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<p>A critical challenge in solar-driven water splitting is developing efficient photocatalysts for the oxygen evolution reaction without relying on metal cocatalysts. Herein, we address this challenge by employing amide linkage engineering in donor–acceptor covalent organic polymers (COPs). Two such polymers, COP-M and COP-I, were synthesized via straightforward sol–gel condensation of acyl chlorides (donor) and melamine (acceptor). The inherent donor–acceptor structure of these COPs imparts an appropriate bandgap (~ 2.9&#xa0;eV), facilitating effective intramolecular charge separation. Remarkably, these metal-free COPs exhibit intrinsic visible-light-driven oxygen evolution activity without any metal cocatalysts. Their performance can be enhanced approximately fivefold by introducing Co<sup>2+</sup>, with COP-M achieving an optimal O<sub>2</sub> evolution rate of 106&#xa0;μmol/h. Both experimental and theoretical analyses suggest that the polar amide bond enhances surface hydrophilicity and modulates the thermodynamic barrier for initial water activation. Additionally, enhanced charge separation and transfer kinetics within the symmetrical donor–acceptor architecture of COP-M underscore its enhanced performance. This study emphasizes the collaborative role of amide linkages and donor–acceptor motifs in designing metal-free polymer photocatalysts, offering a strategy for artificial photosynthesis.</p>

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Amide-Linked Donor–Acceptor Covalent Organic Polymer Photocatalysts for Visible-Light-Driven Water Oxidation Without Metal Cocatalysts

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年5月25日

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  • Kai Yu,
  • Mingwen Zhang,
  • Dengke Chen,
  • Shuyang Lin,
  • Xiuqiang Lu,
  • Yibin Chen,
  • Yudiao Lin,
  • Zhaoyu Wang,
  • Zhitao Chen,
  • Wenqing Yang,
  • Liren Xiao,
  • Wei Ren,
  • Chenglong Ru,
  • Zhi-An Lan

摘要

A critical challenge in solar-driven water splitting is developing efficient photocatalysts for the oxygen evolution reaction without relying on metal cocatalysts. Herein, we address this challenge by employing amide linkage engineering in donor–acceptor covalent organic polymers (COPs). Two such polymers, COP-M and COP-I, were synthesized via straightforward sol–gel condensation of acyl chlorides (donor) and melamine (acceptor). The inherent donor–acceptor structure of these COPs imparts an appropriate bandgap (~ 2.9 eV), facilitating effective intramolecular charge separation. Remarkably, these metal-free COPs exhibit intrinsic visible-light-driven oxygen evolution activity without any metal cocatalysts. Their performance can be enhanced approximately fivefold by introducing Co2+, with COP-M achieving an optimal O2 evolution rate of 106 μmol/h. Both experimental and theoretical analyses suggest that the polar amide bond enhances surface hydrophilicity and modulates the thermodynamic barrier for initial water activation. Additionally, enhanced charge separation and transfer kinetics within the symmetrical donor–acceptor architecture of COP-M underscore its enhanced performance. This study emphasizes the collaborative role of amide linkages and donor–acceptor motifs in designing metal-free polymer photocatalysts, offering a strategy for artificial photosynthesis.