Voltage Decay of Li‐Rich Layered Oxides: Mechanism, Modification Strategies, and Perspectives

Li‐rich layered oxides (LLOs) have been considered as the most promising cathode materials for achieving high energy density Li‐ion batteries. However, they suffer from continuous voltage decay during cycling, which seriously shortens the lifespan of the battery in practical applications. This review comprehensively elaborates and summarizes the state‐of‐the‐art of the research in this field. It is started from the proposed mechanism of voltage decay that refers to the phase transition, microscopic defects, and oxygen redox or release. Furthermore, several strategies to mitigate the voltage decay of LLOs from different scales, such as surface modification, elemental doping, regulation of components, control of defect, and morphology design are summarized. Finally, a systematic outlook on the real root of voltage decay is provided, and more importantly, a potential solution to voltage recovery from electrochemistry. Based on this progress, some effective strategies with multiple scales will be feasible to create the conditions for their commercialization in the future. Voltage decay in Li‐rich layered oxide cathode results from the combined interaction of phase changes, microscopic defects and oxygen redox or release during the material cycle. Strategies to suppress voltage decay revolve around maintaining structural stability, including surface coating, surface chemical treatment, elemental doping, regulation of components, control of defects and morphology design.