Enabling structure/interface regulation for high performance Ni-rich cathodes

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 SrZrO${}_3$ coating and Sr/Zr co-doping is employed to strengthen the structure/interface stability and the Li${}^{+}$ transport mobility of LiNi${}_{0.85}$Co${}_{0.10}$Mn${}_{0.05}$O${}_2$ (NCM). Perovskite-type SrZrO${}_3$ 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. (© 2023 Wiley‐VCH GmbH)