1

A European Aerosol Phenomenology

physical and chemical characteristics of particulate matter
at kerbside, urban, rural and background sites in Europe.
Jean-P. Putaud
1
, Rita Van Dingenen
1
, Urs Baltensperger
2
, Erika Brggemann
3
, Aurlie Charron
4
, M.-Cristina
Facchini
5
, Stefano Decesari
5
, Sandro Fuzzi
5
, Robert Gehrig
6
, Hans-C. Hansson
7
, Roy M. Harrison
4
, Alan M.
Jones
4
, Paolo Laj
8
, Gundi Lorbeer
9
, Willy Maenhaut
10
, Nikolaos Mihalopoulos
11
, Konrad Mller
3
, Finn
Palmgren
12
, Xavier Querol
13
, Sergio Rodriguez
13
, Jrgen Schneider
9
, Gerald Spindler
3
, Harry ten Brink
14
, Peter
Tunved
7
, Kjetil Trseth
15
, Ernest Weingartner
2
, Alfred Wiedensohler
3
, Peter Whlin
12
,

Frank Raes
1
1
European Commission, Joint Research Centre, Ispra, Institute for Environment & Sustainability, Italy
2
Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, Villigen, Switzerland
3
Institut fr Troposphrenforschung, Leipzig, Germany
4
University of Birmingham, Division of Environmental health and Risk Management, Birmingham, UK
5
Istituto di Scienze dellAtmosfera e dellOceano, Consiglio Nazionale delle Ricerche, Bologna, Italy
6
Swiss Federal Laboratories for Materials Testing and Research, Dbendorf, Switzerland
7
Institute of Applied Environmental Research, University of Stockholm, Stockholm, Sweden
8
Laboratoire de Mtorologie Physique, Universit Blaise Pascal, Aubire, France
9
Umweltbundesamt, Wien, Austria
10
Ghent University, Institute for Nuclear Sciences, Department of Analytical Chemistry, Gent, Belgium
11
Environmental Chemical Processes Laboratory, University of Crete, Heraklion, Greece
12
National Environmental Research Institute, Roskilde, Denmark
13
Instituto de Ciencias de la Tierra, Consejo Superior de Investigaciones Cientficas (CSIC), Barcelona, Spain
14
Netherlands Energy Research Foundation (ECN), Petten, The Netherlands
15
Norwegian Institute for Air Research (NILU), Kjeller, Norway
EUR 20411 EN
2002
2
Legal Notice
Neither the European Commission nor any person
acting on behalf of the Commission is responsible for the use
which might be made of this publication.
Its content does not necessarily reflect the official view of the European Commission
Additional copies are available from:
Ms. Ana Gallego-Romero
Joint Research Centre
Institute for Environment and Sustainability
TP 290
I-21020 Ispra
Also available on the JRC/IES/CCU world wide web site at:
http://ies.jrc.cec.eu.int/Download/cc
3
Summary
This report synthesizes data on aerosol (= Particulate Matter, PM) physical and chemical
characteristics, which were obtained in European aerosol research activities at free-
troposphere, natural, rural, near-city, urban, and kerbside sites over the past decade. It covers
only two (nearby) sites in the semi-arid Mediterranean area, and lacks data from Eastern
Europe. The data include PM10 and/or PM2.5 mass concentrations, aerosol particle size
distributions, PM10 and/or PM2.5 chemical composition and size segregated chemical
composition. Such data sets are more comprehensive than those currently provided by air
quality monitoring networks (e.g. EMEP, EUROAIRNET), and are essential to elucidate the
sources of the aerosols, their effect on human health, their role in the radiation balance of the
atmosphere, and to validate atmospheric models. Data available from 34 sites in Europe
(called The Network) were reviewed. They were processed and plotted to allow
comparisons in spite of differences in the sampling and analytical techniques used in various
studies. A number of conclusions are drawn among which the following:
- Background annual average PM10 and PM2.5 mass concentrations for continental Europe
are 7.0 4.1 and 4.8 2.4 g m
-3
, respectively. This background is not only due to natural
sources, but also to long range transport of anthropogenic particles.
- The EU 2005 annual average PM10 standard of 40 g m
-3
is exceeded at a few sites in
The Network. At all near city, urban and kerbside sites, the EU 2010 annual average
PM10 standard of 20 g m
-3
, as well as the US-EPA annual average PM2.5 standard of 15
g m
-3
are exceeded. In certain regions, PM10 and PM2.5 in cities are strongly affected by
the regional aerosol background.
- There is no universal (i.e. valid for all sites) ratio between PM2.5 and PM10 mass
concentrations, although fairly constant ratios do exist at individual sites. There is no
correlation between PM mass concentration on the one hand, and total particle number
concentration or chemical composition on the other hand.
- Observations of PM2.5/PM10 ratios, particle size distributions and chemical composition
indicate that traffic is responsible for the high PM10 and PM2.5 concentrations in urban
areas, either through the contribution of carbonaceous species and nitrate in the fine and
coarse fraction of the aerosol (at near-city and urban background sites) or due to the
contribution of re-suspended dust to the coarse fraction (at kerbside sites).
- At polluted sites PM10, PM2.5 and other aerosol parameters are significantly higher
during winter. This is at least partially due to meteorology: the dispersion of pollutants is
least in winter, when the mixed boundary layer height is reduced. However, measurements
show that the condensation in the particle phase of semi-volatile species like nitrate and
(unspecified) organics is also favored by cold temperatures.
- Sulfate and organic matter are the two main contributors to the annual average PM10 and
PM2.5 mass concentrations, except at kerbside sites where mineral dust (including trace
elements) is a main contributor to PM10. On days when PM10 > 50 g m
-3
, nitrate and
organic matter become the main contributors to PM10 and PM2.5
- Black carbon contributes 5-10% to PM2.5 and somewhat less to PM10 at all sites,
including the natural background sites. Its contribution increases to 15-20% at some of the
kerbside sites.
More data are known to be available within the scientific community, which could enrich the
present data set and strengthen the conclusions made above. Most of them are not made
available yet. The investment in new approaches, which would bridge the technological gap
between scientific measurements and regulatory monitoring is also needed.
4
0
2
4
6
8
10
12
14
0.01 0.1 1 10 100
Particle aerodynamic diameter Dp (m)
d
M
/
d
L
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p

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)
PM2.5
PM10
TSP
PM10
PM2.5
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1
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1
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1
Fine mode particles Coarse mode particles
5
1. Aerosol Particles / Particulate Matter / Aerosols
Aerosol particles in the atmosphere arise from natural sources such as wind-borne dust, sea-
spray and emission of biogenic volatile organic compounds. They also arise from a range of
anthropogenic activities, in particular the combustion of fossil fuels. Emitted directly as
particles (primary aerosol) or formed in the atmosphere by (often photochemical) conversion
of gaseous precursors (secondary aerosol), atmospheric particles range in size from a few
nanometers (nm) to tens of micrometers (m). Particles smaller than 1 m diameter generally
have atmospheric concentrations in the range of 100 to 100.000s cm
-3
; those exceeding 1 m
diameter typically exhibit concentrations less than 10 cm
-3
. A detailed description of the
atmospheric processes leading to the formation of aerosols can be find in Raes et al., 2000.
Aerosol particles are denominated in a number of ways
An aerosol is a gas in which solid particles or droplets are suspended. Hence aerosol
refers to both the gas phase and the particles (and droplets). The consideration of both phases
is important because many of the relevant components are semi-volatile and exchange mass
between the gas phase and the particle phase. In the atmospheric aerosol, these compounds
include water, nitrate and a range of (often unspecified) organic compounds.
With aerosol particles one clearly refers to the particles and droplets of the aerosol.
Often aerosol(s) is used instead of aerosol particles, when it is clear from the context that
aerosol particles are meant: e.g. the aerosol number concentration clearly means the number
concentration of aerosol particles.
Particulate Matter is another way of referring to these particles. For one reason or the
other, the climate effects community tends to use aerosol particles, whereas the health
effects community prefers to use particle matter or PM.
PMx then means the mass of particles with an aerodynamic diameter lower than x m (see
Annex 2).
Figure 1 Figure 1 Figure 1 Figure 1 illustrates which fractions of the Total Suspended Particles (TSP) are
accounted for by PM2.5 and PM10 measurements. In this example illustrating measurements
performed at an urban site in Sweden, PM10 comprises most of the TSP mass. PM2.5
includes the fine particle mode, but also a significant fraction of the coarse particle mode.
6
Aerosols & Climate
The intergovernmental Panel on Climate Change (IPCC 2001) states that the effect of aerosols on climate might be as
large but opposite in sign (i.e. cooling) than that of the long-lived greenhouse gasses. However, some aerosol types like
black carbon and mineral dust can lead to warming.
PM & Health
EU standards for Particulate Matter (PM10)
24-hour limit value 50 g/m PM10 to be met 1 jan 2005
not to be exceeded > 35 times/year.
50 g/m PM10 to be met 1 jan 2010
not to be exceeded 7 times/year
annual standard 40 g/m PM10 to be met 1 jan 2005
20 g/m PM10 to be met 1 jan 2010
US-EPA PM standards for PM10 and PM2.5
24-hour limit value 65 g/m PM2.5
3-year average of 98% percentile
annual standard 50 g/m PM10 (3-yr average)
15 g/m PM2.5 (3-yr average)
B
O
X

2
B
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X

2
B
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2
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2
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1
B
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1
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1
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1
7
2. Policy context
Today, the interest in aerosols is high mainly because of their effect on human health and their
role in climate change. They have also a determining effect on visibility and contribute to the
soiling of monuments.
Aerosols and Health:
Epidemiological studies show that an increase in PM10 mass concentration by 10 g m
-3
results in an increase of 0.5 -1.5% in premature total mortality in case of short term/episodic
exposure, and in an increase up to 5 % in premature total mortality in case of long term/life
long exposure (Wilson and Spengler, 1996). At yet, there is no indication which physical or
chemical PM characteristic is responsible for these effects. However, recent research seems to
indicate that PM10 is associated with respiratory responses and PM2.5 with cardio-vascular
diseases (Wyzga, 2002). Legislation in the EU and US is therefore expressed in terms of
target values for PM10 and PM2.5 (= the mass of particles with a diameter below 10 m or
2.5 m, respectively) (see BOX 1). Because of the undifferentiated nature of the metric PM
mass and the many sources contributing to it, implementing such a legislation might be
unnecessarily costly. Ideally, health effects of aerosol particles should be related to a well-
defined set of physical or chemical aerosol characteristics, which can be related to a well-
defined set of sources. Major research programs are devoted to understand the effects of
aerosols on health and to the apportionment of their sources.
Aerosols and Climate:
Observations and model calculations show that the increase in the atmospheric aerosol burden
is delaying the global warming expected from the increase in greenhouse gasses (GHG: CO
2
,
CH
4
, N
2
O, halocarbons). Whereas the increase in GHGs since pre-industrial times is
producing a warming of 2.4 Wm
-2
, the overall cooling effect of aerosols might be up to 2.5
Wm
-2
(IPCC, 2001) (see BOX 2). The latter value is composed of contributions by e.g.
sulfate and organic particles, which cool, and black carbon, which heats. International and EU
climate change policies aim at reducing the emissions of GHGs by implementing the Kyoto
Protocol. It is expected that negotiations of reductions beyond the Kyoto Protocol might
consider also the role of aerosols (Hansen et al., 2000). The effect on climate of policies to
reduce adverse effects of aerosols on health (see above) also needs to be addressed. As with
the health issue, knowledge about physical and chemical aerosol characteristics and their
relationship with sources is important, to develop cost-effective mitigation policies.
Aerosol Modelling
Numerical models describing aerosol particle emissions and production, transport,
transformation and removal have become accepted tools to extrapolate monitoring data
(Council Directive 96/62/EC on ambient air quality). They are used in source apportionment
studies and, obviously, they are the only tools to assess the effects of future changes in aerosol
and aerosol precursor emissions. The calculation of e.g. PM10 levels or radiative forcing must
necessarily be based on a description of the emissions of the individual chemical species and
how they transform and mix in the atmosphere. Models with this capability are becoming
available (Hass et al., 2002) but need testing and validation against fundamental data such as
the aerosol particle size distribution and chemical composition.
8
Free Troposphere
Natural background
Rural background
Near-city
Urban background
Kerbside
Falkenberg
Birkenes
Copenhagen
Bologna
Puy de Dme
Mte Foia
Sagres
Leipzig
Melpitz
Jungfraujoch
Basel
Zrich
Chaumont
Bern
Ispra
Milano
Aspvreten
Sevettijarvi
Wien
Illmitz
Skredalen
Harwell London
Waasmunster
Gent
Finokalia
Marseille
Barcelona
Monagrega
Hohenpeissenberg
35 N
40 N
45 N
50 N
55 N
60 N
65 N
70 N
-10 W -05 W 00 W 05 W 10 W 15 W 20 W 25 W 30 W
Aerosol Optical Depth at 555 nm, August 1997 Source: TNO FEL
Seasonal data set
F
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Full year data set
9
3. Presentation of the results
The present aerosol phenomenology
1
synthesizes physical and size-resolved aerosol data
collected during the last 10 years. Such data are presently not measured in regulatory
monitoring networks (such as EMEP and EUROAIRNET), but rather in research projects.
Here we consider only projects providing data representative for a site during at least a season
(i.e. minimum 6 weeks of continuous measurements). Additionally we requested that at least
two of the parameters listed below were measured simultaneously. This provides a minimum
of consistency check and allows to investigate the correlation
1
between parameters. However,
in a few cases, this requirement was not fulfilled. The parameters considered are:
PM10 and/or PM2.5 mass concentrations
Aerosol particle number size distributions
PM10 and/or PM2.5 chemical composition
Size-segregated chemical composition.
The methods used to measure these parameters and the uncertainties arising from comparing
data produced by different institutes using different techniques are described at length in
Annex 2.
Figure 2 Figure 2 Figure 2 Figure 2 shows the location of the 34 sites, operated by 14 institutes. Their
coordinates are given in Annex 1. We will refer to these sites as The Network.
We have categorised the sampling sites using criteria proposed by the European Environment
Agency (Larssen et al., 1999). Among those criteria are the distance of the station from large
pollution sources such as cities, power plants and major motorways and the traffic volume.
Natural Background distance form large pollution sources > 50 km
Rural Background distance form large pollution sources 10 50 km
Near City Background distance form large pollution sources 3 10 km
Urban Background < 2500 vehicles/day within a radius of 50 m
To which we have added the
Free troposphere above the mixed boundary layer
Kerbside within street canyons
In the text we will also refer to
Clean sites = free tropospheric, natural and rural background sites,
Polluted sites = near-city, urban background and kerbside sites
Figure 3 shows the sites projected on a satellite retrieved aerosol optical depth
(AOD) picture for the month of August 1997 (Gonzales et al., 2000). Background AOD
values are about a factor 5 to 10 lower than in the most polluted areas. Fig. 3 shows that The
Network covers a wide range of aerosol pollution conditions. However it lacks data from
Eastern Europe, and it contains few sites that are representative for the semi-arid conditions in
the Mediterranean area.

1
Phenomenology: the branch of philosophy that deals with what you see, hear, feel, etc., in contrast to what may
actually be real or true about the world
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11
3.1 PM10 and PM2.5 mass concentrations.
PM10 mass concentrations are started to be monitored by national and international (EMEP,
EUROAIRNET) air quality networks, where they are replacing Total Suspended Particle
(TSP) measurements. Here we show yearly statistics regarding 24-hr averaged PM10 and
PM2.5 concentrations observed at 23 sites in The Network.
Figures 4a and 4b Figures 4a and 4b Figures 4a and 4b Figures 4a and 4b show the 5, 25, 50 (median) 75 and 95 % percentiles
of 24-hr integrated PM10 and PM2.5 mass concentrations, as well as their annual averages.
PM10 and PM2.5 annual average concentrations both vary by more than a factor of 10
between their lowest (Sevettijarvi, FIN) and highest values (Wien, A; Bologna, I). This
variation is larger than that for annually averaged ozone values, which in Europe range from
about 35 to 105 g m
-3
, hence a factor of 3 only (EMEP/CCC 5/2002). This shows that PM
mass concentration is more sensitive to local sources than ozone.
Fig. 4a and 4b show that the 5% percentile values at rural and near city (and even in some of
the urban) background sites are similar to the annual average concentrations observed at
natural background sites. This means that the former sites encounter natural background
conditions in about 5% of the days. A European continental background concentration is
derived here by taking the average of the natural background annual mean concentrations and
of the rural and near city background 5% percentile values. We obtain values of 7.0 g m
-3
(
4.1) and 4.8 g m
-3
( 2.4) for PM10 and PM2.5, respectively. This latter value is about 5-10
times lower than the highest values observed in The Network, which is similar to what was
observed for the AOD values in Fig. 3. However, this background is not purely natural: the
presence of black carbon (BC) in the aerosol at natural background sites (see Figs 11-15)
indicates that also these sites are affected by (long range transport of) anthropogenic sources.
When sites are ordered according to the EEA criteria, PM10 and PM2.5 annual average
concentrations do not gradually (i.e. monotonically) increase when moving from near-city
background to urban background to kerbside sites. In fact, concentration at kerbsides in one
city might be lower than at urban background sites elsewhere (e.g. compare PM2.5 at
Barcelona, E, and Bologna, I). This has also been observed in a compilation of PM10 data in
the EMEP/EUROAIRNET networks (EMEP/CCC 4/2002). This shows that the regional
aerosol background level can strongly influence PM concentrations in cities. Near-city sites
located downwind of large urban areas show comparable PM average concentrations (e.g.
WaasmunsterGent, MelpitzLeipzig). However, the kerbside site in London (London-M)
shows higher PM than the urban background site (London-B), which again shows higher PM
concentration than a rural site upwind of London (Harwell).
Only a few sites exceed the EU annual PM10 standard of 40 g m
-3
targeted by 2005, whereas
all near-city, urban background and kerbside sites are above the EU annual PM10 standard of
20 g m
-3
targeted for 2010. These data are consistent with those obtained from larger
networks, which show that annual average PM10 concentrations reach 50 g m
-3
in Western
Europe and up to 60-70 g m
-3
in Eastern Europe (EMEP/CCC 5/2001). The 95 and 75 %
PM10 percentiles indicate that the EU 24-hour PM10 limit value of 50 g m
-3
are exceeded
more than 18 and 90 times a year, respectively, at most near-city, urban background and
kebside sites. Targets are 35 exceedences a year by 2005 and 7 exceedences a year by 2010.
As of today the EU has not put forward any PM2.5 limit values. However the annual average
PM2.5 mass concentration at all near-city and urban background sites and at kerbside sites
exceeds the US-EPA standard of 15 g m
-3
. The EMEP/EUROAIRNET database does not
hold PM2.5 data.
12
y = 0.57x
y = 0.85x
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0 10 20 30 40 50 60 70 80 90 100 110 120
PM 10 (g/m)
P
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5


(

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Sevettijarvi (FIN)
Skreadalen (N)
Birkenes (N)
Chaumont (CH)
Waasmunster (B)
Gent (B)
Bologna (I)
Zuerich (CH)
Basel (CH)
Barcelona (E)
Bern (CH)
0%
20%
40%
60%
80%
100%
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)
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P
M
2
.
5
/
P
M
1
0
PM10<20 g/m
20<PM10<50 g/m
PM10>50 g/m
average
F
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13
Figure 5 Figure 5 Figure 5 Figure 5 shows averages of simultaneously measured PM2.5 vs. PM10 mass
concentrations for 11 sites of The Network. For each site, data were grouped and averaged
over 10 g m
-3
-wide PM10 bins (e.g. 30<PM10<40 g m
-3
).
PM2.5 and PM10 mass concentrations are clearly correlated with a mean PM2.5/PM10 ratio
= 0.730.02 (95% confidence level). However, a closer look to the PM2.5/PM10 ratios shows
that they range from 0.5 to 0.9. For a given site the PM2.5/PM10 ratio can be fairly constant.
This is due to the fact that meteorology (dispersion) is the main factor controlling PM mass
concentrations. It also suggests that the intensities of fine (PM2.5) and coarse (PM10-PM2.5)
aerosol sources covary.
However, no universal PM2.5/PM10 ratio can be proposed. This is expected given the
different sources contributing to PM2.5 and PM10-PM2.5. Lower ratios are observed for
kerbside sites (Barcelona, E, Bern, CH), which suggests a large contribution of re-suspended
road dust to the PM10-PM2.5 fraction. Higher ratios are observed at natural, rural, near-city
and urban background sites where secondary aerosol sources, which produce fine particles,
are predominant.
Figure 6 Figure 6 Figure 6 Figure 6 shows the PM2.5/PM10 ratio for the different sites, further categorized
according to the levels of PM10 mass concentration. The higher the PM10 concentration, the
higher the PM2.5/PM10 ratio, indicating that pollution periods are predominantly due to
increases in the PM2.5 mass concentration. This is true except at the kerbside sites, which
again indicates the large contribution of re-suspended road dust to high PM10 concentrations
at such sites.
PM mass concentration as indicator
As a result of the health effects found during the London smog and other similar pollution catastrophes, PM
mass concentration has been used for decades as a measure of air pollution. First, Total Suspended Particle
mass (TSP) was used, but as understanding grew concerning sampling errors for larger particles, it was
replaced by a standardized inlet with a 50% aerodynamic cut-off at Dp = 10 m (PM10).
To facilitate source-receptor analysis, a dichotomous sampler based on virtual impaction with a 2.5 m cut-off
was then developed by US-EPA.
PM2.5 is considerably less influenced by coarse particle material than PM10, but still can contain a
considerable mass fraction of super micron particles originating from coarse particle sources, as Saharan
dust and suspended road wear. PM1 contains both local primary and secondary particles, e.g. as seen in
combustion engine exhaust but also in long-range transported aerosols. However, PM1 is negligibly
influenced by natural sources as e.g. Saharan dust storms and road dust. Using PM1 would facilitate
determining whether health effects are really related with the fine fraction particles. If so, the regulation should
focus only on combustion processes representing the main sources of primary particles and gases leading to
secondary aerosol formation.
B
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3
14
Natural Rural Near-City Urban Kerbside
0
10
20
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60
70
80
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DJF winter
MAM spring
JJA summer
SON fall
F
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a
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15
Figures 7a Figures 7a Figures 7a Figures 7a and 7b 7b 7b 7b show the seasonal average of PM10 and PM2.5 mass
concentrations.
At the polluted sites PM10 and PM2.5 mass concentrations are higher during winter, except at
Waasmunster (B). At the natural and rural background sites, the seasonal variations are less
pronounced: PM10 and PM2.5 are slightly higher during summer, but this observation is not
corroborated by data from other sites given later in Fig. 9a. This will be discussed more
carefully together with the chemical data in Fig. 13.
The fact that similar seasonal variations are observed for PM10 and PM2.5 might indicate that
they are driven by meteorology or that variations in PM2.5 control variations in PM10 (Fig. 5
shows indeed that PM2.5 represents about 70% of the PM10 mass).
The large seasonal variations in e.g. Ispra (I), Zrich (CH), Basel (CH), Bologna (I), Bern
(CH), and Wien (A) are at least partly due to the larger stratification of the atmosphere (lower
mixing heights) in more continental regions during winter.
The fact, however, that seasonal variations are different in nearby clean and polluted sites (see
e.g. Chaumont and Zrich, CH), indicates that other process are also at work. Long-range
transport patterns to rural sites might vary with seasons. We also conjecture that at the
polluted sites in winter there is a larger contribution of ammonium nitrate aerosol and organic
matter, which are semi-volatile and condense into the aerosol phase at cold temperatures. This
will be confirmed by the number size distributions in Fig. 8 and the chemical composition in
Fig. 14.
PM in the Mediterranean Area
PM concentrations in the Mediterranean area are strongly influenced by 3 particularities:
- the vicinity of the sea shore for many regions
- the frequent occurrence of Saharan dust transport episodes and of local soil dust suspension in arid areas
- the complex orography surrounding the Western Mediterranean and the specific meteorological context.
This can be illustrated by the example of Spain, where current studies have evidenced differences in the PM
composition and size distribution in different regions (Eastern, North, South and Central Spain and the
Canaries).
The annual mean marine aerosol load in PM10 reaches 25% at the Canaries and 16% in Northern Spain (6-
10% at the Canaries and 2-4% in the other areas in PM2.5).
In Eastern Spain, PM10 concentrations are highly influenced by the occurrence of African dust. Around 10
African dust events/year take place, which are characterized by 24-hr mean mineral dust concentrations usually
> 25g/m
3
. They induce 15-20 exceedences of the 2005-2010 PM10 EU 24-hr limit value per year at the urban
sites, 2-5 at the rural sites (Rodrguez et al., 2002a, b). The annual mean mineral dust load in PM10 ranges
from 37% at kerbside and 30% at urban background to 13-20% at rural background sites, which underlines the
importance of dust re-suspension. The mineral dust load in PM2.5 averages 21% at urban sites of the Canaries,
17% at kerbside sites and 8-13% at urban background sites.
Because of the large regional variations in the mineral dust and sea spray levels and due to the fact that these
PM components mainly occurs in the 1-10 m fraction of PM, the PM1 contribution to PM10 is significantly
variable: 52-62% in Central and Northern Spain, 40% in Southern and Eastern Spain and 21% at the Canaries.
Regional sea breeze re-circulation episodes are associated with weak pressure gradient conditions, which
inhibit the air mass renovation and favor the accumulation of air pollutants in the regional atmosphere. They
lead to high O3 (Millan et al., 1997) and PM (Rodrguez et al., 2002) levels at rural sites. In contrast, Central and
Northern Europe are mainly affected by the Westerly mid-latitudes general circulation, often associated with
westerly winds, depressions and rain, which favor the air mass scavenging.
These are key points that differentiate the Southern and Northern Europe regarding to the control of PM levels.
B
O
X

4
16
(page left intentionally blank)
17
3.4 Particle size distributions and derived properties
We collected aerosol particle distributions from 15 sites of The Network. No particle number
size distributions were collected in semi-arid Mediterranean areas. Sites were selected where
measurements lasted long enough to calculate seasonal averages.
From the size distributions the aerosol number and surface area concentrations were derived
by integrating the size distribution from Dp=10 nm upwards.
The size distributions were measured with Differential Mobility Analyzers and typically do
not include particles with Dp >800 nm (see Annex 1). Most size distributions were measured
in dry (RH <20%) conditions, except at the sites located in UK, where they were measured
without RH control.
Particle size distributions
surface area
0
20
40
60
80
100
120
0.001 0.01 0.1 1 10
Diameter (m)
d
S
/
d
l
o
g
D
p

(

/
c
m

)
number
0
500
1000
1500
2000
0.001 0.01 0.1 1 10
Diameter (m)
d
N
/
d
l
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D
p

(
#
/
c
m

)
volume
0
1
2
3
4
5
6
0.001 0.01 0.1 1 10
Diameter (m)
d
V
/
d
l
o
g
D
p

(

/
c
m

)
Atmospheric particles are polydisperse over a size range of about 3 orders of magnitude. Hence their
number, surface and volume (mass) distribution versus particle size differ much from each other, as illustrated
above for a typical continental aerosol. This is a consequence of the fact that surface area and volume are
proportional to the 2
nd
and 3
th
power of particle size respectively.
Most particles are found below 0.1 m diameter, whereas most of the volume is found above that size.
Particular events, like long-range Saharan dust transport, can lead to a dominating mass mode in the super-
m size range, even if the number of particles in that range is negligible in the total number.
As aerosol number and mass refer to different portions of the size distributions, these parameters are
governed by different processes, and consequently they have different life times. This implies that in general
no straight correlation can be expected between number and volume (or PM2.5, PM10), unless both are
controlled by strong direct emission or strong meteorological processes (e.g. dilution, wet scavenging). In
fact, a reduction of PM2.5 may lead to an increase in particle number, because a reduction of the particle
surface area also reduces the scavenging rate of ultrafine particles by bigger ones, hence increases the
lifetime of the former ones.
Aerosol surface area contributes mostly in the range between 0.1 and 1m, which corresponds broadly to the
PM2.5 range, hence some correlation may be expected for those two parameters.
B
o
x

5
18
Free Troposphere
Natural Rural Urban Kerbside Near-City
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Aspvreten (S)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
London-Marylebone (GB)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Harwell (GB)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Hohenpeissenberg (D)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
London-Bloomsbury (GB)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Ispra (I)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Milano-Bresso (I)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Jungfraujoch (CH)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Melpitz (D)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Leipzig 97-98 (D)
F
i
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8
a
F
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8
a
F
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8
a
F
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8
a
particle diameter between 0.001 and 1 m
number concentration as dN/dLog(Dp) between 10
2
and 10
5
morning traffic
afternoon
night
X axis
Y axis
19
Figure 8a Figure 8a Figure 8a Figure 8a shows particle number size distributions from 10 sites of The Network during summer. Shown are the median (thick lines) and
25 and 75% percentile (thin lines) distributions, during 3 periods of the day (morning hours, afternoon, night). Log-normal mode parameters for 3-
mode fittings of the number size distributions can be found in http://ies.jrc.cec.eu.int/Download/cc .
Morning size distributions are expected to be largely influenced by traffic (rush hours in cities), and afternoons are the most intensive photochemistry
periods. The aerosol observed during night time (little local emissions, no photochemistry) should indicate the local background. The arrows indicate
that Melpitz (D) and Ispra (I) are downwind of Leipzig (D) and Bresso-Milano (I), respectively.
At kerbside and urban background sites, particle number size distributions are dominated by a mode with a maximum at Dp = 20 - 30 nm, but also
show a second mode with a maximum around 100 nm. Part of this mode is to be attributed to the regional background (see below). However, the
particle number concentration in both modes increases during morning hours. This is most visible at the kerbside site, indicating that these two modes
are related to / affected by traffic. Measurements of car emissions on test benches attribute the mode of the smallest particles to nucleation of exhaust
gasses, and the mode of larger particles to primary emissions of soot particles.
The rural, near-city and urban background distributions show also a maximum around Dp =10 - 30 nm, during the afternoon. We conjecture that this is
due to nucleation of new particles in the local atmosphere. Major research programs have been undertaken recently to understand such nucleation
events and their role in sustaining the atmospheric particle number concentration (e.g.: Kulmala et al., 2001, http://venda.uku.fi/quest/, http://www.isas-
dortmund.de/2002/e/staff/hoffmann/nucvoc/nucvoc1.html).
In moving from kerbside to natural background sites there is a gradual decrease in the number concentration and a gradually decreasing contribution of
particles with Dp = 10 - 30 nm. This can generally be explained as follows: the clean sites are mainly affected by transport of aerosol particles from the
polluted regions. During transport dilution reduces the number concentration, whereas coagulation removes the smaller particles from the size
distribution (small particles collide with the bigger ones).
The most persistent mode in the particle number size distribution at all sites is the one centered around 100 - 200 nm. As mentioned before, it can result
of primary emissions, but also of growth of smaller particles by condensation and cloud processing (Raes et al., 2000). Aerosol removal processes are
very ineffective in this size range, the particles can travel long distances and will contribute to the regional and continental backgrounds. They
contribute to the rather constant PM2.5 mass concentrations in urban background and downwind near-city sites (see Figs. 4b, 9a).
20
s
Free Troposphere
Natural Rural Urban Kerbside Near-City
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Melpitz (D)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Leipzig 97-98 (D)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
London-Marylebone (GB)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Harwell (GB)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Hohenpeissenberg (D)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
London-Bloomsbury (GB)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Ispra (I)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Aspvreten (S)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Jungfraujoch (CH)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Copenhagen - Jagtvej (DK)
1.E+02
1.E+03
1.E+04
1.E+05
0.001 0.01 0.1 1
Milano-Bresso (I)
particle diameter between 0.001 and 1 m
number concentration as dN/dLog(Dp) between 10
2
and 10
5
morning
afternoon
night
X axis
Y axis
F
i
g

8
b
F
i
g

8
b
F
i
g

8
b
F
i
g

8
b
21
Fig 8b shows particle number size distributions from 10 sites of The Network during winter. Shown are the median (thick lines) and 25 and
75% percentile (thin lines) distributions, during 3 periods of the day (morning hours, afternoon, night). Log-normal mode parameters for two-mode
fittings of the number size distributions can also be found in http://ies.jrc.cec.eu.int/Download/cc .
At Ispra (near-city site), urban background and kerbside sites, winter time distributions are shifted towards larger numbers and diameters compared
with the summer time distributions in Fig 8a, specially during afternoons. Increased diameters can be explained by the condensation of semi-volatile
species, which is favored by cold temperatures in winter. At the rural sites, a higher concentration during summer compared to winter is evident for the
10-30 nm particles during the afternoon, which confirms the photochemical nature of these particles.
22
Natural Rural Near-city Urban Kerbside
0
10
20
30
40
50
60
J
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-
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(
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2
.
5

(

g
/
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)
0
10000
20000
30000
40000
50000
60000
J
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(
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-
S
C

(
D
)
N
(
D
p
>
1
0
n
m
)
,

#
/
c
m

DJF winter
MAM spring
JJA summer
SON autumn
F
i
g

9
a
F
i
g

9
a
F
i
g

9
a
F
i
g

9
a
F
i
g

9
b
F
i
g

9
b
F
i
g

9
b
F
i
g

9
b
23
Figure 9 shows the seasonal average of a) PM2.5 mass and b) particle number
concentrations, for those sites where both measurements are available simultaneously. These
sites are different from those plotted in Fig. 7, where we showed the sites where simultaneous
PM10 and PM2.5 data are available. However the same conclusions can be made for what
concerns PM2.5: there is no gradual (monotonic) increase in PM2.5 when ordering the sites
from natural background to kerbsides according to the EEA criteria, and PM2.5 mass
concentrations can be fairly similar at near-city, urban background and kerbside sites.
PM2.5 mass concentrations are again highest during winter in the polluted sites. At the clean
sites a maximum in summer is not observed as in Fig. 7b.
Among the sites in Fig. 9 and excluding the free tropospheric site (Jungfraujoch, CH), the
annual average PM2.5 concentration varies by a factor of about 3 between its minimum
(Aspvreten, S) and maximum value (London-M, GB). The annual average particle number
concentration, however, varies by a factor of about 10 between the same sites. This is
explained by the fact that the high number concentrations in urban and kerbside sites are due
to particles with Dp < 100 nm, which hardly contribute to the PM2.5 mass concentration.
The large seasonal variations in PM2.5 mass concentrations are generally not related to large
seasonal variations in particle number concentrations. Large PM2.5 mass concentrations
during cold seasons are therefore due to the fact that particles are on average larger (size
distributions are shifted towards larger diameter) due to the condensation of semi-volatile
species.
24
0
10
20
30
40
0 10 20 30 40 50 60
PM2.5 , g/m
P
a
r
t
i
c
l
e

v
o
l
u
m
e
,

/
c
m

y = x / 1.5
y = x / 1.7
0
1000
2000
3000
4000
5000
6000
7000
8000
0 10 20 30 40 50 60
PM2.5 , g/m
P
a
r
t
i
c
l
e

n
u
m
b
e
r

(
D
p
>
1
0
0

n
m
)
,

#
/
c
m

0
10000
20000
30000
40000
50000
60000
0 10 20 30 40 50 60
PM2.5 , g/m
P
a
r
t
i
c
l
e

n
u
m
b
e
r

(
D
p
>
1
0
n
m
)
,

#
/
c
m

F
i
g

1
0
a
F
i
g

1
0
a
F
i
g

1
0
a
F
i
g

1
0
a
F
i
g

1
0
b
F
i
g

1
0
b
F
i
g

1
0
b
F
i
g

1
0
b
F
i
g

1
0
c
F
i
g

1
0
c
F
i
g

1
0
c
F
i
g

1
0
c
25
Figure 10 shows the relationship between the seasonal average PM2.5 mass
concentration and a) the corresponding number concentration of particles with Dp > 10 nm,
b) particles with Dp > 100 nm and c) the particle volume concentration. The different colors
refer to the different sites ( natural, rural, near-city, urban, kerbside) and the
different symbols refer to the different seasons (square=DJF, triangle=MAM, circle=JJA,
diamond=SON).
Comparison of Figs 10a and 10b shows that 70-80% of the particles have a Dp < 100 nm. The
size-segregated composition of the aerosol at two polluted sites (see Fig. 16) suggests that
these particles mainly consist of carbonaceous material.
At the clean sites, there is a good linear correlation between PM2.5 and the particle number
concentrations. This is consistent with the notion that at those sites local sources of small
particles do not contribute much to the seasonal average number concentration, and that the
observed aerosol is mainly transported from elsewhere.
At the polluted sites the relationship between PM2.5 and the number of particles with Dp > 10
nm, seems to differ for near-city background, urban background and kerbside sites, and no
single relationship between PM2.5 and number (Dp > 10nm) can be proposed. In general the
particle number (Dp > 10 nm) increases more than proportionally to PM2.5 mass.
PM2.5 mass and sub-micron particle volume concentrations are fairly well correlated. The
ratio PM2.5 / volume corresponds to the aerosol density, which is expected to range between
1.5 and 1.7 (Mc Murry et al., 2002). The data point falling above the lines can be explained
only by experimental artefacts. For most points corresponding to rural, near-city and urban
background sites (located below the lines), the sub-micron aerosol mass accounts only for a
part of the PM2.5 mass. This confirms what was shown as the example on Fig. 1, that PM2.5
comprises a significant fraction of coarse-mode particles.
26
0
10
20
30
40
50
60
S
e
v
e
t
t
i
j
a
r
v
i

(
F
I
N
)
S
k
r
e
a
d
a
l
e
n

(
N
)
B
i
r
k
e
n
e
s

(
N
)
C
h
a
u
m
o
n
t

(
C
H
)
M
o
n
a
g
r
e
g
a

(
E
)
I
l
l
m
i
t
z

(
A
)
W
a
a
s
m
u
n
s
t
e
r

(
B
)
M
e
l
p
i
t
z

9
6
-
9
9

(
D
)
I
s
p
r
a

(
I
)
Z
u
e
r
i
c
h

(
C
H
)
B
a
s
e
l

(
C
H
)
G
e
n
t

(
B
)
B
o
l
o
g
n
a

(
I
)
B
a
r
c
e
l
o
n
a

(
E
)
B
e
r
n

(
C
H
)
W
i
e
n

(
A
)
P
M
1
0

(

g
/
m

)
BC
OM
unacc.
NO3
NH4
nssSO4
sea salt
min. dust
0
10
20
30
40
50
60
S
e
v
e
t
t
i
j
a
r
v
i

(
F
I
N
)
S
k
r
e
a
d
a
l
e
n

(
N
)
B
i
r
k
e
n
e
s

(
N
)
C
h
a
u
m
o
n
t

(
C
H
)
M
o
n
a
g
r
e
g
a

(
E
)
I
l
l
m
i
t
z

(
A
)
W
a
a
s
m
u
n
s
t
e
r

(
B
)
M
e
l
p
i
t
z

9
6
-
9
9

(
D
)
I
s
p
r
a

(
I
)
Z
u
e
r
i
c
h

(
C
H
)
B
a
s
e
l

(
C
H
)
G
e
n
t

(
B
)
B
o
l
o
g
n
a

(
I
)
B
a
r
c
e
l
o
n
a

(
E
)
B
e
r
n

(
C
H
)
W
i
e
n

(
A
)
P
M
1
0
-
P
M
2
.
5

(

g
/
m

)
BC
OM
unacc.
NO3
NH4
nssSO4
sea salt
min. dust
0
10
20
30
40
50
60
S
e
v
e
t
t
i
j
a
r
v
i

(
F
I
N
)
S
k
r
e
a
d
a
l
e
n

(
N
)
B
i
r
k
e
n
e
s

(
N
)
C
h
a
u
m
o
n
t

(
C
H
)
M
o
n
a
g
r
e
g
a

(
E
)
I
l
l
m
i
t
z

(
A
)
W
a
a
s
m
u
n
s
t
e
r

(
B
)
M
e
l
p
i
t
z

9
6
-
9
9

(
D
)
I
s
p
r
a

(
I
)
Z
u
e
r
i
c
h

(
C
H
)
B
a
s
e
l

(
C
H
)
G
e
n
t

(
B
)
B
o
l
o
g
n
a

(
I
)
B
a
r
c
e
l
o
n
a

(
E
)
B
e
r
n

(
C
H
)
W
i
e
n

(
A
)
P
M
2
.
5

(

g
/
m

)
BC
OM
unacc.
NO3
NH4
nssSO4
sea salt
min. dust
NB: For Chaumont, Monagrega, Melpitz, Zrich, Basel, Barcelona and Bern, only a subset of the
samples collected for PM mass concentrations were used for chemical analyses. As a consequence,
annual mean PM concentrations presented here can differ form the values shown in Fig. 3a and 3b.
F
i
g

1
1
a
F
i
g

1
1
a
F
i
g

1
1
a
F
i
g

1
1
a
F
i
g

1
1
c
F
i
g

1
1
c
F
i
g

1
1
c
F
i
g

1
1
c
F
i
g

1
1
b
F
i
g

1
1
b
F
i
g

1
1
b
F
i
g

1
1
b
Natural Rural Near-City Urban Kerbside
27
3.5 PM10 and PM2.5 chemical composition
Chemical characterization of aerosol particles is still affected by many problems related to
both sampling and analysis (see Annex 2).
Here we focus on aerosol chemical data when they can be compared with the PM10 or PM2.5
mass obtained in the same experiment. This allows a check of internal consistency of the data.
Figure 11 shows absolute annual average concentrations of the main aerosol
components in a) PM10, b) PM2.5 (the fine fraction) c) PM10-PM2.5 (the coarse
fraction). Numerical values are given in Annex 3.
Black carbon (BC), nitrate (NO
3
-
), and ammonium (NH
4
+
) concentrations result directly from
measurements. Organic matter concentrations (OM) were calculated by multiplying organic
carbon (OC) concentrations by a factor of 1.4 (e.g. Eatough et al., 1996) to account for the
non-C atoms contained in particulate OM. Sea-spray was clearly identified as a component of
the aerosol at sites located < 50 km from seashore. For consistency, the sea-salt concentration
was calculated from Na
+
and Cl
-
concentrations, even when the purely marine origin of Na
+
was not obvious. Likewise, non-sea-salt sulfate (nssSO
4
2-
) concentrations were calculated
from measured SO
4
2-
, Na
+
, and a standard sea water composition. The total amount of mineral
dust (min. dust), including silicates, carbonates, and minor amounts of calcium sulfate and
trace elements, was directly determined, or estimated based on measurements of tracers such
as Al or non-sea-salt Ca
2+
(see Annex 2).
Full chemical characterisations of the aerosol are still rarely achieved due to the large range of
methods needed to quantify the various aerosol components. Consequently, the unaccounted
mass (obtained as the difference between the gravimetrically measured aerosol mass
concentration and the sum of the aerosol component concentrations) can include different
species for the various sites of the network. The table below specifies what components make
up the unaccounted mass for each site. When all main aerosol components are analyzed (i.e.
at 9 sites only), the remaining unaccounted mass fraction (unknown) is thought to contain
residual water associated with the aerosol, or non-C atoms associated with particulate organic
matter which are not adequately accounted for by using a molecular mass - to - carbon mass
ratio of 1.4 (see Annex 2).
Site Aerosol components making-up the unaccounted mass
Sevettijarvi (FIN) unknown OM
Skreadalen (N) unknown NH4
+
NO3
-
OM
Birkenes (N) unknown NH4
+
NO3
-
OM
Chaumont (CH) unknown
Monagrega (E) unknown
Illmitz (A) unknown
Waasmunster (B) unknown NH4
+
NO3
-
OM
Melpitz (D) unknown sea salt OM
Ispra (I) unknown min. dust
Zuerich (CH) unknown
Basel (CH) unknown
Gent (B) unknown NH4
+
NO3
-
OM
Bologna (I) unknown
Barcelona (E) unknown
Bern (CH) unknown
Wien (A) unknown
28
0%
20%
40%
60%
80%
100%
S
e
v
e
t
t
i
j
a
r
v
i

(
F
I
N
)
S
k
r
e
a
d
a
l
e
n

(
N
)
B
i
r
k
e
n
e
s

(
N
)
C
h
a
u
m
o
n
t

(
C
H
)
M
o
n
a
g
r
e
g
a

(
E
)
I
l
l
m
i
t
z

(
A
)
W
a
a
s
m
u
n
s
t
e
r

(
B
)
M
e
l
p
i
t
z

9
6
-
9
9

(
D
)
I
s
p
r
a

(
I
)
Z
u
e
r
i
c
h

(
C
H
)
B
a
s
e
l

(
C
H
)
G
e
n
t

(
B
)
B
o
l
o
g
n
a

(
I
)
B
a
r
c
e
l
o
n
a

(
E
)
B
e
r
n

(
C
H
)
W
i
e
n

(
A
)
P
M
1
0

c
o
m
p
o
s
i
t
i
o
n
BC
OM
unacc.
NO3
NH4
nssSO4
sea salt
min. dust
0%
20%
40%
60%
80%
100%
S
e
v
e
t
t
i
j
a
r
v
i

(
F
I
N
)
S
k
r
e
a
d
a
l
e
n

(
N
)
B
i
r
k
e
n
e
s

(
N
)
C
h
a
u
m
o
n
t

(
C
H
)
M
o
n
a
g
r
e
g
a

(
E
)
I
l
l
m
i
t
z

(
A
)
W
a
a
s
m
u
n
s
t
e
r

(
B
)
M
e
l
p
i
t
z

9
6
-
9
9

(
D
)
I
s
p
r
a

(
I
)
Z
u
e
r
i
c
h

(
C
H
)
B
a
s
e
l

(
C
H
)
G
e
n
t

(
B
)
B
o
l
o
g
n
a

(
I
)
B
a
r
c
e
l
o
n
a

(
E
)
B
e
r
n

(
C
H
)
W
i
e
n

(
A
)
P
M
2
.
5

c
o
m
p
o
s
i
t
i
o
n
BC
OM
unacc.
NO3
NH4
nssSO4
sea salt
min. dust
0%
20%
40%
60%
80%
100%
S
e
v
e
t
t
i
j
a
r
v
i

(
F
I
N
)
S
k
r
e
a
d
a
l
e
n

(
N
)
B
i
r
k
e
n
e
s

(
N
)
C
h
a
u
m
o
n
t

(
C
H
)
M
o
n
a
g
r
e
g
a

(
E
)
I
l
l
m
i
t
z

(
A
)
W
a
a
s
m
u
n
s
t
e
r

(
B
)
M
e
l
p
i
t
z

9
6
-
9
9

(
D
)
I
s
p
r
a

(
I
)
Z
u
e
r
i
c
h

(
C
H
)
B
a
s
e
l

(
C
H
)
G
e
n
t

(
B
)
B
o
l
o
g
n
a

(
I
)
B
a
r
c
e
l
o
n
a

(
E
)
B
e
r
n

(
C
H
)
W
i
e
n

(
A
)
P
M
1
0

-

P
M
2
.
5

c
o
m
p
o
s
i
t
i
o
n
BC
OM
unacc.
NO3
NH4
nssSO4
sea salt
min. dust
F
i
g

1
2
a
F
i
g

1
2
a
F
i
g

1
2
a
F
i
g

1
2
a
F
i
g

1
2
b
F
i
g

1
2
b
F
i
g

1
2
b
F
i
g

1
2
b
F
i
g

1
2
c
F
i
g

1
2
c
F
i
g

1
2
c
F
i
g

1
2
c
Natural Rural Near-City Urban Kerbside
29
Figure 12 shows the annual averaged chemical composition of a) PM10 b) PM2.5
(the fine fraction), and c) PM10 PM2.5 (the coarse fraction).
Where all main aerosol components were measured they typically accounted for about 70% or
more of the PM10 and PM2.5 mass.
All compounds are present in both the fine and the coarse fraction.
Mineral compounds and sea salt contribute more to the coarse fraction, whereas ammonium
(NH
4
+
), non-sea-salt-sulfate (nssSO
4
2-
) and organic matter (OM) contribute more to the fine
fraction. Black carbon (BC) and nitrate (NO
3
-
) contribute more to the fine fraction, but their
contribution to the coarse fraction is only slightly less. OM in the fine fraction may result
from primary emissions from combustion processes or from the oxidation of volatile organic
compounds (VOC), whereas OM in coarse fraction may also include biological debris. Nitrate
in the fine fraction is bound by ammonia, whereas in the coarse fraction it is bound by
alkaline sea-salt and/or mineral dust particles. Black carbon in the coarse mode is difficult to
explain. Tire debris or soot deposited on re-suspended dust might account for a part of it, but
it might also result from an artifact of the measuring methods, which transforms OM into BC
by charring during the analysis.
Depending on the relative contribution of the fine and coarse fractions, the chemical
composition of PM10 and PM2.5 can be significantly different (e.g. Barcelona, E) or similar
(e.g. Bologna, I).
We obtain the following grand average compositions (%) by averaging the annual mean
contributions of each component to either PM10, PM10-PM2.5 and PM2.5:
PM10 PM2.5 PM10-PM2.5
N
a
t
u
r
a
l

&

R
u
r
a
l
B
a
c
k
g
r
o
u
n
d
N
e
a
r
-
c
i
t
y

&

U
r
b
a
n
B
a
c
k
g
r
o
u
n
d
K
e
r
b
s
i
d
e
N
a
t
u
r
a
l

&

R
u
r
a
l
B
a
c
k
g
r
o
u
n
d
N
e
a
r
-
C
i
t
y

&

U
r
b
a
n
B
a
c
k
g
r
o
u
n
d
K
e
r
b
s
i
d
e
N
a
t
u
r
a
l

&

R
u
r
a
l
B
a
c
k
g
r
o
u
n
d
N
e
a
r
-
C
i
t
y

&

U
r
b
a
n
B
a
c
k
g
r
o
u
n
d
K
e
r
b
s
i
d
e
Black Carbon
6 5 13 8 8
17 17 17 17
4 3 7
Organic Matter
16 16 16 16 20 20 20 20 22 22 22 22 23 23 23 23 22 22 22 22 29 29 29 29
4
8 88 8 10 10 10 10
Nitrate 7
15 15 15 15 10 10 10 10
5
17 17 17 17
11
8 88 8
7
8 88 8
Ammonium 6 7 4 8 10 7 1 1 0
Sulfate
19 19 19 19 13 13 13 13 10 10 10 10 29 29 29 29 17 17 17 17 13 13 13 13
3 5 5
Sea salt
8 4 3 3 3 1
20 20 20 20 9 99 9
6
Mineral dust
10 10 10 10
9
19 19 19 19
5 7 8
21 21 21 21 22 22 22 22 37 37 37 37
Unknown (*) 28 27 19 20 17 15 40 46 28
(*) calculated only when all the main aerosol components were measured.
The following data however show that the aerosol composition does change at a given site,
e.g. depending on the degree of pollution at the site.
30
0%
10%
20%
30%
40%
50%
S
e
v
e
t
t
ija
r
v
i
(
F
I
N
)
S
k
r
e
a
d
a
le
n

(
N
)
B
ir
k
e
n
e
s

(
N
)
P
u
y

d
e

D
o
m
e

(
F
)
C
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5
Natural Rural Near-city Urban Kerbside Natural Rural Near-city Urban Kerbside
Fig 13a Fig 13a Fig 13a Fig 13a Fig 13b Fig 13b Fig 13b Fig 13b
NB: Puy de Dme is a mountain site, where particles have to go through clouds before reaching the sampling station
31
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5
Figures 13a and 13b show the annual mean relative contribution of the individual species to PM10 and PM2.5, respectively,
further categorized according PM10 mass concentration.
There is a gradual decrease in the contribution of sulfate when moving from clean to polluted sites. It should be noted, however, that the measurements
at the natural background sites date from the early 1990s, whereas the other data date from around 2000, and that over large regions there has been a
40% reduction in sulfate concentrations during the 1990s. No single relationship between sulfate contribution and PM mass concentration is valid for
all sites.
Despite the large sampling and analytical uncertainties for black carbon and organic matter, their contribution to PM10 and PM2.5 seems to be fairly
constant and independent of PM10 mass concentration, as for sulfate. The fact that BC contribution to PM10 and PM2.5 is rather constant indicates
that even natural background sites are contaminated by long range transport of anthopogenic aerosol (BC is a tracer of combustion processes).
At kerbside sites, the contribution of mineral dust to PM10 is high, compared to urban background sites. This indicates once more the contribution of
traffic to the re-suspension of road dust. The mineral dust contribution decreases with increasing PM10, indicating that mineral dust itself does not lead
to high PM pollution events.
Nitrate contribution to PM10 and PM2.5 is low at the natural background sites, higher at near-city and urban background sites, and low again at
kerbside sites. Low contributions of nitrate at the natural background sites can be explained by the absence of local sources of NOx, precursor of
particulate NO
3
-
. The time needed to form particulate NO
3
-
from NOx might explain that nitrate contribution to PM10 and PM2.5 is higher at the near-
city sites, near by large NOx sources such as urban centers, than at kerbside sites. The contribution of nitrate to PM10 increases with the PM10 mass
concentration at all polluted sites, indicating that nitrate is important in governing high PM pollution events.
PM10 > 50 g/m 20 < PM10 < 50 g/m PM10 < 20 g/m Average
32

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5
Fig 14b Fig 14b Fig 14b Fig 14b Fig 14a Fig 14a Fig 14a Fig 14a
Natural Rural Near-city Urban Kerbside Natural Rural Near-city Urban Kerbside
33
0%
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50%
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5
Figures 14a and 14b show the seasonal average contributions of each species to PM10 and PM2.5 respectively. Numerical
values are available in http://ies.jrc.cec.eu.int/Download/cc . The most striking observation is the seasonality in the nitrate and organic matter
contribution to PM10 and PM2.5. Contributions of nitrate are up to 10 times higher during winter than during summer. This is quite different from the
seasonality of the other species (except organic matter), which excludes a pure explanation by meteorological dilution effects. Enhanced condensation
of nitrate and organic matter during cold periods could explain these observations. However, they might also be at least partially due to sampling
artifacts. The contribution of mineral dust to PM10, and to a lesser extent to PM2.5 is generally the highest in spring-summer at rural to urban
background sites. This might be related to farming activity intensity or precipitation or desert dust episode frequency.
DJF winter MAM spring JJA summer SON autumn
34
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM10 (g/m)
S
O
4

c
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t
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b
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n

t
o

P
M
1
0
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM10 (g/m)
N
O
3

c
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n
t
r
i
b
u
t
i
o
n

t
o

P
M
1
0
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM2.5 (g/m)
S
O
4

c
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b
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n

t
o

P
M
2
.
5
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM2.5 (g/m)
N
O
3

c
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b
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o

P
M
2
.
5
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM2.5 (g/m)
M
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l

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2
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5
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM2.5 (g/m)
B
C

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P
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2
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5
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM2.5 (g/m)
O
M

c
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o

P
M
2
.
5
0%
10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM10 (g/m)
M
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l

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10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM10 (g/m)
B
C

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P
M
1
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10%
20%
30%
40%
50%
0 10 20 30 40 50 60 70 80
PM10 (g/m)
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c
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F
i
g

1
5
F
i
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1
5
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i
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1
5
F
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1
5
35
Figure 15 shows the correlation between the contribution of the individual species
and the PM10 and PM2.5 mass, respectively. Data points are seasonal averages. The different
colours refer to the different sites ( natural, rural, near-city, urban, kerbside) and
the different symbols refer to the different seasons (square=DJF, triangle=MAM, circle=JJA,
diamond=SON).
Noticeable are the opposite trends of sulfate and nitrate. The contribution of sulfate decreases
whereas the contribution of nitrate increases with increasing PM. As mentioned earlier, the
decreasing trend in sulfate might be due to the fact that the measurements at the clean sites
date from the beginning of the 1990s, when sulfur emissions where higher than around 2000.
When using annual averages, like in Table on p. 29, sulfate and organic matter are the major
components to both PM2.5 and PM10. Fig. 15, however shows that at high PM2.5 or PM 10
values, i.e. those values that matter for human health, nitrate and organic matter are the major
contributors to PM. This is partially due to the fact that the highest PM2.5 mass
concentrations are found during winter, when nitrate and semi-volatile organic matter are
more stable in the particle phase.
PM2.5 or PM10 mass concentrations cannot be used as surrogates for the mass concentrations
of any individual components.
36
0
2
4
6
8
10
12
14
16
18
0.05-0.09 0.09-0.16 0.16-0.30 0.30-0.60 0.60-1.0 1.0-1.8 1.8-3.1 3.1-6.2 6.2-9.9
aerodynamic diameter (m)
d
M
/
d
L
o
g

D
p

(

g
/
m

)
BC
OM
unacc.
NH4
nssSO4
sea salt
min. dust
0
5
10
15
20
25
30
35
40
0.05-0.14 0.14-0.42 0.42-1.2 1.2-3.5 3.5-10
aerodynamic diameter (m)
d
M
/
d
L
o
g
D
p

(

g
/
m

)
BC
OM
unacc.
NO3
NH4
nssSO4
sea salt
min. dust
F
i
g

1
6
b
F
i
g

1
6
b
F
i
g

1
6
b
F
i
g

1
6
b
F
i
g

1
6
a
F
i
g

1
6
a
F
i
g

1
6
a
F
i
g

1
6
a
37
3.4 Size-segregated aerosol chemistry
Figure 16 Figure 16 Figure 16 Figure 16 shows examples of median size segregated aerosol chemical
composition observed at a) Gent (B) and b) Bologna (I) for the September-October periods
1999 and 2000, respectively (Maenhaut et al., 2002; Matta et al., in press).
Size distributions of BC, SO
4
2-
and mineral dust are similar at the two sites. BC and SO
4
2-
are
found mainly in the sub-micron aerosol fraction, whereas mineral dust is mainly in the coarse
fraction (as sea-salt in Gent). Particulate organic matter (OM) and NO
3
-
are also mainly in the
sub-micron fraction in Bologna, but are quite evenly distributed over the 50 nm 10 m size
range in Gent. NO
3
-
was not measured in the samples collected at Gent, but if we assume that
most of the unknown component was actually NO
3
-
, then NO
3
-
was also evenly distributed in
Gent. OM and NO
3
-
, which are two aerosol components particularly difficult to sample and
measure accurately, make up an important fraction of the particles with a diameter 0.3<Dp<1
m. Particles smaller than about 100 nm (i.e. more than 70% of the atmospheric particles)
consist mostly of carbonaceous components (OM and BC).
38
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39
Conclusions
1. The Network covers a wide variety of environmental conditions but only in Western
Europe: it has only two (nearby) sites that might be representative for semi-arid
Mediterranean conditions, and it lacks data from Eastern Europe. (Fig. 2, 3)
2. Background annual average ( std deviation) PM10 and PM2.5 mass concentrations for
continental Europe are 7.0 4.1 g m
-3
and 4.8 2.4 respectively. Median values (
median absolute deviation) are 8.0 1.0 and 5.0 1.4 g m
-3
, respectively. (Fig. 4)
3. A few sites in The Network exceed the EU 2005 annual PM10 standard of 40 g m
-3
. All
near-city background, urban background and kerbside sites exceed the EU 2010 annual
PM10 standard of 20 g m
-3
, as well as the USEPA annual PM2.5 standard of 15 g m
-3
.
PM concentrations in background city sites in some areas in Europe can be as high as
PM concentrations at kerbside sites in other parts of Europe, which shows the
importance of the regional aerosol background. (Fig. 4)
4. Considering all sites in The Network, PM2.5 and PM10 mass concentrations are
correlated with a correlation coefficient R = 0.95. However the PM2.5/PM10 ratio
(0.73 0.15) is too variable to propose a European-wide valid PM2.5 to PM10 ratio. At a
given site, the correlation between PM2.5 and PM10 is much better, with R ranging
between 0.978 and 0.998. Site-specific PM2.5/PM10 ratios range between 0.57 and 0.85.
(Fig. 5)
5. Most PM10 mass is present in the PM2.5 fraction, but PM2.5 also contains a significant
part of the coarse particle mode. (Fig. 1)
6. PM2.5/PM10 ratios increase with the PM10 concentration, except at kerbside sites.
Hence, pollution events (high PM10) are characterized by more fine aerosol, except at
kerbside sites where coarse re-suspended dust contributes more to PM10. (Fig. 6)
7. Particle (Dp > 10 nm) number concentrations increase more than proportionally to PM
mass. Number size distribution measurements explain this by a higher contribution of
small (Dp < 100 nm) particles when moving from clean to polluted sites. (Fig. 8, 9,
10)
8. Particle size distribution measurements show that most (70-80%) particles have a
diameter Dp < 100 nm. At polluted sites those particles consist mainly of carbonaceous
material (black carbon and organic matter). Large daily variations in the number
concentration of those particles are observed, which are linked to the traffic source
strength (in polluted sites) or to photochemical processes (in clean sites) (Fig. 8, 10,
16)
9. Considering data from all sites in The Network, no useful universal correlation is
found between PM2.5 or PM10 on the one hand and the particle (Dp > 10 nm) number
concentration on the other. The correlation is fairly good at clean sites but deteriorates in
polluted sites. (Fig. 9)
40
10. When all main chemical components of the aerosol are measured, they account for about
70% or more of the PM10 and PM2.5 mass. The rest is thought to be due to the presence
of water or to the underestimation of the molecular mass to carbon mass ratio when
calculating organic matter concentrations. (Fig. 12)
11. Sulfate and organic matter are the two main contributors to the annual average PM2.5
and PM10 mass concentration, except at kerbside sites, where mineral dust (including
trace elements) and black carbon are main contributors to PM10 and PM2.5,
respectively. Nitrate is the third most important contributor to PM2.5 and the fourth to
PM10. (Table on p. 29, Fig. 14)
12. No clear correlation exists between PM2.5 or PM10 mass concentrations on the one
hand, and chemical composition on the other, except for nitrate, which contribution
increases with increasing PM2.5 and PM10. When selecting only polluted conditions
(PM10 > 50 g m
-3
), then nitrate becomes the main contributor to PM10 and PM2.5
together with organic matter. (Fig. 13, 15)
13. At polluted sites PM2.5 and PM10 mass concentrations, as well as the particle (Dp > 10
nm) number concentration are highest during winter. Only the relative contribution of
nitrate (and to a lesser extent organic matter) has a similar seasonal behavior, indicating
the role of low temperatures in bringing semi-volatile ammonium nitrate and organic
matter from the gas phase to the particulate phase. (Fig. 7, 9, 14)
14. Black carbon contributes 5-10% to PM2.5 and somewhat less to PM10 at all sites,
including the clean background sites. Its contribution increases to 15-20% at some of the
kerbside sites. (Fig. 13, 15)
15. Points 6, 7,8, 13 and 14 above indicate that traffic is responsible for the high PM10 and
PM2.5 concentrations. This is either through the role of nitrate aerosols in the fine and
coarse fraction of the aerosol (at near-city and urban background sites) or due to the
contribution of re-suspended dust to the coarse fraction (at kerbside sites). (Fig 8, 9,
10, 13)
41
Concluding comments
The present analysis of simultaneously measured physical and chemical aerosol
characteristics shows that research programs can provide fundamental data to understand the
sources and transformation of aerosols. They could also be used to assess their effects on
human health and climate, but this is outside the scope of this report.
Simultaneous measurements allow for consistency checks between the data at a single site,
however the lack of harmonization of measuring techniques between research groups renders
a comparison between sites more difficult. Monitoring networks aim at harmonized
approaches, but are (presently) weak in providing the full range of aerosol parameters, needed
for assessing their effects.
Documenting temporal and spatial variation in aerosol characteristics is needed for both
process studies and modeling effort supports. The research community must work together
with the user community (health, climate, visibility, , legislators) to bridge the gap between
scientific measurement programs and monitoring programs. The establishment of a number of
super-sites, like the ones funded by the EPA in the United States
(http://www.epa.gov/ttn/amtic/supsites.html), is presently being discussed in Europe and
might offer a solution. The development of such a network should be considered a high
priority, and requires a strong link between regulatory monitoring networks (e.g. EMEP) and
the research community (e.g. EU, ESA-GMES, WMO-GAW and national research programs)
as well. There is currently an evolving cooperation between the major networks in this respect
i.e. through the EU FP5 GMES project CREATE (Construction, Use and Delivery of an
European Aerosol Database) to which both EMEP and the World Data Centre for Aerosols
under the WMO are involved. Further, the impact of particulate matter on global change also
calls for a close cooperation with non European activities.
However, apart from an investment in new measurement/monitoring approaches, funds
should also be made available for analyzing existing data. More research data are known to be
available. The fact that they are not analyzed has also to do with a funding system, which
tends to pay for generating new data rather than fully analyzing existing ones.
42
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43
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46
Annex 1. Data availability, instruments and sampling devices
Institute Site Lat Long Altitude Category Period Number size distribution,
relative humidity
PM10 sampling
for chemical analysis
PM2.5 sampling
for chemical analysis
PM10 mass
measurements
PM2.5 mass
measurements
Size segregated
chemical composition
Ghent Univ. Sevettijarvi (FIN) 69.35 28.50 130 natural Nov 93 - Jan 96 Virtual impactor Virtual impactor weighing (40% RH) weighing (40% RH)
Ghent Univ. Skreadalen (N) 58.82 6.72 465 natural Feb 91 - Feb 96 Stacked Filter Unit Stacked Filter Unit weighing (50% RH) weighing (50% RH)
ITM Aspvretren (S) 58.80 17.40 20 natural Jan 00 - Dec 00 DMPS (11-450 nm), dry TEOM - 50C
Ghent Univ. Birkenes (N) 58.38 8.25 190 natural Feb 91 - Feb 96 Stacked Filter Unit Stacked Filter Unit weighing (50% RH) weighing (50% RH)
NERI Copenhagen-Jagtvej (DK) 55.70 12.55 10 kerbside Feb 00 - Mar 00 DMPS (6-700 nm), dry
IfT Falkenberg (D) 52.00 14.13 60 rural Jul 98 - Aug 98 DMPS (3-800 nm), dry Estimated from volume
U. Birmingham Harwell (UK) 51.57 -1.32 125 rural May 98 - Nov 00 SMPS (12-437 nm), amb. TEOM - 50C TEOM - 50C
IfT Melpitz 97-99 (D) 51.53 12.93 86 near-city Dec 96 - Nov 97 DMPS (3-750 nm), dry Hi Vol sampler
Partisol (weekly) Partisol (weekly)
weighing (50% RH)
weighing (50% RH) weighing (50% RH)
IfT Melpitz 99 -01 (D) 51.53 12.93 86 near-city Dec 99 - Nov 01 Hi Vol sampler
Partisol (weekly) Partisol (weekly)
weighing (50% RH)
weighing (50% RH) weighing (50% RH)
U. Birmingham London-Bloomsbury (UK) 51.52 -0.13 30 urban Mar 98 - Nov 00 SMPS (12-437 nm), amb TEOM - 50C TEOM - 50C
U. Birmingham London-Marylebone (UK) 51.52 -0.15 30 kerbside Mar 98 - Nov 00 SMPS (12-437 nm), amb TEOM - 50C TEOM - 50C
IfT Leipzig-SC (D) 51.42 12.23 90 kerbside Oct 97 - Nov 97 DMPS (3 - 750 nm), dry Estimated from volume
IfT Leipzig 97-99 (D) 51.35 12.43 90 urban Aug 97 - Feb 99 DMPS (3 - 750 nm), dry Estimated from volume
IfT Leipzig 99-01 (D) 51.35 12.43 90 urban Feb 99 - Apr 01 DMPS (3 - 800 nm), dry Estimated from volume
Ghent Univ. Waasmunster (B) 51.12 4.08 20 near-city Jul 94 - Nov 95 Stacked Filter Unit Stacked Filter Unit weighing (50% RH) weighing (50% RH)
Ghent Univ. Gent (B) 51.02 3.73 10 urban May 93 - July 94
Sep 99 - Oct 99
Stacked Filter Unit Stacked Filter Unit weighing (50% RH) weighing (50% RH)
10-st. MOUDI + 12-st. SDI
Umveltbudesamt Illmitz (A) 48.23 16.36 117 rural Oct 99 - Oct 00
IfT Hohenpeissenberg (D) 47.80 11.02 988 rural Apr 98 - Aug 00 DMPS (3 - 677 nm), dry Estimated from volume
Umveltbudesamt Wien-Spittelauer Lnde (A) 47.75 16.75 160 kerbside Oct 99 - Oct 00
PSI Jungfraujoch (CH) 47.55 7.98 3580 free troposph. Jun 97 - May 98 SMPS (19 -788 nmm), dry Estimated from volume
EMPA Basel (CH) 47.53 7.58 316 urban Jan 98 - Mar 99 Hi Vol sampler Hi Vol sampler weighing (50% RH) weighing (50% RH)
EMPA Zrich-Wiedikon (CH) 47.37 8.53 415 kerbside Jul 98 - Feb 99 Hi Vol sampler weighing (50% RH)
EMPA Zrich (CH) 47.37 8.53 409 urban Jan 98 - Mar 99 Hi Vol sampler Hi Vol sampler weighing (50% RH) weighing (50% RH)
EMPA Chaumont (CH) 47.05 7.58 1136 rural Jan 98 - Mar 99 Hi Vol sampler Hi Vol sampler weighing (50% RH) weighing (50% RH)
EMPA Bern (CH) 46.95 7.43 545 kerbside Jan 98 - Mar 99 Hi Vol sampler Hi Vol sampler weighing (50% RH) weighing (50% RH)
EMPA Payerne (CH) 46.80 6.93 409 rural May 98 - Oct 98 Hi Vol sampler weighing (50% RH)
JRC Ispra (I) 45.82 8.63 209 near-city Feb 00 - Dec 00 DMPS (5-800 nm), dry Klein Filter Gert Klein Filter Gert weighing (30% RH) weighing (30% RH)
LaMP Puy de Dome (F) 45.77 2.97 1465 rural Feb 00 - Mar 01 CPC + PCASP, amb ELPI & SDI Impactors ELPI & SDI Impactors weighing (50% RH) weighing (50% RH) ELPI & SDI Impactors
JRC Milano-Bresso (I) 45.53 9.20 130 urban May 98 - Jun 98 DMPS (5-800 nm), dry Virtual impactor Virtual impactor weighing (20% RH) weighing (20% RH)
ISAC Bologna (I) 44.53 11.29 88 urban Jan 00 - Dec 00 6-st. Berner impactor 6-st. Berner impactor weighing (20% RH) weighing (20% RH) 6-st. Berner impactor
JRC Marseille-Vallon Dol (F) 43.35 5.40 150 urban Jun 01 - Jul 01 DMPS (7-566 nm), dry 9-st. Berner impactor 9-st. Berner impactor TEOM-SES & weighing weighing (20% RH) 9-st. Berner impactor
CSIC Barcelona (E) 41.37 2.12 30 kerbside Jun 99 - Jun 00 Hi Vol sampler Hi Vol sampler weighing (50% RH) weighing (50% RH)
CSIC Monagrega (E) 40.50 -0.20 598 rural Mar 99 - Jul 00 Hi Vol sampler weighing (50% RH)
IfT Mte. Foia (P) 37.32 -8.62 902 rural Jun 97 - Jul 97 DMPS (3 - 750 nm), dry weighing (60% RH) weighing (60% RH)
IfT Sagres (P) 36.98 -8.95 50 rural Jun 97 - Jul 97 DMPS (3 - 788 nm), dry 6-st. Berner impactor weighing (60% RH) weighing (60% RH) 6-st. Berner impactor
U. of Crete Finokalia (GR) 35.32 25.67 150 natural Jul 00 - Jan 01 11-st. Berner impactor 11-st. Berner impactor weighing (50% RH) 11-st. Berner impactor
DMPS: Differential Mobility Particle Sizer SMPS: Scanning Mobility Particle Sizer TEOM: Tapered Element Oscillating Microbalance CPC: Condensation Particle Counter PCASP: Passive Cavity Aerosol Spectrometer Probe
SES: Sample Equilibration System
47
Annex 1 (contd). Analytical techniques for chemical analyses
Institute Site Category Period Sampling substrate Min. SO4
2-
NH4
+
NO3
-
sea salt OC EC
Ghent Univ. Sevettijarvi (FIN) natural Nov 93 - Jan 96 polycarbonate PIXE & INAA PIXE & IC Ion Chromatography Ion Chromatography INAA light reflectance
Ghent Univ. Skreadalen (N) natural Feb 91 - Feb 96 polycarbonate PIXE & INAA PIXE INAA light reflectance
ITM Aspvretren (S) natural
Ghent Univ. Birkenes (N) natural Feb 91 - Feb 96 polycarbonate PIXE & INAA PIXE INAA light reflectance
NERI Copenhagen-Jagtvej (DK) kerbside Feb 00 - Mar 00
IfT Falkenberg (D) rural Jul 98 - Aug 98
U. Birmingham Harwell (UK) rural
IfT Melpitz 97-99 (D) near-city Dec 96 - Nov 97 quartz (Hi Vol)
PTFE (Low Vol)
estim. from nssCa
2+
IfT Melpitz 99 -01 (D) near-city Dec 99 - Nov 01 quartz (Hi Vol)
PTFE (Low Vol)
estim. from nssCa
2+
Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography
U. Birmingham London-Bloomsbury (UK) urban
U. Birmingham London-Marylebone (UK) kerbside
IfT Leipzig-SC (D) kerbside
IfT Leipzig 97-99 (D) urban
IfT Leipzig 99-01 (D) urban
Ghent Univ. Waasmunster (B) near-city Jul 94 - Nov 95 polycarbonate PIXE & INAA PIXE INAA light reflectance
Ghent Univ. Gent (B) urban May 93 - July 94
Sep 99 - Oct 99
polycarbonate
polycarbonate + Al
PIXE & INAA
PIXE
PIXE
PIXE
INAA
PIXE thermo-optical EGA
light reflectance
thermo-optical EGA
Umveltbudesamt Illmitz (A) rural Oct 99 - Oct 00 quartz (Hi Vol) estim. from nssCa
2+
IfT Hohenpeissenberg (D) rural
Umveltbudesamt Wien- Spittelauer Lnde (A) kerbside Oct 99 - Oct 00 quartz (Hi Vol) estim. from nssCa
2+
PSI Jungfraujoch (CH) free troposph.
EMPA Basel (CH) urban Jan 98 - Mar 99 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + coulometry EGA + coulometry
EMPA Zrich-Wiedikon (CH) kerbside Jul 98 - Feb 99 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + coulometry EGA + coulometry
EMPA Zrich (CH) urban Jan 98 - Mar 99 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + coulometry EGA + coulometry
EMPA Chaumont (CH) rural Jan 98 - Mar 99 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + coulometry EGA + coulometry
EMPA Bern (CH) kerbside Jan 98 - Mar 99 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + coulometry EGA + coulometry
EMPA Payerne (CH) rural May 98 - Oct 98 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + coulometry EGA + coulometry
JRC Ispra (I) near-city Feb 00 - Dec 00 quartz Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + NDIR EGA + NDIR
LaMP Puy de Dome (F) rural Feb 00 - Mar 01 Teflon, polyc., quartz Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography
JRC Milano-Bresso (I) urban May 98 - Jun 98 quartz + cellulose ashing Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + NDIR EGA + NDIR
ISAC Bologna (I) urban Jan 00 - Dec 00 Aluminum estim. from nssCa
2+
Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + NDIR EGA + NDIR
JRC Marseille-Vallon Dol (F) urban Jun 01 - Jul 01 quartz + cell. +alu ashing Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography EGA + NDIR EGA + NDIR
CSIC Barcelona (E) kerbside Jun 99 - Jun 00 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography
CSIC Monagrega (E) rural Mar 99 - Jul 00 quartz ICP-MS Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography
IfT Mte. Foia (P) rural Jun 97 - Jul 97 Tedlar + Alu C Z E C Z E C Z E C Z E
IfT Sagres (P) rural Jun 97 - Jul 97 Tedlar + Alu C Z E C Z E C Z E C Z E EGA + NDIR EGA + NDIR
U. of Crete Finokalia (GR) natural Jul 00 - Jan 01 polycarbonate Ion Chromatography Ion Chromatography Ion Chromatography Ion Chromatography
PIXE: Proton Induced X-Ray Emission IC: Ion Chromatography INAA: Instrumental Neutron Activation Analysis EGA: Evolved Gas Analysis ICP-MS: Inductively Coupled Plasma - Mass Spectroscopy NDIR: Non Dispersive Infra Red
CZE: Capillary Zone Electrophoresis
48
y = 1.12x + 1.83
R
2
= 0.84
0
10
20
30
40
50
0 10 20 30 40 50
Gravimetric PM10 (g/m)
T
E
O
M

/

S
E
S

P
M
1
0


(

g
/
m

)
y = 0.96x + 0.32
R
2
= 0.92
0
10
20
30
40
50
0 10 20 30 40 50
Gravimetric PM10 (g/m)
T
E
O
M

/

S
E
S

P
M
1
0


(

g
/
m

)
y = 0.89x - 0.48
R
2
= 0.89
0
50
100
150
0 50 100 150
Gravimetric PM10 (g/m)
T
E
O
M

/

S
E
S

P
M
1
0


(

g
/
m

)
y = 0.55x + 2.48
R
2
= 0.60
0
10
20
30
40
0 10 20 30 40
Gravimetric PM10 (g/m)
T
E
O
M

/

S
E
S

P
M
1
0


(

g
/
m

)
F
i
g

A
2

a
F
i
g

A
2

b
F
i
g

A
2

c
F
i
g

A
2

d
49
Annex 2. Data consistency
Various groups using different techniques obtained the data compiled in this document (see
Annex 1). Difficulties with comparing these data and possible sources of uncertainties are
discussed below. This discussion is mainly based on studies performed in the EUROTRAC
AEROSOL sub-project framework (http://aerosol.web.psi.ch/). We decided not to disregard
any of the data sets because of these uncertainties, since often the ranges of change in aerosol
particle properties discussed are larger than these uncertainties. A note is made in case the
uncertainties compromise our conclusions.
2.1 PM10 and PM2.5 sampling heads
Based on inertial impaction, aerosol sampling heads let pass particles with an aerodynamic
diameter (Dae) smaller than a certain cut-off (for a spherical particle of diameter Dp and
density , Dae = Dp
1/2
). Around the most often used cut-off diameters (2.5 and 10 m
aerodynamic diameter), the aerosol mass concentration is usually quite low, so that a slight
error in the cut-off diameters leads to small changes in PM mass concentrations.
2.2. PM mass concentrations: sampling artifacts
The PM mass concentrations compiled in this report were measured off-line by measuring the
mass of aerosol collected on a filter or an impactor foils, or on-line using tapered element
oscillating micro-balances (TEOM).
The European norm EN12341 recommends sampling on quartz filters and weighing them at
50% relative humidity for the determination of PM10 mass concentrations. However,
sampling on inert filters (Teflon and quartz) leads to variable losses of NH
4
NO
3
at T > 10 C
(Hering and Cass, 1999), and to both positive and negative artifacts for particulate organic
matter OM (Eatough et al., 1993, 1996). In contrast, negative artifacts in impactors due to the
volatilization of semi-volatile compounds at low pressure and to losses on impactor walls are
generally < 4% (Hering et al., 1997).
In Europe, the amount of NH
4
NO
3
and OM collected on quartz fiber filters, cascade impactors
and artifact free wet aerosol collectors was compared during laboratory (Petten wind tunnel,
1999) and field (Pipapo 1998, Melpitz Intercomp, 2000) experiments. Preliminary data can be
found in the EUROTRAC-AEROSOL annual reports 200 and 2001 (see
http://aerosol.web.psi.ch/). These experiments demonstrated that in summer time conditions
(T > 20 C) up to 100% of NH
4
NO
3
and can be lost from quartz fiber filters, even for
sampling times of a few hours (Schaap et al., in preparation). For carbonaceous aerosol, the
concentrations derived from cascade impactors were on average 65 (10) % of that obtained
with quartz filters, due to the loss of semi-volatile carbon from the impactors or to the
adsorption of volatile carbon in the filters or both (Even et al., in preparation). Such artifacts
can obviously affect significantly the determination of PM concentrations and seasonal
variations in NO
3
and OM contributions to PM.
On the other hand, at 50% relative humidity, aerosol particles can contain up to 30% of water
(see Guidelines for concentration and exposure response measurement of fine and ultra fine
PM in http://www.who.int/peh/air/PM/pmtoc.htm). This may be an important source of
inconsistency between the PM mass concentrations determined according to the EN 12341
norm and TEOMs. TEOMs indeed dry the sampled air stream to limit the quantity of water
associated with aerosol particles. Routine TEOMs do this by heating the inlet at 50 C,
whereas TEOMs equiped with a sample equilibration system (SES) achieve RH < 30% by
sampling through dryers and heating at 30 C only. Several studies, covering a range of
50
ambient conditions have demonstrated that because of these problems routine TEOMs
underestimate PM10 measurements by up to 35%, when compared with the EN 12341
reference method (http://www.defra.gov.uk/environment/airquality/airbornepm/ap00.pdf,
http://europa.eu.int/comm/environment/air/finalwgreporten.pdf, and Allen et al., 1997). This
underestimation is more severe in winter than in summer, because in summer the ambient and
instrument temperatures are more comparable. Fig. A2 shows a comparison of 24hr
averaged PM10 mass concentrations obtained with a TEOM operating at 30C with a SES
and gravimetric measurements at RH 20% at Monagrega (E) in (a) winter and (b) summer,
Marseille (F) surroundings in summer (c) and a Milan (I) suburb in winter (d). Fig A2a and
A2b indicate that losses of semi-volatile components are generally more important in a
TEOM (even at 30 C) than on quartz fiber filters. Fig A2c and A2d show a reasonable
agreement between these two techniques in summer time at a site characterised by low
NH
4
NO
3
aerosol content (Marseille) and acceptable losses in winter time at a site
characterised by high NH
4
NO
3
aerosol content (Milan).
Given the range of measuring conditions used (see Annex 1), a 35% difference between
gravimetric PM10 measurements carried out at 50% RH and on-line measurements using
TEOMs seems therefore to be an upper limit, and the PM10 mass concentrations shown in
this report are comparable within 35 %. This conclusion can be extended to the PM2.5 data.
2.3. Particle size distribution and number concentration
Particle size distributions were measured using differential mobility analysers (DMA)
connected to a particle counter (CPC). Some systems worked in scanning mode (SMPS),
others in step modes (DMPS). Standard deviations among 11 SMPS and DMPS instruments
was shown be < 22% and < 10% for sizing and counting, respectively (Dahmann et al., 2001).
The size measured by the DMA is affected by the RH at which the DMA is operating, and
should therefore be specified. Most size distributions were obtained at RH<20. % (see Table
1) and therefore comparable. Size distributions were generally not corrected for diffusion
losses of small particles (Dp 20nm), except for Jungfraujoch data.
The particle concentration is obtained by integrating the number size distribution. As the
range of particle diameters measured by various groups is different (Table 1), we considered
the number of particles with Dp > 10 nm when comparing of number concentrations between
sites. Number concentrations obtained in this way are expected to be comparable within 10%.
2.4. Aerosol chemical composition analyses
On top of sampling artifacts (2.2), the accuracy and consistency of analytical techniques have
to be considered when comparing aerosol chemical composition determined by different
laboratories using different methods (Annex 1).
The measurement of inorganic species in aerosol particles is straightforward and results from
different laboratories are usually within 10% for all major species except Ca
2+
(Putaud et al.,
2000).
The accurate determination of the concentration of the organic carbon (OC) in aerosol
particles remains challenging. Several intercomparisons organised in the framework of
EUROTRAC AEROSOL (e.g. Schmid et al, 2000) showed that the uncertainty in the
determination of total carbon (TC) is < 10%. It is however important to split TC between
organic carbon (OC) and black carbon (BC). The latter is exclusively emitted by combustion
processes, whereas OC consists of primary and secondary species from anthropogenic and
biogenic origins. The split between OC and BC is instrumentally defined and largely varies
51
from a method to another. Most OC data presented in this report were provided by
laboratories, which participate to the on-going Eurotrac-AEROSOL carbon shoot out. The
last (yet unpublished) results of this intercomparison indicate that their determination of OC
agree within 25%. The method used for analyzing samples collected in Austria generally
leads to twice higher EC values due to charring. Consequently, OC data derived from this
method are expected to be 20% lower. The determination of particulate organic matter (OM)
concentrations is also affected by the content of hetero-atoms (H, O, N, etc) is currently not
measured. To account for these atoms, molecular-to-carbon ratios between 1.2 and 1.7 were
proposed as correction factors (Gray et al., 1986; Malm et al., 1994; Eathough et al., 1996;
Hegg et al., 1997, Turpin et al., 2000). We consistently used a ratio equal to 1.4 to convert
organic carbon (OC) to organic matter (OM) concentrations.
The use of elemental analysis (e.g. PIXE, INAA, ICP-MS, ICP-AE) permits to obtain the
concentrations of many heavy elements but not of elements lighter than Na. Consequently, C
and N containing compounds were not determined by the laboratories using exclusively this
kind of technique. In contrast, specific tracers of various sources can be determined with these
methods. For instance, the amount and origin of mineral dust can be determined by measuring
Al, Fe, and other possible soil constituents. Experimental data show that SiO
2
/Al
2
O
3
ratio in
PM10 in most places range from 2.5 to 3.5. When quartz filters are used and Si cannot be
determined, SiO
2
values were indirectly assessed by multiplying Al
2
O
3
concentrations by a
factor of 3. When elemental techniques are not available, only the total amount of refractory
particulate compounds can be determined (by ashing ashless filter and weighing the residue).
Extended data sets show that in Western continental Europe, this total amount of mineral dust
is correlated with the amount of non-sea-salt Ca
2+
. When it was impossible to determine
mineral dust concentrations using others techniques, it was estimated by multiplying nssCa
2+
concentrations by 4.5.
The aerosol fraction called mineral dust therefore includes all non water soluble and non-
carbonaceous components and consists of soil dust, road dust, fly ash and minor elements.
Considering the various techniques used to assess this aerosol fraction, the uncertainties in
mineral dust concentrations are as large as 100%.
Another difficulty in comparing the aerosol chemical composition is that all main aerosol
components were not always analyzed by all groups. The difference between the
gravimetrically measured aerosol mass and the sum of the quantified aerosol components is
called unaccounted mass. For sites where some major components of the aerosol (e.g. OM,
NH
4
+
, NO
3
-
, sea-salt, mineral dust, BC) were not analyzed, the unaccounted mass fraction
includes one or several of these components, as specified in the Table on p. 27.
The discussion above shows how the chemical characterization of aerosol particles is still
affected by many problems related to both sampling and analysis. In this report we show only
aerosol chemical data when they can be compared with the PM10 or PM2.5 mass obtained in
the same experiment. This allows a check of internal consistency of a data set, hence a
minimum of quality control. However, a single laboratory may be able to perform total mass
and chemical mass determinations in a consistent way (e.g. avoiding or not positive and
negative artifacts for both determinations in the same way). Experiments in which all aerosol
components were measured are typically account for 70% of the PM10 and PM2.5 mass or
more. The remaining unknown fraction is thought to contain residual water associated with
the aerosol, or hetero-atoms associated with particulate organic matter which are not
adequately accounted for by using a molecular-to-carbon ratio of 1.4. This level of chemical
mass closure assures us that no large problems (uncertainties of more than a factor of 2) exist
in weighing and analysing the aerosol. Mass closure does not exclude, however, that the mass
and chemical measurements are affected by sampling artefacts, which can amount to 35%
(see above).
52
Annex 3. Log-normal mode parameters for three-mode fittings of the number size distributions
Particle number distributions are represented by the sum of 3 log-normal distributions:
( )

]
]
]
]
,
,

,


3
1
2
2
ln 2
ln ln
exp
ln 2
) (
ln
i gi
gi p
gi
i
p
p
D D
N
D
D d
dn

with
gi gi i
D N , , the fitted parameters (integrated number, geometric standard deviation, and geometric mean count diameter respectively).
Total number, surface area and volume are obtained from:
3 2 1
N N N N + + ( )
gi i gi i
N D S S S S S
2 2
3 2 1
ln 2 exp , + +
(
,
\
,
(
j
+ +
gi i gi i
N D V V V V V

2 3
3 2 1
ln
2
9
exp
6
,
S U M M E R S U M M E R S U M M E R S U M M E R
Category Site (country) Period N
1
(#/cm) D
g1
(m)
g1
N
2
(#/cm) D
g2
(m)
g2
N
3
(#/cm) D
g3
(m)
g3
N

(#/cm) V

(m/cm)
morning 343 0.059 1.76 180 0.149 1.61 524 1.02
afternoon 358 0.053 1.71 286 0.139 1.54 643 1.02
night 389 0.060 1.75 178 0.154 1.56 568 1.01
morning 71 0.024 1.53 1534 0.073 1.63 324 0.232 1.39 1929 4.40
afternoon 185 0.026 1.56 1364 0.085 1.61 276 0.246 1.38 1825 4.63
night 160 0.040 1.56 1718 0.082 1.70 224 0.245 1.38 2101 4.48
morning 993 0.027 1.54 639 0.059 1.38 1415 0.104 1.86 3047 4.83
afternoon 2089 0.028 1.53 553 0.060 1.36 1459 0.114 1.69 4101 4.10
night 1790 0.047 1.76 553 0.070 1.42 773 0.153 1.61 3116 4.57
morning 367 0.012 1.52 1192 0.036 2.00 1185 0.105 1.99 2743 6.36
afternoon 468 0.013 1.61 1629 0.030 2.00 1241 0.115 1.90 3337 6.59
night 94 0.024 1.74 1668 0.051 1.94 557 0.161 1.64 2319 4.55
morning 3467 0.013 2.00 1142 0.056 1.49 1460 0.117 1.84 6069 6.78
afternoon 2938 0.013 1.95 3989 0.032 2.00 1356 0.123 1.73 8283 5.66
night 1011 0.014 1.73 2228 0.058 1.65 1023 0.158 1.66 4262 7.53
morning 632 0.010 1.93 2575 0.030 1.87 3609 0.095 1.89 6817 10.25
afternoon 638 0.010 1.69 2508 0.027 1.61 4863 0.093 1.90 8010 13.03
night 256 0.018 1.73 2084 0.047 1.71 2859 0.120 1.81 5199 12.80
morning 3461 0.025 1.49 7412 0.059 2.00 10873 7.04
afternoon 4933 0.027 1.56 5572 0.067 2.00 10505 7.64
night 3047 0.033 1.85 3373 0.073 2.00 6421 6.19
morning 12921 0.016 1.99 3360 0.050 1.65 2431 0.113 1.97 18712 15.65
afternoon 7751 0.011 1.78 5422 0.041 2.00 599 0.189 1.55 13773 6.69
night 3711 0.015 2.00 5118 0.043 1.96 676 0.185 1.62 9505 7.96
morning 3664 0.014 1.37 12914 0.025 1.56 13961 0.059 2.00 30539 13.41
afternoon 3187 0.014 1.40 10981 0.027 1.58 11527 0.061 2.00 25696 12.34
night 2917 0.014 1.40 5233 0.024 1.68 6178 0.068 2.00 14329 9.05
morning 24092 0.021 1.77 26919 0.037 2.00 6872 0.111 1.74 57883 26.28
afternoon 23586 0.020 2.00 13734 0.030 1.57 18452 0.074 1.97 55771 32.19
night 16333 0.017 1.84 8192 0.029 1.79 9670 0.072 2.00 34195 16.89
Mode 2
urban Milano-Bresso (I)
near-city Melpitz (D)
near-city Ispra (I)
rural Harwell (GB)
kerbside London-M (GB)
urban London-B (GB)
urban Leipzig (D)
rural Hohenpeissenberg (D)
free trop. Jungfraujoch (CH)
natural Aspvreten (S)
Mode 3 Total (from fittings) Mode 1
53
W I N T E R W I N T E R W I N T E R W I N T E R
Category Site (country) Period N
1
(#/cm) D
g1
(m)
g1
N
2
(#/cm) D
g2
(m)
g2
N
3
(#/cm) D
g3
(m)
g3
N

(#/cm) V

(m/cm)
morning 123 0.033 1.80 40 0.066 1.96 33 0.115 1.48 196 0.11
afternoon 184 0.031 1.99 49 0.077 2.00 28 0.116 1.45 261 0.17
night 102 0.033 1.78 75 0.048 2.00 31 0.121 1.49 209 0.10
morning 287 0.024 1.51 716 0.058 1.55 425 0.198 1.52 1428 3.99
afternoon 374 0.022 1.72 711 0.061 1.66 354 0.209 1.44 1439 3.38
night 20 0.011 1.42 1170 0.049 1.75 410 0.199 1.49 1600 3.79
morning 758 0.033 1.42 338 0.061 1.34 871 0.116 1.75 1967 3.03
afternoon 670 0.032 1.39 426 0.058 1.36 854 0.113 1.71 1950 2.41
night 520 0.036 1.37 400 0.063 1.34 746 0.130 1.63 1666 2.60
morning 363 0.014 1.64 1119 0.048 2.00 247 0.180 1.50 1729 2.14
afternoon 1173 0.010 1.63 1839 0.035 2.00 633 0.138 1.79 3645 4.37
night 80 0.013 1.40 1086 0.040 2.00 432 0.140 1.74 1599 2.84
morning 3433 0.013 1.78 1925 0.059 1.76 507 0.200 1.65 5865 7.54
afternoon 3784 0.012 1.81 1762 0.051 1.70 603 0.177 1.62 6149 5.33
night 1756 0.021 2.00 995 0.067 1.57 743 0.163 1.87 3494 10.38
morning 6889 0.041 1.84 6067 0.125 1.62 12956 19.06
afternoon 4731 0.035 1.91 7416 0.110 1.71 12147 19.39
night 2908 0.052 1.74 9541 0.118 1.62 12449 24.06
morning 15390 0.027 1.67 9736 0.068 2.00 25127 14.21
afternoon 14511 0.027 1.69 11314 0.066 2.00 25824 15.08
night 5633 0.026 1.69 5477 0.070 2.00 11110 8.57
morning 21319 0.018 1.98 1911 0.079 1.51 1724 0.161 1.80 24954 19.30
afternoon 16231 0.016 2.00 2474 0.063 1.65 2085 0.145 1.90 20790 22.36
night 9775 0.017 2.00 1869 0.064 1.63 1580 0.153 1.90 13223 19.56
morning 13577 0.031 1.66 15806 0.114 1.83 29383 63.77
afternoon 12013 0.028 1.71 19267 0.096 2.00 31280 77.16
night 4398 0.029 1.71 12060 0.123 1.74 16457 47.32
morning 11442 0.018 2.00 40878 0.025 1.60 24044 0.066 2.00 76364 33.39
afternoon 11478 0.023 2.00 37570 0.026 1.61 31623 0.066 2.00 80671 43.00
night 12069 0.021 1.56 13212 0.031 2.00 4531 0.087 2.00 29812 15.32
morning 23020 0.025 1.71 9274 0.075 1.95 32295 15.72
afternoon 13342 0.024 1.74 5830 0.073 2.00 19172 10.73
night 5798 0.034 1.97 648 0.165 1.64 6446 5.52
Leipzig (D)
Milano-Bresso (I)
London-M (GB)
Copenhagen-J (DK)
urban
kerbside
kerbside
Jungfraujoch (CH)
Aspvreten (S)
Harwell (GB)
Hohenpeissenberg (D)
Melpitz (D)
Ispra (I)
London-B (GB)
near-city
near-city
urban
urban
free trop.
natural
rural
rural
Mode 1 Mode 2 Mode 3 Total (from fittings)
NB: fittings give a reliable parametric description of the sub-micron aerosol size distribution. The 9 mode parameters can be used to calculate any property that has to be derived
from size distributions for different periods of the day. However, one should be careful in comparing single modes of different sites. Often, more solutions for a 3-mode description
of a given distribution can be given, resulting in the same sum, but with significantly different mode parameters. Therefore, no statements can be made on trends or properties of
single modes.
54
Annex 3 (contd). PM10 annual average chemical composition
Category Site (Country) min. dust sea salt nssSO4 NH4 NO3 unacc. OM BC PM10 PM2.5 Min/PM10 SO4/PM10 NO3/PM10 OM/PM10 BC/PM10
natural Sevettijarvi (FIN) 0.30 0.95 1.26 0.17 0.06 1.51 NM 0.24 4.50 3.41 0.07 0.28 0.01 NM 0.05
natural Skreadalen (N) 0.48 1.11 1.43 0.53 0.63 3.29 NM 0.54 8.01 5.05 0.06 0.18 0.08 NM 0.07
natural Birkenes (N) 0.71 1.08 1.80 0.58 0.71 2.48 NM 0.58 7.94 4.92 0.09 0.23 0.09 NM 0.07
rural Chaumont (CH) 1.88 0.21 1.98 0.76 0.53 2.90 1.69 0.58 10.52 8.09 0.18 0.19 0.05 0.16 0.06
rural Monagrega (E) 4.14 0.67 2.87 1.03 2.10 3.55 2.25 0.64 17.30 NM 0.24 0.17 0.12 0.13 0.04
rural Illmitz (A) 1.02 0.20 4.17 2.10 2.71 6.34 5.40 1.99 23.92 19.94 0.04 0.17 0.11 0.23 0.08
near-city Waasmunster (B) 3.76 3.49 5.98 NM NM 22.57 NM 1.51 39.55 25.58 0.10 0.15 NM NM 0.04
near-city Melpitz 96-99 (D) 3.34 NM 3.40 2.13 3.90 17.19 NM 1.27 24.17 16.85 0.14 0.14 0.16 NM 0.05
near-city Ispra (I) NM NM 3.20 1.66 2.97 11.12 8.12 1.52 29.51 24.50 NM 0.11 0.10 0.28 0.05
urban Zuerich (CH) 2.85 0.29 3.50 1.92 3.38 5.47 5.00 2.09 24.50 18.98 0.12 0.14 0.14 0.20 0.09
urban Basel (CH) 3.15 0.46 3.88 1.96 3.21 5.71 4.98 1.97 25.77 17.85 0.12 0.15 0.12 0.19 0.08
urban Gent (B) 3.67 3.62 7.28 NM NM 20.52 NM 1.97 39.80 26.39 0.09 0.18 NM NM 0.05
urban Bologna (I) 4.92 1.26 4.80 4.22 9.37 9.41 9.29 3.04 44.23 35.82 0.11 0.11 0.21 0.21 0.07
kerbside Barcelona (E) 13.71 2.31 6.91 2.82 6.42 5.20 12.38 3.11 52.85 34.61 0.26 0.13 0.12 0.23 0.06
kerbside Bern (CH) 7.64 1.41 3.23 1.43 3.35 8.41 9.07 5.67 40.22 22.65 0.19 0.08 0.08 0.23 0.14
kerbside Wien (A) 5.88 0.95 5.08 2.12 4.52 14.74 10.61 10.68 54.58 38.51 0.11 0.09 0.08 0.19 0.20
Concentrations in g/m
Unacc.: difference between PM mass and the sum of the quantified PM components (unaccounted mass)
NM: not measured
55
Annex 3 (contd). PM2.5 annual average chemical composition
Category Site (Country) min. dust sea salt nssSO4 NH4 NO3 unacc. OM BC PM10 PM2.5 Min/PM2.5 SO4/PM2.5 NO3/PM2.5 OC/PM2.5 BC/PM2.5
natural Sevettijarvi (FIN) 0.15 0.46 1.29 0.15 0.02 1.12 NM 0.23 4.50 3.41 0.04 0.38 0.01 NM 0.07
natural Skreadalen (N) 0.18 0.29 1.28 NM NM 2.33 NM 0.48 8.01 5.05 0.04 0.25 NM NM 0.10
natural Birkenes (N) 0.25 0.34 1.61 NM NM 1.59 NM 0.52 7.94 4.66 0.05 0.35 NM NM 0.11
rural Chaumont (CH) 0.77 0.11 2.41 0.84 0.29 1.71 1.70 0.42 10.52 8.09 0.10 0.01 0.10 0.21 0.05
rural Monagrega (E)
rural Illmitz (A) 0.26 0.11 3.97 2.04 2.28 4.12 5.49 1.66 23.92 19.94 0.01 0.01 0.10 0.21 0.08
near-city Waasmunster (B) 0.98 1.13 5.04 NM NM 15.12 NM 1.42 39.55 25.58 0.04 0.20 NM NM 0.06
near-city Melpitz 96-99 (D) 1.80 NM 2.69 1.99 3.43 10.83 NM NM 24.17 16.85 0.11 0.16 0.20 NM NM
near-city Ispra (I)
urban Zuerich (CH) 1.18 0.17 3.27 1.84 2.68 3.60 4.44 1.66 24.50 18.98 0.06 0.17 0.14 0.23 0.09
urban Basel (CH) 1.40 0.25 3.80 1.83 2.47 2.57 4.21 1.54 25.77 17.85 0.08 0.21 0.14 0.24 0.09
urban Gent (B) 1.05 1.31 6.17 NM NM 13.70 NM 1.83 39.80 26.39 0.04 0.23 NM NM 0.07
urban Bologna (I) 2.89 0.84 4.62 4.12 8.54 7.55 8.24 2.91 44.23 35.82 0.08 0.13 0.24 0.23 0.08
kerbside Barcelona (E) 3.79 0.81 5.60 3.31 4.27 1.96 11.89 2.98 52.85 34.61 0.11 0.16 0.12 0.34 0.09
kerbside Bern (CH) 1.35 0.21 2.67 1.40 2.32 4.07 6.68 3.95 40.22 22.65 0.06 0.12 0.10 0.29 0.17
kerbside Wien (A) 2.37 0.41 4.44 2.18 3.57 7.84 8.62 9.10 54.58 38.51 0.06 0.12 0.09 0.22 0.24
Concentrations in g/m
Unacc.: difference between PM mass and the sum of the quantified PM components (unaccounted mass)
NM: not measured
For Melpitz, averages are calculated from 7-day integrated samples
For Wien, PM2.5 samples were not collected on the same days as PM10 samples