Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification
Abstract Electro-oxidation is a promising green technology for decentralized wastewater purification. However, its efficacy is primarily constrained by the selectivity and efficiency of hydroxyl radical (•OH) generation through one-electron water oxidation. In this study, we elucidate the mechanism...
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Nature Portfolio
2025-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-59722-1 |
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| author | Sen Lu Xuechuan Li Guan Zhang Shaobin Wang |
| author_facet | Sen Lu Xuechuan Li Guan Zhang Shaobin Wang |
| author_sort | Sen Lu |
| collection | DOAJ |
| description | Abstract Electro-oxidation is a promising green technology for decentralized wastewater purification. However, its efficacy is primarily constrained by the selectivity and efficiency of hydroxyl radical (•OH) generation through one-electron water oxidation. In this study, we elucidate the mechanism of electronic metal-support interactions (EMSI) of Ni single-atoms on antimony-doped tin oxide anode (Ni/ATO) to enhance •OH production and overall water treatment efficiency. We experimentally and theoretically investigate both the structural evolution process and micro-interface mechanisms associated with the EMSI effects induced by Ni single-atoms. The optimized electronic structures in the interfacial catalysts under EMSI conditions and the co-catalytic role of Ni single-atoms synergistically facilitate selective and efficient •OH generation, resulting in over a fivefold increase in its steady-state concentration and tenfold enhancement in pseudo-first-order rate constant of sulfamethoxazole degradation compared to those on bare ATO. With the EMSI, rapid electron transfer channels were established for a marked enhancement in the adsorption, conversion, and dissociation of interfacial H2O molecules. Notably, it is revealed that Ni single-atoms serve as co-catalytic sites, exhibiting a “H-pulling effect” that is crucial for •OH generation. The Ni/ATO anode demonstrates great efficiency in degrading various refractory organic pollutants, and effectively treats real pharmaceutical wastewater with low energy consumption. Furthermore, it presents remarkable stability and adaptability, while maintaining a minimal environmental footprint during wastewater treatment processes. This work addresses the theoretical gaps between EMSI effects and co-catalysis in electro-oxidation systems, while providing a robust technological solution for wastewater purification. |
| format | Article |
| id | doaj-art-d9bb4019286e4b879f77f00e8e0b8cc2 |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-05-01 |
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| spelling | doaj-art-d9bb4019286e4b879f77f00e8e0b8cc22025-08-20T02:15:00ZengNature PortfolioNature Communications2041-17232025-05-0116111410.1038/s41467-025-59722-1Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purificationSen Lu0Xuechuan Li1Guan Zhang2Shaobin Wang3State Key Laboratory of Urban Water Resource and Environment, School of Ecology and Environment, Harbin Institute of Technology, Shenzhen (HITSZ)State Key Laboratory of Urban Water Resource and Environment, School of Ecology and Environment, Harbin Institute of Technology, Shenzhen (HITSZ)State Key Laboratory of Urban Water Resource and Environment, School of Ecology and Environment, Harbin Institute of Technology, Shenzhen (HITSZ)School of Chemical Engineering, The University of AdelaideAbstract Electro-oxidation is a promising green technology for decentralized wastewater purification. However, its efficacy is primarily constrained by the selectivity and efficiency of hydroxyl radical (•OH) generation through one-electron water oxidation. In this study, we elucidate the mechanism of electronic metal-support interactions (EMSI) of Ni single-atoms on antimony-doped tin oxide anode (Ni/ATO) to enhance •OH production and overall water treatment efficiency. We experimentally and theoretically investigate both the structural evolution process and micro-interface mechanisms associated with the EMSI effects induced by Ni single-atoms. The optimized electronic structures in the interfacial catalysts under EMSI conditions and the co-catalytic role of Ni single-atoms synergistically facilitate selective and efficient •OH generation, resulting in over a fivefold increase in its steady-state concentration and tenfold enhancement in pseudo-first-order rate constant of sulfamethoxazole degradation compared to those on bare ATO. With the EMSI, rapid electron transfer channels were established for a marked enhancement in the adsorption, conversion, and dissociation of interfacial H2O molecules. Notably, it is revealed that Ni single-atoms serve as co-catalytic sites, exhibiting a “H-pulling effect” that is crucial for •OH generation. The Ni/ATO anode demonstrates great efficiency in degrading various refractory organic pollutants, and effectively treats real pharmaceutical wastewater with low energy consumption. Furthermore, it presents remarkable stability and adaptability, while maintaining a minimal environmental footprint during wastewater treatment processes. This work addresses the theoretical gaps between EMSI effects and co-catalysis in electro-oxidation systems, while providing a robust technological solution for wastewater purification.https://doi.org/10.1038/s41467-025-59722-1 |
| spellingShingle | Sen Lu Xuechuan Li Guan Zhang Shaobin Wang Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification Nature Communications |
| title | Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification |
| title_full | Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification |
| title_fullStr | Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification |
| title_full_unstemmed | Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification |
| title_short | Unlocking single-atom induced electronic metal-support interactions in electrocatalytic one-electron water oxidation for wastewater purification |
| title_sort | unlocking single atom induced electronic metal support interactions in electrocatalytic one electron water oxidation for wastewater purification |
| url | https://doi.org/10.1038/s41467-025-59722-1 |
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