Persistent sulfate formation from London Fog to Chinese haze

Gehui Wang1,2,3,4,5, Renyi Zhang1,2,6, Mario Gómez1,7,2, Lingxiao Yang1,8, Misti Levy Zamora1, Min Hu6, Yun Lin9,1, Jianfei Peng1,6, Song Guo1,6, Jingjing Meng10,3,5,11, Jianjun Li3,5, Chunlei Cheng3,5,11, Tafeng Hu9,3,12, Yanqin Ren3,5,11, Yuesi Wang13,3,5, Jian Gao14, Junji Cao3,5, Zhisheng An15,3,5, Weijian Zhou3,5,16, Guohui Li3,5, Jiayuan Wang3,5,11, Pengfei Tian1,17, Wilmarie Marrero-Ortiz1,2, Jeremiah Secrest1,2, Zhuofei Du6, Jing Zheng6, Dongjie Shang6, Limin Zeng6, Min Shao6, Weigang Wang18,19,1,20, Yao Huang3,5,11, Yuan Wang21, Yujiao Zhu1,22, Yixin Li1, Jiaxi Hu9,1, Bowen Pan1, Cai Li1,23, Yu-Ting Cheng10,3,5,11, Yuemeng Ji24, Fang Zhang15,1, Daniel Rosenfeld1,25, Peter S. Liss1,26, Robert A. Duce1, C. E. Kolb27,1, Mario J. Molina10,28
1Department of Atmospheric Sciences, Texas A&M University, College Station, TX 77843;
2Department of Chemistry, Texas A&M University, College Station, TX 77840;
3Key Laboratory of Aerosol Chemistry and Physics, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an, 710061, China
4School of Geographic Sciences, East China Normal University, Shanghai 200062, China
5State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China
6State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
7Department of Chemistry and Biochemistry, Florida International University, Miami, FL 33199;
8School of Environmental Science and Engineering, Shandong University, Jinan 250100, China
9Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, China
10Department of Atmospheric Sciences, Texas A&M University, College Station, TX 77843;
11University of Chinese Academy of Sciences, Beijing, 100049, China
12University of Maryland; and S.M., National Center for Atmospheric Research.
13Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China
14Chinese Research Academy of Environmental Sciences, Beijing 100000, China;
15Beijing Normal University, Beijing 100875, China
16Xi'an Jiaotong University, Xi'an, 710049, China
17Key Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, China
18Beijing National Laboratory for Molecular Sciences
19Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
20State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
21Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91125;
22Key Laboratory of Marine Environmental Science and Ecology, Ministry of Education, Ocean University of China, Qingdao, 266100, China
23School of Electrical Engineering, Wuhan University, Wuhan 430072, China
24School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou 510006, China
25Program of Atmospheric Sciences, Institute of Earth Sciences, The Hebrew University of Jerusalem, Jerusalem 91904, Israel;
26School of Environmental Sciences, University of East Anglia, Norwich NR4 7TJ, United Kingdom
27Aerodyne Research, Inc., Billerica, MA 01821-3976;
28Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093

Tóm tắt

Significance Exceedingly high levels of fine particulate matter (PM) occur frequently in China, but the mechanism of severe haze formation remains unclear. From atmospheric measurements in two Chinese megacities and laboratory experiments, we show that the oxidation of SO 2 by NO 2 occurs efficiently in aqueous media under two polluted conditions: first, during the formation of the 1952 London Fog via in-cloud oxidation; and second, on fine PM with NH 3 neutralization during severe haze in China. We suggest that effective haze mitigation is achievable by intervening in the sulfate formation process with NH 3 and NO 2 emission control measures. Hence, our results explain the outstanding sulfur problem during the historic London Fog formation and elucidate the chemical mechanism of severe haze in China.

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