A comprehensive study about the in-cloud processing of nitrate through coupled measurements of individual cloud residuals and cloud water

Guohua Zhang, Xiaodong Hu, Wei Sun, Yuxiang Yang, Ziyong Guo, Yuzhen Fu, Haichao Wang, Shengzhen Zhou, Lei Li, Mingjin Tang, Zongbo Shi, Duohong Chen, Xinhui Bi*, Xinming Wang

*Corresponding author for this work

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Abstract

While the formation and evolution of nitrate in airborne particles are extensively investigated, little is known about the processing of nitrate in clouds. Here we present a detailed investigation on the in-cloud formation of nitrate, based on the size-resolved mixing state of nitrate in the individual cloud residual and cloud-free particles obtained by single particle mass spectrometry, and also the mass concentrations of nitrate in the cloud water and PM2.5 at a mountain site (1690ma.s.l. - above sea level) in southern China. The results show a significant enhancement of nitrate mass fraction and relative intensity of nitrate in the cloud water and the cloud residual particles, respectively, reflecting a critical role of in-cloud processing in the formation of nitrate. We first exclude the gas-phase scavenging of HNO3 and the facilitated activation of nitrate-containing particles as the major contribution for the enhanced nitrate, according to the size distribution of nitrate in individual particles. Based on regression analysis and theoretical calculations, we then highlight the role of N2O5 hydrolysis in the in-cloud formation of nitrate, even during the daytime, attributed to the diminished light in clouds. Nitrate is highly related (R2Combining double low line1/40.6) to the variations in [NOx][O3], temperature, and droplet surface area in clouds. Accounting for droplet surface area greatly enhances the predictability of the observed nitrate, compared with using [NOx][O3] and temperature. The substantial contribution of N2O5 hydrolysis to nitrate in clouds with diminished light during the daytime can be reproduced by a multiphase chemical box model. Assuming a photolysis rate at 30 of the default setting, the overall contribution of N2O5 hydrolysis pathway to nitrate formation increases by 1/420 in clouds. Given that N2O5 hydrolysis acts as a major sink of NOx in the atmosphere, further model updates would improve our understanding about the processes contributing to nitrate production in cloud and the cycling of odd nitrogen.

Original languageEnglish
Pages (from-to)9571-9582
Number of pages12
JournalAtmospheric Chemistry and Physics
Volume22
Issue number14
DOIs
Publication statusPublished - 27 Jul 2022

Bibliographical note

Funding Information:
Financial support. This work has been funded by the Natural Science Foundation of Guangdong Province (grant no. 2019B151502022), National Natural Science Foundation of China (grant nos. 42077322, 41775124, and 41877307), Youth Innovation Promotion Association CAS (grant no. 2021354), and Guangdong Foundation for Program of Science and Technology Research (grant no. 2020B1212060053).

Publisher Copyright:
© 2022 The Author(s).

ASJC Scopus subject areas

  • Atmospheric Science

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