Meng Junchen, Yin Mengjia, Guo Kairui, Zhou Xingping, Xue Zhigang
Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, People's Republic of China.
Nanomicro Lett. 2025 May 6;17(1):248. doi: 10.1007/s40820-025-01768-3.
Solid polymer electrolytes (SPEs) have garnered considerable interest in the field of lithium metal batteries (LMBs) owing to their exceptional mechanical strength, excellent designability, and heightened safety characteristics. However, their inherently low ion transport efficiency poses a major challenge for their application in LMBs. To address this issue, covalent organic framework (COF) with their ordered ion transport channels, chemical stability, large specific surface area, and designable multifunctional sites has shown promising potential to enhance lithium-ion conduction. Here, we prepared an anionic COF, TpPa-COOLi, which can catalyze the ring-opening copolymerization of cyclic lactone monomers for the in situ fabrication of SPEs. The design leverages the high specific surface area of COF to facilitate the absorption of polymerization precursor and catalyze the polymerization within the pores, forming additional COF-polymer junctions that enhance ion transport pathways. The partial exfoliation of COF achieved through these junctions improved its dispersion within the polymer matrix, preserving ion transport channels and facilitating ion transport across COF grain boundaries. By controlling variables to alter the crystallinity of TpPa-COOLi and the presence of -COOLi substituents, TpPa-COOLi with partial long-range order and -COOLi substituents exhibited superior electrochemical performance. This research demonstrates the potential in constructing high-performance SPEs for LMBs.
固态聚合物电解质（SPEs）因其出色的机械强度、优异的可设计性和更高的安全特性，在锂金属电池（LMBs）领域引起了广泛关注。然而，其固有的低离子传输效率对其在LMBs中的应用构成了重大挑战。为了解决这个问题，具有有序离子传输通道、化学稳定性、大比表面积和可设计多功能位点的共价有机框架（COF）显示出增强锂离子传导的巨大潜力。在此，我们制备了一种阴离子型COF，即TpPa-COOLi，它可以催化环状内酯单体的开环共聚反应，用于原位制备SPEs。该设计利用了COF的高比表面积来促进聚合前体的吸收，并催化孔内的聚合反应，形成额外的COF-聚合物连接点，增强离子传输途径。通过这些连接点实现的COF部分剥离改善了其在聚合物基质中的分散性，保留了离子传输通道，并促进离子跨COF晶界传输。通过控制变量来改变TpPa-COOLi的结晶度和-COOLi取代基的存在，具有部分长程有序和-COOLi取代基的TpPa-COOLi表现出优异的电化学性能。这项研究展示了构建用于LMBs的高性能SPEs的潜力。
