Effects of heterogeneous reaction with NO2 on ice nucleation activities of feldspar and Arizona Test Dust

Lanxiadi Chen; Chao Peng; Jingchuan Chen; Jie Chen; Wenjun Gu; Xiaohong Jia; Zhijun Wu; Qiyuan Wang; Mingjin Tang

doi:10.1016/j.jes.2022.04.034

Effects of heterogeneous reaction with NO₂ on ice nucleation activities of feldspar and Arizona Test Dust

J Environ Sci (China). 2023 May:127:210-221. doi: 10.1016/j.jes.2022.04.034. Epub 2022 May 4.

Authors

Lanxiadi Chen¹, Chao Peng², Jingchuan Chen³, Jie Chen³, Wenjun Gu², Xiaohong Jia², Zhijun Wu³, Qiyuan Wang⁴, Mingjin Tang⁵

Affiliations

¹ State Key Laboratory of Organic Geochemistry, Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangdong-Hong Kong-Macao Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China; CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China; University of Chinese Academy of Sciences, Beijing 100049, China.
² State Key Laboratory of Organic Geochemistry, Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangdong-Hong Kong-Macao Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China.
³ State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China.
⁴ Key Laboratory of Aerosol Chemistry and Physics, State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China.
⁵ State Key Laboratory of Organic Geochemistry, Guangdong Key Laboratory of Environmental Protection and Resources Utilization, Guangdong-Hong Kong-Macao Joint Laboratory for Environmental Pollution and Control, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China; CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China; University of Chinese Academy of Sciences, Beijing 100049, China. Electronic address: mingjintang@gig.ac.cn.

PMID: 36522054
DOI: 10.1016/j.jes.2022.04.034

Abstract

Mineral dust is an important type of ice nucleating particles in the troposphere; however, the effects of heterogeneous reactions on ice nucleation (IN) activities of mineral dust remain to be elucidated. A droplet-freezing apparatus (Guangzhou Institute of Geochemistry Ice Nucleation Apparatus, GIGINA) was developed in this work to measure IN activities of atmospheric particles in the immersion freezing mode, and its performance was validated by a series of experimental characterizations. This apparatus was then employed to measure IN activities of feldspar and Arizona Test Dust (ATD) particles before and after heterogeneous reaction with NO₂ (10±0.5 ppmv) at 40% relative humidity. The surface coverage of nitrate, θ(NO₃^-), increased to 3.1±0.2 for feldspar after reaction with NO₂ for 6 hr, and meanwhile the active site density per unit surface area (n_s) at -20°C was reduced from 92±5 to <1.0 cm^-2 by about two orders of magnitude; however, no changes in nitrate content or IN activities were observed for further increase in reaction time (up to 24 hr). Both nitrate content and IN activities changed continuously with reaction time (up to 24 hr) for ATD particles; after reaction with NO₂ for 24 hr, θ(NO₃^-) increased to 1.4±0.1 and n_s at -20°C was reduced from 20±4 to 9.7±1.9 cm^-2 by a factor of ∼2. Our work suggests that heterogeneous reaction with NO₂, an abundant reactive nitrogen species in the troposphere, may significantly reduce IN activities of mineral dust in the immersion freezing mode.

Keywords: Aerosol-cloud interaction; Heterogeneous reaction; Ice nucleation; Mineral dust; Nitrogen oxides.