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<p>Promoting the photocatalytic proton-coupled electron transfer (PCET) kinetics in the two-electron oxygen reduction reaction (2e<sup>−</sup> ORR) is crucial for the photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production. Herein, four kinds of covalent organic frameworks (COFs) were successfully prepared <i>via</i> a sub-stoichiometric strategy through a one-step solvothermal method. Among them, B<sub>1.5</sub>T<sub>1</sub>-COF with polar aldehyde groups displays a high photocatalytic H<sub>2</sub>O<sub>2</sub> generation rate of 1081.8 µmol·g<sup>−1</sup>·h<sup>−1</sup>, which is 3 times higher than that of B<sub>1</sub>T<sub>1.5</sub>-COF and 2 times higher than that of B<sub>1</sub>T<sub>1</sub>-COF. Through the corresponding experiments and density functional theory (DFT) calculation, the photocatalytic mechanism is revealed that B<sub>1.5</sub>T<sub>1</sub>-COF with free aldehyde groups can raise the PCET kinetics for 2e<sup>−</sup> ORR with the aid of a stable transfer channel for e<sup>−</sup> and a favorable hydrogen donation for H<sup>+</sup>. This work might provide some insights for design and preparation of COFs with functional groups through a sub-stoichiometric strategy to modulate their photocatalytic activities.</p>

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Sub-stoichiometric Covalent Organic Frameworks with Boosted Photocatalytic Production of Hydrogen Peroxide via Promoting Proton-coupled Electron Transfer Kinetics

  • 期刊论文

  • 发表日期：

    2025年3月13日

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  • Shengrong Yan,
  • Bingyan Zhang,
  • Wenhao Liu,
  • Fang Duan,
  • Yujie Li,
  • Yanyan Ren,
  • Shuanglong Lu,
  • Mingliang Du,
  • Mingqing Chen

摘要

Promoting the photocatalytic proton-coupled electron transfer (PCET) kinetics in the two-electron oxygen reduction reaction (2e− ORR) is crucial for the photocatalytic hydrogen peroxide (H2O2) production. Herein, four kinds of covalent organic frameworks (COFs) were successfully prepared via a sub-stoichiometric strategy through a one-step solvothermal method. Among them, B1.5T1-COF with polar aldehyde groups displays a high photocatalytic H2O2 generation rate of 1081.8 µmol·g−1·h−1, which is 3 times higher than that of B1T1.5-COF and 2 times higher than that of B1T1-COF. Through the corresponding experiments and density functional theory (DFT) calculation, the photocatalytic mechanism is revealed that B1.5T1-COF with free aldehyde groups can raise the PCET kinetics for 2e− ORR with the aid of a stable transfer channel for e− and a favorable hydrogen donation for H+. This work might provide some insights for design and preparation of COFs with functional groups through a sub-stoichiometric strategy to modulate their photocatalytic activities.