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<p>Two-dimensional covalent organic frameworks (2D COFs) have garnered considerable scientific interest on account of their special aggregated structures consisting of extended molecular sheets stacked in layers to form periodic columnar <i>π</i> arrays and open porous channels. The configurable functional groups and controllable molecular stacks in 2D COFs offer a programmable platform for developing advanced luminescent systems. However, precise manipulation of their photophysical properties and thorough understanding of their excited state dynamics remain fundamentally challenging. Here we report two imine-linked 2D COF powders that exhibit thermally activated delayed fluorescence, in which long-range order and dense stacking minimize the singlet–triplet splitting energy and promote reverse intersystem crossing. By engineering interlayer stacking modes and external environments, dynamic manipulation of photoluminescence from delayed fluorescence to phosphorescence is established in 2D COFs. Specifically, the interlayer insertion of solvent molecules and cryogenic rigidification enhance phosphorescence emissions of 2D COFs at 77 K. We observe photoactivated room temperature phosphorescence behaviour with lifetimes of up to 1.26 s and exceptional long-term stability exceeding 20 months from embedded COF dispersions in three-dimensional crosslinked epoxy matrix by in situ polymerization. The potential applications of these COF@epoxy composites in three-dimensional manufacturing, antibacterial treatment and erasable light printing are demonstrated.</p>

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Dynamic manipulation of photoluminescence in two-dimensional covalent organic frameworks

  • 期刊论文

  • 发表日期：

    2026年3月16日

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  • Jingjing Guo,
  • Shuai Bi,
  • Ting He,
  • Yu Cheng,
  • Shihuai Wang,
  • Zhifang Wang,
  • Xiaobin Dong,
  • Yue Zhao,
  • Zujin Zhao,
  • Ben Zhong Tang,
  • Yanli Zhao

摘要

Two-dimensional covalent organic frameworks (2D COFs) have garnered considerable scientific interest on account of their special aggregated structures consisting of extended molecular sheets stacked in layers to form periodic columnar π arrays and open porous channels. The configurable functional groups and controllable molecular stacks in 2D COFs offer a programmable platform for developing advanced luminescent systems. However, precise manipulation of their photophysical properties and thorough understanding of their excited state dynamics remain fundamentally challenging. Here we report two imine-linked 2D COF powders that exhibit thermally activated delayed fluorescence, in which long-range order and dense stacking minimize the singlet–triplet splitting energy and promote reverse intersystem crossing. By engineering interlayer stacking modes and external environments, dynamic manipulation of photoluminescence from delayed fluorescence to phosphorescence is established in 2D COFs. Specifically, the interlayer insertion of solvent molecules and cryogenic rigidification enhance phosphorescence emissions of 2D COFs at 77 K. We observe photoactivated room temperature phosphorescence behaviour with lifetimes of up to 1.26 s and exceptional long-term stability exceeding 20 months from embedded COF dispersions in three-dimensional crosslinked epoxy matrix by in situ polymerization. The potential applications of these COF@epoxy composites in three-dimensional manufacturing, antibacterial treatment and erasable light printing are demonstrated.