Electrochemical and mechanical properties and chemical stability of Li₁₀GeP₂S₁₂/Al₂O₃ composite electrolytes

Sulfide-type solid electrolytes for all-solid-state lithium-ion batteries are required to have high ionic conductivity, high (electro) chemical stability, and suitable mechanical properties. Compositing different materials is widely performed in developing multifunctional materials. However, only a few studies have investigated sulfide electrolytes due to the concern of lowering ionic conductivity. In this study, composite electrolytes comprising Li10GeP2S12 (LGPS)-type electrolytes and nanosized Al2O3 are fabricated by a solid-state reaction. Al2O3 particles are mainly located in the voids between LGPS particles, whereas very limited oxygen content is substituted for sulfur in the LGPS structure. LGPS–Al2O3 composites exhibit ionic conductivities of ∼5 mS cm−1 without significant changes by compositing Al2O3. LGPS–Al2O3 composites are softer and have higher atmospheric stability than uncomposed LGPS. All solid-state cells that use air-exposed LGPS–Al2O3 as a separator layer exhibit an improved cycle retention compared with that using air-exposed LGPS. These results demonstrate that electrolyte compositing is an effective means of improving other properties while maintaining high lithium ionic conductivity.