Interfacial Reviving of the Degraded LiNi_0.8Co_0.1Mn_0.1O₂ Cathode by LiPO₃ Repair Strategy

Abstract Nickel‐rich cathode materials, owing to their high energy density and low cost, are considered to be one of the cathodes with the most potential in next‐generation lithium‐ion batteries. Unfortunately, this kind of cathode with highly active surface is easy to react with H₂O and CO₂ when exposed to ambient air, resulting in the formation of lithium impurities and interfacial phase transition as well as deterioration of the electrochemical properties. In this work, the evolution mechanism of the structure and interface of LiNi_0.8Co_0.1Mn_0.1O₂ during air‐exposure is systematically investigated. Furthermore, a facile reviving strategy is proposed to restore the degraded LiNi_0.8Co_0.1Mn_0.1O₂ by using LiPO₃ as the repair agent. The lithium impurities on the surface of the degraded sample can transform into the repair/coating layer, and part of the rock salt phase on the subsurface can revive to layered phase after repair heat treatment. As a result, the optimized cathode delivers an initial discharge capacity of 198.3 mAh g⁻¹ at 0.1C and a capacity retention of 85.5% after 50 cycles. Although slightly lower than the bare sample (201 mAh g⁻¹ and 88%), they are obviously higher than the exposed samples (166.5 mAh g⁻¹ and 40.4%). The regenerated electrochemical properties should be attributed to the multifunctional repair layer that can efficiently reduce the surface lithium impurities, prevent the corrosion of electrolyte, and improve the interfacial Li⁺ diffusion kinetics. This work can effectively reduce the waste of the degraded Ni‐rich ternary materials and realize the transformation of “waste” into wealth.