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<p>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 H<sub>2</sub> and O<sub>2</sub> 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 ({P<sub>2</sub>W<sub>17</sub>V}) possesses 1-electron redox active and sequential proton-electron transfer behavior, while the tri-vanadium substituted cluster ({P<sub>2</sub>W<sub>15</sub>V<sub>3</sub>}) 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 O<sub>2</sub> evolution using BiVO<sub>4</sub> photocatalyst and stable H<sub>2</sub> production with a high Faraday efficiency of over 98.5% in the electrolysis subsystem.</p>

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Tunable multi-electron redox polyoxometalates for decoupled water splitting driven by sunlight

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月17日

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  • Li-Ping Cui,
  • Shu Zhang,
  • Yue Zhao,
  • Xin-Yue Ge,
  • Le Yang,
  • Ke Li,
  • Liu-Bin Feng,
  • Ren-Gui Li,
  • Jia-Jia Chen

摘要

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.