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- Title
A novel pathway of atmospheric sulfate formation through carbonate radicals.
- Authors
Liu, Yangyang; Deng, Yue; Liu, Jiarong; Fang, Xiaozhong; Wang, Tao; Li, Kejian; Gong, Kedong; Bacha, Aziz U.; Nabi, Iqra; Ge, Qiuyue; Zhang, Xiuhui; George, Christian; Zhang, Liwu
- Abstract
Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. Nonetheless, we show here that CO 2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO 3⚫-). This potentially active intermediate CO 3⚫- is routinely overlooked in atmospheric chemistry concerning its effect on sulfate formation. The present work demonstrates that the SO 2 uptake coefficient is enhanced by 17 times on mineral dust particles driven by CO 3⚫-. Importantly, upon irradiation, mineral dust particles are speculated to produce gas-phase carbonate radical ions when the atmospherically relevant concentration of CO 2 presents, thereby potentially promoting external sulfate aerosol formation and oxidative potential in the atmosphere. Employing a suite of laboratory investigations of sulfate formation in the presence of carbonate radicals on the model and authentic dust particles, ground-based field measurements of sulfate and (bi)carbonate ions within ambient PM, together with density functional theory (DFT) calculations for single electron transfer processes in terms of CO 3⚫- -initiated S(IV) oxidation, a novel role of carbonate radical in atmospheric chemistry is elucidated.
- Subjects
MINERAL dusts; DUST; SULFATE aerosols; RADICAL ions; CHEMICAL reactions
- Publication
Atmospheric Chemistry & Physics, 2022, Vol 22, Issue 13, p9175
- ISSN
1680-7316
- Publication type
Article
- DOI
10.5194/acp-22-9175-2022