Tackling the Interfacial Issues of Spinel LiNi_0.5Mn_1.5O₄ by Room-Temperature Spontaneous Dediazonation Reaction

The detrimental interfacial side reactions, inducing electrolyte decomposition and transition-metal dissolution, are regarded as “arch-criminal” for the utilization of spinel LiNi0.5Mn1.5O4 (LNMO) in high-power Li-ion batteries (LIBs). To conquer this issue, herein, we construct a thin polyphenyl film onto the surface of LNMO via the spontaneous dediazonation of C6H5N2+BF4– at room temperature. This conductive film facilitates the Li+ transport within cathode and at LNMO|electrolyte interface while reinforcing the compatibility of LNMO against electrolyte by efficiently suppressing the electrolyte decomposition catalyzed by LNMO and even the transition-metal dissolution. Consequently, polyphenyl-grafted LNMO exhibits improved electrochemical performances, e.g., the considerable discharge capacity of 136.7 mAh g–1 at low current density (0.1C), excellent rate capability, and long-term cyclability with a reversible capacity of 107.4 mAh g–1 along with high capacity retention of ∼85% after cycling 500 times, that are superior to those of the pristine LNMO counterpart. All these results demonstrate that our strategy is instrumental in solving the interface issues with respect to the spinel LNMO cathode, impelling the development of LNMO-based batteries with high energy density.