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Environ Sci Technol. 2019 Oct 7. doi: 10.1021/acs.est.9b05149. [Epub ahead of print]

Radical Formation by Fine Particulate Matter Associated with Highly Oxygenated Molecules.

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Multiphase Chemistry Department , Max Planck Institute for Chemistry , 55128 Mainz , Germany.
Institute of Inorganic and Analytical Chemistry , Johannes Gutenberg University , 55128 Mainz , Germany.
State Key Laboratory of Multiphase Flow in Power Engineering , Xi'an Jiaotong University , Xi'an 710049 , China.
School of Chemical and Biomolecular Engineering , Georgia Institute of Technology , Atlanta , Georgia 30332 , United States.
Centre for Atmospheric Science, Department of Chemistry , University of Cambridge , Cambridge CB2 1EW , United Kingdom.
Institute for Atmospheric and Earth System Research/Physics Faculty of Science , University of Helsinki , FI-00014 Helsinki , Finland.
École polytechnique fédérale de Lausanne , Lausanne 1015 , Switzerland.
School of Space and Environment , Beihang University , Beijing 100191 , China.
Physics Institute , University of São Paulo , São Paulo 05508-900 , Brazil.
Environmental Engineering Department , Federal University of Paraná , Curitiba , Paraná 81531-980 , Brazil.
Chemical Engineering Department , Federal University of Paraná , Curitiba , Paraná 81531-970 , Brazil.
School of Technology , Amazonas State University , Manaus , Amazonas 69065-020 , Brazil.
Key Laboratory of Aerosol Chemistry and Physics, State Key Laboratory of Loess and Quaternary Geology , Institute of Earth and Environment, Chinese Academy of Sciences , Xi'an , 710061 , China.
School of Geography, Earth and Environmental Sciences , University of Birmingham , Birmingham B15 2TT , United Kingdom.
Institute of Surface-Earth System Science , Tianjin University , Tianjin 300072 , China.
College of Environmental Sciences and Engineering , Peking University , Beijing 100871 , China.
Scripps Institution of Oceanography , University of California San Diego , San Diego , California 92093 , United States.
Department of Chemistry , University of California , Irvine , California 92697-2025 , United States.
Department of Environmental Sciences , University of Basel , Klingelbergstrasse 27 , 4056 Basel , Switzerland.


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.


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