Regulating interfacial chemistry and kinetic behaviors of F/Mo co-doping Ni-rich layered oxide cathode for long-cycling lithium-ion batteries over −20 °C–60 °C

Abstract

Ni-rich layered oxide cathodes have shown promise for high-energy lithium-ion batteries (LIBs) but are usually limited to mild environments because of their rapid performance degradation under extreme temperature conditions (below 0 °C and above 50 °C). Here, we report the design of F/Mo co-doped LiNi0.8Co0.1Mn0.1O2 (FMNCM) cathode for high-performance LIBs from −20 to 60 °C. F– doping with high electronegativity into the cathode surface is found to enhance the stability of surface lattice structure and protect the interface from side reactions with the electrolyte by generating a LiF-rich surface layer. Concurrently, the Mo6+ doping suppresses phase transition, which blocks Li+/Ni2+ mixing, and stabilizes lithium-ion diffusion pathway. Remarkably, the FMNCM cathode demonstrates excellent cycling stability at a high cutoff voltage of 4.4 V, even at 60 °C, maintaining 90.6% capacity retention at 3 C after 150 cycles. Additionally, at temperatures as low as −20 °C, it retains 77.1% of its room temperature capacity, achieving an impressive 97.5% capacity retention after 500 cycles. Such stable operation under wide temperatures has been further validated in practical Ah-level pouch-cells. This study sheds light on both fundamental mechanisms and practical implications for the design of advanced cathode materials for wide-temperature LIBs, presenting a promising path towards high-energy and long-cycling LIBs with temperature adaptability.