Surface and Interfacial Modulation of Lithium‐Rich Manganese Layered Oxide Cathode Materials: Progress and Challenges

Abstract Exhibiting exceptional energy density and capacity, lithium‐rich manganese‐based layered oxide (LLOs) cathode materials have garnered considerable attention and are emerging as strong contenders for future lithium‐ion battery systems. However, the manner in which they are employed in practice is hindered by several challenges, such as voltage fading, exhibiting a low initial coulombic efficiency, and suboptimal cycling stability, mainly attributed to oxygen depletion and phase transformation phenomena. The current review primarily centers on recent progress in addressing these issues through surface and interfacial modification techniques, including surface doping, coating, and oxygen vacancy engineering. Other strategies, such as spinel phase engineering and hybrid coating layers, are also discussed as potential solutions to enhance electrochemical performance, stability, and capacity retention. Additionally, exploration advancements in electrolyte design aimed at stabilizing the LLOs/electrolyte interface, reducing side reactions, and enabling the development of a stable solid electrolyte interphase (CEI). The review concludes by highlighting ongoing challenges, particularly in improving long‐term cycling stability, and proposes prospective research directions aimed at further unlocking the potential of LLOs cathode materials for practical battery applications.