Covalent organic frameworks (COFs) hold great promise for electrochemical energy storage because of their high surface area, readily accessible redox-active sites, and environment-friendly chemical composition. In this study, the synthesis of a redox-active pyrene-containing polyimide COF (PICOF-1) by linker exchange using an imine-linked COF as a template is reported and its performance in sodium-ion batteries (SIBs) is demonstrated. The reported synthetic route based on linker exchange mitigates the challenges typically encountered with crystallizing chemically stable polyimide COFs from typical condensation reactions; thus, facilitating their rapid synthesis and purification. Using this approach, PICOF-1 exhibits high crystallinity with very low refinement parameters R_P and R_WP of 0.415% and 0.326%, respectively. PICOF-1 has a high Brunauer–Emmette–Teller (BET) surface area of 924 m² g⁻¹ and well-defined one-dimentional (1D) channels of 2.46 × 1.90 nm, which enable fast ion transport and charge transfer, reaching a capacity at 0.1 C of almost nearly as its theoretical capacity and maintaining 99% Coulombic efficiency over 175 cycles at 0.3 C. The study demonstrates that imine-linked COFs are effective templates for integrating carbonyl-rich polyimide moieties into high-surface COFs to advance electrochemical energy storage applications.

中文翻译：

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用于可充电钠离子电池的二维聚酰亚胺共价有机骨架的模板合成

共价有机框架 (COF) 具有高表面积、易于接近的氧化还原活性位点和环境友好的化学成分，因此在电化学储能方面具有广阔前景。在这项研究中，报道了使用亚胺连接的 COF 作为模板通过接头交换合成具有氧化还原活性的含芘聚酰亚胺 COF (PICOF-1)，并展示了其在钠离子电池 (SIB) 中的性能。报道的基于接头交换的合成路线减轻了典型缩合反应中结晶化学稳定的聚酰亚胺 COF 通常遇到的挑战；因此，促进它们的快速合成和纯化。使用这种方法，PICOF-1 表现出高结晶度和非常低的细化参数R _P和R_WP分别为 0.415% 和 0.326%。^{PICOF-1 具有 924 m 2}  g ⁻¹的高 Brunauer-Emmette-Teller (BET) 表面积和 2.46 × 1.90 nm 的明确定义的一维 (1D) 通道，可实现快速离子传输和电荷转移，达到在 0.1 C 下的容量几乎接近其理论容量，并在 0.3 C 下在 175 个循环中保持 99% 的库仑效率。研究表明，亚胺连接的 COF 是将富含羰基的聚酰亚胺部分整合到高表面 COF 中以推进的有效模板电化学储能应用。