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<p>The investigation of charge carrier kinetics has long been a cornerstone of polymer photocatalysis research. However, the role of proton transport behavior in photocatalytic processes has often been underappreciated, despite its fundamental importance in proton-coupled electron-transfer reactions. Addressing this gap, we present a novel BF2-bridged covalent organic framework (C2-COF-BF2) that undergoes post-synthetic modification with boron trifluoride, designed to confer a dual functional advantage. Specifically, the incorporated BF<sub>2</sub> moieties are engineered to induce a donor-acceptor effect and potentially serve as continuous supply sites for activated protons. This bifunctional role not only enhances charge separation and migration while suppressing electron-hole recombination but also facilitates proton transport, thereby enabling improved performance in both photocatalytic hydrogen evolution reaction (HER) and H<sub>2</sub>O<sub>2</sub> production. Remarkably, the photocatalytic HER performance of C2-COF-BF2 (AQY<sub>450 nm</sub> = 8.78%) ranks among the highest efficiencies reported for COF-based photocatalysts to date. These findings highlight an innovative pathway for advancing the rational design of COF photocatalysts, offering a synergistic optimization of charge carrier kinetics and mass transfer processes to achieve unprecedented photocatalytic efficiency.</p>

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Modulating pyrene-based covalent organic framework via BF2 functionalization for facilitated photocatalytic proton-coupled electron-transfer reductions

  • 期刊论文

  • 发表日期：

    2025年7月21日

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  • Zhipeng Luo,
  • Xiaowen Chen,
  • Wanxiang Yang,
  • Yu Chang,
  • Shipeng Zhu,
  • Fengtao Zhang,
  • Wei Lin,
  • Gang Xu,
  • Guan-E Wang,
  • Xiong Chen

摘要

The investigation of charge carrier kinetics has long been a cornerstone of polymer photocatalysis research. However, the role of proton transport behavior in photocatalytic processes has often been underappreciated, despite its fundamental importance in proton-coupled electron-transfer reactions. Addressing this gap, we present a novel BF2-bridged covalent organic framework (C2-COF-BF2) that undergoes post-synthetic modification with boron trifluoride, designed to confer a dual functional advantage. Specifically, the incorporated BF2 moieties are engineered to induce a donor-acceptor effect and potentially serve as continuous supply sites for activated protons. This bifunctional role not only enhances charge separation and migration while suppressing electron-hole recombination but also facilitates proton transport, thereby enabling improved performance in both photocatalytic hydrogen evolution reaction (HER) and H2O2 production. Remarkably, the photocatalytic HER performance of C2-COF-BF2 (AQY450 nm = 8.78%) ranks among the highest efficiencies reported for COF-based photocatalysts to date. These findings highlight an innovative pathway for advancing the rational design of COF photocatalysts, offering a synergistic optimization of charge carrier kinetics and mass transfer processes to achieve unprecedented photocatalytic efficiency.