Mechanical Properties of Li_10.35Ge_1.35P_1.65S₁₂ with Different Particle Sizes

Abstract

Mechanical properties of Li_10.35Ge_1.35P_1.65S₁₂(LGPS) solid electrolytes with different grain sizes were investigated via indentation tests. Hand-milled LGPS (HM LGPS, d₅₀:1.32 µm) and wet-milled LGPS (WM LGPS, d₅₀:0.46 µm) powders were uniaxially pressed to obtain pellet samples. The HM LGPS and WM LGPS pellets had a similar bulk density of 1.63 g cm^–3. At the initial loading/unloading, the WM LPGS pellet showed a large deformation owing to a decrease in cavities compared with the HM LGPS. In the subsequent cycles, both pellets exhibited elastic deformation behavior in the pressure range up to 20 N. The elastic modulus and relative residual depth of HM LGPS and WM LGPS were 21.7 GPa and 0.41 GPa and 0.75 and 0.71, respectively. This result revealed that WM LGPS is more elastically deformable and less plastically deformable than HM LGPS, which could be associated with the grain boundary strengthening interpreted by the Hall-Petch relation. Based on these mechanical properties, the superior cycle stability at the In-Li electrode/WM LGPS electrolyte interface during charging/discharging was discussed. Controlling the mechanical properties of sulfide solid electrolytes by the grain size is important for suppressing physical degradation in all-solid-state batteries.