Spontaneous Oxygen−Carbonate Synergistic Photoactivation as a Novel Pathway for Atmospheric Radicals
Carbonate is a common component of soil and coarse atmospheric particulate matter, while few studies have focused on its photochemical reactivity. We present a novel photoactivation mechanism of carbonate and O<sub>2</sub> in the absence of additional potent oxidants. Under light conditions, carbonate ions (CO<sub>3</sub><sup>2-</sup>), O<sub>2</sub>, and H<sub>3</sub>O<sup>+</sup>/OH<sup>-</sup> could spontaneously form a complex and generate CO<sub>3</sub><sup>-</sup> and HO<sub>2</sub>/O<sub>2</sub><sup>-</sup> radicals through an electron transfer process. Under these conditions, the H<sub>2</sub>O<sub>2</sub> production in 1 mM Na<sub>2</sub>CO<sub>3</sub> solution was 0.37 ± 0.10 μg·L<sup>-1</sup> and the cumulative concentration of OH radicals in 4 h was 34.6 nM. The proposed mechanism could be a potential source of atmospheric oxidizing capacity, and the reactive species produced by the CO<sub>3</sub><sup>2-</sup>-O<sub>2</sub> photoactivation process could promote secondary sulfate production. Our findings underscore the importance of carbonate atmospheric reactivity, especially at special reaction surfaces such as air-water interfaces and microdroplets.
Authors
- Peng Zhang (ORCID: https://orcid.org/0000-0002-0620-7673)
- Jiarong Liu (ORCID: https://orcid.org/0009-0005-0831-2636)
- Biwu Chu (ORCID: https://orcid.org/0000-0002-7548-5669)
- Tianzeng Chen (ORCID: https://orcid.org/0000-0001-8123-0534)
- Jincai Zhao (ORCID: https://orcid.org/0000-0003-1449-4235)
- Yanqiang Cao
- Wenjing Song (ORCID: https://orcid.org/0000-0003-1916-8607)
- Yonghong Wang (ORCID: https://orcid.org/0000-0003-2498-9143)
- Qingxin Ma (ORCID: https://orcid.org/0000-0002-9668-7008)
- Ge Tian (ORCID: https://orcid.org/0009-0007-5153-7704)
- Chuncheng Chen (ORCID: https://orcid.org/0000-0003-4034-8063)
- Yujing Mu (ORCID: https://orcid.org/0000-0002-7048-2856)
- Xiuhui Zhang (ORCID: https://orcid.org/0000-0001-9570-7882)
- Hao Li (ORCID: https://orcid.org/0000-0002-1002-6357)
- Pengfei Liu (ORCID: https://orcid.org/0000-0001-6237-3759)
- Jun Liu (ORCID: https://orcid.org/0000-0002-3065-799X)
- Zhuo Wang (ORCID: https://orcid.org/0000-0002-4069-9501)
- Shuying Li (ORCID: https://orcid.org/0000-0003-0786-5931)
- Hong He (ORCID: https://orcid.org/0000-0001-8476-8217)
Institutions
- Beijing Institute of Technology (CN)
- Ministry of Education of the People's Republic of China (CN)
- Chinese Academy of Sciences (CN)
- Beijing National Laboratory for Molecular Sciences (CN)
- Institute of Urban Environment (CN)
- Research Center for Eco-Environmental Sciences (CN)
- University of Chinese Academy of Sciences (CN)
- Molecular Sciences Institute (US)
Publication Details
- Journal
- Environmental Science & Technology
- Published
- 2025-09-17
- DOI
- https://doi.org/10.1021/acs.est.5c05652
- Citations
- 3
- Primary Topic
- Atmospheric chemistry and aerosols
- Type
- article
- Field-Weighted Citation Impact
- 3.90