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<p>Covalent organic frameworks with three-dimensional networks and interconnected porous structures show promising advantages for hydrogen peroxide photocatalysis. However, 3D COFs are typically constructed from 3D-oriented knots with less conjugation and insufficient light absorption, which significantly inhibits their performance. Herein, we present a universal defect engineering approach by systematically replacing <i>T</i><sub><i>d</i></sub> knots with trigonal planar ligands and modifying linear linkers with electron-withdrawing/donating groups to achieve simultaneous enhancement of light absorption and precise electronic tuning of 3D donor-acceptor structures. Experimental results and theoretical analysis reveal that the optimized 3D COF with planar ligands induced defects and fluorine functional groups (COF-300-D-F), which achieve an H<sub>2</sub>O<sub>2</sub> production rate of 19.09 mmol g<sup>−1</sup> h<sup>−1</sup> and apparent quantum yield of 11.95% at 400 nm with benzyl alcohol as sacrificial agent. Moreover, the material maintains long-term stability during continuous operation exceeding 96 hours and exhibits high activity in photocatalytic benzylamine coupling reactions.</p>

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Defective three-dimensional covalent organic frameworks for enhanced hydrogen peroxide photosynthesis and organic transformation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月27日

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  • Tengteng Dong,
  • Xiaohui Xu,
  • Li Chen,
  • Jiani Yang,
  • Mengchao Guo,
  • Mi Zhou,
  • Min Xu,
  • Weichao Xue,
  • Xiancheng Ren,
  • Shuang Li,
  • Chong Cheng

摘要

Covalent organic frameworks with three-dimensional networks and interconnected porous structures show promising advantages for hydrogen peroxide photocatalysis. However, 3D COFs are typically constructed from 3D-oriented knots with less conjugation and insufficient light absorption, which significantly inhibits their performance. Herein, we present a universal defect engineering approach by systematically replacing Td knots with trigonal planar ligands and modifying linear linkers with electron-withdrawing/donating groups to achieve simultaneous enhancement of light absorption and precise electronic tuning of 3D donor-acceptor structures. Experimental results and theoretical analysis reveal that the optimized 3D COF with planar ligands induced defects and fluorine functional groups (COF-300-D-F), which achieve an H2O2 production rate of 19.09 mmol g−1 h−1 and apparent quantum yield of 11.95% at 400 nm with benzyl alcohol as sacrificial agent. Moreover, the material maintains long-term stability during continuous operation exceeding 96 hours and exhibits high activity in photocatalytic benzylamine coupling reactions.