In-cloud processes of methacrolein under simulated conditions - Part 2: Formation of secondary organic aerosol

被引:58
|
作者
El Haddad, I. [1 ,2 ,3 ]
Liu, Yao [1 ,2 ,3 ]
Nieto-Gligorovski, L. [1 ,2 ,3 ]
Michaud, V. [4 ]
Temime-Roussel, B. [1 ,2 ,3 ]
Quivet, E. [1 ,2 ,3 ]
Marchand, N. [1 ,2 ,3 ]
Sellegri, K. [4 ]
Monod, A. [1 ,2 ,3 ]
机构
[1] Univ Aix Marseille 1, CNRS, UMR 6264, Lab Chim Provence,Equipe IRA, F-13331 Marseille 3, France
[2] Univ Aix Marseille 2, CNRS, UMR 6264, Lab Chim Provence,Equipe IRA, F-13331 Marseille 3, France
[3] Univ Aix Marseille 3, CNRS, UMR 6264, Lab Chim Provence,Equipe IRA, F-13331 Marseille 3, France
[4] Univ Clermont Ferrand, Observ Phys Globe Clermont Ferrand, UMR 6016, Lab Meteorol Phys, F-63177 Aubiere, France
关键词
MASS-SPECTROMETRY; AQUEOUS-PHASE; CHEMICAL-COMPOSITION; DICARBOXYLIC-ACIDS; OXIDATION-PRODUCTS; OLIGOMER FORMATION; ISOPRENE; PHOTOOXIDATION; MODEL; PACIFIC;
D O I
10.5194/acp-9-5107-2009
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The fate of methacrolein in cloud evapo-condensation cycles was experimentally investigated. To this end, aqueous-phase reactions of methacrolein with OH radicals were performed (as described in Liu et al., 2009), and the obtained solutions were then nebulized and dried into a mixing chamber. ESI-MS and ESI-MS/MS analyses of the aqueous phase composition denoted the formation of high molecular weight multifunctional products containing hydroxyl, carbonyl and carboxylic acid moieties. The time profiles of these products suggest that their formation can imply radical pathways. These high molecular weight organic products are certainly responsible for the formation of secondary organic aerosol (SOA) observed during the nebulization experiments. The size, number and mass concentration of these particles increased significantly with the reaction time: after 22 h of reaction, the aerosol mass concentration was about three orders of magnitude higher than the initial aerosol quantity. The evaluated SOA yield ranged from 2 to 12%. These yields were confirmed by another estimation method based on the hygroscopic and volatility properties of the obtained SOA measured and reported by Michaud et al. (2009). These results provide, for the first time to our knowledge, strong experimental evidence that cloud processes can act, through photooxidation reactions, as important contributors to secondary organic aerosol formation in the troposphere.
引用
收藏
页码:5107 / 5117
页数:11
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