Measurements of secondary organic aerosol from oxidation of cycloalkenes, terpenes, and m-xylene using an Aerodyne aerosol mass spectrometer

被引:234
|
作者
Bahreini, R
Keywood, MD
Ng, NL
Varutbangkul, V
Gao, S
Flagan, RC
Seinfeld, JH
Worsnop, DR
Jimenez, JL
机构
[1] CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91125 USA
[2] CALTECH, Dept Chem Engn, Pasadena, CA 91125 USA
[3] Aerodyne Res Inc, Billerica, MA 01821 USA
[4] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA
[5] Univ Colorado, CIRES, Boulder, CO 80309 USA
关键词
D O I
10.1021/es048061a
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The Aerodyne aerosol mass spectrometer (AMS) was used to characterize physical and chemical properties of secondary organic aerosol (SOA) formed during ozonolysis of cycloalkenes and biogenic hydrocarbons and photo-oxidation of m-xylene. Comparison of mass and volume distributions from the AMS and differential mobility analyzers yielded estimates of "effective" density of the SOA in the range of 0.64-1.45 g/cm(3), depending on the particular system. Increased contribution of the fragment at m/z 44, CO2+ ion fragment of oxygenated organics, and higher "Delta" values, based on ion series analysis of the mass spectra, in nucleation experiments of cycloalkenes suggest greater contribution of more oxygenated molecules to the SOA as compared to those formed under seeded experiments. Dominant negative "Delta" values of SOA formed during ozonolysis of biogenics indicates the presence of terpene derivative structures or cyclic or unsaturated oxygenated compounds in the SOA. Evidence of acid-catalyzed heterogeneous chemistry, characterized by greater contribution of higher molecular weight fragments to the SOA and corresponding changes in "Delta" patterns, is observed in the ozonolysis of alpha-pinene. Mass spectra of SOA formed during photo-oxidation of m-xylene exhibit features consistent with the presence of furandione compounds and nitro organics. This study demonstrates that mixtures of SOA compounds produced from similar precursors result in broadly similar AMS mass spectra. Thus, fragmentation patterns observed for biogenic versus anthropogenic SOA may be useful in determining the sources of ambient SOA.
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页码:5674 / 5688
页数:15
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