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

被引：145

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.

引用

页数：6

共 59 条

[1] Secondary organic aerosols from aromatic hydrocarbons and their contribution to fine particulate matter in Atlanta, Georgia
Al-Naiema, Ibrahim M.
Offenberg, John H.
Madler, Carter J.
Lewandowski, Michael
Kettler, Josh
Fang, Ting
Stone, Elizabeth A.
[J]. ATMOSPHERIC ENVIRONMENT, 2020, 223
[2] Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications
Canagaratna, M. R.
Jimenez, J. L.
Kroll, J. H.
Chen, Q.
Kessler, S. H.
Massoli, P.
Hildebrandt Ruiz, L.
Fortner, E.
Williams, L. R.
Wilson, K. R.
Surratt, J. D.
Donahue, N. M.
Jayne, J. T.
Worsnop, D. R.
[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2015, 15 (01) : 253 - 272
[3] Chemical Compositions of Black Carbon Particle Cores and Coatings via Soot Particle Aerosol Mass Spectrometry with Photoionization and Electron Ionization
Canagaratna, Manjula R.
Massoli, Paola
Browne, Eleanor C.
Franklin, Jonathan P.
Wilson, Kevin R.
Onasch, Timothy B.
Kirchstetter, Thomas W.
Fortner, Edward C.
Kolb, Charles E.
Jayne, John T.
Kroll, Jesse H.
Worsnop, Douglas R.
[J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2015, 119 (19) : 4589 - 4599
[4] Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: implications for oxidation of intermediate volatility organic compounds (IVOCs)
Chan, A. W. H.
Kautzman, K. E.
Chhabra, P. S.
Surratt, J. D.
Chan, M. N.
Crounse, J. D.
Kuerten, A.
Wennberg, P. O.
Flagan, R. C.
Seinfeld, J. H.
[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (09) : 3049 - 3060
[5] SOA formation from photooxidation of naphthalene and methylnaphthalenes with m-xylene and surrogate mixtures
Chen, Chia-Li
Li, Lijie
Tang, Ping
Cocker, David R., III
[J]. ATMOSPHERIC ENVIRONMENT, 2018, 180 : 256 - 264
[6] The "dual-spot" Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation
Drinovec, L.
Mocnik, G.
Zotter, P.
Prevot, A. S. H.
Ruckstuhl, C.
Coz, E.
Rupakheti, M.
Sciare, J.
Mueller, T.
Wiedensohler, A.
Hansen, A. D. A.
[J]. ATMOSPHERIC MEASUREMENT TECHNIQUES, 2015, 8 (05) : 1965 - 1979
[7] Detection of particle-phase polycyclic aromatic hydrocarbons in Mexico City using an aerosol mass spectrometer
Dzepina, Katja
Arey, Janet
Marr, Linsey C.
Worsnop, Douglas R.
Salcedo, Dara
Zhang, Qi
Onasch, Timothy B.
Molina, Luisa T.
Molina, Mario J.
Jimenez, Jose L.
[J]. INTERNATIONAL JOURNAL OF MASS SPECTROMETRY, 2007, 263 (2-3) : 152 - 170
[8] Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies
Ervens, B.
Turpin, B. J.
Weber, R. J.
[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (21) : 11069 - 11102
[9] Evolution of brown carbon in wildfire plumes
Forrister, Haviland
Liu, Jiumeng
Scheuer, Eric
Dibb, Jack
Ziemba, Luke
Thornhill, Kenneth L.
Anderson, Bruce
Diskin, Glenn
Perring, Anne E.
Schwarz, Joshua P.
Campuzano-Jost, Pedro
Day, Douglas A.
Palm, Brett B.
Jimenez, Jose L.
Nenes, Athanasios
Weber, Rodney J.
[J]. GEOPHYSICAL RESEARCH LETTERS, 2015, 42 (11) : 4623 - 4630
[10] Primary and secondary organic aerosols in Fresno, California during wintertime: Results from high resolution aerosol mass spectrometry
Ge, Xinlei
Setyan, Ari
Sun, Yele
Zhang, Qi
[J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2012, 117

← 1 2 3 4 5 6 →