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Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO2

Authors :
Liu, T.
Wang, X.
Hu, Q.
Deng, W.
Zhang, Y.
Ding, X.
Fu, X.
Bernard, F.
Zhang, Z.
Lü, S.
He, Q.
Bi, X.
Chen, J.
Sun, Y.
Yu, J.
Peng, P.
Sheng, G.
Fu, J.
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou
Merck & Co. Inc
Beijing Technology and Business University
School of Earth and Space Sciences
Peking University [Beijing]
Laboratoire LERMPS (LERMPS)
Université de Technologie de Belfort-Montbeliard (UTBM)
National Central University [Taiwan] (NCU)
Ningbo University of Technology (NBUT)
Zhejiang University
Unité de recherche Pathologie végétale et phytobactériologie
Institut National de la Recherche Agronomique (INRA)
Laboratoire de Génie Civil et Génie Mécanique (LGCGM)
Université de Rennes 1 (UR1)
Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes)
Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
College of Materials Science and Optoelectronic Technology
University of Chinese Academy Sciences
State Key Laboratory of Organic Geochemistry
Chinese Academy of Sciences [Changchun Branch] (CAS)
Center for Nonlinear Science (CNS-GATECH)
Georgia Institute of Technology [Atlanta]
Franche-Comté Électronique Mécanique, Thermique et Optique - Sciences et Technologies (UMR 6174) (FEMTO-ST)
Université de Franche-Comté (UFC)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Mécanique et des Microtechniques (ENSMM)-Université de Technologie de Belfort-Montbeliard (UTBM)
University of Science and Technology of China [Hefei] (USTC)
Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC)
Institute of Atmospheric Physics [Beijing] (IAP)
Chinese Academy of Sciences [Beijing] (CAS)-Chinese Academy of Sciences [Beijing] (CAS)
Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes)
Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)
Source :
Atmospheric Chemistry and Physics, Atmospheric Chemistry and Physics, European Geosciences Union, 2016, 16 (2), pp.675-689. ⟨10.5194/acp-16-675-2016⟩, Atmospheric Chemistry and Physics, 2016, 16 (2), pp.675-689. ⟨10.5194/acp-16-675-2016⟩
Publication Year :
2016
Publisher :
HAL CCSD, 2016.

Abstract

International audience; Sulfur dioxide (SO 2) can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs), but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust (GVE) and SO 2 , a typical pollutant from coal burning, are directly co-introduced into a smog chamber, in this study, to investigate the formation of secondary organic aerosols (SOA) and sulfate aerosols through photooxidation. New particle formation was enhanced, while substantial sul-fate was formed through the oxidation of SO 2 in the presence of high concentration of SO 2. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO 2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs), formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO 2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60-200 % in the presence of high concentration of SO 2. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (R 2 = 0.97) between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) resolved OA's relatively lower oxygen-to-carbon (O : C) (0.44 ± 0.02) and higher hydrogen-to-carbon (H : C) (1.40 ± 0.03) molar ratios for the GVE / SO 2 mixture, with a significantly lower estimated average carbon oxidation state (OS c) of −0.51 ± 0.06 than −0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO 2 might be a significant explanation for the lower SOA oxidation degree.

Details

Language :
English
ISSN :
16807316 and 16807324
Database :
OpenAIRE
Journal :
Atmospheric Chemistry and Physics, Atmospheric Chemistry and Physics, European Geosciences Union, 2016, 16 (2), pp.675-689. ⟨10.5194/acp-16-675-2016⟩, Atmospheric Chemistry and Physics, 2016, 16 (2), pp.675-689. ⟨10.5194/acp-16-675-2016⟩
Accession number :
edsair.dedup.wf.001..d42220c06aa79391740551efb014220c
Full Text :
https://doi.org/10.5194/acp-16-675-2016⟩