Unlocking the Power of Three: A “Three Birds with One Stone” Strategy for Exceptional Structural Stability and Rate Performances in Nickel‐Rich Cathode Materials

Abstract Nickel‐rich cathode materials hold immense potential for electric vehicle batteries due to their high energy density and cost‐effectiveness. However, structural degradation and capacity fading during high‐rate operation hinder their widespread adoption. This groundbreaking study presents a novel “three birds with one stone” strategy to simultaneously optimize microstructure, lattice oxygen stability, and surface modification in LiNi _0.97 Co _0.02 Mn _0.01 O ₂ (NCM97) cathode materials. By introducing Mo ions through a facile one‐step method, a porous structure is achieved for stress dissipation, Li ₂ MoO ₄ spinel coating for improved interfacial stability, and rigid Mo─O bonds for lattice oxygen stabilization. This holistic approach significantly enhances the structural stability and electrochemical performance of NCM97, resulting in higher capacity retention and superior rate performance. The modified NCM97 boasts an impressive initial capacity of 232.6 mAh g ⁻¹ at 0.1C and 182.3 mAh g ⁻¹ at 5C, along with an exceptional capacity retention rate of 80.6% after 300 cycles at 5C. Most notably, when integrated into a pouch full cell with a graphite anode, the NCM97‐Mo cathode achieves a remarkable 88.4% capacity retention after 800 cycles at 2C. This innovative strategy paves the way for the industrial development of high energy density nickel‐rich cathode materials, revolutionizing the electric vehicle battery landscape.