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<p>Photocatalytic hydrogen evolution by noble-metal-free systems holds great promise for sustainable conversion of solar energy to hydrogen, and it is crucial and challenging to develop highly efficient photocatalysts. This study presents a framework dyad based on metal-organic frameworks and photoactive covalent organic frameworks, which are synchronously constructed through covalent linkages. The experimental and density functional theory calculation results show that the interfacial covalent linkages and intimate contact of the framework dyads improve the visible-light absorption efficiency, promote the separation and migration of the photogenerated charge carriers, and provide sufficient active sites for water activation, thus accelerating the photocatalytic reaction kinetics for hydrogen generation. The hydrogen evolution rate of this dyad is as high as 7.696 mmol g<sup>−1</sup> h<sup>−1</sup> in the absence of the additional cocatalysts and photosensitizers, which is significantly enhanced compared to their individual counterparts and their physical mixture. This work provides an elegant approach for the development of noble-metal free double framework photocatalytic systems for solar energy conversion.</p>

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Synchronous covalent linkage of double framework dyads for boosting photocatalytic hydrogen evolution

  • 期刊论文

  • 发表日期：

    2025年4月15日

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  • Zhijie Liu,
  • Tiantian Ma,
  • Jun Liang,
  • Duanhui Si,
  • Taotao Liu,
  • Fushuai Zhang,
  • Jian Sheng,
  • Qiao Wu,
  • Ruihu Wang

摘要

Photocatalytic hydrogen evolution by noble-metal-free systems holds great promise for sustainable conversion of solar energy to hydrogen, and it is crucial and challenging to develop highly efficient photocatalysts. This study presents a framework dyad based on metal-organic frameworks and photoactive covalent organic frameworks, which are synchronously constructed through covalent linkages. The experimental and density functional theory calculation results show that the interfacial covalent linkages and intimate contact of the framework dyads improve the visible-light absorption efficiency, promote the separation and migration of the photogenerated charge carriers, and provide sufficient active sites for water activation, thus accelerating the photocatalytic reaction kinetics for hydrogen generation. The hydrogen evolution rate of this dyad is as high as 7.696 mmol g−1 h−1 in the absence of the additional cocatalysts and photosensitizers, which is significantly enhanced compared to their individual counterparts and their physical mixture. This work provides an elegant approach for the development of noble-metal free double framework photocatalytic systems for solar energy conversion.