Increasing Contribution of Chlorine Chemistry to Wintertime Ozone Formation Promoted by Enhanced Nitrogen Chemistry

Creators: Chen, Gaojie^{1, 2}; Xu, Lingling¹; Yu, Shaocai^{3, 4}; Xue, Likun⁵; Lin, Ziyi^{1, 2}; Yang, Chen^{1, 2}; Ji, Xiaoting^{1, 2}; Fan, Xiaolong¹; Tham, Yee Jun⁶; Wang, Haichao⁶; Hong, Youwei¹; Li, Mengren¹; Seinfeld, John H.⁷; Chen, Jinsheng¹

1. Institute of Urban Environment
2. University of Chinese Academy of Sciences
3. Zhejiang Gongshang University
4. Zhejiang University
5. Shandong University
6. Sun Yat-sen University
7. California Institute of Technology

Abstract

Chlorine (Cl) radicals strongly affect atmospheric oxidation and the fate of pollutants. Despite several observations, the potential impacts of nitrogen chemistry associated with NO₂ on Cl chemistry are poorly understood. Here, we provided direct field evidence that the nitrogen chemistry enhancements triggered by the increased NO₂ drove daytime nitrate (NO₃^-) photolysis and nighttime NO₃-N₂O₅ reactions, significantly promoting the increases in the concentrations of ClNO₂ and Cl₂ after the Chinese Spring Festival. The enhancement in the Cl chemistry facilitated the elevations of both O₃ and atmospheric oxidation capacity during the winter daytime. Our findings highlighted the importance of nitrogen chemistry induced by the increased NO₂ in enhanced Cl chemistry.

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Acknowledgement

This work was funded by the National Natural Science Foundation of China (U22A20578, 42277091, 72361137007, 42175084, and 21577126), the Science and Technology Department of Fujian Province (2022L3025), the National Key Research and Development Program (2022YFC3700304), STS Plan Supporting Project of the Chinese Academy of Sciences in Fujian Province (2023T3013), Guangdong Basic and Applied Basic Research Foundation (2022A1515010852), and the Fundamental Research Funds for the Central Universities, Sun Yat-sen University (23hytd002), and Xiamen Atmospheric Environment Observation and Research Station of Fujian Province.

Supplemental Material

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.4c09523.

Detailed information on the study site, observational instruments, calibration results, box model setting and output parameters, and differences of observed parameters and simulation results between the periods after and during the Spring Festival (PDF)

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