Synchronous Tailoring Surface Structure and Chemical Composition of Li‐Rich–Layered Oxide for High‐Energy Lithium‐Ion Batteries

A phase‐gradient outer layer with “layered‐coexisting phase‐spinel” structure accompanied by decreasing nickel content is self‐induced and formed successfully, which endows fast ion diffusion channels, suppressed voltage decay, and good cyclic stability for Li‐rich–layered cathode materials. This finding sheds light on a universal principle for simultaneously tailoring structure and composition of electrode materials.