ARTICLE IN PRESS

AE International – Europe

Atmospheric Environment 38 (2004) 6547–6555

[Link]/locate/atmosenv

Speciation and origin of PM10 and PM2.5 in selected

European cities
X. Querola,, A. Alastueya, C.R. Ruiza, B. Artiñanob, H.C. Hanssonc,
R.M. Harrisond, E. Buringhe, H.M. ten Brinkf, M. Lutzg, P. Bruckmannh,
P. Straehli, J. Schneiderj
a
Instituto do Ciencias de la Tierra del CSIC, C/Luis Solé y Sabaris s/n, 08028 Barcelona, Spain
b
CIEMAT, Avda. Complutense 22, 28040 Madrid, Spain
c
Institute of Applied Environmental Research, University of Stockholm, Stockholm, Sweden
d
University of Birmingham, Division of Environmental Health & Risk Management, Edgbaston, Birmingham B15 2TT, UK
e
Rijksinstituut voor Volksgezondheid en Milieu, Bilthoven, The Netherlands
f
ECN, bld 004, PO Box 1, 1755 ZG Petten, Netherlands
g
Senate Department of Urban Development, Unit IX D, BrückenstraX e 6, 10173 Berlin, Germany
h
Landesumweltamt NRW, Wallneyer StraX e 6, 45133 Essen, Germany
i
Swiss Agency for the Environment, Air Pollution Control Division, CH 3003 Berne, Switzerland
j
Federal Environment Agency, Department of Air Quality Control, Vienna, Austria
Received 16 February 2004; received in revised form 7 June 2004; accepted 7 August 2004

Abstract

PM characteristics of seven selected regions within the European Union (EU) were analysed and compared. Results
of levels and speciation studies of PM10 and PM2.5 (with at least one year of data coverage from 1998 to 2002) at
regional, urban background and kerbside sites were assessed. Based on the examples selected, PM10 levels (annual
mean) ranged from 19 to 24 mg m 3 at regional background sites, from 28 to 42 mg m 3 at urban background, and from
37 to 53 mg m 3 at kerbside sites. PM2.5 levels varied from 8 to 20 mg m 3 at regional background sites, 20 to 30 mg m 3
at urban background and 25 to 40 mg m 3 at kerbside sites. The ratio PM2.5/PM10 is highly dependent on the type of
site and varied widely between different EU regions. Source apportionment results showed that, on an annual average,
the natural contribution (mineral and marine) at EU regional sites was in the range of 4–8 mg m 3 in PM10 decreasing in
PM2.5, but contributions up to 19 mg m 3 were reported for specific locations. At urban sites, carbonaceous aerosols
and secondary inorganic compounds accounted for a major fraction of PM10, and especially of the PM2.5 mass.
Quantitative data on the contributions of the regional background, city background and local traffic to the mean
annual levels of PM10, PM2.5 and major components were supplied. Climatic differences, long-range transport
processes and winter traffic peculiarities (the latter in northern countries) contributed to the increase of PM10 and
PM2.5 masses. At kerbside sites, an important dust contribution to PM2.5 is highlighted.
r 2004 Elsevier Ltd. All rights reserved.

Keywords: PM10; PM2.5; EU; Urban; Road traffic; Source apportionment; Regional contribution

Corresponding author. Fax: +34 93 4110012

E-mail address: [Link]@[Link] (X. Querol).

1352-2310/$ - see front matter r 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/[Link].2004.08.037
 ARTICLE IN PRESS
6548 X. Querol et al. / Atmospheric Environment 38 (2004) 6547–6555

1. Introduction Given the difficulty of reporting general PM composi-

tional characteristics for the EU, case studies on PM
Atmospheric particulate matter (PM) is made up of a speciation performed during 1998–2002 in Germany,
mixture of solid and aqueous species which enter the Spain, United Kingdom (UK), The Netherlands, Swe-
atmosphere by anthropogenic and natural pathways. den, Switzerland, and Austria were selected to illustrate
Owing to the large number of natural and anthropogenic different scenarios of PM in the EU. The main aim of
sources, PM may present diverse physical (size, surface this study is not to compile information on PM from
area, density, number) and chemical patterns in different different European sites, but to compare and interpret
areas. In addition to the local and regional anthropogenic PM characteristics of seven selected regions in Europe,
particulate emissions, both the levels and composition of some of them, with varying climatic patterns. Detailed
ambient air PM depend on the climatology (temperature, data on PM characteristics and source apportionment of
humidity, radiation, rain scavenging potential, re-circula- a wide variety of sites in the EU may be found in Putaud
tion of air masses vs. dispersive conditions) and on the et al. (2004) and van Dingenen et al. (2004), or in
geography (topography, soil cover, proximity to arid national reports of Member states (APEG, 1999; Visser
zones or to the coast) of a given region. Therefore, wide et al., 2001; Quass and Kuhlbusch, 2002; Querol et al.,
variations in PM levels and characteristics may be 2003; amongst others).
expected when considering European Union (EU) regions
such as the Mediterranean and Scandinavian countries
with very different climatologic and geographical pat- 2. Methodology
terns. However, the European Community fixed limit
values for ambient concentrations of PM for the whole The aim of this paper was to provide information on
EU. Thus, the Air Quality Directive 1999/30/EC sets PM10 and PM2.5 speciation and origin in selected
out limit values for PM10 and also considers the European cities. The selection did not cover all
possibility of setting PM2.5 standards as a follow-up of possibilities existing across EU, but focused on the
a review foreseen for 2004. Thus, annual and daily limit choice of different climate regions such as Southern
values for PM10 concentrations in ambient Spain or Sweden. Selecting criteria for the sites were
air which should not be exceeded after specific dates based on: (a) coverage of very different climate regions,
were established. The number of times the daily limit (b) availability of at least one year of measurement,
value of 50 mg m 3 exceeds should not be more than 35 (c) performance of measurements with an EU reference
times per year by 2005 and 7 by 2010. The annual limit gravimetric system or with a real time PM measur-
value was 40 and 20 mg m 3, respectively, for the same ing instrument but with data corrected versus
dates. It should be mentioned that the PM10 objectives to the gravimetric reference method. This ensures the
be reached in 2010 are indicative limit values. The recent measurement comparability. Although we know that
II Position Paper on PM produced in the EU proposes this reference method has some sampling artefact
the change of limit values to PM2.5 metrics with the problems, we intended to study the speciation and
suggestion of an annual PM2.5 limit value in the range of origin of PM sampled with this method since EU air
12–20 mg m 3 and a daily limit value of 35 mg m 3 not to quality standards have to be met with this type of
be exceeded more than 35 days a year. measurement.
Moreover, the Member States adopted different The data from the case studies discussed in this paper
strategies for designing the air quality monitoring were obtained from the following sources (Fig. 1):
networks. Thus, data from Airbase 2001 (http://
[Link]/databases/[Link]) show  PM data from Berlin, Germany, in 1998 from
that 71% of the monitoring stations are hotspots Lenschow et al. (2001). Data for 2000–2001 were
(kerbside and industrial sites) in one Member State, obtained from Abraham (2001) (Senate Department
whereas the proportion of hotspot stations in other of Urban Development, Berlin, personal communica-
Member States may drop to 13%. Consequently, tion).
differences among the mean PM levels reported by  PM data from rural and urban background and
different Member States do not necessarily reflect the kerbside sites in Spain for the period 1999–2001 were
degree of particulate pollution. obtained from Querol et al. (2001, 2003), Artiñano et
Source apportionment analysis may contribute to the al. (2003) and Rodrı́guez et al. (2002) and from
evaluation of the origin of PM10 and PM2.5. For these EMEP (Co-operative Programme for Monitoring
studies, the speciation of PM is used to identify and and Evaluation of the Long-Range Transmission of
quantify the PM load from the different emission Air Pollutants in Europe) for 2001.
sources (Thurston and Spengler, 1985; Harrison et al.,  PM data from Sweden for 1999–2001 were extracted
1997a, b; Pio et al., 1996, 1998; Liu et al., 2003; Kim from Areskoug et al. (2004) and Swietlicki et al.
et al., 2003; among others). (2004).
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X. Querol et al. / Atmospheric Environment 38 (2004) 6547–6555 6549

In this study we consider regional background sites to

rural or natural background sites isolated from the
direct influence anthropogenic sources, but representing
the regional background of the areas where the urban
areas are located. Urban background sites are consid-
ered here as those stations located in urban areas but
isolated from the direct influence of traffic or industrial
emissions (far from industrial sources or 425 m from a
high density road traffic way). Finally, kerbside sites are
those located at a very short distance from the road
pavement of a high-density traffic street.
In order to facilitate interpretation, case studies
supplying data on the chemical composition of PM10
and PM2.5, based on similar methods, were selected.
The examples selected had at least one year of data
coverage. Most of them supplied data on speciation at
Fig. 1. Location of the measuring sites selected in this study
classified as urban sites (kerbside sites and background sites) or
least on 1 day in each of 6 days devices. Sample handling
regional background sites. followed specification from standard EN-1234-1 prior to
analysis of the mass concentration. Special attention was
paid to prevent possible volatilisation of PM species
after sampling. High- or low-volume samplers equipped
 PM data for UK were derived from four paired urban with PM10 and PM2.5 or PM10-2.5 and PM2.5 inlets
background and kerbside sites in London and and quartz fibre or Teflon filters were used for sampling.
Birmingham operated by the University of Birming- The levels of PM were obtained in all cases by
ham (Harrison et al., 2003 and 2004). conventional gravimetrical procedures, and ion chroma-
 PM data for The Netherlands were obtained from tography or capillary electrophoresis, and colorimetry
RIVM (Rijksinstituut voor Volksgezondheid en were used to determine the levels of major anions and
Milieu), National Institute of Public Health and the soluble cations. The biggest differences in the methodo-
Environment from The Netherlands. logical procedures were attributed to the different
 PM data for Austria (Vienna and a rural site) were analytical approaches used for determining the levels
supplied by the Federal Environment Agency in of carbonaceous species (i.e. levels of elemental carbon
Vienna. (EC) and carbonaceous organic matter (OC)) and
 PM data for Switzerland (Bern and surroundings) mineral matter. For this reason, to minimise the effect
were provided by the Agency for the Environment of the different methods employed, we compared the
in Bern. levels of total carbon (OC+EC) but we did not consider
the levels of OC and EC separately. As regards the
For most of the studies PM characteristics measured mineral (or crustal) elements, different approaches were
for background, urban, and kerbside sites of the same used. In the case studies of Spain and The Netherlands,
region were compared by decomposing PM parameters the mineral load was estimated from the addition of
in regional and urban background levels and kerbside SiO2, Al2O3, Fe, Ca, P, Ti, K, Mg and Mn levels. In the
contributions following the methodology of Lenschow German study, the difference between the gravimetric
et al. (2001). Using this methodology, a simple source PM levels and the sum of the levels of carbonaceous
apportionment analysis is carried out by considering the matter, sulphate, nitrate, ammonium and chloride
scenario of an urban background as an ‘‘island’’ of were used to represent the mineral and water loads. In
elevated PM-levels arising from a regional background, case studies from the UK, the mineral load was
and on top definite peak concentrations due to traffic indirectly determined from the measured Fe and Ca
hotspots at kerbside sites. Consequently, PM10 and concentrations.
PM2.5 measurements performed in these three typical It should be noted that some data presented here
locations (regional background, urban background and correspond to the 1998–1999 measurements and that the
kerbside sites), including speciation, have been used as levels of PM for a given site may currently be lower.
basic information for a source apportionment analysis. However, downward trends showed a reverse in 2002
The basic data used are levels and relative contributions and 2003 at least in Germany, e.g. the 12 month PM10
to total mass presented here are given as long-term average until September 2003 in Berlin reached levels
means. The main advantage of this strategy is the similar to those recorded five years earlier. Preliminary
simplicity of the method and the consequent low impact data evaluation suggests that large-scale episodes with
of mathematical artefacts on the data treatment. elevated PM levels were more frequent because of
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6550 X. Querol et al. / Atmospheric Environment 38 (2004) 6547–6555

durable anticyclonic and dry weather conditions in urban background sites, the highest PM10 levels were
Central Europe, resulting in higher regional PM back- recorded in Spain and Germany, where annual PM10
ground concentrations. mean varied from 28 to 42 mg m 3. In the other urban
background case studies PM10 levels reached around
25 mg m 3, with the lowest values recorded in Sweden
3. Discussion of results and conclusions (17–23 mg m 3). A similar variation was found for
kerbside stations. The highest values were obtained in
3.1. PM levels Austria, Germany and Spain: 37–55 mg m 3 (with
particularly high values for 1998). In The Netherlands
Results on levels and source apportionment of PM10 and the United Kingdom PM10 at kerbside sites varied
and PM2.5 at regional and urban background and from 30 to 35 mg m 3, and from 26 to 51 mg m 3 in
kerbside sites obtained from the above EU case studies Sweden.
are summarised in Tables 1 and 2. As for PM2.5, average levels at regional background
Average PM10 levels at regional background sites sites ranged from 7 to 20 mg m 3 for all the case studies.
ranged from 14 to 24 mg m 3, with the exception of Maximum levels were measured in Austria (20 mg m 3)
Sweden where PM10 levels were lower (8–16 mg m 3). At and minimum values in Sweden (7 mg m 3). Similar

Table 1
Mean annual levels (mg m 3) of PM10, PM2.5, organic and elemental carbon (OC+EC), mineral elements, marine contribution and
secondary inorganic aerosols (SIA) recorded at regional background (RB), urban background (UB) and roadside stations (RS) in the
examples of the different countries in the EU studied
3
mg m

PM10 OC+EC Mineral Marine SIA PM2.5 OC+EC Mineral Marine SIA

Austria
RB 24 7 1 2 9 20 7 0.4 0.2 8
UB — — — — — — — — — —
RS 53 21 4 2 11 38 17 0.7 0.6 9
Germany
RB 19 5 3* 2 8 __ — — — —
UB 28–38 8 5* 2 13 22–30 7 3* 1 11
RS 37–51 13 14* 2 13 25–39 10 3* 1 11
Spain
RB 21 3 6 2 7 14 3 2 0.7 5
UB 31–42 7 10 2 7 19–25 6 3 0.7 8
RS 45–55 13 16 2 9 28–35 10 5 0.7 9

Sweden
RB 8–16 1–2 2–4 1–4 3–5 7–13 1–2 1–3 1–3 3–5
UB 17–23 2–3 7–9 1–4 3–5 8–15 2–3 2–4 1–3 3–5
RS 26–51 5–6 17–36 1–4 3–5 13–18 5–6 4–6 1–3 3–5
The Netherlands
RB 22 5 2 4 6 14 3 0.6 0.6 6
UB 25 5 3 4 10 20 5 0.6 0.6 9
RS 30 7 6 4 10 20 7 0.7 0.6 9
United Kingdom
RB — — — — — — — — — —
UB 25 9 5 2 8 16 8 2 0.3 6
RS 35 18 7 2 8 24 16 2 0.3 6

Switzerland
RB 14–24 4.5 2 0.2–0.5 7 18 4 1 0.2–0.5 8
UB 24 6 2 0.2–0.5 9 19 5 1 0.2–0.5 8
RS 42 13 6 0.2–0.5 10 22 8 1 0.2–0.5 7
*
Unaccounted mass: mineral matter+water+other unaccounted components.
Table 2
Mean annual levels (mg m 3) of PM10, PM2.5, organic and elemental carbon (OC+EC), mineral elements, marine contribution and secondary inorganic aerosols (SIA), and the
equivalent contributions to bulk mass concentrations (% wt), recorded at regional background (RB), urban background (UB) and kerbside stations (RS) in Central, Northern and
Southern EU based on the data reported from the examples from Austria, Berlin, Spain, Sweden, Switzerland, The Netherlands and United Kingdom

Central EU (examples from Australia, Berlin, Northern EU (13 sites in Sweden) Southern EU (10 sites in Spain)
Switzerland, The Netherlands, UK)

X. Querol et al. / Atmospheric Environment 38 (2004) 6547–6555

RB UB RS RB UB RS RB UB RS
3
mg m
PM10 14–24 24–38 30–53 8–16 17–23 26–51 14–21 31–42 45–55
OC+EC 4–7 6–9 13–21 1–2 2–3 5–6 2–5 4–9 10–18
Mineral matter 1–2 3–5 4–8 2–4 7–9 17–36 4–8 8–12 10–18

ARTICLE IN PRESS
Marine aerosols 2–4* 2–4* 2–4* 1–4 1–4 1–4 2–4# 2–4# 2–4#
SIA 7–9 7–13 8–13 3–5 3–5 3–5 5–9 6–11 6–11
PM2.5 12–20 16–30 22–39 7–13 8–15 13–19 12–16 19–25 28–35
OC+EC 3–7 5–8 8–16 1–2 2–3 5–6 2–4 4–8 8–12
Mineral matter 0.5–2 0.4–2 1–2 1–3 2–4 4–6 1–3 2–5 4–6
Marine aerosols 0.2–1 0.2–1 0.2–1 1–3 1–3 1–3 0.2–1 0.2–1 0.2–1
SIA 6–8 6–11 7–11 3–5 3–5 3–5 4–8 7–10 6–10
%
PM10
OC+EC 30–35 20–30 40–45 12–15 12–15 12–20 15–25 12–25 25–37
Mineral matter 5–10 10–15 12–15 20–30 35–45 65–70 12–40 25–30 25–37
Marine aerosols 5–20 5–12 5–8 12–30 5–15 4–6 5–20 5–10 3–8
SIA 35–55 30–35 25–28 30–40 15–25 10–15 35–45 20–27 13–25
PM2.5
OC+EC 30–40 25–35 35–45 15 20–35 30–40 17–30 20–35 30–40
Mineral matter 2–8 2–8 5 15–25 25–30 30–40 8–20 10–20 10–15
Marine aerosols 2–5 1–3 1–2 12–25 12–20 5–15 2–5 1–3 1–2
SIA 35–55 35–40 27–35 35–45 30–35 20–25 17–30 20–35 30–40
*
7 mg m 3 in coastal areas of The Netherlands.
#
11 mg m 3 in the Canary Islands.

6551
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6552 X. Querol et al. / Atmospheric Environment 38 (2004) 6547–6555

levels were obtained in Spain and The Netherlands trend detected for regional background concentrations
(14 mg m 3). At urban background sites, the highest in 2002 and 2003 in Germany with respect to the
PM2.5 levels were recorded in Spain and Germany, downwards tendency observed in the last decade (see II
where the annual PM2.5 mean varied from 20 to Position Paper on PM from the European Commission).
30 mg m 3. In other case studies, PM2.5 levels ranged However, the differences may also be attributed to the
from 15 to 20 mg m 3, with the exception of Sweden different sources and structure of the regional PM
(8–15 mg m 3). Finally, at kerbside sites, PM2.5 levels background data used for these studies. Given the
ranged from 25 to 39 mg m 3 in Spain, Austria, and higher consistency of the recent data set, the results of
Germany, from 20 to 24 mg m 3 in The Netherlands and John and Kuhlbusch (2004) probably offer a more
the UK, and from 13 to18 mg m 3 in Sweden. robust picture with regional PM background around
It should be pointed out that in the Netherlands there Berlin accounting for about half of the peak concentra-
is very little difference between the PM10 levels tions recorded in the city centre.
registered at urban background and kerbside stations The PM10 regional background contribution mea-
(29–37 mg m 3 and 31–37 mg m 3 in 2001, respectively). sured at urban background sites may be estimated at
However, in most of the case studies, the PM10 levels around 50–65% for most of the examples considered
recorded at kerbside sites are higher with respect to and at 50–93% in Sweden and The Netherlands. As for
urban background sites by 30–50%. The large contribu- PM2.5, this regional background contribution varies
tion of long-range transport determined for PM10 in from 60 (Spain) to 95 (Sweden) %.
The Netherlands (Visser et al., 2001) could account for The ratio PM2.5/PM10 could vary widely between
these low differences in PM10 levels at urban and different EU regions depending on the type of site. Thus,
kerbside sites. However, it should be noted that the at regional background sites PM2.5/PM10 ranges from
criteria used in The Netherlands for the definition of 0.6 to 0.8. At urban background sites, the PM2.5/PM10
kerbside stations could differ from those employed in ratio ranges from 0.4–0.5 (in the Canary Islands and
other member states, i.e. in Amsterdam a monitoring Southern Spain) to 0.8 in The Netherlands, Germany
station facing an open canal adjacent to the quiet and Northern and Central areas in Spain. Finally, the
premises of the State Bank is defined as a street-canyon. PM2.5/PM10 ratios at kerbside sites are usually 0.6–0.7.
The level and composition of the Dutch kerbside station Lower ratios (0.4) were obtained at some kerbside
falls within the usual range defined for urban back- sites in Sweden and in the Canary Islands, indicating
ground stations in other examples reported in this study. the strength of road dust emissions (road and tyre
Bearing in mind the range of PM10 levels for the abrasion, sanding, salting) and the African dust inputs,
different types of stations, it can be concluded that the respectively.
regional, city background, and local traffic contributions
to the total kerbside PM10 are estimated to be 35–50%, 3.2. PM speciation and source apportionment
10–35% and 30–45%, respectively. However in The
Netherlands and Sweden these contributions are Based on the above results, the following quantitative
50–75%, 15–35% and 1–20% and 30–65%, 5–30%, estimations on source apportionment may be obtained:
and 35–55%, respectively. Similar conclusions can also
be drawn for PM2.5 levels given that the above  The marine contribution to PM10 attains 2–4 mg m 3

contributions are estimated to be 35–50, 20–35 and for most of the examples considered, but it may
30–40% for most of the examples and 60–70%, 5–25% account for up to 7 mg m 3 in coastal areas in The
and 15–25% and 40–65%, 5–30%, 20–35% for The Netherlands and for up to 11 mg m 3 as an annual
Netherlands and Sweden. At least in Berlin, the spatial mean for the Canary Islands. This contribution to
distribution of PM2.5 compared with PM10 seems to be PM2.5 falls (0.2–0.8 mg m 3), reaching 2 mg m 3 in
more homogeneous with relatively less PM2.5 input Southern Sweden.
from local traffic. This may reflect a smaller share of  Mean regional mineral contribution to PM10 (mainly
local non-exhaust traffic PM emissions, which consists of a natural origin) ranges from 5.5 mg m 3 in the
mainly of coarse particles, in PM2.5. Eastern and Southern Iberian Peninsula to around
A recent study based on a 12 month monitoring 2 mg m 3 for the remaining areas, with the exception
campaign starting in October 2001 in Berlin and the of the Canary Islands (8 mg m 3).
surrounding rural areas (John and Kuhlbusch, 2004)  Therefore, it can be deduced that, as a mean, the
shows a larger share of regional background PM (about natural input to PM10 in Europe varies from
50% with only 25% contribution of urban background E8 mg m 3 in Spain to E4 mg m 3 in most Northern
and local traffic) at kerbside sites in Berlin city centre and Central Europe. These values represent the
when compared with results for 1998 (37%) obtained by minimum natural contribution is not taken into
Lenschow et al., 2001. These different regional con- account here. In PM2.5 the marine and natural
tributions could be partially related to an increasing mineral regional contributions decrease significantly
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X. Querol et al. / Atmospheric Environment 38 (2004) 6547–6555 6553

with respect to PM10, but these are still present in similar pattern is observed for PM2.5, where
around 3 mg m 3 in Spain and around o1.5 mg m 3 in OC+EC contributions are reduced by 10–20% with
Central Europe. Sporadically, African dust outbreaks respect to PM10.
over Southern EU may induce very high PM10 and  Based on the OC+EC data presented, it may be
PM2.5 levels. Daily PM2.5 levels of up to 70 mg m 3 stated that the OC+EC regional contribution to
with 480% mineral dust have been measured for PM10 ranges from 1 (Sweden) to 5 (Berlin) mg m 3
some of those events over Spain. for most of the examples considered. The urban
 At urban sites, the mineral contribution ranges from background OC+EC contribution, mainly related to
3 to 5 mg m 3 in Central Europe, and accounts for traffic emissions, varies from 1 (Sweden) to 8 (Berlin)
7–9 mg m 3 in Sweden and for 10 mg m 3 in Spain. At mg m 3. The local contribution of OC+EC at kerb-
kerbside sites the mineral contribution accounts for side sites, related to traffic exhaust emissions, tyre and
4–7 mg m 3 in Central Europe, 16 mg m 3 in Spain and pavement abrasion, ranged from 3 (Sweden) to 9
17–36 mg m 3 in Sweden. The relatively high values (UK) mg m 3. Given that OC+EC are mainly
recorded in Berlin (14 mg m 3) are attributed to the accumulated in the PM2.5 fraction, their contribu-
fact that mineral contribution, water and other tions to PM2.5 follow a pattern similar to that
unaccounted compounds are considered together. A described for PM10.
clear differentiation was also evident for the mineral  The contribution of secondary inorganic aerosols
contribution to PM2.5 at urban background stations, (SIA, from traffic, industrial emissions including
varying from 0.4 to 0.7 mg m 3 for most EU examples, power generation, and agriculture) ranged from 3 to
2 mg m 3 for the UK, 2–4 mg m 3 for Sweden, and 9 mg m 3 for PM10 and from 3 to 8 mg m 3 for PM2.5
2–5 mg m 3 in Spain. at regional sites. The concentrations are somewhat
 Consequently at urban background sites, the mineral lower, 3–5 mg m 3, in Sweden. SIA levels are very
city background contribution attributed to demoli- similar in urban areas, but in intensively industria-
tion, construction and road dust accounts for lised regions or heavily polluted urban areas, there is
5 mg m 3 in Spain and Sweden, and for 2–4 mg m 3 an input of secondary inorganic aerosols from 2 to
in PM10 in the remaining case studies. In PM2.5 this 5.5 mg m 3 for PM10 and from 1 to 5 mg m 3 for
contribution is still slightly higher in Spain and PM2.5 on top of the above contributions.
Sweden (1 mg m 3) than in the other areas
(0.4–0.6 mg m 3). The local mineral contribution at The studies on source apportionment analysis carried
road sites, which corresponds to the road dust out at kerbside sites demonstrate that the major
emissions from the street where the monitoring contribution sources are traffic (including exhaust and
station is located, accounts for 9–24 mg m 3 in abrasion products), which accounts for 35–55% of
Sweden, 6 mg m 3 in Spain and for 1–5 mg m 3 for PM10 and 40–60% of PM2.5, and industry, while
the rest of the examples considered. As for PM2.5, accounting for 15–25% of PM10 and around 20% of
this contribution ranges from a mean of 2–3 mg m 3 in PM2.5. In line with Lenschow et al. (2001), John and
Spain and Sweden to o0.5 mg m 3 in the remaining Kuhlbusch (2004) confirm that the transport sector
examples. These differences in levels of crustal contributes to 53% of PM10 at traffic hotspots in the
components may be attributed largely to the higher centre of Berlin. This city is an example of a large
soil-resuspension effect during dry conditions in the agglomeration without heavy industry in continental
southern EU countries, whereas higher rainfall in the Europe. The bulk of the 25% contribution from
northern countries may help to clean the road dust industry and power plants is regarded as secondary
from streets. However, sites in Sweden show quite PM10 originating from sources outside the agglomera-
high road dust emissions as a result of the use of tion. Given the extensive use of the best available
studded tyres, sanding and salting of roads during the technology to curb primary PM emissions from com-
winter and spring period. bustion in Berlin, road transport accounts for 80% of
 The contribution of organic and elemental carbon PM10 kerbside concentrations in Berlin, if the regional
(OC+EC) to PM10, mostly arising from traffic, background PM10 is ignored. Thus, any strategy
woodsmoke and cooking, and specific industrial designed to reduce PM10 pollution must focus on the
emissions, at regional background sites ranges from traffic sector. However, in the light of the findings of
1 mg m 3 in Sweden to 7 mg m 3 in Austria. At urban earlier studies by Düring et al. (2002), half of this traffic
background sites this contribution increases for all contribution can be attributed to non-exhaust emissions
countries, with the exception of The Netherlands, such as re-suspension and abrasion, which cannot be
ranging from 2 to 9 mg m 3. At kerbside sites, the addressed by focusing exclusively on vehicle emissions
OC+EC contribution usually ranges from 13 to control technology. The same conclusions are obtained
21 mg m 3, with the exception of Sweden and The for PM10 in Spain, where similar OC+EC and road
Netherlands where it is estimated to be 5–7 mg m 3. A dust contributions from local traffic are measured at
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6554 X. Querol et al. / Atmospheric Environment 38 (2004) 6547–6555

kerbside sites. However, the PM10 kerbside traffic 2004. Concentrations and sources of PM10 and PM2.5 in
contributions of OC+EC in the UK and Switzerland Sweden. Atmospheric Environment, in press.
are 2 to 4 times higher than that of road dust. As Artiñano, B., Salvador, P., Alonso, D.G., Querol, X., Alastuey,
discussed above, these differences are even higher for A., 2003. Characterisation of PM10 and PM2.5 in Madrid
PM2.5, the highest road dust contributions being those (Spain): an analysis of main sources and high concentration
episodes. Environmental Pollution 125, 453–465.
from Spain and Sweden.
Düring, I., Jacob, J., Lohmeyer, A., Lutz, M., Reichenbãcher,
The fraction of PM attributable to transboundary
W., 2002. Estimation of the ‘‘non-exhaust pipe’’ PM10
anthropogenic pollution was estimated at 8–16 mg m 3 emissions of roads for practical traffic air pollution
PM10 and 7–13 mg m 3 PM2.5 (depending on the region modelling, Proceedings of the 11th International Sympo-
of Sweden) and at 11 mg m 3 of PM10 for The Nether- sium Transport and Air Pollution, June 2002, Graz,
lands (Areskoug et al., 2004; Visser et al., 2001). Austria, 19.21.
Quantitative data from chemical speciation of PM in Harrison, R.M., Smith, D.J.T., Pio, C.A., Castro, L.M., 1997a.
Spain showed that, on average, the natural input reaches Comparative receptor modelling study of airborne particu-
17, 24 and 38% of PM10, and 11, 16 and 26% of PM2.5 late pollutants in Birminghan (United Kingdom), Coimbra
at kerbside, urban background and regional background (Portugal) and Lahore (Pakistan). Atmospheric Environ-
sites, respectively. In some places such as the Canary ment 31, 3309–3321.
Harrison, R.M., Deacon, A.R., Jones, M.R., Appleby, R.S.,
Islands these contributions may even reach higher
1997b. Sources and processes affecting concentrations of
proportions (40–65%). Peak values of PM10 and
PM10 and PM2.5 particulate matter in Birminghan (UK).
PM2.5 daily levels, of up to 300 and 70 mg m 3, Atmospheric Environment 31, 4103–4117.
respectively, attributable to African dust outbreaks have Harrison, R.M., Jones, A.M., Lawrence, R.G., 2003. A
been reported at a number of air quality monitoring pragmatic mass closure model for airborne particulate
stations in the South of Europe. Moreover, very high matter at urban background and roadside sites. Atmo-
contributions of marine aerosols to PM10 may be spheric Environment 37, 4927–4933.
obtained in coastal areas of Northern Europe (annual Harrison, R.M., Jones, A.M., Lawrence, R.G., 2004. Major
contributions of up to 7 mg m 3 have been reported for component composition of PM10 and PM.5 from roadside
The Netherlands). and urban background sites. Atmospheric Environment 38,
4531–4538.
John, A., Kuhlbusch, T., 2004. Ursachenanalyse von Fein-
staub(PM10)-lmmissionen in Berlin auf der Basis von
Acknowledgements Messungen der Staubinhaltsstoffe am Stadtrand, in der
innenstadt und in einer StraXenschlucht (Cause analysis of
The authors would like to thank the Environmental PM10-pollution in Berlin based on measurements of PM
Agencies, Departments and Ministries of Austria, components at the periphery, in the city centre and in a
street canyon). Final report on behalf of the Senate
Germany, The Netherlands, Spain, Sweden, Switzer-
Department for Urban Development, Berlin, Germany,
land, and United Kingdom, for supporting and promot-
Senatsverwaltung für stadtentwicklung, Berlin, IX D and
ing the studies by supplying the data for this study. We VIII A2.
would also like to thank the PM working group from the Kim, E., Hopke, P.K., Paatero, P., Edgerton, E.S., 2003.
Clean Air for Europe Programme from D.G. Environ- Incorporation of parametric factors into multilinear recep-
ment (European Commission) for allowing us to publish tor model studies of Atlanta aerosol. Atmospheric Environ-
this study. We would also like to express our gratitude to ment 37 (36), 5009–5021.
2 anonymous referees for their valuable comments and Lenschow, P., Abraham, H.J., Kutzner, K., Lutz, M., PreuX,
suggestions. J.D., Reichenbächer, W., 2001. Some ideas about the
sources of PM10. Atmospheric Environment 35 (Suppl. 1),
123–133.
Liu, W., Hopke, P.K., Han, Y., Yi, S.-M., Holsen, T.M.,
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