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Titel |
Fossil versus contemporary sources of fine elemental and organic carbonaceous particulate matter during the DAURE campaign in Northeast Spain |
VerfasserIn |
M. C. Minguillón, N. Perron, X. Querol, S. Szidat, S. M. Fahrni, A. Alastuey, J. L. Jimenez, C. Mohr, A. M. Ortega, D. A. Day, V. A. Lanz, L. Wacker, C. Reche, M. Cusack, F. Amato, G. Kiss, A. Hoffer, S. Decesari, F. Moretti, R. Hillamo, K. Teinilä, R. Seco, J. Peñuelas, A. Metzger, S. Schallhart, M. Müller, A. Hansel, J. F. Burkhart, U. Baltensperger, A. S. H. Prévôt |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 11, no. 23 ; Nr. 11, no. 23 (2011-12-06), S.12067-12084 |
Datensatznummer |
250010238
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Publikation (Nr.) |
copernicus.org/acp-11-12067-2011.pdf |
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Zusammenfassung |
We present results from the international field campaign DAURE
(Determination of the sources of atmospheric Aerosols in Urban and Rural
Environments in the Western Mediterranean), with the objective of
apportioning the sources of fine carbonaceous aerosols. Submicron fine
particulate matter (PM1) samples were collected during February–March
2009 and July 2009 at an urban background site in Barcelona (BCN) and at a
forested regional background site in Montseny (MSY). We present radiocarbon
(14C) analysis for elemental and organic carbon (EC and OC) and source
apportionment for these data. We combine the results with those from
component analysis of aerosol mass spectrometer (AMS) measurements, and
compare to levoglucosan-based estimates of biomass burning OC, source
apportionment of filter data with inorganic composition + EC + OC, submicron bulk
potassium (K) concentrations, and gaseous acetonitrile concentrations.
At BCN, 87 % and 91 % of the EC on average, in winter and summer,
respectively, had a fossil origin, whereas at MSY these fractions were
66 % and 79 %. The contribution of fossil sources to organic carbon (OC)
at BCN was 40 % and 48 %, in winter and summer, respectively, and 31 %
and 25 % at MSY. The combination of results obtained using the 14C
technique, AMS data, and the correlations between fossil OC and fossil EC
imply that the fossil OC at Barcelona is ∼47 % primary whereas at
MSY the fossil OC is mainly secondary (∼85 %). Day-to-day variation
in total carbonaceous aerosol loading and the relative contributions of
different sources predominantly depended on the meteorological transport
conditions. The estimated biogenic secondary OC at MSY only increased by
∼40 % compared to the order-of-magnitude increase observed for
biogenic volatile organic compounds (VOCs) between winter and summer, which
highlights the uncertainties in the estimation of that component. Biomass
burning contributions estimated using the 14C technique ranged from
similar to slightly higher than when estimated using other techniques, and the
different estimations were highly or moderately correlated. Differences can
be explained by the contribution of secondary organic matter (not included
in the primary biomass burning source estimates), and/or by an
overestimation of the biomass burning OC contribution by the 14C
technique if the estimated biomass burning EC/OC ratio used for the
calculations is too high for this region. Acetonitrile concentrations
correlate well with the biomass burning EC determined by 14C. K is a
noisy tracer for biomass burning. |
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