A Simple Gas–Solid Treatment for Surface Modification of Li‐Rich Oxides Cathodes

Abstract Li‐rich layered oxides with high capacity are expected to be the next generation of cathode materials. However, the irreversible and sluggish anionic redox reaction leads to the O 2 loss in the surface as well as the capacity and voltage fading. In the present study, a simple gas–solid treatment with ferrous oxalate has been proposed to uniformly coat a thin spinel phase layer with oxygen vacancy and simultaneously realize Fe‐ion substitution in the surface. The integration of oxygen vacancy and spinel phase suppresses irreversible O 2 release, prevents electrolyte corrosion, and promotes Li‐ion diffusion. In addition, the surface doping of Fe‐ion can further stabilize the structure. Accordingly, the treated Feox‐2 % cathode exhibits superior capacity retention of 86.4 % and 85.5 % at 1 C and 2 C to that (75.3 % and 75.0 %) of the pristine sample after 300 cycles, respectively. Then, the voltage fading is significantly suppressed to 0.0011 V per cycle at 2 C especially. The encouraging results may play a significant role in paving the practical application of Li‐rich layered oxides cathode.