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DOI10.5194/acp-22-9175-2022
A novel pathway of atmospheric sulfate formation through carbonate radicals
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
发表日期2022
ISSN1680-7316
EISSN1680-7324
起始页码9175
结束页码9197
卷号22期号:13页码:23
英文摘要Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. Nonetheless, we show here that CO2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO3 center dot-). This potentially active intermediate CO3 center dot- is routinely overlooked in atmospheric chemistry concerning its effect on sulfate formation. The present work demonstrates that the SO2 uptake coefficient is enhanced by 17 times on mineral dust particles driven by CO3 center dot-. Importantly, upon irradiation, mineral dust particles are speculated to produce gas-phase carbonate radical ions when the atmospherically relevant concentration of CO2 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 CO3 center dot--initiated S(IV) oxidation, a novel role of carbonate radical in atmospheric chemistry is elucidated.
学科领域Environmental Sciences; Meteorology & Atmospheric Sciences
语种英语
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号WOS:000825489800001
来源期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/273552
作者单位Fudan University; Beijing Institute of Technology; Ministry of Education, China; Centre National de la Recherche Scientifique (CNRS); UDICE-French Research Universities; Universite Claude Bernard Lyon 1
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GB/T 7714
Liu, Yangyang,Deng, Yue,Liu, Jiarong,et al. A novel pathway of atmospheric sulfate formation through carbonate radicals[J],2022,22(13):23.
APA Liu, Yangyang.,Deng, Yue.,Liu, Jiarong.,Fang, Xiaozhong.,Wang, Tao.,...&Zhang, Liwu.(2022).A novel pathway of atmospheric sulfate formation through carbonate radicals.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(13),23.
MLA Liu, Yangyang,et al."A novel pathway of atmospheric sulfate formation through carbonate radicals".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.13(2022):23.
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