Comprehensive Review of Li‐Rich Mn‐Based Layered Oxide Cathode Materials for Lithium‐Ion Batteries: Theories, Challenges, Strategies and Perspectives

Abstract Lithium‐rich manganese‐based layered oxide cathode materials (LLOs) have always been considered as the most promising cathode materials for achieving high energy density lithium‐ion batteries (LIBs). However, in practical applications, LLOs often face some key problems, such as low initial coulombic efficiency, capacity/voltage decay, poor rate performance and poor cycle stability. It seriously shortens the lifespan of lithium‐ion batteries and hinder the large‐scale commercial application of LLOs. Herein, firstly, the basic theories of LLOs were systematically reviewed, including the structural characteristics, the working mechanism of LLOs, the preparation methods of LLOs (liquid phase co‐precipitate method, sol‐gel method, hydrothermal synthesis method, solid phase method, low heat solid‐phase method, high temperature solid‐state method etc.), and electrochemical characteristics of LLOs (first charge discharge characteristics and reversible efficiency, cycling performance, high and low temperature performance and thermal stability etc.). Then, key challenges faced by LLOs were systematically discussed. Finally, the LLOs modification strategies used to address these challenges (element doping, surface modification, defect engineering, structural and morphological control etc.) were elaborated in detail. This important review provides potential insights and directions for further improving the electrochemical performance of LLOs, and provides a necessary theoretical basis for accelerating the large‐scale commercial application of LLOs. It possesses important scientific research value and far‐reaching social significance.