Y.N. Han, G.R. Wang *, X.X. Ren, M.Z. Yang, Z.T. Li * and Z.-S. Wu *

New Carbon Materials, 2025, accepted.

Lithium-rich manganese-based layered oxides (LRMO) possess the advantages of high specific capacity, high voltage, and low cost, making them a promising candidate of cathode materials for next-generation high-energy lithium-ion batteries. However, LRMO still faces key scientific challenges such as low initial Coulombic efficiency, poor rate capability, and fast voltage decay, which prevent them from the demanding requirements of lithium-ion batteries in high-end applications such as aerospace, medical equipment, and advanced electric vehicles. To gain a comprehensive understanding of LRMO, this review systematically discusses the crystal structure, key challenges, and main modification strategies of LRMO, and provides an outlook on future prospectives. First, the crystal structure and energy storage mechanism of LRMO are elaborated in detail, and the key challenges it faces are discussed, including densification of the crystal structure (irreversible reactions in the bulk and surface) and degradation of electrochemical performance (voltage decay, reduced initial Coulombic efficiency, and poor rate capability). Subsequently, the modification strategies for LRMO are summarized and explored, including enhancing lithium-ion diffusion rate and crystal structure stability through element doping (bulk doping, surface doping, and concentration gradient doping); suppressing harmful side reactions between LRMO and the electrolyte through surface coating to enhance structural stability during the cycling process (including phosphate coating, carbon-based coating, metal oxide coating, and conductive polymer coating); and improving the electrochemical performance of LRMO through binder and electrolyte optimization strategies. Finally, this review deeply elaborates on prospective views and future directions, providing comprehensive and detailed guidance for the rational design and scalable production of next-generation LRMO cathode materials towards high-energy-density lithium-ion batteries.