Redox‐active covalent organic frameworks (COFs) have been demonstrated as promising organic electrodes in many electrochemical devices. However, their inherently low conductivity significantly hinders the full utilization of their internal redox‐active sites. To address this issue, a simple solvothermal method is used to in situ polymerize 2,4,6‐triformylphloroglucinol (TP) and p‐phenylenediamine (PA) on the surface of carbon nanotubes (CNTs), generating a nanocable‐like COF‐based nanocomposite, TpPa‐COF@CNT nanocables, which contain abundant β‐ketoenamine groups. By combining the high specific surface area and dense active sites of COFs with the superior conductivity of CNTs, the TpPa‐COF@CNT nanocables as the anode in potassium‐ion batteries displayed excellent performance. The reason is that the isomerization between the enolic and keto forms reinforces the stability of molecular architecture, while the transformation of active sites from C=N to C=O improves the K+ adsorption capability. Notably, the TpPa‐COF@CNT nanocable anode exhibits a high reversible capacity of 446.1 mAh g−1 at 0.1 A g−1 and maintains 282.5 mAh g−1 even after 2000 cycles at a higher current density of 2.0 A g−1. Additionally, a full battery assembled with 3,4,9,10‐Perylenetetracarboxylic dianhydride heat‐treated at 450 °C as the cathode retains a reversible capacity of 273.6 mAh g−1 after 200 cycles at 0.1 A g−1.

中文翻译：

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用于高性能钾离子电池的碳纳米管上共价有机框架的原位生长


氧化还原活性共价有机框架 （COF） 已被证明是许多电化学器件中很有前途的有机电极。然而，它们固有的低电导率严重阻碍了其内部氧化还原活性位点的充分利用。为了解决这个问题，使用一种简单的溶剂热方法在碳纳米管 （CNT） 表面原位聚合 2,4,6-三甲酰间苯三酚 （TP） 和对苯二胺 （PA），生成一种类似纳米电缆的基于 COF 的纳米复合材料，TpPa-COF@CNT纳米电缆，其中包含丰富的 β-酮胺基团。通过将 COF 的高比表面积和致密的活性位点与 CNT 的卓越导电性相结合，作为钾离子电池负极的 TpPa-COF@CNT 纳米电缆表现出优异的性能。原因是 enolic 和 keto 形式之间的异构化增强了分子结构的稳定性，而活性位点从 C=N 到 C=O 的转变提高了 K+ 吸附能力。值得注意的是，TpPa-COF@CNT 纳米电缆阳极在 0.1 A g-1 时表现出 446.1 mAh g-1 的高可逆容量，即使在 2.0 A g-1 的较高电流密度下经过 2000 次循环后也能保持 282.5 mAh g-1。此外，在 450 °C 下热处理的 3,4,9,10-苝四羧酸二酐组装的完整电池，因为阴极在 0.1 A g-1 下循环 200 次后仍保持 273.6 mAh g-1 的可逆容量。