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Evolution of aqSOA from the Air–Liquid Interfacial Photochemistry of Glyoxal and Hydroxyl Radicals

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    Evolution of aqSOA from the Air–Liquid Interfacial Photochemistry of Glyoxal and Hydroxyl Radicals
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    • Fei Zhang
      Fei Zhang
      Department of Environmental Science & Engineering, Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Fudan University, Shanghai, 200433, China
      Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      More by Fei Zhang
    • Xiaofei Yu
      Xiaofei Yu
      Environmental and Molecular Science Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      More by Xiaofei Yu
    • Xiao Sui
      Xiao Sui
      Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      More by Xiao Sui
    • Jianmin Chen*
      Jianmin Chen
      Department of Environmental Science & Engineering, Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Fudan University, Shanghai, 200433, China
      Institute of Atmospheric Sciences, Fudan University, Shanghai, 200433, China
      *(J.C.) Phone: 021-6564-2298; e-mail: [email protected]
      More by Jianmin Chen
    • Zihua Zhu*
      Zihua Zhu
      Environmental and Molecular Science Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      *(Z.Z.) Phone: 1-509-371-6240; e-mail: [email protected]
      More by Zihua Zhu
      Orcidhttp://orcid.org/0000-0001-5770-8462
    • Xiao-Ying Yu*
      Xiao-Ying Yu
      Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      *(X.-Y.Y.) Phone: 1-509-372-4524; e-mail: [email protected]
      More by Xiao-Ying Yu
      Orcidhttp://orcid.org/0000-0002-9861-3109
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2019, 53, 17, 10236–10245
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    https://doi.org/10.1021/acs.est.9b03642
    Published July 30, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    The effect of photochemical reaction time on glyoxal and hydrogen peroxide at the air–liquid (a–l) interface is investigated using in situ time-of-flight secondary ion mass spectrometry (ToF–SIMS) enabled by a system for analysis at the liquid vacuum interface (SALVI) microreactor. Carboxylic acids are formed mainly by reaction with hydroxyl radicals in the initial reactions. Oligomers, cluster ions, and water clusters formed due to longer photochemistry. Our results provide direct molecular evidence that water clusters are associated with proton transfer and the formation of oligomers and cluster ions at the a–l interface. The oligomer formation is facilitated by water cluster and cluster ion formation over time. Formation of higher m/z oligomers and cluster ions indicates the possibility of highly oxygenated organic components formation at the a–l interface. Furthermore, new chemical reaction pathways, such as surface organic cluster, hydration shell, and water cluster formation, are proposed based on SIMS spectral observations, and the existing understanding of glyoxal photochemistry is expanded. Our in situ findings verify that the a–l interfacial reactions are important pathways for aqueous secondary organic aerosol (aqSOA) formation.

    Copyright © 2019 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.9b03642.

    • Seven text sections, four tables, 28 figures, and one scheme about the experimental operation procedures and additional experimental data (PDF)

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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2019, 53, 17, 10236–10245
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.9b03642
    Published July 30, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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