Elemental and organic carbon in PM10: a one year ...
嚜激lemental and organic carbon in PM10: a one year
measurement campaign within the European Monitoring
and Evaluation Programme EMEP
K. E. Yttri, W. Aas, A. Bjerke, J. N. Cape, F. Cavalli, D. Ceburnis, C. Dye,
L. Emblico, M. C. Facchini, C. Forster, et al.
To cite this version:
K. E. Yttri, W. Aas, A. Bjerke, J. N. Cape, F. Cavalli, et al.. Elemental and organic carbon in PM10: a
one year measurement campaign within the European Monitoring and Evaluation Programme EMEP.
Atmospheric Chemistry and Physics, 2007, 7 (22), pp.5711-5725. ?hal-00296378?
HAL Id: hal-00296378
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Atmos. Chem. Phys., 7, 5711每5725, 2007
7/5711/2007/
? Author(s) 2007. This work is licensed
under a Creative Commons License.
Atmospheric
Chemistry
and Physics
Elemental and organic carbon in PM10: a one year measurement
campaign within the European Monitoring and Evaluation
Programme EMEP
K. E. Yttri1 , W. Aas1 , A. Bjerke1 , J. N. Cape7 , F. Cavalli6 , D. Ceburnis2 , C. Dye1 , L. Emblico3 , M. C. Facchini3 ,
C. Forster1 , J. E. Hanssen1 , H. C. Hansson4 , S. G. Jennings2 , W. Maenhaut5 , J. P. Putaud6 , and K. T?rseth1
1 Norwegian
Institute for Air Research, P.O. Box 100, 2027 Kjeller, Norway
of Experimental Physics, National University of Ireland, Galway, Ireland
3 CNR, Institute of Atmospheric Sciences and Climate, Via P. Gobetti 101, 40129 Bologna, Italy
4 Department of Applied Environmental Science, Stockholm University, 10691 Stockholm, Sweden
5 Department of Analytical Chemistry, Institute for Nuclear Sciences, Ghent Univ., Proeftuinstraat 86, 9000 Ghent, Belgium
6 European Commission, Joint Research Centre, Institute for Environment and Sustainability, TP 460, 21020 Ispra (VA), Italy
7 Centre for Ecology & Hydrology, Edinburgh Research Station, Bush Estate, Penicuik, Midlothian, EH260QB, UK
2 Department
Received: 8 February 2007 每 Published in Atmos. Chem. Phys. Discuss.: 19 March 2007
Revised: 17 September 2007 每 Accepted: 19 October 2007 每 Published: 19 November 2007
Abstract. In the present study, ambient aerosol (PM10 ) concentrations of elemental carbon (EC), organic carbon (OC),
and total carbon (TC) are reported for 12 European rural
background sites and two urban background sites following
a one-year (1 July 2002每1 July 2003) sampling campaign
within the European Monitoring and Evaluation Programme,
EMEP (). The purpose of the campaign
was to assess the feasibility of performing EC and OC monitoring on a regular basis and to obtain an overview of the
spatial and seasonal variability on a regional scale in Europe.
Analyses were performed using the thermal-optical transmission (TOT) instrument from Sunset Lab Inc., operating according to a NIOSH derived temperature program.
The annual mean mass concentration of EC ranged from
0.17㊣0.19 ?g m?3 (mean ㊣ SD) at Birkenes (Norway) to
1.83㊣1.32 ?g m?3 at Ispra (Italy). The corresponding range
for OC was 1.20㊣1.29 ?g m?3 at Mace Head (Ireland) to
7.79㊣6.80 ?g m?3 at Ispra. On average, annual concentrations of EC, OC, and TC were three times higher for rural
background sites in Central, Eastern and Southern Europe
compared to those situated in the Northern and Western parts
of Europe. Wintertime concentrations of EC and OC were
higher than those recorded during summer for the majority of the sites. Moderate to high Pearson correlation coefficients (rp ) (0.50每0.94) were observed for EC versus OC
Correspondence to: K. E. Yttri
(key@nilu.no)
for the sites investigated. The lowest correlation coefficients
were noted for the three Scandinavian sites: Aspvreten (SE),
Birkenes (NO), and Virolahti (FI), and the Slovakian site
Stara Lesna, and are suggested to reflect biogenic sources,
wild and prescribed fires. This suggestion is supported by
the fact that higher concentrations of OC are observed for
summer compared to winter for these sites.
For the rural background sites, total carbonaceous material
accounted for 30㊣9% of PM10 , of which 27㊣9% could be
attributed to organic matter (OM) and 3.4㊣1.0% to elemental
matter (EM). OM was found to be more abundant than SO2?
4
for sites reporting both parameters.
1
Introduction
The environmental relevance of the carbonaceous aerosol
comprises a number of important topics, such as direct and
indirect climate forcing, and air quality. The high number of organic species reported to be associated with ambient fine aerosols have a wide range of different physical
and chemical properties, of which impact on human health
and cloud formation largely remains unknown. Furthermore,
black carbon is the principal light absorbing species in the
atmosphere, significantly affecting the Earth*s radiative balance (Ramanathan et al., 2001).
Published by Copernicus Publications on behalf of the European Geosciences Union.
5712
K. E. Yttri et al.: Elemental and organic carbon in PM10 : a one year measurement
Quantification of the carbonaceous content of the ambient
aerosol on the basis of single species is an insurmountable
task due to their sheer number, their various chemical and
physical properties and the complex aerosol matrix. Thus,
operational definitions of bulk carbonaceous material, such
as elemental carbon (EC) and organic carbon (OC), have
been established.
Long-term monitoring data of EC and OC is not yet available on a regional scale in Europe, although the importance of such data has been emphasized by e.g. Kahnert et
al. (2004). Monitoring of EC and OC needs to rely on both
robust and cost-efficient techniques, but at the same time a
satisfactory quality of the data must be maintained. This
poses particular challenges due to artefacts associated with
sampling of particulate OC. It is well known that quartz fibre filters adsorb organic gases (Kirchstetter et al., 2001),
and that a shift in the equilibrium between the filter, the organic constituents collected on the filter, and gaseous organic
compounds may lead to both positive and negative artefacts
during prolonged sampling. Positive artefacts arise from adsorption of gaseous organic compounds on the filter, while
negative artefacts result from evaporation of gaseous organic
material from particles collected on the filter. However, the
exact magnitude of the artefacts is difficult to address or measure by simple methods.
Significant differences have been reported for levels of
EC and OC when comparing various analytical techniques
(Schmid et al., 2001). Whereas the total carbon (TC) content corresponds well between the most commonly used analytical approaches, the recommendation made by Schmid et
al. (2001) is that only methods that account for charring during analysis should be applied when analysing for the sample content of EC and OC. Thus, methods such as thermaloptical reflectance (TOR) and thermal-optical transmittance
(TOT) should be applied. Still, differences of a factor of two
have been reported for EC when comparing the two most
commonly applied analytical protocols, NIOSH (National
Institute of Occupational Safety and Health) method 5040
and IMPROVE (Interagency Monitoring of Protected Visual
Environments) (Schmid et al., 2001; Chow et al., 2001).
Thus, in order to provide EC/OC data of high quality within
a monitoring network, a standardized protocol needs to be
established both for analysis and sampling of these carbonaceous fractions.
To assess the feasibility of performing EC and OC monitoring on a regular basis, and to obtain an overview of the
spatial and seasonal variability of EC and OC on a regional
scale in Europe, a one-year campaign was conducted at 12
rural background sites and two urban background sites in 13
European countries. The dataset benefits from the fact that
one instrument, a thermal-optical transmission instrument,
which corrects for charred organic carbon during analysis,
has been used to quantify the sample content of EC and OC.
It is our belief that the present dataset will contribute in a
positive way to the understanding of concentrations of carAtmos. Chem. Phys., 7, 5711每5725, 2007
bonaceous aerosols in the European rural background environment, and that it will be useful for the validation of the
EMEP model performance, in particular. Below, we present
a descriptive overview of the campaign and the major findings obtained.
2
Experimental work
2.1 Aerosol sampling
The EMEP EC/OC campaign was conducted during the period 1 July 2002 to 1 July 2003. Table 1 provides an overview
of the 14 sampling sites included in the campaign and the
sampling equipment used, whereas the spatial distribution of
the sites is shown in Fig. 1. 11 of the 14 sites are established
EMEP sites, which fulfils the criteria of a regional background site stated by EMEP (
ccc/manual/index.html). The Penicuick (UK) site is also a
rural background site, but not an EMEP site, whereas Ghent
(BE) and San Pietro Capofiume (S.P.C.) (IT) are both urban
background sites. Aerosol sampling was performed using
CEN (European Committee for Standardization) approved
or equivalent PM10 gravimetric samplers, collecting one 24h sample every week (starting Tuesday mornings 7 AM).
Aerosols were collected on pre-heated (850? C, 3.5 h) quartz
fibre filters; 47-mm and 8 inch℅10 inch quartz fibre filters
were purchased from Whatman (QM-A), whereas 150-mm
quartz fibre filters were purchased from Munktell (MK 360).
To minimize differences in the adsorptive capacity, filters
were picked from the same batch number. The quartz fibre
filters were conditioned at 20㊣1? C and 50㊣5% RH (relative
humidity) for 48 h before and after exposure and weighed
for obtaining PM10 mass concentration. The 47-mm filters
were transported back and forth in petri slides, whereas the
8 inch℅10 inch and the 150-mm quartz fibre filters were enclosed in sealed aluminium foil. All quartz fibre filters were
stored at 4? C before being analysed.
Field blanks were assigned to each fourth day of sampling,
and treated in exactly the same manner regarding preparation, handling, transport and storage as the filters being exposed.
All filter preparations, pre-heating, conditioning and
weighing, were performed at the Norwegian Institute for Air
Research (NILU) (EMEP - Chemical Coordinating Centre).
2.2 Thermal-optical transmission analysis
The samples (n=684) content of EC, OC, and TC, were
quantified using the thermal-optical transmittance (TOT) instrument from Sunset laboratories Inc, operating according
to a NIOSH derived temperature programme (Table 2). The
※8785 Air Particulate Matter On Filter Media§ reference material from The National Institute of Standards and Technology (NIST) (Klouda et al., 2005) was used to test the
7/5711/2007/
K. E. Yttri et al.: Elemental and organic carbon in PM10 : a one year measurement
5713
Table 1. Sampling sites and operational parameters of the sampling equipment used at the various sites. The sites are ordered from south to
north by latitude.
Sampling sites
(EMEP code)
Country
Site category
Aerosol
sampler
Braganza (PT01)
Ispra (JRC) (IT04)
Illmitz (AT02)
Stara Lesna (SK04)
Kos?etice (CZ03)
Langenbru?gge (DE02)
Kollumerwaard (NL09)
Mace Head (IR31)
Penicuik (GB46)
Birkenes (NO01)
Aspvreten (SE12)
Virolahti (FI17)
Portugal
Italy
Austria
Slovakia
The Czech republic
Germany
Holland
Ireland
Great Britain
Norway
Sweden
Finland
Rural background
Rural background
Rural background
Rural background
Rural background
Rural background
Rural background
Rural background
Rural background
Rural background
Rural background
Rural background
San Pietro Capofiume
(S.P.C.) (IT08)
Ghent (BE02)
Italy
Belgium
10
Kollumerwaard (NL)
Filter face
velocity (cm s?1 )
Hi-Vol (Sierra)
KFG
Partisol
Partisol
FH 95 SEQ
Hi-Vol (Digitel)
KFG
KFG
Partisol
KFG
Gent Filter Unit
KFG
8§℅10§
47
47
47
47
150
47
47
47
47
47
47
1133
38
16.7
16.7
38
500
38
38
16.7
38
17
38
46
48
24
22
53
54
53
48
23
46
23
50
Urban background
Gent Filter Unit
47
17
23
Urban background
Gent Filter Unit
47
17
24
10
Birkenes (NO)
4
2
?g m-3
6
6
4
0
TC
OC
10
OC
4
TC
EC
10
Ghent (BE)
?g m-3
?g m-3
6
4
EC
Langenbr邦gge (DE)
6
4
2
0
0
TC
10
OC
TC
EC
10
Penicuik (GB)
8
OC
EC
Stara Lesna (SK)
8
?g m-3
?g m-3
OC
8
2
6
4
2
6
4
2
0
0
TC
10
OC
EC
TC
OC
10
Mace Head (IE)
8
EC
Illmitz (AT)
8
?g m-3
?g m-3
4
0
OC
8
6
4
2
6
4
2
0
0
10
OC
EC
TC
Ispra (IT)
10
Braganza (PT)
10
8
6
4
6
4
2
2
TC
OC
EC
10
6
4
OC
EC
EC
Ko?etice (CZ)
6
4
2
0
TC
OC
8
2
0
0
San Pietro Capofiume (IT)
8
?g m-3
?g m-3
8
?g m-3
TC
?g m-3
6
2
TC
EC
Virolahti (FI)
8
6
0
TC
EC
10
2
2
0
Aspvreten (SE)
8
8
?g m-3
?g m-3
8
Flow rate
(l min?1 )
?g m-3
10
Filter size
(d)(mm)
0
TC
OC
EC
TC
OC
EC
Fig. 1. Spatial distribution of the sampling sites participating in the campaign and their annual mean concentration of EC, OC and TC
(?g m?3 ) for the period 1 July 2002每1 July 2003.
7/5711/2007/
Atmos. Chem. Phys., 7, 5711每5725, 2007
5714
K. E. Yttri et al.: Elemental and organic carbon in PM10 : a one year measurement
Table 2. Quartz parameter temperature program.
MODE
MODE 1
Step 1
Step 2
Step 3
Step 4
MODE 2
Step 1
Step 2
Step 3
Step 4
Step 5
Step 6
Step 7
Carrier gas
Temperature (? C)
Time (s)
100% He
100% He
100% He
100% He
220
360
525
850
60
60
60
90
98% He/2% O2
98% He/2% O2
98% He/2% O2
98% He/2% O2
98% He/2% O2
98% He/2% O2
98% He/2% O2
550
650
720
790
820
860
890
30
30
30
40
30
20
40
performance of the temperature programme. The result is
presented in Sect. 3.1.
2.2.1 WSOC analysis
A total of 71 samples were subjected to WSOC (Watersoluble organic carbon) analysis. Before analysis, parts of
each filter were soaked in Milli-Q water (7 ml for low volume
filters and 20 ml for high volume filters) and subjected to sonication (30 min) for extraction of the WSOC. The water extracts were filtered using PTFE-membrane single-use syringe
filters (Sartorius Minisart SRP 15). The dissolved organic
material was then quantified using a Shimadzu TOC liquid analyzer (model TC5000A). This instrument also allows
for determination of inorganic (carbonate) carbon following
acidification. The inorganic carbon was subtracted from the
dissolved organic carbon in order to obtain the WSOC fraction. However, the concentrations of inorganic carbon were
negligible most of the time. The water-insoluble organic carbon (WINSOC) was quantified by subtracting WSOC from
OC. The WSOC analysis was performed at the Institute of
Atmospheric Sciences and Climate of the Italian National
Research Council (ISAC-CNR).
3
Results and discussion
3.1 Uncertainties in EC/OC measurements
The precision and the detection limits of the TOT instrument
were determined by the variability of the EC and OC concentrations on exposed filters and on filter blanks, respectively.
The precision was found to be satisfactory with a relative
standard deviation below 5%.
The level of EC on the filed blanks was negligible, whereas
the OC concentration ranged from 0.41每1.94 ?g cm?2
(Fig. 2). When converting ?g cm?2 to ?g m?3 , the range
Atmos. Chem. Phys., 7, 5711每5725, 2007
for OC was 0.1每1.0 ?g m?3 ; however, the concentration was
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