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Insights into the secondary fraction of the organic aerosol in a Mediterranean urban area: Marseille
El Haddad I., Marchand N., Termine-Roussel B., Wortham H., Piot C., Besombes J.-L., Baduel C., Voisin D., Armengaud A., Jaffrezo J.-L.
Atmospheric Chemistry and Physics 11, 5 (2011) 2059-2079 - http://hal.archives-ouvertes.fr/hal-00608071
Articles dans des revues avec comité de lecture
Chimie/Autre
Insights into the secondary fraction of the organic aerosol in a Mediterranean urban area: Marseille
Imad El Haddad () 1, Nicolas Marchand 1, Brice Termine-Roussel 1, Henri Wortham 1, 2, Christine Piot 3, 4, Jean-Luc Besombes () 4, Christine Baduel 3, Didier Voisin () 3, Alexandre Armengaud 5, J.-L. Jaffrezo () 3
1 :  Laboratoire Chimie Provence (LCP)
http://lc-provence.fr
Université de Provence - Aix-Marseille I – CNRS : UMR6264
Université de Provence LCP, Equipe Instrumentation et Reactivité Atmosphérique (case 29) 3, place V Hugo 13331 Marseille Cedex 3
France
2 :  Université d'Aix-Marseille
Laboratoire Chimie Provence
Laboratoire Chimie Provence (UMR 6264), Équipe Instrumentation et Réactivité Atmosphérique, 3 place Victor Hugo, 13331 Marseille Cedex 3, France
France
3 :  Laboratoire de glaciologie et géophysique de l'environnement (LGGE)
http://lgge.obs.ujf-grenoble.fr
CNRS : UMR5183 – OSUG – INSU – Université Joseph Fourier - Grenoble I
Domaine Universitaire 54 Rue Molière - BP 96 38402 ST MARTIN D HERES CEDEX
France
4 :  Laboratoire de Chimie Moléculaire et Environnement (LCME)
Université de Savoie
Campus Scientifique de Savoie-Technolac Le Bourget du Lac Cedex
France
5 :  Regional Network for Air Quality Monitoring
Atmo-PACA
146 rue Paradis 13006 Marseille
France
CHANG
A comprehensive aerosol characterization was conducted at Marseille during summer, including organic (OC) and elemental carbon (EC), major ionic species, radiocarbon (14C), water-soluble OC and HULIS (HUmic LIke Substances), elemental composition and primary and secondary organic markers. This paper is the second paper of a two-part series that uses this dataset to investigate the sources of Organic Aerosol (OA). While the first paper investigates the primary sources (El Haddad et al., 2010), this second paper focuses on the secondary fraction of the organic aerosol. In the context of overall OC mass balance, primary OC (POC) contributes on average for only 22% and was dominated by vehicular emissions accounting on average for 17% of OC. As a result, 78% of OC mass cannot be attributed to the major primary sources and remains un-apportioned. Radiocarbon measurements suggest that more than 70% of this fraction is of non-fossil origin, assigned predominantly to biogenic secondary organic carbon (BSOC). Therefore, contributions from three traditional BSOC precursors, isoprene, $\alpha $-pinene and β-caryophyllene, were considered. These were estimated using the ambient concentrations of Secondary Organic Aerosol (SOA) markers from each precursor and laboratory-derived marker mass fraction factors. Secondary organic markers derived from isoprene photo-oxidation (ie: 2-methylglyceric acid and 2-methyltetrols) do not exhibit the same temporal trends. This variability was assigned to the influence of NOx concentration on their formation pathways and to their potential decay by further processing in the atmosphere. The influence of changes in isoprene chemistry on assessment of isoprene SOC contribution was evaluated explicitly. The results suggest a 60-fold variation between the different estimates computed using different isoprene SOC markers, implying that the available profiles do not reflect the actual isoprene SOC composition observed in Marseille. Using the marker-based approach, the aggregate contribution from traditional BSOC was estimated at only 4.2% of total OC and was dominated by α-pinene SOC accounting on average for 3.4% of OC. As a result, these estimates underpredict the inexplicably high loadings of OC. This underestimation can be associated with (1) uncertainties underlying the marker-based approach, (2) presence of other SOC precursors and (3) further processing of fresh SOC, as indicated by organosulfates (RSO4H) and HUmic LIke Substances (HULIS) measurements.
Anglais
2011

Atmospheric Chemistry and Physics
Publisher European Geosciences Union (EGU)
ISSN 1680-7316 (eISSN : 1680-7324)
internationale
07/03/2011
11
5
2059-2079

http://www.atmos-chem-phys.net/11/2059/2011/acp-11-2059-2011.html

ADEME under the PRIMEQUAL2 grant no. 0001135 (FORMES program) ; ARTEMIS program
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