Manipulating Interfacial Nanostructure to Achieve High-Performance All-Solid-State Lithium-Ion Batteries

All-solid-state lithium-ion batteries (ASSLIBs) have gained substantial attention worldwide due to their intrinsic safety and high energy density. However, the large interfacial resistance of ASSLIBs, which originates from the interfacial reactions and inferior electrode-electrolyte contact between electrodes and solid electrolytes, dramatically constrains their electrochemical performance. Here a dual shell interfacial nanostructure is rationally designed to enable high-performance ASSLIBs, in which the inner shell LiNbO3 suppresses the interfacial reactions while the outer shell Li10GeP2S12 enables intimate electrode-electrolyte contact. As a result, the dual shell structured Li10GeP2S12@LiNbO3@LiCoO2 exhibits a high initial specific capacity of 125.8 mAh g(-1) (1.35 mAh cm(-2)) with an initial Coulombic efficiency of 90.4% at 0.1 C and 87.7 mAh g(-1) at 1 C. More importantly, in situ X-ray absorption near edge spectroscopy was performed for the first time to reveal the interfacial reactions between Li10GeP2S12 and LiCoO2. This dual shell nanostructure demonstrates an ideal interfacial configuration for realizing high-performance ASSLIBs.