Toward next-generation cathodes for lithium-ion batteries: progress and prospects of single-crystal lithium-rich manganese-based oxides

Abstract

Amid global efforts to achieve green economy and accelerate sustainable energy transformation, lithium-ion batteries have become a cornerstone for electric transportation and stationary storage systems. To meet increasing requirements for energy density, cycling durability, and operational safety, the development of high-performance cathode materials is critical. Single-crystal lithium-rich manganese-based layered oxides (SCLRMs) have gained increasing attention owing to their high specific capacity, structural coherence, and favorable interfacial stability. This review summarizes recent progress in the controlled synthesis, structural regulation, and performance optimization of SCLRMs. Key modification strategies, including compositional modification, surface engineering, and morphology design, are evaluated with respect to their roles in enhancing electrochemical behavior and suppressing degradation. Emphasis is placed on the integration of multi-dimensional and multi-scale characterization techniques to elucidate the evolution of nanoscale architectures, interfacial chemistry, and redox mechanisms during operation. Furthermore, artificial intelligence (AI) assisted approaches are highlighted for their potential in accelerating materials discovery and guiding performance-driven design. These developments are expected to enable the integration of SCLRMs into next-generation battery frameworks that not only exhibit high energy density and long cycle life but also support the emergence of smart battery systems with enhanced reliability, safety, and autonomous diagnostic capabilities. By consolidating recent advancements and outlining core challenges, this review provides critical insights into the progress and prospects of SCLRMs as next-generation cathode materials for lithium-ion batteries.