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全固态锂电池可以实现电池高能量密度和高安全性兼顾，同时有望提升其循环寿命，是当前学术研究和产业发展的热点方向。富锂锰基正极材料具有高克容量和低成本等优势，是高比能全固态锂电池发展的重要方向。采用富锂锰基正极材料构建全固态锂电池，解决正极材料与固态电解质的固–固界面接触问题，有助于提升全固态锂电池的电化学性能。本文简述了富锂锰基正极和固态电解质材料的特性，详述了采用不同固态电解质的富锂锰基全固态锂电池在正极侧面临的界面失效等问题和挑战，以及构筑稳定界面的研究进展，并展望了富锂锰基全固态锂电池的正极及界面改性的研究重点和发展方向。
Abstract：Extended Abstract All-solid-state lithium batteries(ASSLBs) emerge as a pivotal direction for next-generation energy storage systems due to their high energy density, intrinsic safety, and extended cycle life. Lithium-rich manganese-based layered oxides(LLOs) with their exceptional specific capacity(i.e., >300 m A·h/g) and cost-effectiveness are regarded as a promising cathode candidate for high-energy-density ASSLBs. However, critical challenges such as poor solid-solid interfacial contact between LLOs and solid electrolytes, irreversible lattice oxygen loss, and interfacial side reactions hinder their practical implementation. This review comprehensively analyzes the structural characteristics of LLOs, the anionic oxygen redox(OAR) mechanism, and interfacial challenges in ASSLBs, while systematically summarizing modification strategies across sulfide-, halide-, oxide-, and polymer-based solid electrolyte systems. The high capacity of LLOs primarily originates from OAR, where reversible O2-/O-redox contributes to extra capacity. However, oxygen release and transition metal(TM) migration lead to voltage decay and structural degradation. To address these issues, gradient doping and surface coating are developed to stabilize lattice oxygen and suppress phase separation. Compared to polycrystalline materials, single-crystal LLOs exhibit superior mechanical stability and interfacial contact, effectively mitigating crack propagation caused by volume changes. In sulfide-based systems, the space charge layer(SCL) effect and sulfur oxidation at high voltages are the main limiting factors. Strategies such as LLOs surface sulfurization, uniform dispersion by liquid-phase mixing, and functional coatings can effectively reduce the interfacial resistance and enhance the OAR reversibility. For halide electrolytes, the introduction of carbon additives and ion-conductive coatings can establish a continuous conductive transport network. Oxide-based systems benefit from co-sintering LLO with garnet-type Li7La3Zr2O12 and Li3BO3 sintering aids to improve interfacial densification, although Mn/La interdiffusion in co-sintering requires further attention. Polymer electrolytes, especially those formed by in-situ polymerization of propane sultone-based materials, are able to form a thin and uniform cathode-electrolyte interface(CEI), thereby widening the electrochemical stability window. A critical finding across these systems is the importance of mechanical-electrochemical coupling at interfaces. "Soft-contact" interfaces with flexible ion-conductive layers are essential to accommodate volume changes. Halide electrolytes have a unique compatibility with LLOs via minimizing SCL effects, while sulfide systems demand a precise control of oxidation-prone components to prevent degradation. Summary and prospects Future research should prioritize advanced characterization techniques to elucidate dynamic structural evolution and interfacial degradation pathways during OAR. Material optimization, such as designing Co-free LLOs with gradient TM distribution and single-crystal morphology, can enhance intrinsic Li+/electronic conductivity and structural integrity. Innovations in electrolytes, including hybrid organic-inorganic composites or high-entropy sulfides can balance ionic conductivity(32 m S/cm) and interfacial stability. Scaling up production processes for sulfide/halide electrolytes and addressing their moisture sensitivity are also crucial steps toward commercialization. In summary, interfacial stability remains a cornerstone for high-performance LLOs-based ASSLBs. ASSLBs are poised to achieve energy densities of exceeding 1000 W·h/kg via synergizing material design, interface engineering, and mechanistic understanding, paving a way for their application in electric vehicles and grid-scale storage.
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基本信息:
DOI：10.14062/j.issn.0454-5648.20240858
中图分类号:O646;TM912
引用信息:
[1]郭志强,郭现伟,刘世奇,等.富锂锰基全固态锂电池正极界面研究进展[J].硅酸盐学报,2025,53(06):1700-1713.DOI:10.14062/j.issn.0454-5648.20240858.
基金信息:
国家自然科学基金项目(U23A20577,52372168); 国家重点研发计划(2022YFB2404401)
2024-12-31
2024
2025-05-02
2025-04-29
2025
1
2025-05-19
2025-05-19
2025-05-19