Radical Formation by Fine Particulate Matter Associated with Highly Oxygenated Molecules

Author(s):Show less -

Tong, Haijie ^[1] ; Zhang, Yun ^[2] ; Filippi, Alexander ^[1] ; Wang, Ting ^{[1, 3]} ; Li, Chenpei ^{[1, 3]} ; Liu, Fobang ^{[1, 4]} ; Leppla, Denis ^[2] ; Kourtchev, Ivan ^[5] ; Wang, Kai ^{[2, 6]} ; Keskinen, Helmi-Marja ^[7] ; Levula, Janne T. ^[7] ; Arangio, Andrea M. ^{[8, 1]} ; Shen, Fangxia ^[9] ; Ditas, Florian ^[1] ; Martin, Scot T. ^{[10, 11]} ; Artaxo, Paulo ^[12] ; Godoi, Ricardo H. M. ^[13] ; Yamamoto, Carlos I. ^[14] ; de Souza, Rodrigo A. F. ^[15] ; Huang, Ru-Jin ^[16] ; Berkemeier, Thomas ^[1] ; Wang, Yueshe ^[3] ; Su, Hang ^[1] ; Cheng, Yafang ^[1] ; Pope, Francis D. ^[17] ; Fu, Pingqing ^[18] ; Yao, Maosheng ^[19] ; Poehlker, Christopher ^[1] ; Petaja, Tuukka ^[7] ; Kulmala, Markku ^[7] ; Andreae, Meinrat O. ^{[1, 20]} ; Shiraiwa, Manabu ^[21] ; Poeschl, Ulrich ^[1] ; Hoffmann, Thorsten ^[2] ; Kalberer, Markus ^{[5, 22]}

Affiliation:Show less -

^[1] Max Planck Inst Chem, Multiphase Chem Dept, D-55128 Mainz - Germany

^[2] Johannes Gutenberg Univ Mainz, Inst Inorgan & Analyt Chem, D-55128 Mainz - Germany

^[3] Xi An Jiao Tong Univ, State Key Lab Multiphase Flow Power Engn, Xian 710049, Shaanxi - Peoples R China

^[4] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 - USA

^[5] Univ Cambridge, Ctr Atmospher Sci, Dept Chem, Cambridge CB2 1EW - England

^[6] Aarhus Univ, Dept Chem, Langelandsgade 140, DK-8000 Aarhus - Denmark

^[7] Univ Helsinki, Phys Fac Sci, Inst Atmospher & Earth Syst Res, FI-00014 Helsinki - Finland

^[8] Ecole Polytech Fed Lausanne, CH-1015 Lausanne - Switzerland

^[9] Beihang Univ, Sch Space & Environm, Beijing 100191 - Peoples R China

^[10] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 - USA

^[11] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 - USA

^[12] Univ Sao Paulo, Phys Inst, BR-05508900 Sao Paulo - Brazil

^[13] Univ Fed Parana, Environm Engn Dept, BR-81531980 Curitiba, Parana - Brazil

^[14] Univ Fed Parana, Chem Engn Dept, BR-81531970 Curitiba, Parana - Brazil

^[15] Amazonas State Univ, Sch Technol, BR-69065020 Manaus, Amazonas - Brazil

^[16] Chinese Acad Sci, Inst Earth & Environm, State Key Lab Loess & Quaternary Geol, Key Lab Aerosol Chem & Phys, Xian 710061, Shaanxi - Peoples R China

^[17] Univ Birmingham, Sch Geog Earth & Environm Sci, Birmingham B15 2TT, W Midlands - England

^[18] Tianjin Univ, Inst Surface Earth Syst Sci, Tianjin 300072 - Peoples R China

^[19] Peking Univ, Coll Environm Sci & Engn, Beijing 100871 - Peoples R China

^[20] Univ Calif San Diego, Scripps Inst Oceanog, San Diego, CA 92093 - USA

^[21] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 - USA

^[22] Univ Basel, Dept Environm Sci, Klingelbergstr 27, CH-4056 Basel - Switzerland

• Document type: Journal article
• Source: Environmental Science & Technology; v. 53, n. 21, p. 12506-12518, NOV 5 2019.
• Web of Science Citations: 2

Abstract

Highly oxygenated molecules (HOMs) play an important role in the formation and evolution of secondary organic aerosols (SOA). However, the abundance of HOMs in different environments and their relation to the oxidative potential of fine particulate matter (PM) are largely unknown. Here, we investigated the relative HOM abundance and radical yield of laboratory-generated SOA and fine PM in ambient air ranging from remote forest areas to highly polluted megacities. By electron paramagnetic resonance and mass spectrometric investigations, we found that the relative abundance of HOMs, especially the dimeric and low-volatility types, in ambient fine PM was positively correlated with the formation of radicals in aqueous PM extracts. SOA from photooxidation of isoprene, ozonolysis of alpha- and beta-pinene, and fine PM from tropical (central Amazon) and boreal (Hyytiala, Finland) forests exhibited a higher HOM abundance and radical yield than SOA from photooxidation of naphthalene and fine PM from urban sites (Beijing, Guangzhou, Mainz, Shanghai, and Xian), confirming that HOMs are important constituents of biogenic SOA to generate radicals. Our study provides new insights into the chemical relationship of HOM abundance, composition, and sources with the yield of radicals by laboratory and ambient aerosols, enabling better quantification of the component-specific contribution of source- or site-specific fine PM to its climate and health effects. (AU)

• FAPESP's process: 17/17047-0 - Aerosol and clouds life cycles in Amazonia: biogenic emissions, biomass burning and impacts on ecosystem
• Grantee: Paulo Eduardo Artaxo Netto
• Support Opportunities: Research Program on Global Climate Change - Thematic Grants