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

Abstract Carbonate radical anion ( $${{\rm{CO}}}_{{3}^{.-}}$$ 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...

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Main Authors: Yangyang Liu, Xiao Li, Qiuyue Ge, Xiaozhong Fang, Tao Wang, Wenbo You, Wei Wang, Lifang Xie, Kejian Li, Kedong Gong, Le Yang, Runbo Wang, Jilun Wang, Licheng Wang, Minglu Ma, Tingting Huang, Hongbo Fu, Jianmin Chen, Xinyi Dong, Liwu Zhang
Format: Article
Language:English
Published: Nature Portfolio 2025-02-01
Series:npj Climate and Atmospheric Science
Online Access:https://doi.org/10.1038/s41612-025-00905-4
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Summary:Abstract Carbonate radical anion ( $${{\rm{CO}}}_{{3}^{.-}}$$ 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 $${{\rm{CO}}}_{{3}^{.-}}$$ CO 3 . − gives a significantly overlooked contribution (~54.4%) to overall secondary sulfate formation during dust storm-relevant episodes and ~236.3% increase of SO2 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 SO2 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.
ISSN:2397-3722