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<p>Covalent organic frameworks (COFs) are emerging as a versatile class of crystalline porous polymers, yet their application in charge-related energy storage is hindered by intrinsically low electrical conductivity. Here we report the design and synthesis of a single-crystalline two-dimensional (2D) COF (<b>TBP-COF</b>) constructed from a newly developed tetrabenzo[a,c,h,j]phenazine (TBP) monomer and a pyrene-based linker. The incorporation of the planar <i>π</i>-extended TBP unit endows the framework with long-range <i>π</i>-conjugation, structural rigidity, and abundant redox-active sites. Benefiting from these features, <b>TBP-COF</b> exhibits exceptional chemical and thermal stability as well as a high specific surface area. Moreover, leveraging the strong <i>π</i>-<i>π</i> interactions between the extended TBP backbone and carbon nanotubes (CNTs), we developed an interfacial co-assembly strategy to construct <b>TBP-COF@CNT</b> hybrid composites. This approach enables the formation of intimately integrated architectures in which single-crystalline <b>TBP-COF</b> domains are uniformly anchored on CNT networks, ensuring efficient charge transport and mechanical integrity. When evaluated as anode materials for lithium-ion batteries, <b>TBP-COF@CNT</b> composites deliver high specific capacity, outstanding rate capability, and excellent cycling stability, surpassing their pristine counterpart. This work introduces TBP as a new <i>π</i>-conjugated building block for COFs and demonstrates a generalizable strategy to engineer highly conductive COF-based hybrid materials for advanced electrochemical energy storage.</p>

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Large π-conjugated building blocks enable highly crystalline 2D covalent organic frameworks for high-performance lithium-ion batteries

  • 期刊论文

  • 发表日期：

    2026年7月24日

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  • Shuo Wang,
  • Yu Wu,
  • Hui Liu,
  • Jialin Cui,
  • Xuhan Zheng,
  • Guoxing Li,
  • Shiwei Liu,
  • Yingjie Zhao

摘要

Covalent organic frameworks (COFs) are emerging as a versatile class of crystalline porous polymers, yet their application in charge-related energy storage is hindered by intrinsically low electrical conductivity. Here we report the design and synthesis of a single-crystalline two-dimensional (2D) COF (TBP-COF) constructed from a newly developed tetrabenzo[a,c,h,j]phenazine (TBP) monomer and a pyrene-based linker. The incorporation of the planar π-extended TBP unit endows the framework with long-range π-conjugation, structural rigidity, and abundant redox-active sites. Benefiting from these features, TBP-COF exhibits exceptional chemical and thermal stability as well as a high specific surface area. Moreover, leveraging the strong π-π interactions between the extended TBP backbone and carbon nanotubes (CNTs), we developed an interfacial co-assembly strategy to construct TBP-COF@CNT hybrid composites. This approach enables the formation of intimately integrated architectures in which single-crystalline TBP-COF domains are uniformly anchored on CNT networks, ensuring efficient charge transport and mechanical integrity. When evaluated as anode materials for lithium-ion batteries, TBP-COF@CNT composites deliver high specific capacity, outstanding rate capability, and excellent cycling stability, surpassing their pristine counterpart. This work introduces TBP as a new π-conjugated building block for COFs and demonstrates a generalizable strategy to engineer highly conductive COF-based hybrid materials for advanced electrochemical energy storage.