Rare Earth Lattice Optimization Towards High‐Performance Ni‐Rich Layered Cathodes

Abstract High‐Ni layered oxide cathode materials are promising cathode materials for high‐energy‐density lithium‐ion batteries (LIBs). However, high‐Ni layered oxide cathodes still face issues, such as rapid structural collapse and surface parasitic reactions. Herein, a universal strategy using rare earth (La, Pr, Sm, Eu, Tb, Ho, etc.) lattice‐optimized spray‐drying preparation combined with the integration of a solid‐state synthesis process for preparing spherically high‐Ni cathodes is probed. This practical method synergizes rare earth lattice optimization and an artificial coating strategy for high‐performance high‐Ni LiNi 0.84 Co 0.12 Al 0.03 Ho 0.01 O 2 cathodes. The doping of Ho mitigates the mixing of Li + and Ni 2+ ions, and the suitable ionic radius ofHo element enlarges the plane spacing and promotes the rapid diffusion of Li + within the particles without causing significant lattice distortion. The cathodes show a high capacity of 223.7 mAh g −1 at 0.2 C and keep an ultra‐stable cycling stability even after 1200 cycles at the full‐cell level. This work provides a facile and highly efficient strategy for designing spherical, high‐capacity, and long‐cycle‐life high‐Ni layered oxide cathodes for practically sustainable LIBs.