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

被引：135

作者：

Wang, Junfeng ^{[1
,2
]}

Ye, Jianhuai ^{[2
]}

Zhang, Qi ^{[3
]}

Zhao, Jian ^{[4
]}

Wu, Yangzhou ^{[5
]}

Li, Jingyi ^{[1
]}

Liu, Dantong ^{[5
]}

Li, Weijun ^{[5
]}

Zhang, Yange ^{[6
]}

Wu, Cheng ^{[7
]}

Xie, Conghui ^{[4
]}

Qin, Yiming ^{[2
]}

Lei, Yali ^{[2
]}

Huang, Xiangpeng ^{[1
]}

Guo, Jianping ^{[8
]}

Liu, Pengfei ^{[9
]}

Fu, Pingqing ^{[10
]}

Li, Yongjie ^{[11
]}

Lee, Hyun Chul ^{[12
]}

Choi, Hyoungwoo ^{[12
]}

Zhang, Jie ^{[13
]}

Liao, Hong ^{[1
]}

Chen, Mindong ^{[1
]}

Sun, Yele ^{[4
]}

Ge, Xinlei ^{[1
]}

Martin, Scot T. ^{[2
]}

Jacob, Daniel J. ^{[2
]}

机构：

[1] Nanjing Univ Informat Sci & Technol, Collaborat Innovat Ctr Atmospher Environm & Equip, Sch Environm Sci & Engn, Jiangsu Key Lab Atmospher Environm Monitoring & P, Nanjing 210044, Peoples R China

[2] Harvard Univ, John A Paulson Sch Engn & Appl Sci, Cambridge, MA 02138 USA

[3] Univ Calif Davis, Dept Environm Toxicol, Davis, CA 95616 USA

[4] Chinese Acad Sci, Inst Atmospher Phys, Beijing 100029, Peoples R China

[5] Zhejiang Univ, Sch Earth Sci, Dept Atmospher Sci, Hangzhou 310027, Peoples R China

[6] Minjiang Univ, Inst Oceanog, Fuzhou 350108, Peoples R China

[7] Jinan Univ, Inst Mass Spectrometry & Atmospher Environm, Guangzhou 510632, Peoples R China

[8] Chinese Acad Meteorol Sci, State Key Lab Severe Weather, Beijing 100081, Peoples R China

[9] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA

[10] Tianjin Univ, Inst Surface Earth Syst Sci, Tianjin 300072, Peoples R China

[11] Univ Macau, Fac Sci & Technol, Dept Civil & Environm Engn, Macau 999078, Peoples R China

[12] Samsung Adv Inst Technol, Gyeonggi Do 16678, Suwon Si, South Korea

[13] Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA

来源：

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA | 2021年 / 118卷 / 08期

基金：

中国国家自然科学基金;

关键词：

secondary organic aerosol; fossil-fuel combustion emissions; polycyclic aromatic hydrocarbons; aqueous-phase oxidation; BLACK CARBON; BROWN CARBON; MASS-SPECTROMETRY; VERTICAL CHARACTERIZATION; SOURCE APPORTIONMENT; OPTICAL-PROPERTIES; PHASE REACTIONS; PHOTOOXIDATION; PARTICLES; EVOLUTION;

D O I：

10.1073/pnas.2022179118

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Secondary organic aerosol (SOA) produced by atmospheric oxidation of primary emitted precursors is a major contributor to fine particulate matter (PM2.5) 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.

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页数：6

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