Enabling Structure/Interface Regulation for High Performance Ni‐Rich Cathodes

Abstract

Further commercialization of Ni‐rich layered cathodes is hindered by severe structure/interface degradation and kinetic hindrance that occur during electrochemical operation, which leads to safety risks and reduced range in electric vehicles (EVs). Herein, by selecting elements with different solubility properties, a multifunctional strategy that synchronously fabricates perovskite‐type SrZrO₃ coating and Sr/Zr co‐doping is employed to strengthen the structure/interface stability and the Li⁺ transport mobility of LiNi_0.85Co_0.10Mn_0.05O₂ (NCM). Perovskite‐type SrZrO₃ protective layers formed on the particle surface can substantially mitigate the unexpected interfacial side reactions and surface phase transitions. In addition, a robust crystal framework is constructed by optimizing local O coordination through the introduction of strong Zr−O bonds. Notably, Li⁺ diffusion kinetics is effectively improved due to expanded cell parameters and O‐Li‐O slab spacing with the incorporation of large‐diameter Sr pillar ions, as revealed by X‐ray diffraction. As a result, the Sr/Zr‐modified NCM achieves a remarkable capacity retention of 99.4% after 200 cycles at 1 C, and a high rate capacity of 168.9 mAh g⁻¹ at 10 C. This work opens new avenues to develop high‐performance NCM cathodes with high energy and high power for EVs with long calendar life.