<p>As a means of addressing the intrinsically poor electrical conductivity and sluggish ion transport of covalent organic frameworks (COFs) that limit their capacitive performance, this study demonstrates that embedding electron-deficient, highly symmetric triazine rings into the backbone enhances electrochemical activity and ion accessibility. Herein, COF-R<sub>TAPB</sub> and COF-R<sub>TAPT</sub> were synthesized via Schiff base condensation of tris(4-aminophenyl)amine (TAPA) with 1,3,5-tris(<i>p</i>-formyl phenyl)benzene (TFPB) and 2,4,6-tris(4-formylphenyl)-1,3,5-triazine (TFPT), respectively. Compared to their benzene-centered counterparts, the triazine rings impart strong electronegativity and electron-withdrawing characteristics, effectively enhancing the intrinsic electrical conductivity of the COF material. Furthermore, their highly symmetric planar structure is conducive to forming more ordered pore channels, thereby facilitating ion diffusion. Electrochemical measurements reveal that the triazine-incorporated COF-R<sub>TAPT</sub> significantly outperforms COF-R<sub>TAPB</sub>, delivering specific capacitance of 291&#xa0;F&#xa0;g<sup>−1</sup> at 0.1&#xa0;A&#xa0;g<sup>−1</sup> and demonstrating excellent stability with a capacitance retention of 105.63% after 10,000 cycles, which may be attributed to the progressive activation of the electrode material or improved surface wetting during cycling. By elucidating the superior electronic structures, morphological features, and electrochemical properties of triazine-based COFs over traditional phenyl-based analogs, this work provides a strategy for the rational design of advanced COF materials for supercapacitor applications.</p>

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Comparison Study on the Capacitive Properties of Covalent Organic Frameworks Synthesized Using Triphenylaldehyde with Benzene and Triazine Cores and Triphenylamine-Based Amine as Building Blocks

  • Zijing Zheng,
  • Shanxin Xiong,
  • Yukun Zhang,
  • Shuai Zhang,
  • Qingyong Duan,
  • Hepeng Lu,
  • Xiaoqin Wang,
  • Jinhang Li,
  • Ming Gong

摘要

As a means of addressing the intrinsically poor electrical conductivity and sluggish ion transport of covalent organic frameworks (COFs) that limit their capacitive performance, this study demonstrates that embedding electron-deficient, highly symmetric triazine rings into the backbone enhances electrochemical activity and ion accessibility. Herein, COF-RTAPB and COF-RTAPT were synthesized via Schiff base condensation of tris(4-aminophenyl)amine (TAPA) with 1,3,5-tris(p-formyl phenyl)benzene (TFPB) and 2,4,6-tris(4-formylphenyl)-1,3,5-triazine (TFPT), respectively. Compared to their benzene-centered counterparts, the triazine rings impart strong electronegativity and electron-withdrawing characteristics, effectively enhancing the intrinsic electrical conductivity of the COF material. Furthermore, their highly symmetric planar structure is conducive to forming more ordered pore channels, thereby facilitating ion diffusion. Electrochemical measurements reveal that the triazine-incorporated COF-RTAPT significantly outperforms COF-RTAPB, delivering specific capacitance of 291 F g−1 at 0.1 A g−1 and demonstrating excellent stability with a capacitance retention of 105.63% after 10,000 cycles, which may be attributed to the progressive activation of the electrode material or improved surface wetting during cycling. By elucidating the superior electronic structures, morphological features, and electrochemical properties of triazine-based COFs over traditional phenyl-based analogs, this work provides a strategy for the rational design of advanced COF materials for supercapacitor applications.