气候变化领域集成服务门户(CCPortal): A More Important Role for the Ozone-S(IV) Oxidation Pathway Due to Decreasing Acidity in Clouds

CCPortal

DOI	10.1029/2020JD033220
	A More Important Role for the Ozone-S(IV) Oxidation Pathway Due to Decreasing Acidity in Clouds
	Li J.; Zhu C.; Chen H.; Fu H.; Xiao H.; Wang X.; Herrmann H.; Chen J.
发表日期	2020
ISSN	2169897X
卷号	125 期号:18
英文摘要	Clouds significantly affect the Earth's radiation budget and play a critical role in atmospheric sulfate formation. The pathways of S(IV) oxidations have recently caused a controversial attention under severe haze episodes due to the variable acidity and water content in aerosol particles. In this study, a total of 158 cloud samples were collected from 2014 to 2018 at the summit of Mt. Tai, China, to explore the roles of atmospheric oxidants in aqueous S(IV) oxidation. The results showed that the averaged pH value of cloud water increased dramatically from 3.86 (Guo et al., 2012, https://doi.org/10.1016/j.atmosenv.2012.07.016) in 2007–2008, ~5.5 in 2014, to ~6.4 in 2018, respectively, while water soluble secondary ions (SO42−, NO3− and NH4+) and S(IV) decreased significantly. The four pathways of S(IV) oxidation by O3, H2O2, NO2, and trace metal-catalyzed autooxidation were further discussed, and the roles in S(IV) oxidation pathways were found changing significantly with pH value in clouds. The rate of H2O2 pathway contributed about 95.8% for S(IV) oxidation when pH was less than 4.0. For pH around 5.0, the rate of O3 pathway became comparable with the H2O2 pathway, and it accounted more than 95.2% for the total S(IV) oxidation rate when pH was larger than 6.0. Based on the long-term field measurement, this study indicated that the high concentration of O3 and the increasing trend of pH promoted a shift of the dominant S(IV) oxidation from H2O2 pathway in a previous study (Shen et al., 2012, https://doi.org/10.1016/j.atmosenv.2012.07.079) to O3 pathway in clouds. ©2020. American Geophysical Union. All Rights Reserved.
语种	英语
来源期刊	Journal of Geophysical Research: Atmospheres
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/185738
作者单位	Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan Tyndall Centre, Institute of Atmospheric Sciences, Fudan University, Shanghai, China; Center for Excellence in Urban Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Science, Xiamen, China; School of Environmental Science and Engineering, Shandong University, Qingdao, China; Atmospheric Chemistry Department (ACD), Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany; Shanghai Institute of Eco-Chongming (SIEC), Shanghai, China
推荐引用方式 GB/T 7714	Li J.,Zhu C.,Chen H.,et al. A More Important Role for the Ozone-S(IV) Oxidation Pathway Due to Decreasing Acidity in Clouds[J],2020,125(18).
APA	Li J..,Zhu C..,Chen H..,Fu H..,Xiao H..,...&Chen J..(2020).A More Important Role for the Ozone-S(IV) Oxidation Pathway Due to Decreasing Acidity in Clouds.Journal of Geophysical Research: Atmospheres,125(18).
MLA	Li J.,et al."A More Important Role for the Ozone-S(IV) Oxidation Pathway Due to Decreasing Acidity in Clouds".Journal of Geophysical Research: Atmospheres 125.18(2020).