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: | , , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-02-01
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| Series: | npj Climate and Atmospheric Science |
| Online Access: | https://doi.org/10.1038/s41612-025-00905-4 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Yangyang Liu |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-3958e14b629a4f648963ebe3d46f14ee |
| institution | DOAJ |
| issn | 2397-3722 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Climate and Atmospheric Science |
| spelling | doaj-art-3958e14b629a4f648963ebe3d46f14ee2025-08-20T02:48:11ZengNature Portfolionpj Climate and Atmospheric Science2397-37222025-02-018111210.1038/s41612-025-00905-4Carbonate radical ion as a key driver of rapid atmospheric sulfate formationYangyang Liu0Xiao Li1Qiuyue Ge2Xiaozhong Fang3Tao Wang4Wenbo You5Wei Wang6Lifang Xie7Kejian Li8Kedong Gong9Le Yang10Runbo Wang11Jilun Wang12Licheng Wang13Minglu Ma14Tingting Huang15Hongbo Fu16Jianmin Chen17Xinyi Dong18Liwu Zhang19Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversitySchool of Atmospheric Sciences, Nanjing UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversitySchool of Atmospheric Sciences, Nanjing UniversityShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan UniversityAbstract 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.https://doi.org/10.1038/s41612-025-00905-4 |
| spellingShingle | 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 Carbonate radical ion as a key driver of rapid atmospheric sulfate formation npj Climate and Atmospheric Science |
| title | Carbonate radical ion as a key driver of rapid atmospheric sulfate formation |
| title_full | Carbonate radical ion as a key driver of rapid atmospheric sulfate formation |
| title_fullStr | Carbonate radical ion as a key driver of rapid atmospheric sulfate formation |
| title_full_unstemmed | Carbonate radical ion as a key driver of rapid atmospheric sulfate formation |
| title_short | Carbonate radical ion as a key driver of rapid atmospheric sulfate formation |
| title_sort | carbonate radical ion as a key driver of rapid atmospheric sulfate formation |
| url | https://doi.org/10.1038/s41612-025-00905-4 |
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