Surface Gradient Ni‐Rich Cathode for Li‐Ion Batteries

Abstract Nickel‐rich layered oxide cathode material LiNi_xCo_yMn_zO₂ (NCM) has emerged as a promising candidate for next‐generation lithium‐ion batteries (LIBs). These cathode materials possess high theoretical specific capacity, fast electron/ion transfer rate, and high output voltage. However, their potential is impeded by interface instability, irreversible phase transition, and the resultant significant capacity loss, limiting their practical application in LIBs. In this work, a simple and scalable approach is proposed to prepare gradient cathode material (M‐NCM) with excellent structural stability and rate performance. Taking advantage of the strong coordination of Ni²⁺ with ammonia and the reduction reaction of KMnO₄, the elemental compositions of the Ni‐rich cathode are reasonably adjusted. The resulted gradient compositional design plays a crucial role in stabilizing the crystal structure, which effectively mitigates Li/Ni mixing and suppresses unwanted surficial parasitic reactions. As a result, the M‐NCM cathode maintains 98.6% capacity after 200 cycles, and a rapid charging ability of 107.5 mAh g⁻¹ at 15 C. Furthermore, a 1.2 Ah pouch cell configurated with graphite anode demonstrates a lifespan of over 500 cycles with only 8% capacity loss. This work provides a simple and scalable approach for the in situ construction of gradient cathode materials via cooperative coordination and deposition reactions.