Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-19-12295-2019 |
Relative humidity and O-3 concentration as two prerequisites for sulfate formation | |
Fang, Yanhua1,2; Ye, Chunxiang1,2; Wang, Junxia1,2; Wu, Yusheng1,2; Hu, Min1,2; Lin, Weili3; Xu, Fanfan1,2; Zhu, Tong1,2 | |
2019-10-02 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2019 |
卷号 | 19期号:19页码:12295-12307 |
文章类型 | Article |
语种 | 英语 |
国家 | Peoples R China |
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 similar to 45 % or an O-3 concentration threshold of similar to 35 ppb, allowing us to first introduce the idea that RH and O-3 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 O-3 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, 03, has previously been shown to be unimportant. The seasonal variations in sulfate formation could be accounted for by variations in the RH and O-3 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 O-3 (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. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000488979300006 |
WOS关键词 | HEAVY HAZE ; MULTIPHASE OXIDATION ; SECONDARY FORMATION ; EVOLUTION PROCESSES ; INORGANIC AEROSOLS ; NITROGEN-DIOXIDE ; PM2.5 ; CHEMISTRY ; POLLUTION ; CHINA |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/187570 |
专题 | 地球科学 |
作者单位 | 1.Peking Univ, Coll Environm Sci & Engn, BIC ESAT, Beijing 100871, Peoples R China; 2.Peking Univ, Coll Environm Sci & Engn, SKL ESPC, Beijing 100871, Peoples R China; 3.Minzu Univ China, Coll Life & Environm Sci, Beijing 100081, Peoples R China |
推荐引用方式 GB/T 7714 | Fang, Yanhua,Ye, Chunxiang,Wang, Junxia,et al. Relative humidity and O-3 concentration as two prerequisites for sulfate formation[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(19):12295-12307. |
APA | Fang, Yanhua.,Ye, Chunxiang.,Wang, Junxia.,Wu, Yusheng.,Hu, Min.,...&Zhu, Tong.(2019).Relative humidity and O-3 concentration as two prerequisites for sulfate formation.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(19),12295-12307. |
MLA | Fang, Yanhua,et al."Relative humidity and O-3 concentration as two prerequisites for sulfate formation".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.19(2019):12295-12307. |
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