Sulfate formation is dominated by manganese-catalyzed oxidation of SO2 on aerosol surfaces during haze events

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作者
Weigang Wang
Mingyuan Liu
Tiantian Wang
Yu Song
Li Zhou
Junji Cao
Jingnan Hu
Guigang Tang
Zhe Chen
Zhijie Li
Zhenying Xu
Chao Peng
Chaofan Lian
Yan Chen
Yuepeng Pan
Yunhong Zhang
Yele Sun
Weijun Li
Tong Zhu
Hezhong Tian
Maofa Ge
机构
[1] Chinese Academy of Sciences,State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistr
[2] University of Chinese Academy of Sciences,State Key Joint Laboratory of Environmental Simulation and Pollution Control, Department of Environmental Science
[3] Peking University,Key Laboratory of Aerosol Chemistry and Physics, State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment
[4] Chinese Academy of Sciences,The Institute of Chemical Physics, School of Chemistry and Chemical Engineering
[5] Institute of Atmospheric Environment,State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics
[6] Chinese Research Academy of Environmental Sciences,Department of Atmospheric Sciences, School of Earth Sciences
[7] State Environmental Protection Key Laboratory of Quality Control in Environmental Monitoring,State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment
[8] China National Environmental Monitoring Centre,undefined
[9] Beijing Institute of Technology,undefined
[10] Chinese Academy of Sciences,undefined
[11] Zhejiang University,undefined
[12] Beijing Normal University,undefined
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摘要
The formation mechanism of aerosol sulfate during wintertime haze events in China is still largely unknown. As companions, SO2 and transition metals are mainly emitted from coal combustion. Here, we argue that the transition metal-catalyzed oxidation of SO2 on aerosol surfaces could be the dominant sulfate formation pathway and investigate this hypothesis by integrating chamber experiments, numerical simulations and in-field observations. Our analysis shows that the contribution of the manganese-catalyzed oxidation of SO2 on aerosol surfaces is approximately one to two orders of magnitude larger than previously known routes, and contributes 69.2% ± 5.0% of the particulate sulfur production during haze events. This formation pathway could explain the missing source of sulfate and improve the understanding of atmospheric chemistry and climate change.
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