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<p>Two-dimensional sp<sup>2</sup> carbon-conjugated covalent organic frameworks (2D sp<sup>2</sup>c-COFs), linked by olefin bonds, stand out in photo/electro catalysis and organic electronics, owing to the fast electron-hole separation and transportation in fully conjugated skeletons. However, the synthesis of highly crystalline 2D sp<sup>2</sup>c-COFs remains a formidable challenge, constrained by the inherently poor self-correcting capacity of robust olefin linkages and the limited adaptability of rigid 2D extended frameworks. Here, we show the synthesis of highly crystalline 2D sp<sup>2</sup>c-COFs from corresponding imine-linked COFs through imine-to-olefin transformation. The resulting 2D sp<sup>2</sup>c-COFs maintain their high crystallinity and porosity, with complete conversion of imine bonds to olefin bonds. In addition, the imine-to-olefin transformation leads to a significant redshift (ca. 250 nm) of the light absorption edge and a sixfold increase of photocurrent. Especially, the transformed 2D sp<sup>2</sup>c-COF shows a record photocatalytic hydrogen evolution rate up to 4006 µmol g<sup>−1</sup> h<sup>−1</sup> without metal co-catalyst under simulated sunlight irradiation. The findings highlight the importance of imine-to-olefin linkage transformation in enhancing the photocatalytic properties of 2D COFs.</p>

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Highly crystalline 2D sp2c-COFs synthesized via linkage transformation for metal-free photocatalysis with exceptional hydrogen production

  • 期刊论文

  • 发表日期：

    2026年1月4日

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  • Shengxu Li,
  • Haoyong Yang,
  • Junyi Han,
  • Quanquan Yang,
  • Qunji Xue,
  • Tao Zhang

摘要

Two-dimensional sp2 carbon-conjugated covalent organic frameworks (2D sp2c-COFs), linked by olefin bonds, stand out in photo/electro catalysis and organic electronics, owing to the fast electron-hole separation and transportation in fully conjugated skeletons. However, the synthesis of highly crystalline 2D sp2c-COFs remains a formidable challenge, constrained by the inherently poor self-correcting capacity of robust olefin linkages and the limited adaptability of rigid 2D extended frameworks. Here, we show the synthesis of highly crystalline 2D sp2c-COFs from corresponding imine-linked COFs through imine-to-olefin transformation. The resulting 2D sp2c-COFs maintain their high crystallinity and porosity, with complete conversion of imine bonds to olefin bonds. In addition, the imine-to-olefin transformation leads to a significant redshift (ca. 250 nm) of the light absorption edge and a sixfold increase of photocurrent. Especially, the transformed 2D sp2c-COF shows a record photocatalytic hydrogen evolution rate up to 4006 µmol g−1 h−1 without metal co-catalyst under simulated sunlight irradiation. The findings highlight the importance of imine-to-olefin linkage transformation in enhancing the photocatalytic properties of 2D COFs.