Passivation of the Cathode-Electrolyte Interface for 5 V-Class All-Solid-State Batteries

An all-solid-state battery is a potentially superior alternative to a state-of-the-art lithium-ion battery owing to its merits in abuse tolerance, packaging, energy density, and operable temperature ranges. In this work, a 5 V-class spinel LiNi_0.5Mn_1.5O₄ (LNMO) cathode is targeted to combine with a high-ionic-conductivity Li₆PS₅Cl (LPSCl) solid electrolyte for developing high-performance all-solid-state batteries. Aiming to passivate and stabilize the LNMO-LPSCl interface and suppress the unfavorable side reactions such as the continuous chemical/electrochemical decomposition of the solid electrolyte, oxide materials including LiNbO₃, Li₃PO₄, and Li₄Ti₅O₁₂ are rationally applied to decorate the surface of pristine LNMO particles with various amounts through a wet-chemistry approach. Electrochemical characterization demonstrates that the composite cathode consisting of 8 wt % LiNbO₃-coated LNMO and LPSCl in a weight ratio of 70:30 delivers the best electrochemical performance with an initial discharge capacity of 115 mA h g^-1 and a reversible discharge capacity of 80 mA h g^-1 at the 20th cycle, suggesting that interfacial passivation is an effective strategy to ensure the operation of 5 V-class all-solid-state batteries.