Secondary organic aerosol production from aqueous photooxidation of glycolaldehyde: Laboratory experiments

被引:138
作者
Perri, Mark J. [1 ]
Seitzinger, Sybil [2 ]
Turpin, Barbara J. [1 ]
机构
[1] Rutgers State Univ, Dept Environm Sci, New Brunswick, NJ 08901 USA
[2] Rutgers State Univ, Inst Marine & Coastal Sci, NOAA CMER Program, New Brunswick, NJ 08901 USA
基金
美国国家科学基金会; 美国海洋和大气管理局;
关键词
Secondary organic aerosol; Cloud processing; Glycolaldehyde; Oligomer; Particulate matter; Oxalic acid; Glycolic acid; Malonic acid; Succinic acid; Electrospray ionization mass spectrometry; Fourier transform ion cyclotron resonance mass spectrometry; Isoprene; RADICAL-INITIATED OXIDATION; SOLUBLE DICARBOXYLIC-ACIDS; MASS-SPECTROMETRY; ATMOSPHERIC CHEMISTRY; MARINE ATMOSPHERE; ARCTIC AEROSOLS; RATE CONSTANTS; OXALIC-ACID; CLOUD; MECHANISMS;
D O I
10.1016/j.atmosenv.2008.11.037
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Organic particulate matter (PM) formed in the atmosphere (secondary organic aerosol; SOA) is a substantial yet poorly understood contributor to atmospheric PM. Aqueous photooxidation in clouds, fogs and aerosols is a newly recognized SOA formation pathway. This study investigates the potential for aqueous glycolaldehyde oxidation to produce low volatility products that contribute SOA mass. To our knowledge, this is the first confirmation that aqueous oxidation of glycolaldehyde via the hydroxyl radical forms glyoxal and glycolic acid, as previously assumed. Subsequent reactions form formic acid, glyoxylic acid, and oxalic acid as expected. Unexpected products include malonic acid, succinic acid, and higher molecular weight compounds, including oligomers. Due to (1) the large source strength of glycolaldehyde from precursors such as isoprene and ethene, (2) its water solubility, and (3) the aqueous formation of low volatility products (organic acids and oligomers), we predict that aqueous photooxidation of glycolaldehyde and other aldehydes in cloud, fog, and aerosol water is an important source of SOA and that incorporation of this SOA formation pathway in chemical transport models will help explain the current under-prediction of organic PM concentrations. (C) 2008 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1487 / 1497
页数:11
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