气候变化领域集成服务门户(CCPortal): Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation

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DOI	10.5194/acp-22-973-2022
	Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation
	Yin, Hang; Dou, Jing; Klein, Liviana; Krieger, Ulrich K.; Bain, Alison; Wallace, Brandon J.; Preston, Thomas C.; Zuend, Andreas
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	973
结束页码	1013
卷号	22 期号:2 页码:41
英文摘要	Iodine and carbonate species are important components in marine and dust aerosols, respectively. The non-ideal interactions between these species and other inorganic and organic compounds within aqueous particle phases affect hygroscopicity, acidity, and gas-particle partitioning of semivolatile components. In this work, we present an extended version of the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model by incorporating the ions I-, IO3-, HCO3-, CO32-, OH-, and CO2(aq) as new species. First, AIOMFAC ion interaction parameters for aqueous solutions were determined based on available thermodynamic data, such as water activity, mean molal activity coefficients, solubility, and vapor-liquid equilibrium measurements. Second, the interaction parameters for the new ions and various organic functional groups were optimized based on experimental data or, where data are scarce, alternative estimation methods such as multiple linear regression or a simple substitution by analogy approach. Additional bulk water activity and electrodynamic balance measurements were carried out to augment the database for the AIOMFAC parameter fit. While not optimal, we show that the use of alternative parameter estimation methods enables physically sound predictions and offers the benefit of a more broadly applicable model. Our implementation of the aqueous carbonate-bicarbonate-CO2( aq) system accounts for the associated temperature-dependent dissociation equilibria explicitly and enables closed- or open-system computations with respect to carbon dioxide equilibration with the gas phase. We discuss different numerical approaches for solving the coupled equilibrium conditions and highlight critical considerations when extremely acidic or basic mixtures are encountered. The fitted AIOMFAC model performance for inorganic aqueous systems is considered excellent over the whole range of mixture compositions where reference data are available. Moreover, the model provides physically meaningful predictions of water activity under highly concentrated conditions. For organic-inorganic mixtures involving new species, the model-measurement agreement is found to be good in most cases, especially at equilibrium relative humidities above similar to 70 %; reasons for deviations are discussed. Several applications of the extended model are shown and discussed, including the effects of ignoring the auto-dissociation of water in carbonate systems, the effects of mixing bisulfate and bicarbonate compounds in closed- or open-system scenarios on pH and solution speciation, and the prediction of critical cloud condensation nucleus activation of NaI or Na2CO3 particles mixed with suberic acid.
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:000747691900001
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/273404
作者单位	McGill University; Swiss Federal Institutes of Technology Domain; ETH Zurich; McGill University
推荐引用方式 GB/T 7714	Yin, Hang,Dou, Jing,Klein, Liviana,et al. Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation[J],2022,22(2):41.
APA	Yin, Hang.,Dou, Jing.,Klein, Liviana.,Krieger, Ulrich K..,Bain, Alison.,...&Zuend, Andreas.(2022).Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(2),41.
MLA	Yin, Hang,et al."Extension of the AIOMFAC model by iodine and carbonate species: applications for aerosol acidity and cloud droplet activation".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.2(2022):41.