Legacy Problems in

Urban Geochemistry
During the “Great
Smog Event” in London
in 1952, conductors
Stefano Albanese1 and Domenico Cicchella2 walked in front of buses
holding torches or flares
in order to see street
1811-5209/12/0008-0423$2.50 DOI: 10.2113/gselements.8.6.423 signs. R EPRODUCED WITH
PERMISSION OF BBC

M
odern cities are affected by multiple sources of contamination and FROM THE
pollution, the effects of which overlap in space and time. Toxic metal FIRST SETTLEMENTS
contamination, organic pollution, smog, acid rain, and greenhouse TO THE MEGACITIES
OF THE 21st CENTURY
gas accumulation are the most widespread legacies of an often uncontrolled
Pollution problems first arose when
growth that has deeply changed the geochemical character of the urban more than just a few people began
environment over the last four millennia. Even though progress has changed living together in the earliest
human habits and positively influenced the quality of city life, the past is villages and towns. The “Neolithic
Revolution” (8000 –5000 BC)
frequently a hidden source of environmental problems with the potential to represents the starting point in the
affect the health of current and future urban residents. history of the city, with the estab-
lishment of permanent villages in
KEYWORDS : urban environment, megacities, toxic metals, smog, acid rain,
which groups of people became
public health
agrarian and sedentary. With the
progress of technology, the domes-
INTRODUCTION tication of animals, and the inven-
tion of more effective tools for agriculture, for example, the
Urban areas now accounts for more than 60% of the
iron plough, food production also increased. This agricul-
populations of most of the world’s developed countries.
tural surplus could be used to feed an urban population
As conditions deteriorate, urban residents have only two
engaged in activities other than farming, for example,
options: they can cohabit with progressive environmental
the production of manufactured goods that improved the
degradation or they can move away from the city into
quality of life. It was probably during this period that the
the countryside (where that still exists!), thus sacrificing a
environment of villages and towns started to be affected
whole range of facilities and quality of life of one kind in
by pollution from waste disposal and primitive manufac-
favor of a healthier environment. However, many people
turing. The extent of pollution increased proportionally
cannot realistically abandon the city for reasons of business
with the growth of cities.
or employment, while others are addicted to the pace and
chaos of the urban environment and cannot even imagine As early as 400 BC, Hippocrates associated the city with
living without smog and noise. pollution and ill health. Streams and rivers running
through a settlement often served as both the prime
Over the last 4000 years, technological progress has
source of drinking water and the public sewer. The fi rst
changed the livability and quality of urban environ-
pollution of the environment was likely human excre-
ments, not always influencing them for the better. Such
ment and animal waste dumped directly into the street.
progress has often left a long-term legacy of environmental
For centuries the streets of major urban centers worldwide
problems that have the potential to negatively affect the
were fouled with horse feces and urine, and often with
health of succeeding generations. For example, a study by
the dead bodies of the animals themselves. An inscription
David and Zimmerman (2010) supports the hypothesis that
dating back to 440–430 BC found near the Acropolis of
the increase of cancer incidence in industrialized societies
Athens reports that leather tanning and disposal of waste
is a consequence of the effect of environmental conditions
were not permitted in the Ilissos River upstream from the
on the quality of life. These researchers studied nearly a
Temple of Heracles, since these activities would result in
thousand mummies from ancient Egypt and South America
air and water pollution and possibly in the mortality of
dating back some 3000 years and found that very few of
animals and children.
the ancient individuals had suffered from cancer: the few
tumors observed were mostly benign, unlike today when In 61 BC, Lucius Annaeus Seneca, the famous Roman
cancer causes nearly one-third of total deaths. philosopher, wrote in his Epistulae Morales ad Lucilium
(Liber XVII-XVIII, Epistula 104): “As soon as I walked
away from the heavy air of Rome and from the stench of
steaming kitchens spewing pestilential vapors and soot
onto the city, I felt a feeling of well-being…” At almost the
1 University of Napoli “Federico II”
Department of Earth Sciences same time, the lyric poet Horace (Quintus Horatius Flaccus)
Via Mezzocannone 8, 80134 Napoli, Italy complained about the annoying fumus (smoke) covering
E-mail: stefano.albanese@unina.it the city and blackening buildings (Neumann 1979).
2 University of Sannio
Domestic activities (heating and cooking), together with
Department of Biological, Geological and Environmental Sciences
Via dei Mulini 59/A, 82100 Benevento, Italy the production of metal tools, were probably the most
E-mail: cidom@unisannio.it common sources of contamination in ancient urban

E LEMENTS , V OL . 8, PP. 423–428 423 D ECEMBER 2012

environments. The widespread poisoning of Roman
citizens due to lead (Pb) water pipes is the subject of a
historical debate on causes contributing to the decline of
the Roman Empire (Retief and Cilliers 2006 and references
therein). Although it is not possible to know if lifelong Pb
uptake by its urban citizens was responsible for the demise
of the Roman Empire, researchers have demonstrated that
domestic water supplies made of or sealed by Pb were
widespread throughout Roman cities, that leaded paints
and compounds were present in medicines and cosmetics,
that wine was prepared in pewter or leaded containers,
and that “syrup of wine” (sapa) was added to food; all of
these were sources of Pb poisoning in the daily lives of the
Romans (Retief and Cilliers 2006 and references therein).
During Roman times, the need for large amounts of Pb,
together with metals like Cu, Zn, and Hg, for the manufac-
ture of weapons and tools created a strong demand for
mining and metalworking. This generated an additional
source of environmental pollution, and such activities were
prohibited in the vicinity of many cities (Nriagu 1996).
Urban lead pollution is discussed in detail by Filippelli et
al. (2012 this issue).
At its peak, the Roman Empire probably used 80,000 tons
of lead annually. Needleman and Needleman (1985) quote
sources that estimate an annual lead production during
the fi rst two centuries BC of approximately four kilograms
per capita, which equates to two-thirds of the annual per
capita lead consumption in the United States during the
1970s. As a consequence, Pb and Hg pollution related to
metalworking and the production of weapons within the
Roman Empire between 600 BC and 300 AD was so intense
that the concentration of these elements in the troposphere
increased globally, as recorded in Greenland ice (FIG. 1;
Hong et al. 1994).
Anthropogenic metallurgical impacts during the medieval
era were much smaller and seem to have affected more
restricted areas as compared to those of the Roman period.
However, from Europe to the Far East, smoke generated
from the burning of coal in the furnaces of blacksmiths,
from manufacturing activities, and from domestic heating
was a source of Cu and Pb pollution in urban environments
(Griffi n 2007). After 1400 AD, urban pollution probably
increased in conjunction with a new period of economic
expansion. Metal production in Europe reached its peak
about 1530 AD, after which mining and metal produc-
tion declined as a result of increased exploitation of metal
resources in the Americas (Nef 1987). The historical data on
lead and silver production in Europe are remarkably consis-
FIGURE 1 Pb concentration in Greenland ice over the last
8000 years. FROM HONG ET AL. (1994), REPRINTED WITH
PERMISSION FROM AAAS
E LEMENTS
tent with the history of atmospheric pollution recorded in
the varved lake sediments of northern Sweden (Brännvall
et al. 1999).
Extreme deterioration of urban air quality accompanied
the advent of the Industrial Revolution in the middle of
the 18th century, as a consequence of the invention of the
coal-fi red steam engine. The steam engine, together with
other advances in technology that led to more produc-
tive manufacturing processes, caused investors to transfer
manufacturing plants away from naturally flowing waters
outside the city and into urban centers where labor was
more abundant, thus generating a massive increase in the
number of urban factories. As a consequence, the environ-
mental quality of industrial cities greatly deteriorated as
a result of the large increase in atmospheric emissions
produced by the burning of fossil fuels and the local
disposal of waste.
Even though the Industrial Revolution caused a huge rural-
to-urban migration, only 15% of the world’s population
lived in cities at the beginning of the 1900s: it was only
in the 1950s that urban growth peaked, with a population
expansion of more than 3% per year. In the early 1960s,
the transition of the urban economy from the production
of goods to the provision of services represented the birth
of the modern (postindustrial) city. Today, more than half
the world’s people live in cities and, at present, there are
about 20 cities worldwide with a population of 10 million
or greater and 30 with a population exceeding 7 million
(United Nations 2012). These numbers are expected to
grow considerably in the near future. Urban areas with
more than about 5 million people are called megacities,
and such concentrations of people and their activities have
environmental consequences at urban, regional, conti-
nental, and global scales.
UNDERSTANDING THE LEGACY
Air
In modern cities, the major source of contamination is
fossil fuel combustion, particularly motor vehicle exhaust.
Such emissions introduce particulate metals (e.g. Pb, As,
Cr, Hg), volatiles (e.g. oxides of C, S, N), volatile organic
compounds (VOCs), and polycyclic aromatic hydrocarbons
(PAHs)—all of which are harmful—into the troposphere,
onto the soil through the fallout process, and then into
urban water courses via storm-water runoff (Albanese and
Breward 2011).
Since the beginning of the Industrial Revolution in the
mid-1700s, the atmospheric concentration of CO2 has
increased by about 30%. Recent data indicate that the
current growth rate of this greenhouse gas is comparable
to that recorded during the 1980s (Hansen and Sato 2004).
If this global emission growth rate is maintained, the
atmospheric CO2 concentration will reach 500 ppmv by
the end of this century, a value that is almost double the
preindustrial (280 ppmv) baseline concentration (FIG. 2).
Bellucci et al. (2012 this issue) discuss the urban green-
house gas problem in more detail.
In 1911, the term smog, a contraction of the words smoke
and fog, was introduced into the scientific lexicon. Its
fi rst use was in reference to the air-quality situation in
Glasgow and Edinburgh, Scotland, where in 1909 more
than a thousand people died from exposure to a mixture
of smoke, fog, and sulfurous gases. At the beginning of
the 20 th century, coal-fi red electrical power plants and
domestic heating were the major sources of air pollution
in urban areas; coal was still the most widely used fuel until
424 D ECEMBER 2012

The concentration of CO2 in the atmosphere has
FIGURE 2
greatly increased across the last two centuries, from a
preindustrial concentration of about 280 ppmv to about 390 ppmv
in 2010 (ppmv = parts per million by volume). This increase has
closely followed the growth in emissions from fossil fuels. CO2
concentration data are from Antarctica ice-core measurements
(before 1958) (Etheridge et al. 1998) and from Mauna Loa (after
1958) (Keeling et al. 2009).
the transition from solid fuels to oil and gas in the 1940s.
The global rise in the use of motor vehicles for individual
and family transport happened shortly thereafter.
However, a more global awareness of the danger to human
health arising from urban air pollution was reached only
after the “Great Smog” event, which affected London in
December 1952. The dense fog produced a sudden rise
in mortality, with 3500–4000 more people dying than
would normally have been expected, due to pneumonia,
bronchitis, tuberculosis, and heart failure. The smog was
generated by the combined emissions of local industry and
approximately one million coal-fi red stoves and home-
heating fireplaces across the city, aided by unfavorable local
weather conditions. Thousands of tons of black soot, tar
particles, and sulfur dioxide accumulated in the air from
FIGURE 3 Effect of photochemical smog on the skyline of Mexico City. SOURCE : YU
E LEMENTS
the combustion of coal. The exceptional number of deaths
spurred the British government to pass the 1956 Clean Air
Act, which gave local governments the authority to provide
funds to households to exchange their coal-fi red heaters
for cleaner sources of energy, such as gas, oil, smokeless
coal, and electricity.
Also in the early 1950s, the adjective photochemical was
added to the traditional term smog to introduce a new
concept in air pollution. First observed in Los Angeles, this
condition results from complex photochemical reactions
related primarily to UV radiation in sunlight. The forma-
tion of photochemical smog involves precursors such
as nitrogen oxides (NOx, including NO, N2O, and NO2 ),
carbon monoxide (CO), sulfur dioxide (SO2 ), unburned
hydrocarbons, and eye irritants such as formaldehyde,
interacting to form a mixture of compounds in the lower
layers of the troposphere (FIG. 3). Generally, these precur-
sors are emissions produced by the combustion of fossil
fuels, mostly by motor vehicles.
Photochemical smog is the result of a sequence of chain
reactions, generally leading to the formation of ozone (O3)
and some reactive organic compounds, such as peroxy-
acetyl nitrate (PAN), that are harmful to human health,
specifically affecting the eyes, nasal passages, and lungs.
In addition to contributing to photochemical smog, sulfur
oxides (SOx) and, to a lesser extent, NOx are also implicated
in the formation of “acid rain.” The term generally refers
to the process whereby these gases react in the atmosphere
with water, oxygen, and other chemicals to form various
acidic compounds (Menz and Seip 2004). Fallout from the
atmosphere can occur either as wet deposition, in the form
of rain, snow, fog, dew, etc. containing dilute sulfuric acid
(H 2 SO4) and nitric acid (HNO3), or as dry deposition of
SOx and NOx (FIG. 4).
For several decades, rainfall, snow, fog, and dew with
pH values between 2 and 5, significantly lower than the
common natural value of 5–6, have been recorded in many
parts of the world. In urban areas, the accumulation of
acids, through either wet or dry deposition, accelerates the
decay of both buildings and historic cultural monuments
(FIG. 5).
YU
425 D ECEMBER 2012

FIGURE 4 The acid rain cycle. The chemical precursors to acid
rain can be from natural sources, such as decaying
vegetation and volcanic emissions, or from anthropogenic sources,
primarily sulfur dioxide (SO2) and nitrogen oxides (NOx) produced
by the combustion of fossil fuels. When present in the atmosphere,
these gases react with water, oxygen, and other chemicals to form
weak sulfuric acid and nitric acid solutions. VOC = volatile organic
compounds; NOx = nitrogen oxides.
SOURCE : WWW.EPA .GOV /ACIDRAIN /WHAT/INDEX.HTML
With the rise in the use of diesel fuels, sulfate deposition
was accompanied by the accumulation of soot responsible
for the formation of the black crust that covers European
monuments from Florence to London (Bonazza et al. 2004).
This black crust is mostly made of a noncarbonate-carbon
fraction, and the surfaces of the stone monuments affected
by blackening usually show intercrystalline decohesion and
the development of fractures fi lled by black particles and,
eventually, gypsum (Bonazza et al. 2004).
Soil
Metals and metalloids adsorbed to particulate matter are
also produced by combustion processes. These are gener-
ally deposited on the ground either in elemental or in
compound form after a variable residence period in the air.
Such materials are generally enriched in the soils of devel-
oped urban centers. Furthermore, the chemistry of modern
urban soils has become even more complex and compli-
cated as a result of decades and even centuries of contribu-
tions from several previously unrecognized sources, such
as the oxidation of paints covering the exterior walls of
buildings, the rupture of underground sewage pipes, the
use of herbicides along public roads and in private gardens,
E LEMENTS
and the mechanical wear of automobile parts (tires, brakes,
engine belts, mufflers, etc.) that contain high levels of toxic
elements (TABLE 1). Toxic elements introduced into urban
soils from the atmospheric deposition of dusts (derived
from both industrial processes and fossil-fuel combustion)
represent a major concern for human health because they
are highly bioavailable, owing to their easily extractable
form (Albanese 2008; Filippelli et al. 2012).
Throughout the 20 th century, Pb was one of the elements
most contaminating urban environments (FIG. 6). This was
a consequence of urban smelters, lead’s use as a pigment
and drying agent in paint, and its presence as tetraethyl
lead in gasoline (Cicchella et al. 2008a) for use as an
antiknock additive (Filippelli et al. 2012).
Generally, urban soils are a sink for most of the solid and
chemical pollutants deposited by atmospheric fallout.
The legacy problem described above for leaded gasoline is
today compounded by the additional problem of catalytic
converters, which introduce platinum group elements
(PGEs), mainly Pt and Pd, into the environment. Cicchella
et al. (2008b) showed that high PGE concentrations overlap
substantially with Pb anomalies in the soils across the city
road network in Naples, Italy.
Another negative legacy of the early industrial history
of many cities is the presence of urban brownfield sites,
which are abandoned industrial sites that release inorganic
and organic pollutants to the surroundings (Thornton et
al. 2008). Such sites often represent a real health risk for
residents: it is estimated that there are between 400,000
and 500,000 brownfields in the USA (Litt and Burke 2002),
300,000 to 1.5 million in Europe (van Calster 2004), and
over 30,000 in Canada (NRTEE 2003). As large metropol-
itan centers grow and expand outward, brownfield sites are
often attractive locations for residential redevelopment.
To avoid harm to human health, it is important that this
situation be recognized and that brownfield sites be appro-
priately remediated before being put to alternative use.
The Bagnoli brownfield area in the western sector of the
city of Naples is a didactic example of how a former indus-
trial site can continue, even after several years, to represent
a risk to both the environment and local residents by
releasing metals and organic compounds to the surround-
ings. Albanese et al. (2010) showed that westward-flowing
groundwater contaminated by the Bagnoli industrial site
has produced striking contamination levels of toxic metals,
PAHs, and polychlorinated biphenyls (PCBs) in the marine
sediments of the Gulf of Naples estuary.
FIGURE 5 A sandstone
statue in
Westphalia, Germany,
photographed in 1908
(left) and again in 1968
(right). PHOTO : H ERR
SCHMIDT-THOMSEN
426 D ECEMBER 2012
 this end within Europe through the Urban Wastewater
Treatment Program and the Integrated Pollution Control
and Prevention Program, which are a part of the European
Union Water Framework Directive.

As a consequence of such national and international legisla-

tion, water pollution from point sources has been greatly
reduced in postindustrial cities, so that today, storm-water
runoff has become one of the most important sources of
pollution to urban stream waters. Indeed, the creation of
impervious surfaces throughout urban environments as
a consequence of paved streets, parking lots, sidewalks,
building roofs, and residential lawns causes rapid runoff
and collection of rainfall, which, in turn, allows storm-
water runoff to collect inorganic and organic contami-
nants as well as entrain sediment from construction sites
and roadways.

Storm waters have become a major environmental issue at

FIGURE 6 Interpolated Pb-content distribution in topsoil in
Naples, Italy. The majority of sampled soils (73%)
have a Pb content that exceeds the local background values
(<80 mg/kg). Pb concentrations exceed the 100 mg/kg residential/
recreational intervention limit in 62% of sampled soils, and 2%
exceed the commercial/industrial intervention limit of 1000 mg/kg.
A Pb-isotope investigation demonstrated that vehicular traffic is
the predominant source of Pb pollution in Naples.
FIGURE BY DOMENICO CICHELLA
Water
As previously discussed, water pollution has been an urban
environmental problem since cities were fi rst established,
despite the development of the fi rst urban sewer systems
in the Middle East more than 3000 years ago. In the latter
half of the 19th century and into the 20 th century (Staley
and Pierson 1899), many cities constructed extensive sewer
systems as part of a trend of municipal sanitation programs
to help control outbreaks of disease. In 1972 the United
States enacted the Clean Water Act to control water pollu-
tion. Since that time, many nations have followed this
example and developed legislation to conserve surface-water
resources. Today, there is a transnational initiative toward
the urban scale, especially in cities equipped with obsolete
and/or combined sewage treatment plants that accept both
urban drainage and sanitary waters. Such plants are not
capable of receiving and treating the great volumes of
water generated during large rain events and, as a conse-
quence, frequently produce overflows of untreated water
that severely pollute receiving water bodies downstream.
Furthermore, obsolete treatment plants are generally
characterized by a low removal efficiency of contaminants
from the final effluent, especially salts, soluble phosphorus,
bacteria, endocrine-disrupting chemicals (EDCs), and
pharmaceutical and personal-care products (PPCPs), which
have only recently been recognized as a potential human
health threat (see Wong et al. 2012 this issue). Although
often less persistent in the environment than conventional
contaminants, EDCs and PPCPs have been detected in the
urban watercourses of several world cities (Ellis 2006 and
references therein). They form two groups of the so-called
emerging contaminants—compounds used in everyday life,
such as pharmaceuticals (antibiotics, steroid hormones,
antidepressants), domestic and industrial detergents, plasti-
cizers, antifungals and antibacterial agents, and various
industrial additives—that are suspected to be harmful to
health if ingested into the human body.
CONCLUSIONS
The urban environment arguably represents the most
complex system of interactions between humans and
their environment. The multiplicity of the sources, the
multilayered stratification of pollutants, the complexity

TABLE 1 ANTHROPOGENIC SOURCES OF HEAVY METALS IN URBAN SOILS

INDUSTRY/SOURCE Cu Pb Zn Sn Cd Hg Ni V Cr As Sb Others
General urban activity + + + +
Mining (coal) + + +
Smelting ( nonferrous) + + + + + + + + +
Iron-and-steel work + + + + + + Ca, P2O5
Heavy engineering, toolmaking + + + + + Mn, Mo, W
Metal plating and fining + + + + + +
Electronics + + + + + + REEs, rarer elements
Ceramics, glass + + + Mn, Co, U, REEs
Incinerators + +
Domestic coal-burning and coal-fired
+ + + + +
power stations (ashes)
Vehicles, transport + + + + + + Ba, Mn
Crematoria +

SOURCE : R EIMANN AND DE C ARITAT (1998 and references therein); REEs = rare earth elements

E LEMENTS 427 D ECEMBER 2012

of exposure pathways, and the changes induced on the
environment make it difficult to assess the role that each
phenomenon has had on the quality of life of urban
populations and on the development of specific environ-
mental problems or public health issues. Today, awareness
of urban environmental problems is certainly higher than
in the past, since people living in cities every day encounter
difficulty in breathing or in fi nding a healthy place where
their children can play. National and local governments,
although with different levels of involvement, have put in
place countermeasures to reduce pollution and to improve
the quality of life of citizens. Unfortunately, urban dwellers
often still do not perceive the worsening of the environ-
mental conditions to be dependent on their own behavior.
Although they may complain about the degradation of the
city environment, urban citizens do not necessarily act
to reduce their contribution to pollution by minimizing
unnecessary energy and material consumption, utilizing
sensible waste-recycling measures, or limiting the use of
personal motor vehicles. Also, time has a big influence on
the effects of urban contaminants on public health due
to their frequently long residence time in contaminated
media. For example, the presence of contaminants such
as toxic metals and PCBs can be easily forgotten, causing
future generations to be exposed to dangers of which they
are unaware. Although cities may be the worst places to live
in terms of human health, the perceived benefits of urban
life cause cities to continue growing and expanding. For
long-established cities, expansion is toward the outer areas
of the urban domain, which in the past were frequently the
location of industrial activities likely to have left contami-
nated soils and buried toxic wastes as a legacy of their
former presence.
Today, geochemical mapping at the urban scale is the
primary tool for understanding the complexity of the
distribution patterns of contaminants, especially in soil
(see Filippelli et al. 2012). Its main objectives are to deter-
mine the baseline abundances of potentially toxic elements
and to identify areas with concentration values exceeding
prescribed guidelines; in such areas, it is necessary to assess
the risks to human health and to start reclamation prior
to residential development

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