Photoactivation of Chlorine and Its Catalytic Role in the Formation of Sulfate Aerosols

Yiqun Cao, Jiarong Liu, Qingxin Ma*, Chunyan Zhang, Peng Zhang, Tianzeng Chen, Yonghong Wang, Biwu Chu, Xiuhui Zhang, Joseph S. Francisco*, Hong He*

*Corresponding author for this work

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Abstract

We present a novel mechanism for the formation of photocatalytic oxidants in deliquescent NaCl particles, which can greatly promote the multiphase photo-oxidation of SO2 to produce sulfate. The photoexcitation of the [Cl--H3O+-O2] complex leads to the generation of Cl and OH radicals, which is the key reason for enhancing aqueous-phase oxidation and accelerating SO2 oxidation. The mass normalization rate of sulfate production from the multiphase photoreaction of SO2 on NaCl droplets could be estimated to be 0.80 × 10-4 μg·h-1 at 72% RH and 1.33 × 10-4 μg·h-1 at 81% RH, which is equivalent to the known O3 liquid-phase oxidation mechanism. Our findings highlight the significance of multiphase photo-oxidation of SO2 on NaCl particles as a non-negligible source of sulfate in coastal areas. Furthermore, this study underscores the importance of Cl- photochemistry in the atmosphere.

Original languageEnglish
Pages (from-to)1467-1475
Number of pages9
JournalJournal of the American Chemical Society
Volume146
Issue number2
DOIs
Publication statusPublished - 17 Jan 2024

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Cao, Y., Liu, J., Ma, Q., Zhang, C., Zhang, P., Chen, T., Wang, Y., Chu, B., Zhang, X., Francisco, J. S., & He, H. (2024). Photoactivation of Chlorine and Its Catalytic Role in the Formation of Sulfate Aerosols. Journal of the American Chemical Society, 146(2), 1467-1475. https://doi.org/10.1021/jacs.3c10840