Effect of particle phase oligomer formation on aerosol growth

被引:15
作者
Vesterinen, M.
Lehtinen, K. E. J.
Kulmala, M.
Laaksonen, A.
机构
[1] Univ Kuopio, Dept Phys, FIN-70211 Kuopio, Finland
[2] Finnish Meteorol Inst, Kuopio Unit, Kuopio, Finland
[3] Univ Helsinki, Dept Phys Sci, Div Atmospher Sci, Helsinki, Finland
基金
芬兰科学院;
关键词
oligomer; monoterpene; dimerisation; SOA;
D O I
10.1016/j.atmosenv.2006.10.024
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
We study theoretically the effect of oligomer formation on secondary organic aerosol (SOA) growth following ozonolysis of alpha-pinene. Our goal is to show qualitatively, using a simplified condensational growth model, that the formation of involatile oligomers can induce the condensation growth of aerosols even if the secondary organic species formed in the oxidation reactions are rather volatile and therefore poorly condensable. The closed system studied consists of a single effective gas-phase oxidation product, and a seed aerosol population consisting of monodisperse ammonium sulphate particles. The oligomer formation is described as an effective dimerisation reaction between the monomers in the aerosol phase. By varying the dimerisation constant until our model results match the results from earlier smog-chamber studies, we are able to make order-of-magnitude estimations of the unknown dimerisation rates needed to induce the observed SOA growth. We also make model simulations using atmospheric alpha-pinene and ozone concentrations, and find that the effective dimerisation rate inducing SOA growth in the atmosphere has to be considerably higher than that causing SOA growth in smog-chamber conditions. (c) 2006 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1768 / 1776
页数:9
相关论文
共 20 条
[1]  
[Anonymous], 1970, HIGHLY DISPERSED AER
[2]  
[Anonymous], ATMOS CHEM PHYS DISC, DOI DOI 10.5194/acpd-4-2905-2004
[3]   Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions - Part 1: aldehydes and ketones [J].
Barsanti, KC ;
Pankow, JF .
ATMOSPHERIC ENVIRONMENT, 2004, 38 (26) :4371-4382
[4]   Mathematical model for gas-particle partitioning of secondary organic aerosols [J].
Bowman, FM ;
Odum, JR ;
Seinfeld, JH ;
Pandis, SN .
ATMOSPHERIC ENVIRONMENT, 1997, 31 (23) :3921-3931
[5]   Gas-phase terpene oxidation products: a review [J].
Calogirou, A ;
Larsen, BR ;
Kotzias, D .
ATMOSPHERIC ENVIRONMENT, 1999, 33 (09) :1423-1439
[6]  
Chang Raymond., 1981, Physical Chemistry with Applications to Biological Systems, V2nd
[7]   The effect of water on gas-particle partitioning of secondary organic aerosol.: Part I:: α-pinene/ozone system [J].
Cocker, DR ;
Clegg, SL ;
Flagan, RC ;
Seinfeld, JH .
ATMOSPHERIC ENVIRONMENT, 2001, 35 (35) :6049-6072
[8]   Particle phase acidity and oligomer formation in secondary organic aerosol [J].
Gao, S ;
Ng, NL ;
Keywood, M ;
Varutbangkul, V ;
Bahreini, R ;
Nenes, A ;
He, JW ;
Yoo, KY ;
Beauchamp, JL ;
Hodyss, RP ;
Flagan, RC ;
Seinfeld, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (24) :6582-6589
[9]   Formation of organic aerosols from the oxidation of biogenic hydrocarbons [J].
Hoffmann, T ;
Odum, JR ;
Bowman, F ;
Collins, D ;
Klockow, D ;
Flagan, RC ;
Seinfeld, JH .
JOURNAL OF ATMOSPHERIC CHEMISTRY, 1997, 26 (02) :189-222
[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