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DOI	10.5194/acp-19-12295-2019
	Relative humidity and O3 concentration as two prerequisites for sulfate formation
	Fang Y.; Ye C.; Wang J.; Wu Y.; Hu M.; Lin W.; Xu F.; Zhu T.
发表日期	2019
ISSN	16807316
起始页码	12295
结束页码	12307
卷号	19 期号:19
英文摘要	Sulfate formation mechanisms have been discussed extensively but are still disputed. In this work, a yearlong particulate matter (PM2:5) sampling campaign was conducted together with measurements of gaseous pollutant concentrations and meteorological parameters in Beijing, China, from March 2012 to February 2013. The sulfur oxidation ratio (SOR), an indicator of secondary sulfate formation, displayed a clear summer peak and winter valley, even though no obvious seasonal variations in sulfate mass concentration were observed. A rapid rise in the SOR was found at a relative humidity (RH) threshold of ∼ 45% or an O3 concentration threshold of ∼ 35 ppb, allowing us to first introduce the idea that RH and O3 concentrations are two prerequisites for rapid sulfate formation via multiphase reactions. In the case of the RH threshold, this is consistent with current understanding of the multiphase formation of sulfate, since it relates to the semisolid-To-liquid phase transition of atmospheric aerosols. Correlation analysis between SOR and aerosol water content (AWC) further backed this up. In the case of the O3 concentration threshold, this is consistent with the consumption of liquid oxidants in multiphase sulfate formation. The thresholds introduced here lead us to a better understanding of the sulfate formation mechanisms and sulfate formation variations. H2O2 might be the major oxidant of sulfate formation, since another liquid-phase oxidant, O3, has previously been shown to be unimportant. The seasonal variations in sulfate formation could be accounted for by variations in the RH and O3 prerequisites. For example, over the year-long study, the fastest SO2-To-sulfate conversion occurred in summer, which was associated with the highest values of O3 (and also H2O2) concentration and RH. The SOR also displayed variations with pollution levels; i.e.The SOR increased with PM2:5 in all seasons. Such variations were primarily associated with a transition from the slow gas-phase formation of sulfate to rapid multiphase reactions, since RH increased higher than its prerequisite value of around 45% as pollution evolved. In addition, the selfcatalytic nature of sulfate formation (i.e.The formation of hydrophilic sulfate aerosols under high RH conditions results in an increase in aerosol water content, which results in greater particle volume for further multiphase sulfate formation) also contributed to variations among the pollution scenarios. © 2019 Copernicus GmbH. All rights reserved.
语种	英语
scopus关键词	aerosol; atmospheric pollution; concentration (composition); formation mechanism; ozone; pollutant; pollution monitoring; relative humidity; seasonal variation; sulfate; threshold; water content
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/144122
作者单位	BIC-ESAT and SKL-ESPC, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China; College of Life and Environmental Sciences, Minzu University of China, Beijing, 100081, China
推荐引用方式 GB/T 7714	Fang Y.,Ye C.,Wang J.,et al. Relative humidity and O3 concentration as two prerequisites for sulfate formation[J],2019,19(19).
APA	Fang Y..,Ye C..,Wang J..,Wu Y..,Hu M..,...&Zhu T..(2019).Relative humidity and O3 concentration as two prerequisites for sulfate formation.Atmospheric Chemistry and Physics,19(19).
MLA	Fang Y.,et al."Relative humidity and O3 concentration as two prerequisites for sulfate formation".Atmospheric Chemistry and Physics 19.19(2019).