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<p>The photocatalytic synthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) represents a sustainable and environmentally friendly alternative to traditional industrial methods. However, its practical application is limited by the instability of organic photocatalysts, primarily caused by superoxide radical (·O<sub>2</sub><sup>−</sup>) induced degradation. Herein, we developed a novel conjugated polymer photocatalyst, Ethyl-AQ, which mitigates this limitation by suppressing ·O<sub>2</sub><sup>−</sup> generation by 70% and facilitating the formation of oxygen-centered organic radicals (OCORs) as intermediates for H<sub>2</sub>O<sub>2</sub> generation. Mechanistic studies revealed that the promotion of the generation of OCORs in Ethyl-AQ arises from its ability to direct photogenerated electrons to the carbonyl groups of anthraquinone (AQ), enabled by the enhanced electron-donating properties of its ethyl-functionalized donor. In contrast, Sulfonyl-AQ, containing electron-withdrawing substituents on its donor, is unable to effectively transfer photogenerated electrons to the AQ carbonyl groups, inhibiting the generation of OCORs and predominantly relying on the less stable ·O<sub>2</sub><sup>−</sup> pathway for H<sub>2</sub>O<sub>2</sub> production. Consequently, Ethyl-AQ demonstrated exceptional durability, maintaining consistent performance over 20 catalytic cycles without observable degradation, whereas Sulfonyl-AQ experienced significant degradation after only five cycles. This work highlights a strategic approach to enhancing the durability of organic photocatalysts for H<sub>2</sub>O<sub>2</sub> production.</p>

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Enhancing photocatalyst stability for hydrogen peroxide synthesis through promoting oxygen-centered organic radical formation

  • 期刊论文

  • 发表日期：

    2025年3月31日

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  • Pan Jiang,
  • Zuoming Chen,
  • Huijie Yan,
  • Shufang Liu,
  • Yuyan Huang,
  • Xiangqiong Jiang,
  • Xin Wu,
  • Xiantai Zhou,
  • Yu-Xin Ye,
  • Gangfeng Ouyang

摘要

The photocatalytic synthesis of hydrogen peroxide (H2O2) represents a sustainable and environmentally friendly alternative to traditional industrial methods. However, its practical application is limited by the instability of organic photocatalysts, primarily caused by superoxide radical (·O2−) induced degradation. Herein, we developed a novel conjugated polymer photocatalyst, Ethyl-AQ, which mitigates this limitation by suppressing ·O2− generation by 70% and facilitating the formation of oxygen-centered organic radicals (OCORs) as intermediates for H2O2 generation. Mechanistic studies revealed that the promotion of the generation of OCORs in Ethyl-AQ arises from its ability to direct photogenerated electrons to the carbonyl groups of anthraquinone (AQ), enabled by the enhanced electron-donating properties of its ethyl-functionalized donor. In contrast, Sulfonyl-AQ, containing electron-withdrawing substituents on its donor, is unable to effectively transfer photogenerated electrons to the AQ carbonyl groups, inhibiting the generation of OCORs and predominantly relying on the less stable ·O2− pathway for H2O2 production. Consequently, Ethyl-AQ demonstrated exceptional durability, maintaining consistent performance over 20 catalytic cycles without observable degradation, whereas Sulfonyl-AQ experienced significant degradation after only five cycles. This work highlights a strategic approach to enhancing the durability of organic photocatalysts for H2O2 production.