粒子表面和体积反应的有效质量调节模型

IF 3 2区 化学 Q3 CHEMISTRY, PHYSICAL
The Journal of Physical Chemistry A Pub Date : 2026-09-10 Epub Date: 2026-08-29 DOI:10.1021/acs.jpca.6c02721
Pascale S. J. Lakey, Manabu Shiraiwa
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引用次数: 0

摘要

大量调节是一个关键的过程,它控制着气溶胶和云层中气态物质的吸收系数。有效质量调节系数(αeff)用一个简单的解析方程来解释体扩散和反应的动力学限制。在这项工作中,αeff通过包括表面反应和体积调节而得到扩展。大范围动力学参数的系统模拟表明,在有效侵深达到准平衡时,α - eff方法与基准动力学多层模型具有良好的一致性。αeff方法可以量化软表面和体过程对总体吸收的贡献。与其他两种模型(Wilson et al., 2022; Prophet and Wilson, 2025)的比较表明,当吸收受到挥发性物质的大量扩散限制时,或者当表面反应在高表面覆盖条件下占主导地位时,α - eff方法更准确地预测吸收系数。所开发的方法为分析实验测量和开发大尺度模型的吸收参数化提供了有用的工具。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Effective Mass Accommodation Model for Surface and Bulk Reactions in Particles

Mass accommodation is a critical process, controlling uptake coefficients of gaseous species in aerosols and clouds. The effective mass accommodation coefficient (αeff) was developed to account for kinetic limitations of bulk diffusion and reactions with a simple analytical equation. In this work, αeff is extended by including surface reactions and bulk accommodation. Systematic simulations over a wide range of kinetic parameters demonstrate excellent agreement between the αeff method and a benchmark kinetic multilayer model once quasi-equilibrium is achieved in the effective penetration depth. The αeff method can quantify the contributions of surface and bulk processes to overall uptake. Comparisons with two other models (Wilson et al., 2022; Prophet and Wilson, 2025) show that the αeff method more accurately predicts uptake coefficients when uptake is limited by bulk diffusion of volatile species or when surface reactions dominate under high surface coverage conditions. The developed method provides a useful tool for analyzing experimental measurements and developing uptake parametrizations for large-scale models.

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来源期刊
The Journal of Physical Chemistry A
The Journal of Physical Chemistry A 化学-物理:原子、分子和化学物理
CiteScore
5.20
自引率
10.30%
发文量
922
审稿时长
1.3 months
期刊介绍: The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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