Stepwise Dopant Selection Process for High‐Nickel Layered Oxide Cathodes

Abstract NCM‐based lithium layered oxides (LiNi1–x–yCoxMnyO2) have become prevalent cathode materials in state‐of‐the‐art lithium‐ion batteries. Higher energy densities can be achieved in these materials by systematically increasing the nickel content; however, this approach commonly results in inferior cycle stability. The poor cycle retention of high‐nickel NCM cathodes is generally attributed to chemo‐mechanical degradation (e.g., intergranular microcracks), vulnerability to oxygen‐gas evolution, and the accompanying rocksalt phase formation via cation mixing. Herein, the feasibility of doping strategies is examined to mitigate these issues and effective dopants for high‐nickel NCM cathodes are theoretically identified through a stepwise pruning process based on density functional theory calculations. Specifically, a sequential three‐step screening process is conducted for 38 potentia…