Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface
Abstract Decentralized water treatment technologies, designed to align with the specific characteristics of the water source and the requirements of the user, are gaining prominence due to their cost and energy-saving advantages over traditional centralized systems. The application of chemical water...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-58917-w |
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| author | Jian-Hua Chen Wan-Ting Li Kun-Yu Cai Hui-Jie Tu Zi-Tong Long Shoaib Akhtar Lin-Dong Liu |
| author_facet | Jian-Hua Chen Wan-Ting Li Kun-Yu Cai Hui-Jie Tu Zi-Tong Long Shoaib Akhtar Lin-Dong Liu |
| author_sort | Jian-Hua Chen |
| collection | DOAJ |
| description | Abstract Decentralized water treatment technologies, designed to align with the specific characteristics of the water source and the requirements of the user, are gaining prominence due to their cost and energy-saving advantages over traditional centralized systems. The application of chemical water treatment via heterogeneous advanced oxidation processes using peroxide (O–O) represents a potentially attractive treatment option. These processes serve to initiate redox processes at the solid-water interface. Nevertheless, the oxidation mechanism exemplified by the typical Fenton-like persulfate-based heterogeneous oxidation, in which electron transfer dominates, is almost universally accepted. Here, we present experimental results that challenge this view. At the solid-liquid interface, it is demonstrated that protons are thermodynamically coupled to electrons. In situ quantitative titration provides direct experimental evidence that the coupling ratio of protons to transferred electrons is almost 1:1. Comprehensive thermodynamic analyses further demonstrate that a net proton-coupled electron transfer occurs, with both protons and electrons entering the redox cycle. These findings will inform future developments in O–O activation technologies, enabling more efficient redox activity via the tight coupling of protons and electrons. |
| format | Article |
| id | doaj-art-3bf6fb2a4dba4a2983285a4fc2662e87 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-3bf6fb2a4dba4a2983285a4fc2662e872025-08-20T03:53:32ZengNature PortfolioNature Communications2041-17232025-04-0116111110.1038/s41467-025-58917-wProton-coupled electron transfer controls peroxide activation initiated by a solid-water interfaceJian-Hua Chen0Wan-Ting Li1Kun-Yu Cai2Hui-Jie Tu3Zi-Tong Long4Shoaib Akhtar5Lin-Dong Liu6Interdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest UniversityInterdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest UniversityInterdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest UniversityInterdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest UniversityInterdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest UniversityInterdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest UniversityInterdisciplinary Research Centre for Agriculture Green Development in Yangtze River Basin, Department of Environmental Sciences and Engineering, College of Resources and Environment, Southwest UniversityAbstract Decentralized water treatment technologies, designed to align with the specific characteristics of the water source and the requirements of the user, are gaining prominence due to their cost and energy-saving advantages over traditional centralized systems. The application of chemical water treatment via heterogeneous advanced oxidation processes using peroxide (O–O) represents a potentially attractive treatment option. These processes serve to initiate redox processes at the solid-water interface. Nevertheless, the oxidation mechanism exemplified by the typical Fenton-like persulfate-based heterogeneous oxidation, in which electron transfer dominates, is almost universally accepted. Here, we present experimental results that challenge this view. At the solid-liquid interface, it is demonstrated that protons are thermodynamically coupled to electrons. In situ quantitative titration provides direct experimental evidence that the coupling ratio of protons to transferred electrons is almost 1:1. Comprehensive thermodynamic analyses further demonstrate that a net proton-coupled electron transfer occurs, with both protons and electrons entering the redox cycle. These findings will inform future developments in O–O activation technologies, enabling more efficient redox activity via the tight coupling of protons and electrons.https://doi.org/10.1038/s41467-025-58917-w |
| spellingShingle | Jian-Hua Chen Wan-Ting Li Kun-Yu Cai Hui-Jie Tu Zi-Tong Long Shoaib Akhtar Lin-Dong Liu Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface Nature Communications |
| title | Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface |
| title_full | Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface |
| title_fullStr | Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface |
| title_full_unstemmed | Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface |
| title_short | Proton-coupled electron transfer controls peroxide activation initiated by a solid-water interface |
| title_sort | proton coupled electron transfer controls peroxide activation initiated by a solid water interface |
| url | https://doi.org/10.1038/s41467-025-58917-w |
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