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<p>Photocatalytic hydrogen evolution using solar energy is a promising approach for sustainable energy conversion, yet homogeneous metal cluster catalysts often suffer from instability and inefficient charge separation. Herein, we report a confinement strategy by embedding bimetallic trinuclear Fe<sub>2</sub>M (M = Co, Ni, Zn) clusters into a thiazole-based covalent organic framework (COF). The resulting COF@Fe<sub>2</sub>M hybrids combine the redox activity of metal clusters with the photoactive and porous architecture of COFs. Among them, COF@Fe<sub>2</sub>Co exhibits the highest activity, achieving 93.16 mmol g<Stack> <sub>co</sub> <sup>−1</sup> </Stack> h<sup>−1</sup> of H<sub>2</sub> in a 10 h irradiation, 5.8 times that of the physical mixture. Spectroscopic and electrochemical studies reveal efficient interfacial charge transfer, while density functional theory (DFT) calculations show that the Fe<sub>2</sub>Co cluster has the most favorable electronic structure and hydrogen adsorption energy. This work offers a rational platform for designing efficient hybrid photocatalysts.</p>

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Confinement engineering of metal clusters within covalent organic frameworks for enhanced photocatalytic hydrogen evolution

  • 期刊论文

  • 发表日期：

    2026年1月4日

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  • Yuchen Wang,
  • Yong Zheng,
  • Wenjie Shi,
  • Dichang Zhong,
  • Tongbu Lu

摘要

Photocatalytic hydrogen evolution using solar energy is a promising approach for sustainable energy conversion, yet homogeneous metal cluster catalysts often suffer from instability and inefficient charge separation. Herein, we report a confinement strategy by embedding bimetallic trinuclear Fe2M (M = Co, Ni, Zn) clusters into a thiazole-based covalent organic framework (COF). The resulting COF@Fe2M hybrids combine the redox activity of metal clusters with the photoactive and porous architecture of COFs. Among them, COF@Fe2Co exhibits the highest activity, achieving 93.16 mmol g co −1 h−1 of H2 in a 10 h irradiation, 5.8 times that of the physical mixture. Spectroscopic and electrochemical studies reveal efficient interfacial charge transfer, while density functional theory (DFT) calculations show that the Fe2Co cluster has the most favorable electronic structure and hydrogen adsorption energy. This work offers a rational platform for designing efficient hybrid photocatalysts.