Water Promotes the Oxidation of SO2 by O-2 over Carbonaceous Aerosols

He Guangzhi; He Hong

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Water Promotes the Oxidation of SO2 by O-2 over Carbonaceous Aerosols

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Severe haze episodes typically occur with concurrent high relative humidity. Here, the vital role of water in promoting the oxidation of SO2 by O-2 on carbonaceous soot surfaces was identified at the atomic level by first-principles calculations. Water molecules can dissociate into surface hydroxyl groups through a self-catalyzed process under ambient conditions. The surface hydroxyl groups, acting as facilitators, can significantly accelerate the conversion of SO2 to SO3 (precursor of particulate sulfate) over soot aerosols by reducing the reaction barriers. Specifically, the hydroxyl groups activate the reactants and stabilize the transition states and products through hydrogen-bonding interactions, making the reactions both thermodynamically and kinetically more favorable at room temperature. The findings indicate that atmospheric humidity plays an important role in enhancing the atmospheric oxidation capacity, thus exacerbating SO2 oxidation and severe haze development. Also, this study unravels a mechanism of surface hydroxyl-assisted O-2 and H2O dissociation over metal-free carbocatalysts under normal conditions.

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《Environmental Science & Technology: ES&T》 |2020年第12期|7070-7077|共8页
作者
He Guangzhi; He Hong;
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作者单位

Chinese Acad Sci, State Key Joint Lab Environm Simulat & Pollut Con, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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正文语种英语
中图分类环境科学、安全科学;
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Water Promotes the Oxidation of SO2 by O-2 over Carbonaceous Aerosols

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