Enhanced organic aerosol formation induced by inorganic aerosol formed in laboratory photochemical experiments

IF 3.9 3区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Journal of Aerosol Science Pub Date : 2024-10-23 DOI:10.1016/j.jaerosci.2024.106481
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Abstract

Atmospheric inorganic gases such as NOx, SO2, and NH3 have diverse effects on the formation of secondary organic aerosol (SOA). A comprehensive investigation is necessary to fully understand the atmospheric processing of SOA. In this study, we examined the photooxidation of xylene isomers in the presence of inorganic gases using a combined facility comprising a smog chamber (SC) and an oxidation flow reactor (OFR). SC experiments at higher xylene concentrations and humid conditions revealed SOA yields of 37%, 39%, and 39% with NH3, compared to 15%, 11%, and 13% without NH3, for o-, m-, and p-xylene, respectively. This increase was primarily attributed to the enhanced formation of secondary inorganic aerosol (SIA) in the presence of NH3, consequently increasing aerosol surface area and aerosol water content (AWC). Vapor wall losses (VWL), estimated using a kinetic method, were substantial even with the elevated aerosol surface area provided by SIA. Additional photochemical reactions in the OFR showed a gradual increase in SOA mass and yield over an atmospheric equivalent aging time of 0.5–4.0 days. In the OFR, the SOA yield increased significantly when negligible xylene remained after SC reactions. Fresh SOA formation in the OFR might have decreased the oxygen-to-carbon ratio and oxidation state of carbon, which gradually increased with increasing OFR aging. High OH radical exposure in the OFR likely caused the photodegradation of SC-formed ON, as evidenced by an abrupt decrease in the NO+/NO2+ ratio measured. This study indicates that SOA formation potential of the aromatic hydrocarbon is highly underestimated without considering the combined effects of inorganic gases along with aging.

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实验室光化学实验中形成的无机气溶胶诱发有机气溶胶形成增强
氮氧化物、二氧化硫和 NH3 等大气无机气体对二次有机气溶胶(SOA)的形成有多种影响。要全面了解 SOA 在大气中的形成过程,就必须进行全面调查。在这项研究中,我们使用由烟雾室(SC)和氧化流动反应器(OFR)组成的组合设施,考察了二甲苯异构体在无机气体存在下的光氧化过程。在较高二甲苯浓度和潮湿条件下进行的烟雾室实验显示,对于邻二甲苯、间二甲苯和对二甲苯,有 NH3 的 SOA 产量分别为 37%、39% 和 39%,而无 NH3 的 SOA 产量分别为 15%、11% 和 13%。这种增加主要归因于在 NH3 的存在下二次无机气溶胶(SIA)的形成增强,从而增加了气溶胶表面积和气溶胶含水量(AWC)。根据动力学方法估算,即使二次无机气溶胶增加了气溶胶表面积,气壁损失(VWL)仍然很大。在 0.5-4.0 天的大气等效老化时间内,OFR 中的其他光化学反应显示 SOA 的质量和产量逐渐增加。在 OFR 中,当 SC 反应后二甲苯残留量可忽略不计时,SOA 生成量会显著增加。OFR 中新 SOA 的形成可能降低了氧碳比和碳的氧化态,随着 OFR 老化时间的延长,氧碳比和碳的氧化态逐渐增加。在 OFR 中暴露于大量 OH 自由基可能会导致 SC 形成的 ON 光降解,测量到的 NO+/NO2+ 比率突然下降就是证明。这项研究表明,如果不考虑无机气体和老化的综合影响,芳香烃形成 SOA 的潜力会被严重低估。
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来源期刊
Journal of Aerosol Science
Journal of Aerosol Science 环境科学-工程:化工
CiteScore
8.80
自引率
8.90%
发文量
127
审稿时长
35 days
期刊介绍: Founded in 1970, the Journal of Aerosol Science considers itself the prime vehicle for the publication of original work as well as reviews related to fundamental and applied aerosol research, as well as aerosol instrumentation. Its content is directed at scientists working in engineering disciplines, as well as physics, chemistry, and environmental sciences. The editors welcome submissions of papers describing recent experimental, numerical, and theoretical research related to the following topics: 1. Fundamental Aerosol Science. 2. Applied Aerosol Science. 3. Instrumentation & Measurement Methods.
期刊最新文献
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