Fast sulfate formation from oxidation of SO2 by NO2 and HONO observed in Beijing haze

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作者
Junfeng Wang
Jingyi Li
Jianhuai Ye
Jian Zhao
Yangzhou Wu
Jianlin Hu
Dantong Liu
Dongyang Nie
Fuzhen Shen
Xiangpeng Huang
Dan Dan Huang
Dongsheng Ji
Xu Sun
Weiqi Xu
Jianping Guo
Shaojie Song
Yiming Qin
Pengfei Liu
Jay R. Turner
Hyun Chul Lee
Sungwoo Hwang
Hong Liao
Scot T. Martin
Qi Zhang
Mindong Chen
Yele Sun
Xinlei Ge
Daniel J. Jacob
机构
[1] Nanjing University of Information Science and Technology,Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, School of Environmental Science and Engineering
[2] Harvard University,John A. Paulson School of Engineering and Applied Sciences
[3] Chinese Academy of Sciences,State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics
[4] Zhejiang University,Department of Atmospheric Sciences, School of Earth Sciences
[5] Nanjing University,School of Atmospheric Sciences
[6] Shanghai Academy of Environmental Sciences,State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex
[7] Chinese Academy of Sciences,State Key Laboratory of Urban and Regional Ecology Research Center for Eco
[8] Chinese Academy of Meteorological Sciences,Environmental Sciences
[9] Washington University in Saint Louis,State Key Laboratory of Severe Weather
[10] Samsung Advanced Institute of Technology,Department of Energy, Environmental and Chemical Engineering
[11] University of California Davis,Department of Environmental Toxicology
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摘要
Severe events of wintertime particulate air pollution in Beijing (winter haze) are associated with high relative humidity (RH) and fast production of particulate sulfate from the oxidation of sulfur dioxide (SO2) emitted by coal combustion. There has been considerable debate regarding the mechanism for SO2 oxidation. Here we show evidence from field observations of a haze event that rapid oxidation of SO2 by nitrogen dioxide (NO2) and nitrous acid (HONO) takes place, the latter producing nitrous oxide (N2O). Sulfate shifts to larger particle sizes during the event, indicative of fog/cloud processing. Fog and cloud readily form under winter haze conditions, leading to high liquid water contents with high pH (>5.5) from elevated ammonia. Such conditions enable fast aqueous-phase oxidation of SO2 by NO2, producing HONO which can in turn oxidize SO2 to yield N2O.This mechanism could provide an explanation for sulfate formation under some winter haze conditions.
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