Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight
Abstract It remains a great challenge to explore redox mediators with multi-electron, suitable redox potential, and stable pH buffer ability to simulate the natural solar-to-fuel process. In this work, we present a defect engineering strategy to design soluble multi-electron redox polyoxometalates m...
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| 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/s41467-025-58622-8 |
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| author | Li-Ping Cui Shu Zhang Yue Zhao Xin-Yue Ge Le Yang Ke Li Liu-Bin Feng Ren-Gui Li Jia-Jia Chen |
| author_facet | Li-Ping Cui Shu Zhang Yue Zhao Xin-Yue Ge Le Yang Ke Li Liu-Bin Feng Ren-Gui Li Jia-Jia Chen |
| author_sort | Li-Ping Cui |
| collection | DOAJ |
| description | Abstract It remains a great challenge to explore redox mediators with multi-electron, suitable redox potential, and stable pH buffer ability to simulate the natural solar-to-fuel process. In this work, we present a defect engineering strategy to design soluble multi-electron redox polyoxometalates mediators to construct a photocatalysis-electrolysis relay system to decouple H2 and O2 evolution in solar-driven water splitting. The appropriate use of vanadium atoms to replace tungsten in the Dawson-type phosphotungstate successfully regulated the redox properties of the molecular clusters. Specifically, the single vanadium substitution structure ({P2W17V}) possesses 1-electron redox active and sequential proton-electron transfer behavior, while the tri-vanadium substituted cluster ({P2W15V3}) exhibits 3-electron redox active and cooperative proton electron transfer behavior. Based on the developed multi-electronic redox mediator with pH buffering capacity, suitable redox potential (0.6 V), and fast electron exchange rate, we build a photocatalysis-electrolysis relay water splitting system. This system allows for high capacity of solar energy storage through photocatalytic O2 evolution using BiVO4 photocatalyst and stable H2 production with a high Faraday efficiency of over 98.5% in the electrolysis subsystem. |
| format | Article |
| id | doaj-art-1d1adf8ca4a44e19a1deccb16b4d11af |
| institution | DOAJ |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-1d1adf8ca4a44e19a1deccb16b4d11af2025-08-20T03:18:28ZengNature PortfolioNature Communications2041-17232025-04-0116111210.1038/s41467-025-58622-8Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlightLi-Ping Cui0Shu Zhang1Yue Zhao2Xin-Yue Ge3Le Yang4Ke Li5Liu-Bin Feng6Ren-Gui Li7Jia-Jia Chen8State Key Laboratory for Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory for Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of SciencesState Key Laboratory for Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory for Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory for Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory for Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of SciencesState Key Laboratory for Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityAbstract It remains a great challenge to explore redox mediators with multi-electron, suitable redox potential, and stable pH buffer ability to simulate the natural solar-to-fuel process. In this work, we present a defect engineering strategy to design soluble multi-electron redox polyoxometalates mediators to construct a photocatalysis-electrolysis relay system to decouple H2 and O2 evolution in solar-driven water splitting. The appropriate use of vanadium atoms to replace tungsten in the Dawson-type phosphotungstate successfully regulated the redox properties of the molecular clusters. Specifically, the single vanadium substitution structure ({P2W17V}) possesses 1-electron redox active and sequential proton-electron transfer behavior, while the tri-vanadium substituted cluster ({P2W15V3}) exhibits 3-electron redox active and cooperative proton electron transfer behavior. Based on the developed multi-electronic redox mediator with pH buffering capacity, suitable redox potential (0.6 V), and fast electron exchange rate, we build a photocatalysis-electrolysis relay water splitting system. This system allows for high capacity of solar energy storage through photocatalytic O2 evolution using BiVO4 photocatalyst and stable H2 production with a high Faraday efficiency of over 98.5% in the electrolysis subsystem.https://doi.org/10.1038/s41467-025-58622-8 |
| spellingShingle | Li-Ping Cui Shu Zhang Yue Zhao Xin-Yue Ge Le Yang Ke Li Liu-Bin Feng Ren-Gui Li Jia-Jia Chen Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight Nature Communications |
| title | Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight |
| title_full | Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight |
| title_fullStr | Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight |
| title_full_unstemmed | Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight |
| title_short | Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight |
| title_sort | tunable multi electron redox polyoxometalates for decoupled water splitting driven by sunlight |
| url | https://doi.org/10.1038/s41467-025-58622-8 |
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