Why the Synthesis Affects Performance of Layered Transition Metal Oxide Cathode Materials for Li‐Ion Batteries

The limited cyclability of high-specific-energy layered transition metal oxide (LiTMO₂) cathode materials poses a significant challenge to the industrialization of batteries incorporating these materials. This limitation can be attributed to various factors, with the intrinsic behavior of the crystal structure during the cycle process being a key contributor. These factors include phase transition induced cracks, reduced Li active sites due to Li/Ni mixing, and slower Li⁺ migration. In addition, the presence of synthesis-induced heterogeneous phases and lattice defects cannot be disregarded as they also contribute to the degradation in performance. Therefore, gaining a profound understanding of the intricate relationship among material synthesis, structure, and performance is imperative for the development of LiTMO₂. This paper highlights the pivotal role of structural play in LiTMO₂ materials and provides a comprehensive overview of how various control factors influence the specific pathways of structural evolution during the synthesis process. In addition, it summarizes the scientific challenges associated with diverse modification approaches currently employed to address the cyclic failure of materials. The overarching goal is to provide readers with profound insights into the study of LiTMO₂.