Lithium-rich manganese-based layered oxides (LMLOs) are considered to be one type of the most promising materials for next-generation cathodes of lithium batteries due to their distinctive anionic redox processes contributing ultrahigh capacity and energy density. Unfortunately, their practical applications are still plagued by several challenges such as undesirable interfacial reactions and structural evolution, as well as voltage hysteresis/recession, in which irreversible anionic redox behavior bears the brunt as the primacy factor. Undoubtedly, a deep understanding of anionic redox reaction mechanisms and irreversible behavior of oxygen species is crucial in order to provide essential guidance for modification strategies for LMLOs. In this paper, the fundamental understanding of intricate anionic redox reaction mechanisms from thermodynamics models to kinetic anionic redox reaction pathways is comprehensively reviewed, and the existing challenges of LMLOs related with irreversible oxygen reaction behavior are analyzed. Furthermore, numerous representative modification strategies for overcoming these challenges, coupled with their underlying mechanisms for regulating anionic redox reversibility are summarized. In addition, the aspects of multi-scale structural modifications, integration of interdisciplinary technologies, and application in quasi-/all-solid-state battery systems are given some emphasis in terms of further improvement of LMLOs-based cathode materials for advanced lithium batteries-based energy storage systems.

中文翻译：

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从反应机制到调节策略了解锂离子和锂金属电池的富锂锰基层状氧化物中的晶格氧氧化还原行为

富锂锰基层状氧化物（LMLO）因其独特的阴离子氧化还原过程提供超高容量和能量密度而被认为是下一代锂电池阴极最有前途的材料之一。不幸的是，它们的实际应用仍然受到一些挑战的困扰，例如不良的界面反应和结构演化，以及电压滞后/衰退，其中不可逆的阴离子氧化还原行为首当其冲。毫无疑问，深入了解阴离子氧化还原反应机制和氧物种的不可逆行为至关重要，以便为 LMLO 的修饰策略提供必要的指导。本文全面回顾了从热力学模型到动力学阴离子氧化还原反应路径等复杂阴离子氧化还原反应机制的基本理解，并分析了LMLO与不可逆氧反应行为相关的现有挑战。此外，还总结了克服这些挑战的众多代表性修饰策略，及其调节阴离子氧化还原可逆性的基本机制。此外，在进一步改进先进锂电池LMLOs正极材料方面，还重点关注多尺度结构修饰、跨学科技术集成以及在准/全固态电池系统中的应用。基于能量存储系统。