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<p>Vinylene-linked covalent organic frameworks (COFs) are renowned for their excellent organic semiconducting properties, attributed to their in-plane <i>π</i>-conjugated and robust structures. However, their synthesis remains challenging due to the complexity of reaction pathways and the limited availability of building units containing reactive methyl groups, which hinders their practical application. Herein, two vinylene-linked benzotristhiazole-based 2D COFs with high crystallinity were constructed via Aldol condensation reaction. Notably, the incorporation of fluorine atoms into the COF framework significantly enhanced its photocatalytic activity. Specifically, the fluorinated COF (BTZ-F) exhibited substantially improved performance in the selective oxidation of organic sulfides compared to its non-fluorinated counterpart (BTZ-H). A synergistic combination of experimental characterization and theoretical calculations revealed that fluorination significantly modulates the electronic structure of the framework, thereby promoting efficient charge separation and transfer. Further mechanistic investigations revealed that both electron-transfer and energy-transfer pathways are involved in the oxidation of phenyl methyl sulfide, providing deeper insights into the enhanced photocatalytic efficiency of the fluorinated framework.</p>

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Fluorination of vinylene-linked benzotristhiazole-based covalent organic frameworks for enhanced photocatalytic performance

  • 期刊论文

  • 发表日期：

    2026年3月18日

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  • Yuancheng Wang,
  • Zhipeng Luo,
  • Wenyu Zhou,
  • Luxi Tan,
  • Xin Zhao,
  • Jialin Cui,
  • Xiong Chen,
  • Yingjie Zhao

摘要

Vinylene-linked covalent organic frameworks (COFs) are renowned for their excellent organic semiconducting properties, attributed to their in-plane π-conjugated and robust structures. However, their synthesis remains challenging due to the complexity of reaction pathways and the limited availability of building units containing reactive methyl groups, which hinders their practical application. Herein, two vinylene-linked benzotristhiazole-based 2D COFs with high crystallinity were constructed via Aldol condensation reaction. Notably, the incorporation of fluorine atoms into the COF framework significantly enhanced its photocatalytic activity. Specifically, the fluorinated COF (BTZ-F) exhibited substantially improved performance in the selective oxidation of organic sulfides compared to its non-fluorinated counterpart (BTZ-H). A synergistic combination of experimental characterization and theoretical calculations revealed that fluorination significantly modulates the electronic structure of the framework, thereby promoting efficient charge separation and transfer. Further mechanistic investigations revealed that both electron-transfer and energy-transfer pathways are involved in the oxidation of phenyl methyl sulfide, providing deeper insights into the enhanced photocatalytic efficiency of the fluorinated framework.