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ATMOSPHERIC

ENVIRONMENT
PERGAMON

Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33


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Some ideas about the sources of PM10


P. Lenschow, H.-J. Abraham, K. Kutzner, M. Lutz*,
J.-D. PreuB, W. Reichenbficher
Department of Urban Development, Berlin, Germany
Received 3 May 2000; received in revised form 18 January 2001; accepted 24 January 2001

Abstract
In Berlin, about 50% of the urban background PM10 concentration is due to long range transport--mainly
secondary aerosols (ammonium nitrate and ammonium sulphate) and natural sources. At kerbside sites on main streets
the PM10-concentration is up to 40% higher than the urban background. Half of this additional pollution is due to
motor vehicle exhaust emission and tyre abrasion and the other half is due to resuspended soil particles. On the basis of
comparison of the main chemical components at stations in the regional and urban background and a station at the
kerbside of a busy street, we estimate the source apportionment for the main source groups. Possible reduction
measures are discussed. 2001 Elsevier Science Ltd. All rights reserved.
Keywords. Source apportionment; Chemical composition; Secondary aerosols; Resuspension by traffic; Measures of reduction

1. Introduction
Concentrations of airborne particles have been measured in Berlin over almost 30 years. Exposure to huge
emissions of sulphur dioxide and particulate matter in
the 1970s and 1980s, especially in the then East Berlin
and in the surrounding industrial agglomerations of
East Germany, created a strong need to measure these
and other pollutants at up to 43 measuring sites
(SenStadt, 1998). Recorded series of air pollution data
showed strikingly high levels of total suspended
particulates (TSP) and sulphur dioxide concentration
until the early 1990s, which led to smog alarms and
traffic bans in the western part of the then divided city of
Berlin. So, public pressure on the need for abatement of
air pollution became strong and so was the necessity for
identifying the sources of air pollution where control
measures would have to be taken. Hence, surveys on the
emission from all sectors led to a rather detailed

*Corresponding author. Present address: Senatsverwaltung


fuer Stadtentwicklung-IX D-, Brueckenstrasse 6, D-10173
Berlin, Germany.
E-mail address: martin.lutz@senstadt.verwalt-berlin.de
(M. Lutz).

emission register of Berlin for all major pollutants which


has been updated regularly (SenStadt, 1998).
The reunification of the city in 1989 led to a total
reconstruction of the heating systems in the east, to an
abandonment of high-sulphur lignite as a fuel in this
part of the city as it had already been since 1981 in the
western part, a total restructuring of the industrial and
electricity sector in east Germany and so to an accelerated reduction of emissions of particulate matter and
sulphur dioxide from these sources. The situation thus
looks a lot better than illustrated in OECD (1999), one
of the rare comparisons of air pollution between a larger
number of cities in the world. Since 1993 the levels of
suspended particulates have again fallen by about one
third and the concentration of sulphur dioxide has
dropped far below the limit values of EC-Directive
99/30/EC (EC, 1999). However, as shown in this paper,
it is still necessary to assess sources of air pollution-especially as regards the levels of fine particles smaller
than 10pro (PM10). Among other things, the above
mentioned Directive sets tough limits for PM10 for 2005
and a further preliminary set of even tougher limit
values for 2010. As these new limit values were based on
recent findings on health effects from exposure to fine
particles they are by far more stringent than those in the
previous legislation. Together with the Air Quality

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o f 100 km 2. The city is situated in the N o r t h e r n G e r m a n


Lowlands less than 100km west o f G e r m a n y ' s border
with Poland and a r o u n d 200 km northwest o f the more
industrialised so-called "Black Triangle" o f the borders
o f G e r m a n y , Poland and the Czech Republic. It has a
m o d e r a t e climate with 50% winds from Southwest to
N o r t h w e s t (mainly maritime influence) and 30% winds
f r o m Southeast to N o r t h e a s t (mainly continental influence), average wind speed o f 3 m s 1 ( 1 0 m above r o o f
tops in the built up area) and yearly mean temperature
o f 8.8C ( - 0 . 5 C in January, 17.9C in July).
The n u m b e r o f passenger cars and light duty vehicles
(LDV) totalled 1.1 million at the end o f 1999 which
means 323 cars per 1000 inhabitants (73% with threeway catalytic converter, 15% diesel) and the n u m b e r o f
heavy duty vehicles (HDV) is 100000. This is still a
rather low vehicle density in c o m p a r i s o n with other
cities o f similar size.
There are 13 bigger c o m b i n e d power and heating
plants with a capacity o f 2800 M W electrical power run
with coal, oil and natural gas. They all meet the G e r m a n
emission limits. The coal and oil p o w e r plant are
equipped with flue gas desulphurisation, denitrification
and filters. One domestic waste incineration plant exists
with a capacity o f 376000 tonnes waste per a n n u m
equipped with flue gas filters o f a very high technical
standard. There is nearly no heavy industry. Fuel used
for domestic heating consists o f 30% natural gas, 20%

F r a m e w o r k Directive 96/62/EC (EC, 1996) authorities


in n o n - a t t a i n m e n t z o n e s are required to assess PM10
pollution, including investigation into the origins o f air
pollution, its major sources, and pollution which might
be i m p o r t e d from other regions.
F o r Berlin, the following questions arise:
Will the PM10-1imits be met in 2005 without
additional action or are the current reduction regulations sufficient? If not:

W h a t are the major sources (industry, transport,


domestic, agriculture etc.)?
H o w do sources inside the agglomeration which are
directly accessible to the local authorities contribute
to the PM10 pollution?
W h a t sort o f additional action should be taken at
regional, national, EC or U N - E C E levels?

This paper aims to get first answers for those questions and to identify further areas o f investigation so as
to gain a more reliable basis for a b a t e m e n t plans and
programmes.

2. Some basic information about Berlin and its


monitoring network
With a surface area o f 8 9 0 k m 2 and 3.4 million
inhabitants Berlin is G e r m a n y ' s largest single c o n u r b a tion. 1.12 million people live in the inner city in an area

Table 1
Annual emissions of various source sectors in Germany and Berlin (1998)a'b
Particles PM10

Plants subjected
to licensing
Domestic
heating
Households
Small
industries
Traffic (motorvehiclesonly)
Resuspension
by traffic
Traffic (other)
Use of soIvents
Agriculture
(cattle)
Agriculture
(fertilize0
Other sources
(construction,etc)
Sum of all sources

Sulphur dioxide

Oxides of nitrogen

Volatile organiccompounds

Ammonia

Gerlnany

Berlin

Germany

Berlin

Germany

Berlin

Germany

Berlin

Germany

kt

kt

kt

kt

kt

kt

kt

kt

kt

95

38.8

1.9 20.3 1119

86.6

7.9

71.3 564

31.7

7.5

24.8

140

8.2

2.2

3.8

1.3

29

11.8

0.5 5.3

102

7.9

2.5

22.6 103

5.8

3.0

9.9

1.0

1.7

2.0

0.1

37

2.9

0.0

0.4

38

2.1

1.0

3.3

3.3
0.3

10.0
10.0

17.2
17.2

43

17.6

2,4 25.6 30

2.3

0.5

4.5

856

48.1

17.0 56.3 409

24.0

28.0

48.3

43

17.6

2,4 25.6

20

8.2

0,2 2.6

0.4

0.1

1.3

220

12.4

1.7

3.1
58.7

2.8

4.8
525

84.0

70

l 1.2

22

3.5

11
245

4.5

1.5

0.0

1.8 19.2
9.4

1292

11.1

0.0

0.0
1780

30.2

5.6

0.0

56
5

53
I000

42
1705

2.5

4.0
58.0

6.9

625

~Remarks: (1) All emissions extrapolated from data of 1995, (2) natural emissions not included, (3) use of solvents in Berlin is
included in households and light industry.
bData sources: Berlin: Senatsverwaltung fuer Stadtentwicklung, Germany: according to Umweltbundesamt Berlin and minutes of
expert hearing III 2.2 H 50231-18/11 and Ehrlich et al. (2000).

P. Lenschow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

light oil (sulphur content less than 0.2%) and 15%


lignite (sulphur content less than 1%). 30% are supplied
by district heating and 5% by electricity. The annual
mean emissions are shown in Table 1 together with
German total emission data.
In 1999 the Berlin air pollution monitoring network
(Berliner Luftguete Messnetz, BLUME) consisted of 21
stations. Particulate matter is currently measured at 18
stations (see Fig. 1). A majority of 12 automatic instruments (radiometric monitors Eberline FH62IN) still
measure TSP as was required by the recently repealed
Directive 80/779/EEC (EC, 1980).
The automatic network has been fitted to gravimetric
TSP-measurement in 1988 with a constant factor (1.34)
after gravimetric reference measurements at nine collocated background stations with about 100 daily samples
each and correlation coefficients of 0 . 9 4 < r < 0 . 9 8
(TUEV, 1989). Gravimetric reference measurements of
PM10 were performed during a measuring campaign in
1996 at three urban background stations and three
stations near streets with 72-100 daily samples (Air
Consult, 1997). The gravimetric reference measurements
are made using low volume samplers (Kleinfilterger/it
GS050) and high volume samplers (Digitel DHA80).
After the elimination of 8% of data with PM 10/TSP less
than 0.5 or more than 1.2 comparison of PM10 and TSP
series resulted in conversion factors of 0.76-0.79 at the
investigated urban background sites and slightly higher
values of 0.82-0.85 at the three traffic sites with
correlation coefficients of 0.953 < r < 0.967. Taking into
account the uncertainties of the measurement techniques, the low correlation and the microlocation of
measuring instruments an overall factor of 0.8 is
considered as an appropriate approximation when
estimating PM10 concentrations on the basis of TSP
measurements with the Berlin BLUME network. The
same factor has been used by federal institutions in
Germany to gain an overview of the PM10 pollution.
There have been two campaigns to measure and
chemically analyse PM10 and PM2.5. The first was from
November 1989 to October 1990 at an urban background station (and three other stations) in Berlin and
the rural EMEP station Waldhof, about 180 km west of
the town (Israel et al., 1992). The second was in 1998 at
one urban background and one traffic station in Berlin
(Abraham, 1999). These measurements have been made
with teflon filters on Dichotomous Samplers (PM10 and
PM2.5) and quartz filters on Digital DHA80 (TSP) in
1989/1990 and with quartz filters on Kleinfiltergeraet
GS050 (PM10 and PM2.5) in 1998. Before and after
exposure the filters are stored for more than 24h at
40 50% relative humidity and temperatures of
20 _+ 2C. The methods used for chemical analysis were
ion chromatography after extraction with ethanol or
acetone and water for the ions and three step thermography (350C and 620C with helium, 700C with

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monitoring stations
E~] urban background
traffic

(a)
" "

1999 a n n ~ M l O
(PMIO~

concentrations
~'/,,,
PMIO=O,8xTSP) ~ r
o 2
"

(b) 1999 90.14-percentiio (equivalent to 36. highest


daUy mean of PM10 concentration) . . . . . . . . . . .

"

~
|f

(PM10 measurementin bold/italics, otherval~JesPMlO=O,SxTSP) ~

(c)

6 km

~" T
2 4 o km

Windroses of suspended particulates

Fig. I. Spatial distribution of suspended particulates in Berlin


(1999).
helium plus 20% oxygen) for elemental carbon (EC) and
organic carbon (OC). The organic material (OM) is
derived by multiplying OC with a factor 1.2 (Israel et al.,
1992; VDI, 1999). In this paper all ions are displayed
without their charges.
Since no chemical analyses were available in the
regional background in 1998 these values are estimated
from 1996 data (Umweltbundesamt, 1997) and lowest

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P. Lenschow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

concentrations of carbonaceous material measured at


other stations in the region.
There are differences between the results of the
continuous automatic measurements and the results of
the measuring campaigns that are mainly due to small
sample size of the campaigns. Therefore, we avoid cross
comparisons that could be affected by these differences.

sources like traffic, tram and sandy pavements have high


influence at these points.
The 90th percentiles (Fig. lb) show nearly the same
spatial distribution as the annual means with lowest
values at the borderline and highest values in the inner
city near streets.
As Fig. lc shows, the PM concentration is higher
when the wind blows from the east (continental
influence) than from the west (maritime influence). In
the inner city, the background concentration for the east
wind sectors (80-170 ) is higher than the west sectors
(250-340 ) by a factor of 1.5-2.0 depending on the year.
The measurements show that in 1999 the PM10 limit
value of 4 0 g g m -3 as annual average was exceeded at
one traffic site (Fig. la). The second PM10 limit value of
50 gg m -3 as 24 h mean not to be exceeded more than 35
times per year is equivalent to a limit for the 90th
percentile of 50 ggm -3. As shown in Fig. lb, this limit
value is exceeded more frequently throughout the city by
up to 35% at stations with high influence of traffic.
The situation looks even worse with regard to the
indicative limit values for 2010 laid down in ECDirective 99/30/EC (EC, 1999) of 20ggm -3 as annual
mean, with not more than seven peaks above 50 ggm 3.
This short term limit is equivalent to a limit of the 98th
percentile of 501agm 3. In 1999 the measured 98th
percentiles go up to 100 lagm -3.
It should be noted that in 1998 and 1999 westerly
winds were more frequent than normal (and easterly

3. Present situation of P M I O

Fig. 1 shows the annual mean concentrations and


relevant percentiles of PM10 as well as windroses of
suspended particulate matter (SPM) at 18 automatic
stations in Berlin. Six of them (one suburban, two urban
background and three kerbside stations) measure PM 10.
To give full information about the distribution in the
city, the concentrations of the 12 TSP-stations are scaled
down to PM10 by the above-mentioned factor of 0.8.
As seen in Fig. la, in 1999 the annual mean values
of PM10 in Berlin lay between 18 and 2 5 g g m -3 near
the border line, 27-33ggm -3 in the inner city and
39-41ggm 3 at the two kerbside stations near main
roads ( > 50 000 vehicles per day) in street canyons and
37ggm -3 near the inner city highway ring (180000
vehicles per day). Two stations in the eastern part of the
town with 38 and 39ggm -3 do not fit into the
concentration field of the background stations. Local

160

160
F

140

120 1-

.-..

I|

100
E
60

* TSP

/
.

' .

' . . . .

. . . .

,.

,.

--4--S02

140

120

. . . .

lOO

ti

bl

t ' -

,...

80

8
I.-

60

60 " i ' "


40 . . . . .

40

20

20

ol

1988

t989

1990

1991

1992

1993

1994

1998

1996

1997

Fig. 2. Monthly averages of TSP and S02 in the urban background.

1998

II 0
1999

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P. Lenschow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

winds less frequent). With the usual distribution of


winds the concentrations would have been higher than
recorded.
In order to meet the short-term limit values for
2005 also in hot spots with intense traffic the PM10pollution must drop by at least 27% by 2005. In order
to develop an efficient abatement strategy more information is needed about the future trend and the sources
of PM10.

4. Long-term changes in the characteristics


of suspended particulate matter

Time series of monthly mean values of TSP and SO2


at three urban background stations in the inner city of
Berlin show a distinct downward trend (Fig. 2). In
summer there was always much more TSP than SO2.
However, in winter in the period before 1991 peak levels
of both substances were quite similar, while since 1991
much less SO2 than TSP has been found all over the
year. A special feature of TSP is that the downward
trend seems to remain on a high level with winter peaks
sometimes nearly vanishing, whereas SO2 still shows
clear winter peaks.
The annual averages and the 98th percentiles of TSP
concentrations measured in the urban background are

90

',

.......
7o

.......

This behaviour may be due to better particle filters in


plants, less emission of smoke from domestic heating
(the use of lignite in domestic heating has been reduced
b y a b o u t 90% since 1990), and much better car engines.
The lower reduction of EC can be attributed to the
relative growth of influence of traffic, the influence of

?,:

.........
.;.

a strong reduction by about 50% of unresolved


particles (mainly soil particles) and of OM,
a medium reduction of about 20% of SO4 and EC, and
a much smaller reduction of NO3 and NH4.

80

subject to nearly the same trend (Fig. 3). This is


understandable if the main sources are subject to the
same trends, or if the main sources react similar to the
changes of climate influences. From this we infer that
relative changes of annual averages may be taken in the
first approximation as representative for the changes of
higher percentiles.
Table 2 depicts the decrease of TSP, PM10 and PM2.5
between 1990 and 1998 on the basis of annual mean
concentrations measured at the urban background
stations Fasanenstrasse in 1990 and Nansenstrasse in
1998. The last column of the table shows that the
decrease of PM2.5 is less pronounced than of PM 10 and
even less than TSP.
As shown in Fig. 4, the development of the Berlin
urban background since 1990 shows

..: ........

il
\i

.11
,

........................

"%,.

......

'

,,. . . . . . . . . . . . . . . .

........
.,, . . . . . . . .

',

240

,,

. A."a'averoo'TSP

"

:l,'. . . . . . . .

~ ........

,, . . . . . . . .

,,. . . . .

160

A 60

4o

200

iii

ii

120 1
o
D.

=3
e-

<

30 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

80

20

40
10
,,
,,

1988

1989

t990

1991

1992

1993

1994

1995

1996

1997

1998

Fig. 3. Annual averages and 98-percentilesof daily mean concentration in the urban background.

1999

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P. Lenschow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

One can clearly recognise from Fig. 4 and Table 3 that


in the busy street the PM10-pollution is up to 40%
higher than in the surrounding urban background. Near
the street there is a higher share of EC, OM and soil.
It should be mentioned here that the method used to
measure carbonaceous material does not perfectly
separate EC from OM. Tests with extraction of OM
with a mixture of 1 part of toluene and 3 parts of N , N dimethylformamide before thermographic analysis have
revealed that about 30M0% of PM10 EC and 50-60%
of PM2.5 EC may really be OM. Near streets where high
concentrations of EC and OM are measured, the
differences are not as distinct as in the background.
For the source apportionment we could not take this
finding into account.

tyre abrasion and the less restrictive emission limits for


HDV in comparison with passenger cars. The lower
reduction of SO4, NO3 and NH4 may be due to former
limitations in the small scale conversion of SO2 and N O ,
in the atmosphere and perhaps emissions of NH3 from
the growing number of cars with catalytic converters
(Kirchner et al., 2000).

5. Main chemical composition of PMI0


The main chemical components of PMI0 in 1990 and
1998 are shown in Table 3 and Fig. 4.
About one third of the mass of PM10 in the urban
background is attributable to inorganic secondary
aerosols originating from Europe-wide gaseous emissions. Another third is carbonaceous material, mainly
emitted by motor vehicles and by lignite and coal
combustion in stoves, but also secondary aerosol of
organic matter from anthropogenic and natural sources.
The remaining third consists of soil and ash particles,
sea spray and water.

6. Source apportionment
For the first approximation of the source apportionment presented in this paper, assumptions are made in
three steps.
The field structure of PM10-concentrations in the
Berlin region (Fig. 1) suggests that concentrations
measured at only one carefully sited station per type
can be taken as representative for other stations of the
three types "traffic", "urban background" and "regional
background" as shown schematically in Fig. 5. So in the
first step it is assumed that

Table 2
Average concentrations of TSP, PM10 and PM2.5 in the urban
background Fasanenstrasse in 1990 (Israel et al., 1992),
Nansenstrasse in 1998 (Abraham, 1999)

TSP
PM10
PM2.5

1990
ggm -3

1998
pgm 3

Reduction
%

77
58
39

43
38
30

44
34
23

Urban background
Nansenstr

the kerbside station Frankfurter Allee at a busy main


street with a traffic flow of about 60 000 vehicles per
day with a HDV-share of 3.4% and a LDV-share of
7.1% is representative of the influence of traffic on air
pollution near streets,

Traffic site Frankfurter Allee


I

Difference
traffic - urban background
I

] 998

Vl
II

III V ~ 6 7

3.3

11,0

,7

5].5

I
Fasanen

1991
l

Ill

DNO3

II Eso4
III E]NH4
IV Florganie matter(OM)
V Belemental carbon (EC)
Vt D soil+water

Fig. 4. Chemical composition of PM10 in the city of Berlin (ggm 3).

\IV

14,3

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P. Lenschow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

Table 3
Average concentation of PM10 and PM2.5 and main chemical components in the city of Berlin and the regional background ~
Type

UB
Berlinb
Fasanenstr.

RB
Waldhofb

TR
Berlin
Frankfurter All.

UB
Berlinc
Nansenstr.

RB
Neuglobsowd

PM10 (i.tgm-3)
OM (gg m -3)
EC (~tgm 3)
SO4 (ggm -3)
N O 3 (ggm 3)
NH4(lag m -3)
C1 (ggm -3)
Unresolved (ggm 3)
PM2.5 (ggm 3)
OM (I,tgm -3)
EC (ggm 3)
S O 4 (,t.tgm-3)
NO3 (I.tgm 3)
NH4 (ggm -3)
C1 (ggm 3)
Unresolved (gg m -3)
Start (MM.JJ)
End (MM.JJ)
No. of cases
Sample (h)

57.6
15.0
6.3
9.3
4.3
3.7
0.7
19.0
39.2
10.1
5.3
7.8
3.3
3.9
0.4
8.8
10,89
10,90
254
12

26.9
5.8
2.1
4.9
3.0
2.4
0.7
8.7
18.6
4.0
1.7
4.2
2.2
2.2
0.2
4.3
10.89
10.90
313
12

51.5
11.0
9.0
5.7
4.6
3.3
0.8
17.9
38.6
9.4
7.7
5.6
4.3
3.8
0.7
7.8
02.98
12.98
33
24

37.7
7.5
5.1
6.1
4.4
3.4
0.7
11.2
30.2
7.0
4.7
5.5
3,7
3.7
0.5
5.6
02.98
12.98
33
24

18.6
3.0
1.8
3.9
2.4
2.0
5.5

01.98
12.98
24

aUB: urban background, RB: regional background, TR: Traffic, Unresolved: mainly metal oxides (soil) and water (Israel et al.,
1992).
bIsrael et al (1992).
~Abraham (1999).
a Guessed after Umweltbundesamt (1997).

In the second step, it is assumed that

1, near traffic station (Frankforter Allee)


2. urban backgroond stations
(N ansenstrasse; Fasanenstrage)
3. regional background stations
(Waldhof; Neuglobsow)

PM [pg/rn3]
601

Tra.,c

regional

background

Fig. 5. Schematic horizontal profile of the ambient PM10


concentration.

the urban background station Nansenstrasse in the


inner city is taken as representative of the urban
background level, and
the rural stations Waldhof, 180 km from Berlin and
Neuglobsow, 100 km from Berlin are representatives
for regional background levels in 1990 and 1998,
respectively, only marginally influenced by the city.

the differences of particulate matter and its chemical


components between the traffic station and the urban
background station can be attributed to the local
influence of traffic on the adjacent street,
the differences between the urban background station
and the rural background station can be attributed to
the sources of the agglomeration and
the concentrations of particulate matter at the rural
background station can be attributed to global
sources with little contribution from the agglomeration.

We assume that there is a natural background of


5 . g g g m -3 due to primary and secondary emission of
wind blown dust, pollen, volcanic eruptions, thunderstorms, oceans and other sources and apportion this as
shown in Table 4a. In the third step, it is assumed that

the relative influence of the German source groups


can be taken as representative for all sources outside
the agglomeration,
the emissions of SO2, NOx and NH3 shown in Table
1 are the sources for the concentrations of SO3, NO3
and NH4 in Table 3, respectively, and

P. Lensehow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

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P. Lenschow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

the major source groups contribute to ambient


concentrations of primary and secondary particles
in proportions as their emissions displayed in Table 1
with the following modifications.
In Table 1 besides the gaseous emissions there is only
one category "particles PM10", that has to be combined
with EC, OM and the unresolved portion of the
measurements. For the partitioning of traffic, we used
emission data from the "Handbook for emission factors
of motor vehicles" (Keller et al., 1999), according to
which 60% of the diesel emissions of passenger cars and
LDV and 40% of the emissions of HDV consist of EC.
The other part is counted as primary OM. Taking into
account that 14% of all vehicles are diesel-engine cars,
and 3.5% LDV and 3.4-5% HDV with diesel motors,
this gives an average EC-partition of about 50%. The
particle emissions of petrol cars are neglected in the
handbook. We, therefore, included a small proportion
of the volatile organic compounds as secondary material
to the primary organic particulates.
The difference between the traffic station and the
urban background station consists solely of carbonaceous material (55%) and unresolved rests (45%). We
assume that the carbonaceous material stems from the
exhaust emissions of vehicles with 20% tyre abrasion
(Rauterberg-Wulff, 1998, 2000) and the unresolved rest
from resuspension of road dust, mainly soil.
From the differences of the unresolved rests of PM10
and PM2.5 (Table 3) near the street it can be deduced
that the resuspended particulates include a high
proportion of about 70% coarse particles. These will
be deposited within a range of some kilometres. Therefore, for the apportionment of the urban sources only
50% are taken into account and for the German sources
2O%.
In the scale of the agglomeration there is a high
dependency of ambient concentrations on the stack
height of emissions. The Berlin plant subjected to
licensing have stack heights of 50 150 m. To take this
into account we assumed that they contribute only 20%
of their emission to the urban background. The factor is
derived from dispersion calculations of the Berlin Air
Pollution Management Plan for the years 1994-2000
(SenStadt, 1995). For most relevant sources outside the
agglomeration, which lie more than 50 km away, the
emission heights are not taken into account.
The coupling of the emissions of Table 1 with the
ambient concentrations of Table 3 is shown in Table 4a
which gives the results of our source apportionment of
PM10 in as much detail as possible. The relative
contributions of the main sources in the three spatial
source groups are compared in Table 4b. Similar
investigations have been conducted by e.g., Harrison
et al. (1997), Chow et al. (1996) and Thurston and
Spengler (1985). But in our paper we tried to get a full

$31

balance between the measured concentration of PM10


with its components and our knowledge about the
emissions and to discriminate between the three spatial
groups of sources.
The comparison of secondary aerosols in the urban
background and regional background by different
laboratories shows that in the urban background there
seems to be a surplus of NO3 that is as large as the
regional background, the surplus of NH4 amounts to
about 70% and SO4 to 60%. It is difficult to understand
this and to identify the reasons. Therefore, we think that
there is an urgent need for comparable measurements
and chemical analyses in the regional background as
well as in the urban agglomeration.

7. Results

In Berlin, the ambient concentration of PM10 near


busy streets is about 40% higher than in the urban
background. 55% of this additional pollution consists of
carbonaceous material resulting from exhaust emissions
and tyre abrasion. 45% of the additional PM10pollution can be attributed to resuspended soil material.
From the PM2.5 measurements (Table 3) it can be
calculated that one third (2.2ggm 3) of the resuspension is PM2.5 and two thirds coarser material.
The difference of urban background and regional
background data shows that about 50% of the urban
background pollution is caused by emissions specific to
the agglomeration. Half of this contribution is due to
traffic emissions and 15% to domestic heating and
households.
If the regional background concentration is attributed
to all sources outside the agglomeration, with negligible
influence of the specific sources of the agglomeration,
about 55% of the urban background pollution is caused
by long range transport from outside the region and by
natural sources such as pollen and wind-borne soil. The
main contributors to this part of the ambient concentration are power plants and other industrial plant with
about 35%, and traffic and nature with about 20% each.
As Fig. lc shows, the average concentrations of SPM
are much higher with south-easterly than with westerly
winds. This is also valid for the PM 10 concentration in
the regional background. Therefore, it has to be taken
into account that sources lying south to south-east of
Berlin have high impact on PM10-concentrations in the
town.
According to Table 4b, traffic is the most important
group of sources (50%) causing high PM10 pollution in
a busy street. About one quarter of the traffic influence is
exhaust emissions and tyre abrasion in the individual
street, a further quarter is resuspension of soil particles
in the individual street and the remaining half is traffic

$32

P. Lenschow et al. / Atmospheric Environment 35 Supplement No. 1 (2001) $23-$33

influence on the city background--containing also the


regional background.
The second group of sources is combustion
(24%)--from individual stove for heating apartments
through to big power plants. About two thirds of it
consists of secondary aerosols, mostly sulphate and
nitrate, formed from Europe-wide SO2- and NO~emissions. One third is due to a source typical for
eastern European cities: emission from lignite combustion in stoves to heat apartments.
The third group consists of various natural sources
(12%).
These three groups are the sources of about 90% of
PM10 pollution in a busy street. In the urban background the partition is similar but shifted to combustion
(traffic 31%, combustion 33%, natural origin 14%).
It should be noted that the results of the PM10 source
apportionment presented here should be considered as a
preliminary estimate based on a first set of data.
Comparing these results with those from other cities
would help to improve this analysis and gradually
remove factors of uncertainty.

8. Future development

1.

2.

3.

4.

The Directive on National Emission Ceilings


proposed by the European Commission (CEC,
1999) with SO2, NOx and NH3 emissions in Europe
decreasing by about 50% until 2010 will also result
in a reduction of PM10 by about 15% within the
last years before that date.
As the impact of the traffic sector is not confined to
exhaust emissions but also includes tyre abrasion
and resuspended soil particles, even zero-emissionvehicles still cause about half the PM 10 pollution of
"dirty" vehicles. Therefore, the reduction of the
traffic impact will be much smaller than the
reduction of exhaust emission. We, therefore,
expect that the continuous replacement of old cars
(e.g. with ages more than 10 years) by new ones
with lower emissions will cause a reduction of
exhaust emissions of about 8% per year (Keller
et al., 1999) but a reduction of PM10 concentrations of only 1-2% per year.
The introduction of cleaner fuels by 2005 according
to EC Directive 98/70/EC (EC, 1998) will result in a
decrease of PM10 pollution by about 1-2%.
Therefore, Germany is promoting introduction of
these fuels in 2001 by reducing the tax rate.
In an important step in Berlin, the total public bus
fleet of 1200 buses will be equipped with particle
filters (CRT) by the end of 2000. This big step will
reduce the PM10 pollution by about 2% (corresponds to a 10% reduction of the carcinogenic EC-

5.

6.

pollution). Particle filters also trap ultrafine


particles quite effectively.
The further substitution of lignite by gas, light
heating oil or district heating is still a quite
important development.
A very important problem is the reduction of the
resuspended soil particles by traffic. We still do not
know how to reduce the significant influence of
about 5% in the urban background and up to 15%
near urban main streets.

In conclusion, there is a lack of effective measures to


control PM10 emissions with the aim of attaining the
limit values, in particular the short-term limit value of
PM 10 for 2005 in the vicinity of traffic sources. As this is
probably a widespread problem, it is necessary to
intensify mutual exchange of experiences between
European cities on investigations about the sources of
PM10 pollution as well as on the development of
effective control strategies. Apart from that, it is also
necessary--as planned by the European Commission-to review and investigate, what part of the PM mixture
actually affects human health. This ought to be followed
by a definition of appropriate limit values, with the aim
of avoiding costly and possibly ineffective or even
regrettable abatement strategies.

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