Covalent organic frameworks (COFs) possessing a well-defined structure and abundant functional groups are prospective pseudocapacitive electrode materials. However, their intrinsic poor electrical conductivity and stacking problems usually impede the utilization of their active sites. Herein, we conduct an in situ growth of polyimide COFs (donated as NTDA COFs) enriched with carbonyl groups on multiwalled carbon nanotubes (MWCNTs). An impressive capacitance of 467 F g^–1 at 1 A g^–1 is achieved for the as-prepared NTDA/MWCNTs composite, significantly surpassing both the pure MWCNTs (60.3 F g^–1) and NTDA COFs (284.4 F g^–1). No decay of capacitance is observed after 10,000 cycles at 10 A g^–1. The assembled device NTDA/MWCNTs//activated carbon reaches a high energy density of 17 Wh kg^–1 at 750 W kg^–1 while keeping superior charging/discharging stability of 89.5% after cycling for 19,000 times at 10 A g^–1. In situ Fourier transform infrared (in situ FT-IR) tests together with the exploration of electrode kinetics show that the boosted capacitance of NTDA/MWCNTs is mainly donated by the redox reactions of carbonyl groups on NTDA COFs, which is largely activated by MWCNTs.

中文翻译：

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具有多壁碳纳米管的聚酰亚胺基共价有机框架中羰基的活化，以提高赝电容


具有明确结构和丰富官能团的共价有机框架 （COFs） 是前瞻性的伪电容电极材料。然而，它们固有的导电性差和堆叠问题通常会阻碍其活性位点的利用。在此，我们在多壁碳纳米管 （MWCNT） 上进行了富含羰基的聚酰亚胺 COFs（捐赠为 NTDA COFs）的原位生长。所制备的 NTDA/MWCNTs 复合材料在 1 A g^–1 时实现了令人印象深刻的 467 F g^–1 电容，明显超过了纯 MWCNT （60.3 F g^–1） 和 NTDA COF （284.4 F g^–1）。在 10 A g^–1 下循环 10,000 次后，未观察到电容衰减。组装装置 NTDA/MWCNTs//活性炭在 750 W kg^–1 时达到 17 Wh kg^–1 的高能量密度，同时在 10 A g^–1 下循环 19,000 次后仍保持 89.5% 的优异充放电稳定性。原位傅里叶变换红外（原位 FT-IR）测试以及电极动力学的探索表明，NTDA/MWCNTs 的增强电容主要是由 NTDA COF 上的羰基氧化还原反应提供的，而 NTDA COF 在很大程度上被 MWCNT 激活。