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Better constraints on sources of carbonaceous aerosols using a combined C-14 - macro tracer analysis in a European rural background site

Gilardoni, S.; Vignati, E.; Cavalli, F.; Putaud, J. P.; Larsen, B. R.; Karl, M.; Stenström, Kristina LU ; Genberg, Johan LU ; Henne, S. and Dentener, F. (2011) In Atmospheric Chemistry and Physics 11(12). p.5685-5700
Abstract
The source contributions to carbonaceous PM2.5 aerosol were investigated at a European background site at the edge of the Po Valley, in Northern Italy, during the period January-December 2007. Carbonaceous aerosol was described as the sum of 8 source components: primary (1) and secondary (2) biomass burning organic carbon, biomass burning elemental carbon (3), primary (4) and secondary (5) fossil organic carbon, fossil fuel burning elemental carbon (6), primary (7) and secondary (8) biogenic organic carbon. The mass concentration of each component was quantified using a set of macro tracers (organic carbon OC, elemental carbon EC, and levoglucosan), micro tracers (arabitol and mannitol), and C-14 measurements. This was the first time that... (More)
The source contributions to carbonaceous PM2.5 aerosol were investigated at a European background site at the edge of the Po Valley, in Northern Italy, during the period January-December 2007. Carbonaceous aerosol was described as the sum of 8 source components: primary (1) and secondary (2) biomass burning organic carbon, biomass burning elemental carbon (3), primary (4) and secondary (5) fossil organic carbon, fossil fuel burning elemental carbon (6), primary (7) and secondary (8) biogenic organic carbon. The mass concentration of each component was quantified using a set of macro tracers (organic carbon OC, elemental carbon EC, and levoglucosan), micro tracers (arabitol and mannitol), and C-14 measurements. This was the first time that C-14 measurements covered a full annual cycle with daily resolution. This set of 6 tracers, together with assumed uncertainty ranges of the ratios of OC-to-EC, and the reference fraction of modern carbon in the 8 source categories, provides strong constraints to the source contributions to carbonaceous aerosol. The uncertainty of contributions was assessed with a Quasi-Monte Carlo (QMC) method accounting for the variability of OC and EC emission factors, the uncertainty of reference fractions of modern carbon, and the measurement uncertainty. During winter, biomass burning composed 64% (+/- 15%) of the total carbon (TC) concentration, while in summer secondary biogenic OC accounted for 50% (+/- 16%) of TC. The contribution of primary biogenic aerosol particles was negligible during the entire year. Moreover, aerosol associated with fossil sources represented 27% (+/- 16%) and 41% (+/- 26%) of TC in winter and summer, respectively. The contribution of secondary organic aerosol (SOA) to the organic mass (OM) was significant during the entire year. SOA accounted for 30% (+/- 16 %) and 85% (+/- 12 %) of OM during winter and summer, respectively. While the summer SOA was dominated by biogenic sources, winter SOA was mainly due to biomass burning and fossil sources. This indicates that the oxidation of semi-volatile and intermediate volatility organic compounds co-emitted with primary organics is a significant source of SOA, as suggested by recent model results and Aerosol Mass Spectrometer measurements. Comparison with previous global model simulations, indicates a strong underestimate of wintertime primary aerosol emissions in this region. The comparison of source apportionment results in different urban and rural areas showed that the sampling site was mainly affected by local aerosol sources during winter and regional air masses from the nearby Po Valley in summer. This observation was further confirmed by back-trajectory analysis applying the Potential Source Contribution Function method to identify potential source regions. (Less)
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type
Contribution to journal
publication status
published
subject
in
Atmospheric Chemistry and Physics
volume
11
issue
12
pages
5685 - 5700
publisher
Copernicus Gesellschaft Mbh
external identifiers
  • wos:000291939800010
  • scopus:79959937206
ISSN
1680-7324
DOI
10.5194/acp-11-5685-2011
project
MERGE
language
English
LU publication?
yes
id
5698fee9-7026-4391-91d5-a6d6529e02bb (old id 2049304)
date added to LUP
2011-07-26 13:14:58
date last changed
2017-11-05 03:04:15
@article{5698fee9-7026-4391-91d5-a6d6529e02bb,
  abstract     = {The source contributions to carbonaceous PM2.5 aerosol were investigated at a European background site at the edge of the Po Valley, in Northern Italy, during the period January-December 2007. Carbonaceous aerosol was described as the sum of 8 source components: primary (1) and secondary (2) biomass burning organic carbon, biomass burning elemental carbon (3), primary (4) and secondary (5) fossil organic carbon, fossil fuel burning elemental carbon (6), primary (7) and secondary (8) biogenic organic carbon. The mass concentration of each component was quantified using a set of macro tracers (organic carbon OC, elemental carbon EC, and levoglucosan), micro tracers (arabitol and mannitol), and C-14 measurements. This was the first time that C-14 measurements covered a full annual cycle with daily resolution. This set of 6 tracers, together with assumed uncertainty ranges of the ratios of OC-to-EC, and the reference fraction of modern carbon in the 8 source categories, provides strong constraints to the source contributions to carbonaceous aerosol. The uncertainty of contributions was assessed with a Quasi-Monte Carlo (QMC) method accounting for the variability of OC and EC emission factors, the uncertainty of reference fractions of modern carbon, and the measurement uncertainty. During winter, biomass burning composed 64% (+/- 15%) of the total carbon (TC) concentration, while in summer secondary biogenic OC accounted for 50% (+/- 16%) of TC. The contribution of primary biogenic aerosol particles was negligible during the entire year. Moreover, aerosol associated with fossil sources represented 27% (+/- 16%) and 41% (+/- 26%) of TC in winter and summer, respectively. The contribution of secondary organic aerosol (SOA) to the organic mass (OM) was significant during the entire year. SOA accounted for 30% (+/- 16 %) and 85% (+/- 12 %) of OM during winter and summer, respectively. While the summer SOA was dominated by biogenic sources, winter SOA was mainly due to biomass burning and fossil sources. This indicates that the oxidation of semi-volatile and intermediate volatility organic compounds co-emitted with primary organics is a significant source of SOA, as suggested by recent model results and Aerosol Mass Spectrometer measurements. Comparison with previous global model simulations, indicates a strong underestimate of wintertime primary aerosol emissions in this region. The comparison of source apportionment results in different urban and rural areas showed that the sampling site was mainly affected by local aerosol sources during winter and regional air masses from the nearby Po Valley in summer. This observation was further confirmed by back-trajectory analysis applying the Potential Source Contribution Function method to identify potential source regions.},
  author       = {Gilardoni, S. and Vignati, E. and Cavalli, F. and Putaud, J. P. and Larsen, B. R. and Karl, M. and Stenström, Kristina and Genberg, Johan and Henne, S. and Dentener, F.},
  issn         = {1680-7324},
  language     = {eng},
  number       = {12},
  pages        = {5685--5700},
  publisher    = {Copernicus Gesellschaft Mbh},
  series       = {Atmospheric Chemistry and Physics},
  title        = {Better constraints on sources of carbonaceous aerosols using a combined C-14 - macro tracer analysis in a European rural background site},
  url          = {http://dx.doi.org/10.5194/acp-11-5685-2011},
  volume       = {11},
  year         = {2011},
}