Stack Pressure Dependence of Li Stripping/Plating Performance in All-Solid-State Li Metal Cells Containing Sulfide Glass Electrolytes.

Sulfide-based all-solid-state Li/S batteries have attracted considerable attention as next-generation batteries with high energy density. However, their practical applications are limited by short-circuiting due to Li dendrite growth. One of the possible reasons for this phenomenon is the contact failure caused by void formation at the Li/solid electrolyte interface during Li stripping. Herein, we studied the operating conditions, such as stack pressure, operating temperature, and electrode composition, that could potentially suppress the formation of voids. Furthermore, we investigated the effects of these operating conditions on the Li stripping/plating performance of all-solid-state Li symmetric cells containing glass sulfide electrolytes with a reduction tolerance. As a result, symmetric cells with Li-Mg alloy electrodes instead of Li metal electrodes exhibited high cycling stability at current densities above 2.0 mA cm, a temperature of 60 °C, and stack pressures of 3-10 MPa. In addition, an all-solid-state Li/S cell with a Li-Mg alloy negative electrode operated stably for 50 cycles at a current density of 2.0 mA cm, stack pressure of 5 MPa, and temperature of 60 °C, while its measured capacity was close to a theoretical value. The obtained results provide guidelines for the construction of all-solid-state Li/S batteries that can reversibly operate at high current densities.