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<p>Although covalent organic framework (COF)-based photocatalysts show advantages in visible-light-driven photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production, enhancing the photogenerated carrier transfer efficiency to boost overall H<sub>2</sub>O<sub>2</sub> production remains challenging. Here, based on Schiff base reactions of 2,4,6-triformylphloroglucinol (Tp) with <i>p</i>-phenylenediamine (Pa) and 3,6-pyridazinediamine (Dz), a COF/COF type-II heterojunction, TpPa/TpDz, was constructed. TpPa/TpDz achieved a photocatalytic H<sub>2</sub>O<sub>2</sub> production of 24.42 mmol g<sup>−1</sup> h<sup>−1</sup> in pure water, demonstrating exceptional performance among organic material-based photocatalysts under comparable conditions. Mechanism studies revealed that the almost complete separation of the highest occupied and lowest unoccupied molecular orbitals in the type-II heterojunction allows efficient and directional transport of photogenerated carriers, enabling efficient photocatalytic H<sub>2</sub>O<sub>2</sub> synthesis. This work illustrates the advantages of the design of COF-based heterojunction photocatalysts for H<sub>2</sub>O<sub>2</sub> production, offering insights and strategies for developing high-performance COF-based systems for the synthesis of value-added products.</p><p></p>

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Engineering a covalent organic framework-based type-II heterojunction for enhanced photocatalytic H2O2 synthesis

  • 期刊论文

  • 发表日期：

    2025年9月24日

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  • Hongyan Guo,
  • Shiyong Wang,
  • Xin Chen,
  • Jingfang Kou,
  • Guoqiang He,
  • Zhengping Dong,
  • Yong Yan

摘要

Although covalent organic framework (COF)-based photocatalysts show advantages in visible-light-driven photocatalytic hydrogen peroxide (H2O2) production, enhancing the photogenerated carrier transfer efficiency to boost overall H2O2 production remains challenging. Here, based on Schiff base reactions of 2,4,6-triformylphloroglucinol (Tp) with p-phenylenediamine (Pa) and 3,6-pyridazinediamine (Dz), a COF/COF type-II heterojunction, TpPa/TpDz, was constructed. TpPa/TpDz achieved a photocatalytic H2O2 production of 24.42 mmol g−1 h−1 in pure water, demonstrating exceptional performance among organic material-based photocatalysts under comparable conditions. Mechanism studies revealed that the almost complete separation of the highest occupied and lowest unoccupied molecular orbitals in the type-II heterojunction allows efficient and directional transport of photogenerated carriers, enabling efficient photocatalytic H2O2 synthesis. This work illustrates the advantages of the design of COF-based heterojunction photocatalysts for H2O2 production, offering insights and strategies for developing high-performance COF-based systems for the synthesis of value-added products.