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<p>The development of robust and efficient heterogeneous photocatalysts for water oxidation is a significant challenge in solar fuel production. Polyoxometalate-metal-organic framework composites (POM@MOFs) represent a promising platform, yet achieving optimal electronic interaction remains a key goal. We demonstrate that electronic communication between polyoxometalates (POMs) and metal-organic frameworks (MOFs) enhances charge transfer kinetics while suppressing electron-hole recombination, with maximum efficiency achieved through precise size-matching between MOF cavities and encapsulated POMs. This principle is illustrated by Co4@UiO-67 (C1), where encapsulation of Na₁₀[(PW₉O₃₄)₂Co₄(H₂O)₂] in UiO-67’s cavities creates a leaching-proof composite. This confinement prevents aggregation, yielding excellent photocatalytic water oxidation performance (283 TONs)—surpassing prior Co4@MOF systems. Mechanistic insights from photoluminescence reveal efficient charge separation, while post-catalytic analysis confirms structural integrity and reusability. Overall, this work introduces a new paradigm in the design of POM@MOF composites, positioning C1 as a robust, recyclable, and highly active photocatalyst for heterogeneous water oxidation.</p><p></p>

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Precise size-matching between guest polyoxometalates and host metal-organic frameworks enables enhanced photocatalytic water oxidation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月10日

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  • Waqas Ali Shah,
  • Xusheng Dai,
  • Xiaowei Zhai,
  • Yuanyuan Zhao,
  • Yalei Zhang,
  • Shujun Li

摘要

The development of robust and efficient heterogeneous photocatalysts for water oxidation is a significant challenge in solar fuel production. Polyoxometalate-metal-organic framework composites (POM@MOFs) represent a promising platform, yet achieving optimal electronic interaction remains a key goal. We demonstrate that electronic communication between polyoxometalates (POMs) and metal-organic frameworks (MOFs) enhances charge transfer kinetics while suppressing electron-hole recombination, with maximum efficiency achieved through precise size-matching between MOF cavities and encapsulated POMs. This principle is illustrated by Co4@UiO-67 (C1), where encapsulation of Na₁₀[(PW₉O₃₄)₂Co₄(H₂O)₂] in UiO-67’s cavities creates a leaching-proof composite. This confinement prevents aggregation, yielding excellent photocatalytic water oxidation performance (283 TONs)—surpassing prior Co4@MOF systems. Mechanistic insights from photoluminescence reveal efficient charge separation, while post-catalytic analysis confirms structural integrity and reusability. Overall, this work introduces a new paradigm in the design of POM@MOF composites, positioning C1 as a robust, recyclable, and highly active photocatalyst for heterogeneous water oxidation.