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Carbonate radical ion as a key driver of rapid atmospheric sulfate formation

Liu Yangyang,Li Xiao,Ge Qiuyue,Fang Xiaozhong,Wang Tao,You Wenbo,Wang Wei,Xie Lifang,Li Kejian,Gong Kedong,Yang Le,Wang Runbo,Wang Jilun,Wang Licheng,Ma Minglu,Huang Tingting,Fu Hongbo,Chen Jianmin,Dong Xinyi,Zhang Liwu

Carbonate radical anion ( \({{\rm{CO}}}_{{3}^{.-}}\) ) is generally considered as a marginal intermediate that rarely regulates atmospheric-relevant reactions of significance. Unexpectedly, in this work, employing a suit of the in-field measurements, lab-based validations, improved kinetic numerical calculations, and chemical transport modeling, we demonstrate that \({{\rm{CO}}}_{{3}^{.-}}\) gives a significantly overlooked contribution (~54.4%) to overall secondary sulfate formation during dust storm-relevant episodes and ~236.3% increase of SO 2 uptake over mineral dust pathway during haze-relevant periods. GEOS-Chem modeling results further emphasize the important position of this radical ion in dust-driven SO 2 oxidation chemistry. Our finding leaves this active intermediate no longer a marginal oxidant currently prevailing in the framework of the atmospheric science community. More importantly, after considering this rapid dust-driven sulfate formation channel mediated by carbonate radicals during pollution episodes, this study provides a clear indication that high priority should be given to reducing alkaline soil dust emissions to achieve benefits for air quality.