在雾霾事件期间，硫酸盐的形成主要是由气溶胶表面上锰催化的SO氧化作用所主导。
Sulfate formation is dominated by manganese-catalyzed oxidation of SO on aerosol surfaces during haze events.
作者信息
Wang Weigang, Liu Mingyuan, Wang Tiantian, Song Yu, Zhou Li, Cao Junji, Hu Jingnan, Tang Guigang, Chen Zhe, Li Zhijie, Xu Zhenying, Peng Chao, Lian Chaofan, Chen Yan, Pan Yuepeng, Zhang Yunhong, Sun Yele, Li Weijun, Zhu Tong, Tian Hezhong, Ge Maofa
机构信息
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China.
University of Chinese Academy of Sciences, Beijing, China.
出版信息
Nat Commun. 2021 Mar 31;12(1):1993. doi: 10.1038/s41467-021-22091-6.
The formation mechanism of aerosol sulfate during wintertime haze events in China is still largely unknown. As companions, SO and transition metals are mainly emitted from coal combustion. Here, we argue that the transition metal-catalyzed oxidation of SO on aerosol surfaces could be the dominant sulfate formation pathway and investigate this hypothesis by integrating chamber experiments, numerical simulations and in-field observations. Our analysis shows that the contribution of the manganese-catalyzed oxidation of SO on aerosol surfaces is approximately one to two orders of magnitude larger than previously known routes, and contributes 69.2% ± 5.0% of the particulate sulfur production during haze events. This formation pathway could explain the missing source of sulfate and improve the understanding of atmospheric chemistry and climate change.
中国冬季雾霾事件期间气溶胶硫酸盐的形成机制在很大程度上仍不为人知。作为伴生物，二氧化硫（SO）和过渡金属主要来自煤炭燃烧。在此，我们认为气溶胶表面过渡金属催化的二氧化硫氧化可能是硫酸盐形成的主要途径，并通过结合室内实验、数值模拟和实地观测来研究这一假设。我们的分析表明，气溶胶表面锰催化的二氧化硫氧化贡献比先前已知途径大约高1至2个数量级，并且在雾霾事件期间对颗粒态硫生成的贡献为69.2%±5.0%。这一形成途径可以解释硫酸盐缺失的来源，并增进对大气化学和气候变化的理解。
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