Radical Formation by Fine Particulate Matter Associated with Highly Oxygenated Molecules

H. Tong, Y. Zhang, A. Filippi, T. Wang, C. Li, F. Liu, D. Leppla, I. Kourtchev, K. Wang, H.-M. Keskinen, J.T. Levula, A.M. Arangio, F. Shen, F. Ditas, S.T. Martin, P. Artaxo, R.H.M. Godoi, C.I. Yamamoto, R.A.F. De Souza, R.-J. HuangT. Berkemeier, Y. Wang, H. Su, Y. Cheng, F.D. Pope, P. Fu, Maosheng Yao, C. Pöhlker, T. Petäjä, M. Kulmala, M.O. Andreae, M. Shiraiwa, U. Pöschl, T. Hoffmann, M. Kalberer

Research output: Contribution to journalArticle

8 Citations (Scopus)

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 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.
Original languageEnglish
Pages (from-to)12506–12518
Number of pages13
JournalEnvironmental Science and Technology
Volume53
Issue number21
Early online date19 Sep 2019
DOIs
Publication statusPublished - 5 Nov 2019
Externally publishedYes

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    Tong, H., Zhang, Y., Filippi, A., Wang, T., Li, C., Liu, F., ... Kalberer, M. (2019). Radical Formation by Fine Particulate Matter Associated with Highly Oxygenated Molecules. Environmental Science and Technology, 53(21), 12506–12518. https://doi.org/10.1021/acs.est.9b05149