Li Siyu, Ou Yang, Zhang Yifan, Luo Wen, Wu Yang, Wang Yong
Department of Chemical Engineering, School of Environmental and Chemical Engineering, Shanghai University, 99 Shang da Road, Shanghai, 200444, P. R. China.
Chemistry. 2025 Jul 25;31(42):e202501264. doi: 10.1002/chem.202501264. Epub 2025 Jul 10.
Lithium-sulfur batteries (LSBs) are promising next-generation energy storage systems due to their high theoretical energy density and cost-effectiveness. However, challenges such as polysulfide shuttle, sluggish redox kinetics, and electrode instability hinder their practical applications. Covalent organic frameworks (COFs), featuring high porosity, tunable functionality, and structural regularity, have emerged as versatile materials to address these issues. This review systematically summarizes recent advances in COF-based strategies for LSBs, including their multifunctional roles as sulfur hosts, separators/interlayers, and catalytic additives. The predominant catalytic mechanisms associated with COFs are further elucidated, with specific focus being placed on electrostatic field catalysis, supramolecular channel catalysis, redox-mediated catalysis, and metal-coordination catalysis. While conventional characterization techniques have been extensively described in previous reviews, particular emphasis is placed on the application of in situ characterization techniques, such as Raman spectroscopy, Fourier transform infrared spectroscopy, and X-ray diffraction (XRD), which offer mechanistic insights into COF-catalyzed polysulfide conversion. This review aims to provide a comprehensive understanding of the structure-function-performance relationship of COFs and guide the rational design of next-generation COF-based materials for high-performance LSBs.
锂硫电池（LSBs）因其高理论能量密度和成本效益而成为很有前景的下一代储能系统。然而，多硫化物穿梭、缓慢的氧化还原动力学和电极不稳定性等挑战阻碍了它们的实际应用。共价有机框架（COFs）具有高孔隙率、可调节的功能和结构规则性，已成为解决这些问题的多功能材料。本文综述系统总结了基于COF的锂硫电池策略的最新进展，包括它们作为硫宿主、隔膜/中间层和催化添加剂的多功能作用。进一步阐明了与COFs相关的主要催化机制，特别关注静电场催化、超分子通道催化、氧化还原介导催化和金属配位催化。虽然传统表征技术在以往的综述中已有广泛描述，但本文特别强调原位表征技术的应用，如拉曼光谱、傅里叶变换红外光谱和X射线衍射（XRD），这些技术为COF催化的多硫化物转化提供了机理见解。本文旨在全面理解COFs的结构-功能-性能关系，并指导高性能锂硫电池下一代基于COF的材料的合理设计。
