气候变化领域集成服务门户(CCPortal): Heterogeneous interactions between SO2and organic peroxides in submicron aerosol

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DOI	10.5194/acp-21-6647-2021
	Heterogeneous interactions between SO2and organic peroxides in submicron aerosol
	Wang S.; Liu T.; Jang J.; Abbatt J.P.D.; Chan A.W.H.
发表日期	2021
ISSN	1680-7316
起始页码	6647
结束页码	6661
卷号	21 期号:9
英文摘要	Atmospheric models often underestimate particulate sulfate, a major component in ambient aerosol, suggesting missing sulfate formation mechanisms in the models. Heterogeneous reactions between SO2 and aerosol play an important role in particulate sulfate formation and its physicochemical evolution. Here we study the reactive uptake kinetics of SO2 onto aerosol containing organic peroxides. We present chamber studies of SO2 reactive uptake performed under different relative humidity (RH), particulate peroxide contents, peroxide types, and aerosol acidities. Using different model organic peroxides mixed with ammonium sulfate particles, the SO2 uptake coefficient ( SO2 ) was found to be exponentially dependent on RH. SO2 increases from 10-3 at RH 25% to 10-2 at RH 71% as measured for an organic peroxide with multiple O-O groups. Under similar conditions, the kinetics in this study were found to be structurally dependent: organic peroxides with multiple peroxide groups have a higher SO2 than those with only one peroxide group, consistent with the reactivity trend previously observed in the aqueous phase. In addition, SO2 is linearly related to particle-phase peroxide content, which in turn depends on gas-particle partitioning of organic peroxides. Aerosol acidity plays a complex role in determining SO2 uptake rate, influenced by the effective Henry's Law constant of SO2 and the condensed-phase kinetics of the peroxide-SO2 reaction in the highly concentrated aerosol phase. These uptake coefficients are consistently higher than those calculated from the reaction kinetics in the bulk aqueous phase, and we show experimental evidence suggesting that other factors, such as particle-phase ionic strength, can play an essential role in determining the uptake kinetics. SO2 values for different types of secondary organic aerosol (SOA) were measured to be on the order of 10-4. Overall, this study provides quantitative evidence of the multiphase reactions between SO2 and organic peroxides, highlighting the important factors that govern the uptake kinetics. © Author(s) 2021.
语种	英语
scopus关键词	aerosol; formation mechanism; reaction kinetics; relative humidity; sulfate; sulfur dioxide
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/246925
作者单位	Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, ON M5S 3E5, Canada; Department of Chemistry, University of Toronto, Toronto, ON M5S 3H6, Canada
推荐引用方式 GB/T 7714	Wang S.,Liu T.,Jang J.,et al. Heterogeneous interactions between SO2and organic peroxides in submicron aerosol[J],2021,21(9).
APA	Wang S.,Liu T.,Jang J.,Abbatt J.P.D.,&Chan A.W.H..(2021).Heterogeneous interactions between SO2and organic peroxides in submicron aerosol.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(9).
MLA	Wang S.,et al."Heterogeneous interactions between SO2and organic peroxides in submicron aerosol".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.9(2021).