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Mechanistic insight into the competition between interfacial and bulk reactions in microdroplets through N2O5 ammonolysis and hydrolysis

Author

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  • Ye-Guang Fang

    (Beijing Normal University
    National Centre for Nanoscience and Technology)

  • Bo Tang

    (Beijing Normal University)

  • Chang Yuan

    (Beijing Normal University)

  • Zhengyi Wan

    (University of Pennsylvania)

  • Lei Zhao

    (Beijing Normal University)

  • Shuang Zhu

    (Beijing Normal University)

  • Joseph S. Francisco

    (University of Pennsylvania)

  • Chongqin Zhu

    (Beijing Normal University)

  • Wei-Hai Fang

    (Beijing Normal University)

Abstract

Reactive uptake of dinitrogen pentaoxide (N2O5) into aqueous aerosols is a major loss channel for NOx in the troposphere; however, a quantitative understanding of the uptake mechanism is lacking. Herein, a computational chemistry strategy is developed employing high-level quantum chemical methods; the method offers detailed molecular insight into the hydrolysis and ammonolysis mechanisms of N2O5 in microdroplets. Specifically, our calculations estimate the bulk and interfacial hydrolysis rates to be (2.3 ± 1.6) × 10−3 and (6.3 ± 4.2) × 10−7 ns−1, respectively, and ammonolysis competes with hydrolysis at NH3 concentrations above 1.9 × 10−4 mol L−1. The slow interfacial hydrolysis rate suggests that interfacial processes have negligible effect on the hydrolysis of N2O5 in liquid water. In contrast, N2O5 ammonolysis in liquid water is dominated by interfacial processes due to the high interfacial ammonolysis rate. Our findings and strategy are applicable to high-chemical complexity microdroplets.

Suggested Citation

  • Ye-Guang Fang & Bo Tang & Chang Yuan & Zhengyi Wan & Lei Zhao & Shuang Zhu & Joseph S. Francisco & Chongqin Zhu & Wei-Hai Fang, 2024. "Mechanistic insight into the competition between interfacial and bulk reactions in microdroplets through N2O5 ammonolysis and hydrolysis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46674-1
    DOI: 10.1038/s41467-024-46674-1
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    1. Vinícius Wilian D. Cruzeiro & Mirza Galib & David T. Limmer & Andreas W. Götz, 2022. "Uptake of N2O5 by aqueous aerosol unveiled using chemically accurate many-body potentials," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
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