气候变化领域集成服务门户(CCPortal): Mass accommodation and gas-particle partitioning in secondary organic aerosols: Dependence on diffusivity; volatility; particle-phase reactions; and penetration depth

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DOI	10.5194/acp-21-1565-2021
	Mass accommodation and gas-particle partitioning in secondary organic aerosols: Dependence on diffusivity; volatility; particle-phase reactions; and penetration depth
	Shiraiwa M.; Pöschl U.
发表日期	2021
ISSN	1680-7316
起始页码	1565
结束页码	1580
卷号	21 期号:3
英文摘要	Mass accommodation is an essential process for gas particle partitioning of organic compounds in secondary organic aerosols (SOA). The mass accommodation coefficient is commonly described as the probability of a gas molecule colliding with the surface to enter the particle phase. It is often applied, however, without specifying if and how deep a molecule has to penetrate beneath the surface to be regarded as being incorporated into the condensed phase (adsorption vs. absorption). While this aspect is usually not critical for liquid particles with rapid surface bulk exchange, it can be important for viscous semi-solid or glassy solid particles to distinguish and resolve the kinetics of accommodation at the surface, transfer across the gas particle interface, and further transport into the particle bulk. For this purpose, we introduce a novel parameter: An effective mass accommodation coefficient eff that depends on penetration depth and is a function of surface accommodation coefficient, volatility, bulk diffusivity, and particlephase reaction rate coefficient. Application of eff in the traditional Fuchs Sutugin approximation of mass-Transport kinetics at the gas particle interface yields SOA partitioning results that are consistent with a detailed kinetic multilayer model (kinetic multilayer model of gas particle interactions in aerosols and clouds, KM-GAP; Shiraiwa et al., 2012) and two-film model solutions (Model for Simulating Aerosol Interactions and Chemistry, MOSAIC; Zaveri et al., 2014) but deviate substantially from earlier modeling approaches not considering the influence of penetration depth and related parameters. For highly viscous or semi-solid particles, we show that the effective mass accommodation coefficient remains similar to the surface accommodation coefficient in the case of low-volatility compounds, whereas it can decrease by several orders of magnitude in the case of semi-volatile compounds. Such effects can explain apparent inconsistencies between earlier studies deriving mass accommodation coefficients from experimental data or from molecular dynamics simulations. Our findings challenge the approach of traditional SOA models using the Fuchs Sutugin approximation of mass transfer kinetics with a fixed mass accommodation coefficient, regardless of particle phase state and penetration depth. The effective mass accommodation coefficient introduced in this study provides an efficient new way of accounting for the influence of volatility, diffusivity, and particle-phase reactions on SOA partitioning in process models as well as in regional and global air quality models. While kinetic limitations may not be critical for partitioning into liquid SOA particles in the planetary boundary layer (PBL), the effects are likely important for amorphous semi-solid or glassy SOA in the free and upper troposphere (FT UT) as well as in the PBL at low relative humidity and low temperature. © 2021 Institute of Electrical and Electronics Engineers Inc.. All rights reserved.
语种	英语
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/168786
作者单位	Department of Chemistry, University of California, Irvine, CA 92697, United States; Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, 55128, Germany
推荐引用方式 GB/T 7714	Shiraiwa M.,Pöschl U.. Mass accommodation and gas-particle partitioning in secondary organic aerosols: Dependence on diffusivity; volatility; particle-phase reactions; and penetration depth[J],2021,21(3).
APA	Shiraiwa M.,&Pöschl U..(2021).Mass accommodation and gas-particle partitioning in secondary organic aerosols: Dependence on diffusivity; volatility; particle-phase reactions; and penetration depth.Atmospheric Chemistry and Physics,21(3).
MLA	Shiraiwa M.,et al."Mass accommodation and gas-particle partitioning in secondary organic aerosols: Dependence on diffusivity; volatility; particle-phase reactions; and penetration depth".Atmospheric Chemistry and Physics 21.3(2021).