Radical Formation by Fine Particulate Matter Associated with Highly Oxygenated Molecules

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 investiga...

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Bibliographic Details
Published in:	Environmental science & technology Vol. 53; no. 21; pp. 12506 - 12518
Main Authors:	Tong, Haijie, Zhang, Yun, Filippi, Alexander, Wang, Ting, Li, Chenpei, Liu, Fobang, Leppla, Denis, Kourtchev, Ivan, Wang, Kai, Keskinen, Helmi-Marja, Levula, Janne T, Arangio, Andrea M, Shen, Fangxia, Ditas, Florian, Martin, Scot T, Artaxo, Paulo, Godoi, Ricardo H. M, Yamamoto, Carlos I, de Souza, Rodrigo A. F, Huang, Ru-Jin, Berkemeier, Thomas, Wang, Yueshe, Su, Hang, Cheng, Yafang, Pope, Francis D, Fu, Pingqing, Yao, Maosheng, Pöhlker, Christopher, Petäjä, Tuukka, Kulmala, Markku, Andreae, Meinrat O, Shiraiwa, Manabu, Pöschl, Ulrich, Hoffmann, Thorsten, Kalberer, Markus
Format:	Journal Article
Language:	English
Published:	Easton American Chemical Society 05-11-2019 American Chemical Society (ACS)
Subjects:	Abundance Aerosols aromatic compounds atmospheric chemistry Climate effects Electron paramagnetic resonance Forests INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Isoprene Laboratories Naphthalene Organic chemistry oxides Oxygenation Particulate emissions Particulate matter Particulates Photooxidation Pinene Radicals Relative abundance Spectrometry Tropical forests Urban areas Volatility Yield
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Summary:	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 α- and β-pinene, and fine PM from tropical (central Amazon) and boreal (Hyytiälä, 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 Xi’an), 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.
Bibliography:	SC0006680 USDOE Office of Science (SC), Biological and Environmental Research (BER)
ISSN:	0013-936X 1520-5851
DOI:	10.1021/acs.est.9b05149