Chamber studies of secondary organic aerosol growth by reactive uptake of simple carbonyl compounds

被引:289
作者
Kroll, JH
Ng, NL
Murphy, SM
Varutbangkul, V
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
关键词
D O I
10.1029/2005JD006004
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] Recent experimental evidence indicates that heterogeneous chemical reactions play an important role in the gas-particle partitioning of organic compounds, contributing to the formation and growth of secondary organic aerosol in the atmosphere. Here we present laboratory chamber studies of the reactive uptake of simple carbonyl species ( formaldehyde, octanal, trans, trans-2,4-hexadienal, glyoxal, methylglyoxal, 2,3-butanedione, 2,4-pentanedione, glutaraldehyde, and hydroxyacetone) onto inorganic aerosol. Gas-phase organic compounds and aqueous seed particles ( ammonium sulfate or mixed ammonium sulfate/ sulfuric acid) are introduced into the chamber, and particle growth and composition are monitored using a differential mobility analyzer and an Aerodyne Aerosol Mass Spectrometer. No growth is observed for most carbonyls studied, even at high concentrations ( 500 ppb to 5 ppm), in contrast with the results from previous studies. The single exception is glyoxal (CHOCHO), which partitions into the aqueous aerosol much more efficiently than its Henry's law constant would predict. No major enhancement in particle growth is observed for the acidic seed, suggesting that the large glyoxal uptake is not a result of particle acidity but rather of ionic strength of the seed. This increased partitioning into the particle phase still cannot explain the high levels of glyoxal measured in ambient aerosol, indicating that additional ( possibly irreversible) pathways of glyoxal uptake may be important in the atmosphere.
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页码:1 / 10
页数:10
相关论文
共 73 条
[21]   RATE CONSTANTS AND MECHANISMS FOR THE REACTION OF OH (OD) RADICALS WITH ACETYLENE, PROPYNE, AND 2-BUTYNE IN AIR AT 297 +/- 2K [J].
HATAKEYAMA, S ;
WASHIDA, N ;
AKIMOTO, H .
JOURNAL OF PHYSICAL CHEMISTRY, 1986, 90 (01) :173-178
[22]   Determination of airborne carbonyls: Comparison of a thermal desorption/GC method with the standard DNPH/HPLC method [J].
Ho, SSH ;
Yu, JZ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (03) :862-870
[23]   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
[24]   Uptake of acetone into sulfuric-acid solutions [J].
Imamura, T ;
Akiyoshi, H .
GEOPHYSICAL RESEARCH LETTERS, 2000, 27 (09) :1419-1422
[25]   Heterogeneous interaction of formaldehyde with cold sulfuric acid: Implications for the upper troposphere and lower stratosphere [J].
Iraci, LT ;
Tolbert, MA .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1997, 102 (D13) :16099-16107
[26]   Organic aerosol growth by acid-catalyzed heterogeneous reactions of octanal in a flow reactor [J].
Jang, M ;
Lee, S ;
Kamens, RM .
ATMOSPHERIC ENVIRONMENT, 2003, 37 (15) :2125-2138
[27]   Semiempirical model for organic aerosol growth by acid-catalyzed heterogeneous reactions of organic carbonyls [J].
Jang, MS ;
Czoschke, NM ;
Northcross, AL .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (01) :164-174
[28]   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
[29]   Particle growth by acid-catalyzed heterogeneous reactions of organic carbonyls on preexisting aerosols [J].
Jang, MS ;
Carroll, B ;
Chandramouli, B ;
Kamens, RM .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2003, 37 (17) :3828-3837
[30]   Atmospheric secondary aerosol formation by heterogeneous reactions of aldehydes in the presence of a sulfuric acid aerosol catalyst [J].
Jang, MS ;
Kamens, RM .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (24) :4758-4766