Surface Modification of Nickel‐Rich Cathode Materials by Ionically Conductive Materials at Room Temperature

Nickel‐rich cathode materials (LiNixMnyCo1−x−yO2, NMC) are promising to push the limits of lithium‐ion batteries to higher energy density. This approach is favored in practical applications including electric vehicles and aviation transportation. However, the instability of the NMC at charged state results in safety concerns and poor cycling stability. Surface coating is a practical and effective strategy to address this. Cubic Li7La3Zr2O12 (LLZO) is an ideal coating material regarding the low electron transfer rate and high Li+ conductivity. Thus, a LLZO coating layer can suppress the parasitic reactions in the electrode/electrolyte interface without deteriorating the lithium migration. However, high‐temperature calcination seems to inevitably create the chemical couplings between NMC and LLZO, leading to the interdiffusion and degradation of NMC and LLZO crystal structures. This work presents a simple mechanochemical method to effectively coat LLZO on the NMC particle surface. The coated cathode demonstrates superior electrochemical performance compared with the pristine NMC cathode.