Particle phase acidity and oligomer formation in secondary organic aerosol

被引:296
作者
Gao, S
Ng, NL
Keywood, M
Varutbangkul, V
Bahreini, R
Nenes, A
He, JW
Yoo, KY
Beauchamp, JL
Hodyss, RP
Flagan, RC
Seinfeld, JH
机构
[1] CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91125 USA
[2] CALTECH, Dept Chem Engn, Pasadena, CA 91125 USA
[3] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[4] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[5] Univ Houston, Dept Math, Houston, TX 77204 USA
[6] CALTECH, Dept Chem, Pasadena, CA 91125 USA
关键词
D O I
10.1021/es049125k
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A series of controlled laboratory experiments are carried out in dual Teflon chambers to examine the presence of oligomers in secondary organic aerosols (SOA) from hydrocarbon ozonolysis as well as to explore the effect of particle phase acidity on SOA formation. In all seven hydrocarbon systems studied (i.e., alpha-pinene, cyclohexene, 1-methyl cyclopentene,cycloheptene, 1-methylcyclohexene, cyclooctene, and terpinolene), oligomers with MW from 250 to 1600 are present in the SOA formed, both in the absence and presence of seed particles and regardless of the seed particle acidity. These oligomers are comparable to, and in some cases, exceed the low molecular weight species (MW < 250) in ion intensities in the ion trap mass spectra, suggesting they may comprise a substantial fraction of the total aerosol mass. It is possible that oligomers are widely present in atmospheric organic aerosols, formed through acid- or base-catalyzed heterogeneous reactions. In addition, as the seed particle acidity increases, larger oligomers are formed more abundantly in the SOA; consequently, the overall SOA yield also increases. This explicit effect of particle phase acidity on the composition and yield of SOA may have important climatic consequences and need to be considered in relevant models.
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收藏
页码:6582 / 6589
页数:8
相关论文
共 19 条
[1]   Global distribution and climate forcing of carbonaceous aerosols [J].
Chung, SH ;
Seinfeld, JH .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2002, 107 (D19) :AAC14-1
[2]   State-of-the-art chamber facility for studying atmospheric aerosol chemistry [J].
Cocker, DR ;
Flagan, RC ;
Seinfeld, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (12) :2594-2601
[3]   Effect of acidic seed on biogenic secondary organic aerosol growth [J].
Czoschke, NM ;
Jang, M ;
Kamens, RM .
ATMOSPHERIC ENVIRONMENT, 2003, 37 (30) :4287-4299
[4]  
Gaskell SJ, 1997, J MASS SPECTROM, V32, P677, DOI 10.1002/(SICI)1096-9888(199707)32:7<677::AID-JMS536>3.3.CO
[5]  
2-7
[6]   Aerosol-chamber study of the α-pinene/O3 reaction:: influence of particle acidity on aerosol yields and products [J].
Iinuma, Y ;
Böge, O ;
Gnauk, T ;
Herrmann, H .
ATMOSPHERIC ENVIRONMENT, 2004, 38 (05) :761-773
[7]  
*IPCC, 2001, CLIM CHANG CONTR WOR
[8]   Heterogeneous atmospheric aerosol production by acid-catalyzed particle-phase reactions [J].
Jang, MS ;
Czoschke, NM ;
Lee, S ;
Kamens, RM .
SCIENCE, 2002, 298 (5594) :814-817
[9]   Aerosol formation in the cyclohexene-ozone system [J].
Kalberer, M ;
Yu, J ;
Cocker, DR ;
Flagan, RC ;
Seinfeld, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (23) :4894-4901
[10]   Identification of polymers as major components of atmospheric organic aerosols [J].
Kalberer, M ;
Paulsen, D ;
Sax, M ;
Steinbacher, M ;
Dommen, J ;
Prevot, ASH ;
Fisseha, R ;
Weingartner, E ;
Frankevich, V ;
Zenobi, R ;
Baltensperger, U .
SCIENCE, 2004, 303 (5664) :1659-1662