A solid-state electrolyte (SSE) is the core component for fabricating solid-state batteries competitive with the currently commercial Li-ion batteries. In the present study, a LiBH4·1/2NH3-MgO nanocomposite has been developed as a fast Li-ion conductor. The conductive properties depend strongly on the size of MgO nanopowders. By adding MgO nanoparticles, the first-order transition at 55 °C observed in the crystalline LiBH4·1/2NH3 is suppressed due to the conversion of LiBH4·1/2NH3 into the amorphous state. When the size of MgO decreases from 163.6 to 13.9 nm, the MgO amount required for the phase-transition suppression of LiBH4·1/2NH3 decreases linearly from 92 to 75 wt %, accompanied by a significant enhancement of ionic conductivity. The optimized nanocomposite with 75 wt % MgO of size 13.9 nm exhibits a pronouncedly high conductivity of 4.0 × 10-3 S cm-1 at room temperature, which is 20 times higher than that of the crystalline LiBH4·1/2NH3. Furthermore, a smaller size MgO contributes to a higher electrochemical stability window (ESW) owing to the stronger interfacial interaction via B-O bonds, i.e., an ESW of 4.0 V is achieved with the addition of 75 wt % MgO of size 13.9 nm.
Keywords: hydrides; interfacial effects; ionic conductor; nanocomposite; solid-state electrolyte.