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<p>Covalent organic frameworks (COFs) are porous crystalline nanomaterials with great potential, but the limited symmetry and connectivity of their building units often lead to single topological structures and insoluble aggregate products, hindering detailed structure-property investigations and applications. To address these challenges, we introduce a “ligand spatial-driven topological-morphological regulation” strategy. By precisely modulating methoxy group substitution on ligands, we control interlayer non-covalent interactions in imine-based COFs, inducing dynamic “depolymerization-reconstruction” behavior. This allows for the construction of 2D COF topoisomers (sql and kgm) and 1D crystalline polymer. Iodine adsorption studies show that interlayer stacking and pore environments greatly affect guest molecule transport. The para-methoxy COF (<i>p</i>DMTA-sql) achieves high iodine uptake (6.16 g g<sup>−1</sup>), attributed to strong interlayer interactions and effective utilization of active sites, while the ortho-methoxy COF (<i>o</i>DMTA-kgm) exhibits thermally induced solubility, enabling the solution-processable fabrication of COF aerogels and thin films. The macroscopic shaped COFs show excellent iodine adsorption in both gas and liquid phases, as well as superior organic pollutant capture and oil-water separation capabilities. This work highlights the role of non-covalent interactions in topological evolution, framework stability, and solubility via rational ligand design, broadening the structural design and processing of COF materials and offering new insights for efficient environmental sorbents.</p>

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Spatial ligand design unlocks topological diversity and solution-processing shaping of covalent organic frameworks

  • 期刊论文

  • 发表日期：

    2026年1月7日

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  • Bo Jiang,
  • Ting Jiang,
  • Kaifu Yu,
  • Xiang Pei,
  • Yang Li,
  • Lijian Ma

摘要

Covalent organic frameworks (COFs) are porous crystalline nanomaterials with great potential, but the limited symmetry and connectivity of their building units often lead to single topological structures and insoluble aggregate products, hindering detailed structure-property investigations and applications. To address these challenges, we introduce a “ligand spatial-driven topological-morphological regulation” strategy. By precisely modulating methoxy group substitution on ligands, we control interlayer non-covalent interactions in imine-based COFs, inducing dynamic “depolymerization-reconstruction” behavior. This allows for the construction of 2D COF topoisomers (sql and kgm) and 1D crystalline polymer. Iodine adsorption studies show that interlayer stacking and pore environments greatly affect guest molecule transport. The para-methoxy COF (pDMTA-sql) achieves high iodine uptake (6.16 g g−1), attributed to strong interlayer interactions and effective utilization of active sites, while the ortho-methoxy COF (oDMTA-kgm) exhibits thermally induced solubility, enabling the solution-processable fabrication of COF aerogels and thin films. The macroscopic shaped COFs show excellent iodine adsorption in both gas and liquid phases, as well as superior organic pollutant capture and oil-water separation capabilities. This work highlights the role of non-covalent interactions in topological evolution, framework stability, and solubility via rational ligand design, broadening the structural design and processing of COF materials and offering new insights for efficient environmental sorbents.