Wang Yang-Jie, Li Hai-Xin, Zhang Jun-Jie, Zhuang Jin-Liang
School of Chemistry and Materials Science, Guizhou Normal University, Guiyang, 550025, P. R. China.
Chemphyschem. 2025 Jul 28:e2500315. doi: 10.1002/cphc.202500315.
Lithium-sulfur batteries (LSBs) have attracted significant attention due to their high theoretical energy density and cost-effectiveness. However, their practical application is hindered by issues such as the shuttle effect of lithium polysulfides (LiPSs), sluggish redox kinetics, and the insulating nature of sulfur. Covalent organic frameworks (COFs) have emerged as a promising class of porous crystalline materials for enhancing the performance of LSBs due to their tunable structures, high surface areas, and well-defined pore environments. This review systematically summarizes the latest progress in COF-based materials for LSBs, focusing on their applications in cathodes and functional separators. For cathodes, COFs and their derived composites serve as sulfur hosts, leveraging their high surface area and functionalized pore structures to immobilize LiPSs and facilitate sulfur utilization. In separators, COFs and COF-based composites enable efficient suppression of LiPSs migration through physical confinement, chemical adsorption, and catalytic acceleration of sulfur species transformation. Despite these advancements, the practical application of COFs either as host or functional separators faces challenges such as intrinsic low conductivity, structural stability, and large-scale synthesis. Finally, the challenges and perspectives are provided regarding the future design of COF-based cathodes and functional separators for high-performance LSBs.
锂硫电池（LSBs）因其高理论能量密度和成本效益而备受关注。然而，多硫化锂（LiPSs）的穿梭效应、缓慢的氧化还原动力学以及硫的绝缘性质等问题阻碍了它们的实际应用。共价有机框架（COFs）作为一类有前途的多孔晶体材料出现，因其结构可调、高比表面积和明确的孔环境而可用于提高锂硫电池的性能。本文综述系统总结了用于锂硫电池的基于COF的材料的最新进展，重点关注它们在阴极和功能隔膜中的应用。对于阴极，COFs及其衍生复合材料用作硫宿主，利用其高比表面积和功能化孔结构固定LiPSs并促进硫的利用。在隔膜中，COFs和基于COF的复合材料通过物理限制（ confinement）、化学吸附和催化加速硫物种转化来有效抑制LiPSs迁移。尽管有这些进展，但COFs作为宿主或功能隔膜的实际应用面临诸如固有低电导率、结构稳定性和大规模合成等挑战。最后给出了关于用于高性能锂硫电池的基于COF的阴极和功能隔膜未来设计的挑战和展望。
