Environ. Sci. Technol.

2009, 43, 4620–4625

exposure to elevated levels of particulate matter (PM) in cities,

A Focus on Particulate Matter and and a staggering 1.8 million are similarly affected by smoke
Health from indoor solid fuel use (1). Together they rival “overweight
and obesity” as causes of premature death. In Europe, it has
been estimated that life expectancy is reduced by an average
ARMISTEAD G. RUSSELL* of 9 months as a result of exposure to anthropogenic fine
Georgia Institute of Technology particles (2). PM impacts go beyond health, including
climatological concerns (3, 4). It is the recognition of the
See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.

extent of PM-related health impacts that has led to this Focus

BERT BRUNEKREEF
issue with papers on topics tackling research challenges in
Universiteit Utrecht areas ranging from measurement to health (denoted by bold
reference numbers (5-24)).
Downloaded via 223.255.230.38 on February 15, 2022 at 10:50:03 (UTC).

Such research is timely: the U.S. EPA is in the middle of

Through analytical characterization, and toxicity end
epidemiologic studies, the health implications of airborne
particulate matter are slowly being elucidated.
SHUTTERSTOCK
its review of the Particulate Matter National Ambient Air
Quality Standards (PM-NAAQS), with a decision on revising
the standard in 2011. EPA’s supporting review (3) concludes
that there are likely causal relationships between both PM2.5
(PMd means particles with diameter < d µm) and PM10 with

cardiovascular and respiratory morbidity and mortality. Any

decision by the EPA administrator is likely to be controversial,
as it was with the last revision in 2006. While attention will
be on the fine, or PM2.5 standard, other issues include the
importance of ultrafine (PM0.1 [nanoparticles]), coarse
(PM10-2.5), and supercoarse (d >10 µm) sizes (25) and whether
particles of different composition or source have heightened
health concerns. Controversy was likewise experienced in
Europe when the 2008 decisions led to standards that in
several ways are less stringent than they were before and
certainly less tight than those in the U.S. (26).

Particles in the air might be tiny, but they are not benign.
An estimated 811,000 people worldwide die prematurely from
4620 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 43, NO. 13, 2009
Measurement
A major complexity in linking PM to health involves
measurement. Particles come in sizes ranging over 5 orders
of magnitude from about 2 nm to larger than 100 µm (for
examples, see figures in (8, 22, 23)), and can contain hundreds
of compounds. Health impacts are tied to both size and
composition (discussed below), driving the development of
new instrumentation.
Measuring aerosol (or particle) size distributions com-
monly has been done optically (e.g., optical particle counters
[OPCs]), but optical instruments have size-detection limita-
tions larger than the smallest particles of interest. Conden-
sation particle counters (CPCs) extend this range by growing
small particles with condensing vapors (27). Equilibrating
particle charge distribution and then separating them by
their mobility (large particles experience more drag), as is
done in electrical mobility analyzers (EMAs), allowed in-
vestigators to quantify even smaller particles. Currently, in
situ devices can quantify the number of particles down to
about 2 nm, which contain just a few molecules.
If both the size and composition is desiredsas is usually
the casesthe most common approach for characterizing the
size-resolved chemical composition of an aerosol has been
to use an impactor, which relies on the inertia of particles
to separate them from air (e.g., a multiorifice uniform deposit
impactor [MOUDI] (28)). Multiple stages allow for collecting
particles of increasingly small sizes, though this approach is
10.1021/es9005459  2009 American Chemical Society
Published on Web 06/01/2009
limited for particles below about 10 nm and sampling times
can be long. Aerosol mass spectrometers (AMSs e.g., (29))
can characterize PM size and composition in near real time,
though such instruments have limitations in terms of size
range and the type of compositional information provided.
As an alternative, McMurry et al. (8) present the adaptation
of an EMA to collect nanoparticles for chemical analysis. To
collect enough mass, the instrument operates at a low
resolution and a high flow rate. Sampled aerosol is then
quantified using off-line techniques. Looking forward, de-
velopment of cost-effective instruments to provide continu-
ous PM composition analysis is of most interest for providing
the type of information desirable for epidemiologic studies
and to support future regulation.
Emissions to Concentration: Sources, Controls,
Formation, and Transformation
A particle’s life can begin in a variety of ways (e.g., (30)),
including direct emission or formation in the atmosphere.
Characterizing emissions is difficult, being complicated by
measurement device limitations discussed above, and more.
No two sources are identical, and even emissions from the
same source will change with time and operating conditions.
Additionally, since particles undergo a variety of chemical
and physical transformations in the atmosphere, what is
measured at the source may not be what will be found in the
atmosphere. This is particularly true for organic species (31).
In this issue, three manuscripts address such complexities.
Grieshop et al. (7), investigating wood combustion and diesel
engine emissions, show that prior measurements of PM
emissions may overlook that a fraction of the semivolatile
organic compounds (SVOCs) and intermediate volatility
organic compounds (IVOCs) can evaporate when being
diluted with ambient air. In their presented analysis, they
use the concept of volatility distributions (or basis set), a
useful construct to facilitate atmospheric simulation (e.g.,
(17)), wherein the oxidation of organic compounds is
modeled as leading to a modificationstypically loweringsof
the vapor pressure. Murphy et al. (23) simultaneously
measured gases and particles in the stack of a post-Panamax
ship, as well as measuring the evolution of the emitted
particles using an airplane. The shipboard measurements
included characterizing the size-resolved chemical composi-
tion using an impactor, while the aircraft contained a suite
of technologies, including an AMS, CPC, and EMA. The range
of instruments allowed detailed investigation of PM proper-
ties: they found that the organic matter content increased,
relative to sulfate, and was primarily a hydrocarbon-like
material (having a low O to C ratio). Pakbin et al. (12)
examined emissions of PM from a diesel engine using
advanced control technologies. Both continuously regen-
erating technology (CRT) and having a selective catalytic
reduction (SCRT) device following the CRT showed reduc-
tions of organic species by about two or more orders of
magnitude.
Under certain conditions, particles can be formed directly
in the atmosphere from molecules with a very low vapor
pressure (e.g., sulfuric acid) forming molecular clusters which
then nucleate to form nanoparticles with diameters on the
order of 2 nm and can then grow further. One of the surprises
uncovered in the past decade is just how common these
nucleation events may be (e.g., 32, 33). Nieminen et al. (22)
push the limits of PM size measurements, using a chemical
ion mass spectrometer (CIMS) to measure individual sulfuric
acid molecules, and a combination of instruments to find
size-resolved particle concentrations down to just 2 nm. This
allowed them to follow the birth and growth of new particles.
Such information is critical to understanding the nucleation
process as different theories now compete to elucidate
empirical measurements.
A large fraction of the observed PM mass, however, is
added to preexisting particles by gas-to-particle conversion,
primarily from secondary organic matter (SOA) and sulfate.
While PM growth from inorganic species tends to be better
understood and quantified, the amount of SOA formed is
quite uncertain (e.g., (34)). Organic PM is of growing concern
as there is evidence that organic material may have greater
health impacts than sulfate (e.g., 35, 36). Gaseous organic
compounds that were once thought to have rather negligible
contribution to organic aerosol formation appear to be
anything but insignificant, as they can oxidize and oligimerize
to form low vapor pressure products (37, 38). Chan et al. (6)
conduct laboratory experiments of the oxidation of 2-methyl-
3-buten-2-ol (MBO), a compound emitted in pine forests,
finding it likely contributes little to SOA formation. MBO is
but one of hundreds of organic gases in the atmosphere.
Alternatively, Kourtchev et al. (10) approach understanding
SOA formation by measuring the chemical and size char-
acteristics of PM in a forest. They utilize a range of instruments
(e.g., MOUDIs and filter-based measurements, followed by
GC/MS analysis to give detailed organic speciation) to show
the importance of oxidation products of biogenically emitted
VOCs. The dominant mode of both secondary and primary
organic compounds was in the 0.1-1 µm range. Like in other
studies, only a fraction of the observed particulate organic
carbon is identified.
Presto et al. (20) pick up on the results of Grieshop et al.
(7), showing that the compounds that may have evaporated
during dilution can then oxidize and condense. Contrary to
other studies, they find that aerosol formation can increase
at higher NOx levels which can help explain the increased
oxygenated organic levels in cities.
Knowing the source of PM is of essential importance to
control ambient concentrations effectively. Given how a
particle is transformed in the atmosphere, identifying the
source is complicated (39). Beddows et al. (14) use a statistical
(or receptor) approach, somewhat different from the typical
species balance approach, conducting cluster analysis on
detailed particle size distribution measurements taken at
four sites: roadside, a ground-level and an elevated location
in London, and a more rural location. Their results show
that about 15 types of clusters are consistently found,
suggesting that this approach can be used for source
apportionment.
Murphy et al. (17) apply a chemical transport model (CTM)
to study regional scale PM dynamics. Here, they implement
volatility basis functions (discussed above and (7, 20)) to
simulate the evaporation of a fraction of the SVOC and IVOC
emissions, as well as to follow the atmospheric chemistry,
transport, and transformation of other gaseous and PM
emissions. Using this added flexibility appears to better
capture the regional dynamics of organic carbon PM. Major
uncertainties remain, including inputs such as emission rates
and speciation, as well as model process descriptions such
as resuspension of dust, nucleation, and the details of SOA
formation. Further, the question of how well we can quantify
the contribution of specific sources to ambient concentra-
tions remains open (40).
Concentration to Exposure
Being able to understand the sources of PM at the scale of
an urban area does not mean a similar understanding is
available for how individuals (or even populations) are
exposed. Individuals move from one microenvironment to
another, spending a large amount of time in buildings and
vehicles with limited time outdoors, such that an individual’s
exposure may not be similar to ambient measurements and
the corresponding emissions (41). Exposure modelingslinking
air quality model results with a model that simulates time-
VOL. 43, NO. 13, 2009 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 4621
activity patterns of thousands of individuals and pollutant
infiltration in to microenvironmentssplays a key role in
NAAQS reviews to estimate the distribution of population
exposures (42). However, given the lack of fundamental data
and process descriptions, this approach is largely limited to
the fine fraction of PM (PM2.5). Considerable work is required
to address ultrafine, coarse, and supercoarse exposures.
We spend most of our time indoors, notably in our own
homes. It is difficult to study indoor exposures to air pollution
on a large scale, so most of our information is from studies
information on differences in exposure among five trans-
portation modes: walking, cycling, and vehicular travel by
bus, car, or taxi. Not surprisingly, the highest percentage of
explained variance was found for PM0.1 counts, which were
lower for walking and cycling, and higher for the three in-
vehicle modes. However, the inhaled dose, could of course
still be higher in the more active modes of transport in view
of the higher levels of exertion associated with walking and
cycling.

SHUTTERSTOCK
in limited numbers of homes, such as that presented by Chen
and Hildemann (5), who analyzed PM size fractions and PM
components. PM in the fraction larger than 2.5 µm was found
to be strongly influenced by human activity. Previous work
(43) indicated that the smaller particles are much harder to
resuspend, which may be a reason for the findings reported
herein. Such elevated indoor exposures are of interest given
the emerging evidence of PM10-2.5 health effects, though we
have very little direct evidence of health effects of such
exposure from indoor environments.
A relatively new way to look at linking sources to potential
exposure is using intake fraction (44), applied herein by Ries
et al. (15), to assess the importance of wood smoke emissions
on exposure. While one source may emit a large amount of
PM, the amount of that material that actually makes it to a
human’s breathing zone might be rather small due to the
source’s characteristics; e.g., the source is not near a
populated area. Such knowledge can guide policies to more
effectively address sources leading to the greatest potential
exposure.
Over the past decade or so, interest in within-city contrasts
in air pollution exposure has soared. This was fuelled by
observations of high exposures to specific pollutants and
PM components near streets and of adverse health effects
among subjects living near roadways. Such near-roadways
exposures are complex as such regions can contain elevated
levels of both ultrafine (PM0.1) and supercoarse (d > 10 µm)
particles that are not present at such high levels further away
due to their limited lifetime. As a consequence, the need for
developing methods to estimate distributions of exposure Exposure to Dose
on a short spatial scale has increased. As making personal
measurements for long periods on large numbers of subjects Let’s say that we actually could quantify the PM to which an
is usually impossible, some form of modeling is needed. individual is exposed, the next question is ‘What fraction is
Dispersion modeling of the short spatial distribution has its actually taken up by the body?’, that is, the dose. Lungs are
limitations, and the use of land use regression (LUR) models quite complicated, and different parts of the respiratory
has proliferated. Overviews of the pros and cons of such system will see particles of many sizes and composition. While
models have been published recently (45). The measurement both laboratory and numerical modeling studies are often
effort to establish a database as input into the LUR models used to address lung deposition (e.g., 46, 47), Londahl et al.
can be substantial, especially when active sampling for PM (9) used subjects exposed to PM along a busy street, sized
or other substances is required. Larson et al. (11) provide an resolved pollutant measurements, and computer modeling
elegant example of mobile monitoring, obtained from to identify the deposition of PM1 particles in the lung. They
equipment mounted in a van that was driven along various find, in part, that there is a difference between the deposition
intersections and streets in Vancouver, BC. The amount of rates of hydrophobic and curbside particles, largely deter-
variance explained in the data acquired from this program mined by their hygroscopicity. Such results can be used to
was comparable to the variance explained by models based evaluate recent model developments, such as recent source-
on measurements obtained from more intensive stationary to-dose modeling that estimates the spatial- and source-
monitoring, which is promising. specific intake of pollutants (48).
With the increased interest in traffic pollution, including
not only exhaust emissions but also road, brake, and tire
PM Health Effects
dust, the question inevitably arises as to what extent PM is associated with a wide variety of cardiovascular- and
exposures to air pollution are elevated while in traffic. Early respiratory-based health effects, with responses to exposure
studies focused primarily on exposure to VOCs and CO, but being both acute (e.g., increased hospital admittances for
more recently emphasis has shifted to particle metrics, as is respiratory disease or premature mortality from cardiovascular
done by Miller-Schulze et al. (24), studying taxi drivers in disease) and chronic (reduced longevity in cities with higher
Shenyang, China. Measurements inside and outside taxis, as PM levels); there are also indications of reproductive and
well as at the drivers’ homes, found elevated levels of some developmental effects (3). Studies to better understand such
particulate nitro-polycyclic aromatic hydrocarbons (NPAHs) responses typically take one of three forms: clinical, toxicologic,
in taxis, but other NPAHs appear to be formed in the or epidemiologic.
atmosphere, leading to more uniform, albeit still elevated, Toxicology. Specific mechanisms that lead PM to have the
levels near roads. Nieuwenhuijsen et al. (19) provide range of observed health impacts are still quite uncertain, and

4622 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 43, NO. 13, 2009
given the variety and degree of observed health associations,
it is likely that more than one is involved. Mechanistic studies,
including those using human exposure to concentrated PM,
have considerably increased our insights into how PM causes
pulmonary and cardiovascular effects (49, 50). Pulmonary effects
are associated with cellular injury and inflammation, and,
increasingly researchers are finding that reactive oxygen species
(ROS), either in the PM or produced by stimulated cells, can
play a role (3). PM species of most interest include metals and
some oxygenated organics (e.g., quinones). Hypothesized
responses include up-regulating antioxidant enzymes, cell
death, allergic immune response, impairing lung defense, and
DNA damage (3, 51, 52). Damage can also continue to other
parts of the body (e.g., the cardiovascular system).
A few studies suggest that working in traffic is associated
with increased levels of specific biomarkers (e.g., (53)). Wei et
al. (21) used repeated urine sampling of two campus security
guards exposed to heavy traffic. Postwork-shift urinary con-
centrations of 8-OHdG, a biomarker for oxidative DNA damage,
were associated with on-site measurements of PM2.5 as well as
PAH and metal content.
Recent toxicologic or epidemiologic studies show that there
is still much inconsistency in findings related to different size
fractions. Duvall (54) in a U.S. based in vitro study of particles
collected in six urban areas did not find that coarse PM (PM10-2.5)
was associated with markers of lung injury or inflammation,
whereas PM2.5 was. In contrast, Wegesser et al. (55) in a study
of PM10-2.5 collected in a hot, rural area in the southwest U.S.
found that PM10-2.5 was associated with pro-inflammatory
effects in the lungs of mice after intratracheal instillation.
Gerlofs-Nijland et al. (18), using PM-exposed hypersensitive
rats, found that PM10-2.5 actually led to a stronger effect per
mass than fine particles, and that the positive correlations were
associated with particles containing PAHs and metals.
Epidemiology. Given the many complexities and uncer-
tainties in identifying the responsible biological mechanisms,
the primary approach used to link PM to various health end
points is through epidemiologic analyses. Whereas this research
provides a very comprehensive and broad picture, the inevitable
inconsistencies between at least some of the studies lead to
further questions and difficulties of interpretation. One such
question relates to the health effects of PM in different size
fractions. The focus from a regulatory point of view in both
North America and, more recently, Europe, has been on PM2.5.
However, it is not so clear whether larger, but still inhalable
particles up to 10 µm in aerodynamic diameter are less harmful.
A 2005 review of the evidence for PM10-2.5 and PM2.5 effects on
mortality (56) found very little evidence of effects of PM10-2.5 on
mortality independent from those of PM2.5.
Intriguing results come from a time series study in Barcelona
(16) showing effects of PM10-2.5 and PM1 on cardiovascular and
cerebrovascular mortality, and effects of the “in between”
PM2.5-1 fraction on respiratory mortality. This being a single-
city study, the statistical power to truly separate effects of
different size fractions from each other is not large, suggesting
replication in larger data sets rather than changes in regulatory
practice are warranted at this time. Wilson et al. (57) found
PM10-2.5 had a considerable effect on cardiovascular mortality
in Phoenix, AZ, but only when assessed for a population living
fairly close to the monitor. However, in another large U.S. study
of 3,700,000 cardiovascular and 1,700,000 respiratory hospital
admissions, there were no associations between PM10-2.5 and
admissions after adjustment for PM2.5 (58).
The new studies, along with the EPA review, suggest that
the balance is shifting toward stronger evidence for PM10-2.5
leading to premature mortality, but it needs to be recognized
that these relatively small, single-city studies are reporting effect
estimates for PM2.5 many times larger than those found in large
multicenter studies (59). It remains to be seen what the verdict
of effects of PM10-2.5 on mortality will be after more and larger
studies have been published. An example is the Multi-Ethnic
Study of Atherosclerosis (MESA) AIR study (13), one of the most
ambitious studies on the health effects of air pollution ever
undertaken. Studying an existing cohort of subjects participating
in a study on atherosclerosis development, the investigators
are first conducting a very detailed exposure assessment, ranging
from personal and in-home monitoring to modeling and
assessment of how individuals spend their time (i.e., time
activities), to be followed by epidemiologic analyses. First results
of the exposure assessment show a fairly large variation of PM2.5
exposures between cities, but within at least some cities the
variation is small. As this study is further extended over the
next several years, its size and detail should provide more
definitive results than previously available.
Looking Forward
The link between PM and adverse health effects is becoming
more clear, though a number of questions remain open that
hinder our ability to set policies that would provide the greatest
benefits. Worldwide, much of the harm, currently, comes from
indoor exposure to burning solid fuels, a problem that could
be mitigated relatively straightforwardly (60). Exposure to
outdoor-generated PM is more complex. Research areas that
appear to present the greatest challenges and hold keys to
significant health benefits include understanding SOA forma-
tion both from a fundamental and operational standpoint,
linking sources to exposure, and identifying what component
or size of PM is most responsible for the observed health effects.
While the specific mechanisms that lead to the various health
effects associated with exposure to PM are still unclear and
need to be elucidated, current evidence tends to suggest that
the organic fraction and/or metals appear to be of most concern,
and act via oxidative stress. Studies of the impacts of coarse,
fine, and ultrafine particles are conflicting, and there is very
little information about the potential impacts of supercoarse
particles. It is apparent that multiple approaches are required.
Combining mechanistic studies of concentrated real world
ambient particles with observational studies of subjects exposed
to PM with the same characteristics will further improve our
insights into which particle exposures really matter. Such
information can then identify appropriate control programs
and hopefully improve everyone’s health and well-being.
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