气候变化领域集成服务门户(CCPortal): Impact of non-ideality on reconstructing spatial and temporal variations in aerosol acidity with multiphase buffer theory

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DOI	10.5194/acp-22-47-2022
	Impact of non-ideality on reconstructing spatial and temporal variations in aerosol acidity with multiphase buffer theory
	Zheng, Guangjie; Su, Hang; Wang, Siwen; Pozzer, Andrea; Cheng, Yafang
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	47
结束页码	63
卷号	22 期号:1 页码:17
英文摘要	Aerosol acidity is a key parameter in atmospheric aqueous chemistry and strongly influences the interactions of air pollutants and the ecosystem. The recently proposed multiphase buffer theory provides a framework to reconstruct long-term trends and spatial variations in aerosol pH based on the effective acid dissociation constant of ammonia (K(a,NH3)). However, non-ideality in aerosol droplets is a major challenge limiting its broad applications. Here, we introduced a non-ideality correction factor (c(ni)) and investigated its governing factors. We found that besides relative humidity (RH) and temperature, c(ni), is mainly determined by the molar fraction of NO3- in aqueous-phase anions, due to different NH4+ activity coefficients between (NH4)(2)SO4-and NH4NO3-dominated aerosols. A parameterization method is thus proposed to estimate c(ni) at a given RH, temperature and NO3- fraction, and it is validated against long-term observations and global simulations. In the ammonia-buffered regime, with c(ni) correction, the buffer theory can reproduce well the K(a,NH3) predicted by comprehensive thermodynamic models, with a root-mean-square deviation similar to 0.1 and a correlation coefficient similar to 1. Note that, while c(ni), is needed to predict K(a,NH3) levels, it is usually not the dominant contributor to its variations, as similar to 90 % of the temporal or spatial variations in K(a,NH3) are due to variations in aerosol water and temperature.
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:000739109800001
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/273029
作者单位	Max Planck Society; Max Planck Society; Max Planck Society
推荐引用方式 GB/T 7714	Zheng, Guangjie,Su, Hang,Wang, Siwen,et al. Impact of non-ideality on reconstructing spatial and temporal variations in aerosol acidity with multiphase buffer theory[J],2022,22(1):17.
APA	Zheng, Guangjie,Su, Hang,Wang, Siwen,Pozzer, Andrea,&Cheng, Yafang.(2022).Impact of non-ideality on reconstructing spatial and temporal variations in aerosol acidity with multiphase buffer theory.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(1),17.
MLA	Zheng, Guangjie,et al."Impact of non-ideality on reconstructing spatial and temporal variations in aerosol acidity with multiphase buffer theory".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.1(2022):17.