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基于一维共价有机框架的高压柔性钠离子电池阴极材料

High Voltage Flexible Sodium-Ion Battery Cathode Materials Based on 1D Covalent Organic Framework.

作者信息

Liu Shuai, Leung Puiki, Zuo Yong, Sun Meng, Wei Lei, Walsh Frank C, Zhao Tianshou, Liao Qiang

机构信息

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.

出版信息

Adv Sci (Weinh). 2025 Aug;12(31):e05311. doi: 10.1002/advs.202505311. Epub 2025 Jun 23.

Abstract

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.

摘要

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。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c5c9/12376503/7dc87e85fc48/ADVS-12-e05311-g002.jpg

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