Aqueous production of secondary organic aerosol from fossil-fuel emissions in winter Beijing haze

Junfeng Wang; Jianhuai Ye; Qi Zhang; Jian Zhao; Yangzhou Wu; Jingyi Li; Dantong Liu; Weijun Li; Yange Zhang; Cheng Wu; Conghui Xie; Yiming Qin; Yali Lei; Xiangpeng Huang; Jianping Guo; Pengfei Liu; Pingqing Fu; Yongjie Li; Hyun Chul Lee; Hyoungwoo Choi; Jie Zhang; Hong Liao; Mindong Chen; Yele Sun; Xinlei Ge; Scot T Martin; Daniel J Jacob

doi:10.1073/pnas.2022179118

Aqueous production of secondary organic aerosol from fossil-fuel emissions in winter Beijing haze

Proc Natl Acad Sci U S A. 2021 Feb 23;118(8):e2022179118. doi: 10.1073/pnas.2022179118.

Authors

Junfeng Wang^{1

2}, Jianhuai Ye², Qi Zhang³, Jian Zhao⁴, Yangzhou Wu⁵, Jingyi Li¹, Dantong Liu⁵, Weijun Li⁵, Yange Zhang⁶, Cheng Wu⁷, Conghui Xie⁴, Yiming Qin², Yali Lei², Xiangpeng Huang¹, Jianping Guo⁸, Pengfei Liu⁹, Pingqing Fu¹⁰, Yongjie Li¹¹, Hyun Chul Lee¹², Hyoungwoo Choi¹², Jie Zhang¹³, Hong Liao¹, Mindong Chen¹, Yele Sun⁴, Xinlei Ge¹⁴, Scot T Martin², Daniel J Jacob¹⁵

Affiliations

¹ Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China.
² John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138.
³ Department of Environmental Toxicology, University of California, Davis, CA 95616.
⁴ Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China.
⁵ Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, Hangzhou 310027, China.
⁶ Institute of Oceanography, Minjiang University, Fuzhou 350108, China.
⁷ Institute of Mass Spectrometry and Atmospheric Environment, Jinan University, Guangzhou 510632, China.
⁸ State Key Laboratory of Severe Weather, Chinese Academy of Meteorological Sciences, Beijing 100081, China.
⁹ School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332.
¹⁰ Institute of Surface-Earth System Science, Tianjin University, Tianjin 300072, China.
¹¹ Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Macau 999078, China.
¹² Samsung Advance Institute of Technology, Gyeonggi-do, Suwon-si 16678, Republic of Korea.
¹³ Department of Atmospheric Science, Colorado State University, Fort Collins, CO 80523.
¹⁴ Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China; caxinra@163.com djacob@fas.harvard.edu.
¹⁵ John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138; caxinra@163.com djacob@fas.harvard.edu.

Abstract

Secondary organic aerosol (SOA) produced by atmospheric oxidation of primary emitted precursors is a major contributor to fine particulate matter (PM_2.5) air pollution worldwide. Observations during winter haze pollution episodes in urban China show that most of this SOA originates from fossil-fuel combustion but the chemical mechanisms involved are unclear. Here we report field observations in a Beijing winter haze event that reveal fast aqueous-phase conversion of fossil-fuel primary organic aerosol (POA) to SOA at high relative humidity. Analyses of aerosol mass spectra and elemental ratios indicate that ring-breaking oxidation of POA aromatic species, leading to functionalization as carbonyls and carboxylic acids, may serve as the dominant mechanism for this SOA formation. A POA origin for SOA could explain why SOA has been decreasing over the 2013-2018 period in response to POA emission controls even as emissions of volatile organic compounds (VOCs) have remained flat.

Keywords: aqueous-phase oxidation; fossil-fuel combustion emissions; polycyclic aromatic hydrocarbons; secondary organic aerosol.

Publication types

Research Support, Non-U.S. Gov't