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<p>Slightly structural variation often leads to huge changes in the properties of the covalent organic frameworks (COFs). The atom-level precisely arranged structures of COFs make it possible to understand the structure-performance relationship. Here, four highly crystalline imine-linked benzothiadiazole-based COFs were constructed from precisely designed monomers. The effects of imine linkage orientation, the π bridge between the benzothiadiazole unit and imine linkage on the photocatalysis performance were systematically studied. It is noted that photocatalytic performance can be dramatically improved when the imine carbon atoms are attached to the pyrene-based unit. In addition, the extension of the π bridge in the benzothiadiazole units could obviously enhance the photocatalytic hydrogen evolution and weaken the hydrogen peroxide generation. The PC-NPB containing the diphenylbenzothiadiazole building block exhibited the highest hydrogen evolution rate of 15.7 mmol h<sup>−1</sup> g<sup>−1</sup>, 4.4 times higher than that of non-phenyl-substituted benzothiadiazole-containing PC-NB. Interestingly, PC-NB displayed the highest hydrogen peroxide generation rate of 1376 µmol h<sup>−1</sup> g<sup>−1</sup>, 2.8 times higher than that of PC-NPB.</p>

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Structural regulation of imine-linked benzothiadiazole-based covalent organic frameworks for efficient photocatalysis

  • 期刊论文

  • 发表日期：

    2025年3月19日

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  • Xin Zhao,
  • Yuancheng Wang,
  • Guangchao Han,
  • Guoye Yu,
  • Guanshi Ren,
  • Xiang Li,
  • Tongyang Zhang,
  • Lishui Sun,
  • Yingjie Zhao

摘要

Slightly structural variation often leads to huge changes in the properties of the covalent organic frameworks (COFs). The atom-level precisely arranged structures of COFs make it possible to understand the structure-performance relationship. Here, four highly crystalline imine-linked benzothiadiazole-based COFs were constructed from precisely designed monomers. The effects of imine linkage orientation, the π bridge between the benzothiadiazole unit and imine linkage on the photocatalysis performance were systematically studied. It is noted that photocatalytic performance can be dramatically improved when the imine carbon atoms are attached to the pyrene-based unit. In addition, the extension of the π bridge in the benzothiadiazole units could obviously enhance the photocatalytic hydrogen evolution and weaken the hydrogen peroxide generation. The PC-NPB containing the diphenylbenzothiadiazole building block exhibited the highest hydrogen evolution rate of 15.7 mmol h−1 g−1, 4.4 times higher than that of non-phenyl-substituted benzothiadiazole-containing PC-NB. Interestingly, PC-NB displayed the highest hydrogen peroxide generation rate of 1376 µmol h−1 g−1, 2.8 times higher than that of PC-NPB.