Advanced strategies to boost sustainable high-rate Ni-rich cathodes toward durable LIBs

Abstract

The rapid rise in demand for high-performance lithium-ion batteries (LIBs) highlights the importance of high-rate nickel-rich cathode materials as a key step toward next-generation LIBs, offering high discharge capacity, increased energy density, stable operating voltage, and cost-effectiveness. However, issues such as cation mixing, side reactions, microcrack formation, and thermal instability limit their rate capability and long-term durability. This review provides a detailed assessment of these challenges. It outlines strategies to overcome them, including surface coating, doping, core–shell structures, full-concentration gradients, and particle or additive engineering. Surface coatings improve surface stability and ion transport, while doping methods, including pillar and gradient doping, reduce cation mixing and strengthen structural stability. Core–shell and full-concentration gradients designs relieve mechanical stress and suppress phase transitions, and advanced particle engineering reduces microcrack formation. Computational tools such as density functional theory and machine learning, together with in-situ characterization, provide valuable insights into degradation mechanisms, enabling more precise material optimization. Importantly, combined and modified approaches that integrate multiple strategies show the greatest potential to address these challenges while maintaining sustainability and scalability. This work clarifies operational mechanisms, aiding researchers in developing advanced high-rate Ni-rich cathode LIBs for future energy storage.