Organosulfates from glycolaldehyde in aqueous aerosols and clouds: Laboratory studies

Organosulfates from glycolaldehyde in aqueous aerosols and clouds: Laboratory studies
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DOI:
10.1016/j.atmosenv.2010.03.031
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发表时间:
2010-07
影响因子:
5
通讯作者:
M. Perri;Y. Lim;S. Seitzinger;B. Turpin
M. Perri;Y. Lim;S. Seitzinger;B. Turpin
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
M. Perri;Y. Lim;S. Seitzinger;B. Turpin

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酸性种子颗粒上的二次有机气溶胶 (SOA) 形成增强; SOA 也会在酸性硫酸盐普遍存在的云处理反应过程中形成。最近的一些研究集中在大气气溶胶或烟雾室实验中有机硫酸盐的鉴定,以及这些产品的形成机制。我们鉴定了在硫酸存在下稀乙醇醛水溶液的实验室羟基自由基氧化过程中形成的几种有机硫酸盐产物。我们提出了一种自由基-自由基反应机制,该机制与我们的实验条件下这些产物的形成一致。使用动力学模型,我们估计有机硫酸盐在云处理过程中由这些前体形成的有机物中所占比例不到 1%。然而,在湿酸性气溶胶中,前体高度浓缩,酸性硫酸盐占气溶胶质量的近一半,这种自由基-自由基反应可以解释大量有机硫酸盐的产生。
Secondary organic aerosol (SOA) formation is enhanced on acidic seed particles; SOA also forms during cloud processing reactions where acidic sulfate is prevalent. Recently several studies have focused on the identification of organosulfates in atmospheric aerosols or smog chamber experiments, and upon the mechanism of formation for these products. We identify several organosulfate products formed during the laboratory OH radical oxidation of dilute aqueous glycolaldehyde in the presence of sulfuric acid. We propose a radical–radical reaction mechanism as being consistent with formation of these products under our experimental conditions. Using a kinetics model we estimate that organosulfates account for less than 1% of organic matter formed from these precursors during cloud processing. However, in wet acidic aerosols, where precursors are highly concentrated and acidic sulfate makes up close to half of the aerosol mass, this radical–radical reaction could account for significant organosulfate production.