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Uptake of N2O5 by aqueous aerosol unveiled using chemically accurate many-body potentials

Author

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  • Vinícius Wilian D. Cruzeiro

    (University of California San Diego
    University of California San Diego)

  • Mirza Galib

    (University of California)

  • David T. Limmer

    (University of California
    Kavli Energy NanoScience Institute
    Lawrence Berkeley National Laboratory
    Lawrence Berkeley National Laboratory)

  • Andreas W. Götz

    (University of California San Diego)

Abstract

The reactive uptake of N2O5 to aqueous aerosol is a major loss channel for nitrogen oxides in the troposphere. Despite its importance, a quantitative picture of the uptake mechanism is missing. Here we use molecular dynamics simulations with a data-driven many-body model of coupled-cluster accuracy to quantify thermodynamics and kinetics of solvation and adsorption of N2O5 in water. The free energy profile highlights that N2O5 is selectively adsorbed to the liquid–vapor interface and weakly solvated. Accommodation into bulk water occurs slowly, competing with evaporation upon adsorption from gas phase. Leveraging the quantitative accuracy of the model, we parameterize and solve a reaction–diffusion equation to determine hydrolysis rates consistent with experimental observations. We find a short reaction–diffusion length, indicating that the uptake is dominated by interfacial features. The parameters deduced here, including solubility, accommodation coefficient, and hydrolysis rate, afford a foundation for which to consider the reactive loss of N2O5 in more complex solutions.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28697-8
    DOI: 10.1038/s41467-022-28697-8
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    References listed on IDEAS

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    1. Ben D. MacArthur & Richard O. C. Oreffo, 2005. "Bridging the gap," Nature, Nature, vol. 433(7021), pages 19-19, January.
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    Cited by:

    1. 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.

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