Liu Shuai, Leung Puiki, Zuo Yong, Sun Meng, Wei Lei, Walsh Frank C, Zhao Tianshou, Liao Qiang
Chongqing Univ, Key Lab Low Grade Energy Utilizat Technol & Syst, MOE, Chongqing, 400030, China.
A National Innovation Center for Industry-Education Integration of Energy Storage Technology, School of Energy and Power Engineering, Chongqing, 400044, China.
Adv Sci (Weinh). 2025 Aug;12(31):e05311. doi: 10.1002/advs.202505311. Epub 2025 Jun 23.
Covalent organic frameworks (COFs) have emerged as promising electrode materials for sodium-ion batteries (SIBs) due to their well-ordered porous structures that facilitate ion storage and transport. However, conventional 2D and 3D COFs often require post-processing, such as ball milling or carbon compositing, to enhance electrochemical performance. In this study, a 1D imine-linked COF, N,N,N',N'-Tetrakis(4-aminophenyl)-1,4-phenylenediamine-2,6-pyridinedicarboxaldehyde (TP-PDA), is synthesized via a one-step Schiff base reaction, achieving a fully conjugated and porous structure that enables efficient sodium-ion transport. TP-PDA is insoluble in organic electrolytes, ensuring stable cycling performance. The material exhibits a high average discharge potential of 3.1 V and delivers a discharge capacity of 124 mAh g at 3 A g after 1800 cycles, with a capacity retention exceeding 90%. In a full-cell configuration with a hard carbon anode, the battery maintains a stable capacity of 122 mAh g after 10 000 cycles at 1 A g without noticeable capacity degradation. Furthermore, the flexible pouch cell retains its electrochemical integrity under bending conditions, demonstrating its potential for flexible and wearable energy storage applications.
共价有机框架（COFs）因其有序的多孔结构有利于离子存储和传输，已成为钠离子电池（SIBs）颇具前景的电极材料。然而，传统的二维和三维COFs通常需要进行后处理，如球磨或碳复合，以提高电化学性能。在本研究中，通过一步席夫碱反应合成了一种一维亚胺连接的COF，即N,N,N',N'-四（4-氨基苯基）-1,4-苯二胺-2,6-吡啶二甲醛（TP-PDA），实现了全共轭和多孔结构，从而实现高效的钠离子传输。TP-PDA不溶于有机电解质，确保了稳定的循环性能。该材料表现出3.1 V的高平均放电电位，在1800次循环后，在3 A g的电流密度下放电容量为124 mAh g，容量保持率超过90%。在与硬碳负极组成的全电池配置中，该电池在1 A g的电流密度下经过10000次循环后，保持122 mAh g的稳定容量，且无明显容量衰减。此外，柔性软包电池在弯曲条件下保持其电化学完整性，展示了其在柔性和可穿戴储能应用中的潜力。
