fication of forests.
industrial applications, many still in use today In addition to human health and regional prob-
[21] and is a component of compact fluorescent lems, the economic problems caused by air pollu-
light bulbs. Coal combustion–based electricity tion are recognized by governments. For example,
generation is one of mercury’s major atmospheric Environment Canada recognizes that illness and
emission sources. Mercury is toxic to humans and, mortality resulting from air pollution can cause
once in the environment, can be methylated, workers to miss work and thereby have an adverse
whereupon it can easily bind to proteins and affect on the productivity of industry [24]. Eco-
enter the food chain [21]. nomic problems arising from air pollution are
discussed below along with other problems cur-
rently recognized by government agencies.
Currently Recognized Air Pollution
Problems Health
Human health is often the primary concern
Before resources can be committed to monitoring related to air pollution, and a great deal of
air pollution, the nature and extent of the problems work has been done to connect various air pol-
air pollution creates must be understood. Fenger [5] lutants to health risks. Table 4 identifies some of
cites three types of air pollution problems. These are the health problems associated with the different
local problems such as health effects and damage to air pollutants. The references given are exam-
goods and capital, regional problems such as acidi- ples of studies that have made connections
fication, and global problems such as climate between pollutants and health problems. Thus,
change. As air pollution problems scale up in phys- Table 4 should not be interpreted as an exhaus-
ical area (from regional to global, for example), their tive and critical review of the current state of
effects tend to scale up in terms of time. For exam- knowledge regarding air pollutant health
ple, an air quality episode may aggravate asthma in a effects. In some cases, many more studies have
population over the course of the episode (hours to confirmed these connections. However, in many
days), whereas acidification will impact the environ- cases, the underlying mechanisms that would
ment for decades and climate change will have conclusively demonstrate a cause and effect
impacts potentially lasting millennia [22]. The prob- relationship have yet to be identified. At the
lems receiving the most government recognition are present time, PM2.5 is considered to be one of
the local problems. Regional problems are recog- the pollutants of greatest concern [13, 25, 26],
nized by most governments, while some global but it is made up of thousands of chemicals that
problems are only recently appearing on the air can each have different types of effects. Ultra-
pollution agenda of some authorities (for example, fine particles are a subsize of PM2.5, and they
the US EPA only gained powers to regulate CO2 warrant further study to better understand the
emissions as of December, 2009). range of impacts on health they may cause.
Nowhere is the hierarchy of air pollution prob- The health effects of air pollution are usually
lems more apparent than in the US EPA’s division more pronounced in urban populations [5]. Urban
between primary and secondary air quality stan- settings tend to host more combustion
dards. Primary standards are set to protect public (of transportation and heating fuels, for example)
health, while secondary standards are set to miti- per area, leading to more emission of air pollution
gate regional problems, such as acidification, and per area than in rural settings. The higher population
biosphere damage [2]. There are no tertiary stan- densities of urban settings results in greater air pol-
dards set to mitigate global problems. However, in lution population exposure. With over half of all
392 Air Pollution Monitoring and Sustainability

Air Pollution Monitoring and Sustainability, Table 4 Air pollutants and their health effects. COPD stands for
chronic obstructive pulmonary disease. This table
Pollutant Associated health problems Reference
NO2 COPD, allergic response, increase in respiratory illness, increased airway [20, 27,
responsiveness to stimuli, lung inflammation, decreased pulmonary function, 28]
immunological changes, eye irritation
SO2 COPD, respiratory symptoms [20, 27]
CO COPD, Congestive heart failure, decreased time to onset of angina, behavioral [20, 27]
effects, developmental effects
O3 Lung inflammation, COPD, aggravation of asthma, eye and nose irritation, [20, 27,
pneumonia, increased airway responsiveness to stimuli, centroacinar fibrosis, 29–31]
immunological changes, excess mortality
PM10 Exacerbation of cardiac disease, lung cancer, allergic response, infant [25, 28,
mortality 32–34]
PM2.5 Acute and chronic cardiovascular effects, increased incidence of allergies, [13, 25,
excess mortality, lung cancer 35, 36]
Ultrafine PM Cardiorespiratory mortality, pulmonary stress, mitochondrial and DNA [37–41]
damage, potentially other effects as yet proven
Manganese (Mn) Parkinson’s Disease [42]
Mercury (Hg) Nervous system damage [43]
Lead (Pb) Reproductive problems, behavioral deficiencies in offspring, damage to lungs, [19, 20]
nervous system damage, lowered IQ, hypertension, coronary heart disease,
reproductive effects in women
Volatile organic Cancer [9]
compounds (VOC)s
Dioxins and furans Cancer, deficiencies in the immune system, reproductive and developmental [16]
abnormalities, nervous system damage, endocrine disruption, pulmonary
problems including bronchitis, altered testosterone levels, nausea, loss of
appetite, rashes, liver damage, and many others

people currently living in cities and the urban popu- Regional Problems
lation expected to grow to 70% of all people by 2050 Regional air pollution problems impact large areas
[26], the health impacts of air pollution will continue and substantially alter ecologies. Regional prob-
to be a challenge. Long-range transportation of air lems that have been recognized by governments
pollution and local point sources can make the health include acid deposition, damage to wildlife and
effects of air pollution a significant risk in rural ecosystems, and reduced visibility. In some areas
settings as well. of the globe, many of these problems have been
A cohort study of six US cites started in 1974 and substantially mitigated by changes in practice.
followed up through the present time, the “Harvard
Six Cities Study,” found that the average life expec- Acid Deposition Acid deposition is the settling
tancy in the dirtiest city studied (corrected for indi- of acidic air pollutants on land or water. The
vidual risk factors) was 2 years lower than in the pollutants contributing most significantly to acid
least dirty city [44]. This 2 year gain in average life deposition are oxidized sulfur and nitrogen com-
expectancy is equivalent to what would be expected pounds. When “wet deposited” (deposited on land
if all forms of cancer in the USA were eliminated by precipitation after being taken up in cloud
[44]. Indeed, as air quality has improved across the droplets) sulfur is usually in the form of SO42
USA in recent decades, life expectancy has risen due to oxidation of SO2 during atmospheric trans-
[45]. Thus it can be seen that the health effects of air port. When “dry deposited” (directly deposited
pollution pose a substantial problem while mitiga- from air onto Earth’s surface), it is usually in the
tion can offer substantial benefits. forms of SO2 and particulate SO42 [46]. NOx
Air Pollution Monitoring and Sustainability 393

reacts with water to form acids either while air- nature of acid deposition, it is likely that much
borne or after dry deposition. more area is threatened.
On a regional scale, farther downwind from
emission sources, wet deposition is the major acid Damage to the Biosphere In addition to the
deposition mechanism and has earned acid deposi- damages to forests and wildlife caused by acid
tion the popular name “acid rain,” though dry deposition, there are other damages caused by
deposition makes substantial contributions to eco- other forms of air pollution. Grantz et al. [55]
system acidification [46]. Acid deposition reduces provides Guderian’s categories of effects of air
ecosystem Acid Neutralizing Capacity (ANC) pollutants on ecosystems:
[47], making future influxes of acids more difficult
to cope with. It also has deleterious effects on soils, • Accumulation of pollutants in plants and other
vegetation, and aquatic ecosystems. ecosystem components (e.g., soil, water)
Leaching of soil nutrients is a major impact of • Damage to humans as a result of pollutant
acid deposition. Acids deposited in soil react accumulation
with the soil’s base cations (largely Ca2+ but • Shifts in competition causing changes in spe-
also Mg2+ and K+) and increase their mobility cies diversity
in soils, causing them to leach out of soils and • Disruption of biogeochemical cycles
making them unavailable for plant uptake • Disruption of stability and reduction in self-
[47]. Base cations can be the limiting factor in regulation capabilities
forest development and their loss has been iden- • Breakdown of stands and associations
tified as the source of decline in many forests • Expansion of denuded zones
[48]. Increased acidity in soils also negatively
impacts the microbial community in the soil, on Many of these types of impacts have been
which plant life depends, notably decreasing bio- observed and linked to particular pollutants. For
logical nitrogen fixation rates [49]. Acid deposi- example, mercury has been shown to be toxic to
tion stresses plant root systems and leaves [50] microorganisms, plants, and animals [56], and tox-
and can leach nutrients (Ca, Mg, and K) from icity of other heavy metals such as lead has also been
leaves just as it does from soils [51]. Acid and/or confirmed [19]. By binding to proteins, mercury can
nitrogen deposition have also been seen to also accumulate in organisms and ecosystems [21].
increase risk of winter injury in Red Spruce Ground-level ozone (O3) is a known hazard,
[52]. Acid deposition lowers the pH of lakes leading to reduced production of fine roots in
and streams, negatively affecting organisms at some trees [57], reduced tree growth [58], and
all levels of the aquatic biosphere in terms of damage to a plant’s photosynthetic systems
production and growth in lakes with low natural [59]. The reduced activity of plant life as a result
ANC [53]. Acute mortality and reproductive fail- of ozone will reduce an ecosystem’s ability to
ure has been a result among fish and some species store carbon and thereby exacerbates climate
have even been lost entirely [53]. change [60]. Damage and reduced yields of plants
Governments in North America and Europe will reduce the availability of food for wild ani-
have addressed acid deposition by limiting the mals, stressing those populations as well.
use of sulfur-rich fuels and introducing technolo-
gies to reduce emissions of chemicals that even- Visibility
tually result in acid deposition. Acid deposition Air Pollution (mostly particles) can reduce visi-
has been substantially reduced as a result of these bility. Severe visibility problems arising from
strategies, though many of its effects persist. poor air quality have recently been experienced
China has not yet addressed acid rain to the extent in some Chinese cities [61]. Human enjoyment of
that North American and European governments the environment is impeded by poor visibility and
have, and today almost 30% of China’s area suf- in extreme cases poor visibility poses a safety
fers from acid rain [54]. Given the transboundary hazard in aviation.
394 Air Pollution Monitoring and Sustainability

Economy meaning that American taxpayers are providing


Restricted activity and lost work days due to ill- substantial economic recompense for air pollu-
ness incurred by air pollution are included in the tion’s damage to crops.
costs of poor air quality [20]. These are costs There are a number of services of economic
both to the individual suffering the illness value delivered by ecological systems, including
(in terms of income) and to industry (in terms of dilution and treatment of wastes, employment,
lost productivity). Time lost by caregivers, for sequestration of carbon, provision of oxygen, and
example, the parents that miss work to care for production of goods such as timber, potable water,
an ill child, also results in financial costs and irrigation water [55]. The US EPA, 1997 [20]
[62]. Healthcare costs, including the fees of adds pesticides and drugs to the list of products
healthcare professionals and operating costs, are derived from ecosystems as well as recreation,
also a problem. Pain and suffering has a cost that reduced runoff, and reduced erosion to the list of
can be estimated by the price an individual is services of economic value. Efforts have been
willing to pay to avoid experiencing it [62]. Sim- made to estimate some of the economic effects of
ilarly, the amount people are willing to pay to air pollution’s impacts on ecosystems such as wet-
avoid risk of premature death can be used to lands, forests, and aquatic ecosystems, but realistic
estimate the cost of mortality [63]. estimates are difficult to reach [20]. Both the data
Loss of detail in carvings, discoloration of and the tools to make complete estimates are
materials, failure of protective coatings, and struc- lacking [20], as is the discourse to address some
tural failure are some of the outcomes of material forms of ecosystem damage. The effects of local
damage from air pollution [64]. These outcomes wilderness areas on property value are easier to
are the result of acid deposition on materials and estimate and work has been done in this area
oxidation from pollutants like ozone. Delucchi’s [70]. Such estimates can quantify some portion of
[65] review of cost estimates in the literature the costs of the expansion of denuded zones and the
yielded an estimate of $0.1–3 billion in material limitations to ecosystem development discussed
damage annually in the USA from ozone. SOx and above. However, property values are just one of
PM are estimated to do at least as much damage as many economic impacts associated with pollution,
ozone [65]. Mayerhofer et al. [64] estimated that leaving complete costs figures out of reach.
the damage from 1995 levels of air pollution cost An evaluation of the cost-effectiveness of the
Europe 2.3–5.3 trillion European Currency Units Clean Air Act (USA) over the 1970–1990 period
(ECU, 1995 value) in that year. Calcareous rock showed that the cost of compliance with the act
(marble and limestone) is vulnerable to air pollu- was $523 billion and gave the central estimate of
tion [66], and many historical monuments and the economic benefits as $22.2 trillion [20]. This
structures are made of such materials. estimate of benefits does not include complete
Ozone can enter plant leaves and damage evaluations of ecosystem benefits. The 1990
enzymes critical to photosynthesis, reducing the amendments to the Clean Air Act created
metabolism of plants and limiting plant growth market-based mechanisms for trading of SO2 in
[67, 68]. Ozone, other oxidants, SOx, and NOx are an effort to reduce emissions and emissions were
thought to be responsible for 90% of damage to reduced by 40% between 1990 and 2007. Over the
plants from air pollution [68]. Damage to crops same period, 25 member countries of the EU
results in less revenue for agricultural producers. reduced SO2 emissions by 70% using conven-
Murphy et al. [67] estimate that in 1990, anthro- tional, non-market-based legislation [71].
pogenic ozone caused $2.8–5.8 billion in damage
to 8 major crops in the USA (corn, soybeans, Global Problems
wheat, alfalfa hay, cotton, grain sorghum, rice, Air pollution and its effects do not respect national
barley). Barley and soybeans are particularly sen- boundaries. Regardless of the location of the point
sitive to damage from SO2 [67]. Subsidies to these of emission, some problems arising from air pol-
crops in the USA are on the order of billions [69], lution affect multiple countries. Some, like the
Air Pollution Monitoring and Sustainability 395

destruction of the ozone layer and climate change, including economic costs, and global problems.
are a problem for all life on Earth. Effects on health and the global economy are far
from negligible, and the urgency of regional and
Ozone Layer Destruction While tropospheric global environmental problems is apparent. None
ozone can be harmful, the stratospheric ozone of these problems at their current magnitude are
layer prevents much of the sun’s ultraviolet radia- compatible with sustainability. If the Earth’s
tion from reaching the Earth’s surface. Anthropo- growing civilization is to be sustainable, under-
genic chlorofluorocarbons (CFCs) emitted to the standing air pollution in an effort to minimize its
atmosphere can act to convert stratospheric ozone direct and indirect impacts must be a priority.
into oxygen through a series of reactions. Once the
reactions are complete, the destructive capacity of
the CFCs is left intact. The reaction series is able
Motivations Behind Monitoring Air
to begin again, destroying more ozone through a
Pollution
catalytic process [72]. In the mid- 1980s, a large
hole in the ozone layer above the Antarctic was
Immediate benefits of air pollution monitoring
documented, as was the general depletion of
include knowledge of when and where standards
stratospheric ozone. The damage to the ozone
are violated and the ability to communicate health
layer led to the Montreal Protocol, which legis-
risks. Communication of health risk can be
lated reductions in the production of ozone-
accompanied by warnings that can guide behavior
depleting substances such as CFCs [73]. While
of individuals, populations, and industry and
existing ozone-depleting substances will, over
reduce human exposure to air pollution.
decades, be removed from the atmosphere [72],
While minimizing health problems and ensur-
other factors affecting stratospheric ozone chem-
ing that standards are adhered to are important,
istry, many of which are anthropogenic, make for
there are deeper motivations for the monitoring of
some uncertainty about whether the ozone layer
air pollution. Establishing and quantifying con-
will ever return to the pre-1980s levels [73].
nections between air pollution and the related
impacts depends on measurements such as those
Climate Change Air pollutants such as methane
made through monitoring and related air pollution
and nitrous oxide are greenhouse gases and, as
research. For example, epidemiological studies of
such, act to increase the Earth’s trapping of elec-
associations between air pollution and related
tromagnetic radiation, leading to the increase in
hospital admissions could not occur without air
global average temperatures often referred to as
pollution monitoring. By proving connections
global warming or climate change. Some Green-
between air pollution and problems, monitoring
house Gases (GHGs) are affected by air pollution
and the related research influence air pollution
through chemical reactions [74], and GHGs such
policy. It is anticipated, but not guaranteed, that
as CO2 are co-emitted with primary pollutants,
continued improvement of policy will drive
especially during fossil fuel combustion. Ozone
improved mitigation efforts and hence avoidance
in particular affects the lifetime of GHGs
of the problems associated with air pollution.
[74]. Other effects of climate change include such
global problems as rising sea levels, likely extinc-
tion of 15–30% of species (with a 2 °C increase in Air Quality Warnings
global average temperatures), reduced agricultural Monitoring of air pollution yields data on present
productivity, and fresh-water shortages [75]. air quality conditions that can be used to provide
health warnings. For example, Canada’s Air
Summary of Air Pollution Problems Quality Health Index (AQHI) combines data on
The motivating factors behind air pollution mon- ozone, PM, and NO2 to produce an AQHI value
itoring include understanding air pollution’s ranging from 1 to 10+. Advice associated with
impacts on human health, regional problems the AQHI is given in Table 5 and ranges from
396 Air Pollution Monitoring and Sustainability

Air Pollution Monitoring and Sustainability, Table 5 Canadian air quality health index (AQHI) and related health
advice [76]
Air Health advice
quality
health
index At risk populations General population
1–3 Enjoy your usual outdoor activities Ideal air quality for outdoor activities
4–6 Consider reducing or rescheduling strenuous No need to modify your usual outdoor activities
activities outdoors if you are experiencing unless you experience symptoms such as coughing
symptoms and throat irritation
7–10 Reduce or reschedule strenuous activities Consider reducing or rescheduling strenuous
outdoors. Children and the elderly should also activities outdoors if you experience symptoms such
take it easy as coughing and throat irritation
10+ Avoid strenuous activities outdoors. Children Reduce or reschedule strenuous activities outdoors,
and the elderly should also avoid outdoor especially if you experience symptoms such as
physical exertion coughing and throat irritation

“Enjoy” usual activity to “Avoid” strenuous out- 4. At what rate and by what process is a given
door activity. pollutant rendered benign in the environment?
Ideally, this health advice, if followed, would 5. What are the health effects of a specific pol-
reduce the impact of air pollution by reducing the lutant or set of pollutants?
rate of exposure. Air Quality Indices designed to 6. What is a population’s or an individual’s expo-
inform the public and potentially alter behavior sure to a specific pollutant or set of pollutants?
exist in the USA, China, Europe, and other areas 7. What are the effects of a specific pollutant or
of the globe [14]. set of pollutants on outcomes other than
health?
Research 8. What is a given practice’s effect on air pollu-
Research serves the function of improving the tion levels (e.g., how does highway driving
understanding of air pollution, how it behaves, its affect air pollution levels)?
sources, and its connection to the problems it causes. 9. How are levels of air pollutants changing (are
It can also lead to advancement of monitoring tech- they decreasing as expected given current pol-
niques. In an effort to classify research questions icies or are they rising in particular regions)?
typically asked in the field of air pollution research, 10. How does a specific instrument, method, or
a survey of research questions from 40 articles type of analysis perform?
pertaining to air pollution published in early 2010 Investigations of these questions inform the air
in peer reviewed journals was performed. Research quality monitoring community, are informed by the
questions appearing in this snapshot of the literature data collected by said community, and guide inter-
tend to be related to the following broad questions: pretations of data. They provide information on the
nature of air pollution, the connections between air
1. What is the nature of a given pollutant or set pollution and problems, and the effects of human
of pollutants (in terms of pollutant properties, behavior on air pollution. They also allow progress
distribution, and transport patterns in the in the air pollution monitoring field.
atmosphere)?
2. Can we improve our understanding of the Questions Regarding the Nature of Air
factors influencing air quality (e.g., meteoro- Pollution
logical factors)? Research questions of types 1–4 are important to
3. What chemical or physical mechanisms the development of the understanding of the
explain some yet unexplained observations? nature of air pollution and specific pollutants.
Air Pollution Monitoring and Sustainability 397

Fundamental questions such as these aid in design or underappreciated issues may be found to be of
of mitigation strategies, monitoring strategies and great importance, thus warranting a change in
technologies, and can inform policy. They can monitoring. Furthermore, relationships between
also suggest reasons why pollution is a problem air pollution and its impacts can change over
and which kinds of problems can be expected time, meaning that the nature of established rela-
from particular pollutants. tionships requires continual monitoring.
Questions of type 4 are directly relevant to Weatherhead and Anderson’s 2006 [73] study is
sustainability. A sustainable system would not an example of the understanding of a relationship
involve emissions rates higher than the rate at changing as a result of continued questioning. The
which pollutants are rendered benign. Answers assumption was that the ozone layer would regain
to questions of type 4 should inform allowable its former abilities as CFC concentrations
rates of emissions. declined. However, other anthropogenic factors
are playing a role in reducing the rate of recovery,
Questions Connecting Air Pollution to despite a decline in CFCs [73]. Airborne PM is
Problems another example. Monitoring first dictated that
Question types 5–7 help to establish connections total suspended particulate (TSP) be measured.
between air pollution and the problems that make However, monitoring evolved with increased
air pollution a subject of concern and make moni- understanding of health effects and the nature of
toring a necessary mitigation strategy. Without PM. This increased understanding, itself facili-
questions such as these, other types of air pollution tated by monitoring, recommended that attention
questions loose much of their practical application. be paid to specific size fractions of PM, first PM10,
These questions are central in “risk-based” air pol- and later PM2.5. If connections to problems are not
lution management strategies, which frame accept- continually reviewed, monitoring can lose it rele-
able levels of pollution in terms of the degree to vance to its objectives.
which their effects are deemed acceptable.
Examination of these questions shows how Research Questions and the Development of
established air pollution objectives affect the Air Pollution Monitoring Questions about the
research agenda. As has been discussed, govern- nature of air pollution can aid development of new
ments tend to emphasize the impacts of air pollu- monitoring technologies and deployment strate-
tion on health, some selected environmental gies. For example, Miffre, et al. [77] reveals infor-
issues, and the economy. As a result, research mation about the differences between air pollution
questions of types 5–7 more frequently attempt concentrations at ground level and at 50 m above
to make connections to these issues as opposed to ground. The findings show when it is valid to
issues given less attention such as the effects of air assume that ground-level monitoring is sufficient
pollution on overall quality of life or the health of in estimating concentrations at higher elevations
other species. (Climate change is a notable excep- and when it is not. This study and studies asking
tion, however, and does receive much attention). similar questions directly inform how much infor-
Question 7 covers a broad area of research and mation can be taken from a given monitoring
is often split into several questions investigating practice and when more monitoring is necessary,
the effects of air pollution on climate change, increasing the potential for optimally efficient
acidification, ozone depletion, economic dam- monitoring. Questions connecting air pollution
ages, and other unintended consequences of air to problems can guide monitoring so that it is
pollution. If the focus of air pollution monitoring more likely to take place at the point in a pollut-
is to shift toward sustainability, these types of ants life-cycle that is most directly related to the
questions will join health-related questions as problems of concern. If monitoring can take place,
questions of central importance. where it is most relevant to problems arising from
Questions connecting air pollution to impacts air pollution, it will be more efficient and will
require continual study. Previously unrecognized yield the most relevant and useful results.
398 Air Pollution Monitoring and Sustainability

Questions of type 8 can direct monitoring to • Inputs for the further development of models
the areas where there is likely to be air pollution which can improve predictive capacity.
by developing an understanding of which prac- • Information necessary to prove links between
tices are likely to create the most pollution and pollution concentrations and effects.
which are relatively benign, requiring less moni-
toring. Questions of type 9 bring about under- Typical observations made during monitoring
standing of how changes in practice impact air include concentrations in ambient air (in ppm, mg/m3,
pollution concentrations and whether current pol- particles/m3, mol/L, etc.), rates of emission, typi-
icies are effective. Type 10 questions can lead to cal concentration ranges, rates of change of con-
development of new technologies and strategies centration, and concentration profiles. It is in
for monitoring, as well as improvements to terms of ambient concentration that pollution
existing techniques. standards are set. For example, the European stan-
dard for ozone is set such that the maximum
concentration of ozone averaged over any 8 h
Current Air Pollution Monitoring period of the day should not exceed 120 mg/m3.
Practices Thus, it can be seen that monitoring is important
to ensuring that air quality standards are adhered
Common pollutants (Criteria pollutants, CACs) to, and that public health and the environment are
are routinely monitored in the USA, Canada, protected.
Europe, throughout Asia, and elsewhere. Net-
works of in situ monitoring stations in these
regions provide constant measures of air quality In Situ Monitoring
and help governments and concerned organiza- Air quality monitoring stations exist in the hun-
tions determine how close they are to meeting dreds in some countries and in the thousands
their air quality goals. Precipitation chemistry globally, covering continental areas and forming
monitoring also provides data on pollutants in networks that contribute the bulk of information
air. Satellite remote sensing and air quality models to assessments of outdoor air quality. Instruments
complement the data collected by monitoring sta- capable of detecting specific pollutants (NOx,
tions to form a more complete picture of air qual- SOx, PM2.5, etc.) draw in ambient air and accu-
ity and can offer the advantage of consistent rately measure the pollutant mass per standard
methods across the globe. Stack emissions for volume of air. This type of monitoring, referred
point sources are occasionally monitored in to as in situ monitoring, results in the least uncer-
some countries to complement the ambient con- tainty as compared to satellite remote sensing and
centration data collected by monitoring networks, model estimates. It is important to recognize that
though more often large emitters estimate their the in situ data from a given monitoring location
emissions using mass-based flow balances for are only for the specific geographic location and,
their site and rates of activity. Numerical model- thus, during the process of site selection, the issue
ing of air pollution can be a stand-in when mea- of spatial representativeness must be considered
sured data are sparse, it can be used in conjunction in the context of monitoring objectives.
with other forms of monitoring, and can help Most existing stations measure near ground
predict the effects of changes in emissions pat- level (~3–10 m) so that air pollution at the expo-
terns. Craig et al. [14] list the outcomes of moni- sure height of the general populace can be quan-
toring air pollution as follows: tified. Figure 1 shows the location of ozone
monitoring stations throughout North America.
• Ability to describe risks and detect potential It is largely through such networks of stations
future risks. that an area’s compliance with current air quality
• Documentation of trends, which can demon- standards is determined. Networks are also a pri-
strate the impacts of policies. mary tool in the tracking of progress toward air
Air Pollution Monitoring and Sustainability 399

YT

NT NU

NF

BC MB
AB
QC
SK

PE
ON NB
NS

0 495,000 990,000 1,980,000 m

Air Pollution Monitoring and Sustainability, Fig. 1 Ozone monitoring station locations throughout North America

quality goals, and they provide the necessary SO42, NO3, Ca2+, and Na+ [79]. These data
baseline measurements for judging whether pro- are valuable in tracking the acidity of rain over
gress is occurring [78]. Despite there being over time and in studying wet deposition. The identity
1,000 stations in Fig. 1, there are relatively large and concentrations of ions discovered through
unmonitored areas. Network design to minimize precipitation chemistry monitoring can also pro-
the impact of this inevitable incomplete coverage vide information about the sources of pollutants,
remains an ongoing challenge and, as described as in Thepanondh et al. [81]. By monitoring the
below, models and remotely sensed observations concentration of wet-deposited air pollutants in
are helping to fill in the gaps. precipitation, precipitation chemistry monitoring
acts as a valuable element of air pollution
monitoring.
Precipitation Chemistry Monitoring
By collecting and analyzing precipitation, sta-
tions and networks in North America (e.g., Satellite Remote Sensing
CAPMoN, NADP [79]), Asia (e.g., EANET Satellites can observe electromagnetic radiation from
[80]), throughout other continents, and over the the atmosphere and Earth’s surface to infer informa-
Ocean [81] can collect data on air pollution. tion about concentrations of aerosols and trace gases
Precipitation samples can provide information in the atmosphere. Pollutants that can be observed by
on pH and the mass of various ions such as satellites include PM, tropospheric O3, NO2, CO,
400 Air Pollution Monitoring and Sustainability

HCHO, and SO2 [82]. Figure 2 shows satellite- pollutant concentrations and distributions to iden-
observed NO2 concentrations in Eastern China. tify sources [82]. Point source data can be used to
Satellites can be used to analyze and forecast air model forward in time to obtain estimates of future
quality, provide information on tropospheric air pollutant concentration. Together, satellite obser-
pollution, and be used in conjunction with com- vation and computer modeling can increase the
puter models. Analyses made possible by satellites certainty of air quality estimates [83] and the attri-
include observation of events too large in scale to bution of pollutants to specific sources. Satellite
be appreciated using monitoring stations on Earth’s observations can also achieve spatial resolution of
surface. Such events include the difference in pollutant concentration over an area that could only
regional NO2 concentrations between average con- be replicated by a large number of ground-based
ditions in China and the period surrounding Chi- monitoring stations, a number that could only
nese New Year illustrated by Fig. 2. Many spatial come at great cost [83].
features related to typical emissions and those Another advantage of satellite observations is
resulting from the change in emissions are better global uniformity. Satellites should ideally be able
characterized and hence understood using the sat- to measure regions equally well across the globe,
ellite observations. Forecasting is made possible by in developed and developing countries, using the
observation of synoptic scale meteorology. Obser- same measurement techniques and producing data
vations of surface air quality can be combined with in a uniform format. In reality, differences in sur-
other observations such as those from monitoring face albedo, vertical mixing, aerosol optical
stations and point source emissions monitoring to depth, and other factors create inconsistencies in
increase certainty of pollutant concentration mea- the surface concentrations estimated from satellite
surements. Computer modeling aided by satellite data for different regions. However, once these
remote sensing allows for pollution source appor- technical challenges have been overcome, this
tionment by working backward from present global uniformity should facilitate simpler

Chinese new year Rest of winter

40°N Beijing Beijing

Shanghai Shanghai
30°N
Hangzhou Hangzhou

105°E 115°E 125°E 105°E 115°E 125°E

0 5 10 15 20 25 30 35
NO2 column density ( × 1015 molecule cm–2)

Air Pollution Monitoring and Sustainability, shows columns from all other days during the period in
Fig. 2 Ozone Monitoring Instrument retrieved NO2 col- question. Satellite measurement can show regional scale
umns over Eastern China. All data for January 25 to March effects which would be difficult to discern with a surface
5 were averaged for years 2005–2010. The left image monitoring network. Free use of tropospheric NO2 column
shows only overpasses taken between Chinese New Year data from the OMI sensor from www.temis.nl is acknowl-
and 2 weeks after Chinese New Year. The right image edged [84]
Air Pollution Monitoring and Sustainability 401

international cooperation in studies and provide a area sources, and it is sometimes useful to think of
standard set of data for the comparison of global vehicle emissions as arising from area (or line)
cities’ air pollution footprints. Satellite observa- sources. Monitoring emissions from any of these
tions also allow for the tracking of these city sources requires cooperation from industry and
footprints over time, allowing for a record of the government [78]. Efforts made toward achieving
trend toward sustainability. These advantages sustainability will rely on accurate and timely
make satellite observation an important evolving emissions monitoring data both to inform model-
tool in global cooperation in the pursuit of sus- based decision making and to ensure that emission
tainability. Developing methods for using reduction goals are achieved.
satellite-derived data to provide information on
sustainability should be a priority in future. Numerical Modeling
Air quality models use input from meteorological
Emissions Monitoring models and emissions from point and area sources
Emissions monitoring provides data on the rates to estimate air pollutant levels and deposition
of emissions from pollution sources. These data amounts based upon current understanding of rel-
make for strong inputs into air quality models evant chemical and physical processes. Models
[78], can ensure that emissions are not exceeding can predict chemical changes in air pollutants
permitted values (either legally permitted or per- over time [14], clarifying links between secondary
mitted with respect to sustainability), and lead to pollutants and sources. Models can estimate
confirmation that emissions are decreasing over changes in air pollution concentrations that
time in compliance with regulations. Emissions would result from changes in practice (i.e., emis-
trading schemes are dependent on emissions mon- sions), making modeling a valuable tool in policy
itoring. Figure 3 shows a Google Earth image of design and analysis of proposed policy
point sources of air pollution in North America. [78]. While originally developed mainly for this
Continuous Emissions Monitoring Systems purpose, models are increasingly being used to
(CEMS) quantify gas or particulate emissions by provide optimal estimates of air pollutant concen-
taking measurements as pollution is released. trations over areas where data do not exist.
CEMS are common for some major stationary Approaches for using models in conjunction
sources in the USA and Europe, where their use with in situ monitoring data and satellite data are
is mandated by legislation [85, 86]. PEMS rapidly evolving [83, 90]. This practice can lead to
(Predictive Emissions Monitoring Systems) use the most complete, consistent spatial-temporal
emissions factors and activity indicators (e.g., picture of air pollutant levels on the regional to
fuel use, engine types, duty cycles) in calculations global scale and is also valuable for identifying
that estimate emissions without measuring them. weaknesses in current emission inventories.
CEMS and PEMS are commonly applied to sta- These “fused” data (data derived from multiple
tionary sources or point sources, but emissions types of observations) can extend estimates of the
monitoring can also be applied to mobile sources impact of air pollution has on health and the
such as locomotives [87] and ships [88]. Sources environment, helping to better document prob-
too numerous to be monitored as individual lems and improve research. Increasing interest in
sources are often treated as “area sources” providing the public with future air quality infor-
[89]. To treat sources such as residential furnaces mation, which as described above can help reduce
or urban fuel stations as single sources would not impacts, has led to models that are optimized for
be practical, so emissions from these sources are forecasting on a daily basis.
often calculated and treated as emissions not from Regardless of their application, air quality
the individual sources but from the bulk of those models require evaluation to assess the reliability
sources of a given type over an area. Agricultural of their results. Any model being used to inform
sources such as livestock operations and emis- policy should have each of its aspects verified,
sions of N2O from fertilizers would be considered including its design, methods for representing
402 Air Pollution Monitoring and Sustainability

Environment Environnement
Canada Canada

NPRI INDUSTRIAL SECTORS


ALUMINUM
CEMENT, LIME AND OTHER NON-METALLIC MINERALS
CHEMICALS
ELECTRICITY
IRON AND STEEL
MANUFACTURING, OTHER
METALS (EXCEPT ALUMINUM AND IRON AND STEEL)
MINING AND QUARRYING
OIL AND GAS PIPELINES AND STORAGE
OILSANDS AND HEAVY OIL
PETROLEUM AND COAL PRODUCTS REFINING AND MFG.
PLASTICS AND RUBBER
PULP AND PAPER
TRANSPORTATION EQUIPMENT MFG.
UPSTREAM OIL AND GAS
WASTE TREATMENT AND DISPOSAL
WATER AND WASTEWATER SYSTEMS
WOOD PRODUCTS
OTHER (EXCEPT MANUFACTURING)

Air Pollution Monitoring and Sustainability, National Pollutant Release Inventory (NPRI) at http://
Fig. 3 Google Earth image showing point sources of air www.ec.gc.ca/inrp-npri/default.asp?lang¼En&n¼1D892B9
pollution in North America. USA layer available from the F-1#npri. Both include source specific data on tonnage of
US EPA at http://www.epa.gov/air/emissions/where.htm. criteria pollutants emitted. Legend for USA sites at top left,
Canadian layer available from Environment Canada’s legend for Canadian sites at bottom left

processes, input data (e.g., emissions), and numer- standards and which areas require the most
ical methods [78]. When supported by detailed pollution-abatement planning.
measurements, evaluation exercises also identify Policies on air pollution centre on concentra-
specific weaknesses in models and possible ways tion standards and emission standards. Standards
to improve future versions. are often set based on concentrations deemed
achievable using the Best Available Technology
(BAT) for emissions reduction (an example of a
Policy and Air Pollution Standards “command and control” strategy), the effects of
Air pollution policy is a major influence on mon- air pollution deemed acceptable (an example of
itoring and monitoring is a major influence on “risk-based” strategy), or a hybrid of the two
policy. Policies determine legally acceptable con- strategies [91].
centrations of air pollutants. Monitoring shows While monitoring and the related science is
which pollutants must be subject to improved one influence on policy and standards, it is not
Air Pollution Monitoring and Sustainability 403

the only influence. Political and economic consid- example of the difference between the two
erations also play a role and can make for situa- terms. A critical load is what has been deter-
tions where environmental damage is accepted mined to be close to the maximum amount of
despite preventability. Monitoring alone cannot pollution an ecosystem can tolerate. (In the case
deliver sustainability without policy and practices of Environment Canada’s Acid Rain critical
in accordance with the information it yields. loads, the aim is to protect 95% of lakes, based
on surface area, from acidification beyond crit-
Concentration Standards Assessing compli- ical levels.). A target load, the pollutant load
ance with standards is the primary goal of the aimed for in policy, is the load deemed achiev-
majority of air pollution monitoring [92]. These able once “other factors (such as ethics, scien-
standards are in the form of maximum allowable tific uncertainties, and social and economic
concentrations of air pollutants. Table 6 gives effects) are balanced with environmental
standards for some major world regions, which considerations.”[1]. Though the Canada-Wide
are often expressed as an average concentration Acid Rain Strategy for Post-2000 set the long-
over a specific time period, for some major world term goal of meeting the critical load, in the
regions. short term this system of standard setting deter-
mines a level of pollution slightly more than
Emissions Standards Figure 4 shows how emis- what could be sustained (the critical load) and
sions reduction programs play a part in achieving aims to allow more pollution than that
concentration standards once air quality goals are (by aiming for the target load). The critical and
established. Emission reduction programs can target load system has also been applied in areas
involve encouragement of energy efficiency, of Europe. The different grades of Chinese air
changes in practices (e.g., switching to cleaner quality standards in Table 6 are another example
fuels, use of emissions controls technology), and of standards not based on the recommendations
redesign of processes. They can also include set- of the air pollution monitoring community or on
ting of emissions standards, which limit emissions the basis of sustainability. The different grades
from particular sources or classes of sources. For are assigned based on land use (e.g., residential
example, vehicles in Europe must not exceed the vs industrial) and the economic realities of those
allowable emissions under the “Euro” class of areas, not on changes in the definition of sus-
emissions standards for CO, NOx, certain classes tainability from area to area. Policy-makers con-
of hydrocarbons, and PM [93]. sider much more than what is sustainable when
Monitoring is integral to the “Establishment of setting standards, and when doing so, the ten-
Air Quality Goals” and “Track and Evaluate Pro- dency is to make standards less stringent, mean-
gress” stages of Fig. 4 and informs the under- ing sustainability is sacrificed further.
standing of “Current Ambient Air Quality.”
Monitoring not only informs policy development, Polluters can also play a role in affecting air
but also the assessment of policy effectiveness. quality standards. There are concerns that setting
stringent air pollution standards will cause pollut-
Non-environmental Considerations in the Set- ing industries to relocate to “pollution haven”
ting of Standards Air pollution monitoring is countries where standards are more lax, though
one influence on policy and concentration stan- the idea that moving to one of these havens actu-
dards, but politics, economics, and other consid- ally benefits businesses is dubious [96]. Fear of
erations also play a role [14]. There are at times such moves can erode the economic base of a
differences between what the scientific data rec- policy-maker’s purview, providing an incentive
ommend as the concentration standard and what to weaken standards. Fredriksson and Gaston
the concentration standard is in law. The usage of [97] review a number of cases in which environ-
“critical loads” and “target loads” in the in the mental policy was weakened by business lobbies
Eastern Canada Acid Rain Programs is a telling representing polluters. Clearly, pollution policy
404 Air Pollution Monitoring and Sustainability

Air Pollution Monitoring and Sustainability, Table 6 Air quality standards by world region
Standards
USA primary standards China [54]
Averaging Europe [94] [95] Grade 1 Grade 2 Grade 3
Pollutant period Conc. Conc. Conc. Conc. Conc.
CO 1h 35 ppm 10 mg/m3 10 mg/m3 20 mg/m3
CO 8h 10,000 mg/ 9 ppm
m3
CO 24 h 4 mg/m3 4 mg/m3 6 mg/m3
NO2 1h 200 mg/m 3
120 mg/ 240 mg/ 240 mg/
m3 m3 m3
NO2 24 h 80 mg/m3 120 mg/ 120 mg/
m3 m3
NO2 1 year 40 mg/m3 0.053 ppm 40 mg/m3 80 mg/m3 80 mg/m3
SO2 1h 350 mg/m3 0.075 ppm 150 mg/ 500 mg/ 700 mg/
m3 m3 m3
SO2 24 h 125 mg/m3 0.14 ppm 50 mg/m3 150 mg/ 250 mg/
m3 m3
SO2 1 year 0.03 ppm 20 mg/m3 60 mg/m3 100 mg/
m3
Lead (Pb) 3 months 0.15 mg/m3
Lead (Pb) 1 year 0.5 mg/m 3

O3 1h 160 mg/ 200 mg/ 200 mg/


m3 m3 m3
O3 8h 120 mg/m3 0.075 ppm
Benzene 1 year 5 mg/m3
PAHs 1 year 1 ng/m3
PM10 24 h 150 mg/m3 50 mg/m3 150 mg/ 250 mg/
m3 m3
PM10 1 year 40 mg/m3 100 mg/ 150 mg/
m3 m3
PM2.5 24 h 35 mg/m3
PM2.5 1 year 25 mg/m 3
15 mg/m3
Arsenic (As) 1 year 6 ng/m3
Cadmium 1 year 5 ng/m3
(Cd)
Nickel (Ni) 1 year 20 ng/m3

making is the result of many disparate influences. concentrations [54]. In the case of the USA, it must
Amid social, political, and economic debates be noted that the trend in average concentrations of
involving varying interests, the goal of sustain- most criteria air pollutants is downward [98]. How-
ability is often minimized or even lost. ever, in the USA, in 2007, 21% of sites monitoring
PM2.5 exceeded the 24 h standard of 35 mg/m3,
Violations of Concentration Standards Unfor- 23% of sites monitoring lead showed concentra-
tunately, standards are targets, not guarantees of tions in excess of the 0.15 mg/m3 standard, and
maximum concentrations. As of 2004, 20.2% of 57% of sites monitoring O3 exceeded the
Chinese cities exceeded Grade III standards, 0.075 ppm standard [99]. The UK’s ozone standard
though this rate was an improvement over the is exceeded several times each year [89]. In record-
53.8% of cities exceeding Grade III standards in ing exceedences of standards, air pollution moni-
1991 and was part of an overall trend of decreasing toring demonstrates the need for continued
Air Pollution Monitoring and Sustainability 405

Current ambient air Scientific evidence of


quality health effects

Policy environment
Government commitment
Establish air quality goals Economic impacts
Cultural/social conditions
Stakeholder participation

Determine emissions Develop emissions


reduction reductions programmes

Track and evaluate


Implement programmes
progress

Air Pollution Monitoring and Sustainability, Fig. 4 Steps in the emissions reduction cycle including policy lead-up.
Figure is based on [99] and [14]

improvements in emissions abatement and shows air pollution problems [101]. The concept of crit-
where the need is greatest. It also demonstrates that ical load is an example of a scientific tool that aids
standards and monitoring alone cannot lead to air pollution problem solving [101]. It is also an
sustainability. Strong enforcement of standards example, as discussed above, of scientific knowl-
must make air pollution a consideration in the edge being used as a framework but not being
development and uptake of technologies. fully respected by the political process. While
science is the basis of policy’s discourse, as well
The Effects of Air Pollution Science on as the basis for policy evolution, there is room for
Policy Air pollution policy, like all environmental improvement in how science and policy cooperate
policy, is dependent on research and the state of in achieving sustainability.
science. If science has not developed the discourse
to describe an air pollution issue, there are no Policy and Air Pollution Standards:
grounds or even terms to support policy-based mit- Conclusion Policy sets standards by which the
igation. For example, it is believed that different results of air pollution monitoring are judged.
species of air pollutants may act together to produce Concentration standards indicate accepted levels
more severe health impacts than either species of air pollution in ambient air, and emissions
would produce if acting alone, but the current under- standards are measures of how much any source
standing of synergistic interactions is inadequate to can contribute to air pollution. Political, social,
support this level of policy development [100]. and economic considerations often influence stan-
Air pollution science is also critical in identi- dards and result in more lax standards than science
fying the most significant contributors to pollution or sustainability would recommend. Even in these
[100] and can use this and other information to cases of standards not consistent with sustainabil-
recommend optimally cost-effective solutions to ity, standards are often exceeded. Much of air
406 Air Pollution Monitoring and Sustainability

pollution monitoring is designed to assess com- Europe and, in Canada, lead is almost
pliance with standards [92], but neither standards undetectable in the atmosphere [5]. Regulations
nor standards-oriented monitoring alone will controlling particulate were the most cost-
ensure sustainability. effective regulations the US government put into
The current air pollution monitoring establish- force [44], and human life expectancy has
ment can contribute to ultimate sustainability increased as air quality has improved in the
through ongoing scientific assessment in support USA [45].
of increasingly appropriate concentration stan- Countries managing air pollution have seen a
dards. Monitoring and the related research can decline in ambient HAP concentration, with ben-
show, and have shown, that in many cases lower zene, 1,3-butadiene, styrene, xylenes, and toluene
ambient air pollution concentrations are possible, concentrations decreasing by at least 5% per year
necessary, and cost effective. Thus, new policy in the USA from 2000 to 2005 [99]. A major
and better standards are encouraged through the factor in this success was the control of emissions
results of monitoring. Translating air pollution from chemical plants, dry cleaners, coke ovens,
monitoring into policies that support sustainabil- and incinerators. The continued reduction in
ity may be a considerable challenge. Hurdles may CFCs discussed above is a landmark success in
include political and economic dampening of the air quality policy and international policy in
recommendations of science, and ongoing viola- general.
tions of existing standards. However, progress is In many cases, serious efforts to reduce the
essential as without monitoring sustainability presence of a pollutant in the environment can
becomes virtually impossible to verify. Further, succeed. Air pollution monitoring brings prob-
if monitoring is to verify sustainability, it needs lems to attention so that these efforts can be
to be based on goals and policies that balance the made. It also tracks the impacts of pollution mit-
social, environmental and economic aspects of igation strategies, indicating success when it is
sustainability. The monitoring community can achieved and allowing for comparison of the
play an important role in establishing such holistic effectiveness of different strategies. If not for
standards for air quality. monitoring, the successes mentioned here would
be impossible to quantify or prove. Adaptive man-
agement strategies would also be impossible.
Past and Ongoing Success in Air
Pollution Mitigation

In general, OECD countries have seen concentra- Outstanding Problems and Challenges
tions of most major (or criteria) air pollutants
decrease since the introduction of pollution man- The successes mentioned above are not unmiti-
agement programs. One of the biggest victories gated. pH and ANC in ecosystems damaged by
has been sulfur emissions, which were the focus acid rain are not recovering in proportion to
of acid rain reduction programs. Sulfur emissions, decreases in acidifying emissions [47]. The
again, in OECD countries, are much lower than Ozone layer’s recovery is not proceeding in pro-
they were in the past [5]. Acid rain is decreasing in portion to decreases in CFC emissions but is being
the USA [99], Canada [98], and elsewhere. NO2, retarded by other anthropogenic air pollutants
thanks largely to the use of catalytic converters in [73]. Catalytic converters used to decrease NO2
vehicles, is on the decline in most European cities emissions cause a net increase in fuel use, pro-
[5], throughout the USA [99], and Canada mpting Fenger [5] to comment we may have mit-
[102]. Limitations on lead in gasoline have led igated one problem by aggravating another.
to substantial reductions of lead in air. Concentra- Reduction in NO2 emissions have not led to the
tions of lead are consistently below the WHO reductions in tropospheric ozone that were hoped
concentration guidelines throughout Western for [12].
Air Pollution Monitoring and Sustainability 407

The story of lead as a gasoline additive is an emissions standards are not set to serve sustain-
example of how reduction of a pollutant does not ability. Air quality objectives that will allow the
always result in greater sustainability. With lead no eventual recognition of sustainability once it has
longer an acceptable fuel additive, methyl been achieved, or even how far away sustainabil-
tert-butyl ether (MTBE) was used to perform its ity currently is, are lacking. The biosphere is still
function. However, MTBE was later found to be a being damaged by air pollution. Acid rain is
powerful contaminant of water and a likely carcin- declining in developed countries, but is still
ogen [103]. Now bio-ethanol is being discussed as beyond the critical load, is increasing in some
a less poisonous fuel octane booster than MTBE, regions, and totally unmonitored in others. Thus,
but it introduces its own risks of soil and ground- despite progress in recent decades, there is little
water contamination and can lead to increased reason to believe that we currently have a sustain-
emissions of NOx and organics [104], not to men- able burden of pollutants in our atmosphere. Thus,
tion stresses on global food supplies and agricul- there are considerable challenges remaining for
tural resources (i.e., land and water). While the air pollution monitoring community in rela-
legislation such as the USA’s Clean Air Act was tion to sustainability.
successful in reducing emissions from gasoline, it
did not eliminate the environmental threat of fuel
oxygenates. More holistic systems and policies, Current Air Pollution Monitoring and
rather than the reactionary phasing out of particular Sustainability
pollutants, are necessary to truly solve the problem.
Further, when implementing such policies, we Diverse techniques contribute to the monitoring
need to anticipate potential associated conse- of pollution in the atmosphere. This monitoring
quences and be prepared for follow-up monitoring allows for air quality advisories, research into the
so that we can detect any resulting impacts. nature and sources of air pollution, evaluation of
In addition to the problems remaining after the conformity with standards, and assessment of
emissions and ambient concentrations of pollut- the need for additional or alternate regulations or
ants have been reduced, there are instances where policies. All of these outcomes of air pollution
reductions in concentrations elude the efforts of monitoring reduce the burden of air pollution on
policy, technology, and behavioral changes. Over human society and the environment. Unfortu-
half of the population of the USA lives in counties nately, what is learned and understood is not pro-
where air quality standards are exceeded [99]. O3 portionate to action taken. Pollution is still
in populated areas such as those in Southern eroding the capacity for sustainability. Improve-
Ontario is continuing a long-term trend of increas- ments on all fronts are necessary, including
ing concentrations [105] despite decreases in improvements in air pollution monitoring, the
concentration of precursors, leading to questioning associated science, practices, the thinking that
of the fundamental scientific assumptions underpins them, and the social response they
surrounding tropospheric ozone concentrations receive. Determination of what constitutes a sus-
[106]. Background ozone is increasing in parts of tainability standard or threshold will also require
the northern hemisphere, and this increase may be further work.
linked to intercontinental transport of pollutants
[107]. Ozone and PM concentrations also continue
to be challenges throughout the USA [99]. Future Directions: Monitoring to
Despite the effort and advances made in Promote Greater Sustainability
research, policy, and environmental practice, air
pollution is still a health problem, a visibility In redesigning the air pollution monitoring com-
problem, and an economic problem. Further, munity and the larger air pollution establishment
only weak links exist between air quality objec- for sustainability, there are a number changes to be
tives and sustainability. Concentration and made to current practices. There are both broad, or
408 Air Pollution Monitoring and Sustainability

institutional, changes and specific changes to be form, and accelerated learning and research. Stud-
made. The institutional changes will be more diffi- ies with these goals in mind have been performed
cult to affect in that they require overcoming cur- infrequently, and they are fertile ground for new
rent inertia. These changes are discussed research.
immediately below. Specific changes are discussed
in the “Monitoring More Effectively” section. Both Natural Capital Natural capital is a metaphor
types of change will help the science of air pollu- used to describe the natural features of ecosystems
tion monitoring encourage sustainability. that do work or provide services for humans and
the biosphere. It is useful in that it draws attention
to these features and their indispensable services
Changes in Institutional Practices
such as clean air, potable water, food, and building
Institutional changes that would make air pollu-
materials while drawing comprehensible analogs
tion monitoring more relevant to sustainability
to economic concepts. Pollution that makes air a
include the expansion of the conventional goals
health risk, destruction of the ozone layer by air
of air pollution monitoring, working across intel-
pollutants, acidification of ecosystems via acid
lectual disciplines, and involving the general pub-
rain, and alteration to the climate by air pollutants
lic in the monitoring process.
such as black carbon aerosol are all examples of
air pollution destroying natural capital. All of
Expansion of Goals Air pollution monitoring
Guderian’s categories [55] (“Damage to the Bio-
practices are largely determined by the goals
sphere” section) are ways in which air pollution
underlying air pollution mitigation strategies.
depletes natural capital. Natural capital is often
When assessment of health impacts is the goal,
extended to include the capacity of systems to
more monitoring happens in populated urban
assimilate waste, such as the atmosphere’s capac-
areas. The hierarchy of goals in current air pollu-
ity to assimilate air pollution, and the life support
tion mitigation tends to prioritize human health,
functions provided by ecosystem components,
then visibility, then ecosystems [55], then possi-
such as the ozone layer’s UV blocking
bly the prevention of economic damage from air
capabilities [108].
pollution, or even climate stability in rare cases.
The assessment of the cost-effectiveness of the
Often studies are oriented toward only one of
US Clean Air Act, as mentioned, gave a mid-value
these goals.
of the benefits of the Act of $22.2 trillion but
could not include the further benefits of preserva-
Sustainability requires holistic thinking and if tion of natural capital [20]. All production and
sustainability is the aim, prioritizing based on a consumption in the human economy depends on
hierarchy of problems alone can reduce the poten- natural capital [108, 109]. Minimum estimates of
tial benefits. Prioritizing air pollution impacts the value of natural capital and ecosystem services
immediately affecting humans (e.g., health exceed the value of the human economy [110,
effects) over environmental impacts is self- 111]; yet, the discourse for the quantification of
defeating. In the long term, it is possible that the natural capital has yet to be fully developed. Fur-
loss of ecosystem services arising from these thermore, efforts to monitor and quantify pollu-
lower-priority environmental effects may be the tion’s impact on natural capital are rare [112],
greater consequence to humans [55]. Holistic making the inclusion of natural capital loss in
thinking would take into account many more the Clean Air Act’s benefits or in the cost-benefit
goals in air pollution mitigation than health, visi- analysis of new air quality policy options near
bility, ecosystem damage, economic loss, and cli- impossible. Data on natural capital are limited
mate. A holistic system would involve monitoring and thus far unsatisfactory, and types of natural
air pollution with goals such as the development capital, such as types more vulnerable to air
of natural capital, resilience in human and natural pollution versus types more vulnerable to
systems, environmental justice, improved urban other damages, have yet to be disaggregated
Air Pollution Monitoring and Sustainability 409

[113]. Assessment of loss of natural capital must for adaptation at worst, possibly allow for avoid-
become a priority for the air pollution monitoring ance of the worst consequences of system shocks,
community, as should the categorization of types and expose opportunities to take advantage of
of natural capital vulnerable to air pollutants. upcoming changes at best. The development of
Mechanisms to ensure that natural capital is fairly appropriate atmospheric indicators of ecological
recognized in policy development need to be system shifts would be a major research project
installed at the international level. and require much innovative air pollution moni-
Critical natural capital, natural capital that can- toring. One aspect of such indicators would be
not be lost without irreparable terminal damage to placing the concentration of air pollutants in the
ecosystems and thereby similar damage to the context of the capacity of systems to continue to
human economy, must also be considered. This absorb more pollution without major changes in
critical natural capital cannot be lost or exchanged their behavior [114]. Indicators could also include
and, therefore, is literally priceless [108]. Critical- how the dynamic capacity (ability to reorganize
ity of natural capital can be judged in terms of around changes) of environmental sinks (e.g., the
source and sink functions (sources of ecosystem atmosphere) are affected by continued pollution
services and pollution sinks) and life support [114]. These types of indicators would be along
functions [114]. Examples of critical natural cap- the lines of damage-oriented metrics used in life-
ital would be keystone species or keystone pro- cycle assessment methods.
cesses [108], which can be affected by air Resilient systems are contrasted with vulnera-
pollution. There is a certain level of natural capital ble systems, in which small changes can cause
that must be maintained to preserve the biosphere disastrous consequences. The resilience of the
and hence humanity. Unfortunately, where this human population is a sustainability-relevant met-
level lies is not yet understood, especially in ric to be developed. Resilience in this population
terms of atmospheric aerosol loading and chemi- comes under fire when exposure to pollution
cal pollution [115], two areas directly relevant to increases human vulnerability to disease, as has
the air pollution monitoring community. Air pol- been shown to be a likely outcome of exposure to
lution monitoring and air pollution science must some air pollutants [117, 118]. Monitoring to
be oriented toward defining where atmospheric expose the development of vulnerabilities would
natural capital becomes critical, how air pollution be a useful endeavor in the promotion of resil-
is damaging natural capital, and the quantification ience. It would also be useful to show how the
of natural capital savings from emissions reduc- allocation of the most polluted land to the most
tions. Air pollution monitoring could also provide vulnerable populations (babies, young people), as
data on the development and redevelopment of in Mitchell and Dorling [119], and the associated
natural capital. increases in asthma, other respiratory illnesses,
and allergies are affecting the ability of humans
Resilience A sustainable system must be resilient to reorganize around potential atmospheric
to external shocks and major changes, but the changes. Development of such indicators will
socio-ecological concept of resilience encom- rely on air pollution monitoring data.
passes more than an expectation of a return to
business as usual. Socio-ecological resilience is Socio-ecological Justice The social justice of
not only the ability of a system to retain basic environmental protection is a fundamental tenet
functions despite a shock. It is also the capacity of sustainable development [119]. Environmental
for renewal, reorganization, and development justice is concerned with equal access to a clean
[109]. Air pollution monitoring should accept environment and equal protection from risks asso-
the possibility of major system changes and mon- ciated with environmental impurities [119]. Cur-
itor for gradual atmospheric change as early warn- rently, economically disadvantaged communities
ing signs of upcoming system shifts [114, are often more exposed to air pollution than more
116]. Early warnings would allow for preparation affluent communities [117]. Poorer individuals
410 Air Pollution Monitoring and Sustainability

are more likely to live near roadways, resulting in where environmental injustice exists. As O’Neill
greater exposure [117]. In their study of London, et al. [117] state, “Science and public policy
MacKerron and Mourato [120] observed that would benefit from additional research that inte-
communities with the least car ownership are grates the theory and practice from both air pollu-
exposed to the highest concentration of pollutants, tion and social epidemiologies to gain a better
while the cleanest air tends to be in communities understanding of this issue.”
where car ownership is greatest. Marshall et al.
[121] shows that lower-income neighborhoods Improved Urban Form Design of urban form
tend to have higher walkability (resulting in less can mitigate exposure and reduce emissions
auto emissions), but also higher NO concentra- [5]. Urban sprawl results in increased automobile
tions, while higher income neighborhoods tend to dependency and the associated emissions
have lower NO and O3 concentrations. In these [122]. Many studies have witnessed the negative
cases, the injustice is that the people polluting the correlation between urban density and per capita
most impose the cost of their pollution on those transportation emissions [123]. Frank et al. [124]
polluting least. Identification of such injustices makes the connection between neighborhood
should be a focus of air pollution monitoring. walkability and reduced vehicle emissions. The
Routine increased exposure itself may enhance US EPA has acknowledged the relationship
the impacts of air pollution on socioeconomically between urban form and emissions through its
disadvantaged groups by weakening normal bio- program of offering urban nonattainment areas
logical resistance [117] or promoting atheroscle- emissions credits for “smart growth” development
rosis [118]. Housing stock in poorer practices [123]. Conventionally, air pollution mit-
neighborhoods can have higher rates of off- igation has been technology oriented, and Stone
gassing of some allergens and expose occupants [123] claims that the EPA’s program of emissions
to other risk factors of asthma sensitization and credits for intelligent urban design is an acknowl-
exacerbation [117]. These phenomena require edgement that the technological approach alone is
greater documentation by air pollution monitoring not sufficient to solve air pollution problems. This
agencies so that they can be addressed. recognition reinforces the point that sustainable
Often young families cannot afford to live in solutions must be holistic and that no single ave-
more affluent neighborhoods and must purchase nue leads to sustainability. Air pollution problems
lower cost housing. This situation has lead to cannot be solved by dealing with the emission
findings such as those of Mitchell and Dorling sources alone, there must be systemic redesign
[119], that pollution in London is most concen- of the landscapes that create demand for emitting
trated where young children and their parents live. activities.
London wards with a high proportion of all babies The air pollution monitoring community can
in the city tend to have much higher than average play a role in urban design for emissions reduc-
concentrations of NO2. This injustice is exposing tion. One major contribution would be taking
pregnant women, children, and babies (segments stock of various types of urban forms that exist
of the population very vulnerable to the health and the contribution of those forms to emissions.
effects of air pollution) to greater air pollution Tang and Wang [125] look at the four different
concentrations than those more resistant. urban forms on the Macau peninsula and associate
Much environmental justice work has been form with emissions and air pollution. Observa-
done in the USA to attempt to redress the effects tions connecting road width, road curvature, and
of the frequent location of landfills and polluting congestion with emissions were made, and it was
industries in black and indigenous communities. seen that features such as urban canyons can lead
A lack of empirical evidence led to failure of to increased pollution in areas of cities least
many of the class actions meant to address envi- responsible for total emissions. Other features
ronmental injustice [119]. Air pollution monitor- Tang and Wang [125] recommend for study
ing should be used to supply empirical evidence include street orientation in relation to wind
Air Pollution Monitoring and Sustainability 411

direction, interactions between urban form and for source apportionment, chemical transport
wind speed, building design, green spaces, and modeling, assessment of background levels, and
traffic control schemes. All of these aspects of relationships between pollutants and other effects
urban design require further research to determine [92]. The link between air pollution and urban
their impact on air pollution, while data from form could also be better established if available
monitoring will help to substantiate the under- data were used for that purpose. If priority con-
standing thereby derived. tinues to be given to compliance over other uses of
Designing urban areas for walkability and pub- data, few of the other goals discussed herein will
lic transit will also impact emissions of air pollu- be easily pursued. Chow and Watson [92] give
tion. PODs (Pedestrian-Oriented Development) specific practices that can be implemented to shift
and TODs (Transit-Oriented Development) such emphasis toward research, including calibrating
as those discussed in Newman et al. [126], can instruments to detect lower concentrations,
lower transportation energy demand and thereby decreasing time resolution of sampling, and
reduce emissions from vehicles. A study of reporting data to the level of detection rather
walkability in Vancouver showed that urban than rounding to convenient orders of magnitude.
design had a substantial impact on walkability Policy recommendations are also made, including
and air pollution exposure, and proved an effec- periodic reviews of instrument performance.
tive method for connecting air pollution monitor- Acceleration of learning, of which research is a
ing to urban design and possible future fundamental part, should be more of a focus in
development [127]. Designing for less depen- routine monitoring. Thus resources need to be
dence on automobiles is a very effective strategy allocated to ongoing analysis and interpretation
for using urban form to mitigate air pollution, and of monitoring data.
such design has other sustainability benefits such Folke et al. [116] discuss the relationship
as improved health from physical activity between adaptive capacity and sustainability.
[127]. Of course, designing for urban density To lay claim to sustainability, a society must be
will result in more instances of exposure to able to manage adaptively to socio-ecological
urban air pollution, providing additional incentive changes. This capacity, Folke et al. [116] argue,
to minimize emissions. requires mechanisms that allow governments to
The air pollution monitoring community can learn, meaning that the institutional capacity to
also contribute to improved urban form by uniting learn must be optimized. It is not optimized in
air pollution models with urban design models. the current situation as described by Chow and
Involving the air pollution monitoring community Watson [92], wherein data are primarily oriented
in an integrated design process for cities could toward fulfilling routine functions. Adaptive
lead to reductions in emissions and exposure in capacity also requires spaces for institutional
existing areas by designing new developments to collaboration [116]. Data that are conventionally
decrease the negative impacts of stagnant air less informative than they could be, as air pollu-
within urban canyons. A stronger air quality per- tion monitoring data commonly are [92], are not
spective on urban design could result in more optimally suited for collaborative purposes. The
sustainable places to live. case of the need for fine spatial resolution in the
MacKerron and Mourato [120] study of socio-
Acceleration of Learning and Research The economic distribution of air pollution is an
majority of investment in air pollution monitoring example where routine data would not have
is directed not toward research or improvement of served the study’s interdisciplinary purpose.
research capabilities but toward assessing compli- The capacity to adapt requires not only strong
ance with existing air pollution concentrations data, but the ability to extract maximum infor-
standards [92]. The focus on compliance to the mation from that data. Adaptive capacity, and
exclusion of other objectives reduces the value of therefore sustainability, would be served by the
data acquired in that the data could also be used improvements suggested by Chow and Watson
412 Air Pollution Monitoring and Sustainability

[92], and like improvements concerning the networks. Yi et al. [54] comment that sustainable
acceleration of learning. consumption and production will reduce air pol-
Chow and Watson [92] and Folke et al. [116] are lution, which suggests collaboration with busi-
effectively calling for continual improvement in ness. Agricultural practices are major sources of
capacity to learn on the job. In doing so, they are air pollution [74], suggesting collaboration oppor-
highlighting two essential components of sustain- tunities with the agricultural sector. Further, col-
ability: learning and continual improvement. Rou- laboration between air pollution and climate
tine monitoring must cease to focus solely on change mitigation efforts can deal with major air
compliance. It must ensure that research and pollutants that are also contributors to imbalanced
improvement in the capacity for research are served. radiative forcing [14, 74] while discouraging the
Clearly, development of best practices to ensure implementation of climate strategies that increase
sustainability needs to be a priority in this learning. air pollution [74]. Failing to collaborate will make
air pollution research more difficult and less
Expansion of Goals: Conclusion The conven- rewarding, while collaborating will open new
tional goals of air pollution monitoring influence areas that will inform monitoring priorities.
monitoring practice. Practices thus serve these
goals more than others. There is a need to expand Public Involvement Public involvement and
the set of goals and expand practices accordingly. consultation with the general public can be of sub-
Monitoring to understand impacts on natural cap- stantial benefit to science but are rarely taken advan-
ital is not only essential to sustainability but will tage of. At some levels, there is an aversion to such
improve the economic future of humanity. Resil- involvement as illustrated by a survey taken by the
ience is a concept the air pollution monitoring British Royal Society which showed that 20% of
community can study and apply further. The envi- scientists believed that those scientists seen to
ronmental injustice of air pollution’s distribution engage with the public were less well regarded by
must be addressed for the sake of justice and for their peers [128]. Much value is overlooked when
the health of younger populations. Given the air pollution scientists do not engage with commu-
strong links between air quality and urban form, nities they intend to monitor, including sophisti-
air pollution issues should not be ignored in the cated understanding of local sources of air
design of cities nor urban form ignored in pollu- pollution, how local air pollution changes with
tion studies. Acceleration of learning and research weather, and health effects being experienced
have the potential to increase the efficiency of (even if the sophistication of the knowledge is not
monitoring as well as improve understanding of of the same kind that air pollution scientists gener-
air pollution’s effects and optimal concentrations. ally regard as sophistication) [120]. Citizens often
All of these goals must be adopted if air pollution have or believe they have information that monitor-
monitoring is to holistically pursue sustainability, ing bodies do not have and, even if this information
and sustainability will continue to be elusive if is incorrect, it may affect the ability to implement
approaches are not holistic. policy based on results from air pollution monitor-
ing [129]. Thus, it is a good idea to at least under-
Multidisciplinary Work Attitudes fostering stand how a community feels about its local air
sustainable levels of air pollution in the coming pollution before policy, and possibly even monitor-
decades will value contributions from intellectual ing campaigns are designed. When communities do
disciplines other than air pollution science. Urban take air quality problems seriously, opportunities
planning work can mitigate exposure to air pollu- for progress on air quality issues arise [14].
tion, and it is clear that improved energy effi- Yearly [129] performed two case studies on air
ciency will reduce emissions from fossil fuels pollution and public involvement that illustrate the
[54, 74]. Folke et al. [116] call for consultations value of community input. The first was in Shef-
with communities with local ecological knowl- field, UK, where the local government had
edge [116] such as neighborhoods and Aboriginal implemented a computer model to study the local
Air Pollution Monitoring and Sustainability 413

air quality. Public consultation showed that the public. Sather et al. [131] shows that the public
pubic of Sheffield was not satisfied with the can be directly involved in research activities. The
model [129]. The public criticized the model on Sather et al. [131] study covered a large area
several points, and councilors and researchers felt (~25,000 km2 of the Dallas-Fort Worth
that the community’s and citizen’s groups’ com- Metroplex) and help from volunteers, including
ments were much more detailed, reasoned, and volunteer EPA personnel, 4-H club members,
well supported than expected [129]. Comments Master Gardeners, and retired farmers, was
were acknowledged by those running the model required. At each network site, volunteers were
as insightful and well founded [129]. Issues added able to correctly operate instruments and collect
to the agenda by the suggestion of the citizen’s data of quality. Such involvement is surely repli-
groups included an inquiry into the extent to cable in other settings, would increase the range
which the local council was affected by what the and cost-effectiveness of monitoring, and would
model presented, and consideration of the “value- have positive impacts on a community’s will to
for-money” associated with the modeling strategy reduce air pollution. In addition to sharing of
[129], as opposed to a pollution mitigation strategy. information, public involvement can result in sub-
The second case study was in Bristol, stantial, competent aid in air pollution monitoring.
UK. Community members were asked to use Widespread, hands-on public involvement would
markers to develop a color-coded map of Bristol be one aspect of a more effective effort to com-
that would reflect typical air pollution in the city. municate risks associated with air pollution to the
Not only was the resulting map a reasonable reflec- public, as called for in Craig et al. [14].
tion of actual air pollution in Bristol, there was
valuable information to be found in a comparison Institutional Changes: Conclusion In order to
of Bristol’s air pollution model and the community’s accelerate the progress of the air pollution moni-
map in areas where the two disagreed [129]. Both toring community toward sustainability, there are
studies were valuable and acted as a kind of extended changes the monitoring community must make.
peer review on the policy-related science [129]. Goals must be expanded beyond the conventional
Development of scientific material for public goals of human health, visibility, and documenta-
consumption forces scientists to develop under- tion of ecosystem damage. Work must cross the
standings of other fields, and does not remove boundaries of conventional intellectual disci-
rigor from the work but does demand skill plines to further develop the implications of mon-
[130]. Communication with the public is a sus- itoring data and the tools and metrics used in
tainability issue in that emissions reductions monitoring. Public involvement will improve
recommended by the results of monitoring are research goals in many cases, bring public support
easier to implement with an informed public to air pollution mitigation and, in some cases, aid
supporting policies they feel they helped create the research process itself. Making changes in
[130]. Alternatively, an ill-informed public these directions will help to promote sustainability
can pressure governments to adopt policy for in air pollution monitoring.
the wrong reasons, potentially leading to
unsustainable environmental impacts. O’Neill Monitoring More Effectively
et al. [117] recommends that research not only Changes that can be made to standard monitoring
be communicated to the public, but that air practice discussed here are based on current trends
pollution research should be developed in col- or suggested modifications to practices. They
laboration with the affected communities. include development of the understanding of
Only rarely when scientists are asked about multipollutant impacts, monitoring for universal
interaction with the public do they imagine any- consolidated sustainability metrics, improvements
thing other than a public lecture [130]. This mis- to the use of satellite observations (partially through
take is an extreme example of the idea that one new instrumentation), use of design methodologies
way communication is the only way to involve the for monitoring networks, and removing some of the
414 Air Pollution Monitoring and Sustainability

oversimplifications routinely made in conventional has been applied to rank countries in terms of the
monitoring. These changes can form initial steps state and treatment of their environment, and it
toward improving the air pollution monitoring can help countries define goals and track progress.
community’s contribution to sustainability. It was created in response to a feeling that the
environmental goals of the United Nations Mil-
Multipollutant Monitoring and Science Health lennium Development Goals were poorly defined
risks from air pollution are almost exclusively and that progress toward these goals was difficult
assessed on a single pollutant basis [100]. Health to quantify [131]. A remedy to these complaints is
risks from, for example, ozone, are assessed sep- exactly what consolidated metrics and monitoring
arately from health risks from NOx. In reality, designed with these metrics in mind can provide.
however, people are exposed to many pollutants How well the EPI can describe a country’s envi-
at one time. Pollutants can have synergistic effects ronmental status is limited by the data available
that exacerbate health impacts beyond the sum of [131]. The EPI can only incorporate data for
the health impacts they would have individually which there is already a strong history and tem-
[100]. Air pollution research and the US EPA are poral trend, making it difficult to represent
moving toward multipollutant research and legis- recently recognized sustainability issues. Never-
lation, but available data are inadequate to create theless, the EPI provides countries with an evalu-
legislative models [100]. To develop the required ation as to where they stand relative to their peers,
data, more and better monitoring, as well as a method for tracking progress, and a databased
improved exposure modeling and data processing framework to guide decision making.
are required [100]. The necessary changes will The discipline of life-cycle assessment (LCA)
take time; however, development in this direction contains many examples of consolidated metrics,
is required for accurate assessment of the health similar to the EPI. LCA method and metrics can
impacts of air pollution. be used in attempts to quantify sustainability
[132]. Eco- Indicator 99, for example, quantifies
Design for Consolidated Sustainability Metrics the impacts of activities and pollutant releases;
Environment Canada’s Air Quality Health Index translates these impacts into three metrics related
(AQHI) and the US EPA’s Air Quality Index to health, ecosystem damages, and depletion of
(AQI) are examples of consolidated metrics. resources; and combines these three metrics into a
They incorporate a number of data on different single indicator [133]. The weighting systems that
species of pollutants and atmospheric conditions allow LCA methods such as these to combine
and weight the importance of these data in the disparate data into a single number would encour-
calculation of a single summative statistic. These age the quantification of the relative impacts of
metrics are useful in that they can quickly com- various air pollutants. Were that accomplished,
municate a great deal of information in a form data on different pollutants, pollutants with very
more easily understood by the public than raw different behavior and effects, could be compared
air quality data [78]. Consolidated metrics can on the same scale.
also change behavior in ways that minimize the Designing air pollution monitoring and moni-
impacts of air pollution, as demonstrated by toring campaigns to serve consolidated sustain-
AQHI-informed decisions to limit personal ability metrics means not only providing data for
exposure [78]. metrics like the EPI and Eco-indicator 99, but also
The Environmental Performance Index (EPI) developing novel data sets to strengthen such
is an example of a consolidated metric that can be metrics. Novel data sets would make it possible
used in service of sustainability. The EPI is the a for such a metric to be influenced by sustainability
function of indicators such as urban particulates, issues for which sufficient data do not yet exist.
SOx and NOx emissions, water stress, habitat pro- Collecting data so that loss of resilience, for exam-
tection, pesticide regulation, agricultural water ple, could be incorporated into a metric like the
intensity, and GHG emission per capita [131]. It EPI would encourage nations to take action on
Air Pollution Monitoring and Sustainability 415

previously ignored sustainability issues and pro- management problems, making these estimates
vide governments with the information necessary particularly useful. van Donkelaar et al. [90] also
to do so. It must be borne in mind, however, that suggest that increased satellite coverage could
there are many pitfalls in the design of consoli- further improve the identification of temporal or
dated metrics [134], and only a correctly designed spatiotemporal trends. In contrast, other recent
metric will lead to sound decision making. attempts to estimate PM2.5 concentrations using
A standardized set of data for use with widely satellite-observed AOD with fine spatial resolu-
accepted consolidated metrics would clarify the tion determined that AOD is a poor tool for
design goals of monitoring campaigns, which is assessing spatial PM2.5 patterns [135],
important to the cost-efficiency of monitoring supporting previous suggestions that current sat-
[14]. Information derived would be more similar ellite spatial resolution is not sufficient for the
from campaign to campaign, allowing monitoring intra-urban scale [82]. AOD was also found to
groups to more easily share data. Further devel- contribute little additional information when
opment of consolidated metrics in the direction of incorporated into a predictive model that was
sustainability and the design of monitoring efforts already accounting for land use, emissions
to serve this development would allow the air sources, meteorology, and regional variability
pollution monitoring community to come to a [135]. Thus, the most effective role of satellite
consensus on the types of data to be counted in data is still being established, but this tool has
the metrics and the weighting of these data. the potential to become a valuable and routine
part of air pollution monitoring, providing data
Development of Satellite Observations Satellite where there otherwise may be few and improving
observations can be used in combination with data where routine rigorous monitoring is taking
models and in situ measurements to reduce statisti- place.
cal uncertainty in estimates [83]. Recent work by Martin [82] reviews the many recent improve-
van Donkelaar et al. [90] has made possible the ments in the application of satellite observations
reliable estimation of long-term average PM2.5 con- to assessments of air quality but includes a num-
centration based on satellite-derived data. Aerosol ber of limitations in obtaining accurate pollutant
Optical Depth (AOD) measurements made by the concentrations. Limitations included the need for
MODIS (Moderate Resolution Imaging Spectrora- more ground-level NO2 measurement to validate
diometer) and MISR (Multiangle Imaging Spec- satellite-observed NO2 data and difficulty in
trometer) instruments on the Terra satellite were obtaining high-quality O3 concentration esti-
combined with estimates of aerosol distribution mates. Martin’s work asserts that in terms of
from the Goddard Earth Observing System chemi- instrumentation, air quality monitoring via the
cal transport model (GEOS-chem). Previously, var- current satellites is at a peak but that substantial
iations in meteorology, aerosol composition, and progress could be made with a new generation of
distribution have prevented accurate estimates by instruments, with more satellites in a variety of
satellite observation beyond small regions, but orbits (as opposed to all satellites being in sun-
with the GEOS-Chem model, reliable estimates synchronous orbit as is currently the case). Spe-
were obtained across all midlatitude areas of the cific instrument improvements include a minimi-
globe. The concentration estimates with 10 km2 zation of pixel size, which will reduce the number
spatial resolution were obtained. of pixels obscured by clouds. Work that can be
Many epidemiological studies of PM2.5 expo- accomplished without additional satellites and a
sure are limited by a dearth of monitoring data, new generation of instrumentation includes the
and the improved satellite estimates from the van improvement of models critical to the interpreta-
Donkelaar et al. 2010 work [90], can now provide tion of satellite observations. Better estimations
some of these needed data [90]. The lack of data is from these models will improve information
more pronounced in developing countries, and derived [82]. If the suggested developments can
these countries often have pronounced PM2.5 be made, satellite observations will move closer to
416 Air Pollution Monitoring and Sustainability

delivering spatial and temporal data on a scale that rigorous design principles have been effective in
better relates to ground-level monitoring. that they led to the first generations of information
and significant discoveries relating to air pollution
(and thereby led much of the effective legislation
Design Methodologies for Monitoring on air pollution). Further, these campaigns pro-
Networks vided information that is necessary for the imple-
All monitoring techniques, from measurement of mentation of some of the newer design
ambient pollution levels to computer modeling, methodologies such as the location-allocation
rely on some assumptions and estimates in the methodology, and they have brought the state of
assessment of pollutant concentrations, exposure air pollution science to the point where monitor-
to pollution, risk, and damages from pollution. ing system design methodologies can be created.
Sophisticated design methodologies for monitor- However, now that design methodologies have
ing networks and campaigns have been developed been established, their routine employment can
to ensure that the uncertainties are minimized. improve the information content of monitoring
These methodologies help to ensure that the data and the cost-effectiveness of monitoring
most useful information can be extracted from efforts.
what are often limited data.
Established design methodologies include Overcoming Oversimplifications in
kriging, the use of indices of multivariate effec- Monitoring
tiveness [136], and the location-allocation method Often, the practicalities of air pollution monitor-
[137]. Each method requires an established area to ing necessitate compromises in aspects such as
be monitored and attempts to optimally cover that increased time resolution, assumptions about pop-
area with a given number of monitoring stations. ulation behavior, and assumptions of relative uni-
Kriging involves placing monitoring stations such formity over areas. As methods become more
that mean square prediction error is minimized sophisticated, some of these assumptions can be
[137]. The method employing indices of multivar- eliminated.
iate effectiveness is based on Shannon’s [138] Conventional studies usually assume that the
information theory, as used by Silva and Quiroz basis of exposure to air pollution is the concentra-
[136] which tests various configurations of mon- tion in a given location, often outdoors. However,
itors to optimize the information content of data people move through various exposure situations
collected. The location-allocation method begins in their daily lives, from indoors to “hotspot”
with the creation of a “demand surface,” a surface intersections and through areas of differing land
representing the area to be studied, with higher use. A dynamic activity-based population model
demand areas represented by peaks in the surface. has been suggested to develop a more realistic
Values on the demand surface are increased by sense of actual individual exposure [139]. Use of
variability in pollution concentrations and by this model captures exposure resulting from peo-
proximity to sensitive populations [137]. To ple’s travel in and out of urban areas, rather than
inform the demand surface, an initial pollution assuming a constant number of people within
surface (representing the distribution of pollution cities, as has been the case in conventional studies
over an area) must exist based on previous or [139]. Beckx et al. [139] use of this model showed
ongoing monitoring. Once the demand surface is that conventional static modeling of exposure is
finalized, monitoring stations can be placed at the underestimating population exposure to air
highest demand locations in the area. pollution.
Design methodologies for monitoring net- Some very small areas in cities, such as high
works and sampling campaigns are a relatively traffic intersections, can have much higher pollu-
new development, with many previous networks tion concentrations than the bulk concentrations
and campaigns set up in a subjective manner. in the wider area being monitored through con-
However, past campaigns and networks lacking ventional means. Gokhale and Khare [140]
Air Pollution Monitoring and Sustainability 417

discuss a model for determining the likelihood of complementarity may be one of the most convinc-
air pollution concentration exceedances over ing arguments that these goals actually will pro-
norms at intersections and other areas, where mote sustainability. While sustainability is
exceedances are likely. The model provides the difficult to define, it must connote that solutions
opportunity to probabilistically manage air pollu- to one problem do not exacerbate other problems,
tion on a very fine spatial scale by designing for a but contribute to other solutions.
minimization of exceedances. Models such as Holism, then, must be an aspect of sustainabil-
those of Beckx et al. [139], Burke et al. [141] ity, and the lack of holism in the current air pollu-
and Gokhale and Khare [140] can provide means tion monitoring community may underlie its
for addressing some of the simplifying assump- current shortcomings. Not only is there a need
tions in air pollution monitoring. Since their for more holistic viewpoints encompassing ideas
approaches primarily involve modeling, they from other intellectual disciplines, but there is a
need not increase the cost of air pollution man- need for air pollution mitigation to go beyond
agement excessively. promoting primarily technology-based solutions
to only the immediate impacts. Solutions offered
Monitoring More Effectively: Conclusion today do not address all aspects of the air pollution
There are a number of changes to air pollution problem.
monitoring suggested in the literature and, in To a very large extent, the lack of holism is not
many cases, already under way. These changes, a function of a failing of the air pollution moni-
the development of multipollutant science, moni- toring community, but a result of that community
toring for consolidated metrics, improvements to having strategically chosen battles in the past.
satellite-based monitoring, using monitoring net- Dockery [44] shows how hard advocates of air
work design methodologies, and dealing with pollution mitigation were forced to struggle for
routine oversimplifications will improve the oper- any political action on air pollution in the early
ation of the monitoring community and the quality days of air pollution science, and how the battles
of results. Information, as a common first step were won by presenting irrefutable, solely techni-
toward sustainability and a necessary support for cal and solely scientific evidence proving the very
sustainability policy, will help the air pollution immediate and anthropocentric effects of air pol-
community serve sustainability. Hopefully, these lution. It is only now that less obvious, though
changes will be only the first set of changes in a arguably more dire, effects on humans, the sys-
more fundamental shift toward sustainability. tems they rely on for sustenance, and on non-
human stakeholders are gaining more than a
slight foothold within the political agenda.
Conclusion Dockery [44] also shows the great extent to
which the burden of proof was on those trying to
Air pollution is often seen as a negative but defend people and ecosystems from the damages
unavoidable consequence of human activity. of pollution, and not on the polluters. This burden
While air pollutants are well classified and there is still in place, and problems must be proven in
are a number of commonly recognized problems terms polluters cannot ignore, such as dollar fig-
they create, including negative impacts on human ures and mortality. To a large extent, evidence will
health, environmental damage, and economic need to continue to be in these terms, and moni-
losses, the establishments designed to mitigate toring must be expanded in volume, scope, and
these problems often have a mandate to also pur- abilities to continue to prove the damages from air
sue sustainability. pollution in the normally accepted terms. How-
The recommendations made herein regarding ever, the body of evidence will be more compel-
a shift toward sustainability are largely com- ling and complete if the terms are expanded to
plimentary. Pursuing one of the goals described include goals discussed in this chapter. The terms
would serve other sustainability goals. That have been set as a reaction to refusals of those
418 Air Pollution Monitoring and Sustainability

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band. This gap is called the bandgap. Electrons
Low-Cost Sensors for Indoor and may be thermally excited from the fully occupied
Outdoor Pollution band into the unoccupied band, resulting in lim-
ited conductivity; the solid is then a semiconduc-
Louise Bøge Frederickson1,2, tor. A solid with a large bandgap is an insulator
Emma Amalie Petersen-Sonn1, Yuwei Shen1, and with no bandgap, a conductor. The top of the
Ole Hertel3, Youwei Hong4, Johan Schmidt2 and occupied states is called the Fermi level [1].
Matthew Stanley Johnson1,2 Dynamic range The range of performance of a
1
Department of Chemistry, University of sensor: the analyte concentration range
Copenhagen, Copenhagen, Denmark between the highest observable concentration
2
Airlabs, Copenhagen, Denmark and the detection limit [2].
3
Department of Environmental Science, Aarhus Explosion range and limits The explosion
University, Roskilde, Denmark range specifies the concentration range of a
4
Institute of Urban Environment, Chinese species in air, over which a given compound
Academy of Science, Xiamen, China can burn or explode. This range extends from
the lower to the upper explosive limit and is
often given in % v/v. The lower limit is defined
Article Outline as the lowest concentration where a vapor or
gas will burn or explode, whereas the upper
Glossary limit is the highest concentration at which the
Definition gas or vapor will burn or explode [3, 4].
Introduction Exposure limit The specified threshold of peak
MOx Sensors concentration, or average concentration for a
Optical Sensors certain period, for a hazardous substance, that a
Electrochemical Cells person can be safely exposed to without endan-
Electrochemical Cells and Metal Oxide Sensors gering health. The exposure limit assures
Comparison Between MOx, Electrochemical, and workers’ occupational health and is often
Optical Sensors expressed as an 8 hour time-weighted average
Personal Exposure Monitoring and Installations concentration [3–5].
in the Field MOF Metal-organic frameworks (MOFs) are
Calibration crystalline compounds consisting of metal
The Future: Smart Cities and New Materials ions or metal clusters, which are linked by
Conclusion organic ligands in a regular pattern to form
Bibliography 3D structures with pores [6].
Nanowire A nanowire is a highly conducting
Glossary nanostructure with a diameter in nanometers
[7, 8].
Band gap A solid will have a density of electronic Resolution Resolution can be used in several
states as a function of energy. For example, a senses. First, the temporal resolution of a sen-
certain solid may have a band of fully occupied sor is not the data sampling rate but rather the
states, a gap or energy range in which there are minimum time for a meaningful measurement,
no states, and at higher energies, an unoccupied whether defined by the response time or the
averaging time to get a reasonable signal to
Louise Bøge Frederickson and Emma Amalie Petersen- noise. Spatial resolution refers to the density
Sonn contributed equally. of measurement sites. Measurement resolution
© Springer Science+Business Media, LLC, part of Springer Nature 2021 423
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_1084
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2019, https://doi.org/10.1007/978-1-4939-2493-6_1084-1
424 Low-Cost Sensors for Indoor and Outdoor Pollution

is defined as the lowest concentration differ- limit to the performance of semiconductors and
ence that can be distinguished by a sensor [2]. sensors as there is only a certain concentration
Response time The characteristic time it takes of holes or free electrons that can be pressed
for a sensor to respond to a perturbation [2]. into a certain volume without paying an unac-
Semiconductor A semiconductor is a crystalline ceptable energy penalty [11].
or amorphous substance with a fully occupied
valence band and an empty conduction band,
and an electrical conductivity that increases Definition
with increasing temperature [1]. Semiconduc-
tors have a band gap between the valence and Low-cost sensors for monitoring indoor and out-
conduction bands that can be overcome by door air pollution have been developed and are
thermal excitation. There are two types of available commercially. This entry describes the
semiconductors: intrinsic and extrinsic. An function and performance of the most common
intrinsic semiconductor has a naturally small low-cost sensor technologies. Target pollutants
band gap. When an electron is excited into the include particulate matter (PM), CO2, NO2, O3,
conduction band a hole is left in the valence CO, VOC, SO2, and N2O. Three different types of
band; the electron and hole are mobile and low-cost sensors are considered: Metal oxide
conduct current. In contrast, an extrinsic semi- (MOx) sensors, optical sensors, and electrochem-
conductor is not semiconducting in its pure ical cells. The basic principles, fields of applica-
state but becomes semiconducting through tion, and performance of the sensor types are
the addition of impurities (“dopants”) with ele- detailed in order to contrast and compare them.
ments that may have a deficit or excess of The devices are compared on the basis of param-
electrons relative to the main compound. eters such as sensitivity, selectivity, stability, cost,
There are thus two types of extrinsic semicon- power consumption, and life cycle. Examples of
ductors, p-type (positive charge doped) and installations in the field and for personal exposure
n-type (negative charge doped). For example, monitoring are described. Finally, we consider
a P atom (group V) in a Si crystal (group VI) future developments in the areas of smart cities
has an extra electron that can enter the Si con- and new materials such as nanowires and MOFs.
duction band making a n-type extrinsic semi-
conductor; an Al dopant (Group III) would
yield a p-type. Semiconductors are used as Introduction
gas sensors because oxidizing or reducing
gases change the population of the conduction In the beginning of the nineteenth century, many
band, changing the conductivity. Reducing technologies we have today were not available. At
gases (e.g., NH3, CO, H2) lead to an increase that time, canary birds (Fig. 1) were commonly
in conductivity for n-type and a decrease for used in coal mines to sense when the concentra-
p-type, and the reverse for oxidizing gases tions of toxic gases in the air had reached a haz-
(e.g., NO2, O3, Cl2) [9]. ardous level. Canaries are well-known to be more
Sensor A sensor is a device that transforms sensitive to dangerous gases than humans. The
chemical information into an analytically use- canary birds are especially good at sensing carbon
ful signal [10]. monoxide (CO), which is colorless and odorless,
Sensor Node A sensor node is an instrument that and if a bird died, the miners knew they should
may contain several sensors, a control and data evacuate from the mine immediately. The birds
processing system, and power management. became an integrated part of mining culture, and
Space charge A high density of like charges has some were treated like pets. In some cases, mice
a high space charge; Coulombic repulsion were used to indicate the presence of harmful
limits the ultimate charge density in a given gases. These animals most likely saved the lives
space. The charge density poses a fundamental of many miners [12].
Low-Cost Sensors for Indoor and Outdoor Pollution 425

As sensors become smaller, more accurate, and


cheaper, they are finding use in an increasing
number of applications, beyond the traditional
areas of mining and industry. Low-cost sensors
are unlikely to replace conventional instruments
for accurate measurements of well-mixed gases in
the atmosphere such as CO2 (with the exception of
variable CO2 levels in buildings) but could be
particularly useful for measurements of short-
lived pollutants with sources inside cities, such
as NO2, PM, and O3. In addition to poor time
resolution, current pollution monitoring networks
are expensive (maintenance, staff, instrument
cost, and space), and cities have too few monitor-
ing sites to create an accurate map of a city.
A detailed time-dependent pollution map would
be extremely useful in pollution control efforts, to
pinpoint sources and exposure hot spots and help
Low-Cost Sensors for Indoor and Outdoor Pollution, evaluate remediation strategies. For instance, in
Fig. 1 A typical canary bird urban areas in the USA, there are only ~2–5
sensors per 1000 km2 or per one million people
[13]. A network containing low-cost sensor nodes
Today, we have inexpensive sensors to detect could have orders of magnitude more sites with
gases and particles in indoor and outdoor environ- greatly improved time resolution, and so provide a
ments. For example, some models of cars now pollution map with far higher temporal and spatial
come equipped with low-cost sensors in the ven- resolution. This map could be combined with a
tilation system to detect pollutant levels in the map of population density to visualize pollution
incoming air. This information is useful for con- exposure throughout the day. Such a sensor net-
trolling the ventilation system and reducing expo- work could thereby be a great improvement on
sure when the vehicle is driving on polluted streets today’s measurements and estimates of pollution
in tight traffic. When high pollutant levels are exposure. Anchoring this network to reference
detected, the car shifts to recirculation, reducing sensors would also aid in calibration and improve
pollution exposure for the driver and passengers. accuracy. Accurate, widespread, low-cost sensor
Low-cost sensors are becoming more specific, networks are just starting to become a reality and
accurate, and useful, and with their increasing there is massive potential for their widespread use
utility in new applications, the demand for effec- [14, 15].
tive low-cost sensors is increasing [12]. Low-cost sensors promise to be a vital tool for
The development of a new generation of small, monitoring both the personal exposure of individ-
portable, low-cost sensors and sensor nodes has uals and the pollution observed at specific loca-
been rapid in recent years, although they are typ- tions. These locations could be emissions sources
ically less accurate than conventional instruments. (livestock barns, construction sites, factories,
However, high precision is not always important, pipelines, etc.) or along trafficked routes
as in the example of ventilation in cars where the (highways, shipping lanes, etc.), or polluted
sensor only needs to detect whether pollution areas (ports and industrial parks, neighborhoods,
levels are high or low. There is also a value in etc.) Previously, passive sampling methods have
the speed and density of monitoring promised by been used with some success for personal expo-
low-cost sensors, potentially providing high tem- sure measurements, but this approach signifi-
poral and spatial resolution, respectively. cantly lowers the temporal resolution of the data
426 Low-Cost Sensors for Indoor and Outdoor Pollution

recorded [16]. Accurate, wearable sensors have The Three ‘S’s: Sensitivity, Stability, and
the potential to give much higher quality data in Selectivity
this respect. Increased temporal and spatial reso- The sensitivity of a gas sensor is defined as the
lution mean specific exposure modes (e.g., change of measured signal per change of analyte
“morning commute”) can be distinguished. The concentration. Sensitivity is sometimes confused
advent of low-cost sensor technologies also with the limit of detection, which is the lower limit
means that new applications can be developed. of analyte concentration the sensor can detect under
These could be in areas such as adding sensors certain defined conditions [38]. The stability is the
to drones for remote sensing campaigns, and the ability to produce consistent results over a defined
production of “smart” billboards that can measure period or change in conditions, for example, temper-
and display pollution levels, increasing awareness ature or humidity. (A related metric is the recovery
for citizens [17–19]. time, the time the sensor signal uses to return to its
The United Nations (UN) has defined its vision initial value after a perturbation [2].) A further dis-
for the future in the Sustainable Development tinction is made between “active” and “conservative”
Goals [20]. The 11th goal is “Sustainable Cities stability. Active stability depends on the sensor’s
and Communities.” Low-cost sensors can help cre- ability to give reproducible results during operation
ate more sustainable environments by providing under variable conditions. Conservative stability
information that can promote sustainable govern- describes the ability of the sensor to retain its sensi-
ment policies and healthy individual behaviors in tivity and selectivity after storage [38]. The final “S,”
daily life. Government policies could include emis- selectivity, is based on whether the sensor responds
sions controls on vehicles and factories, planting to a group of analytes or a specific species [38].
green zones, choosing energy infrastructure, and We will use the example of metal oxide gas
changing traffic patterns. Individuals could choose sensors to illustrate sensitivity, selectivity, and sta-
to ride a bicycle instead of driving car, insulate their bility. These sensors typically contain a sensitive
homes, drive low emissions vehicles, and avoid layer, a substrate, electrodes, and a heater. Transduc-
candles and wood stoves. Low-cost sensors can tion of the chemical signal to an electronic signal
contribute by being used to detect wildfires, gas occurs by the following process. In granular metal
leaks, and other public safety events, giving an oxides, Schottky barriers (an electrostatic depletion
early warning to authorities and helping to locate layer formed at the junction) form at grain bound-
the source of the event. Sustainable Development aries as a result of the depletion layer [38]. The
Goal number 13 is “Climate Action” and point depletion layer is a region created when n-type and
13.2 says that society needs to “Integrate climate p-type materials are placed in contact. The concen-
change measures into national policies, strategies tration of current carriers is reduced in this region,
and planning.” By supplying leaders and citizens and their electrical conductivity becomes very sen-
with information about air quality, sensors are a sitive to minor perturbations, for example, the pres-
powerful tool for identifying the problem that ence of an electron donor (Lewis base) or electron
needs to be solved, for example, by characterizing withdrawing (Lewis acid) species adsorbed on the
fugitive emissions, and documenting that solution. surface [10], or space-charge effects [11]. The
The data provided can be implemented in political Schottky barrier height describes the resistance to
goals and strategies [20]. electron transport across the interface [39].
Humans are adversely affected by exposure to For example, suppose that molecular oxygen
air pollution, resulting in exposure limits and leg- adsorbs on the surface. By doing so, it traps an
islation for specific pollutants. Exposure limits electron, changing the concentration of current
take different forms, for example, peak exposure, carriers in the depletion region. At higher temper-
or average exposure over an 8 hour period or a atures, between 100  C and 500  C, ionized
year. Specific examples of uses for low-cost sen- molecular oxygen and atomic oxygen are present
sors with individual pollutants and their main at the surface, with unique effects on the depletion
effects are detailed in Tables 1 and 2. region.
Low-Cost Sensors for Indoor and Outdoor Pollution 427

Low-Cost Sensors for Indoor and Outdoor Pollution, Table 1 Pollutants with their exposure limit and explosion
limit in % v/v
Pollutant Exposure limit Explosion limit (% v/v) Reference
PM2.5 1 year 25 mg/m3 ECa
PM10 24 h 50 mg/m3 ECa
1 year 40 mg/m3
SO2 1h 134 ppb ECa
24 h 48 ppb
NO2 1h 106 ppb ECa
1 year 21 ppb
CO 8h 0.0087 ppb 12.5–74 [21] ECa
O3 8h 61 ppb ECa
H2S 8h 5 ppm 4.3–4.6 [4] ECb
CO2 24 h 1000 ppmc BR d
CH4 8h 1000 ppm 4.5–15 [4] NIOSHe
N2O 8h 25 ppm NIOSHe
As 1 year 0.002 ppb ECa
Cd 1 year 0.001 ppb ECa
Ni 1 year 0.008 ppb ECa
Pb 1 year 5 ppb ECa
Formaldehyde, CH2O 8h 40 ppb 7.0–73 [4] WHOb
1h 100 ppb
Toluene, C7H8 24 h 0.6 ppm WHOb
8h 4.0 ppm
Naphthalene, C10H8 24 h 1.9 ppb WHOb
Benzene, C6H6 1 year 1.6 ppb ECa
a
European Commision [22, 23]
b
World Health Organization [24, 108]
c
Note that CO2 itself is not hazardous at these levels, but rather it is used as an indicator of poor ventilation
d
Bygningsreglementet, the Danish Building Code, Denmark [25]
e
The National Institute for Occupational Safety and Health, USA [21]

The conductance is limited by the Schottky selectivity of the sensors [38]. Stability is an issue
barrier for large crystallites, where the grain size for metal oxide sensors, and this leads to uncertain
is D >> 2L. Here, L is the thickness of the deple- results and false alarms, and these sensors often
tion layer. When the crystallites are larger than 2L, need to be recalibrated or replaced frequently. The
the sensitivity is basically independent of D. When stability can be somewhat increased by calcination
the grains become smaller, gas sensitivity becomes and annealing [38].
size-dependent. Experiments show that nanostruc- It is important to consider the minimum detect-
tured metal oxides have a large increase in sensi- able signal, which depends on the signal-to-noise
tivity when the grain size is reduced to a few ratio (S/N). To describe the optimization of signal-
nanometers. Sensitivity can also be changed by to-noise ratio, a system consisting of an amplifier
adjusting the microstructure and porosity. Several A0 is considered, see Fig. 2. The amplifier has
metal oxides show an increase in gas sensitivity voltage and current noise terms which are inde-
with porosity. Another strategy is to dope the sur- pendent of each other; where nn and in represent
face. By distributing a low concentration of a com- the rms voltage and current noise per Hz½.
pound like Pd, Pt, or Au, the sensitivity can be The signal-to-noise ratio can be expressed as
considerably improved. Furthermore, doping the the signal, ns, divided by the total output voltage
surface with metal nanoparticles influences the [40]
428 Low-Cost Sensors for Indoor and Outdoor Pollution

Low-Cost Sensors for Indoor and Outdoor Pollution, Table 2 Pollutants and their sources with their applications
and main effects
Pollutant Sources [26] Low-cost sensor applications Main effects [24]
CO2 Respiration Elevated indoor concentrations in offices Health: Drowsiness, headache,
Fossil fuel and schools [27] sleepiness, loss of concentration and
combustion Firefighter personal exposure [28] attention, increased heart rate and
Industrial tremor
processes Indicator for indoor air quality
Transportation Climate
Deforestation
Degradation of
soils
Land clearing for
agriculture
NO2 Intrusion of City pollution mapping, personal Climate: Acid rain, tropospheric
stratospheric exposure for professional drivers [29, 30] chemistry
nitrogen oxides Health: Asthma, eye irritation, allergic
Bacterial and responses
volcanic action
Lightning
Fossil fuel
combustion
Biomass and
biofuel
combustion
O3 Photolysis on City pollution map, personal exposure Tropospheric chemistry
NOx and VOCs [29–31] Health: Eye irritation, exacerbates
respiratory conditions
PM, Power plant City pollution map, personal exposure for Climate: Acid rain, changing the
PM10, Industrial cyclists [29–31] nutrient balance, depleting the nutrients
PM2.5 processes in soil, affecting the diversity of
Vehicular traffic ecosystems, damaging forests and farm
Domestic coal crops
burning Heath: Nonfatal heart attacks, irregular
Industrial and heartbeat, asthma, decreased lung
municipal waste function, irritation of the airways
incinerators
Volcanoes
Dust storms
CO Incomplete Indoor use, personal occupational Climate change
combustion of exposure [28, 32] Health: Dizziness, confusion,
carbonaceous unconsciousness and death
engines
Industrial
processes
Power plants
using coal
Waste
incinerators
Oxidation of
hydrocarbons
Plants
Oceans
(continued)
Low-Cost Sensors for Indoor and Outdoor Pollution 429

Low-Cost Sensors for Indoor and Outdoor Pollution, Table 2 (continued)


Pollutant Sources [26] Low-cost sensor applications Main effects [24]
VOC Agriculture City pollution map, personal occupational Climate change
Woodlands exposure, e.g., painters, traffic police, Health: Nose, eye, and throat irritation,
Volatile parking attendants [33]. Shipping loss of coordination, headaches, damage
consumer container and new building monitoring to kidney, liver, and central nervous
products [34] system, cancer
General solvent
use
Transportation
Printing/surface
coating
Industrial
Residential
SO2 Combustion of Monitor ports and shipping routes, Climate change, acid rain
sulfur- monitor volcanoes [35] Health: Irritates the skin and membranes
containing fossil of the nose, eyes, and lungs
fuels
Volcanoes
N2O Agriculture Agricultural emission monitoring [36, 37] Climate change
Fossil fuels Health: Vomiting, headache, increased
combustion sleepiness, and excessive sweating or
Industrial shivering
processes
Biomass burning
Atmospheric
deposition
Human sewage

Low-Cost Sensors for


Indoor and Outdoor
Pollution, Fig. 2
Amplifier and signal source
ns with noise sources nn and
in [40]

ns quickly information can be transmitted over a


S=N ¼ qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffipffiffiffiffiffiffi
4kT Rs þ n2n þ ðin Rs Þ2 Df communication channel in bits per second, and
is expressed as [42]
where k is Boltzmann’s constant, T is absolute
C ¼ B log2 ð1 þ S=N Þ
temperature, Rs is output impedance, and Df is
the frequency bandwidth in Hz. This formula
clearly shows that the signal-to-noise ratio can B is the bandwidth of the channel in Hz.
be improved by reducing T, Rs, and Df. There are several methods for modeling sen-
The Shannon-Hartley theorem [41] defines the sors’ noise, but the simplest technique is the Allan
channel capacity, C, which is a measure of how Variance method which was proposed in 1966 by
430 Low-Cost Sensors for Indoor and Outdoor Pollution

Low-Cost Sensors for


Indoor and Outdoor
Pollution, Fig. 3 Sample
plot of Allan variance
analysis results [43]

σ(τ)
Qu p
m
an ra
t. e
no rat
ise ift
Dr
Ang te
ran
dom le Ra walk
wal o m
k Bias instability rand

David Allan. The method was initially a variance


analysis method for the study of the stability of
oscillators and atomic clocks; however, due to
their functional similarity to sensors, the method
has been adapted to characterize random drift for a
variety of devices [40]. The Allan Variance pre-
sents the root mean square (RMS) random drift
error as a function of averaging time [40], which
means it helps to identify error sources and their
contribution to the overall noise statistics in sen-
sor data. There are five basic noise terms, which
are angle random walk, rate random walk, drift
rate ramp, bias instability, and quantization noise,
see Fig. 3 [44]. Mathematically, the Allan vari-
ance is defined as [43]

Low-Cost Sensors for Indoor and Outdoor Pollution,


1 D 2 E Fig. 4 Allan variance analysis for an NDIR (K30) CO2
1
s2O ðtÞ ¼ ðOkþ1  Ok Þ2 ¼ Okþ1  Ok sensor in study [45]
2 2

To check the data sampling rate effect, differ-


which is related to the power spectral density ent rate data sets should be collected for the sys-
(PSD) of the intrinsic random processes, SO(f), tem. It is also important to be aware of potential
by [43] cross-sensitive compounds when interpreting
Z data. Cross-sensitivity is when the sensor
1
sin4 ðpf tÞ responds to gases other than the target gas
s2O ðtÞ ¼ 4 SOð f Þ df
0 ðpf tÞ2 [40]. An example of a real-life Allan deviation
analysis (the square root of the variance) is
shown in Fig. 4, where a non-dispersive infrared
Since PSD amplitudes depend on the resolu- (NDIR) CO2 sensor (model K30) is introduced to
tion bandwidth, a function of sampling rate, the air from a high-pressure cylinder of a constant
sampling rate affects the Allan variance results. CO2 concentration with averaging times between
A typical theoretical Allan variance plot is shown 10 s and 1000 s. According to this analysis, the
in Fig. 3. Quantization noise is the most important optimum averaging time, when the Allan variance
source of variance over short time scales and drift is at a minimum, is approximately 3 min; longer
is most important at long time scales, etc. averaging times do not reduce the noise [45, 109].
Low-Cost Sensors for Indoor and Outdoor Pollution 431

Factors Affecting Sensitivity and Stability of gas sensors as for when pre-concentrators are
Depending on the point of measurements, meteo- used. These may take the form of metal-organic
rological factors such as wind speed, pressure, framework (MOF) based filters that can reversibly
humidity, and temperature will affect the sensitivity adsorb the target gas over a period of time, before
of a sensor, more precisely the baseline and sensor releasing it as a concentrated burst when heated,
gain. This can be corrected quite precisely using enabling the sensor to effectively operate at lower
generic data from the manufacturer describing how limits of detection and with increased sensitivity
the temperature, humidity, etc. affect the sensor [49]. As mentioned above, however, there is often
signal. For low-cost sensors, such calibrations can a trade-off; one sensor parameter is improved at
be more complex as these kinds of sensors are the cost of another. Pre-concentration is an exam-
often used in mobile applications. Given that the ple of improving sensitivity at the cost of a lower
aim is to monitor ambient air concentrations, a low- sampling rate. Depending on the application, this
cost sensor must be able to operate in both cold and approach is still valuable since loss of perfor-
hot weather posing a challenge for manufacturers mance may not necessarily be detrimental. For
of these sensors. Many applications therefore instance, low selectivity is not an issue for sensors
require continuous calibration, since a given cali- in highly controlled industrial environments, but a
bration may only work for one location, for a high sampling rate may be key for safety, whereas
limited time [46]. Some low-cost sensors must be for atmospheric measurements of well-mixed
re-calibrated every month or even every week. This gases, temporal resolution is a lower priority and
is also due to their low stability leading to sensor the need for sensitivity is high.
aging [47]. As mentioned above, metal oxide sensor
Especially when ppb sensitivity is needed and response can degrade over time, for instance,
for conditions with large temperature variations, a due to poisoning of the metal oxide or physical
better correction than what the manufacturer degradation causing a drift in the signal [50, 51]. If
offers may be required. Such a situation can be a trained personnel are needed to frequently
challenge for low-cost sensors, as data processing recalibrate sensors, then they are no longer a
may be highly resource demanding. If not done low-cost option. However, the loss of stability
correctly, monitoring the other variables and may in some cases be compensated by including
correcting onboard can create a large uncertainty. a high efficiency filter in the sensor system. If the
The calibration procedure may cause false results, sample flow is periodically passed through a filter,
also as many low-cost sensors are made by which removes the target gas, then the zero offset
smaller companies where the sensors are not reg- can be reset, and the sensor effectively
ulated properly [48]. Many users find that manu- recalibrated. Automatic calibration, without the
facturer calibrations will never be sufficient for need for trained operators, is one key to low-cost
ambient air measurements, since there is a sub- sensors becoming viable as an accurate, cost-
stantial difference between laboratory measure- effective source of data.
ments and ambient air measurements with To improve the selectivity of metal oxide sen-
interference from other gasses. sors, an array of sensor nodes can be operated in
combination. As described, metal oxide sensors
Improvements to S.S.S operate by measuring the change in resistance of a
Sensitivity, stability, and selectivity are the key metal oxide semiconductor when free-electrons
parameters for sensor performance and for low- are removed by oxidizing gases. This means that
cost sensors to become more prevalent, improve- oxidizing gasses like O3 and NO2 can be difficult
ments must be made in these areas. to distinguish. If a filter that selectively removes
For instance, when metal oxide sensors are one of these gases is included in the sample
used for gas measurements, filter materials can stream, then the sensor node’s response to indi-
be incorporated into the sensors in a number of vidual pollutants may be distinguished [52]. Alter-
ways. This may be done to improve the sensitivity natively, metal oxide sensors synthesized with
432 Low-Cost Sensors for Indoor and Outdoor Pollution

different metals can be included in an array, each Electronic Structure


will react differently to individual pollutants, A wide variety of electronic structures can be
increasing the dimensions of the signal response. found in metal oxide semiconductors. The struc-
tures can be divided into two main categories:
transition metal oxides and non-transition metal
oxides. The latter can be subcategorized into the
MOx Sensors pre-transition metal oxides and post-transition
metal oxides. The non-transition metal oxides
Metal oxide-based sensor nodes have many have a common s- and p- symmetry in the valence
advantages: low cost of fabrication, a simple orbitals, and for the transition metal oxides, the d-
structure, inertness and stability, robustness in orbitals play an important role. Usually the energy
their applications, and an ability to adapt to a difference between a cation dn and a dn + 1 or dn-1
great variety of gases. However, there are still a configuration is small, and so the transition metal
number of basic problems that need to be solved. oxides often have several stable compositions and
Metal oxide semiconductors have for many electron configurations. This can result in a high
years been based on SnO2. In more recent studies, defect concentration, which leads the transition
other metal oxides have been examined closely metal oxides to have a very complicated bulk
for their properties as gas-sensing materials. The and surface chemistry.
detection process hinges on the change in oxygen Transition metal oxides used in gas sensors
concentration at the surface, which is generated have d0 or d10 configurations. Post-transition
from adsorption and heterogeneous catalytic reac- metal oxides have cations with filled d10 configu-
tions of both oxidizing and reducing species from rations. The most common are ZnO and SnO2.
the gas phase. The conductivity of the semicon- Transition metal oxides, such as TiO2, V2O5, and
ductor depends on the species in the atmosphere WO3, have a d0 configuration [54].
and on the temperature of the sensing element.
The signal that is produced is strongly dependent
on the temperature. Most sensors have a heater Sensing Mechanism
attached beneath the sensor which can be used to The function of the sensors is based on the shift in
heat and thereby regenerate the sensor. Usually, equilibrium that takes place when oxygen is
regeneration is affected at temperatures 50  C chemisorbed on the surface, due to a presence of
higher than the highest temperature for operating a target gas. When oxidizing gases encounter the
the sensing device [53]. sensor, the gas species acts as an electron accep-
The metal oxide semiconductors that have the tor, which results in a resistance increase in n-type
highest sensitivities to molecules adsorbed on semiconductors and a resistance decrease in
their surface, and similarly, to gas phase concen- p-type semiconductors. There are two main
trations, are the materials with predominantly models use to explain how metal oxide detectors
ionic bonding (CdS, ZnS, etc.), although these function. The first is ionosorption and considers
semiconductors usually have low chemical and space-charge effects or changes in the electric
thermal stabilities [54]. There are four main surface potential that are induced when gas
approaches for increasing the selectivity of semi- adsorption, ionization or redox reactions take
conductor sensors. The first is to use filters or place. Ionosorption is the chemisorption of ions.
chromatographic columns to separate gases Chemisorption is adsorption where the involved
based on their physical properties. The second is forces are valence forces, which are the same kind
using catalysts, promoters, or other compounds as as those operating in the formation of chemical
surface additives. The third is to modify the phys- species [56]. The other model concerns oxygen
ical preparation of the material. The fourth is to vacancies which react with gas molecules, and it
characterize the short-term response of the sensor considers the variation of the subsurface/surface
to changes in concentration or temperature [55]. oxygen vacancies and their reduction-reoxidation
Low-Cost Sensors for Indoor and Outdoor Pollution 433

ability, which may lead to changes in the oxygen Sensing Properties


stoichiometry [9]. The sensor properties are determined by the recep-
The metal oxide surface is usually a thin film of tor function, the transducer function, and the util-
an oxide of a transition or heavy metal. The spe- ity factor. The receptor function describes how
cific metal that is used will depend on the appli- each constituent responds to oxygen and target
cation, for example, SnO2 or WO3. The film gases in the surrounding ambient air. The amount
overlies a layer of silicon and is heated to of oxygen adsorbed at this point determines the
200–400  C (depending on application). The sensing properties, and it depends therefore on the
best performance is obtained using a large surface surface area of the sensing material. The trans-
area to increase interaction with the gas. ducer function describes how the response of each
An extensively used gas sensor material SnO2 particle is converted into the response of the
is. It has well-known advantages that include low device. This is a result of the free carrier transport
cost and high sensitivity; however, the disadvan- mechanism between crystals next to each other.
tages concern lack of stability and selectivity. In Usually, a double Schottky barrier model is used
practical applications, several attempts have been to describe this mechanism. The utility factor is
made to overcome these disadvantages, for exam- defined as the degree to which a lowering of the
ple, by using chromatographic columns to sepa- response takes place as a result of diffusion and
rate the components, or by operating at different reaction with target gases through pores of the
temperatures, with different dopants, or by mea- assembly of crystals [9] (Fig. 6).
suring at different frequencies.
For many sensor applications, single crystal Comparison of Different MOx Sensors
silicon (Si) is an attractive substrate based on its Table 3 compares metal oxides as sensors [53].
mechanical stability and the feasibility of integrat- From Table 3, Fig. 7 and [53], it is seen that
ing sensing and signal processing electronics on binary oxides with a band gap of 2–4 eV such as
the same substrate. For chemical sensors, although MoO3, Nb2O5, SnO2, Ta2O5,TiO2, ZnO, and WO3
Si is merely the substrate, the choice is not always have n-type behavior, whereas other binary oxides
straightforward. Silicon has a high material cost per like Co3O4, Cr2O3, CuO, Mn3O4, and NiO exhibit
unit area, but this cost can often be offset by the p-type behavior. Some of the oxides switch
small feature size that can be achieved. Silicon, between p-type and n-type behavior under specific
with or without passivating layers, due to its conditions, which could be due to temperature,
extreme flatness, relatively low cost, and well- presence of a foreign gas in ambient air, or oxygen
established coating procedures, often is the pre- partial pressure. The selectivity of a sensor is
ferred substrate, especially for thin films (Fig. 5). related to its ability to respond to a given gas

Low-Cost Sensors for Indoor and Outdoor Pollution, energy and Fermi level in the semiconductor, EC is the
Fig. 5 This figure shows the energy band diagrams for a conduction band edge, EV is the valence band edge, and FB
metal with an n-type Si semiconductor contact and a metal is the Schottky barrier energy relative to EF [57]
with a p-type Si semiconductor, where EF is the Fermi
434 Low-Cost Sensors for Indoor and Outdoor Pollution

n-type semiconductor
transducer utility
receptor

e–

e–

Electron
depletion layer
target gas

p-type semiconductor

receptor transducer utility

+
h
e–

e–

Hole
accumulation target gas
layer

Low-Cost Sensors for Indoor and Outdoor Pollution, Fig. 6 Diagram of the conduction model and gas-sensing
mechanism based on n-type MOSs and p-type MOSs. The figure is based on Ref. [9]

when it is absorbed by the sensing material. In Temperature cycling is a method whereby the tem-
some cases, this can be achieved more easily by perature dependence of the signal is probed repeat-
adding a specific catalyst to the material, since edly and analyzed to extract useful information, in
catalysts modify the band gap; gases with an ion- particular regarding gas concentrations but also sen-
ization energy resembling the band gap are prefer- sor status. This method can improve performance
entially adsorbed. The band gap of the sensing and in some cases reduce cross-sensitivity
material determines which compounds the sensor [69]. Temperature modulation has several advan-
can detect: the larger the bandgap of the sensing tages; it can give a specific signature for each gas
material, the larger molecules the sensor is capable present, and cycles to higher temperatures can be
of detecting and vice versa, see Table 3 and Fig. 7. used to clean the surface. In addition, the informa-
tion gathered from modulation can give improved
Temperature Cycling sensitivity. There is likely to be a maximum in
Many properties of a semiconductor sensor depend sensitivity linked to the shape of the conductance
on temperature. These include the rates of gas versus temperature curve [55].
adsorption and desorption, the rate of decomposi- One study examined sensor performance for
tion of reducing gases, and the charge-carrier diffu- quasi-continuous temperature cycling. In this
sion length. Furthermore, many of the reactions that study, the temperature cycle consisted of two
take place on the surface of the sensor are exother- 10 s excursions from room temperature to
mic which can change the temperature of the sensor. 400  C and back to room temperature. The path
Because the sensors themselves and the surface down to room temperature was performed over
chemical processes are temperature dependent, the 50 steps, each with a duration of 200 ms. There
relationship is complex. Different gases have differ- was no heating during the remaining part of the
ent characteristic conductance-temperature profiles. cycle.
Low-Cost Sensors for Indoor and Outdoor Pollution 435

Low-Cost Sensors for Indoor and Outdoor Pollution, Table 3 Compounds used as sensors and their corresponding
bandgaps, and the gases they sense
Specific
Sensor compound Sensing [53] z/eV
Tin oxides (35%) SnO2 NH3, CH3CHO, CH3SH, H2S, NO2, C2H5OH, CO2, 3.6 [58]
CO, benzene, o-xylene, SO2, O2, H2, H2O, C4H10, CO
and NO2, NOx, petrol, CH4, O3, C3H8
Mixed oxides (13%) – Humidity, CO2, NOx, hydrocarbons, C2H5OH, NH3, –
NO, O3, NO2, SO2, CH4, LPG (liquefied petroleum
gas), H2S
Zinc oxides (10%) ZnO O2 (in water), CO, CH4, H2, H2O, C2H5OH, C3H8, 3.3 [59]
NO, NO2, CO2, O3, C2H6, n-C4H10
Titanium oxides (7%) TiO2 H2, CO2, O2, CO, CH4, ethanol, methanol, propanol 3.0–3.2 [60]
Tungsten oxides (7%) WO3 H2S, O3, NO, NO2, NOx, NH3 2.6–3.0 [61]
Indium oxides (5%) In2O3 O3, H2, CO, C3H8, NO2 2.7 [62]
Niobium oxides (3%) Nb2O5 NH3, CO, C2H5OH 3.4 [63]
Iron oxides (3%) Fe2O3 H2, CO2, O2, CO, CH4 2.2 [64]
Gallium oxides (3%) b-Ga2O3 O2 4.8–4.9 [65]
Cerium oxides (2%) CeO2 O2 3.2 [66]
Molybdenum oxides (2%) MoO3 NH3, NO2 3.2 [53]
Copper oxides (2%) CuO2 H2, CO2, O2, CO, ethanol 1.4 [53]
Aluminum oxides (2%) Al2O3 Humidity am-Al2O3: 7.0
[67], g-Al2O3:
7.6 [67]
Zirconium oxides (2%) ZrO2 O2, hydrocarbons, NOx, CO, O2, alcohol 3.84–4.51 [68]
Energy

Energy

Acceptor band Donor band CBM

VBM
A B
CuO2 ZnO In2O3 SnO2

Low-Cost Sensors for Indoor and Outdoor Pollution, conduction band (n-type semiconductor (B)). The figure
Fig. 7 The figure to left [1] displays two bands: one that to the right [58] shows the band gaps of four different metal
accepts electrons from the valence band (p-type semicon- oxides
ductor (A)) and one that transfers electrons to the

The temperature cycling mode was used to constant voltage operation. Furthermore, cross-
measure ozone, and the low power sensor was sensitivity could be reduced by simple adapta-
shown to be stable. The reproducibility was tions. The study also showed disadvantages by
greatly improved when compared to standard using temperature modulation in one-minute
436 Low-Cost Sensors for Indoor and Outdoor Pollution

cycles. If the gas concentration changes quickly, it cm3), s is the absorption cross section (e.g., cm2),
may lead to false results. Another disadvantage is and l is the absorption path length (e.g., cm).
that signal rates higher than 1 per minute cannot A wide range of accurate, reliable optical gas
be performed without modelling [69]. detection instruments is available; they do not
qualify as “low cost.” They include photo-
acoustic spectroscopy (PAS) multi-gas analyzers,
cavity ringdown spectrometers (CRDS), tunable
Optical Sensors
diode laser (TDL) spectrometers, Fourier trans-
form infrared (FTIR) spectroscopy, and resonant
Optical sensors are a broad class of devices that
absorption/fluorescence [71–73]. Spectroscopy-
use scattering or absorption of light. They range
based instruments usually have better sensitivity,
from simple components that detect when light
selectivity, and stability [73], and have shorter
levels are above or below a specific level to highly
response and recovery times [71] compared to
sensitive devices for detecting single photons.
nonoptical methods. Often these instruments are
Sensors are combined with wavelength filters or
set up in stationary monitoring stations due to
dispersion elements in order to perform spectro-
their nonportable size, relatively high-cost and
scopic measurements of single components; the
sensitivity to environmental factors (i.e.,
spectroscopy may be refined further by introduc-
weather). Recently, a number of successful, low
ing systems such as atomic emission lamps that
cost, compact optical sensors have been devel-
produce a single wavelength and resonant absorp-
oped which we will detail below.
tion/fluorescence for further increased specificity
and sensitivity. However, one quickly exits the
NDIR
realm of low-cost sensors to which this entry is
One promising low-cost, portable, commercially
confined. Most optical sensors produce an electri-
available family of gas sensors is based on non-
cal signal (voltage or current) that is digitized.
dispersive infrared (NDIR) spectroscopy. The
Optical techniques are widely applied in atmo-
NDIR technique has many advantages such as
spheric pollutant monitoring, especially for par-
high selectivity and limited cross sensitivity
ticulate matter (PM) detection but also for many
which makes it suitable for qualitative analysis.
trace gases [70].
In addition, the output of NDIR sensors responds
Gases can be selectively detected based on
linearly to concentration, and they have low fab-
their infrared (IR) spectra. Each molecule has a
rication cost, fast response, and low power con-
unique set of vibrational frequencies based on the
sumption. Therefore, NDIR gas sensors are the
masses of the atomic nuclei involved and the force
industry standard method of measuring the con-
constants of its chemical bonds, which can be
centrations of CO and CO2 [74]. Generally, an
used as a specific “fingerprint” for that molecule.
NDIR detector consists of a light source, absorp-
A molecule absorbs light at a unique set of ener-
tion cell, wavelength filter and detector (Fig. 8)
gies, determined by these vibrational frequencies.
and is a direct measuring technique determining
The concentration of a target pollutant is deter-
the mole fractions of specific gases that absorb in
mined from its absorption of light using the Beer-
the IR region.
Lambert law:
The components respond differently to envi-
  ronmental conditions, for example, temperature.
I0 The NDIR gas sensor is based on the Beer-
ln ¼A¼nsl
I Lambert law, seen above [75]. The key to making
an NDIR sensor work well is to get sufficient
Here, I0 is the intensity of light before the light flux at a specific wavelength to the detector,
sample and I the intensity after. A is the absorp- and furthermore, to make the absorption path (l)
tivity, determined by the product of n the number long enough to see the target gas even at low
density of gas (e.g., number of gas molecules per number densities (n); the signal is only useful if
Low-Cost Sensors for Indoor and Outdoor Pollution 437

Low-Cost Sensors for


Indoor and Outdoor
Pollution, Fig. 8 Typical
layout of an NDIR gas
sensor

it is larger than the intrinsic noise of the detector Particulate Matter


and amplifier. Particulate matter can be characterized by its total
NDIR has an advantage compared with other mass per unit volume, for example, as mg/m3. The
spectroscopic techniques in the area of energy size distribution of particles is extremely impor-
consumption, since its IR source produces light tant with implications for the health impact of
at wavelengths in the range of 1–15 mm and thus particles and their atmospheric lifetime and role,
can operate at lower temperatures than systems but it is harder to determine than the number
that use near infrared (NIR) or visible light. Dis- density of particles. A useful classification is
advantages of NDIR sensors include spectral often made by looking at the total mass density
interference (crosstalk from other molecules), of particles smaller than a certain threshold, for
and for some gases, a detection limit above ambi- example, PM10 (particles with an aerodynamic
ent concentrations. NDIR systems perform well diameter below 10 mm). Similarly, the terms
for CO2 though as it is present at concentrations of PM2.5, PM1, and PM0.1 are also used. Particles
hundreds of ppm and has strong infrared absorp- with an aerodynamic diameter larger than 2.5 mm
tions. NDIR sensitivity depends on the detector are called “coarse” and could include dust and
signal per unit of IR intensity, and the detection pollen. Those smaller than 2.5 mm, measured as
limit is a function of both sensitivity and signal-to- PM2.5, are “fine” particles and have been associ-
noise ratio. ated with a significantly elevated health risk.
In one study [72], five different NDIR sensors There is increased attention on “ultrafine” nano-
were used to monitor CO2 in a barn of dairy cows. particles, with a size smaller than 0.1 mm, mea-
The NDIR sensors are compared with two com- sured as PM0.1. These particles may be made, e.g.,
monly applied methods: photo-acoustic spectros- as brake dust or diesel soot.
copy (PAS) and an open-path laser (OP-laser). There are both high cost and low-cost devices
Every sensor was calibrated, tested for linearity, for measuring particle mass number concentra-
and sensitivity to static pressure. After the calibra- tion. While PM can be measured by many
tion, the NDIR sensors were exposed to CO2 in methods, only the method based on light scatter-
the barn together with PAS analyzers and an ing, called an optical particle counter (OPC), can
OP-laser for comparison. The tested NDIR sen- be produced at a low cost [76]. We can quickly
sors showed a small variability of 5%, and they note the success of a low-cost particle counter
were sensitive to a static pressure sensitivity of based on components from a smoke detector. The
0.08% of the readings per 1 hPa. It was concluded system employs two chambers: one for ioniza-
that the NDIR CO2 sensors are appropriate for tion using the active element of a smoke detector
multipoint monitoring of CO2 concentrations in and the second using photoionization. Because
livestock barns, and that they are a practical alter- the two chambers have different sensitivities to
native to the OP-laser and PAS methods for mon- fine and ultrafine particles, it is able to discrimi-
itoring averaged spatial or single-point CO2 nate the two size modes with high
concentrations [72]. accuracy [110].
438 Low-Cost Sensors for Indoor and Outdoor Pollution

In the context of optical detection of particles, sensors. All three sensors use IREDs (infrared light
it is important to note that the sizes of aerosol emitting diodes) to generate light. The PM sensors
particles are similar to optical wavelengths. were tested for the linearity of their response, preci-
A practical implication of the scattering of light sion, limit of detection, particle composition, size
is that if the particle is larger than the wavelength, dependence, and the relative humidity and influence
light could be absorbed. If the sizes are similar, of temperature [77]. The working principle of the
light may be scattered in a complex way, and if the GP2Y is sketched in Fig. 9.
particle is much smaller than the wavelength,
there is no interaction. Since visible light is in Linearity, Precision, and Limit of Detection (LOD)
the wavelength range of 380–700 nm, optical The GP2Y sensor gave the highest linearity with R2
particle counters often have extreme difficulty values of 0.9838 and 0.9831. The DSM sensor gave
measuring ultrafine particles; in contrast, optical the lowest R2 values of 0.8914 and 0.8921. The
particle counters that measure PM10, PM2.5, and DSM and the PPD sensors were expected to give
PM1 are commonly available. higher R2 values at smaller particle concentrations.
In one study [77], three low-cost PM sensors When comparing sensors of the same type, the
were tested and compared to three reference instru- linearities of the individual sensors were high, but
ments. The sensors used were the Shinyei they need to be calibrated separately because two
PPD42NS, in the study called “PPD,” the sensors gave the same output in at different concen-
Samyoung DSM501A, called “DSM,” and the trations, e.g., an analog output of 200 in a concen-
Sharp GP2Y1010AU0F, called “GP2Y.” The PPD tration range from 600 to 900 mg/m3. All three
and DSM were quite similar in their setup, while the sensors became saturated at 4 mg/m3 which leads
GP2Y was smaller in geometry. Furthermore, the to the conclusion that they are less useful for mea-
GP2Y has a different orientation than the other two suring extremely high concentrations of particles.

Low-Cost Sensors for


Indoor and Outdoor
Pollution, Fig. 9 Working
principle and critical
parameters of the Sharp
GP2Y low-cost particle
sensor. “PT” and “IRED”
represent the
phototransistor and the
infrared light emitting
diode, respectively
[78]. Particles flow in
through the top and can
scatter light which is
detected by the photon
detector with a “zero
background” geometry,
before flowing out of the
interaction region
Low-Cost Sensors for Indoor and Outdoor Pollution 439

For the three sensors, the standard deviation was Different sensors and instruments showed dif-
used to measure the reproducibility. The standard ferent responses when the particles’ composition
deviation for a concentration range of 0–100 mg/m3 was changed. Some variation in light scattering
varied from 15 to 90 mg/m3. The DSM sensor was can be caused by the variability of the refractive
the one with the lowest standard deviation, with index of different materials. The refractive index
relatively constant and small values. The PPD and correlates with the magnitudes of light scattering
the GP2Y sensors had higher standard deviations at and light absorption. This leads to the conclusion
higher particle concentrations, although the relative that PM sensors may over or underestimate mass
standard deviation of all the sensors decreased concentrations for some types of particles and
when the particle concentration increased. This conditions. The water content of particles is
implies that the sensors were not very accurate dependent on relative humidity. Sensors can
when measuring low concentrations (<200 mg/ achieve a higher accuracy if their calibration is
m3). The sensor which gave the highest LOD tuned to the composition of the particles being
value, 30.2 mg/m3, was the GP2Y. The PPD had studied; in addition, humidity corrections are
the lowest value of 6.44 mg/m3. common.

Effect of Relative Humidity, Temperature, Particle Electrochemical Cells


Size, and Composition
When tested for particle size dependence, it was Electrochemical gas sensors are able to sense a
shown that for the same mass concentration, the target gases that can be oxidized or reduced in
sensors’ output increased with decreasing particle order to generate a current. Often they are
size. The PPD and DSM sensors were shown to be designed so that the gas supply is limited by
more sensitive to larger particles, and the GP2Y diffusion, so that the response is linearly propor-
sensor was shown to be more sensitive to smaller tional to concentration. This allows for simpler
particles. Water is effective at absorbing infrared calibration involving the determination of the
light, which can lead to an overestimation of the baseline offset and the slope of the calibration
particle mass concentration because of reduced curve. In the study in Ref. [48], a general electro-
light intensity. Water vapor may cause failure in chemical sensor is described based on the amper-
the circuits and hereby give false results. Overall, ometric methodology (Fig. 10).
relative humidity has a large effect on the sensors’ Some common target gases for amperometric
output. The temperature was shown to have very sensors are O2, CO, NO2, NO, O3, H2S, and SO2.
little effect on the three PM sensors in the range of The standard amperometric gas sensor can detect
5–32  C [77]. gases in the 1–10,000 ppm range, and some can be
Particle mass concentrations are calculated used for air quality measurements in the ppb
from the size distributions of the particles, and range.
this depends on the composition and size of the The main components of the sensor are a gas
particles. The total mass concentration of the par- chamber, an electrochemical cell, and a reservoir.
ticles, m, can be calculated by The gas chamber determines the access and sen-
sitivity of the sensor, and it sometimes has a filter
  for better selectivity. The usual electrochemical
p 9  
m ¼ M 0 exp 3lnd pg þ ln2 sg cell has either two or three electrodes [79]. In a
6 2
three electrode configuration, the electrodes are
called the working, reference, and counter elec-
where M0 is the total number concentration, dpg is trodes, and they are separated by the so-called
the geometric mean particle size, and sg is the “wetting filters.” The filters are hydrophilic and
geometric standard deviation obtained through a allow ionic contact of the electrodes. In the work-
curve fitting process. ing electrode (WE), either reduction or oxidation
440 Low-Cost Sensors for Indoor and Outdoor Pollution

Low-Cost Sensors for Gas permeable membrane


Indoor and Outdoor
Pollution, Fig. 10 1. seal
Illustration of an
electrochemical cell based Working electrode
on [48]
reference electrode
A
counter electrode

Electrolyte reservoir

wetting filters

of the gas occurs, and typically, the WE is coated gas analyte. The current measured by the sensor
with a catalyst. The catalyst is chosen for a spe- and the mole fraction of the gas analyte are pro-
cific gas, which enters through diffusion to give a portional. The current is described by
high surface area and promote the reaction [48].
In the electrochemical cell, there is an electro- I 1 ¼ Kc
lyte solution which usually consists of mineral
acids or organic solvents with an added salt. The where I1 is the limited current, K is the coefficient
WE is usually supported by a gas porous mem- of proportionality, and c is the molar fraction of
brane. The reservoir accounts for changes in equi- the target gas. Sensor response times are typically
librium electrolyte concentration. Concentration a few seconds. A rapid response time is possible
changes take place because, e.g., the relative because of the overall configuration, in which
humidity changes. The fluid contains hygroscopic analyte diffusion through the membrane
species (acids, salts), leading to a change in supporting the working electrode is the limiting
volume [79]. step [79].
When a target molecule contacts the working
electrode surface, a redox reaction takes place, A Fourth Electrode
triggering another reaction at the counter elec- Some sensors have been made with four elec-
trode. The reference electrode is used to keep the trodes for increased performance at low concen-
working electrode at a constant potential. The tration, for example, for gasses like NO2, O3, CO,
counter electrode does not have a fixed potential NO, H2S, and SO2 that typically occur at ppb
like the working electrode; the potential of the levels in ambient air. The fourth electrode is a
counter electrode can drift. In clean air, the work- second working electrode, often called an “auxil-
ing and counter electrodes have the same poten- iary electrode”; this electrode is not exposed to the
tial, but the potential of the counter electrode target gas. The electrode provides a background
changes when a gas reaches the surface of the current that does not have the faradaic current of
working electrode, and the counter electrode the regular working electrode. The faradaic cur-
must balance the current to compensate. The out- rent comes from the exchange of electrons,
put of the sensor represents the difference between described previously, when the electrochemical
the potentials of the working and the counter reaction occurs. By this method, the fourth elec-
electrodes, and the current signal is usually in trode does not detect the target gas but rather is
the range of 10–100 s of nA per ppm of sensed used to measure and counteract sensor drift.
gas. The output and the concentration of the target A particular example is that measurements of O3
gas are directly proportional [48]. With a suffi- and NO2 are known to suffer from cross-
ciently fast reaction, the mechanism is limited by sensitivity. These two gases react equally on
the mass transfer to the working electrode by the many sensors, but this problem can be addressed
Low-Cost Sensors for Indoor and Outdoor Pollution 441

by using filters to separate the gases [79]. Other over which time the response was compared to a
challenges in using electrochemical sensors reference device. The ozone sensor had a working
include calibration of the sensitivity to the target electrode, a reference electrode, and a counter
gas, and cross-sensitivity for mixtures of gases, electrode, and the range of measurement was
which depend on temperature, humidity, and 0–20 ppm.
pressure [80]. The study found that this method for monitor-
ing ozone can be a useful alternative to other types
Potentiometric Sensors of devices, e.g., semiconductors. Ozone detection
Potentiometric sensors are often used for using electrochemical sensors was shown to have
detecting oxygen. The typical potentiometric sen- a lower cost and low power consumption. One
sor has an oxygen ion solid electrolyte to conduct disadvantage of this sensor was that it can be
current against two electrodes on either side of the affected by other gases such as NO2 and NO,
electrolyte. One of the electrodes is a working and relative humidity. The cross-sensitivity had a
electrode, and the other is a reference electrode. noticeable effect on the voltage of the working
The WE is in contact with an unknown partial electrode; this was corrected for in the analysis.
pressure of oxygen, which is the amount of oxy- Another disadvantage is that the voltages of the
gen to be measured. The reference electrode is in working electrode and the reference electrode
contact with a known partial pressure of oxygen. were found to increase rapidly with relative
The output of the sensor is the potential difference humidity and the flow rate. The increase in the
measured between the working electrode and the working electrode and reference electrode poten-
reference electrode, which is called the electro- tials caused an increased offset voltage. The sen-
motive force (EMF). sor generally took 40 min to overcome the
Typically, the electrodes are made of Pd, Pt, interference [83].
Au, or Ag, but other materials have been used for
sensing a variety of gases. A gas sensor for mea- Intercomparison Study of Electrochemical
suring CO2 was made using a lithium phosphorus Sensors
oxynitride electrolyte, and a sensor for measuring Sensor measurements can suffer from interfer-
chlorine gas was made using MgO-stabilized zir- ences due to exposure and their response to
conia [81] (Fig. 11). co-pollutants. One example is CO2 which has a
high and sometimes variable concentration due to
Ozone Detection sources including human respiration and fossil
A study investigated ozone detection with minia- fuel combustion. In some cases, the crosstalk sig-
ture electrochemical sensors. In the study, the nal can be larger than the signal being measured
surrounding air was investigated for 18 days many orders of magnitude. In two studies [83, 84],

Au wire

Au Li2CO3
sensing electrode
Li2.88PO3.73N0.14
electrolyte EMF V

LiCoO2 + Co3O4
reference electrode

Low-Cost Sensors for Indoor and Outdoor Pollution, Fig. 11 A schematic structure of a potentiometric electro-
chemical cell [82]
442 Low-Cost Sensors for Indoor and Outdoor Pollution

five commercially available electrochemical sen- Except for the O3 sensor, the individual sensor’s
sors were investigated to determine their perfor- sensitivities to the target gas is higher than the
mance relative to more traditional measurement sensor cross-sensitivities to other co-pollutants
technologies. The five investigated commercial by a factor of 10 to 100. The O3 sensor shows
low-cost air pollution sensing systems were similar sensitivities to its target gas O3 and the
designed to measure CO (CO-B4, Alphasense co-pollutant NO2, as has also been reported by
Ltd), O3 (OX-B421, Alphasense Ltd), NO others [85]. Compared to the other sensors, the
(NO-B4, Alphasense Ltd), NO2 (NO2-B4, CO and NO2 sensor have a high specificity to
Alphasense Ltd), and SO2 (SO2-B4, Alphasense their target gases, evidenced by their lower
Ltd). The aim of the studies was to establish the cross-sensitivities. The NO2 sensor has the
selectivity of these sensors to their target com- highest selectivity since it generally has low
pounds, quantitatively characterize chemical cross-sensitivities to co-pollutants, even at the
interference to other pollutants, and evaluate the highest relative humidity values and lower
scale of impacts of co-pollutants. levels of NO2. However, at high concentrations
of CO2, an artifact signal can appear. In some
Chemical Interference of Co-pollutant cases, the absolute interference signal induced
There is a complex set of interconnections by a co-pollutant is very small. However, the
between the sensors’ response to co-pollutants relative amounts of certain co-pollutants to the
and the target species. The individual sensitivi- target species is such that the overall response of
ties and cross-sensitivities of the five sensors a given sensor could be dominated by the
and co-pollutants are presented in Table 4. co-pollutant response [83, 84].

Low-Cost Sensors for Indoor and Outdoor Pollution, co-pollutants (in 103 V ppb1 for O3, NO, NO2, SO2
Table 4 Sensor sensitivities to their target species and 103 V ppm1 for CO2) under four different RH
(in 103 V ppb1) and their cross-sensitivities to other conditions [84]
Sensor
Target gases RH/% OX-B421 CO- B4 NO- B4 NO2- B4 SO2-B4
O3 15 0.44 0.029 0.01 0.002 0.14
30 0.44 0.0007 0.01 0 0.12
45 0.43 0.017 0.014 0 0.14
60 0.45 0.027 0.009 0.004 0.15
CO 15 0.023 0.37 0.012 0.035 0.010
30 0.013 0.35 0.028 0.012 0.015
45 0.009 0.37 0.007 0.007 0.013
60 0.011 0.41 0.004 0.005 0.054
NO 15 0.21 0.003 0.54 0.004 0.060
30 0.09 0.005 0.57 0.001 0.022
45 0.12 0. 0.56 0.013 0.027
60 0.11 0.002 0.55 0.009 0.019
NO2 15 0.44 0.04 0.09 0.42 0.1
30 0.43 0.02 0.09 0.48 0.1
45 0.44 0.03 0.1 0.43 0.1
60 0.44 0.02 0.1 0.45 0.1
SO2 15 0.022 0.02 0.01 0.002 0.19
30 0.01 0.03 0.006 0.005 0.21
45 0.015 0.026 0.004 0.005 0.20
60 0.002 0.023 0.007 0.002 0.22
CO2 15 0.01 0.002 0.009 0.001 0.006
30 0.04 0.007 0.0002 0.002 0.007
45 0.1 0.023 0.014 0.004 0.012
60 0.1 0.058 0.024 0.009 0.010
RH 0.56 0.11 0.20 0.00 0.02
Low-Cost Sensors for Indoor and Outdoor Pollution 443

Electrochemical Cells and Metal Oxide of the low-cost sensors is evaluated by comparing
Sensors their output with the reference data. The Data
Quality Objective (DQO), defined by the
An increasing number of air quality European Air Quality Directive, is a measure of
(AQ) monitoring networks based on low-cost sen- the acceptable uncertainty of the indicative mea-
sors have been deployed. Electrochemical surements. The allowed uncertainties are 50% for
(EC) and metal oxide (MOx) sensors are the two PM10, 30% for O3, and 25% for CO, NOx, and SO2
most common low-cost gas sensors currently used [70]. In this section, NO2 and O3 are selected as
in AQ measuring products. Both types of sensors representative and illustrative target gases to com-
have good sensitivity, fast response time, a wide pare the performance of different sensor nodes.
range of detectable pollutants, and portable size The Table 5 summarizes the campaign results
[86, 87]. However, for a new technology and from the EuNetAir joint exercise [91] and the
deployment, the data quality of the network must CAIRSENSE project [91]. Most of the commercial
be validated. Historically, both EC sensors and platforms that were tested used electrochemical
MOx sensors have a reputation to overcome, and cells to detect NO2 and O3. In the case of NO2, a
their precision and accuracy should be verified in majority of the EC cells performed well, although
real-world situations [88]. both MOx sensors did not show a high correlation
A number of field campaigns have been under- with the reference measurement. The EC cells did
taken to assess the performance of low-cost AQ not work as well for NO2 as for O3, only two out of
sensors in the real world [83, 84, 89]. Typically, five gave accurate results, while MOx sensors were
these campaigns pair a cluster of commercial nodes able to accurately detect O3 [91].
with an established monitoring station using cali- Given the similar performance of EC cells and
brated instruments with a known track record. The MOx sensors for controlled laboratory conditions,
station is typically equipped with standard equip- a possible reason for the performance gap between
ment providing reference measurements of NOx, EC cells and MOx sensors in the real world could
O3, CO, CO2, and SO2. Temperature, relative be the post-measurement calibration algorithm. EC
humidity (RH), pressure, and wind speed are also cells have a relatively simple sensing mechanism
recorded by the station [90, 91]. The performance where the detected current is proportional to the

Low-Cost Sensors for Indoor and Outdoor Pollution, obtained from filed campaigns EuNetAir joint exercise
Table 5 The list of correlation coefficients of tested com- [91] and CAIRSENSE project [90]. Categorized by sensor
mercial sensor with the reference measurement. Results types and target gases [84]
Target gas Platform, model Sensor type Correlation coefficient (r2) Reference
NO2 SNAQ, Alphasense B4 EC 0.84 [91]
ECN, Ciththch 3E50 EC 0.89 [91]
Nanoenvi, Alphasense B4 EC 0.57 [91]
AQMesh, Alphasense B4 EC 0.89 [91]
ENEA, Alphasense B4 EC 0.06 [91]
Cairpol, Cairclip EC 0.57 [90]
AQMesh, Environmental Instruments Ltd EC r < 0.5 [90]
AUTh-ISAG, MiCs-2710 MOx 0.02 [91]
AirQuality Egg MOx r < 0.5 [91]
O3 SNAQ, Alphasense B4 EC 0.14 [91]
AQMesh, Alphasense B4 EC 0.70 [91]
ENEA, Alphasense B4 EC 0.13 [91]
Cairpol, Cairclip EC 0.88 [91]
AQMesh EC r < 0.5 [91]
AUTh-ISAG, MiCs-2610 MOx 0.12 [90]
Nanoenvi, MiCs-OZ-47 MOx 0.77 [90]
444 Low-Cost Sensors for Indoor and Outdoor Pollution

gas concentration. However, there is no simple satisfactory output [2]. The task of creating an
model that can transform the MOx signal ideal sensor is difficult, and research and develop-
(normally resistance) into a concentration. Taking ment continue. The applications of the sensors
metrological variables (temperature, pressure, etc.) typically do not require perfection in all areas at
into account is complicated. It should also be noted once. For example, for monitoring the concentra-
that the same model of EC cells can behave differ- tions of pollution in the environment, the detec-
ently in different systems, e.g., AQMesh tion limit may be relatively high, and a response
Alphasense B4 vs. ENEA Alphasense B4. This time of a few minutes is acceptable, because the
could be due to different applied algorithms, the concentration of pollutants normally changes
design of the electronics, or the sampling method. slowly. In the case of a sensor monitoring, the
In addition, the same platform can perform differ- concentration of a compound in an industrial pro-
ently in different situations, for example, the cess, the sensor does not require a detection limit
AQMesh systems as used in Ref. [91] vs. Ref. [90]. at ppb level and a response time in seconds would
In conclusion, the data quality generated by be desirable.
low-cost sensor platforms has room for improve-
ment, but certainly, they are able to provide low
cost and high time resolution with the trade-off of
Personal Exposure Monitoring and
somewhat compromised data quality. The EC cells
Installations in the Field
are more widely applied in commercial products
and at the present time appear to have a better
It is important to identify the purpose of the expo-
performance record than MOx sensors; however,
sure monitoring, in order to choose the right sen-
MOx sensors also have good potential for real-
sor. There is a wide range of sensors with different
world applications if the right algorithm is applied.
cost, sensitivity, stability, selectivity, accuracy,
robustness, etc. The choice depends on whether
the goal is to raise awareness regarding pollution
Comparison Between MOx, or to accurately measure the specific concentra-
Electrochemical, and Optical Sensors tion of a specific pollutant. Advances in sensor
technology mean that in some cases, individuals
Three types of low-cost gas sensors are compared: can now monitor air pollution levels themselves
MOx sensors, electrochemical sensors, and opti- using relatively cheap, accurate, and straightfor-
cal sensors. The summary is presented in Table 6. ward equipment. Consequently, exposure assess-
An ideal sensor would possess high sensitivity, ment can now be a combination of data from fixed
dynamic range, selectivity and stability, good lin- site measurement stations, modelling, and per-
earity, low detection limit, fast response time, and sonal portable sensors.
a long life cycle. Life cycle is the period of time Awareness of the health and economic costs of
over which the sensor will continuously provide air pollution has increased. Urban environments

Low-Cost Sensors for Indoor and Outdoor Pollution, Table 6 Comparison between MOx, EC, and optical sensors
Sensor type
MOx [54] EC [92] Optical [73]
Sensitivity (ppm-range) High High High
Sensitivity (sub-ppm) Low Medium Low
Selectivity Low High High
Accuracy Low High High
Lifetime High Medium High
Power consumption Low High Low
Cost High Medium Low
Low-Cost Sensors for Indoor and Outdoor Pollution 445

are exposure hot spots due to the concentrations of cost; however, they are cross-sensitive and display
both pollution sources and people, and 96% of nonlinear output signals [17]. The model perfor-
people in large cities are exposed to pollution mance has been evaluated, and the relationship
levels above recommended limits. There are between reference data and collocation-calibrated
over three million deaths each year associated sensor readings displays a minor negative bias at
with poor outdoor air quality [93]. Urban air qual- the higher end of observed concentration levels,
ity is highly dependent on emissions of, for exam- possibly driven by the small number of data points.
ple, fine and ultrafine PM and NO2 from road The approach gives access to air quality monitor-
vehicles, which also contribute to global air ing to a wider group of scientists and citizens;
pollution. however, there are some uncertainties regarding
A study by Carslaw et al. (2013) [94] reports the actual personal exposure levels due to the
measurements of NO, NO2, and NH3 from almost level of user engagement [30].
70,000 vehicles (taxies, buses, and passenger Low-cost pollution monitors have been placed
cars) from 1985 to 2012 in the UK made using a at many stationary locations and are also
remote sensing technique. In this study, emissions employed with mobile platforms. Installations in
are recorded depending on specific vehicle tech- the field are necessary to monitor concentrations
nologies that impact emissions performance. It is of the key pollutants. One example of a field
possible then to compare different vehicles with installation is the Airlabs AirNode-T (#3 and
respect to emissions, for example, the results for #4), developed by the company Airlabs in Copen-
TfL buses and diesel cars show important varia- hagen. The AirNode is a low-cost and low-power
tions in NO2 emissions depending on the vehicle self-contained air quality monitoring platform
manufacturer. By analyzing trends in NOx and measuring PM2.5, PM10, NO2, O3, and CO. The
NO2 at 23 roadside sites in London, the study two AirNodes are mounted at DCMR’s Schiedam
found that total NOx and NO2 emissions have air quality monitoring station in Rotterdam, NL,
only decreased by about 1 and 0.5% annually, and they have been running onsite since
respectively, over the past 10 years. The trends December 19, 2018. A field validation of the
are in agreement with the previously determined AirNodes shows the uncorrected readings from
trends between 2004 and 2009 measured by AirNodes #3 and #4 compared to reference mea-
Carslaw et al. (2011) [95], which suggest that surements at the air quality station over a 40-day
NOx and NO2 concentrations are decreasing period. The reference data was collected by the
more slowly than indicated by emission inventory station operated by the DCMR Environmental Pro-
estimates. tection Agency. The station monitors an array of air
In addition, new vehicle after-treatment tech- pollutants including PM2.5, PM10, NO2, and O3.
nologies have increased the ratio of NO2 to NO The uncorrected readings from AirNodes #3
compared with older vehicles, in particular for and #4 have been plotted against the references
increased engine loads, indicating a challenge in and R2 for the different plots are seen on the
emissions source management [94]. graph. The R2 values show that AirNodes #3 and
Low-cost portable sensors are promising for #4 are most accurate toward O3 and least with
personal exposure monitoring, although such sen- PM2.5 (Fig. 12).
sors not yet have achieved their full market poten-
tial. Many researchers are working on improved
wearable sensors. Piedrahita et al. [17] developed Calibration
low-cost, wearable, air quality monitors (M-Pods)
using the Arduino platform. The M-Pods have two The sensors were calibrated by three different
types of sensors – commercially available metal methods whose performance was then compared.
oxide semiconductor (MOx) sensors for NO2, CO, The three methods were linear regression, multi-
O3, and VOCs, and NDIR sensors for CO2. The variate linear regression, and an artificial neural
MOx sensors show high sensitivity and are low in network.
446 Low-Cost Sensors for Indoor and Outdoor Pollution

Low-Cost Sensors for Hourly average


Indoor and Outdoor 80
R2>0.84* Reference

PM2.5 (ug/m3)
Pollution, Fig. 12
60 Node03
Readings from AirNodes #3
Node04
and #4 compared to 40
reference measurements at
the air quality station over a 20
40-day period
0

80
R2>0.96
60

O3 (ug/m3)
40

20

150
R2>0.93
NO2 (ug/m3)

100

50

0
19/12 28/01

For linear regression calibration, each sensor the sensor system has a connection to a network, it
had a calibration function, which was made by can perform automatic calibrations [96]. Another
assuming linearity between the sensor response study [47] uses forward calibration, backward
and a reference measurement for each pollutant. calibration, and initial calibration. The forward
The multivariate linear regression was made using calibration is the traditional way of calibrating a
the least square method. The artificial neural net- sensor. This method calculates new parameters
work (ANN) is a modelling technique. Two types based on a new set of readings. The disadvantages
of ANN were considered in this study, radial- of this calibration method are that the readings
based functions and multilayer perceptron, which the new parameters are built on lag behind
although the latter gave poor results and was in time. The backwards calibration method calcu-
left out. lates new parameters which are used to both cal-
For the linear regression calibration and the ibrate future readings and recalculate the former
multivariate regression calibration, the R2 values readings of the sensor. The disadvantage with
were high for the O3 sensors, although both backward calibration is that there is a delay before
methods had some deviations. The slope and readings become available. The delay depends on
intercept of the orthogonal regression differed how much time passes between the two measure-
from 1 and 0, respectively. For the ANN methods, ments. The so-called instant calibration calculates
the R2 values were higher, the slope was closer to new parameters more frequently [47].
1, and the intercept was closer to 0. The ANN One study [97] of an array of semiconducting
method seems to have the lowest uncertainties gas sensors uses static chamber calibration. This
compared to the other calibration methods [88]. calibration has two steps. First, the sensor needs to
One study [96] proposes an autocalibration determine the initial setting. Zero air, air without
method. In the study, the sensor output is adjusted pollution, is used to find this value. The second
to the average of the surrounding stations. When step consists of finding the span of the sensor. One
Low-Cost Sensors for Indoor and Outdoor Pollution 447

drawback with this method is that there is no CO, NO2, relative humidity, and temperature.
official standard for “zero air.” Some studies use The next step is to integrate the Internet of Things
pure nitrogen or pure synthetic air, and others use (IoT) in smart cities. The internet of Things is the
ambient air when they consider the area to be integration of the connectivity of the internet with
clean. Yet others use ambient air that has been objects around us, allowing them to send and
filtered to remove some impurities. This study receive data. In smart cities, sensors would be
chose to use clean ambient air to calibrate the connected to a cloud web interface enabling
SO2 sensor, while synthetic air was used to cali- access to sensor data in real-time [101]. The aim
brate the CO sensor [97]. of the Internet of Things is to make the internet
Another method used to calibrate sensors is the more extensive and engaged in day-to-day life.
least-square method. The study in Ref. [98] uses The paradigm has many applications including
this method. The sensor node was placed in a clear using sensors to monitor air pollution. The IoT is
plastic sealed container with a sensor probe, the likely to play an important role in realizing the
GrayWolf Direct Sense IAQ 610. The concentra- smart city dream [102].
tion of gas inside the container was varied by There are three layers to the Internet of Things:
injecting a certain gas. Using the least-square the perception layer, the network layer, and the
method, the collected data were calibrated against application layer. The perception layer consists of
the GrayWolf system [98]. objects that can gather information, measure dif-
ferent elements, and exchange information with
other objects such as sensors for measuring air
The Future: Smart Cities and New pollution. The network layer is responsible for
Materials transferring data from the perception layer to the
application layer. In the application layer, the
There are several definitions of a smart city. One information is gathered and treated, and it aims
description is that a smart city is an advanced city to create smart cities, among other things [103].
that uses information and built elements to create a
more connected and sustainable city and provide for
the needs of citizens. Ideally, the smart city improves Nanowires
the quality of life for people using the city [99]. Nanowires are an emerging technology for sensing
Low-cost sensors are often touted as a technol- nitrogen oxides. A nanowire as the name implies is
ogy that could enable smart cities. Such sensors a wire with a very small diameter typically tens or
could be used for many purposes, for example, hundreds of nanometers. The wire has a low con-
they could act as a monitoring network to indicate ductivity due to its small cross section, and the
fire, explosion, or elevated levels of dangerous conductivity is sensitive to the presence of oxidiz-
pollutants, and they can provide real-time data to ing or reducing gases which can donate or with-
monitor the concentrations of the pollution. Data draw electrons in analogy to their effect on
from the sensors can support decisions and give semiconductors discussed above. To illustrate the
the public access to air quality information. The subject, we will summarize a study of the ability of
sensors in a smart city could be integrated in nanowires made of In2O3 and WO3 to sense NO2,
wireless network [100]. NO, and N2O. The study found that all three nitro-
One real-world example is a study which gen oxides can be sensed by the nanowires. The
investigated the performance of a network of In2O3 nanowire showed the best performance in
wireless sensors for air pollution monitoring. terms of sensitivity and operating temperature; it
The main goal of the study was to monitor outdoor had a diameter of approximately 20 nm. The WO3
air pollution levels at a school. The sensors had a nanowire was also shown to work although it had a
low cost and were able to measure pollution in real lower sensitivity than the In2O3 nanowire. Both
time. The different sensor nodes in the system In2O3 and WO3 nanowires can reliably sense
measured air quality simultaneously, recording N2O, NO, and NO2 [104].
448 Low-Cost Sensors for Indoor and Outdoor Pollution

Low-Cost Sensors for NO2


Indoor and Outdoor NO2
Pollution, Fig. 13 NO2
Schematic illustration of a
network of SnO2 nanowires NO2 Pt wire
on the SiO2/Si substrate [7] NO2

Au Pt Pt
Substrate of SiO2/Si

Another approach for measuring NOx gases is MOFs are attractive because they are not toxic,
porous silicon nanowires. A study examined Si the pore-size can be controlled, they have high
nanowires made by metal-assisted chemical etch- surface areas, the characteristics of sorption are
ing, which increases the sensitivity of the electri- reversible and controllable, and they have an ana-
cal properties for towards NOx gases. The lyte specific adsorption. MOFs designed for spe-
nanowires had a swift response, which is associ- cific VOCs have been shown to successfully detect
ated with the high surface area. The method can be gases with high sensitivity. The analytes can detect
applied to larger scale semiconductors for moni- methanol, ethanol, isopropanol, and acetone at
toring air quality at room temperature [8]. concentration levels of 250–1500 ppm [106].
Nanowire fabrication is typically both expen- An interesting development is the possibility
sive and time-consuming, a drawback towards of using MOFs to detect NH3 as this gas is both
implementing the otherwise promising nanowire important in specific environments linked to live-
sensors. One study investigates nanowires that stock and biogas, and, hard to detect. MOFs with
avoid this problem because they are self- rare earth elements were investigated in a study
assembling. In this study, the nanowires are looking at their ability to detect ammonia. In the
made of SnO2 on Pt electrodes with a Au catalyst. study, they showed that the MOF sensor was able
The nanowires are grown on a Pt/SiO2/Si sub- to detect NH3 at room temperature down to con-
strate, and the sensors were used to measure centrations of 1 ppm. The sensor showed good
NO2. The platinum layer was necessary because stability even in the presence of other gases [6].
the Au layers were consumed as the nanowires Formaldehyde is difficult to detect, and there are
grow. Figure 13 shows the nanowires on the sub- no good low-cost methods for measuring it. One
strate. The sensor measures NO2 as modulated by study investigates a MOF-based self-calibrated
oxygen molecules adsorbed on the surface. Elec- luminesceuce sensors for measuring levels of indoor
trons are extracted from SnO2, which leave oxy- formaldehyde concentrations. The sensor used an
gen ions on the surface. This leads to an increase Ag(I)-Eu(III) functionalized nanocomposite MOF
in the resistance of the nanowire. The study shows sensor. The system showed very good sensitivity
that the sensitivity of the sensor increases linearly and fast response for formaldehyde and had no
with increasing NO2 concentration. The maxi- interference from other pollutants. A key factor
mum temperature was 200  C [7]. was that it had a very high detection limit of ca
51 ppb, which is below the exposure limit of form-
Metal-Organic Frameworks aldehyde. The study suggests that a cheap and rela-
Metal-organic framework (MOF) structures have tively simple molecular material can be used to
recently been studied for their use in sensors for determine formaldehyde concentrations with very
measuring air pollution [6]. The structure of a good selectivity and sensitivity, fast response, and
MOF formed by self-assembly is shown in Fig. 14. good performance at room temperature [107].
Low-Cost Sensors for Indoor and Outdoor Pollution 449

Low-Cost Sensors for


Indoor and Outdoor
Pollution, Fig. 14
Schematic structure of a
self-assembly MOF [105]

Conclusion involve the incorporation of nanowires and metal-


organic frameworks. A study showed that a sensor
In this entry, important concepts related to low-cost with MOFs could detect formaldehyde, a com-
sensors are introduced and focus is given to three pound that is otherwise impossible to detect at
main types of low-cost sensors: metal oxide sensors, ambient levels in real time with a low-cost system,
optical sensors, and electrochemical sensors, along with good selectivity and sensitivity. The future of
with a number of interesting and emerging technol- low-cost sensors is ultimately in smart cities, where
ogies. MOx sensors are often used because of their they can contribute with information about pollu-
low cost, robustness, and simple structure. One of tion levels and provide early warning in cases of
the most common MOx sensors is the SnO2-based pollution-related disasters. Low-cost sensors have
semiconductor. A comparison of various metal proven their value, and their accuracy and value are
oxide-based sensors presented some specific metal only expected to increase with time.
oxide sensors with their target pollutants and their
corresponding band gap. Optical sensors rely on the
detection of light. Optical sensors are especially Bibliography
good at detecting particulate matter and infrared
active gases. Two kinds of optical sensors were 1. Atkins P, de Paula J, Friedman R (2009) Quanta,
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climate change, heatwaves are predicted to occur
Measuring Heatwaves and Their more frequently and with greater severity than
Impacts previously experienced. Despite increasing rele-
vance, formal analysis of heatwaves and their
Benjamin Disher, Brandon Edwards, impacts is limited. Where studies have been
Thomas Lawler and Douglas Radford undertaken, there has been little consensus across
The School of Civil, Environmental and Mining the world as to the most appropriate definition and
Engineering, The University of Adelaide, handling of extreme temperature events.
Adelaide, SA, Australia

Introduction
Article Outline
Heatwaves remain one of the deadliest natural haz-
Glossary ards globally, causing damage across a wide range
Definition of the Subject of industry sectors such as human health and infra-
Introduction structure [1, 2]. In the health domain, heatwaves
Heatwave Indices cause more deaths in major cities than any other
Heatwave Impacts extreme weather events [3], and past heatwaves
Application of Indices to Impact Analysis have caused widespread interruptions and damage
Future Directions to the health, built environment, energy, transport,
Bibliography agricultural, environmental, and water sectors. The
consequences of extreme heat events are underrep-
Glossary resented in research due to challenges in both defin-
ing a heatwave event and measuring its impacts [4].
Exposure The probability of being impacted by Studies conducted suggest that even under
a hazard of a given magnitude. conditions of decreased greenhouse gas emis-
External Drivers Factors which influence the sions, the frequency, intensity, and duration of
vulnerability, hazard, and/or exposure compo- such heat events are likely to worsen in coming
nents of risk. decades [5], with losses in population due to nat-
Hazard The event (here, heatwave) causing risk to ural disasters expected to increase with both cli-
a system or component with a given magnitude. mate change and growth and concentration [6]. In
Indices Quantitative metrics based on atmospheric contrast, current projections of greenhouse gas
parameters and other measurements used to mea- emissions see the frequency, intensity, and dura-
sure the severity of heatwave events. tion of heatwaves increasing significantly, which
Return Period The average period expected are likely to exacerbate the adverse effects of
between a defined magnitude event. heatwaves. In most regions around the world, a
Vulnerability The relationship between a haz- 1 in 20-year hottest day event is likely to become a
ard’s magnitude and the relative damage expe- 1 in 2-year event due to climate change [7].
rienced by the component or system of interest. Consequently, there is a need to quantify the
impact of heatwaves upon these various sectors,
in order to effectively prepare for, and respond to,
Definition of the Subject future heatwave events. Heatwave indicators and
indices can act to transform relevant atmospheric
Heatwaves are widely reported natural hazards parameters into a risk or exposure level for a
that cause a myriad of negative impacts. Due to particular sector (i.e., health, infrastructure, etc.)
© Springer Science+Business Media, LLC, part of Springer Nature 2021 455
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_1102
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2020, https://doi.org/10.1007/978-1-4939-2493-6_1102-1
456 Measuring Heatwaves and Their Impacts

Many different heatwave indices and parameters riverine flooding, and bushfire events. The frame-
have been created in this spirit. work has the capability for integrated and predic-
At present, many indicators and indices cap- tive risk analysis, but not yet been applied to
ture the human health impacts of heatwaves, but heatwaves. Similar frameworks include the
there remains no commonly accepted metric in health-orientated extreme heat vulnerability
this domain [8]. Less research has been under- framework created by Wilhelmi and Hayden
taken to quantify the impact of heatwaves on [12], and the vulnerability assessment and adap-
non-health areas, particularly within the subsets tation framework created by Filosa et al. [13].
of infrastructure (electrical, transport, roads, etc.) These approaches to evaluating risk require the
and agriculture. The existing literature has identi- determination of the hazard, the exposure of
fied some of the broad observed impacts of par- stakeholders to the hazard, and the relationship
ticular heatwaves upon various non- health areas, between the exposure/hazard and the impact that
demonstrating a need for indicators and indices will be observed.
better suited to these areas, alongside understand- Heatwave hazards are often defined using indi-
ing of what drives these adverse outcomes. ces which consider some combination of atmo-
As few attempts at evaluating and predicting spheric variables. These indices are quantitative
the effect of heatwaves on different non-health and allow for the comparison of different
sectors have been made, a primary objective of heatwave events. Relevant in the definition of
this research is to create a standardized approach indices are the atmospheric variables used to cre-
for determining these impacts and identifying ate the index. Examples of different heatwave
suitable indicators which can predict and quantify indices are presented later in this literature review.
these impacts. Validating such a framework The exposure of system components to a given
through case studies and the like will be neces- heatwave event is anticipated to be highly system
sary. Finally, a case for the release of data for and component dependent. An example of expo-
heatwave analysis from non-health sectors such sure may be that electrical infrastructure located
that required analysis may be undertaken will over urban green spaces is exposed to only 80% of
be made. a heatwave’s magnitude due to the cooling effect
The need for a structured framework approach of the land use, compared to electrical infrastruc-
is identified in the critical infrastructure and cli- ture located over roads, which is exposed to 100%
mate change review by Mikellidou et al. [9], of the hazard magnitude. It is anticipated that
which highlights that attempts to quantify impacts using geographical information system (GIS)
to date have failed to discuss interdependencies tools to log components and their properties
and resilience and often varied in analytical and (including exposure) will be beneficial in under-
methodological approach. Mikellidou et al. [9] standing heatwaves and their impacts from a spa-
and Hatvani-Kovacs et al. [10] call for an integra- tial perspective.
tive approach to climate change analysis to under- The hazard intensity and damage relationship
stand heatwave impacts. A need identified by is given in a functional form known as a vulnera-
Hatvani-Kovacs et al. [10] is the ability for pre- bility curve. Papathoma-Köhle et al. [14], for
dictive analysis of heatwave impacts such that example, consider vulnerability curves in the set-
scarce resources may be efficiently utilized. ting of alpine hazards such as landslides, ava-
One approach to natural disaster risk manage- lanches, and debris flow. It is anticipated that
ment, created by Van Delden et al. [11], is the expert stakeholder analysis from those familiar
Unified Natural Hazard Risk Mitigation Explor- with individual systems will be required for
atory Decision Support System (UNHaRMED). understanding the impacts of heatwaves. By
The UNHaRMED framework uses the risk trian- understanding the impacts of heatwaves, and
gle approach (hazard-exposure-vulnerability) to their drivers, it will be possible to identify which
determine the risk of natural hazards and is cur- indices will be most relevant to the impacts, and
rently in use for earthquakes, coastal inundation, how the impacts may change with changes in
Measuring Heatwaves and Their Impacts 457

heatwave events into the future, as characterized change the association of impacts to events
by the indices. [4]. Tong et al. [18] show that for only a small
Accounting for external drivers allows for the change in definition was able to have appreciable
exploration of a dynamic system which evolves impacts on the change in predicted health
over time, subject to drivers such as climate outcomes.
change, population changes, and land use man- Two common approaches to defining
agement. The incorporation of GIS tools allows heatwaves are established by Lee [4]:
for spatial variation in the measurement of risk,
where vulnerability, hazard, and exposure factors 1. Determine an absolute temperature which must
may vary with location. be exceeded over a set number of days.
Through the creation of a framework which 2. Determine a relative temperature which must
can determine a level of heatwave risk, it is stip- be exceeded over a set number of days.
ulated that an increased ability to understand and
implement risk mitigation strategies will be In defining the relative temperature, two
yielded. approaches are commonly used, either setting
Given this definition of risk, the following the limit as a percentile of historical temperatures
literature review seeks to cover the breadth of (i.e., 90th percentile) or as a threshold above a
indices used to define heatwave events and the qualitative definition of “normal” temperatures.
observed impact of the extreme temperature Extensions to the above approaches may
events and, where attempts have been made, sum- include incorporating (i) a shorter period of higher
marize progress in determining the relationship temperatures which must occur within the longer
between the events (indices) and their impacts. period, in some cases referred to as a multiple
Understanding current knowledge of impacts threshold index [16], (ii) overnight temperatures,
and indices will aid in developing a framework and/or (iii) shade temperatures.
for assessing the risk to various stakeholders asso- Considerable work has been undertaken to cre-
ciated with heatwave events and how this risk may ate an index which best captures heatwave
change with different future scenarios. impacts. Table 1 provides a summary of current
heatwave indices, the considerations made in the
calculation of each index, and whether the index
Heatwave Indices aims to capture a measure of the intensity of the
event. There are many indices and area-specific
Efforts have been made to define and measure thresholds adopted by different government bod-
heatwaves using a range of indices, with no con- ies; however, Table 1 looks to capture the breadth
sistent definition being used to evaluate these of unique measures, with preference to those cap-
events [15]. These indices were often created tured in literature. For the purposes of evaluating
such that the output of the index corresponds to intensity, temperature-adjusted or average temper-
the damage the heatwave would cause on a spe- ature measures are not considered as measuring
cific sector [16]. There is no standardized index intensity.
for the assessment of heatwave impacts on health Another distinction between indices is the out-
[17] or indeed for any sector. The complexity of put of the index. Indices are seen to provide a
industry-specific indices results in the loss of gen- binary yes/no classification of whether a heatwave
erality of such indices [16]. As the impact on has occurred; some indices (the EHF, EEHD, and
different sectors drives which atmospheric param- EEHN) go further and provide a measure of the
eters of heatwaves are most relevant, it is neces- intensity of the heatwave (typically by measuring
sary to use heatwave indices that best align with the level of the index above the defined threshold).
the sector being considered. The choice of defini- Many of the indices in Table 1 were created
tion, and by extension index, is not trivial, with with the intended application in health sectors;
the method of definition able to fundamentally Robinson [19] goes as far as to state that
458 Measuring Heatwaves and Their Impacts

Measuring Heatwaves and Their Impacts, Table 1 Index register, inputs, considerations and outputs of existing
heatwave indices
Max. Min. Relative Intensity
Index Description temperature temperature humidity Other output Reference
Excess heat Based on excess X X X Nairn and
factor (EHF) heat indices Fawcett [20]
(EHIs) –
minimum/max
temperature
average over
3 days
Excess heat Minimum/max X X Nairn et al.
index temp. Average [21]
acclimatization over 3 days, less
(EHI(accl.)) the mean
max/min temp
over the
preceding
30 days
Excess heat Min/max temp. X X Nairn et al.
index absolute Average over [21]
(EHI(sig.)) 3 days, less the
95th percentile
of this average
historically
Three-day The lowest X Scalley et al.
maximum maximum [22]
temperature temperature
(3DMT) over a three-day
period. NSW
and QLD in
Australia use
the 90th
percentile for
the specific date
as a threshold
Daily average Average of X Scalley et al.
temperature maximum and [22]
(DAT) minimum
temperature
over 1 day.
Victoria uses
this index with a
threshold
between 30  C
and 34  C
Three-day The DAT X X Scalley et al.
average with averaged over a [22]
activation three-day
temp. (3DAT) period.
A threshold of
32  C is applied
in South
Australia and
Western
Australia
(continued)
Measuring Heatwaves and Their Impacts 459

Measuring Heatwaves and Their Impacts, Table 1 (continued)


Max. Min. Relative Intensity
Index Description temperature temperature humidity Other output Reference
Heatwave The average X Fischer and
frequency heat wave Schär [23]
(HWF90) frequency,
where
heatwaves are
defined as
6 consecutive
days exceeding
the 90th
percentile of the
historical
control period
(1961–1990)
Heatwave The annual X Fischer and
number number of heat Schär [23]
(HWN90) waves, where
heatwaves are
defined as
6 consecutive
days exceeding
the 90th
percentile of the
historical
control period
(1961–1990)
Heatwave The X Fischer and
amplitude “amplitude” or Schär [23]
(HWA90) average peak
temperature of
the hottest
heatwave per
summer
Heatwave The average X Fischer and
Duration duration of the Schär [23]
(HWD90) longest
heatwave per
summer
Combined hot The average X Fischer and
days and number of days Schär [23]
tropical nights with both
(CHT) maximum
temperatures
exceeding 35  C
and minimum
temperature
exceeding 20  C
Apparent The average X X Steadman
temperature number of days [24],
(Ta_105F) with a Steadman
maximum [25]
humidity-
corrected
apparent
temperature
exceeding
(continued)
460 Measuring Heatwaves and Their Impacts

Measuring Heatwaves and Their Impacts, Table 1 (continued)


Max. Min. Relative Intensity
Index Description temperature temperature humidity Other output Reference
40.6  C
(105  F). Ta is
based on the
relationship
between
humidity and
temperature and
is based on
human heat
exchange. Also
referred to as the
heat index
Daytime high The heat index X X X Robinson
and nighttime (Ta) is expected [19]
low heat index to reach 40.6  C
(Ta max/min) with a minimum
temperature not
below 26.7  C
over a period of
at least 48 h
Heatwave The daily X Frich et al.
duration index maximum [26]
(HWDI) temperature of
more than
5 consecutive
days exceeds
the normal
average
maximum
temperature by
5  C, the normal
period being
1961–1990
Predicted mean Predicts the X X Fanger
vote (PMV) human thermal (1970) cited
comfort by Perkins
response to and
bioclimates in Alexander
terms of a [16]; Fanger
psychophysical [27]
scale
Physiological A measure for X X Mayer and
equivalent human thermal Höppe [28]
temperature comfort which
(PET) translates an
actual
bioclimate into
a relatable
indoor
environment in
which the same
thermal stress
would be
experienced
using human
(continued)
Measuring Heatwaves and Their Impacts 461

Measuring Heatwaves and Their Impacts, Table 1 (continued)


Max. Min. Relative Intensity
Index Description temperature temperature humidity Other output Reference
energy balance
models
TX90pct A maximum X Perkins et al.
temperature [8]
threshold based
on the 90th
percentile of
calendar day
temperatures
with a 15-day
window
TN90pct A minimum X Perkins et al.
temperature [8]
threshold based
on the 90th
percentile of
calendar day
temperatures
with a 15-day
window
Universal Predictor for X Lam et al.
thermal climate human thermal [29]
index (UTCI) comfort based
on air
temperature,
relative
humidity, wind
speed (at 10 m
above ground),
and mean
radiant
temperature
(which can be
derived from
globe
temperature)
HWD1/hot The daily X Hansen et al.
days maximum [30], Collins
temperature et al. [31]
above 35  C
(about top 1%)
for 3 or more
consecutive
days
Hot nights Nights with a X Collins et al.
minimum [31]
temperature
equal to, or
above, 20  C
Relatively Days with a X Collins et al.
warm days maximum [31]
temperature in
the upper 95th
percentile
(continued)
462 Measuring Heatwaves and Their Impacts

Measuring Heatwaves and Their Impacts, Table 1 (continued)


Max. Min. Relative Intensity
Index Description temperature temperature humidity Other output Reference
Relatively Nights with a X Collins et al.
warm nights minimum [31]
temperature in
the upper 95th
percentile
EHD/EHN The number of X X Trigo et al.
days/nights over [32]
a period where
the maximum/
minimum
temperature
exceeds the 95th
percentile level
for that measure
Multiple A lower X Meehl and
threshold index threshold T2 Tebaldi [33]
(here the 81st
percentile)
temperature
must span the
duration of the
heatwave event
and contain a
shorter period of
3 days in which
the daily
maximum
temperature
must exceed
threshold T1
(here 97.5th
percentile). The
average daily
maximum
temperature
must be above
T1 for the entire
period
EEHD/EEHN The sum of X X X Trigo et al.
(exceedance exceedance [32]
extreme hot degrees on days/
days/nights) nights over a
period where
the number
maximum/
minimum
temperature
exceeds the 95th
percentile level
for that measure
Measuring Heatwaves and Their Impacts 463

heatwaves cannot be defined without reference to status [42, 43], and those with pre-existing medical
the human condition. The relevance of these indi- conditions [37]. Heatwaves are identified to have
ces in non-health applications is of interest as exacerbated impacts on people suffering from men-
these indices are analyzed. tal health disorders [30]. The accessibility and
affordability of air conditioning in combatting
adverse heat-related health impacts are of particular
Heatwave Impacts importance [44]. During the 2003 heatwave in
Portugal, it was found that the use of air condition-
As highlighted, existing heatwave indices have ing systems in intensive care units led to a 40%
often been tailored to consider the vulnerabilities reduction of deaths, when compared to units which
of the individual sectors, such that realized did not have air conditioning systems (Instituto
heatwave impacts on different sectors are most Nacional de Saúde, cited in [32]). The concept of
accurately indicated by the appropriate index. In energy poverty with respect to being able to afford
order to inform the design of the risk management energy requirements is outlined and linked to
framework as well as provide insight into its health impacts during heatwaves due to air condi-
application, an understanding of the impacts of tioning affordability [42].
heatwaves upon different sectors should be Occupational health impacts of heatwaves are
developed. of economic consequence, where work-related
The impacts of heatwaves are recognized by ambulance call outs and compensation claims
many sector experts, as surveyed by Forzieri et al. increased during heatwave events [45, 46]. It is
[34], summarized in Table 2. The coverage of identified that the impact of delays and other
such impacts in literature lags the views expressed implications with regard to public transport
in Table 2, as shown in the subsequent sector- could greatly impact an individual who relies on
based analysis of the impacts of heatwaves. this service to fulfil activities that allow them to
Figure 1 demonstrates the range of sectors which have access to such necessities as critical medical
heatwaves impact, which are individually consid- assistance and medicine [47].
ered ahead (referred to as impact diagrams). These Figure 2 below describes the range of impacts
diagrams only incorporate impacts which are extreme heat events have on the health sector.
supported by a reference to literature. Note the external drivers affecting the observed
impacts, with some relating to heatwave impacts
Health Sector upon other sectors. These have been color coded
Excess mortality due to heatwaves, especially in depending on which sector the drivers stem from
vulnerable populations, is a well-identified impact and have corresponding dashed line arrows. This
of heatwaves [32, 35–38]. Between 1844 and 2010 highlights the interdependencies between differ-
extreme heat events were responsible for a higher ent heatwave-impacted sectors. Note, this color
death total than all other natural hazards combined coding scheme has been used throughout the
[36]. Long-duration, high-temperature events are review for all related impact diagrams.
seen to have the largest mortality effects [39]. Heat-
related deaths are seen to be increasing over time Built Environments
[35]. Heatwaves occurring earlier in the summer Within buildings and structures, heatwaves can
season were seen to cause greater impact than those cause stresses due to thermal expansion in con-
occurring later [39]. Despite taking such a focus in crete, steel, and insulated glass units. Problems
research, health impacts due to heatwaves often go with protective finishes have also been
undetected [40] or are underreported [4, 41]. reported [48].
A large number of demographics have been Thermal conditions indoors can be poorer than
identified as increasing vulnerability to heatwaves those outdoors during heatwaves [49], depending
including gender [32], age [32], socioeconomic on how heat resilience is considered in building
464 Measuring Heatwaves and Their Impacts

Measuring Heatwaves and Their Impacts, Table 2 Sector sensitivity to heatwaves. Sensitivity of different industries
to the impacts of heatwaves, as adapted from Forzieri et al. [34]
Sector No Low Medium
Energy Solar power plants Hydro power plants Coal power plants
Wind power plants Electricity distribution Gas power plants
Gas pipelines Electricity transmission Oil power plants
Nuclear power plants
Biomass power plants
Geothermal power plants
Transport Inland waterways Local roads
Ports National roads
Airports Motorways
Railways
Industry Metal industry
Mineral industry
Chemical industry
Refineries
Social Education Water and waste
Health Treatment

Measuring Heatwaves
EXTERNAL DRIVERS
and Their Impacts, ENERGY
Fig. 1 Impact diagram
overview. Impact of
heatwaves upon different
sectors HEALTH TRANSPORT
EXTREME
TEMPERATURE
EVENTS
BUILT AGRICULTURE
ENVIRONMENT

WATER ENVIRONMENT

design. Hatvani-Kovacs et al. [49] show that heat- literature [48, 51], leading to increased rates of
resistant design is discouraged by Australia’s mortality and heat-related illness [48]. It is noted
Nationwide Energy Rating Scheme, leading to that through the relationship between the built
an increased reliance on air conditioning than in environment and UHI is not always clear:
traditional buildings. Passive strategies for heat- reintroduction and irrigation of urban greenspaces
resistant design are recommended as an alterna- can reduce local temperatures [10]. Figure 3 dem-
tive to air conditioning reliance [43, 50]. onstrates the impacts of heatwaves upon the built
Poor-quality housing is identified as increasing environment, including a single external driver.
vulnerability of populations to heat-related mor-
tality, often tied to people from poor socioeco- Energy
nomic backgrounds [43]. Extreme temperatures impact electricity genera-
The creation of urban heat islands (UHI) in tion, transmission, distribution, and demand
dense cities due to the removal of urban green [52]. Heatwaves are a source of brownouts and
spaces has received some attention within blackouts (or failure) [52]. Power failures have
Measuring Heatwaves and Their Impacts 465

Measuring Heatwaves
and Their Impacts, Pre-existing
Fig. 2 Health impact Urban Heat Islands
(UHI) & Building Medical Conditions
diagram. Heatwave impacts
and interdependencies upon Design
the health sector Transport
Airconditioning Failure
Failure
HEALTH
Increased
Increased Morbidity
Mortality

Pressure on Occupational Health


Emergency & Safety (OH&S)
Services Losses

Measuring Heatwaves
and Their Impacts, Building
Fig. 3 Built environment
Code
impact diagram. Heatwave
impacts and
interdependencies upon the
built environment sector
BUILT
Increased ENVIRONMENT Urban Heat
Indoor Temp. Island (UHI)

Expansion
Stresses

been observed as a result of heatwaves in Chicago Various modes of renewable energy generation
[35], Melbourne [1], Southeastern Australia [2], are negatively affected by extreme heat events.
and others [53]. High nighttime temperatures also Solar power cells see lower efficiency under con-
increase the vulnerability of electricity transmis- ditions of increased temperature, with increases in
sion systems to failure, as systems cannot shed soil temperatures of solar PV power plants also
excess heat [2]. lowering capacity of underground conductors
Significant energy loss in transmission and [9]. Hydropower generation output is decreased
distribution systems result from heatwave events, due to increased evaporation in reservoirs, and
due to both higher conductor resistivity, higher snow-covered regions face reductions in output
ambient temperatures reducing the effectiveness due to reductions in stream flows [9].
of heat-dissipating transducers, and higher A report from the Grattan Institute [55] estab-
demand [53, 54]. Aivalioti [52] describes how lishes that distribution outages are more than three
network losses in distribution and transmission times as likely on days hotter than 35 degrees
systems increase by 1% for every increase of (an average daily outage per customer of approx-
3 degrees Celsius in ambient temperatures, in imately 2.6 min over the 2009–2018 period) as
systems with already existing losses of 8%. compared to days below 35 degrees (0.7 min per
466 Measuring Heatwaves and Their Impacts

Measuring Heatwaves
and Their Impacts, Peak
Fig. 4 Energy impact Demands
diagram. Heatwave impacts
and interdependencies upon
the energy sector

ENERGY
Power Decreased
Failure Efficiencies

Reduced Renewables
Generation

day per customer). Network sensitivities are which can lead to reduced skid resistance
caused by heat expansion causing wires to sag, [1]. This was seen to occur on major highways
transformer overheating, and an increased ten- in Victoria during the 2009 heatwave and typi-
dency of fuses to blow [55]. Heatwaves can result cally affects regional areas more than inner cities,
in peak demands [49], as observed by South where councils have the ability to invest in heat-
Australia and Victoria in 2009 when temperatures resistant roads [1]. Heatwaves during construction
drove electricity demand to reach record of roadways often result in moisture loss in con-
maximums [56] (Fig. 4). crete which leads to an increased chance of
cracking [53].
Tires are also susceptible to extreme heat
Transport
events. Expanding air increases tire pressure and
Transport infrastructure is reported to have been
therefore increases the chances of a tire blowing
negatively affected during the 2003 heatwaves in
out [53].
the United Kingdom [40]. Public transport is often
Impacts on the transport sector are often diffi-
affected to the point where the economic loss to a
cult to avoid. The trigger point for rail track buck-
city can be high, without changes to maintenance
ling is unknown and is believed to have multiple
regimes, Dobney et al. [57] estimated that during
and hard to measure variables such as how well
extreme summers, the loss due to transport delays
tracks have been maintained over the years [57,
alone could reach GBP 23 million. Public trans-
60]. Figure 5 describes the impacts (and identified
port infrastructure can be damaged in the long
external driver, dependent upon heatwave impacts
term due to heatwaves, and prolonged extreme
from a different sector) of heatwaves upon the
heat is an identified cause of both jointed and
transport sector.
continuously welded track buckling [58,
59]. The number of buckles and thus delays
expected per year are shown to increase without Agriculture
improvements [59]. Almost half of Melbourne’s Past heatwaves have seen significant damage to
trams are Comeng trains, in which air condition- the agriculture sector, more specifically within
ing units are not designed to operate above 34.5 both crops and livestock. Herold et al. [61]

degrees Celsius [2], although the role in this being reported that temperatures above 30 C for a single
the direct cause of train cancellations in the 2009 day have been shown to reduce grain develop-
event is of debate [2]. ment, as supported by the findings of Coumou
Roads and vehicles also show the effects of and Rahmstorf [62] who reported that record-
heatwaves. Case studies highlight “flushing” or breaking hot summers in Western Europe
“bleeding” as an impact of extreme heat on road- (in 2011) and Russia (in 2010) caused grain har-
ways (typically those with a sprayed sealing), vest losses of 12% and 30%, respectively. Further
Measuring Heatwaves and Their Impacts 467

Measuring Heatwaves
and Their Impacts, Power
Fig. 5 Transport impact Failure
diagram. Heatwave impacts
and interdependencies upon
the transport sector

TRANSPORT
Road
Rail Damage
Damage

Delays and Economic


Losses

Measuring Heatwaves
and Their Impacts, Reduced
Fig. 6 Agriculture impact Water
diagram. Heatwave impacts
and interdependencies upon
the agriculture sector

AGRICULTURE
Reduced Livestock
Harvest Deaths

impacts on crops include tree and vine damage, which can occur rapidly at particular thresholds
loss of yield, reduced quality of final products, for temperature, with extreme temperature events
and greater input requirements [60]. suggested to be drivers of ecological response by
While dry spells can be damaging in the short Parmesan et al. [64]. In the wild, species are often
term to many plant species, heat stress more able to adjust to temperature changes; however,
severely affects crops than dry spells in the short there is a tipping point at which species cannot
term. Warming and drying of soil in extreme heat adjust anymore, and species will begin to die
can adversely affect soil, and root damage can also [60]. Many examples of this can be seen in the
occur in warm soils [53]. wild, such as large losses to salmon populations in
When considering livestock, extreme heat Canada due to heat stroke [64]. Waterbodies
events have been observed to result in both live- exposed to heat can rise in temperature, leading
stock deaths and lower fertility rates [60]. Live- to anaerobic conditions at the bottom of the lake
stock also require increased inputs (such as floor and a drop in dissolved oxygen (DO). With-
water), and in the dairy industry, lower yields out adequate volumes of DO, fish respiration
have been observed during heatwaves [60]. decreases [53].
Figure 6 describes the impacts of heatwaves It is not just the deaths of wildlife that increase
upon the agriculture sector (with included external in heatwaves. Continued high temperatures may
driver, stemming from impacts upon another lead to poleward shifts in ecosystem distributions,
sector). constrained animal ranges, and altered gender dis-
tributions and physiological characteristics
Natural Environments [53]. According to Parmesan et al. [64], for
Easterling et al. [63] summarize a variety of dif- many reptile species, “an individual’s sex is deter-
ferent environmental and biological processes mined by the maximum temperature experienced
468 Measuring Heatwaves and Their Impacts

Measuring Heatwaves
and Their Impacts, Reduced
Fig. 7 Environment Water
impact diagram. Heatwave
impacts and
interdependencies upon the
environment sector
ENVIRONMENT
Water Broad Species
Quality Dependent Impacts

during a critical phase of embryonic develop- Application of Indices to Impact Analysis


ment.” The effect of heatwaves is often just a
further stress on an ecosystem, and the magnitude Understanding how impacts change with the
of the damage from a heatwave is related to how exposure of different systems to heatwave events
much stress a system is already under [60]. of different intensities is necessary such that the
Figure 7 describes the impacts of heatwaves risk of such systems degrading or becoming
upon the environment sector, with included driver compromised may be understood. For this rea-
related to heatwave impacts on a different sector. son, determining the functional relationship
between impacts and events (defined by indices)
is of interest. Table 3 provides a summary of
Water
various systems with corresponding indices
The Queensland University of Technology [2]
used and the threshold for each, along with
report finds that water usage increases during
dependency lags and key comments about the
heatwaves. Usage for Melbourne in 2009 was
measurement of heatwave impacts for each
usually between 900 and 1000 ML per day, but
system.
on days above 40  C, it often reached over
All air temperatures in Table 3 are measured at
1500 ML per day [2]. Environmental impacts of
2 m, and it is not documented within the QUT [2]
heatwaves are often unknown [60]; however, if
report how the heat stress response dependencies
ecosystems are damaged by heatwave events, this
were created.
is expected to reduce the quantity of water pro-
duced and increase costs of treatment [60]. Evap-
oration from reservoirs goes up during high Health Domains
temperatures in some reservoirs [2]. Jian et al. [17] demonstrate that the EHF is poten-
Links to other sectors can affect or are affected tially a useful indicator for studying the number of
by water supply. During Melbourne heatwaves in admittances to emergency departments. Trigo
2009, the Queensland University of Technology et al. [32] found that the exceedance extreme
[2] states that problems in water supply arise heat days index was more useful in predicting
when electric motors fail due to the heat or because health impacts than indices based on relative over-
they are indirectly compromised as a result of night temperatures and absolute maximum/mini-
power outages. If peak demands are not accurately mum temperature measures. Analysis by Scalley
forecasted, then a supply shortfall can occur et al. [22] found that the EHF was a better predic-
[60]. Despite some of these shortfalls, water infra- tor for health service utilization during heatwaves
structure is considered one of the most robust sec- when compared to a 3DMT and 3DAT indexes.
tors and is often most capable of functioning in Comparison of ten factors in Brisbane by Tong
high temperatures [2]. et al. [18] found no conclusive evidence as to the
Figure 9 refers to the impacts of heatwaves most appropriate heatwave definition for measur-
upon the water sector, with relevant driver stem- ing health impacts when comparing both relative
ming from impacts on the energy sector shown. and absolute heatwave indices.
Measuring Heatwaves and Their Impacts 469

For the apparent temperature index, several sector). The impact diagrams throughout this
accepted critical thresholds are defined (Granger literature review highlight the range of interde-
and Berechree, cited in [65]): pendencies between different systems, which
existing heatwave indices do not consider. Incor-
• Ta = 32 degrees Celsius and above: Cramps or porating this into the proposed framework is an
exhaustion objective of the proposed research, and using
• Ta = 41 degrees Celsius and above: Heat stroke this in practice would be a breakthrough in the
• Ta = 54 degrees Celsius and above: Heat stroke modeling and understanding of heatwaves – this
or brain hemorrhage very likely however will prove challenging. While Fig. 2
shows that the health sector is most impacted
The creation of the relationship between the by other sectors, this is likely a result of the
index value and the system response (impact) health sector being the predominant focus of
allows for the creation of the vulnerability curves existing heatwave research and not necessarily
which are then able to be used as an input into the an accurate depiction of the interdependencies
conceptual framework of risk assessment, as between sectors.
described in the introduction. Figure 9 reiterates the interdependencies
between heatwave impacts on different sectors
as highlighted by the previous impact diagrams,
Non-health Domains
on a more macroscopic scale. For example,
Currently, there is no proper framework to mea-
heatwave impacts on the energy sector have con-
sure the impacts of heatwaves on most non-health
sequent negative outcomes on the transport,
domains using heatwave indices. Within Table 3,
health, and water sectors, with these impacts
there are temperature thresholds for certain non-
being explicitly named in Figs. 2, 5, and 8.
health domains. Electricity demand, energy trans-
Application of the proposed framework
mission, and transport infrastructure have all been
requires the identification of system components
given threshold limits. Very little literature has
at risk. This will require expert input, from the
been found which applies indices to the study of
relevant sector – for example, the question of
heatwave impacts.
which aspects of temperature are most relevant
to causing failure of distribution systems could
Analysis only be answered by an individual with technical
Apparent in literature but not explicitly expertise in this area. An exploration of some of
highlighted is the interdependencies between these relevant parameters and system components
different sectors – for example, heatwaves caus- as available in existing literature has occurred
ing blackouts (affecting the electricity sector) throughout this review, but the broader applica-
can lead to air conditioning failures, leading to tion of the framework would likely require spe-
higher mortality and morbidity (within the health cialized consultation with experts.

Measuring Heatwaves
and Their Impacts, Power
Fig. 8 Water impact
Failure
diagram. Heatwave impacts
and interdependencies upon
the water sector

WATER
Supply Reduced
Shortfall Water
470 Measuring Heatwaves and Their Impacts

Availability of specific system data is reported and mainstream media appear to be underrepre-
as a barrier in a number of different fields for the sented in the literature, as demonstrated by
prediction of heatwave impacts: rail [57], energy Fig. 10. In this figure, 100% represents the num-
[54], and predictably others (Fig. 9). ber of results which are returned in each search
engine when the term “heatwave” is searched. The
Impacts disconnect between both media (Fig. 10) and
The impact of heatwaves on health has been thor- industry (Table 2) concerns and the focus of liter-
oughly discussed in literature; however, there is a ature (predominately on health impacts) suggests
significant lag between the desire for understand- that there is a requirement for literature to catch up
ing of the impact heatwaves have on non-health in many sectors. The impact of heatwaves on
sectors and existing literature explaining and mea- water demand, for example, is identified as an
suring this impact. area where little to no research has been under-
Many impacts of heatwaves, including impacts taken [10], despite water-sensitive design being
on power and road condition, are documented in identified as a key consideration for adaption to
“gray” literature (such as government reports), climate change [66]. While there is an abundance

Measuring Heatwaves
and Their Impacts, ENERGY
Fig. 9 Heatwave impact
interconnections.
Interconnectivity of
heatwave impacts across HEALTH TRANSPORT
different sectors as
observed in literature

BUILT AGRICULTURE
ENVIRONMENT

WATER ENVIRONMENT

Measuring Heatwaves and Their Impacts, Table 3 Heatwave index response relationship. Responses between a
system and heatwave index as adapted from Queensland University of Technology (QUT) [2]
Index and Dependency,
System threshold ( C) lags Comments
Human mortality DAT: 30 Linear, Threshold varies with location, nonlinear for severe
1–3 days episodes
Mental disorders 3DAT: 28–30 Quadratic, Variable between disorders and medication
1–3 days
Electricity DAT: 25 Quadratic, Variable between load and house types
demand 0–3 days
Energy HWD1: 40 Complex Basslink has different thresholds for Victorian and
transmission Tasmanian ends of link
Transport HWD1: 35 Unknown Different for buckling and discomfort
infrastructure Speed restrictions for UK train transport are enforced
from 36  C [59]
Tourism demand 3DAT: 35 Unknown Other weather factors important
Air quality HWD1: 28–30 Exponential Dependent on presence of hydrocarbons and moisture
(smog)
Measuring Heatwaves and Their Impacts 471

of knowledge about the effect of heat on the non-health domain areas lack indices to effec-
natural environment, there is little knowledge tively predict negative impacts and their severity.
about the effect of heatwaves [53, 60]. That is, Furthermore, some sectors lack understanding as
the effect of sustained periods, and different inten- even to which heatwave-associated atmospheric
sities, of heat on the natural environment is pre- parameters drive adverse outcomes on non-health
dominantly unknown. A symptom of the current domains.
health-orientated focus of heatwaves is that Existing literature shows a desire to understand
impacts of heatwaves and heatwave risk mitiga- and predict these outcomes, with case studies on
tion are formally dealt at an institutional level the 2008 and 2009 heatwaves across major south-
through health services in London [67]. eastern cities in Australia exploring the impacts of
Figure 10 also raises the issue of source reli- these events upon the transport sector (roads and
ability. In order to holistically consider all the railways) and electrical sector [2].
impacts of heatwaves, it is often necessary to
draw upon “gray” literature to explore impacts Indices
which formal literature does not. While these Disagreement exists between the existing indices as
sources can provide valuable information, the to what atmospheric variables should be considered.
credibility as well as quality of the information Of the 30 observed indices, 22 take consideration of
can come into question – for example, Table 3 as maximum temperature, 12 consider minimum tem-
adapted from [2] provides little explanation as to perature, 4 consider relative humidity, and 3 consider
the origin of the dependency/lags between differ- other variables (including wind speed and radia-
ent systems and their heat stress responses, tion). There are only three indices which transform
whereas the impacts and drivers upon human temperature-based metrics into an intensity measure
health are well documented from a range of dif- (the EHF, EEHD, and EEHN).
ferent peer reviewed and credible sources. Many indices rely on the determination of a
While significant efforts have been made temperature threshold, often determined as a
to determine the characteristics of a heatwave given percentile (e.g., the 90th percentile) of his-
that drive adverse human health effects (often torical recorded temperatures for a given region.
capturing these effects through indices), other The use of a historical measure of temperature

80%
Percentage of Searchs with Keyword

70%

60%
Google Web of Science
50%

40%

30%

20%

10%

0%
Health Infrastructure Road Building Power Rail
Key Word searched with "Heatwave" in Database

Measuring Heatwaves and Their Impacts, Fig. 10 Literature coverage of different sectors. Percentage of search
results containing “heatwave” and an additional keyword
472 Measuring Heatwaves and Their Impacts

carries merit where the index is applied to health in which heatwave analysis must be undertaken,
sectors, as the human physiology has evolved to leads to the admission that there is likely no “ulti-
cope with this historical temperature. However, mate” index which is globally applicable for the
when applied to other sectors, such as infrastruc- assessment of heatwave impacts. As an alterna-
ture, a historical measure may be less meaningful tive, it is suggested that a “toolbox” of indices is
such as when considering material properties, for created, with the indices which have been verified
example. for individual sectors noted. The use of different
Indices based on absolute thresholds are iden- hazard-characterizing variables (here indices) for
tified as being not suitable in some regions [16]; the creation of vulnerability curves was coherent
however, absolute thresholds are sometimes nec- with the analysis of natural disaster risk in the
essary when considering the impacts of heatwaves alpine setting presented by Papathoma-Köhle
[16] and can be easier for policy makers and the et al. [14].
general public to interpret [31]. Some indices Considerations must be made for the availabil-
focus on summer season thresholds (such as the ity and practicality of heatwave indices which rely
HWA90), annual thresholds (such as the EHF and on specific data (such as the PMV or PET)
HWN90) (as discussed in Perkins and Alexander [16]. Apparent temperature is identified as one
[16]), or calendar-based thresholds (TX90pct) to index which balances data requirements and spec-
account for heatwaves occurring at different ificity of index results well [16].
times. Existing research has not discussed the It is important to be aware that caution needs to
benefits or drawbacks of the application of these be taken when analyzing return periods for stud-
different classes of thresholds to the performance ied heatwaves. Due to the complexity of the
of the indices. nature in which heatwaves propagate, estimates
A suggested reason for the difference between in the form of “1 in N year” events may assume
the findings on the impact of heatwaves on human climate and urban structure stationarity while also
health may be due to the selection of indices failing to miss vital heatwave drivers [2].
chosen to study the impacts. EEHD and EHF
indices used by Trigo et al. [32] and Scalley
et al. [22], respectively, measure the intensity of Future Directions
the heatwave events, as compared to those used by
Tong et al. [18], which only determine tempera- The occurrence of heatwaves is of concern to a
tures on days are, or are not, “heatwave” days. It is wide range of sectors. Significant research has
stipulated that the intensity then of heatwave been undertaken in studying the impacts of
events is important and not just the heatwave/not heatwaves on health. In accordance with this,
heatwave condition. This comparison highlights many indices which have been developed to mea-
the complexity and importance of selecting an sure heatwaves are, directly or indirectly, centered
appropriate heatwave index. around the human condition. As heatwaves
Karl and Knight [68] identify that while urban- worsen in duration and severity, impacts will
ization tends to increase temperature, it also tends increasingly be felt in non-health domains, such
to decrease moisture supply and thus possibly as infrastructure and electricity. The applicability
reducing Ta (a humidity-adjusted temperature of existing heatwave indices in monitoring and
measure), shown in Table 1. This reflects the predicting impacts on these sectors is of question,
complexity in selecting indices and incorporating and developing a standardized approach to evalu-
required information when evaluating heatwave ating heatwave impacts is vital for planning and
impacts in a changing environment. responding to future extreme temperature events.
Perkins and Alexander [16] acknowledge the In addition to the application of heatwave indi-
inability of many (or all) indices to capture the ces to non-health domains (whether through cre-
range of heatwave characteristics and attributes ation of new indices or modification/application
properly. This, paired with the diversity of sectors of existing ones), the creation of a standardized
Measuring Heatwaves and Their Impacts 473

framework and index “toolbox” for the evaluation 11. Van Delden H, Riddell GA, Vanhout R, Maier HR,
and prediction of heatwave impacts across sectors Newman JP, Zecchin AC, Dandy G (2019)
UNHaRMED framework report: a co-creation
would provide structure to the assessment of approach for the development and use of decision
heatwave impacts on many non-health domains. support systems for disaster risk reduction. Bushfire
Such a framework could be universally applied to and natural hazards CRC, Melbourne
heatwave-affected sectors. 12. Wilhelmi OV, Hayden MH (2010) Connecting people
and place: a new framework for reducing urban vul-
Useful outputs from the framework may include nerability to extreme heat. Environ Res Lett 5:1–7
risk mapping of vulnerable infrastructure/compo- 13. Filosa G, Plovnick A, Stahl L, Miller R, Pickrell
nents of industry sector systems; estimated average D (2017) Vulnerability assessment and adaptation
return periods for impacts; and economic cost eval- framework, 3rd edn. Federal Highway Administra-
tion: Office of Planning, Environment & Realty,
uation under different scenarios.
Washington, DC, pp 1–86
14. Papathoma-Köhle M, Kappes M, Keiler M, Glade
T (2011) Physical vulnerability assessment for alpine
hazards: state of the art and future needs. Nat Hazards
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By-Product By-products are formed in emissions
Industrial Emissions Control control processes due to incomplete mineraliza-
Technologies: Introduction tion. Ideally, pollution is completely broken
down or trapped; often this is not the case.
Szymon Kwiatkowski1, Merve Polat1, Weijia Yu1 Contact Time The contact time t is a crucial
and Matthew Stanley Johnson1,2 metric in characterizing a pollution control
1
Department of Chemistry, University of system, aiding design and allowing compari-
Copenhagen, Copenhagen, Denmark son between different systems. It is the ratio
2
Airlabs, Copenhagen, Denmark between the length of the treatment system l,
for example, the contact region of a scrubber,
catalyst, or adsorbent, and the velocity of air
Article Outline flow v. In all, t ¼ l=v. The treatment system can
be described using a first-order removal rate k,
Glossary linking the pollution’s input and output con-
Definition centrations Cout and Cin [2]:Cout = Cin  ekt
Introduction Energy Intensity The energy intensity in the pol-
Chemical Description of Pollution lution control system can be described using the
Economic Analysis specific energy input (energy input per mass of
Filtration, Thermal Oxidation, Electrostatic air, e.g., J/kg) or the volumetric energy input,
Precipitator, and Cyclone also called the energy density (e.g., J/m3).
Heterogeneous Catalysis Explosion Limits and Range A mixture of a
Scrubbers given combustible compound in the air is typ-
Gas Phase Advanced Oxidation and Vapor ically explosive over a range extending from
Recovery the lower explosion limit to the upper explo-
Green Chemistry sion limit [3]. The limits are given in %(v/v).
Conclusion and Future Prospects The lower limit is the concentration below
Literature which flame cannot spread and vapor doesn’t
ignite from a spark. The upper limit is the
Glossary concentration above which a flame does not
spread. For example, the explosion range
Aerosol Aerosols are suspensions of solid or liquid for ammonia is 15–28% [3]; for methane,
particles in a gas and occur when mixing from 5–15% [3]; for benzene, 1.2–7.8% [3]; and
diffusion and circulation is more rapid than grav- for formaldehyde, 7.0–73% [4].
itational settling. In common usage, “aerosol” Exposure Limit The exposure limit describes
can refer to the particulate matter. Atmospheric the legally allowable average concentration a
particulate matter can be emitted directly (“pri- human can be exposed to for a given period. It
mary aerosol”) or formed in the atmosphere by can be expressed as an 8-hour time-weighted
gas-to-particle conversion processes (“secondary average or a yearly average. Exposure limits
aerosol”). Atmospheric aerosol particles range in assure workers health and safety in different
size from a few nanometers (nm) to tens of fields of employment.
micrometers (mm) in diameter [1]. Externality An externality is a cost or benefit
imposed on a third party unrelated to those
who buy and sell [5]. Positive or negative
Szymon Kwiatkowski and Merve Polat contributed effects on the third party are called positive
equally to the article. and negative externalities, respectively [6]. For
© Springer Science+Business Media, LLC, part of Springer Nature 2021 477
M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7_1083
Originally published in
R. A. Meyers (ed.), Encyclopedia of Sustainability Science and Technology, © Springer Science+Business Media, LLC,
part of Springer Nature 2019, https://doi.org/10.1007/978-1-4939-2493-6_1083-1
478 Industrial Emissions Control Technologies: Introduction

example, if one party buys a tree and plants it, changing the manufacturing process or by modi-
the buyer and seller benefit, and others may also fying the product itself. Pollution control tech-
benefit from the shade and fruit. Or, if one party niques focus on destroying or trapping pollution.
buys a leaf blower with a polluting two-stroke While pollution has been a problem since the
engine, buyer and seller benefit, but others may beginning of human civilization, the modern
be impacted by air pollution and noise. trends of industrialization, population growth,
Global Warming Potential (GWP) The global and urbanization have meant exponential increase
warming potential is a metric that allows direct in both pollution production and exposure. As a
comparison of many different climate forcing consequence a great deal of effort is directed
agents. The GWP represents the amount of toward decoupling economic growth from envi-
heat trapped in the atmosphere by a kilogram ronmental degradation using green solutions and
of the compound of interest relative to the heat more efficient technologies for pollution control.
trapped by a kilogram of CO2. Heat-trapping is A diversity of new techniques have been devel-
determined by integrating the radiative forcing oped, and traditional methods have been refined
over a defined time period called the time hori- and improved. This entry gives an overview of
zon [7]. For example, the global warming many of the current emission control technolo-
potential for methane is 72 over a 20-year gies, describing the advantages of different con-
time horizon [8]. trol systems and their efficiency in pollution
Green Chemistry Green chemistry is a pollu- removal and their utility in various applications.
tion prevention method that focuses on red- It will investigate the economic and regulatory
ucing the use and production of hazardous structure of emissions control and explore its use
substances. in achieving the United Nations’ Sustainable
Pollution Pollution is any substance introduced Development Goals.
into the environment that has harmful effects.
Removal Efficiency The removal efficiency (RE
%) is a measure of a pollution control system. It Introduction
is determined for a specific component based
on its concentration at the inlet (Cin) and outlet Industrial pollution is linked to the industrial rev-
 
(Cout) [2]. RE% ¼ 1  CCout  100. Note that olution that brought together the combined forces
in
of population growth, increased population den-
the removal efficiency, by definition, does not sity and industrial activity. The mass production
consider the formation of by-products. of commodities and goods by industry required
Pressure Drop Pressure drop is a difference in energy obtained from fuel [7]. Fossil fuel (starting
pressure between two defined points [2]. with coal) was mined at an unprecedented scale,
Dp = p2  p1. For example, there will be for heating and power and as a reducing agent.
a pressure drop across any system that resists The engines which powered machines and the
air flow. machines themselves were now being built from
metal, driving the growth of mining and refining
[10]. While the industrial revolution contributed
Definition significantly to industrial pollution, pollution
began thousands of years earlier in the Stone
The aim of industrial emissions control is to pro- Age, where the first cases of dust pollution in
tect human health and minimize environmental humans have been identified. People making
impact by reducing air pollution from industrial stone tools or carving flint from limestone may
emissions. Techniques are traditionally divided have already suffered from silicosis. Further,
into pollution prevention and end-of-pipe control. hominids living 200,000 years ago have been
Pollution prevention focuses on minimizing the discovered with lead poisoning, which may have
possible emissions at the source by modifying or been caused by drinking contaminated water
Industrial Emissions Control Technologies: Introduction 479

[11]. The first known case of metal pollution on a technologies [18]. This entry will introduce indus-
global scale occurred about 2000 years ago during trial air pollution and its impact on the environ-
the Golden Age of Roman civilization. Analysis ment and human health. We will present pollution
of Greenland ice cores showed significant control technologies currently used by industry
increases in atmospheric lead concentrations and discuss their application, efficiency, and
long before the industrial revolution. The Romans advantages. We will also discuss environmental
processed 80,000 tons of lead annually, a rate that policies and regulation of the industrial sector as
would not be reached again until the eighteenth well as the economy of air pollution control and
century. The lead was used for making water pipes its current and future state.
and lining baths and for pots and dishes. The
inefficient smelting process used at the time led
to the emission of around 5% of the annual pro- Chemical Description of Pollution
duction into the atmosphere [12]. A similar phe-
nomenon has been observed for copper at the time We will divide pollution into four classes
when metal coins spread across the Ancient Med- depending on shared physical and chemical prop-
iterranean. Due to the primitive smelting technol- erties, atmospheric sources, and transformations.
ogies, around 15% of all processed copper ended Reduced compounds typically have a biological
up in the air, peaking 2000 years ago with the origin in reduced material produced by photosyn-
astonishing total of 2300 tons released in the thesis, including fossil material used as fuel.
atmosphere annually [13]. More recently, soot Reduced compounds as pollution therefore often
from combustion was seen to impact evolution. result from industrial processes using hydrocar-
Before the industrial revolution, the number of bons, for example, natural gas leaks, solvent and
black and white moths in Europe was similar; fuel evaporation, and biomass. Oxidized com-
however, at some point, the population of white pounds are typically produced by combustion
moths declined significantly. Bernard Kettlewell and may be water-soluble acids. Moreover, the
at the University of Oxford theorized that black particulate material in aerosols may derive from
moths blended more easily with their surround- primary emissions, or it may form from oxidation
ings allowing them to escape predation, because products produced within the atmosphere. Finally,
of widespread pollution and soot. The increase in industrial processes emit refractory elements and
black moths is an example of one way that pollu- compounds such as airborne heavy metals associ-
tion from industry has affected the world we live ated with particulate matter. Despite their low
in [14]. Unfortunately, despite ongoing advances concentrations, they can contribute significantly
in technology and a general rise in human knowl- to environmental degradation and affect human
edge, industrial pollution remains a serious prob- health. We will describe particulate matter, oxi-
lem for mankind and the Earth’s environment. dized compounds, reduced compounds, second-
Studies show air pollution increases the risk of ary organic aerosol, and heavy metals in more
pulmonary disease and cardiovascular disease and detail in the following sections.
decreases quality of life and productivity during
working hours [15, 16]. It increases medical costs Particulate Matter
and cuts life expectancy [17]. Moreover, the Particulate matter (PM) is a pollutant consisting of
industrial sector is one of the largest contributors a mixture of solid and liquid particles of inorganic
to air pollution. However, recent European studies and organic substances suspended in the air
have shown decoupling of industrial production [22]. PM is often divided into PM10 and PM2.5.
from emission of pollution. Industrial emissions PM10 is the total mass of aerosol particles with a
have significantly decreased since 2000, whereas diameter of 10 mm or less, and PM2.5 has a diam-
production has remained steady. This can be eter of 2.5 mm or less. The different sizes have a
attributed to EU legislation and regulation in the diverse impact on health, for example, PM10 is
areas of emission limits and pollution control filtered by the upper respiratory tract, while PM2.5
480 Industrial Emissions Control Technologies: Introduction

can deposit deep in the lungs, introducing foreign and thereby increasing the CO2 concentration in
materials into the bloodstream [22]. Coarse parti- the atmosphere [49].
cles (diameter > 2.5 mm) are formed predomi- NO2 is a pollutant that is a catalyst for the
nantly by weathering of Earth’s crust, dust from formation of photochemical smog and a precursor
industry and roads such as tire wear or dust from of acid rain. Its emission is mostly due to vehicle
vehicle breaks. Fine particles are mainly the prod- exhaust with additional contributions from indus-
ucts of combustion and aerosols nucleation. In the trial facilities such as metal refining, food pro-
EU, the industrial sector is responsible for 17% of cessing, etc.[50]. NO2 is a toxic component of
all emitted PM2.5 [17]. Industrial processes are the urban air.
main source of PM in China followed by station- SO2 can react with other compounds and form
ary combustion involving the power industry, sulfuric acid and sulfate particles. The source of
industry, and residential. The industrial processes the gas is mainly from burning fuel with high
include metallurgical, mineral, and chemical sulfur content (e.g., the shipping industry). Coal
industries and comprise over half of PM emis- naturally contains sulfur. Burning coal for indus-
sions, often due to coal. The production of coal, trial processes leads to SOx formation, which can
coke, sinter, pig iron, steel, cement, brick, lime, further react with atmospheric water and oxygen
etc. also contribute to PM emissions [21]. resulting in acid rain [31].

Oxidized Compounds
The most relevant oxidized compounds emitted Reduced Compounds
from industrial processes are carbon dioxide, sul- The main reduced compounds are ammonia and
fur dioxide, and nitrogen dioxide. volatile organic compounds (VOC). Methane is
The CO2 concentration in the air is 410 ppm also a VOC, but it is often considered separately
[47]. The atmospheric lifetime of CO2 is uncertain from “non-methane VOC” or NMVOC, because
due to the complexity of the reservoirs of CO2 in of its low reactivity and long atmospheric lifetime.
the earth system [48]. For example, there are large The mean concentration of methane in the atmo-
fluxes of CO2 into and out of the ocean with sphere is 1835 ppb, and the exposure limit is
uptake limited ultimately by mixing of water 1000 ppm for 8 hours. Methane is GHG with a
into the deep ocean. Similarly, there is an annual radiative forcing of 0.97 W/m2 and GWP of 72
flux of CO2 into and out of photosynthetic plants over a 20 year time horizon. The main industrial
with complicated long-term storage in, e.g., tree sources of methane are fossil fuel extraction, agri-
trunks and soil [48]. CO2 is a greenhouse gas culture and waste, incomplete biomass burning,
(GHG), and the contribution of a GHG to GWP and man-made wetlands [8].
depends on radiative forcing. CO2 contributes to Benzene is one example of a NMVOC. It is a
global warming with a radiant forcing of 1.67 W/ carcinogen, mainly emitted from burning coal and
m2 [1]. The main source of CO2 is fossil fuel oil and from motor vehicle exhaust. The mean
combustion including coal, natural gas, and oil; concentration in the EU ranges from 0.5 to
cement production and land use change are addi- 1.3 ppb, but since it’s a toxic substance, there is
tional factors. The industrial sector includes no safe level of exposure recommended by the
manufacturing, construction, mining, agriculture, World Health Organization (WHO) [41, 44].
etc. Heat from coal burning is needed in industries Another VOC is formaldehyde, which can be
such as the cement industry, which uses heat for found at highly variable concentrations in the
cement production. It is also used to produce iron, order of 100 ppb in the atmosphere. A primary
steel, chemicals, and petrochemical products. The natural source of formaldehyde is biomass burn-
natural sinks for CO2 are photosynthesis and sol- ing; a lot of secondary formaldehyde is produced
vation in the ocean, but deforestation, land use, by the photochemical oxidation of other VOCs in
and increasing urbanization reduce the natural the atmosphere. Industrial sources of formalde-
green areas limiting the natural sinks for CO2 hyde include chemical manufacturing plants,
Industrial Emissions Control Technologies: Introduction 481

pulp and paper mills, forestry product plants, coal metals are usually present in ambient air at low
processing plants, and the metal industry [42, 44]. levels, their deposition in soils and water leads to a
Ammonia is another atmospheric reduced gas, buildup in the environment. Due to their proper-
and like VOCs its ultimate source can be biolog- ties, heavy metals are very persistent and are not
ical; in addition, large amounts are made in the easily bound or deactivated in the environment.
Haber-Bosch process for use as fertilizer. Ammo- This, combined with their toxicity, can result in
nia is the most common reduced nitrogen species serious adverse health effect even at low concen-
in the air. Ammonia is a corrosive and poisonous tration exposures [55]. Many heavy metals are
gas and is mainly emitted from agriculture accumulated in soils and taken up by plants.
[51]. It’s emitted from manure storage, slurry Some of them can be transferred from one organ-
spreading, and the use of fertilizers. It is a major ism to the other and biomagnified in animals at the
contributor to fixed nitrogen in the environment. top of the food chain. Oral exposure is the main
NH3 deposits in soil, in water, and on vegetation. route for human exposure to heavy metals. Inges-
In excess, nutrient nitrogen can lead to eutrophi- tion of contaminated food and water, in compari-
cation causing severe damage to the aquatic and son with rather low concentrations of heavy
terrestrial environments. It can also decrease the metals in the ambient air, typically has much
pH level of soil and water resulting in acidification more severe adverse effects. Even small emissions
and biodiversity loss [18]. Moreover, recent stud- of heavy metals into atmosphere result in their
ies show that ammonia contributes significantly to deposition into soil. Uptake by plants leads to
the production of regional particulate matter by contamination of the food chain. Therefore, it is
reacting with airborne acids, yielding particle crucial to control atmospheric emissions in order
nuclei [52, 53]. to decrease deposition and reduce heavy metal
intake by humans [18]. The assessment of metal
Secondary Organic Aerosols (SOAs) and metalloid compounds in ambient air is com-
VOCs are important precursors of secondary plicated due to different properties of existing
organic aerosols. In a study [54] in Beijing, con- species and their reactivity, toxicity, and carcino-
tinuous hourly measurements of VOC were genic potential. Hence a good understanding of
conducted to investigate the SOA formation different species and their sources is crucial for
potential and the factors contributing to VOC proper evaluation of adverse health effects.
during hazy episodes. Photochemical oxidation The compounds can be characterized using
of VOC fuel, catalyzed by HOx and NOx radicals, parameters such as water solubility, particle size
produces SOA and ozone in the troposphere distribution, specific surface area, etc. The param-
[7]. During the hazy events, the concentration of eters will play an important role in their toxicity
VOCs was elevated providing both correlation and bioavailability [55]. Metal in ambient air is
and mechanism. Aromatic compounds were encountered mainly as a component of particulate
found to be the dominant contributor to the SOA matter. EU air quality standards measure heavy
formation potential followed by alkenes and metals according to their concentration in PM10.
alkanes. The source profile showed that the sec- However, due to its relatively larger surface area
ond highest VOC emissions came from industry. and its longevity in the atmosphere, fine PM can
In conclusion, the photochemical reactions of have a larger effect on the health impact [56]. Fur-
VOC are the main reason for hazy events due to thermore, fine particles are transported much far-
the production of SOA and ozone by the reactions ther in the atmosphere and affect even the most
of aromatic compounds with OH radicals. remote regions, in contrast to coarse particles
which due to their mass are usually deposited
Heavy Metals near the source. The size of a particle will also
Heavy metals are common air pollutants, and their determine its deposition in living organisms and
long-range transport has a great impact on the how deeply can they penetrate the respiratory
ecosystem and human health. Although heavy system and which organs are affected [55].
482 Industrial Emissions Control Technologies: Introduction

Some of the heavy metals regulated by the well as iron and steel production. Lead in the
EU air quality standards will be described below. atmosphere is bound to a fine particular matter
The main arsenic sources in nature are ore which tends to be associated with long-range
deposits and volcanic activity. Anthropogenic transport. This can explain the presence of lead
emissions come mainly from metal smelters and in polar regions [46]. Atmospheric lead levels in
fuel combustion [56]. Europe have decreased significantly during the
Arsenic is mainly deposited on fine particles last few decades. Airborne lead is currently a
(PM2.5). It can be associated with various long- minor exposure pathway; however, before it was
term effects in humans including irritation of the banned from petrol, transportation was a major
respiratory system, cardiovascular disease, and source of lead exposure, especially in heavy traffic
neurological effects, especially for occupational areas. Long-term exposure to lead decreases cog-
exposure, e.g., smelter workers [57]. nitive performance in both adults and children and
Cadmium occurs predominantly in association leads to anemia, increase in blood pressure, and
with sulfide and zinc ores. It is released naturally reduced fertility in males. Infants and young chil-
into the atmosphere by volcanic eruptions, forest dren are especially sensitive to even a low level of
fires, and vegetation. Additionally, it is emitted as lead, which may result in a decrease in IQ and
a by-product of zinc, lead, and copper production behavioral problems [60].
process as well as the combustion of fossil fuels.
Furthermore, cigarette smoke is an important cad-
mium source [55]. The majority of produced cad- Economic Analysis
mium was used in the past for Ni-Cd battery
production, but recently they have largely been Economics and Policies
replaced by Li-ion and Ni-MH (nickel-metal Industry is a pillar of the world economy. It trans-
hydride) batteries. Cadmium can be found pre- forms raw materials into consumer goods and is a
dominantly in fine particles and hence has a pre- driving force for the economy of both low- and
disposition for long-range transport. Chronic high-income countries. From 2000 to 2013, the
exposure to cadmium can result in osteoporosis world average value added from manufacturing
as a consequence of changes in calcium metabo- (VAM) decreased from 19.2% to 16.3%. This
lism and airway diseases [58]. Cadmium is also trend is attributed to the shift in the world’s econ-
accumulated in the human body, especially in the omy from the industrial sector to more service-
kidneys, leading to kidney damage [55]. oriented sectors and the so-called information
Natural emissions sources of nickel include economy. However, CO2 emissions didn’t follow
soils, vegetation, forest fires, and volcanic activ- the trend of VAM; on the contrary, they are
ity. Man-made emissions consist mainly of com- increasing [61].
bustion, metallurgy, and nickel primary The relationship between economic growth
production (mining, grinding, smelting). Nickel and environmental degradation has been studied
often shows a significant association with coarse for many years and is strongly debated. The envi-
particles, and up to 30% of total nickel emission ronmental Kuznets curve (EKC) hypothesis was
can be found near its source. Data on chronic Ni introduced as an attempt to describe the relation-
exposure in humans is rather scarce and involves ship between environmental pressure (e.g., air
predominantly dermal exposure and allergic reac- pollution) and economic growth (income per
tions [55]. However, recent studies find an asso- capita). The hypothesis assumes an inverse
ciation between cardiopulmonary diseases and U curve relationship between the two variables
PM-deposited nickel species [59]. divided into three phases, distinguished by differ-
Lead is released into the atmosphere by natural ent growth levels of the economies (Fig. 1). In the
processes including volcanic eruption, forest fires, first phase, low CO2 emissions per capita are
and biogenic sources. Anthropogenic emissions related to low levels of industrial activity. How-
are related mainly to fossil fuel combustion as ever, rapid development and extensive production
Industrial Emissions Control Technologies: Introduction 483

Industrial Emissions
Control Technologies:
Introduction,
Fig. 1 Environmental
Kuznets curve

result in the acceleration of environmental pres- are typically easier to quantify than environmental
sure (CO2 emissions) at still relatively low income impacts. Hence the cost-effectiveness of regula-
levels. Increasing GDP shifts the economy from tions is often the subject of criticism [61]. More-
agriculture to industry resulting in an increase in over, restrictive standards in pollution control may
pollution. At this point, the increase in environ- cause regressive income distributions [64].
mental pressure is less than the increase in GDP The main idea of pollution taxes, another pol-
until it reaches a turning point that defines the end lution control policy, is to make pollution expen-
of the second phase. The third phase starts at the sive and thus shift the initiative for pollution
extremum and decreases with increasing income. control from regulators to factory owners
This shift is attributed to a behavioral change in [64]. Emission taxes are very efficient from an
which society sees benefits in the cleaner environ- economic point of view. The regulator can achieve
ment and is willing to pay for environmentally the desired level of air quality by setting emission
friendly products [61]. The turning point of EKC taxes at an appropriate level. Companies will
(the point between second and third phase) has reduce their emissions to avoid the tax, but con-
been estimated by different studies to be between trary to standards, the reduction is dependent on
US$3000 and US$8000 depending on the pollutant decisions made at the firm. If emissions reduction
used for the estimation (SO2, NOx, PM) [62, 63]. is less expensive than paying environmental
Seeing air pollution as an externality taxes, the company will do it. Otherwise, the
(externalized cost) forced governments and econ- company will reduce less and pay more tax [61].
omists to find suitable and cost-effective solutions The final pollution control policy is tradable
to this problem. Standards, including safety, emis- emissions rights, also called a “cap and trade”
sions, and technology, were the first attempts by policy. The policy is based on the idea that com-
governments to control air pollution. They regu- panies must have permits to generate emissions.
late the concentration of pollutants in the ambient Regulators can set the number of emissions cer-
air, emission quantities, or the technology which tificates allowed, and if companies do not comply
firms must adopt in the production process with assigned limits, sanctions are imposed. The
[61]. However, the exact value of the standard is quantity of emissions allowed is chosen to fit the
difficult to determine due to competing priorities desired air quality. Furthermore, the allowances
and incomplete knowledge. In some cases the are tradable. If a company manages to reduce its
chosen concentration is not optimal in an eco- emissions, it is allowed to sell the remaining part
nomic cost-benefit analysis; economic impacts of the permit to others who might need them
484 Industrial Emissions Control Technologies: Introduction

[61]. The EU adopted its own “cap and trade” treaty by themselves. To counteract free riders
policy called the Emissions Trading System and punish countries violating the treaty, sanc-
(ETS). The system faced serious problems during tions have been established. However most IEAs
the economic crisis of 2008–2012. After having don’t contain the sanctions due to their voluntary
traded at almost 30 € per ton of CO2 in 2008, the character. The Kyoto Protocol doesn’t provide
price fell below 3 € in 2013. The reasons for the any option for punishing noncompliance, and
dramatic decrease in price included lower energy even if one should be established by consensus
use due to the economic crisis, generation of an in the future, Article 27 gives the signatories an
allowance surplus in previous years, and alloca- option to withdraw from the treaty within
tion of free allowances for big companies to pre- 1 year [67].
vent carbon leakage [65]. At the beginning of In the end, the efficiency of an IEA might be
2018, the prices for emission allowances in the dependent solely on an outcome of cost-benefit
EU increased. The trend has continued, increasing analysis for each of the signatories. This was
to almost 25 € per ton of CO2 emitted in January embodied in the great success of Montreal Proto-
2019 [66] (Fig. 2). col and, arguably, the impact of the Kyoto Proto-
International environmental agreements (IEA) col [68].
are a mark of good will of the signatories which
believe that it is possible to fight environmental External Cost of Air Pollution
pollution by cooperation. However, cooperation Air pollution and wastewater are two key negative
between so many entities can be very compli- external costs from industrial production that
cated. Game theory analysis was applied to affect the world. Air pollution is a negative exter-
explain the difficulties and find the most effective nality coming from manufacturing, imposing
means of cooperation within the international external costs to people who are not a beneficiary
environmental pollution field. Accession to IEAs of the transaction resulted in the production of
is usually voluntary; therefore to make the coop- pollutants [61]. The cost of air pollution was
eration possible, treaties must be individually investigated by a collaborative study between
rational (cost-benefit analysis has to be positive) the World Bank and the Institute for Health Met-
for all of the parties. Otherwise, they will not join rics and Evaluation at the University of
the treaty or will violate it. A subsequent problem Washington, Seattle. The study estimates that pre-
for international cooperation is “free riders”: non- mature deaths due to air pollution in 2013 cost the
signatory countries who benefit at no cost from the global economy 225 billion dollars in lost labor
efforts of the signatories. There is no third-party [23]. The report contains the cost of damages to
institution which can enforce cooperation at the health and the environment from air pollution in
global level; hence parties have to enforce the 2008–2012. While pollution has a major effect on

Industrial Emissions 30,00


Stock price in  per ton of CO2

Control Technologies:
Introduction, 25,00
Fig. 2 Stock prices in € per
ton of CO2, data retrieved 20,00
from Market Insider [66]
15,00

10,00

5,00

0,00
-09
0
-10
11
-11
11
12
12
12
-13
13
14
-14
-15
-15
16
16
17
-17
18
-18
Jul-1

Jan-

Jun-
Oct-
Jun-
Oct-

Jan-
Mar-

Apr-
Apr-
Feb-

Mar-
Dec

Sep

May

Nov

Aug
Dec
Aug

May

Aug
Industrial Emissions Control Technologies: Introduction 485

global warming, its external costs also include fitting for removal of desired pollutants. The
welfare losses of $1245 billion USD. A decrease equipment should be selected based on several
in productivity in 2013 triggered by sick leaves factors including location, required space, ambi-
cost $30 billion USD in the EU alone [61]. Heavily ent and working conditions, and its contribution to
polluted cities experience a loss of urban compet- waste production. The optimal system must be
itiveness due to talented, educated workers who considered depending on the contaminant charac-
are more willing to move to less polluted areas. teristic and its physical and chemical properties,
Air pollution is the fourth leading fatal health risk as well as reactivity and size distribution, etc. Gas
resulting in a decrease in life expectancy and fatal stream characteristics such as volume flow rate,
diseases such as cancer, heart diseases, and pressure, humidity, and viscosity have to also be
strokes [23]. The damage cost for NH4, NOx, considered as well as unit requirements (power,
n-CH4 VOCs, PM, and SOx was 40–115 billion maintenance, etc.) and operating cost of the sys-
Euro in 2012, and the damage cost of CO2 in 2012 tem [9] (Fig. 3).
was 18–73 billion Euro [23]. Industrial polluters Generally, an air pollution control system
receive the revenue from production, while the operates by delivery of a polluted air stream of
victims of pollution assume the costs due to a known flow rate (Q) and concentrations of pollut-
decreased standard of living and disease ing chemicals (c) at established pressure (p) into
(Table 1). The victims are not able to control or the control system. The system requires adequate
influence production and therefore are bystanders utilities (i.e., power, water, adsorbent materials,
to the pollution surrounding them [61]. etc.), depending on the operation mode, to remove
the unwanted compounds (pollution) from the air
The Development of Pollution Control stream and release clean air into the atmosphere.
The realization of the hazardous effects of air During the process, waste materials will be pro-
pollution during the industrial revolution brought duced, and some of the energy in the form of, e.g.,
the first attempts to restrict high pollution levels. heat, will be lost. Some of the waste and heat can
Pollution was particularly bad in urban areas, be recovered or recycled and sold as commodities.
where most industries were placed at that time.
The abatement acts were aimed at reducing indus-
trial emissions; however, households remained a Filtration, Thermal Oxidation,
significant pollution source [69]. Since the events Electrostatic Precipitator, and Cyclone
of Great London Smog (1952), people started to
give more attention to the adverse effects of air Filtration
pollution. As a consequence, first, the Clean Air Filtration is a simple, efficient, and economical
Act was established in the UK in 1956 followed method for particle removal, also at the high dust
by US Clean Air Act of 1963 which authorized concentrations often seen in industry. A particle
research in pollution monitoring and control on filter is thought wrongly by many to work like a
the national level [70]. Air pollution control sys- sieve, trapping only particles large enough to be
tems are currently an integral part of the industrial stopped by the filter material. The filtration pro-
landscape. Due to the relatively high cost of con- cess, however, is very complicated, and its prin-
trol devices, a large effort is directed towards more ciples are covered in extensive literature [71].
desirable forms of pollution control. Pollution The fibrous filter is built of fine fibers
prevention from waste minimization, alternative (cellulose, glass, plastics) arranged so they are
production techniques (e.g., green chemistry), and perpendicular to the airflow direction. The
improved process control are recently considered removal efficiency of the filters can be simply
the best practice [9]. However if no alternatives expressed as the fraction of the inlet concentration
can be found, the use of adequate control equip- retained by the filter material. The efficiency of
ment must be considered. The control device must the filter can be significantly improved by increas-
comply with regulatory emission policies and be ing the fiber density (decreasing the pore size of
486 Industrial Emissions Control Technologies: Introduction

Industrial Emissions Control Technologies: Introduction, Table 1 Types of pollutants emitted from industry and
their impact, sources, and lifetimes
Yearly
Exposure limit emissions Environmental
Pollutants Lifetime ref: Industrial source in Gga[19] Health impact impacts
PM PM10: PM2.525 mg/m3 Metallurgy, mineral 500 PM2.5 can penetrate PM has a direct
1 day to yearly average, products, and through the lung impact on climate
1 week PM10 40 mg/ chemical industries barrier and in the change by scattering
[1] m3 yearly [21] blood, while PM10 the light and indirect
PM2.5 average [20] PM10 comes can only penetrate by increasing the
1 week to primarily from the lung [22] number of cloud
10 days construction, road, PM affects sensitive condensation nuclei
[1] dust, and regions of the and consequently
resuspension, while respiratory system increasing clouds
PM2.5 is mostly and can cause or lifetime and Earth
combustion product aggravate albedo. PM can also
[1] cardiovascular, lung lead to acidic rain
diseases and cancer and acidification of
[23] the ecosystem, due
to PM formation by
acidic compounds
(NOx, SOx) [24, 25]
CO2 100 years 5000 ppm Coal power plants, 243,000 2000–5000 ppm CO2 is a greenhouse
[8] (9000 mg/m3) road transport, leads to headaches, gas contributing to
in an 8-hour manufacturing sleepiness, poor global warming
period Time- industry [27] concentration, (described in
Weighted increased heart rate, oxidized
Average and nausea compounds)
(TWA) [26] 5000 ppm could lead
to toxicity and
oxygen deprivation
[28]
SO2 4–12h 125 mg/m3 in a Mostly from the 700 Short time exposure SO2 emissions lead
[29] 24-hour period burning of fuel can be felt in to acidification and
[30] containing sulfur 10–15 min and damage to forests
dioxide [31] irritates the nose, and contribute to the
throat, and airways formation of PM
to cause coughing, [23]
wheezing, shortness
of breath, or a tight
feeling around the
chest
Long time exposure
can affect lung
function [32]
NO2 1.8–7.5 h 50 mg/m3 in a Fuel combustion 1,070 The effects of long- Acidifications and
[33] 24-hour period from power plants term exposure to low eutrophication of
[20] and industrial levels are linked to waters and soils.
facilities [23] asthma, diabetes, NO2 can lead to the
lung cancer, stroke, formation of O3 and
and acid rain PM [23]
In high
concentrations, NO2
can cause airway
inflammation and
reduce lung function
[23]
(continued)
Industrial Emissions Control Technologies: Introduction 487

Industrial Emissions Control Technologies: Introduction, Table 1 (continued)


Yearly
Exposure limit emissions Environmental
Pollutants Lifetime ref: Industrial source in Gga[19] Health impact impacts
NH3 1 day [34] 18 mg/ Mainly agriculture, 90 Ammonia has a Ammonia can lead to
m3(25 ppm) in but also various strong odor and in eutrophication and
an 8-hour industrial processes, most cases can be acidification of
period (TWA) transport, and smelled before ecosystems [23]
[35] management of reaching harmful
waste [36, 23] levels
High levels can
cause burning of
airways, severe
burns, and
permanent eye
damage
Low levels can cause
irritation of airways
and irritation of skin
and eyes. Ammonia
is mostly harmful to
people with asthma
or similar conditions
[37]
CH4 12 year 1000 ppm in an Fossil fuel 70 Methane gas in the Methane is a
[8] 8-hour period extraction, environment doesn’t greenhouse gas and
(TWA) [38] agriculture, biomass have an effect on has GWP multiple
burning, and man- human health, but times higher than
made wetlands (rice) high levels of CO2 [41]
[8] methane could
decrease the amount
of oxygen in the air
and result in mood
changes, memory
loss, nausea, and
slurred speech [39,
40]
NMVOC N/A N/A Various sources, 3,400 Short-term exposure VOCs contribute to
including industry, results in irritation of the formation of
paint application, the eyes and ozone from sunlight
road transport, dry- respiratory tract, and nitrogen oxides.
cleaning, and other headaches, VOCs play also a
use of solvent [23] dizziness, and visual key role in the
The overall disorders and formation of
emissions are caused memory impairment, secondary organic
by burning coal and e.g., headaches in compounds [46]
oil and motor vehicle traffic due to
exhaust [42] benzene exposure
(benzene) Long-term exposure
Chemical can lead to
manufacturing, pulp prolonged eye, nose,
and paper mills, and throat irritation,
forestry product chronic headaches as
plants, coal well as loss of
processing [43] coordination and
(formaldehyde) chronic nausea, and
liver, kidney, and
central nervous
(continued)
488 Industrial Emissions Control Technologies: Introduction

Industrial Emissions Control Technologies: Introduction, Table 1 (continued)


Yearly
Exposure limit emissions Environmental
Pollutants Lifetime ref: Industrial source in Gga[19] Health impact impacts
system damage [44]
Some VOCs such as
benzene exposure
can lead to genotoxic
carcinogen [45] and
formaldehyde can in
the long term
(exposure above
0.2 mg/m3) give
cancer [45]
Heavy N/A N/A Various combustion N/A The adverse effects It can be deposited
metals processes and of heavy metals on on terrestrial or water
industrial activities human health are surfaces and then
[23] dependent on their build up in soils and
specific properties sediments. Even low
such as particle size concentration can
distribution, water have adverse effects
solubility, reactivity, on terrestrial and
and carcinogenic aquatic ecosystems.
potency. Their acute Heavy metals are
effects are mostly very persistent. They
associated with have the tendency to
occupational bioaccumulate in
exposure. However, organisms and
even low-level long- biomagnify in food
term exposure can chains [23]
lead to serious
adverse effect on
population such as
respiratory diseases,
renal diseases,
damage to nervous
system, cognitive
impairment, and
cancer [18, 47]
a
The yearly emissions are based on EU emissions inventory report 2016. The data consider only the sector of energy use in
industry and industrial processes and product use

material) and the thickness of the material or pass the surface of the fiber within one particle
reducing fiber diameter. On the other hand, it radius (Fig. 4a). Regardless of the particle size,
will also drastically increase resistance to the air inertia, or Brownian motion, the particle will be
flowing through it, called pressure drop. The best collected [71]. Inertial impaction occurs when the
fibrous filters are those with highest RE% at the carried particle is too big to follow curving
lowest possible pressure drop [71]. To reduce the streamlines near the fiber (Fig. 4b). Its inertia is
pressure drop, one can use pleated fibrous filters so big that it continues its original path and hits
which will increase the effective filtration the filter element even if by following the stream-
area [72]. line it would miss it. This happens usually at high
Particle removal by the filter is based on a few gas velocities and in dense filters [2, 71]. The
deposition mechanisms. Interception occurs when mechanism of diffusion is based on random
the streamline carrying the particle happens to (Brownian) motion of gas particles in the stream.
Industrial Emissions Control Technologies: Introduction 489

Industrial Emissions Control Technologies: Introduction, Fig. 3 Pollution control system

Fine particles are also a subject to this mechanism. finite space on the filter, and at some point, they
Their random motion and change in the flight will clog the filter, blocking the airflow through it
directory increase the probability of hitting the and significantly increasing pressure drop. Parti-
filter fiber (Fig. 4c). cles collected on the filter material tend to accu-
Diffusion appears mostly at low air velocities mulate and form dendrites which initially increase
and by small particles ([2]). The literature also the removal efficiency [71], but ultimately the
describes the mechanism of electrostatic deposi- filter cake will constrict air flow. At this point,
tion, which is very effective but often neglected, the filter should be replaced [74].
due to problems with quantification [71]. The Frequently used for high dust concentrations
electrostatic deposition will be further described and for industrial applications, fabric filtration is
in the section on “Electrostatic Precipitator”. often confused with fibrous filtration. The former
Generally, the smallest removal efficiency for is often a large installation of high-efficiency fil-
fibrous filters is observed at a particle diameter of ters made of woven or felted fabrics. The idea
approximately 300 nm. This is due to different behind the fabric filtration is that their initially
deposition mechanism playing a key role in parti- low particle removal efficiency will increase
cle removal at different particle sizes. Particles with a dust layer building up on the fabric
smaller than 300 nm are mostly subject to diffu- (similar to the vacuum cleaner system). Because
sion. Bigger particles are usually removed by of accumulating dust, the fabric filters operate at a
inertial impaction or interception. Particles much higher pressure drop than other filters [71].
in-between are either too big or too small to be
removed by one of the mechanisms; therefore Thermal Oxidation
their penetration will be higher than for others Thermal oxidation or incineration is a high-
[73]. Diffusion batteries are devices dedicated temperature process in which waste molecules
for removal of very fine particles of a diameter are oxidized and turned into simpler substances
between 2 and 200 nm. They consist of a bundle such as water and carbon dioxide (mineraliza-
of circular or rectangular channels of size in the tion). In order to use thermal oxidation efficiently,
mm range and rely on the deposition of the parti- the inlet gasses must be substances which can be
cles in the channels by diffusion from laminar oxidized, typically VOC and CO [9]. The idea
flow [71]. behind this process is to raise the temperature of
The structure of the filter will change over time the polluting gas to its auto-ignition point in the
due to particle deposition on it. Particles occupy presence of oxygen and maintain this high
490 Industrial Emissions Control Technologies: Introduction

Industrial Emissions
Control Technologies:
Introduction,
Fig. 4 Mechanisms of
filtration: (a) (interception),
(b) (inertial impaction), (c)
(diffusion)

temperature for a time long enough to obtain a significant amount of pollutants including com-
pollutant destruction at wanted or required by pounds which were not present in the gas mixture
regulations level. before thermal oxidation, e.g., formaldehyde
The main principle of operation can be con- (Fig. 5).
cluded in so-called “three Ts” parameter – tem- Construction and maintenance of an efficient
perature, time, and turbulence. The efficiency of thermal oxidizing device requires a considerable
thermal oxidation is dependent on those three design effort. Usually, the temperature, time, and
factors and the availability of oxygen in the sys- removal efficiency of the system are specified by
tem. Sufficiently high temperature and time spent regulations and sometimes selected from experi-
in the system are crucial for the nearly complete ence. The flow of the combustion fuel, size of the
destruction of polluting gasses. Additionally, tur- device, and residence time have to be selected
bulence promotes proper mixing of VOC and according to heat and material balance of the sys-
oxygen molecules and assures that the pollutant tem [9]. Generally, a standard vapor incinerator
will be oxidized before leaving the system consists of only a few simple parts. The polluted
[9]. Incomplete oxidation results in the formation air is directed to the mixing chamber where high
of pollutants such as CO and smaller molecular temperature is maintained by burner fueled with
weight hydrocarbons. Poor combustion may emit fuel gas. The oxidized gases are then discarded
Industrial Emissions Control Technologies: Introduction 491

Industrial Emissions
Control Technologies:
Introduction,
Fig. 5 Regenerative
thermal oxidation
incinerator

from the reaction chamber by the exhaust. Vapor regenerative thermal oxidation, can save up to
incinerators are considered very efficient (RE% of 95% of the energy, making the operation process
99.99) and proven methods for destroying VOC. cheaper but significantly increasing the initial cost
However, they are not recommended for removing of incinerator installation [78]. The technology
gases containing halogenated or sulfur-containing utilizes two chambers packed with heat transfer
compounds. Due to possible corrosive acid gas media (usually ceramics) and combined by a
formation, an additional post-oxidation step for small duct containing the burner (Fig. 5). The
acid control might be necessary [75]. system of valves connects the two chambers, so
To reduce the temperature required for oxida- the waste gas and exhaust clean air can enter and
tion and increase the reaction rate, catalysts can be exit either direction. Initially, the cold polluted air
used. Catalytic incinerators have very similar passes through hot bed 1, is oxidized, and exits the
operation methods as standard thermal incinera- system through the cold bed 2 which is warmed up
tors, but after passing through a flame mixing by passing cleaned air. Next, the direction of the
chamber, the gas goes through the catalyst bed. airflow can be altered; hence very little heat is
Accelerated reaction rate results in lower temper- wasted, and only little fuel is needed to keep the
atures, a shorter residence time, and a smaller desired temperature (Fig. 5) [9].
device [9]. Catalytic incinerators are however
not without their flaws. They can be easily Cyclonic Separation
clogged with PM or poisoned by chemicals pre- Inertial separators such as the cyclone are usually
sent in the vapor such as Pb, Cl, or S. Finally, the used for collecting medium-sized and coarse par-
initial cost of the catalytic oxidizers is much ticles. Inertial separators are cheap, but their
higher than standard thermal oxidizers [76]. removal efficiency is also lower than, e.g., elec-
Energy efficiency in thermal oxidation might trostatic precipitators. Therefore, they are usually
also be achieved via changes in incinerator used as precleaners to reduce loading for other
design. Installation of the heat exchanger in the devices and extend their lifetime. The principle
system might significantly improve the thermal of the method is based on the inertial movement of
efficiency of the device by partial heat recovery particles in the system. After the particulate-laden
from the exhaust gas. Since heat is delivered by gas spirals down the outside of the separator, it is
burning the fuel, a lot of money can be saved by forced to change its direction at the bottom of the
reusing the existing energy to preheat the incom- device. The gas then spirals upward, but the par-
ing waste gas [9]. Heat exchangers are also called ticles keep moving in the original direction (due to
recuperators and can recover ca. 70% of the waste the inertia), which leads to the particles being
heat from exhaust gases [77]. The developed alter- separated from the gas stream. We differentiate
native to the traditional heat exchanger, multiple types of inertial separators including
492 Industrial Emissions Control Technologies: Introduction

cyclone, centrifugal separators, and baffle cham- significantly. The cyclone efficiency is measured
ber. Cyclones and centrifugal separators are both by its collection performance. It’s important for the
often used for industrial purpose. cyclone to be air-tight; otherwise the collected
In cyclonic separators, gas is forced to spin in a particles will be pulled out into the gas stream
vortex through the tube. Centrifugal separators again. Therefore, the whole system must be
use the same circular motion as the cyclone but completely sealed. Other factors concerning oper-
have a rotating vane in the collector itself to both ating and maintenance activities are device erosion
move the air and separate the dust. Centrifugal and fouling. Erosion happens when particles trav-
separators are mostly used for coarse particles, eling the cyclonic path scratch the inside of the
while cyclones are used for fine particles[9] cyclone, which over time can lead to destructions
(Fig. 6). of the cyclone walls and finally leakage. Erosion is
As shown in Fig. 6, particulate-laden air enters often promoted by high dust loading, high inlet
the gas inlet at the top of the cyclone. The gas velocities, and the strike angles. It mostly affects
travels down the cyclonic path, and under the the cone area and can be controlled by proper
influence of centrifugal force, the particles move cyclone diameter and use of thicker materials.
outward to the cone outlet and are collected. Fouling occurs when the particles build up at the
When the gas reaches the cone-shaped section, outlet and cover it. This can lead to the particles
the increased rotational gas velocity helps to getting into the gas stream again. Another factor
keep the dust at the walls. At the reverse rotation, affecting the collection performance is the material
the cleaned gas travels to the clean gas outlet collected on the cyclone wall. Soft and fine dust
above. The dust doesn’t change direction due to will tend to build up on the wall over time. This can
the inertia of the particles and exits the cyclone at be prevented by smoother walls such as electro-
the bottom [9]. polishing walls. Generally, cyclones show better
A cyclone can be used both as a separate device removal efficiency for particles with higher
but also as a multiple-tube cyclone arrangement. density.
The latter can be often found in fossil fuel boilers.
Having multiple cyclones with common inlet and
outlet operating parallel to each other increases the Electrostatic Precipitators
efficiency and throughput of the system An electrostatic precipitator (ESP) is a widely
applied technology for the removal of hazardous
particles from an industrial process. Industrial
ESPs exhibit complex interaction mechanisms
between the electric fields, the fluid flow, and the
particulate flow. The physical system in an ESP
has three sub-systems affecting each other [79]:

– A mixture of gases which flows inside the ESP


(a mixture of exhaust gas)
– A stream of particles which flows along gas
flow and which must be removed (filtered)
– An electric field imposed by suitable external
means which aim to charge electrostatically the
particles

ESPs use electrical forces to move the particles


out of the flowing gas stream onto collector plates.
Industrial Emissions Control Technologies: Introduc- The particles are given an electric charge when
tion, Fig. 6 Mechanism of a cyclone separator [9] passing through the corona, where gaseous ions
Industrial Emissions Control Technologies: Introduction 493

are created. In the center of the flow channel, collected slurry must be handled more carefully
electrodes are maintained at high voltage. These than dry dust, increasing the cost of exposal [9].
electrodes produce an electric field that forces the
particles to the walls. Charged dust particles
migrate to the collecting plate due to Coulombic Heterogeneous Catalysis
forces. When the particles are collected at the
plates, they can be removed, which is usually General Heterogeneous Physics
done by knocking them loose from the plates. Heterogeneous catalysis is a reaction happening at
Then the particles slide down into a hopper and the gas-solid or liquid-solid interface at the catalyzed
are evacuated. Different types of ESP are known, surface. The role of the catalyst is to lower the
some removing particles by intermittent or wash- activation energy (Ea) as seen in Fig. 7. The catalyst
ing with water [9] (Table 2). acts by reducing the energy necessary to proceed
All the above mentioned ESP configurations along the reaction pathway, i.e., the activation
can be operated also with wet walls instead of energy that needs to be surmounted to yield prod-
dry. One of the main advantages of wet precipita- ucts. The activation energy is the energy required to
tors is that the use of water to wash the accumulated overcome the reaction barrier and determines how
material minimizes the possibility of particles fast a reaction occurs. The thermodynamics of the
reentering the cleaning system, which may happen reaction remains unchanged, and only the catalyst
with dry precipitators. On the other hand, the influences the reaction rate [80].

Industrial Emissions Control Technologies: Introduction, Table 2 Different types of ESPs [9]
ESP type Use for Operation method
Plate wire Coal-fired boilers, cement kilns, solid waste, The gas flow between parallel plates of sheet metal
precipitator incinerators, paper mill recovery boilers, and high-voltage electrodes (parallel, discharge
petroleum refining catalytic cracking units, sinter and collecting electrodes are side by side).This
plant, basic oxygen furnaces, open-hearth allows many flow lanes to operate in parallel and is
furnaces, electric arc furnaces, coke oven suited for handling large volumes of gas.
batteries, glass furnaces Sectionalized power supply to obtain higher
operating voltages
Flat plate High-resistivity particles with small mass median The precipitator works by increasing the average
precipitator diameter. The fly ash has been successfully electric field used to collect the particles,
collected by this method increasing surface area for the collection of
particles. The corona-generating electrodes are
placed ahead and behind the flat-plate collecting
zones
Tubular Sulfuric acid plants, coke oven by-product gas It’s placed with high-voltage electrodes running
precipitator cleaning, iron, and steel sinter plants. It’s applied along the axis of the tube. Many tubes are
where the particulate is either wet or sticky operating in parallel to handle an increased gas
flow and tightly sealed to prevent leaks. One-stage
unit: All the gas pass through the electrode region.
High-voltage electrode operates at one voltage the
entire length of the tube. Current varies along the
length as the particles are removed
Wet Remove liquid droplets such as sulfuric acid mist It operates with wet walls. The water flow applied
precipitator from industrial process gas streams intermittently or continuously to wash the
collected particles into a sump of disposal. It must
be handled more carefully than dry
Two-stage Gas flow volumes of 50.000 acfm. It’s not parallel and with the discharge electrode
precipitator Submicrometer sources emitting oil mists, preceding the collector electrodes
smokes, fumes, and other sticky particulates
because there is a little electrical force to hold the
collected particles on the plate
494 Industrial Emissions Control Technologies: Introduction

Industrial Emissions
Control Technologies:
Introduction,
Fig. 7 Potential energy
diagram

Ea (no catalyst)

Energy

Ea (with catalyst)

Reactants

Products

Reactions coordinates

DG is the chemical potential energy called the The adsorption is described by the following
Gibbs free energy. Based on the potential energy reaction:
profile, Gibbs free energy can be negative or pos-
itive. When the reaction is endergonic reaction, AðgÞ þ S  A  S K ads ðAÞ
DG > 0 means the reaction absorbs energy from
the environment (energy added into the system). A is the adsorbate, S is the surface also called
When the reaction is exergonic reaction, DG < 0 the adsorbent that provides a surface for adsorp-
means the reaction releases energy into the envi- tion, and A  S is absorbed species.
ronment (energy out of the system) [81]. The adsorption coefficient Kads(A) depends
An example of a heterogeneous catalyst is upon the surface and temperature. Molecules can
ammonia synthesis using iron oxides on alu- attach to the surface in two different ways because
mina (Al2O3). The Haber-Bosch process is the of the different forces involved called
synthesis of ammonia from nitrogen and hydro- physisorption and chemisorption.
gen gas at high temperature using a supported These two adsorptions differ from each other
catalyst [82]. It is one of the most important as depicted in Fig. 9. Physisorption is a weak
industrial inventions. It allows mass production interaction of valence-saturated species due to
of plant fertilizers used by farmers to grow more van der Waals attraction. The enthalpy of
food and which has enabled the enormous physisorption is in the region of 20 kJ/mol
increase in population through the twentieth [84]. The small enthalpy change wouldn’t lead
century [83]. to bond breaking. The adsorbed reactants don’t
The process illustrated in Fig. 8 is called react, and only small changes in bond energies are
adsorption, where the molecules from gas seen. Chemisorption involves a strong chemical
(or liquid) phase interact and attach to a solid bond. The forces involved are valence forces of
surface. The reverse process of adsorption mean- the same kind as the ones involved in chemical
ing the process which the molecules escape from compounds. The enthalpy of chemisorption is in
the solid surface is called desorption. the region of 200 kJ/mol, which indicates that in
Industrial Emissions Control Technologies: Introduction 495

Industrial Emissions
Control Technologies:
Introduction,
Fig. 8 Haber-Bosch
process

Industrial Emissions
Control Technologies:
Introduction,
Fig. 9 Potential energy
diagram of physisorption
and chemisorption
0

Physisorption
Potential

Chemisorption

Distance between atom and surface

a reaction a chemisorbed compound will form a described by the number of adsorption sites occu-
strong chemical bond with the surface atom [80, pied divided with the number of adsorption sites
84, 85]. As illustrated in Fig. 9, chemisorption has available (S0).
a shorter distance between the atom and the sur-
face. Therefore there is a larger potential due to AS

the strong binding, while the atom and surface are S0
further apart in physisorption resulting in weaker
bond and lesser potential. Dissociative chemi- Adsorption isotherm is the relation between the
sorption appears when bond breaks and the reac- coverage of an adsorbate on a surface and its
tants are being absorbed in two or more concentration in the bulk phase under equilibrium
fragments. at a constant temperature [85]. In adsorption pro-
The concentration of the adsorbed species is cess, the free gas and the adsorbed gas are in
expressed as A  S, and the surface coverage (y) is dynamic equilibrium and coverage which
496 Industrial Emissions Control Technologies: Introduction

depends on the pressure of the overlying gas. The AþS AS K ads ðAÞ
variation of coverage with pressure at a tempera-
ture is called an adsorption isotherm. ASþB!P k2

k ads The rate is defined as R ¼ k 2 yðAÞ  pðBÞ  S 0


p
k des [85]. The mechanism is depicted in Fig. 10 with

k ads the reaction
1þ p
k des
NH2 ðad Þ þ NOðgÞ ! NH2 NO ! N2 þ H2 O
kads is the adsorption rate, kdes is the desorption
rate, and p is the pressure of the adsorbing Catalysis Technology
substance [84]. The most well-known example of the use of catal-
In a bimolecular catalyzed reaction, two possible ysis in pollution control is from the vehicle indus-
mechanisms are possible. In the Langmuir- try, in the form of three-way gasoline catalysts
Hinshelwood mechanism, two species are pre- (TWCs). Invented in the 1970s, the TWC quickly
adsorbed at the surface and then react with each other. became the standard for most gasoline-powered
vehicles. TWCs are able to convert CO and hydro-
AþS AS K ads ðAÞ carbons (HC) to CO2 and water, simultaneously
reducing NOx with high efficiency [88]. TWCs
BþS ÐBS K ads ðBÞ still play a key role in the reduction of exhaust gas
emissions and greatly improved the air quality in
BSþAS !P k 02 urban areas.
The main factors influencing the efficiency of
0
The rate is defined as R ¼ k 2 yðAÞ  yðBÞ  S 0 catalyst are its activity, selectivity, and lifetime.
[85]. The mechanism is depicted in Fig. 10 with The activity of the catalyst in pollution control is
the reaction below described as the ability to convert harmful reac-
tants to harmless products. Although important,
NHþ
4 ðad Þ þ NO2 ðad Þ ! NH4 NO2 ! N2 þ 2H2 O
the activity of the catalyst itself won’t be much
effective without its selectivity toward desired
Eley-Rideal [87] mechanism shows the reac- products. Selectivity ensures that only specific,
tion of an already adsorbed gas-phase species and desired reactions will be accelerated and hence
an adsorbate. plays a key role in minimizing the creation of

Industrial Emissions
Control Technologies:
Introduction,
Fig. 10 Bimolecular
catalyst mechanism [86]
Industrial Emissions Control Technologies: Introduction 497

by-products (waste prevention). The catalyst is and diffuses through it ensuring selective reaction
not consumed during the reaction it supports; of the reagent and NOx under specific temperature
therefore its lifetime should, in theory, be (EPA).
unchanged after the reaction. In practice, how- SCR is very efficient and can operate at signif-
ever, the stability might be reduced by chemical icantly lower temperatures than non-catalytic sys-
interaction of reactants with the active sites of the tems, but their operation and installation cost
catalyst called poisoning. In addition, perfor- increases considerably [91]. Almost all coal-fired
mance is limited by physical blocking of the power plants have installed deNOx systems due to
active sites by species deposited on the catalyst the strict limitation of NOx emission rule. And
and its pores called fouling. Both processes, as 95% of them are using SCR deNOx catalyst.
well as thermal sintering due to high temperatures, However, the activity of commercial SCR cata-
inhibit the catalytic reaction rate and deactivate lysts would decrease because of the complex
the catalyst in the long term [80]. chemical composition in the flue gas of power
Catalytic technology is widely present in plants. Thus, the lifetime of SCR catalysts is nor-
industrial applications such as oil refining, energy, mally around 3 to 4 years. The regeneration and
transport, chemicals, polymers, and textiles but recycling of poisoned or wasted catalysts have
also in pollution control and monitoring. Catalysts become a severe problem.
can be roughly classified into metals (Ag, Pt, Pd),
oxides (MnO2, NiMoO4), and acids (H3PO4, Hydrodesulfurization
H2SO4, zeolites). Each of the classes has its Hydrodesulfurization (HDS) is a catalytic process
advantages and can be used in different applica- widely used to remove sulfur from natural gas and
tions [80]. refined petroleum products, such as gasoline, die-
sel fuel, etc. Its purpose is to reduce SO2 emis-
Selective Catalytic Reduction sions from vehicles, power plants, and industrial
Selective catalytic reduction (SCR) is a chemical processes. The product of this process, hydrogen
reduction reaction via a reducing agent supported sulfide (H2S), can be readily converted into ele-
by a catalyst. SCR is used mainly in fossil fuel mental sulfur or sulfuric acid in petroleum refin-
combustion units and nitric acid plants for reduc- eries. In fact, the majority of world sulfur
tion of nitrogen oxides. The SCR process reduces production comes from its recovery from natural
NOx chemically into molecular nitrogen and gas and petroleum processing [92]. The catalysts
water vapor with the help of nitrogen-based used in HDS are usually based on aluminum
reagent (usually ammonia or urea) and catalyst oxides mixed with metals like Co, Mo, Ni,
(noble metals, molecular sieves, metal oxide, etc. [93] and supported on materials with high
etc.). The SCR catalysts are divided into four surface area, therefore increasing the amount of
groups: (1) V2O5-WO3/TiO2 type, (2) three-way catalytically active sites [80].
catalyst (TWC) type, (3) molecular sieve type, Catalytic removal of VOCs was briefly
and (4) AC-supported type [89]. The TiO2-WO3/ described in a chapter on thermal oxidation. Cat-
V2O5 catalyst is the most widely used commercial alytic incinerators are one of the most efficient
SCR catalyst due to its high De-NOx efficiency methods for the destruction of VOCs from the
and stability. gas effluent [9]. The catalyst can decrease the
Honeycomb catalysts, plate-type catalysts, and required oxidation temperature significantly,
corrugated catalysts are the three most widely therefore allowing VOC conversion to H2O and
used SCR catalyst types [90]. The catalyst type CO2 to occur with much less external heat and
and composition have an influence on the effi- hence at a much lower cost. Among various types
ciency of NOx reduction, lifetime, and its stability. of catalysts, noble metals are highly effective in
Operation works by injection of the reagent into catalytic oxidation. However, their high cost and
the hot waste gas stream. The mixture then enters poor stability, especially in the presence of chlo-
the reaction chamber which contains catalyst bed rine, set back their development. Metal oxides of
498 Industrial Emissions Control Technologies: Introduction

manganese, nickel, and cobalt or acidic oxides Wet Scrubbers


like zeolites or TiO2 have been also extensively Wet scrubbers involve scrubbing pollutant gasses
studied with mixed results [94]. The activity of a with a scrubbing liquid. The technology is primar-
catalyst is highly dependent on the number of ily used for water-soluble toxic gases (e.g., HCl
active sites available for the catalytic reaction to and NH3 [95, 100]). Different types of wet scrub-
occur. Therefore, materials with high porosity and bers are available. The most common are venturi
extensive surface area, like titania and g-alumina, scrubbers, spray towers, cyclonic scrubbers, and
are especially interesting as a support material for wetted filter scrubbers. Spray tower scrubber are
catalysts. This approach has also an economic illustrated in Fig. 11. The cyclonic scrubber is
motivation. Since the reaction takes place on the quite similar to the cyclonic separator, with the
surface, a thin layer of finely dispersed expensive difference that a scrubbing liquid is injected into
material (catalyst) is a very cost-effective idea. In the airstream [9].
some cases catalysts serve as their own support, The common design for wet scrubber technol-
mostly in the shape of spherical pellets. Alterna- ogy is as follows. First the contained gas passes
tively, the catalyst can be mounted on the through a liquid designed to remove the pollutant.
honeycomb-like monolith block. This will result The chemical composition and charge of the liq-
in a high specific area and provide increased cat- uid can differ depending on the gas it captures
alytic activity [94]. (solutions of reagents that specifically target
certain compounds). The liquid may, for example,
just be water for removing dust particles.
Scrubbers The components of a basic scrubber include a
vessel, some type of packing, a fan or blower, a
General Description of Scrubbers reservoir for the scrubber fluid, and a pump for the
Industrial processes produce exhaust gas fluid. There are many options for additional fea-
containing various harmful gases such as SO2 tures and many optional configurations for the
and CO2. The most effective way of reducing air system [101].
pollution is to capture these pollutants at the As seen in Fig. 11, scrubbing liquid is used to
source. Post-combustion pollution removal remove the pollutants. The exhaust gas is moved
methods such as scrubbers are one way to do through the scrubbing liquid which saturates the
it. Scrubber technologies can be divided into wet
scrubbers and dry scrubbers [95]. One of the first
known scrubbers was used in submarines to
remove carbon dioxide. Nowadays however they
are now widely used in all kinds of industries
[96]. The shipping industry depends on high-
sulfur fuel for ships, which during combustion
release SOx and PM into the air. Scrubbers can
remove up to 99% of SOx and 98% of PM and are
an important prospective technology for green
shipping [97]. Furthermore the rendering industry
produces large amounts of VOC, and wet scrub-
bers are used to remove these harmful gases
[98]. Scrubber technology can be used in collab-
oration with other filtration methods to increase
removal efficiency [99]. A hybrid process of wet
scrubbers and biofilters will increase the removal
of VOCs from, e.g., poultry-rendering Industrial Emissions Control Technologies: Introduc-
industries [99]. tion, Fig. 11 Spray towers
Industrial Emissions Control Technologies: Introduction 499

gas. The targeted pollutants are removed from the with acid gases. The reaction occurs and forms
gas and attach to the liquid due to its chemical solid salts, which are collected in a particulate
composition. As the gas is passed through the collection device. This method is effective at cap-
cleaning mist, the remaining contaminants are turing HCl (90%) but less so for SO2 (50%). The
attracted to the mist and left behind [102]. The ratio of alkali added is 1:2, so the method is
removal efficiency increases by increasing resi- limited to small facilities. The effectiveness of
dence time and surface area of the scrubber the technology can be improved by increasing
solution. the flue gas humidity and recycling the reaction
Advantages of the wet scrubber include the products.
small space requirements for the setup. The scrub- The process of dry sorbent injection is as fol-
ber has a high collection efficiency and collects lows: Flue gas enters the cooling tower where
both gases and PM. It’s robust and can handle water is sprayed on the gas to lower the tempera-
high humidity and high temperature. On the ture. The dry reagent is mixed into the flue gas and
other hand, the technology requires high mainte- reacts with it. In the end, it is removed at a dust
nance, which increases the operating cost signifi- collector [9].
cantly. The wet scrubber creates wastewater and Spray dryer absorption combines a spray dryer
wet residuals, presenting a disposal issue. with a dust collector. In the process flue gas enters
the spray dryer and comes in contact with a cloud
Dry Scrubbers of finely atomized droplets of reagent. The flue
Dry scrubbers remove pollutants from the exhaust gas with decreased temperature and increased
gas by using a sorbent. A sorbent is a material that humidity reacts with acid gases and is collected.
absorbs/adsorbs gases or liquids. Dry scrubbers This method has a very high removal efficiency
are primarily used for acidic gases from combus- for acid gases HCl (99%), SO2 (95%), SO3 (99%),
tion (SO2 and HCl) and for removal of odorous and HF (95%).
and corrosive gases from wastewater treatment The advantages of dry scrubbers are that the
plants. Dry scrubber technologies have different technology produces much less waste material
systems, but common to them all is that the device compared to wet scrubbers and is less expensive.
has an acid gas sorbent material going into the gas Some of the disadvantages are that the removal
stream and a control device to remove reaction efficiency is lower, and dry scrubbers can have a
products [103]. difficult time removing several pollutants at once.
The system operates by first cooling the gas. Residual waste is toxic and must be handled by
The emission gases are cooled to make it easier to experts [9, 103].
remove pollutants and other toxins from the gas.
Next, a collection of dry reagents is sprayed into NH3 Removal
an exhaust stream. These chemicals can react Livestock production and animal and human
differently depending on which material they are waste emit NH3 and odorous gases. Atmospheric
specifically targeting for removal. These materials NH3 damages the natural ecosystem and contrib-
neutralize the harmful pollutants in the gas stream utes to particle formation. Ammonia removal can
through a chemical reaction, while others cause be achieved using an acid scrubber. Acid scrub-
the material to react and turn into a different bers are also used for other basic compounds and
substance. The product falls out and is collected many odorants [104].
and disposed of [9].
The two well-known dry scrubbers are dry SOx Removal
sorbent injection and spray dryer absorbers, Sulfur dioxide emission is known to have severe
which remove acid gases such as HCl, SO2, effects on human health and the environment.
SO3, and HF. Sulfur emissions lead to sulfate aerosols that
The dry sorbent injection includes the addition impact climate and health. Sulfate deposition
of alkaline material into the gas stream to react (acid rain) leads to acidification of the
500 Industrial Emissions Control Technologies: Introduction

environment, destroying aqueous habitats and and their by-products. The sorbent of choice for
damaging tree foliage and crops [7]. Combustion most of the scrubbers are limestone (CaCO3) and
of sulfur-containing fossil fuels, especially for lime (CaO). Wet scrubbers, using those materials,
electricity production, is the main cause of SO2 can achieve a removal efficiency of up to 99%.
formation today [105]. Energy generation (51%) Limestone is a common, naturally occurring min-
and energy use in the industrial sector (20%) are eral, and its chemical composition can vary
the major contributors to EU-28 emissions of SOx greatly from source to source and has a significant
[18]. Therefore, power plants are encouraged to effect on product (e.g., gypsum) quality. Lime is
find an effective way to reduce emissions to com- produced by calcination of limestone. It is a
ply with National Emissions Ceilings (NEC) highly reactive material, and its storage requires
Directive (2016/2284/EU). In recent years, thanks special attention due to its irritant properties. The
to the new European air quality standards and caps sludge created after the process of desulfurization
on NOx and SOx emissions, acid rain in Europe is using limestone can either be disposed of or, with
slowly declining, and forests, lakes, and natural the right technology, can be transformed to low
habitats are showing signs of recovery [18]. SOx cost, easily available, marketable gypsum
emissions can be reduced in many ways, includ- (CaSO4  2H2O) by the following reaction:
ing the removal of sulfur before combustion, dur-
ing combustion, or post-combustion. SO2 þ CaCO3 þ 2O2 þ 2H2 O
Desulfurization before combustion is done by ! CaSO4  2H2 O þ CO2
selection of low sulfur fuels or by fuel desulfuri-
zation, e.g., physical preparation of coal. This The gypsum created during the absorption of
method, although quite effective (sulfur reduction SO2 must be then separated from the water, its pH
of 30%), is not economical and, if applied, would adjusted and stored. Water used in the process can
significantly increase the market coal prices be purified and reused. The value of produced
[106]. Combustion controls are primarily used in FGD gypsum depends highly on used technology,
coal-fired plants and work by adding the SO2 the composition of the fuel, and limestone. In
sorbent to the furnace. The post-combustion pro- Europe it’s successfully used as a cement additive,
cess focusses on removing SOx from the flue gas plaster products, etc. [107]. Additionally, ammo-
and is referred to as flue gas desulfurization nia can also be used in the process of desulfuriza-
(FGD). Post-combustion desulfurization can be tion, and its by-product ammonium sulfate is used
carried out with multiple methods. Currently, the worldwide as an agricultural fertilizer [107].
most common processes available on the market
include wet scrubbers, spray dry scrubbers, sor-
bent injections, and combined SO2/NOx removal CO2 Removal
processes. The desulfurization technology can be Carbon dioxide is the largest of the anthropogenic
also classified roughly into regenerable and climate forcing agents that cause global warming.
throwaway, depending on how the sorbent is Anthropogenic emissions of CO2 contribute sig-
treated after the process. nificantly to climate change and have become a
In throwaway technology, the used sorbent is serious global problem. 40% of total CO2 emis-
disposed of or utilized as a by-product. The sor- sions come from fossil-fueled power plants
bent can also be regenerated, and the SO2 released [108]. Since the Kyoto Protocol came into force,
from it can be further processed to sulfuric acid or signatories of the treaty are obligated to reduce
elemental sulfur. The latter method produces GHG emissions. Carbon capture and storage
almost no waste, but the cost of a regenerable (CCS) comprises techniques which trap CO2
FGD is also much higher. from exhaust and store it and hence mitigate cli-
The mechanism of desulfurization in dry and mate change. CSS quickly became a priority for
wet scrubbers was described previously; here we environmental agencies around the world. The
will focus on the materials used in those processes EU countries have managed to successfully
Industrial Emissions Control Technologies: Introduction 501

decouple GHG emissions from economic growth the two critical attributes of membranes, selectiv-
in recent years (1990–2017) and decrease the ity and permeability, has to be made, and one of
emissions of 22% while increasing GDP by 58% the parameters will be sacrificed to the other
[18]. However, there is still much work to be done [108]. However, recent research provides proof
to stabilize atmospheric CO2 levels. There are that advances in membrane materials can signifi-
several natural mechanisms of CO2 fixation, cantly improve separation performance and make
such as ocean fertilization or geological injection membrane technology competitive with other
(creation of carbonates). Reforestation of land and CCS technologies [110]. Various types of adsor-
desert greening are the next natural processes for bents can also be used for CO2 capture. This
CO2 removal from the atmosphere. Further, pho- mainly includes activated carbon and lithium
tosynthesis can be used in photo-bioreactor sys- compounds. Their efficiency is based on CO2
tems in which cyanobacteria or micro-algae can capture capacity and their stability [108].
transform CO2 into useful products such as car- Apart from CO2 being stored, it is also valuable
bohydrates and oxygen [108]. This section how- as a commodity. Flue gas has traditionally been an
ever will focus on industrial technologies for important source of CO2, especially in remote loca-
atmospheric CO2 removal. tions lacking CO2 by-product sources. CO2 is
The major cost in CCS technologies comes widely used in industry, food and beverage produc-
from CO2 capture. This can increase the cost of tion, firefighting, solvent extraction in chemical
electricity production by up to 50% depending on labs, and supercritical fluid chromatography.
techniques used in the process. Hence, there is a Another industrial application of CO2 is in enhanced
strong drive to improve the methods of carbon oil recovery (EOR), where CO2 is used to force oil
capture to make it more cost-effective. The current from beneath the Earth. EOR relies heavily on cheap
methods used in CCS include absorption, adsorp- CO2 sources. Therefore, the viability of CSS
tion, membranes, and biotechnology [108]. Amines depends on CO2 market and oil prices [109, 111].
have been used as sorbents in the natural gas indus-
try for 60 years. The method is well studied and has Bioscrubbers
an efficient recovery rate from the flue gas (up to Livestock is a growing contributor to ammonia,
98%). Nonetheless the absorption process can be VOC, and H2S emissions and can influence O3
further improved in the areas of energy efficiency and SOA formation. Bioscrubbers are a novel and
and stability of the sorbent. In short, the process is innovative technology that could seem like a per-
based on the injection of an amine solution such as fect solution for livestock emissions removal. The
monoethanolamine (MEA) into the flue gas. There, technology is based on the separation of VOCs
CO2 is absorbed by the solution and creates MEA into the aqueous phase and subsequent biological
carbamate. Next, the CO2 product of the absorption treatment of the water in two-unit operations. The
reaction is reheated to release almost pure CO2; the waste is firstly cleaned in an absorber, and the
MEA solution is recycled and reused later. The pollutant gases are transferred from gas to aque-
main disadvantages of MEA absorption are ineffi- ous phase. The water containing the dissolved
cient solvent regeneration (70% of operating cost), pollutants continues to biological treatment in a
rapid equipment corrosion, amine degradation, and bioreactor [104, 112].
high energy consumption [108, 109]. The bioreactor is a tank, aerated with air bub-
The use of membranes for CO2 capture has bles and containing suspended activated sludge.
encountered several problems which must be Microbial biodegradation takes place in a nutrient
addressed before the technology can become the solution in the aqueous phase. Furthermore, pH is
method of choice. Polymeric membranes are not controlled to optimize biological activity. In addi-
resistant to heat or chemicals; therefore, the flue tion to VOC, aerosols are absorbed into the water
gas must be cooled and the chemicals removed phase. pH control is important in order to trap
prior membrane separation, which induces extra H2S, SO2, and other highly water-soluble
costs [108, 109]. Furthermore, the choice between compounds [112].
502 Industrial Emissions Control Technologies: Introduction

The advantages of a bioscrubber include the Membranes are applicable for relatively high
smaller volume of the equipment, better pH con- concentration and low flow rates. The process is
trol, and more reliability and predictability rela- driven by a concentration gradient or pressure
tive to some other methods. Finally there is lower differential between the membrane and flue gas.
occurrence of toxic concentrations in the aqueous The compounds diffuse through the membrane
phase. Disadvantages include limited removal and can be recovered. Silicon rubber-based mem-
efficiency for some compounds. Moreover the branes are one of the better studied and a quite
slowest-growing microorganisms can be washed efficient technology, but they lack resistance
out, the disposal of sludge can be difficult, and the toward some hydrocarbons such as gasoline
operational cost is high [112]. vapors. For this case and others, there is a need
to develop additional, chemically resistant mem-
brane materials. Elastomeric polymers were found
to be versatile materials for membrane produc-
Gas Phase Advanced Oxidation and tion, and their resistance toward organic com-
Vapor Recovery pounds has been tested successfully
[115]. Although membrane recovery seems to be
Vapor Recovery a very promising technique, some problems must
VOCs are among the most common air pollutants be addressed. Membranes’ lifetime suffers from a
emitted from the chemical sector of industry trade-off between permeability and selectivity
[113]. Their emission into the atmosphere and [116], and their recovery cycle is considered to
further reactivity can lead to serious environmen- be relatively slow. Furthermore, the membranes
tal hazards. The realization of VOC’s adverse are rather costly, and their sensitivity toward oper-
effects on human health has brought emissions ating conditions (fouling, bacterial growth)
regulation and resulted in accelerated advance- followed by intense maintenance increases their
ment in the field of VOC removal. Some of the operating cost significantly. Lastly, the disposal of
techniques for VOC control have been presented used membranes causes a burden on the
earlier in the sections on oxidation and catalytic environment [113].
removal. However, in some cases VOCs are of Recovery efficiency depends critically on
economic interest. Certain VOCs are valuable choosing a suitable technique for the process;
compounds, and their recovery might be more therefore it is of great importance to recognize
profitable than removal by destruction and characterize the compounds of interest in
[114]. Therefore, vapor recovery systems have order to fit the method to their properties. First
been designed to deal with the pollution problem the source of the compounds must be identified to
and recover the compounds of interest. Conse- characterize the classes of chemicals the recovery
quently, several advanced separation technologies system has to deal with. The chemical properties
for VOC control have been developed. This (reactivity, toxicity, vapor pressure, solubility,
includes condensation, adsorption, membrane- etc.) must be tabulated. Finally the value of the
based recovery, and absorption process covered compounds must be established, and based on that
in the chapter on scrubbers. knowledge, combined with regulatory demands,
Condensation relies on achieving supersatura- the choice of recovery will be made [114].
tion of VOC in the flue gas by a rapid decrease of The two most common adsorption methods are
temperature or pressurization. The method is most temperature swing adsorption (TSA) and pressure
efficient for VOCs boiling above 50  C at rela- swing adsorption (PSA). The former is achieved
tively high concentration (above 5000 ppm). by adsorbing the flue gas at a lower temperature
Lower boiling compounds require more energy on an adsorbent bed such as activated carbon
for cooling or pressurization. A consideration for which is regenerated at a higher temperature
condensation systems is that the high gas concen- (often over 100  C) to recover the material
trations after condensation might exceed the lower [117]. The cycle of adsorption, regeneration, and
explosive limit (LEL) [113]. cooling of the adsorbent bed requires time, and in
Industrial Emissions Control Technologies: Introduction 503

addition the material has a limited throughput exposure to harmful emissions, in addition to
defined as the space velocity or ratio of the flow of improving regional air quality [120]. Furthermore,
air that can be treated with a given volume of vapor recovery is an important process in chemi-
adsorbent. Altogether, for high throughput a large cal industry. It not only decreases the emission of
bed is required [114]. PSA on the other hand has a environmentally hazardous substances but signif-
much shorter cycle time and hence can achieve high icantly reduces the expense of solvent recovery
throughputs even for a small adsorption bed. PSA is and in some cases can bring profit from the recov-
performed by cycling the pressure between flue gas ery of tradable components. Industrial processes
and adsorbent bed. Adsorption occurs at a pressure such as drying, coating, and gluing produce an
higher than atmospheric, and the regeneration pro- immense amount of solvent vapor which can be
cess occurs at atmospheric pressure. This is in con- either destroyed or reused [121]. Vapor recovery
trast to vacuum swing adsorption (VSA), another is also one of the CCP methods mentioned in the
pressure-dependent technique which desorbs at section on scrubbers. It can be used to reduce CO2
lower pressure, with adsorption occurring at atmo- emissions from large stationary sources such as
spheric pressure. PSA, due to its lower energy fossil-fuel plants and also for direct capture from
requirement, shorter regeneration cycle, and higher ambient air, achieved economically with, e.g.,
regeneration rate, has been established as a superior moisture swing sorbents [122]. The CO2 captured
method over TSA [114, 116, 117]. Furthermore, by an adsorbent can be later recovered and find its
some recent studies suggest that the recovery rate place in a variety of applications.
can be improved by combining thermal and vacuum
techniques in a hybrid technology [118]. Electrical
swing adsorption (ESA) is currently one of the most Gas-Phase Advanced Oxidation (GPAO)
promising new methods. Heat is generated via cur- Gas-phase advanced oxidation (GPAO) is an
rent passing through the adsorbent, without heating emissions control method based on the mecha-
the surroundings. Thus, the techniques offer several nisms that remove pollution from the Earth’s
advantages due to improved energy efficiency, faster atmosphere [123]. In the system, pollutants are
regeneration cycles, and better desorption oxidized, and their oxidations products are
kinetics [117]. removed as particles [124].
Various adsorbent materials can be used for The GPAO process is shown in Fig. 12. Pol-
vapor recovery. One of the most popular adsor- luted air enters the system and is mixed with
bents is activated carbon (AC) [114, 116, ozone. UV-C light photolyzes the ozone to pro-
117]. AC is very effective at adsorbing VOCs duce O(3P), O(1D), HO2, and the OH radical. The
and CO2 but is not very selective, and the use of OH radical is the main driver of the oxidation
more complex multilayer adsorbent beds can be process and oxidizes pollution, in many cases a
necessary if recovery of individual compounds is VOC compound. SOA forms from VOC oxida-
desired. A molecular sieve, thanks to its great tion products and is removed by an electrostatic
selectivity and versatile application, is often a precipitator (ESP) or another particle removal
good alternative. If high flue gas humidity is a technique. As a part of the ESP, the particles are
concern, zeolites can be considered, due to their first charged by a high-voltage (HV) electrode and
superior hydrophobic properties [114]. then collected. The remaining unreacted ozone is
Vapor recovery is applied for environmental finally removed by a MnO2 catalyst, and the clean
protection by emissions control and for recovery air leaves the system [124, 125].
of expensive or tradable compounds. Regulations The OH radical can initiate oxidation of a wide
on gasoline vapor emissions in the EU and USA range of pollutants [123], and in the atmosphere,
have accelerated innovation in the field of VOC all air pollution is removed by a variety of mech-
recovery and resulted in the successful application anism (oxidation, photolysis, deposition). In low
of vapor recovery systems in fuel dispensers NOx conditions, HOx is formed by the photolysis
[119]. Installation of vapor recovery systems in of ozone by UV-C light, which produces O(1D).
service stations can significantly reduce personal O(1D) reacts with water vapor to produce OH
504 Industrial Emissions Control Technologies: Introduction

Particle formation

Polluted air
O3 OH, OH2, O(1D), O(3P)
Clean air
Gas phase products

UV-C HV ESP UV-C O3 catalyst

Industrial Emissions Control Technologies: Introduction, Fig. 12 The GPAO process

radicals. The lifetimes of VOCs are inversely cor- These particles can be effectively removed by
related to OH radical concentrations [125]. high-efficiency particulate air filters (HEPA)
GPAO has been applied to the removal of [125]. In the study by Meusinger et al. [123]
malodorous reduced sulfur compounds (RSC) removal of VOC had an 80% RE. GPAO is effec-
emitted from pig farms. The increase of odorous tive for cleaning VOC at concentrations below the
gas emissions such as ammonia, RSCs, and VOCs combustion limit. The OH radical reacts with
is an issue because it is an issue for neighbors and many species but not all; some notable excep-
because odor itself is regulated in Europe and can tions, with limited treatment, are CH4, CO, and
be a limiting factor in the size of an operation. Wet NO2. In addition the method is not suitable for hot
acid scrubbers are sometimes used for ammonia air streams in which O3 is not stable [125].
control, but they are not suited for RSCs due to The main advantage of GPAO is that the tech-
their low water solubility or chemical properties: nology is applicable to controlling, e.g., RSC emis-
H2S is an acidic gas, as are malodorous organic sions with low energy input [124]. The process has a
acids [124]. The experiments conducted on an much lower volumetric energy input than other
industrial scale including a wet scrubber achieved approaches, in part because chemistry occurs in
a RE of 90% [124]. This shows that the GPAO the gas phase avoiding the large pressure drop
method can have a high performance when oper- caused by surface techniques. GPAO is effective at
ated with other removal technologies. GPAO was pollution levels for which catalysis and combustion
also tested in a Saar region foundry in Germany. are not self-sustaining [125]. The oxidizing OH
The technology was tested against BTEX radicals are resistant to collision with other com-
(benzene, toluene, ethyl benzene, and xylenes) pounds such as H2O, N2, and O2 present in the
and proved to be effective (80–90% removal). system; they persist until they react with pollution.
The produced particles were removed by ESP, In the GPAO method, key parameters such as lamp
and the excess of ozone was controlled with power and ozone concentration can be controlled to
MnO2 catalyst [126]. A study built a proof-of- optimize performance and match treatment to pol-
concept device to test and optimize the process lution load, in contrast to other “on or off” pollution
[125]. The results showed that GPAO is a viable control systems present in the industry [125]. The
control strategy for most VOCs in particular spe- system is easy to scale over many orders of
cies with an OH radical reaction rate constant magnitude [126].
greater than 5  1013 cm3/s. Laboratory experi-
ments with propane, cyclohexane, benzene, and
isoprene were conducted as well. The results Green Chemistry
showed a correlation between residence time and
removal efficiency; longer residence time yields Green chemistry is a branch of sustainable chem-
higher RE. Propane and cyclohexane didn’t result istry and can be described as the design of chem-
in SOA formation, and the particle removal effi- ical products and processes in order to reduce or
ciency by ESP was 85%. eliminate hazardous substances. It aims to prevent
In one test the generated particles were ultra- pollution at the source, at a molecular level, and to
fine, limiting their removal efficiency by the ESP. reduce the negative impacts of industrial
Industrial Emissions Control Technologies: Introduction 505

processes on human health and the environment. damaging to ecosystems, safe to handle by not
The goal of green chemistry is similar to that of being flammable or explosive, degradable in
end-of-pipe pollution control technologies such as nature, and not bioaccumulative.
scrubbers, vapor recovery, GPAO, ESP, cyclones, The E-factor describes the amount of waste
and the others we have discussed. However, generated in the process at chemical industries
instead of treating pollution from the waste and is the ratio of the mass of waste to that of the
streams, green chemistry prevents pollution emis- product. The formula excludes water.
sions by process modification and alternative
manufacturing and through the use of more envi- kg waste

ronmentally friendly materials [127]. kg product
The twelve principles of green chemistry out-
line its scope [127]. Processes aim for low E-factor and if the
E-factor is zero, the process is a truly green
1. Prevent waste. process [130].
2. Maximize the atom economy. In green synthesis, the aim is to maximize the
3. Design less hazardous chemical syntheses. yield of the desired product and minimize
4. Design safer chemicals and products. by-products, simplify operation, and use greener
5. Use safer solvents and reaction conditions. solvents. In industry most of the chemical prod-
6. Increase energy efficiency. ucts are based on carbon from petroleum, and
7. Use renewable feedstocks. waste is a big issue and burden for the environ-
8. Avoid chemical derivatives. ment. Another way to minimize environmental
9. Use catalysts instead of stoichiometric impact is by considering what kind of catalysts
reagents. is used and avoiding toxic components when pos-
10. Design chemicals and products to degrade sible. Hence, there is growing attention on
after use. organocatalysts or enzymes as a more environ-
11. Analyze in real time to prevent pollution. mentally friendly option. Improved analytical
12. Minimize the potential for accidents. techniques and engineering are also key factors
to reduce waste and optimize technology
The main considerations are the use of renew- efficiency [131].
able raw material feedstock and designing the Air pollution’s impact on human health is
synthesis process such that the final product con- increasing. Recent studies show that up to
tains most of the input material, which is also 800,000 Europeans die each year because of air
described as the atom economy. Finally, avoid pollution [132]. As a consequence increasing
waste by restricting the solvents to those that are emphasis has been put on practicing green chem-
nontoxic and biodegradable [7]. istry and developing new environmentally
Atom economy is the proportion of reactant friendly technologies.
atoms that end up in a useful product and is Choice of catalyst is one of the key compo-
calculated by counting the number of atoms of nents of green chemistry. In 2005 the Nobel Prize
the starting materials that end up in desired prod- was awarded for the discovery of a catalytic
ucts and those that end up as a waste. The equation mechanism called metathesis, which has broad
for the atom economy is given by the following applicability in chemical industry. The 2005
equation [128, 129]. Nobel Prize for Chemistry was awarded to Yves
Chauvin, Robert H. Grubbs, and Richard
atom economy=% R. Schrock, for the development of the metathesis
molecular mass of desired products method in organic synthesis. They used supercrit-
¼  100 ical CO2 as a green solvent, aqueous hydrogen
molecular mass of all reactants
peroxide for clean oxidations, and hydrogen, in
Nonhazardous chemicals are defined as com- asymmetric synthesis. Prior to their discovery,
pounds which are less toxic to organisms, less halogenated solvents were frequently used in
506 Industrial Emissions Control Technologies: Introduction

synthesis. However due to their properties and Conclusion and Future Prospects
harmful effects on groundwater and the ozone
layer, the substitution of halogenated compounds Industrial emission control technologies are
with supercritical CO2 brought huge improve- playing a key role in the protection of the environ-
ment in environmental protection [133]. ment and human health. Various techniques
The use of VOCs in paints is damaging for selected precisely to deal with specific pollutants
both the environment and human health. This is have been in use for decades now, and their high
especially true for the oil-based paints which emit removal efficiency was extensively verified. How-
significant amounts of VOCs into the atmosphere. ever, with progress in technology and broader
Therefore, there is increasing demand for pro- knowledge on the environmental impact of air
ducers to create paint that does not give off pollution, new challenges have emerged. Growing
organic solvent vapors. Procter & Gamble and population has led to an increasing number of
Cook Composites and Polymers created a mixture industrial facilities with time, and, climate changes.
of soy oil and sugar that replaces fossil fuel- Addressing these and many other issues requires
derived paint resins and solvents, cutting the con- fresh, out of the box thinking in the areas of air
tent of hazardous volatiles by 50%. Later, pollution control and sustainable development.
Sherwin-Williams developed water-based acrylic In 2015 the United Nations adopted the
alkyd paints with low VOC emissions that can be Agenda for Sustainable Development Goals. The
made from recycled soda bottle plastic (PET), Agenda consists of 17 points and aims to protect
acrylics, and soybean oil [133, 134]. the planet and ensure that all people enjoy peace
Plastic is widely used in containers, bottles, and prosperity. Air pollution was recognized as
and packaging. It’s a growing segment of solid one of the major sustainability concerns and is
waste, and hence, several companies have been directly mentioned in goal 3.9 which seeks a sig-
working to develop plastics that are made from nificant reduction of deaths from air pollution by
renewable, biodegradable sources. NatureWorks- 2030 [138]. Current technology might not be ade-
food makes containers from a polymer called quate to address the Sustainability Goals. There-
polylactic acid branded as Ingeo. They discovered fore, rapid development in the field of pollution
a method where microorganisms convert corn- prevention and remediation will be necessary for
starch into a resin that is just as strong as the years to come. Although efficient, current pollu-
rigid petroleum-based plastic. BASF created tion control systems require constant upgrades.
recently a compostable polyester film called Novel materials for pollutant adsorption are con-
“Ecoflex” (biodegradable bags) [133, 135]. stantly being developed [139], and energy-saving
A significant amount of the diesel fuel used in solutions, better catalysts, and waste generation
transportation evaporates into the atmosphere reduction are developing rapidly [137, 140]. Fur-
where its photooxidation leads to the formation of thermore, the state of pollution control systems
PM, NOx, HC (hydrocarbon), CO, and other haz- can be improved by improved pollution manage-
ardous air pollutants. These pollutants as described ment, including wireless sensor networks [141],
in Table 1 have a negative impact on human health big data analysis, and modeling of long-term sce-
and the environment [136]. The production of die- narios [142]. The future of air pollution control is
sel from sources other than fossil fuels (e.g., bio- based on the regulatory work of environmental
diesel), such as vegetable oil, requires a more agencies around the world. The gradual tightening
efficient solid catalyst to make the process fully of environmental policies designed by EEA and
ecologically friendly. A sugar catalyst is a high- national EPAs are crucial for pollution mitigation
performance catalyst made from naturally occur- and give the groundwork for an international ini-
ring molecules which can be used in this process. tiative such as UN 2030 Agenda. Achieving Sus-
Green synthesis and recyclable materials used in tainable Development Goals will be a tremendous
biodiesels can significantly reduce the pollution effort requiring collaboration of nations and gov-
emissions from the transport sector [137]. ernments throughout the world.
Industrial Emissions Control Technologies: Introduction 507

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Index

A Aerosol mass spectrometry (AMS), 126


Abrasion, 55–57 Aerosol particle mass analyzer (APM), 115–117
Acid deposition, 385, 392–393 Afforestation, 3015
Acid neutralizing capacity (ANC), 385 Agriculture sector, heatwave impacts, 466–467
Activated carbon (AC), 152–153, 503 Airborne nanoparticles, 86, 118
Activated carbon fiber (ACF) filter, 104 APM, 115–117
Activation energy, 493 CNTs, 98–104
Active stability, 426 composition and morphology, measurements of,
Adaptation, 279 125–127
ethical implication, 312 CPC, 121–122
in Europe, 306–307 diffusion, 91, 92
in food security and agriculture, 307 electrospun nanofibers, 94–98
Adaptive capacity, 385 electrostatic deposition, 91, 92
Adsorption isotherm, 495 ESPs, 104
Aerodynamic diameter, 7, 193, 204, 385 fibrous filters, 90
Aerosol, 87, 88, 102, 105, 109, 112, 113, 115, 117, 120, filtration efficiency, 90, 93
125, 239, 385, 479, 481, 499, 501 impaction, 117–120
aerosol-climate interactions, 269–270 inertial impact, 91, 92
aerosol-cloud-precipitation interactions, 268–269 interception, 91, 92
budgets, 252–255 optical measurement, 120–121
burdens, 252–255 particle coagulation, 112–116
challenges, 241 particle diffusion mobility, 125
climate, 263 particle electrical mobility, 123–125
cloud droplet activation, 260–263 particle penetration, 90
definition, 239 QF filtration, 91
dimensions, 241–242 thermophoresis, 109–112
direct effect, 263–264 Airline emission index, 327, 341–343
formation, 241–242 AirNode, 445
global budgets, 252 Air pollution, 89, 279
global burdens, 252–255 Airports, 200
global radiative budget, 263 Air quality, 385
hygroscopicity, 260 index, 195
indirect effect, 264–268 monitoring, 385
multiphase secondary production, 248–252 warnings, 395–396
nature and impacts, 240 Air quality standards and guidelines
optical depth, 239, 385 air quality management framework, 11–13
precipitation, 263 definition, 8
primary formation, 242–244 hazard and risk assessment, 26
removal, 241–242 health impact, 13–17
secondary formation via nucleation, 244–248 impact of socioeconomic status on mortality, 16
spatial distributions, 252–255 National Ambient Air quality Standards, 18–19
vertical distributions, 255–260 ozone, 32–37
water uptake by, 260 paradigm shift, 22–25

© Springer Science+Business Media, LLC, part of Springer Nature 2021 513


M. E. Goodsite et al. (eds.), Air Pollution Sources, Statistics and Health Effects,
https://doi.org/10.1007/978-1-0716-0596-7
514 Index

Air quality standards and guidelines (cont.) Carbon capture and storage (CCS), 302–306, 500, 501
particulate matter, 27–32 Carbon dioxide removal (CDR), 300–302
erocess for developing and issuing National Ambient Carbon nanotubes (CNTs)
Air quality Standards, 19–22 activated carbon fiber filter, 104
sources of information for setting, 26–27 filtration performance, 104
US legal framework for, 17 free-standing SWNT films, 99
WHO guidelines, 25, 40–42 high-filtration efficiency, 98
Albedo feedback, 291 3-layer CNT filter structure, 101
Allan variance method, 429 multi-walled CNTs, 98, 99
American Trucking Associations v. EPA, 21 quartz fiber filters, 102, 103
Ammonia, 481 Catalytic technology, 496–497
Amperometric gas sensor, 439 Centrifugal particle mass analyzer (CPMA), 117
Anthropogenic, 347 Channel capacity, 429
AQMesh systems, 444 Chemical transport model, 373
Aqueous solution concentration, 109 Chemisorption, 432, 494
ARTEMIS project, 61 Chlorofluorocarbon (CFC), 373, 385
Atmospheric chemistry, 281–282 Clean Air Act (CAA), 17, 37, 485
Automobile propulsion technologies, 71 Clean Air Scientific Advisory Committee (CASAC), 19
Average exposure, 53 Climate, 239
Average-speed models, 58 Climate change, 230, 385
Aviation, 327 adaptation (see Adaptation)
Aviation and atmosphere anthropocene, 284–285
air chemistry changes by air traffic, 338–339 ethics and philosophy (see Ethics and philosophy)
airline emission index, 341–343 greenhouse gases, 283–284, 286–289
cloudiness, 335–338 Hadley cell, 292
definition, 327 hydrological cycle, 291
emission reduction policy, 340 mitigation (see Mitigation)
emissions, climatically relevant substances, 329–335 monitoring, 395
European Directive, 340–341 oceans, 289–291
transport sector’s contribution, 339–340 oxygen, 289
Aviation-induced cloudiness (AIC), 327 particulate matter, 283
Avogadro’s number, 91 polar amplification, 291
sixth mass extinction, 293
soil carbon content and permafrost, 292
B
surface temperature, 285–286
Background level, 385
sustainability and (see Sustainability)
Backscattered electrons (BSEs), 126
Climate hazards, 280
Band gap, 423, 433
Climate-related risk, hazard, vulnerability and
Benzene, 480
exposure, 300
Best available technology (BAT), 385
Cloud condensation nuclei (CCN), 283, 307
Bimolecular catalyst mechanism, 496
Cloud droplet activation, 239
Biochar, 301
Coal, 9
Bioenergy with Carbon Capture and Storage
Coarse particles, 194, 207
(BECCS), 301
Coefficient of performance (COP), 149
Biogenic, 347, 385
Cohort study, 347
Biosphere, 279, 385
Cold ironing, 73
damage, 393
Cold-start emissions, 55
Boltzmann distribution, 104
Combustion, 53–55
Boundary layer, 215
Command and control, 385
Brownian motion, 92, 112
Compressed natural gas, 71
Building and street scales, 163
Concentration-response functions (CRFs), 386
Built environment sector
Condensation particle counter (CPC), 121–122
heatwave impacts, 463–465
Conference of the Parties (COP), 280, 340
Buoyancy, 150
Conservative stability, 426
By-products, 482, 497, 501, 505
Consolidated sustainability metrics, 386
Contrails, 327
C Conventional mapping techniques, 231
Cadmium, 482 Corona crises (COVID-19), 1, 2
Cap and trade policy, 483 Coupled chemistry-climate model (CCM), 373
Index 515

Critical load, 386 Eley-Rideal mechanism, 496


Critical natural capital, 386 Emissions
Cross-flow ion mobility spectrometer (CIMS), 125 monitoring, 401
Cross-ventilated system, 151 standards, 403
Cyclonic separation, 491–492 trading, 327
Emissions Trading System (ETS), 484
D Empirical model, 65
Data quality objective, 443 Energy sector, heatwave impacts, 464–466
Deposition velocity, 139 Enforcement, 386
Desulfurization, 500 Engine exhaust particle sizer (EEPS), 118, 124
Deterministic models, 65 Enhanced oil recovery (EOR), 501
Deutsch equation, 105, 106 Environmental ethics, 280
Diesel particulate filter, 47 Environmental Kuznetz Curve (EKC) hypothesis, 483
Differential mobility analyzer (DMA), 117, 121, 125 Environmental management
Differential mobility particle sizer (DMPS), 121 ecological restoration, 298–300
Diffusion, 91 habitat, 298
Dioxins and furans, 390 preservation, 297
Direct air capture (DAC), 304, 305 seeds and plants, 298
Dissolved oxygen (DO), 467 species, 298
Diurnal, 347 Ethical implications
Diurnal losses, 55 adaptation, 312
Double Schottky barrier model, 433 ecological restoration, 315
Dry deposition, 139, 347 geoengineering, 312–313
Dry scrubbers, 499 mitigation, 311
Dust suppressants, 74 preservation, 314–315
Ethics and philosophy
E ecological justice, 314
Eco-driving, 72–73 global justice, 310
Ecological justice, 280, 314 intergenerational justice, 315–317
Ecological restoration, 280, 315 perfect moral storm, 309–310
climate change, 299 Eulerian model, 65
environmental management, 299 Evaporation, 55
Ecosystem, 386 Everhardte-Thornley detector, 126
Electrical aerosol spectrometer (EAS), 118, 124 Exceedance, 347
Electrical mobility, 87, 123–125 Excess heat factor (EHF), 458, 468, 472
Electrical swing adsorption (ESA), 503 Exposure, 280, 386
Electricity generation, 9 limit, 480
Electric low pressure impactor (ELPI), 117, 120 Exposure-response relationship, 23
Electrochemical gas sensors, 439–440 External drivers, 457, 463, 464, 466, 467
chemical interference of co-pollutants, 442 Externality, 483, 484
four electrodes, 440 Extratropical cyclones, 292
and metal-oxide sensors, 443–446 Extrinsic semiconductor, 424
ozone detection, 441
potentiometric sensors, 441
Electromotive force, 441
Electrospinning, 94–95 F
Electrospun nanofibers Face velocity, 90, 95, 98, 101
electrospinning, 94–95 Fast approximate model (FAM), 163
performance of, 95–98 Fast integrated mobility spectrometry (FIMS), 119,
Electrostatic deposition, 91, 92 124, 125
Electrostatic precipitators (ESPs), 75, 492–493 Fast mobility particle sizer (FMPS), 119, 124
advantages and disadvantages, 107 Feedback, 347
collection performance, 109 Fibrous filters, 90
commercial plate-type, 106 Field emission SEM (FESEM), 127
corona discharge, 104 Filtration, 485–489
energy consumption, 107 efficiency, 87, 90, 93, 95, 99, 101, 102, 104, 105, 127
negative mode operation, 105 mechanisms, 92
tube-type electrode, 106 Flat plate precipitator, 493
WESP, 107, 110, 111 Flue gas desulfurization (FGD), 500
516 Index

Formal risk analysis, 24 High-efficiency particulate air (HEPA) filter, 101, 102
Free-standing SWNT films (FSFs), 99, 100, 105 Hockey stick function, 22
Fully computational model (FCM), 163 Holism, 386
Homogeneous nucleation, 239
Hot engine and exhaust conditions, 54
G
Hot-soak losses, 55
Gas-particle concentration (GAC), 109
Hubbert’s peak theory, 296–297
Gas-phase composition processes, 220–224
Hybrid propulsion, 72
Gas phased advanced oxidation (GPAO), 503–504
Hydrodesulfurization (HDS), 497–498
Geoengineering, 307–309
Hydrogen sulfide, 497
Geographical Information System (GIS), 456, 457
Hydrological cycle, 291–292
Geosequestration, 303
Hydropower generation, 465
Gibbs free energy, 494
Hygroscopicity, 239
GISS Surface Temperature Analysis (GISTEMP),
285–286
Global chemical transport model (GEOS-Chem) model, 32
I
Global justice, 280
Impaction, 87, 88, 91, 92, 115, 117–120, 123
individual action, 311
Indoor air pollution, 137
tragedy of the commons, 310
biological, physical and chemical sources of, 138–139
Global temperature change potential (GTP), 327
human interaction with, 140–141
Global warming potential (GWP), 282, 327, 480, 487
Indoor air quality
GP2Y sensor, 438
activated carbon, 152–153
Green chemistry, 504–506
air conditioners, 148–149
Greenhouse effect, 283–284
asthma and allergy, 146–147
Greenhouse gases, 286–289, 386
CO2 as measure of, 147
emission and economic development, 297
gas phase advanced oxidation, 149
emissions, 455
and health, 146–150
Green lighthouse building, 155–158
photocatalysis, 152–154
plants as remediation strategy, 154–155
H remediation methods, 149–157
Haber-Bosch process, 481, 495 sick building syndrome, 146
Hadley cell, 292 sustainable buildings, 155
Harbours, 201 windows, 150–152
Hazardous air pollutants (HAPs), 386 Indoor concentrations of oxidation species, 144
Hazen equation, 106 Industrial air pollution, 486–488
Health sector, heatwave impacts, 463–465 emissions control technologies (see Industrial
Heating, ventilation and air conditioning (HVAC) systems, emissions control technologies)
141, 155 heavy metals, 481–482
Heatwaves, 455, 464, 469, 470–471 oxidized compounds, 480
absolute temperature, 457 particulate matter, 479–480
agriculture sector, 466–467 reduced compounds, 480–481
built environment sector, 463–465 SOAs, 481
energy sector, 464–466 Industrial emissions control technologies
health domains, 468–469 cyclonic separation, 491–492
health sector, 463–465 economics and policies, 482–484
indices, 457–463, 468–469, 471–472 ESPs, 492–493
natural environments, 467–468 external cost of air pollution, 484–485
non-health domains, 469 filtration, 485–489
relative temperature, 457 GPAO, 503–504
return periods, 472 heterogeneous catalysis, 493–498
sector sensitivity, 464 scrubbers, 498–502
transport sector, 466–467 thermal oxidation, 489–491
water sector, 468–469 vapor recovery, 502–503
Heavy metals, 390, 481–482 Industries and public infrastructure, air pollution, 138
Heterogeneous catalysis In situ monitoring, 398–399
catalytic technology, 496–497 Instantaneous model, 59
general heterogenous physics, 493–496 Interception, 92
HDS, 497–498 Intergenerational justice, 280, 315–317
SCR, 497 Intergovernmental Panel on Climate Change (IPCC), 311
Index 517

Internal combustion engines, 53 Meteorological processes, urban air quality


International Civil Aviation Organization (ICAO), 340 building and street scale, 170–173
International Environmental Agreements (IEAs), 484 building and street scale modelling, 178–179
International Maritime Organization (IMO), 340 characteristic regions of flow, 164–165
Internet of Things, 447 complex urban junction, 186–187
Intrinsic semi-conductor, 424 computational models, 174–175
Ionosorption, 432 definition, 163
IPCC, see Intergovernmental Panel on Climate Change mesoscale, 165–167
(IPCC) mesoscale models, 176–177
neighborhood scale, 167–170
neighborhood scale models, 177–178
J output of modelling calculations, 179–186
Jevon’s paradox, 297 urban data, 173–174
Justice trilemma, 317 Methane, 480
Metrics, 347
Microenvironment, 52
K Micro-orifice uniform deposit impactor (MOUDI), 87,
Knudsen number, 91, 92 118, 120, 123
Kyoto Protocol, 340, 484, 500 MIKE URBAN model, 234
Miniature electrical-mobility aerosol spectrometer
(MEAS), 125
L Mitigation, 280
Laboratory animal studies, 23 carbon capture and storage, 302–306
Lagrangian model, 65 carbon dioxide capture, 303
Land carbon sink enhancement, 301 carbon dioxide removal, 300–302
Langmuir-Hinshelwood mechanism, 496 carbon storage, 303–306
Lead (Pb), 390, 482 ethical implication, 311
Leadership in energy and environmental design ocean carbon sink enhancement, 302
(LEED), 155 Mixing ratio, 215
Light scattering, 86, 87, 120, 121, 123 Mobile sources, 7, 17, 347
Linear regression calibration, 446 Mock urban setting test (MUST), 174
Low-cost sensors, 424, 425 Monitoring
calibration, 445–447 acceleration of learning and research, 411–412
electrochemical gas sensors, 439 acid deposition, 392–393
exposure monitoring, 444 air pollutants, 388
factors affecting sensitivity and stability, 431 air pollution, 385
MOx sensors, 432 air pollution mitigation, 406
optical sensors, 436–439 air pollution science on policy, 405
smart city, 447 air quality warnings, 395–396
time-dependent pollution map, 425 changes in institutional practices, 408
uses, 426 climate change, 395
consolidated sustainability metrics, 414–415
criteria pollutants, 389
M damage to biosphere, 393
Marginal abatement cost (MAC), 305 definition, 387
Maritime ship emissions, 49 design methodologies, 416
Matts–Ohnfeldt equation, 106 dioxins and furans, 390
Mechanical ventilation, 141 economy, 394
Mega-cities pollution indices (MPI), 200 emissions monitoring, 401
Megacity, 347 emissions standards, 403
Mercury (Hg), 391 expansion of goals, 408
Mesoscale, 163 global problems, 394
Metal-organic frameworks (MOFs), 423, 448 health, 391–392
Metal oxide (MOx) sensors, 433 heavymetals, 390
advantages, 432 institutional changes, 413
electronic structure, 432 lead (Pb), 390
sensing mechanism, 432–433 mercury (Hg), 391
sensor properties, 433 multidisciplinary work, 412
temperature cycling, 434–436 multipollutant monitoring and science, 414
518 Index

Monitoring (cont.) particle diffusion mobility, 125


non-environmental considerations, 403 particle electrical mobility, 123–125
numerical modeling, 401–402 particle penetration, 90
outstanding problems and challenges, 406–407 QF filtration, 91
overcoming oversimplifications in, 416–417 SEM, 126–127
ozone layer destruction, 395 TEM, 127
particulate matter (PM), 390 thermophoresis, 109–112
policy and air pollution standards, 402–403, 405–406 urban areas, 88
precipitation chemistry monitoring, 399 Nanowire fabrication, 447–448
public involvement, 412 National Air Pollution Control Administration
regional problems, 392 (NAPCA), 17
research, 396 National Ambient Air quality Standards (NAAQS), 8,
research questions, 396–398 18–19
resilience, 409 ozone, 32–36
satellite observations development, 415–416 particulate matter, 28
satellite remote sensing, 399–401 primary and secondary, 18–19
in situ, 398–399 US process for, 19–22
socio-ecological justice, 409 Nationwide Energy Rating Scheme, 464
and sustainability, 388, 407 Natural capital, 386
urban form, 410–411 Natural disaster risk management, 456
violations of concentration standards, 404–405 Natural environments, heatwave impacts, 467–468
visibility, 393 Natural ventilation, 141, 150
volatile organic carbon (VOC), 390 Neighborhood scale, 163
Montreal protocol, 373 Nickel, 482
Mortality, 386 Nitrogen dioxide, 47, 63
Most penetrating particle size (MPPS), 91, 96, 98, 103, 104 Non-dispersive infrared (NDIR) gas sensor, 437
M-Pods, 445 Non-environmental considerations, 403
Multiple-regression models, 59 Non-methane VOC (NMVOC), 480
Multiple Threshold Index, 457, 462 NOx, 215
Multipollutant monitoring, 386 limited, 215
and science, 414
Multi-walled CNTs, 98, 99
O
Ocean alkalinity enhancement, 302
N Ocean carbon sink enhancement, 302
Nanofiber packing density, 97 Ocean fertilization, 302
Nanoparticles (NPs), 118 Oceans, 289–291
AMS, 126 Offices, air pollution in, 138
anthropogenic sources, 87, 88 Open-path laser, 437
APM, 115–117 Operational street pollution model (OSPM), 65
CNTs, 98–104 Opposed migration aerosol classifier (OMAC), 125
CPC, 121–122 Optical particle counter (OPC), 437
deposition mechanism, 88 Optical sensors, 436
diffusion, 91, 92 non-dispersive infrared spectroscopy, 437
electrospun nanofibers, 94–98 particulate matter, 437–439
electrostatic deposition, 91, 92 Outdoor air pollution, 13
engineered, 88 Oxyfuel combustion, 303
ESPs, 104 Oxygen change, 289
fibrous filters, 90 Ozone, 8, 47, 64, 373
filtration efficiency, 90, 93 detection, 441
impaction, 117–120 frequency distribution of simulated daily 8-h-
industrial activities, 88 maximum surface concentrations, 32, 33
inertial impact, 91, 92 GEOS-Chem model, 32
interception, 91, 92 hole, 373
laboratory-engineered, 88 layer, 386
nanotoxicological studies, 89 layer destruction, 395
natural production, 87 NAAQS, 32–36
optical measurement, 120–121 Ozone depleting substance (ODS), 373
particle coagulation, 112–116 Ozonolysis, 144
Index 519

P Rail transport models, 60–61


Particle coagulation, 112–116 Rain, 231
Particle diffusion mobility, 125 Reducing Emissions from Deforestation and forest
Particle electrical mobility, 123–125 Degradation (REDD+), 301
Particle growth, 144 Reforestation, 301
Particle penetration, 90, 101 Refueling losses, 55
Particulate matter (PM), 8, 137, 197, 283, 386, 390, 437– Regional air quality
439, 479–480 air pollutants, 350
definition, 27 atmospheric models, 362
exposure-response relationship, 29, 31 and climate change, 366–369
mortality risk ratios, 30 current air quality legislation and metrics, 364–366
NAAQS, 28 definition, 347–348
Pedestrian-oriented development, 386 ecosystem effects, 360–361
Permafrost, 292 gaseous pollutants, 350–356
Phoresis, 109 health effects, 360–361
Photo-acoustic spectroscopy (PAS), 437 legislation, 348–350
Photocatalysis, 152–154 measurements, 358–360
Photochemical smog, 194 modeling, 362
Photostationary state, 64 monitoring, 348–350
Photostationary steady state, 215 particulate matter/aerosol pollutants, 356–358
Physisorption, 494 regional context, 366
Plate wire precipitator, 493 statistical models, 363
PM10, 215 Removal efficiency, 485, 489, 492, 498, 500, 502, 504, 506
Point sources, 386 Residential air pollution, 137
Policy, air pollution, 385 Resilience, 280, 386
Polyacrylic acid (PAA), 95 Resistance model for dry deposition, 140
Polyacrylonitrile (PAN), 95, 97 Resuspension, 57
Polycyclic aromatic hydrocarbons Reynold’s number, 91, 93
long-range transport of, 209–210 Risk-based policy, 386
sampling artefacts, 209 Road sweeping and washing, 73–74
sources and emissions, 209 Road transport models
Polylactic acid (PLA), 95 abrasion and resuspension, 60
Polymeric nanofiber, 95 combustion, 57–60
Polystyrene latex (PSL), 107 evaporation, 60
Polysulfone (PSU), 97
Polytetrafluoroethylene (PTFE), 97
Polyvinyl alcohol (PVA), 95 S
Polyvinylidene fluoride (PVF), 97 Satellite remote sensing, 399–401
Population exposure, 386 Scanning electron microscopy (SEM), 126–127
Porosity, 163 Scanning mobility particle sizer (SMPS), 118, 123, 124
Potentiometric sensors, 441 Schottky barriers, 426
Preservation, 280 Scrubbers, 498
Pressure drop, 488, 489, 504 bioscrubbers, 501–502
Pressure swing adsorption (PSA), 502 CO2 removal, 500–501
Primary pollutants, 215, 386 dry, 499
Primary standards, 386 NH3 removal, 499
Public transport, 466 SOx removal, 499–500
Purpose-built vehicles, 73 wet, 498–499
Seawater scrubbing, 71
Secondary electrons (SEs), 126
Q
Secondary organic aerosols (SOAs), 481
Quality factor, 90
Secondary pollutants, 215, 387
Quantization noise, 430
Secondary standards, 387
Quartz crystal microbalance (QCM), 117, 118, 120
Selective catalytic reduction, 47
Selective catalytic reduction (SCR), 497
R Selectivity of sensor, 426
Radiative balance, 386 Sensitivity of gas sensor, 426
Radiative forcing (RF), 239, 282, 327, 347 Ship traffic, 201
Rail locomotives, 55 Sick building syndrome, 146
520 Index

Single crystal silicon, 433 passenger and freight transport in EU-27 countries,
Single-sided ventilation, 150 50, 51
Single-walled CNTs, 98 physical barriers, 74–75
Sixth mass extinction, 293 prevention measures, 67–74
Slip flow effect, 93 rail transport models, 60–61
Small-angle X-ray scattering (SAXS), 121 road sweeping and washing, 73–74
Smog, 10, 347 road transport models, 57–60
Smoking impact on ventilation, 142 shipping models, 61
SnO2, 433 traffic management, 74
Socio-ecological justice, 387, 409 transformation process, 63–64
Soils store carbon, 292 transport emissions, 57–62
Solar radiation management (SRM), 307–309 vegetation, 75
Soot particle AMS (SP-AMS), 126 Sustainability
Sound pressure level (SPL), 114 energy consumption, 295–296
Source apportionment, 387 food security, 293–294
Space charge, 424 greenhouse gases emission and economic
Stack-ventilation, 151 development, 297
Stationary sources, 347 health consequences, 294
Statistical model, 65 Hubbert’s peak theory, 296
Steam engines, 9 Jevon’s paradox, 297
Stratosphere, 373 monitoring and, 388, 407
Stratospheric pollution per capita GDP and energy consumption, 296
catalytic ozone loss, 374–375 Sustainable Development Goals (SDGs), 297
definition, 373
middle latitudes and tropics, 377
T
natural ozone layer, 374
Target load, 387
ozone depletion, 376–379
Taylor cone, 94
ozone layer, 374
Temperature inversion, 215, 347
polar ozone loss, 376–377
Temperature swing adsorption (TSA), 502
stratospheric chemistry, 375–376
Temporal, 347
Street canyon, 215
Thermal oxidation, 489–491
Subsidiary Body on Scientific and Technical Advice
Thermohaline circulation, 280
(SBSTA), 340
Thermophoresis, 109–112
Sulfur dioxide, 8
Three-way catalyst (TWC), 496, 497
Surface transportation impacts on air quality, 47–48
Time-of-flight (ToF)-AMS, 126
activity data, 61
Traffic management, 74
air pollution pathways, 51–53
Traffic situation models, 59
air quality legislation, 67
Transboundary pollution, 215
air treatment technologies, 75
Transit-oriented development, 387
automobile propulsion technologies, 71–72
Transmission electron microscopy (TEM), 127
car ownership in European countries, 50
Transport sector, heatwave impacts, 466–467
compressed natural gas, 71
Troposphere, 387
dispersion of pollutant, 62–63
Tubular precipitator, 493
dust suppressants, 74
Two-stage precipitator, 493
eco-driving, 72–73
emission legislation, 67–70
emission processes, 53–57 U
empirical/statistical models, 65 Ultrafine particles, 47, 205
Eulerian and Lagrangian model, 65 Unified Natural Hazard Risk Mitigation Exploratory
fuel legislation, 70 Decision Support System (UNHaRMED), 456
future research, 76–78 United Nations Environmental Programme (UNEP), 195
historical trends, 50–51 Urban air quality, 163, 194
hybrid propulsion, 72 air pollution, 198–199
improved combustion and exhaust aftertreatment, building and street scale, 170–173
70–71 building and street scale modelling, 178–179
liquefied petroleum gas, 71 characteristic regions of flow, 164–165
LPG and CNG, 71 complex urban junction, 186–187
mitigation measures, 74–75 computational models, 174–175
model validation, 77–78 concentration and indices, 199
Index 521

definition, 163 Urban form, 387


geography impact, 201–202 Urban heat islands (UHI), 464
and health effects, 197–198 Urban meteorology, 163
heavy metals, 210 Urban smog, 194
mesoscale, 165–167 Urban surface water management, 229
mesoscale models, 176–177 Utility factor, 433
meteorology impact, 202–203
neighborhood scale, 167–170
neighborhood scale models, 177–178 V
nitrogen dioxide pollution, 204 Vacuum swing adsorption (VSA), 503
origins of, 197 Vapor recovery, 502–503
output of modelling calculations, 179–186 Vehicle operation, 57
particle pollution impact, 204–209 Very short-lived species (VSLS), 373
polycyclic aromatic hydrocarbons, 209–210 Volatile organic compounds (VOCs), 142, 150, 198, 215,
topography impact, 202 284, 390, 480, 481, 485, 489, 491, 497, 498,
trace elements, 210–211 501, 504
urban data, 173–174 limited, 215
Urban atmospheric composition processes Vulnerability, 280
characteristics, motor vehicle and domestic fuel curve, 456, 469, 472
emissions, 220
composition and key pollutants, 218–219
condensed phase composition processes, 224–225 W
definition, 215 Water sector, heatwave impacts, 468–469
dynamics, 217 Wet deposition, 139, 347
evolution of air pollution vs. development, 216 Wet electrostatic precipitation (WESP), 107, 110, 111
gas-phase composition processes, 220–224 Wet precipitator, 493
historical perspective, 216 Wet scrubbers, 498–499
key emission characteristics, 219–220 Wetting filters, 439
meteorology, 217 Whitman v. American Trucking Associations, 21–22
mixing, 217 Winter smog, 194
urban atmospheric composition trends, 225–226 Wire-on-plate ESP (WOPEP), 109
Urban drainage modelling, 229 Wood combustion, 201
challenges in urban surface water, 230–231
flow on surface, 234–235
sewer system design, 231–234 Y
surface runoff, 231–234 Yttria-stabilized zirconia (YSZ), 95, 96
water transport into sewer system, 235

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