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

Ye-Guang Fang, Bo Tang, Chang Yuan, Zhengyi Wan, Lei Zhao, Shuang Zhu, Joseph S. Francisco (), Chongqin Zhu () and Wei-Hai Fang
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Ye-Guang Fang: Beijing Normal University
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

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-46674-1

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