Surface Reconstruction Reduces Internal Stress of Ni‐Rich Cathode Particles

Abstract High‐voltage Ni‐rich layered cathode materials are undoubtedly a powerful driving force for high‐energy density lithium batteries. However, residual lithium impurities on the surface of Ni‐rich materials can cause more severe side reactions under high‐voltage, leading to rapid decay. There is still no reliable mechanistic explanation for this phenomenon. It has been detected that residual alkali on the cathode surface under high voltage can cause obvious side reactions. This side reaction will affect the capacity retention of the material and increase the internal stress of the particles. In addition, the surface reconstruction of Ni‐rich cathodes is achieved through simple chemical reactions, turning waste into treasure. The newly generated Ti‐based layer not only repairs the structure of the nickel‐rich material but also optimizes the material from a dynamic perspective. Removing residual lithium components on the cathode surface effectively reduces the hydrolysis and self‐catalytic side reactions of PF 6 − at the electrolyte cathode interface and suppresses gas generation during cycling, promoting the application of the next generation of high‐energy density Ni‐rich layered cathode‐based lithium batteries with high‐voltage.