{"title":"粒子表面和体积反应的有效质量调节模型","authors":"Pascale S. J. Lakey, Manabu Shiraiwa","doi":"10.1021/acs.jpca.6c02721","DOIUrl":null,"url":null,"abstract":"<p>Mass accommodation is a critical\r\nprocess, controlling\r\nuptake coefficients\r\nof gaseous species in aerosols and clouds. The effective mass accommodation\r\ncoefficient (α<sub>eff</sub>) was developed to account for kinetic\r\nlimitations of bulk diffusion and reactions with a simple analytical\r\nequation. In this work, α<sub>eff</sub> is extended by including\r\nsurface reactions and bulk accommodation. Systematic simulations over\r\na wide range of kinetic parameters demonstrate excellent agreement\r\nbetween the α<sub>eff</sub> method and a benchmark kinetic multilayer\r\nmodel once quasi-equilibrium is achieved in the effective penetration\r\ndepth. The α<sub>eff</sub> method can quantify the contributions\r\nof surface and bulk processes to overall uptake. Comparisons with\r\ntwo other models (Wilson et al., 2022; Prophet and Wilson, 2025) show\r\nthat the α<sub>eff</sub> method more accurately predicts uptake\r\ncoefficients when uptake is limited by bulk diffusion of volatile\r\nspecies or when surface reactions dominate under high surface coverage\r\nconditions. The developed method provides a useful tool for analyzing\r\nexperimental measurements and developing uptake parametrizations for\r\nlarge-scale models.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":"130 36","pages":"7197–7210"},"PeriodicalIF":3.0000,"publicationDate":"2026-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effective Mass Accommodation Model for Surface and Bulk Reactions in Particles\",\"authors\":\"Pascale S. J. Lakey, Manabu Shiraiwa\",\"doi\":\"10.1021/acs.jpca.6c02721\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Mass accommodation is a critical\\r\\nprocess, controlling\\r\\nuptake coefficients\\r\\nof gaseous species in aerosols and clouds. The effective mass accommodation\\r\\ncoefficient (α<sub>eff</sub>) was developed to account for kinetic\\r\\nlimitations of bulk diffusion and reactions with a simple analytical\\r\\nequation. In this work, α<sub>eff</sub> is extended by including\\r\\nsurface reactions and bulk accommodation. Systematic simulations over\\r\\na wide range of kinetic parameters demonstrate excellent agreement\\r\\nbetween the α<sub>eff</sub> method and a benchmark kinetic multilayer\\r\\nmodel once quasi-equilibrium is achieved in the effective penetration\\r\\ndepth. The α<sub>eff</sub> method can quantify the contributions\\r\\nof surface and bulk processes to overall uptake. Comparisons with\\r\\ntwo other models (Wilson et al., 2022; Prophet and Wilson, 2025) show\\r\\nthat the α<sub>eff</sub> method more accurately predicts uptake\\r\\ncoefficients when uptake is limited by bulk diffusion of volatile\\r\\nspecies or when surface reactions dominate under high surface coverage\\r\\nconditions. The developed method provides a useful tool for analyzing\\r\\nexperimental measurements and developing uptake parametrizations for\\r\\nlarge-scale models.</p>\",\"PeriodicalId\":59,\"journal\":{\"name\":\"The Journal of Physical Chemistry A\",\"volume\":\"130 36\",\"pages\":\"7197–7210\"},\"PeriodicalIF\":3.0000,\"publicationDate\":\"2026-09-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry A\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpca.6c02721\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2026/8/29 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry A","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpca.6c02721","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2026/8/29 0:00:00","PubModel":"Epub","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
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。
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.
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.