Aerosols and Environmental Pollution

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Naturwissenschaften (2010) 97:117–131

DOI 10.1007/s00114-009-0594-x

REVIEW

Aerosols and environmental pollution


Ian Colbeck & Mihalis Lazaridis

Received: 20 February 2009 / Revised: 15 July 2009 / Accepted: 16 July 2009 / Published online: 2 September 2009
# Springer-Verlag 2009

Abstract The number of publications on atmospheric Introduction


aerosols has dramatically increased in recent years. This
review, predominantly from a European perspective, sum- An aerosol is defined as a stable suspension of solid and
marizes the current state of knowledge of the role played by liquid particles in a gas. The term aerosol originates from
aerosols in environmental pollution and, in addition, high- military research during World War 1. The name is
lights gaps in our current knowledge. Aerosol particles are associated with Professor F.G. Donnon (Whytlaw-Gray et
ubiquitous in the Earth’s atmosphere and are central to al. 1923), although first publication of the term was due to
many environmental issues; ranging from the Earth’s Schmauss (1920) where it was used as an analogy to
radiative budget to human health. Aerosol size distribution hydrosol, a stable liquid suspension of solid particles.
and chemical composition are crucial parameters that Aerosol particle sizes range from 0.001 to 100 µm, hence,
determine their dynamics in the atmosphere. Sources of the particle sizes span over several orders of magnitude,
aerosols are both anthropogenic and natural ranging from ranging from almost macroscopic dimensions down to near
vehicular emissions to dust resuspension. Ambient concen- molecular sizes (Hinds 1999; Seinfeld and Pandis 2006).
trations of aerosols are elevated in urban areas with lower Particles much greater than 100 µm do not stay airborne
values at rural sites. A comprehensive understanding of long enough to be measured and observed as aerosols. The
aerosol ambient characteristics requires a combination of lower limit is controlled by the size of a cluster of half a
measurements and modeling tools. Legislation for ambient dozen or so molecules: this is the smallest entity of the
aerosols has been introduced at national and international condensed phase that can exist.
levels aiming to protect human health and the environment. Particles in the atmosphere consist of a mixture of solid
particles, liquid droplets, and liquid components contained
Keywords Aerosols . Particulate matter . Aerosol sources . in the solid particles. Particles are variable in relation to
Particle emissions their concentration, as well as to their physicochemical and
morphological characteristics. Particles can be products of
Electronic supplementary material The online version of this article combustion, suspension of soil materials, and suspension of
(doi:10.1007/s00114-009-0594-x) contains supplementary material, sea spray, and can also be formed from chemical reactions
which is available to authorized users. in the atmosphere. It can be concluded that airborne
I. Colbeck (*) particulate matter (PM) is a complex mixture of many
Department of Biological Sciences, University of Essex, different chemical species originating from a variety of
Colchester CO4 3SQ Essex, UK
sources.
e-mail: [email protected]
Aerosols have diverse effects ranging from those on
M. Lazaridis human health to visibility and climate forcing. Aerosols are
Department of Environmental Engineering, also very important for public health and the understanding
Technical University of Crete,
of their dynamics is important for the quantification of their
Polytechneioupolis,
Chania 73100, Greece effects (US-EPA 2004; Position Paper on PM 2004;
e-mail: [email protected] Andreae and Rosenfeld 2008). They are important in
118 Naturwissenschaften (2010) 97:117–131

numerous technological applications such as the delivery of air quality studies and climate impact investigations require
drugs to the lungs, delivery of fuels for combustion, and the information about the vertical distribution of aerosols in the
production of nanomaterials. atmosphere, which is usually not available from existing air
We often assume that air pollution is a modern phenom- quality monitoring networks.
enon and that it has got worse in recent times. However, since During the past decade, sophisticated computational
the dawn of history, mankind has been burning biological and procedures have been developed and successfully tested that
fossil fuel to produce heat. The walls of caves, inhabited permit the retrieval of microphysical properties of particles
millennia ago, are covered with layers of soot and many of the such as volume and surface area concentration, effective
lungs of mummified bodies from Paleolithic times have a radius, refractive index characteristics, and single scattering
black tone (McNeill 2001; Grossi and Brimblecombe 2008). albedo. The variables are derived with inversion algorithms
Zimmerman (2004) concluded that continual exposure of which use the measured optical particle properties as input
early man to campfires in enclosed areas contributed to (Veselovskii et al. 2002, 2004; Ansmann and Müller 2005).
increased incidences of nasal cancer. The nature of air Approaches of combining lidar and sun photometer data
pollution has changed over the millennia. No longer is it have been undertaken recently. A combination of spectrally
predominantly smoke-related and sulfur-related but now it is resolved optical depth measured with sun photometer and
associated with nitrogen oxides, volatile organic compounds, backscatter coefficients measured with Raman lidar was
and PM connected with the growing traffic emissions used to explore the possibility of deriving the microphysical
(Morawska et al. 2008; Fenger 2009). properties mentioned above (Pahlow et al. 2006). Results
Recently, concern has been raised with respect to the from these studies are quite promising but certainly are only
effect of PM on human health, following a number of at the beginning of more detailed investigations.
epidemiological studies in cities with different pollutant Fine particles have intrinsically low sedimentation and
levels (Mauderly and Chow 2008; Position Paper on PM deposition velocities, and their atmospheric residence time
2004). These studies show clear correlations between is of the order of days. Particulate pollutants from source
particulate pollutant levels and adverse health effects. regions in Europe and Russia have been observed in the
Toxicological studies also show an effect to human health Arctic and even in Arctic Canada and Alaska (Xie et al.
from suspended PM but for concentrations much higher 1999). Furthermore, emissions of PM from other continents
than those encountered in ambient air (Schlesinger 1995). reach Europe. A typical example is the Saharan dust
In conjunction with the health studies, extensive research transport from northern Africa to southern parts of Europe
has been devoted to studying ambient concentration levels, (Korcz et al. 2009). Smoke from Canadian forest fires can
emissions, and transport of PM (Keating and Zuber 2007; contribute to European PM concentrations mainly during
Lelieveld et al. 2002; Smolik et al. 2003). Several other the summer (Forster et al. 2001). Long-range transboundary
studies have focused on the European physicochemical air pollution transport is responsible for a significant
characteristics of PM (Position Paper on PM 2004; Putaud fraction of the particulate pollution in European cities
et al. 2004; EMEP 2008a, b; Andreae and Rosenfeld 2008). (EMEP 2005, 2008a, b). A major part of this contribution is
Composition, morphology, physical, and thermodynamic secondary PM in the form of sulfate, nitrate, ammonium,
properties of PM varies with respect to time and location and organic aerosol particles formed by the oxidation of
and quite typically have a seasonal variability (Finlayson- sulfur dioxide, nitrogen oxides, and organic gaseous
Pitts and Pitts 2000; Seinfeld and Pandis 2006; Position species. A recent report on the hemispheric transport of
Paper on PM 2004; EMEP 2005). air pollutants concluded that the impact of intercontinental
Aerosols have the potential to change the global transport of PM on air quality is primarily episodic and
radiation balance. The recent IPCC report (2007) estimated associated with major emission events such as fires or dust
that the effect of aerosols on climate, since the start of the storms. Such transport can also have large impacts on total
industrial era, to be around 20% of that of greenhouse atmospheric column loading and, hence, implications for
gasses. Aerosols are considered to be responsible for a climate change (Keating and Zuber 2007).
negative forcing and, therefore, to have mitigated some of In this review, we briefly describe the physicochemical
the expected global warming over this period. properties of atmospheric aerosols before discussing the
Existing air quality monitoring networks almost exclu- various natural and anthropogenic sources and ambient
sively rely on ground level in situ observations. However, aerosol concentrations. Their impacts on the environment
ground level concentrations can also be influenced by and human health are then evaluated together with current
vertical transport induced by turbulent mass flux. Even international legislation aimed at improving air quality.
more importantly, the direct and indirect climate impact of Examples are taken predominantly from Europe, although
aerosols depends on the total aerosol load in the atmo- the physical and chemical characteristics would be similar
spheric column and its vertical distribution. Therefore, both worldwide.
Naturwissenschaften (2010) 97:117–131 119

Aerosol physicochemical characteristics (Ca, Fe, and Si) as well as sea salt. The fine particles can be
rich in carbon, nitrates, sulfates, and ammonium ions. They
Particles in the atmosphere have a distribution of sizes, and are generally formed by combustion or gas to particle
lognormal distributions are used for their description (Hinds conversion. The particles in the two modes not only differ
1999). The aerosol size distribution is a crucial parameter in origin but also have different atmospheric fates.
that determines the dynamics of aerosols in the atmosphere, Particles can be categorized according to their size based
their transport, deposition, and residence time. Figure 1 on (1) their observed modal distribution (Hinds 1999), (2)
presents typical atmospheric aerosol distributions by num- the 50% cut-off diameter, or (3) from dosimetric variables
ber, surface area, and volume. In practice, the form of size which are related to human exposure. In the latter case, the
distributions, although containing the same modes, can look most common division is PM2.5 and PM10 particles. PM10
very different according to whether the distribution is is defined as PM which passes through a size-selective inlet
plotted as number distribution or mass distribution. The with a 50% efficiency cut-off at 10 µm aerodynamic
reason for this is that particles at the small end of the size diameter, while the cut-off for PM2.5 is 2.5 µm. The
distribution can be very abundant in number, but because division is related with the possibility of PM2.5 particles
mass is proportional to the cube of diameter, such particles penetrating to the lower parts of the human respiratory tract.
may contribute only a small amount of the total mass. In category 1, several subcategories can be observed:
Hence, a size distribution expressed as the number of
& Nucleation mode: Particles with diameter <10 nm,
particles per size fraction will give far more emphasis to the
which are formed through nucleation processes. The
smaller particles than will occur in a distribution expressed
lower limit of this category is not very well defined but
by mass per size fraction. The volume distribution has
is dictated by instrument capability; an ion aerosol
different features than the surface and number distributions.
spectrometer can detect particles down to 1.5 nm,
In addition, one can derive the mass distribution from the
whereas the cut-off for a condensation particles counter
volume distribution data when the particle density is
is not below 3 nm.
known. The volume distribution is usually bimodal with
& Aitken mode: Particles with diameter 10 nm < d <
minimum ∼1 µm (dividing limit between coarse and fine
100 nm. They originate from vapor nucleation or
particles). Coarse particles are generally formed by me-
growth of pre-existing particles due to condensation.
chanical processes such as dust resuspension. They are
& Accumulation mode: Particles with diameter 0.1 µm
typically rich in the naturally occurring crustal material
<d<1 µm. The upper limit coincides with the minimum
of the total particle distribution. Particles in this mode
∆S/∆ log D (µm-2 cm-3) ∆N/∆ log D (cm-3 x 104)

are formed with the coagulation of smaller particles or


a the condensation of vapor constituents. The size of
particles is not increased over this category with
condensational growth. Furthermore, the removal mech-
anisms of particles in this category are very slow and, as
a result, there is an accumulation of particles.
& Ultrafine particles: Particles in the Aitkin and nucle-
ation modes.
b & Fine particles: Includes the nucleation, Aitkin, and
accumulation modes.
& Coarse particles: Particles with diameters between 1
and 10 µm.
Particles can be products of combustion, suspension of
soil materials, and suspension of sea spray and can be also
∆V/∆ log D (µm3 cm-3)

Γ secondarily formed from chemical reactions in the atmo-


sphere (Fig. 2).
While considerable progress has been made in the
understanding of physical and chemical properties of
inorganic aerosols (Seinfeld and Pandis 2006), the knowl-
edge of organic aerosols remains limited due to their
chemical complexity (Kanakidou et al. 2005; Raes and
Fig. 1 Typical ambient aerosol distributions by A number, B surface Hjorth 2007). As a result, experimentally determined
area, and Γ volume fractional aerosol yields (Lazaridis 2008) are mainly used
120 Naturwissenschaften (2010) 97:117–131

Fig. 2 Schematic representation


of the chemical reactions and
processes associated with PM
(adopted from Meng and
Seinfeld 1996). OC organic
carbon, EC elemental carbon

to describe the incorporation of organic matter in the In Europe, anthropogenic sources of aerosols are
particle phase. Aerosol yield is defined as the fraction of a dominant because of widespread urbanization and the large
reactive organic gas that is transformed to aerosol. Mass number of vehicle and combustion sources in both
closure of the PM requires chemical analysis of the industrial and residential locations (Position Paper on PM
secondary inorganic constituents, the carbonaceous frac- 2004). Site-specific projections for background locations in
tion, water, organic mass fraction, and the mineral dust the UK have been performed using a combination of
content. various types of modeling and statistical analysis (Stedman
et al. 2001a, b, 2002).
Biological aerosols may also have considerable influ-
Aerosol sources—emissions ence on the mass size distribution. Primary biological
aerosol particles (PBAP) describe airborne solid particles
Atmospheric aerosols originate from either naturally occur- (dead or alive) that are or were derived from living
ring processes or from anthropogenic activity. Major natural organisms, including microorganisms and fragments of all
aerosol sources include volcanic emissions, sea spray, and varieties of living things. PBAP includes viruses (0.01 µm
mineral dust emissions, while anthropogenic sources <d<0.5 µm where d refers to the particle diameter),
include emissions from industry and combustion processes. bacteria (d≥0.4 µm), algae, spores of lichen mosses, ferns
Sources of PM can be either primary or secondary in and fungi (d≥1.0 µm), pollen (d≥10 µm), plant debris
nature. Primary sources are mainly of natural origin, such as leaf litter, part of insects, human, and animal
whereas secondary particles originate from chemical trans- epithelial cells (usually d>2 µm; Matthias-Maser 1998).
formations of gaseous precursors such as sulfur dioxide, Most biological aerosols arise from fungal spores and
nitrogen oxides, and volatile organic compounds. Recent plant debris but secondary sources include industry
studies have highlighted the importance of biogenic hydro- (textile mills), agriculture (fertilizing), and sewage plants.
carbons (such as terpenes) in the formation of organic Recent findings by Winiwarter et al. (2009) suggest that the
aerosols (Hoffman et al. 1997; Svendby et al. 2008). PBAP contribution to aerosol concentrations in Europe is
Sometimes, the distinction between natural and anthropo- between 2% and 3% with annual PBAP emissions of 233 Gg.
genic sources is not at all clear. For example, smoke, arising This figure can be compared to global-scale emissions for
from natural wildfires, is often categorized as anthropogen- PBAPs in the range from 56 Tg annually (Penner et al. 2001)
ic in origin, while mineral dust entrained into the to a value as high as 1,000 Tg (Jaenicke 2005).
atmosphere from agriculturally eroded regions has been An important characteristic of atmospheric PM is the
considered as a natural source. tremendous variation in size ranging from tens of micro-
Naturwissenschaften (2010) 97:117–131 121

meters to a nanometer size (Hinds 1999). For example, components of PM. Gray and Cass (1998) combined air
combustion-generated particles (vehicle emissions, power trajectories with receptor modeling to apportion the
generation) range in size from 3 nm to 1 µm. Pollen and atmospheric fine carbon particle concentrations in the Los
soil dust is composed of particles mainly above 2 µm, Angeles area. Additionally, ambient data have been used
whereas fly ash from coal combustion produces particles through inverse modeling to improve emission source
ranging from 0.1 to 50 µm. In addition, aerosols in the inventories (Kleeman and Cass 1999).
atmosphere undergo changes in their chemical composition The US-EPA (2004) has performed a comprehensive
and size. This is due to a variety of physical and chemical study on PM emission characteristics and source identifi-
processes such as nucleation (new particle formation), cation. Details and trends on PM emissions in United States
condensation, evaporation, coagulation, deposition (both by sector are also available. The same information on PM
wet and dry), and activation due to water and other gaseous emissions and source apportionment in Europe will be a
species and aqueous phase reactions (Seinfeld and Pandis valuable input for the EMEP framework for further
2006; Finlayson-Pitts and Pitts 2000). providing quantitative information on the effect of country
Emissions inventories are applicable only to emissions emissions on regional aerosol concentrations and their
of primary pollutants; there is no straightforward way of chemical characteristics.
including secondary pollutants. An example on PM Direct emission of natural organic aerosols originates
emissions spatial distribution is given in Fig. 3. Annual from vegetation, soil, oceans, and bioaerosols. Anthropo-
(in tons per year) PM (PM2.5) emissions were derived from genic sources include biomass burning and fossil fuel
the United Nations Economic Commission for Europe/ burning mainly from transport and energy production.
European Monitoring and Evaluation Programme (EMEP) Biomass burning is a very important source of soot particles
database (data available at the website http://www.emep. and a mean emission factor for black carbon is reported by
int). Emissions are available at the EMEP 50×50-km2 grid Andreae and Crutzen (1997) close to 0.59±0.19 g/kg of dry
(132×111 points, polar stereographic projection with real matter. The term black carbon is mainly applied to the
area at latitude 60° N). The EMEP is a program which component of the organic material which is related to the
focuses on background station measurements in rural areas absorption of visible light. Direct emissions of organic
in Europe for several pollutants including PM under the aerosols from vegetation have needle-like shape with length
auspices of the United Nations for Europe (EMEP 2008b). and width up to 200 nm and 30 nm, respectively. Organic
An understanding of atmospheric aerosol source appor- carbon is a complex mixture of thousands of different
tionment is crucial for legislation since control costs for organic compounds (Grosjean 1992) and a very small
reduction of PM emissions are potentially very high. portion (around 10%) of its molecular structure has been
However, the source apportionment task for PM is more characterized.
complex than for gaseous species since a considerable Estimates for black carbon and organic carbon emissions
fraction of atmospheric aerosol mass is formed via using energy statistics were given by Bond et al. (2004).
secondary processes in the atmosphere, which arise from Global emissions for primary organic aerosols (POA) are
the emission of anthropogenic and biogenic precursors. estimated close to 9.1, 34.6, and 3.2 Tg POA year−1 from
An extensive dataset of chemical characteristics from biofuel, vegetation fires, and fuel burning, respectively,
ambient samples is needed for determining the contribution whereas the estimates for black carbon are 1.6, 3.3, and
of various sources to atmospheric concentrations using 3.0 Tg POA year−1. Uncertainties in the above estimates
receptor models (Hopke 2003). Pun and Seigneur (1999) due to the estimation of the emission factors have been
grouped receptor models into three major categories: identified in the literature (Kanakidou et al. 2005). Recent
studies reveal the challenging task to estimate emission
& Models that apportion primary PM using source
factors from individual sources (Fuzzi et al. 2006; Junker
information.
and Liousse 2008).
& Models that apportion primary PM without using source
information.
& Models that apportion primary and secondary PM.
Aerosol ambient concentrations
There are many techniques available in the different
categories including United States Environmental Protec- There is a considerable literature concerning patterns and
tion Agency (US-EPA) regulatory tools for PM apportion- trends of ambient aerosols and their concentration charac-
ment (Chemical Mass Balance and Principle Component teristics. The interested reader is referred to the following
Analysis) as well as recent powerful research tools (e.g. scientific books, papers, and reports (Seinfeld and Pandis
Positive Matrix Factorization, Hybrid methods). Hybrid 2006; Position Paper on PM 2004; Putaud et al. 2004; van
methods have been applied to apportion the secondary Dingenen et al. 2004; EMEP 2005; US-EPA 2004).
122 Naturwissenschaften (2010) 97:117–131

Fig. 3 Emission of PM2.5


in Greece during 1995

European aerosol characteristics Measurements from the EMEP sites indicate that stations in
Central and the continental part of Western Europe typically
In Europe, PM measurements are performed mainly in have higher annual PM10 concentrations than stations in Great
urban areas for the purpose of monitoring human PM Britain and Scandinavian countries. For example during 2004
exposure. Monitoring of PM in rural areas is not as country annual averaged PM10 concentrations ranged from
extensive as in urban areas. Despite this, results presented 5.35 µg/m3 for Norway to 32.13 µg/m3 for Belgium. Similar
in the Position Paper on PM (2004) for the period 1997 to concentrations have been reported for stations in Southern
2001 show that the difference between concentrations of and Western Europe (20.21 and 21.27 µg/m3, respectively).
PM10 at rural and urban sites in Europe can be quite However, sources in Western Europe can be attributed to
narrow. The annual variation of PM concentrations for local anthropogenic emissions (traffic, industries) while
these two site categories is similar for the period 1997 to biogenic emissions, resuspended dust from local sources,
2001. Regional contributions seem to be highly important and Saharan dust events contribute to PM concentrations in
in contributing to PM10 levels observed. Also the level of Southern Europe. A similar spatial distribution of PM10
PM10 at traffic-influenced sites in Europe follows the concentrations over Europe was observed during 2003.
annual variation observed for urban and rural areas, During 2004, the annual limit value of 40 µg/m3 of
although its concentration level is considerably higher. PM10 was not exceeded in any of the EMEP stations.
Naturwissenschaften (2010) 97:117–131 123

PM concentrations at EMEP background rural stations a urban


60
were compared with concentrations measured at other street
stations in Europe via the AIRBASE database. The stations rural

included in AIRBASE are classified into three main station

concentration (ug/m3)
types, namely, traffic, background, and industrial. These 40
station types are further divided according to the type of the
area in which they are situated: traffic sites, urban, and
rural. In Supplementary Material Figs. S1, S2, and S3, the
20
term EMEP1 refers to EMEP stations for which data have
been reported directly to EMEP, whereas the term EMEP2
refers to EMEP stations for which data have been obtained
from the AIRBASE database (EMEP 2005). 0
In Supplementary Material Fig. S1, the annual mean 1996 1997 1998 1999 2000 2001 2002

PM10 concentrations at AIRBASE and EMEP stations


b urban
during 2004 are depicted. It is observed that the PM10 100
street
concentration was higher at traffic stations and stations rural
situated in urban areas. The annual limit value was 80
exceeded at 208 of 1,801 stations during 2004. Most of

concentration (ug/m3)
these stations were background (52) and traffic (92) sites
60
situated in urban areas, specifically in Spain (51) and Italy
(49). Moreover, PM10 concentrations at seven background
rural stations were above the limit value. Concentrations 40
measured at EMEP sites in each country were, on average,
lower than those elsewhere. However, the mean annual 20
PM10 concentration of all the EMEP stations in Spain was
higher than the average concentration for traffic and
0
background rural stations, probably the result of Saharan 1996 1997 1998 1999 2000 2001 2002
dust intrusions. Generally, it is also observed that EMEP2 Fig. 4 PM10, interannual variations, 1997–2001. a Annual average
stations experience higher concentrations than stations and b 36th highest daily value. Average over all stations with reported
reporting PM10 data directly to EMEP. This is because data, per station type. Vertical bars 10th and 90th percentiles (source:
some of EMEP2 stations are situated in urban and suburban Position Paper on PM 2004)
areas (e.g., stations in Belgium) rather than in rural
locations. of the order of 20%, dependent upon station type and
There is evidence to suggest that aerosol loadings in the statistic.
atmosphere are showing a decline in recent years due to a
reduction in primary emissions. Streets et al. (2006) Global aerosol characteristics
reported a two-decadal rate of decline in aerosol loading
of 0.13% year−1. Although the emphasis of this paper is on Europe, it is
Across Europe, emissions of primary PM10 have been important to understand how European PM concentrations
reduced between 1990 and 2000 by 18% and emissions of compare with those elsewhere. Aerosol size distributions
precursors of PM have decreased by more than 18%. can vary in space and time due to differences in emission
Figure 4 shows the annual average and 36th highest daily sources and atmospheric processes. The construction of a
value per year (corresponding to the limit value definition “representative” size distribution necessarily smoothes out
of the European Union [EU] Directive) from 1997 to 2001, many of the features that may be of interest but nonetheless
as mean value for each of the following station classes: has value. Jaenicke (1988) has presented idealized number
rural, urban background, and street (mainly traffic influ- and volume distributions for several classes of tropospheric
enced). Only stations with at least 5 years of data have been aerosols: polar, background, maritime, remote continental,
included (Position Paper on PM 2004). It is evident that, on desert dust storm, rural, urban, and biological aerosols.
average, there was a marked decrease in PM10 concentra- There are dramatic differences in these aerosol size
tion from 1997 to 1999, but this then leveled off, and distributions. For instance, polar aerosols reflect their aged
concentrations have even increased since then. This is the nature as well as their low concentrations, while for the
case both for annual average and for the 36th highest daily urban environment, the maximum particle concentration is
concentration. The average reduction from 1997 to 2001 is observed for small particle sizes and drops off significantly
124 Naturwissenschaften (2010) 97:117–131

toward minimum values of just a few particles per cubic Thailand (Oanh et al. 2006; Oanh and Zhang 2004),
centimeter for particles in the 10 μm range. Anthropogenic Philippines (Cassiday at el. 2007; Oanh et al. 2006),
aerosols have been found everywhere in the atmosphere, Malaysia (Omar et al. 2007), Korea (Pandey et al. 2008),
although in low concentrations under background condi- Vietnam (Oanh et al. 2006), Indonesia (Oanh et al. 2006),
tions (Baltensperger and Furger 2008). and China (Chan and Yao 2008). High levels of PM (PM2.5,
Nowadays, all the developed countries oversee monitor- PM 10) were reported in six Asian cities (Bandung,
ing networks to measure a wide range of air pollutants. Bangkok, Beijing, Chennai, Manila, and Hanoi) by Oanh
Although aerosols in the form of soot had been recognized et al. (2006) within the framework of the Asian regional
as pollution for centuries, they were, until the 1980s, air pollution research network. The average concentrations
registered as a total mass, total suspended particulate matter of PM2.5 and PM10 were in the range 44–168 and
(TSP). In the US, PM10 was introduced in 1987 because TSP 54–262 µg/m 3 in the dry season and 18–104 and
levels were often driven by a few very large particles while 33–180 µg/m3 in the wet season, respectively. An ongoing
health effects generally correlated with smaller-sized par- study by the Clean Air Initiative for Asian Cities
ticles. Finally, in light of health effects data, US-EPA revised (CAI-Asia 2006) shows that, for 20 megacities in Asia,
the PM air quality standard in 1997 to include an indicator on average, TSP and PM10 has decreased from 1993 to
for the fine mode only—namely, a PM2.5 standard. There is a 2004, but ambient levels remain above the World Health
wealth of papers on PM concentrations in North America (e. Organization (WHO) guidelines. An analysis on a per city
g., Cabada et al. 2004; Keeler 2004; National Research basis suggests that PM is the pollutant of concern to most
Council 2004; Sardar et al. 2005; Westerdahl et al. 2005; of the cities. Gurjar et al. (2008) reported that Karachi
Bell et al. 2007; Chow et al. 2008; US-EPA 2008). The ranks as the most polluted megacity for TSP with an
California region shows considerably higher concentrations annual average concentration of 668 µg/m3.
compared to other parts of the United States. PM10 Characterizing the emission sources, concentrations, trans-
concentrations are close to 30 µg/m3 throughout most of port patterns, and impacts is particularly difficult in develop-
the US whereas PM2.5 concentrations are higher in the ing countries where data are scarce, emissions are high, and
Eastern and the industrialized part of the country with lower health impacts are often severe. The first comprehensive
values in the southwest and upper midwest. estimates of particulate emissions in China by size distribution
The number of studies that have examined number size and major components were reported by Zhang et al. (2007).
distribution or number concentration of aerosols in Latin Total particulate emissions, for 2001, were estimated to be
America (Braga et al. 2005; Báez et al. 2007; Seguel et al. 27.4 Tg, of which 17.8 Tg were PM10 and 12.7 Tg PM2.5.
2009), Australasia (Krivácsy et al. 2006; Mejía et al. 2007), Although industrial processes were identified as the major
or Africa (Kuvarega and Taru 2008; Arku et al. 2008) is sources of particles over all three size ranges, residential
relatively few. Of growing importance is the rapid growth biofuel use and transportation sources were becoming
of megacities (with a population of more than ten million). increasingly important for PM10 and PM2.5. It is likely that,
Air pollution from such megacities (Molina and Molina with the introduction of emission control technologies and
2004) not only results in local air pollution but the strategies, there should be significant reductions in primary
emissions of longer-lived pollutants from these centers particulate emissions and, as a result, major changes in the
can affect atmospheric chemistry on a continental and patterns of particle size and species.
global scale (Lawrence et al. 2007). The most severe air Table 1 shows the annual average PM10 concentrations
pollution monitored occurs in developing countries, but in a number of cities worldwide. The concentrations are
even megacities in developed countries often have at least estimates for residential areas as predicted by the Global
one major air pollutant exceeding health guidelines. Over Model of Ambient Particulates. This model was developed
the last decade, the Asian countries have undergone a by the World Bank to estimate concentrations on the basis
substantial growth in development and urbanization cou- of available measurements of PM at population-orientated
pled with motorization and increase in energy use. measurement sites (Pandey et al. 2006). When interpreting
Although a considerable rise has occurred in the types this table, it must be remembered that concentrations are
and number of emission sources of air pollutants in the sensitive to local conditions and, even in the same city,
region, air quality management capabilities are still minimal different locations may experience different concentrations.
(Gurjar et al. 2008). As a consequence, air pollution has From an assessment of actual measurements, the WHO
emerged as a significant threat to the environment, quality (2006) concluded that annual average concentrations of
of life, and health of the population in Asia. Elevated PM10 in urban settings were in the range 40 to 150 µg/m3
concentrations of various pollutants have been found in in Africa, 35 to 220 µg/m3 in Asia, 28 to 127 µg/m3 in
various countries throughout Asia: India (Jain and Khare Australasia, 20 to 60 µg/m3 in North America, and 30 to
2008; Oanh et al. 2006), Bangladesh (Begum et al. 2006), 139 µg/m3 in Europe.
Naturwissenschaften (2010) 97:117–131 125

Table 1 Estimated annual con-


centration of PM10 for 2004 Country City Estimated PM10 concentration (µg/m3)

Argentina Cordoba 58
Australia Sydney 20
Brazil Sao Paulo 40
Canada Toronto 22
Chile Santiago 61
China Beijing 89
Shanghai 101
Colombia Bogota 31
France Paris 11
Germany Berlin 22
Ghana Accra 33
India Delhi 150
Japan Tokyo 40
Mexico Mexico City 51
New Zealand Auckland 14
Russia Moscow 21
South Africa Johannesburg 33
Spain Madrid 30
Thailand Bangkok 79
Ukraine Kiev 35
United Kingdom London 21
United States Los Angeles 34
New York 21
Venezuela Caracas 10
Data from Pandey et al. 2006

It can be concluded from this that PM10 concentrations are the boundary and initial conditions for concentrations of
in Asia and Latin America are generally higher than those chemical species.
in Europe and North America. Asia also experiences Currently, the EMEP model is the main regional regulatory
relatively high background concentrations owing to forest modeling tool in studying photochemical pollutants and
fires and from the widespread use of poor-quality fuels. acidification in Europe and treats the PM10 and PM2.5
Concentrations in rural areas at different global locations fractions of the atmospheric sulfate and nitrate aerosol using
show similar levels of aerosol mass concentration, whereas a three-dimensional model with detailed physicochemical
very low levels of aerosol mass were observed at remote modules (EMEP 2008b). Results show that the annual mean
sites such as Antarctica and the Jungfraujoch. concentrations of regional background PM10 ranged from 5
to 20 µg/m3, whereas the corresponding range for PM2.5 was
from 2 to 15 µg/m3 in 2006 over most of Europe
Aerosol modeling (Supplementary Material Fig. S4). The regions characterized
by the enhanced PM10 and PM2.5 pollution, with concen-
There are currently several three-dimensional Eulerian air trations exceeding 20 and 15 µg/m3, respectively, were the
quality models that are capable of modeling PM processes Benelux countries, central and northern Italy, south of Spain,
in the atmosphere (Pai et al. 2000; Binkowski and Shankar central Europe (the Czech Republic, Slovakia, and Hungary),
1995; Gong et al. 2003). A comprehensive review of and the southern part of the Russian Federation.
available dispersion models is given by Holmes and
Morawska (2006).
Among other available current state-of-the-art tools used Impacts on the environment and human health
for PM modeling are mesoscale or regional-scale photo-
chemical models, such as UAM-AERO (Spyridaki et al. Climate
2006; Sotiropoulou et al. 2004), CMAQ (Lee et al. 2007),
and CAMx (Gaydos et al. 2007). Among the sources of Natural as well as anthropogenic aerosols have the potential
uncertainty that affect the prognoses of the above models to change the global radiation balance, an aspect highlight-
126 Naturwissenschaften (2010) 97:117–131

ed in many studies of global climate change (IPCC 2007). scale atmospheric dynamic processes shaping aerosol and
Aerosols may influence the atmosphere in two important trace gas properties and their coupling with large emission
ways, direct and indirect effects. Direct effects refer to the sources such as megacities is required.
scattering and absorption of radiation with a subsequent Elevated aerosol concentrations tend to shift the cloud
influence on the climatic system and planetary albedo. droplet size distribution to higher number densities with
Indirect effects refer to the increase in available cloud smaller effective radii, resulting in more side-scattering and
condensation nuclei due to an increase in anthropogenic back-scattering in relation to forward-scattering, the out-
aerosol concentration, and thus cloud albedo—the first come being an increased cloud albedo (indirect effect). The
indirect effect (or Twomey effect). The microphysically size-resolved chemical composition of coarse and fine
induced effect on the liquid water content, cloud height, aerosol is at present estimated from measurements at
and lifetime of clouds is the second indirect effect. The selected sites at ground level. The major species include
overall impact results in a cooling effect. The IPCC (2007) sulfate, nitrate, ammonium, sea salt, mineral dust, and
have estimated that the total direct aerosol radiative forcing complex carbonaceous compounds with a highly variable
combined across all aerosol types is −0.5±0.4 W m−2 and composition. Their chemical composition, in turn, affects
that the indirect cloud albedo effect is −0.7 W m−2 [−0.3 their hygroscopic behavior, hence their size and optical
to −1.8 W m−2]. The role of anthropogenic aerosol is still a properties. Establishment of the composition and properties
key factor of uncertainty in understanding and quantifying is very important since it strongly affects the role that
the present and future global climate change. aerosols play in counteracting global warming.
To quantify the impact of aerosols on climate and to assess
the feedback of climate change on aerosols requires a Health
thorough understanding of the physicochemical processes on
the microscale and aerosol evolution in the context of An understanding of the complex sequence of events starting
regional-scale and global-scale circulation. This understand- from the emissions of air pollutants through to human health
ing can only be obtained by combining all available effects is necessary for the prognosis of potential risk to
information from state-of-the-art experimental techniques humans from specific chemical compounds and mixtures of
and modeling tools. This is a challenging task considering them. There is still considerable uncertainty about which
that tropospheric aerosol concentrations are nonlinearly physical and/or chemical characteristics of PM are the most
dependent on the meteorological and chemical variables that important regarding health effects. Various investigations
govern their behavior. An example of air pollution impacts on advocate that ultrafine particles are important as they are
climate can be seen from the albedo effect of black carbon present in the atmosphere in very high numbers relative to
deposition on snow (Hansen and Nazarenko 2004; Stohl et al. their mass and because they may penetrate into the blood-
2006). Contrary changes in climate may also affect air stream leading to systemic effects (Pope et al. 2009).
quality levels as described by Hansson and O’Dowd (2006). There are recent cohort studies which have followed
Large uncertainty in estimating the direct or indirect the successful implementation of the Harvard Six Cities
forcing of aerosol particles is introduced by lack of Study and the American Cancer Society Study (Pope et al.
knowledge about the mixing state of particles. The existing 2009) and they show significant effects of PM levels on
aerosol scheme assumes each of the aerosol components to mortality and morbidity. Long-term average mortality rates
be externally mixed (particles consist of only one compo- were 17% to 26% higher for people living in communities
nent). In reality, condensation and coagulation result in with elevated levels of PM2.5 (US-EPA 2004). Additionally,
internal mixtures (e.g., soot and sulfate) and hence the synergetic effects between the “pollution mixture” of
direct and indirect radiative properties may differ substan- gaseous pollutants and PM on human health are an
tially from a corresponding external mixture. emerging scientific issue.
The optical properties and hence the radiative forcing of In addition to the above findings, other studies re-examined
atmospheric aerosols are determined, in part, by the way in the previous epidemiological findings to ensure the reproduc-
which the various constituents are externally or internally tion and the consistency of earlier results. The Health Effects
mixed. The mixing state must be known to compute the Institute US-wide National Morbidity, Mortality and Air
effective refractive index, water activity, and size distribution Pollution Study (NMMAPS; Samet et al. 2000) is a notable
of the aerosols. Large-scale experiments in remote areas and example of these efforts. The NMMAPS study shows a 0.5%
in the fringe of pollution hot spots (for Europe and Asia) have increase in total nonaccidental mortality associated with a
provided some insight into the physical and chemical 10-µg/m3 increase in the 90 largest US cities where daily
properties of polluted continental aerosol, aging over the average PM10 ranged from 15 to 53 µg/m3. Similar results
ocean, and mixing with air from the free troposphere (Johnson had been previously obtained from the European APHEA
et al. 2001). Further insight and knowledge about the large- study (0.6% per 10 µg/m3) (Katsouyanni 1996) and with
Naturwissenschaften (2010) 97:117–131 127

recent meta-analysis in Europe and North and South Quality Directive (2008/50/EC) came into force (EU 2008).
America (0.7% per 10 µg/m3; Levy et al. 2000). The new directive merges four existing directives into a
Pope et al. (2009) investigated correlations between life single directive on air quality. It sets new standards and
expectancy and PM2.5 air pollution in 51 US metropolitan target dates for reducing concentrations of PM2.5 in
areas. They compared data for the period from the late addition to existing ones for PM10 (details are presented
1970s to the early 1980s with matched data for the period in Supplementary Material Tables 1 and 2).
from the late 1990s to the early 2000s. Air pollution fell in The directive recommends that measurements of fine PM
all areas and bigger reductions in air pollution were at rural background locations should be made in order to
associated with bigger increases in life expectancy, even understand better the impacts of this pollutant and to
after adjustments for the obvious socioeconomic and social develop appropriate policies. It also acknowledges that
variables that affect mortality. They found that a decrease in there is currently no identifiable threshold below which
PM2.5 concentration of 10 µg/m3 was associated with an PM2.5 does not pose a risk to human health. The new
increase in life expectancy of 0.6 years. directive also introduced several features that weaken the
Previous work has shown that increases in PM2.5 previous legislation, including the possibility to discount
concentrations of 10 µg/m3 can result in reduced life natural sources of pollution when assessing compliance
expectancy of 1.11 years in the Netherlands (Brunekreef against limit values. The European Commission has had to
1997), 1.37 years in Finland (Nevalainen and Pekkanen start infringement proceedings against ten member states
1998), and 0.80 years in Canada (Coyle et al. 2003). for failing to comply with the EU’s air quality standard for
However, Krewski (2009) points out that the work by Pope PM10. The exceedances affect 83 million people in 132
et al. is the first to demonstrate an increase in life different air quality zones. However, Directive 2008/50/EC
expectancy resulting from actual reductions in particulate allows member states to request limited time extensions to
air pollution. This study demonstrates that improvements in meet the PM10 standard. The time extensions only apply in
air quality can contribute to significant and measurable those air quality zones which can show that an effort was
improvements in life expectancy. made to achieve the limit values in 2005 but that
Even though the epidemiological studies have shown an compliance was not possible due to specific external
important relationship between PM levels and health circumstances. So far, 11 member states have requested
effects, many important questions remain to be addressed. extensions.
There is a need for a better understanding of the factors Today’s complexity of emission sources and strengths
responsible for the variability in health effects due to PM means that the air pollution picture, and resultant manage-
among geographical regions. Also, there is a clear need to ment challenge, is much more complicated than in the past.
identify the mechanisms by which short-term and long-term Various actions are being planned to combat the threat of
exposure to PM affects the cardiovascular and respiratory climate change. If these are successfully implemented, then
system. The physicochemical features of PM responsible this may have a significant impact on pollutant emissions,
for respiratory allergies, asthma, and health effects in and hence air quality in the twenty-first century. Addition-
general are still not clearly identified. The interaction of ally, there is a general move away from managing
particles with the lungs is not well understood and the concentrations via limit values and towards managing
actual particle properties responsible for the adverse health exposure (Longhurst et al. 2009).
effects are poorly understood. PM10 particles have been
shown to produce free radicals and are likely to exert an
oxidative stress upon the lung (Stone et al. 2007). The Summary
molecular mechanisms of the cellular oxidative damages of
aerosol particles are not well understood. The dynamics of PM in the atmosphere involves various
physical and chemical processes and different time scales.
Aerosol dynamics incorporates a wide range of particle
Legislation sizes from a few nanometers to several hundred micro-
meters. In addition, particles can have different composi-
Ambient air quality standards have been introduced at tions and chemical reactivity and undergo complex physical
national and international levels with the aim to protect transformations (nucleation, condensation, coagulation, and
human health and the environment (e.g., WHO 2006). deposition processes).
Legislation for PM10 concentrations has been implemented Aerosols arise from natural and anthropogenic sources
in the EU. In 1996, the EU adopted the Air Quality and are a mixture of primary emissions and secondary
Framework Directive (96/62/EC), which in turn gave rise to species. Crustal material, biogenic matter, and sea salt
a series of “daughter” directives. In 2008, a new Air comprise the majority of natural aerosols. Anthropogenic
128 Naturwissenschaften (2010) 97:117–131

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115:989–995
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