气候变化领域集成服务门户(CCPortal): A predictive viscosity model for aqueous electrolytes and mixed organic-inorganic aerosol phases

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DOI	10.5194/acp-22-3203-2022
	A predictive viscosity model for aqueous electrolytes and mixed organic-inorganic aerosol phases
	Lilek, Joseph; Zuend, Andreas
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	3203
结束页码	3233
卷号	22 期号:5 页码:31
英文摘要	Aerosol viscosity is determined by mixture composition and temperature, with a key influence from relative humidity (RH) in modulating aerosol water content. Aerosol particles frequently contain mixtures of water, organic compounds, and inorganic ions, so we have extended the thermodynamics-based group-contribution model AIOMFAC-VISC to predict viscosity for aqueous electrolyte solutions and aqueous organic-inorganic mixtures. For aqueous electrolyte solutions, our new, semi-empirical approach uses a physical expression based on Eyring's absolute rate theory, and we define activation energy for viscous flow as a function of temperature, ion activities, and ionic strength. The AIOMFAC-VISC electrolyte model's ion-specific expressions were simultaneously fitted, which arguably makes this approach more predictive than that of other models. This also enables viscosity calculations for aqueous solutions containing an arbitrary number of cation and anion species, including mixtures that have never been studied experimentally. These predictions achieve an excellent level of accuracy while also providing physically meaningful extrapolations to extremely high electrolyte concentrations, which is essential in the context of microscopic aqueous atmospheric aerosols. For organic-inorganic mixtures, multiple mixing approaches were tested to couple the AIOMFAC-VISC electrolyte model with its existing aqueous organic model. We discuss the best-performing mixing models implemented in AIOMFAC-VISC for reproducing viscosity measurements of aerosol surrogate systems. We present advantages and drawbacks of different model design choices and associated computational costs of these methods, of importance for use of AIOMFAC-VISC in dynamic simulations. Finally, we demonstrate the capabilities of AIOMFAC-VISC predictions for phase-separated organic-inorganic particles equilibrated to observed temperature and relative humidity conditions from atmospheric balloon soundings. The predictions for the studied cases suggest liquid-like viscosities for an aqueous electrolyte-rich particle phase throughout the troposphere, yet a highly viscous or glassy organic-rich phase in the middle and upper troposphere.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000768714900001
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/273266
作者单位	McGill University
推荐引用方式 GB/T 7714	Lilek, Joseph,Zuend, Andreas. A predictive viscosity model for aqueous electrolytes and mixed organic-inorganic aerosol phases[J],2022,22(5):31.
APA	Lilek, Joseph,&Zuend, Andreas.(2022).A predictive viscosity model for aqueous electrolytes and mixed organic-inorganic aerosol phases.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(5),31.
MLA	Lilek, Joseph,et al."A predictive viscosity model for aqueous electrolytes and mixed organic-inorganic aerosol phases".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.5(2022):31.