A new parameterization of uptake coefficients for heterogeneous reactions on multi-component atmospheric aerosols

Yike Zhou; Sunling Gong; Chunhong Zhou; Lei Zhang; Jianjun He; Yuesi Wang; Dongsheng Ji; Jianing Feng; Jingyue Mo; Huabing Ke

doi:10.1016/j.scitotenv.2021.146372

A new parameterization of uptake coefficients for heterogeneous reactions on multi-component atmospheric aerosols

Sci Total Environ. 2021 Aug 10:781:146372. doi: 10.1016/j.scitotenv.2021.146372. Epub 2021 Mar 11.

Authors

Yike Zhou¹, Sunling Gong², Chunhong Zhou³, Lei Zhang⁴, Jianjun He³, Yuesi Wang⁵, Dongsheng Ji⁵, Jianing Feng³, Jingyue Mo¹, Huabing Ke¹

Affiliations

¹ Climate and Weather Disasters Collaborative Innovation Center, Nanjing University of Information Science & Technology, Nanjing 210044, China; State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China.
² State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China. Electronic address: gongsl@cma.gov.cn.
³ State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China.
⁴ State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China. Electronic address: leiz09@cma.gov.cn.
⁵ State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China.

PMID: 33784528
DOI: 10.1016/j.scitotenv.2021.146372

Abstract

Based on laboratory studies and field observations, a new parameterization of uptake coefficients for heterogeneous reactions on multi-component aerosols is developed in this work. The equivalent ratio (ER) of inorganic aerosol is used to establish the quantitative relationship between the heterogeneous uptake coefficients and the composition of aerosols. Incorporating the new ER-dependent scheme, the WRF-CUACE model has been applied to simulate sulfate mass concentrations during December 2017 in the Beijing-Tianjin-Hebei region and evaluate the role of aerosol chemical components played in the sulfate formation. Simulated temporal variations and magnitudes of sulfate show good agreement with the observations by using this new scheme. From clean to polluted cases, although both dominant cations and anions increase significantly, the equivalent ratio decreases gradually and is closer to unity, representing the variation of aerosol compositions, which inhibits the heterogeneous uptake of SO₂, with the uptake coefficient decreasing from 1 × 10^-4 to 5.3 × 10^-5. Based on this phenomenon, a self-limitation process for heterogeneous reactions with the increasing secondary inorganic aerosol from clean to polluted cases is proposed.

Keywords: Heterogeneous reactions; Multi-component aerosol; Parameterization; Sulfate; Uptake coefficient.