Garnet-Type Fast Li-Ion Conductors with High Ionic Conductivities for All-Solid-State Batteries.

All-solid-state Li-ion batteries with metallic Li anodes and solid electrolytes could offer superior energy density and safety over conventional Li-ion batteries. However, compared with organic liquid electrolytes, the low conductivity of solid electrolytes and large electrolyte/electrode interfacial resistance impede their practical application. Garnet-type Li-ion conducting oxides are among the most promising electrolytes for all-solid-state Li-ion batteries. In this work, the large-radius Rb is doped at the La site of cubic LiGaLaZrO to enhance the Li-ion conductivity for the first time. The LiGaLaRbZrO electrolyte exhibits a Li-ion conductivity of 1.62 mS cm at room temperature, which is the highest conductivity reported until now. All-solid-state Li-ion batteries are constructed from the electrolyte, metallic Li anode, and LiFePO active cathode. The addition of Li(CFSO)N electrolytic salt in the cathode effectively reduces the interfacial resistance, allowing for a high initial discharge capacity of 152 mAh g and good cycling stability with 110 mAh g retained after 20 cycles at a charge/discharge rate of 0.05 C at 60 °C.