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气溶胶液相水在挥发性有机物形成二次有机气溶胶中的作用。

Role of Aerosol Liquid Water in Secondary Organic Aerosol Formation from Volatile Organic Compounds.

机构信息

Department of Chemistry, University of Toronto , 80 Saint George Street, Toronto, Ontario M5S 3H6, Canada.

出版信息

Environ Sci Technol. 2017 Feb 7;51(3):1405-1413. doi: 10.1021/acs.est.6b04700. Epub 2017 Jan 26.

Abstract

A key mechanism for atmospheric secondary organic aerosol (SOA) formation occurs when oxidation products of volatile organic compounds condense onto pre-existing particles. Here, we examine effects of aerosol liquid water (ALW) on relative SOA yield and composition from α-pinene ozonolysis and the photooxidation of toluene and acetylene by OH. Reactions were conducted in a room-temperature flow tube under low-NO conditions in the presence of equivalent loadings of deliquesced (∼20 μg m ALW) or effloresced (∼0.2 μg m ALW) ammonium sulfate seeds at exactly the same relative humidity (RH = 70%) and state of wall conditioning. We found 13% and 19% enhancements in relative SOA yield for the α-pinene and toluene systems, respectively, when seeds were deliquesced rather than effloresced. The relative yield doubled in the acetylene system, and this enhancement was partially reversible upon drying the prepared SOA, which reduced the yield by 40% within a time scale of seconds. We attribute the high relative yield of acetylene SOA on deliquesced seeds to aqueous partitioning and particle-phase reactions of the photooxidation product glyoxal. The observed range of relative yields for α-pinene, toluene, and acetylene SOA on deliquesced and effloresced seeds suggests that ALW plays a complicated, system-dependent role in SOA formation.

摘要

大气二次有机气溶胶(SOA)形成的一个关键机制是挥发性有机化合物的氧化产物在预先存在的颗粒上凝结。在这里,我们研究了气溶胶液态水(ALW)对α-蒎烯臭氧氧化和 OH 光氧化甲苯和乙炔生成相对 SOA 产率和组成的影响。反应在室温流动管中进行,在低 NO 条件下,在相同的相对湿度(RH = 70%)和壁处理状态下,存在具有相同负载量的潮解(∼20 μg m ALW)或风化(∼0.2 μg m ALW)的硫酸铵种子。当种子潮解而不是风化时,α-蒎烯和甲苯体系的相对 SOA 产率分别提高了 13%和 19%。在乙炔体系中,相对产率增加了一倍,并且在准备 SOA 干燥时,这种增强部分是可逆的,在几秒钟的时间内,产率降低了 40%。我们将乙炔 SOA 在潮解种子上的高相对产率归因于光氧化产物乙二醛的水分配和颗粒相反应。在潮解和风化种子上α-蒎烯、甲苯和乙炔 SOA 的相对产率的观察范围表明,ALW 在 SOA 形成中起着复杂的、依赖于系统的作用。

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