Semi-solid alkali metal electrodes enabling high critical current densities in solid electrolyte batteries

The need for higher energy-density rechargeable batteries has generated interest in alkali metal electrodes paired with solid electrolytes. However, metal penetration and electrolyte fracture at low current densities have emerged as fundamental barriers. Here we show that for pure metals in the Li–Na–K system, the critical current densities scale inversely to mechanical deformation resistance. Furthermore, we demonstrate two electrode architectures in which the presence of a liquid phase enables high current densities while it preserves the shape retention and packaging advantages of solid electrodes. First, biphasic Na–K alloys show K+ critical current densities (with the K-β″-Al2O3 electrolyte) that exceed 15 mA cm‒2. Second, introducing a wetting interfacial film of Na–K liquid between Li metal and Li6.75La3Zr1.75Ta0.25O12 solid electrolyte doubles the critical current density and permits cycling at areal capacities that exceed 3.5 mAh cm‒2. These design approaches hold promise for overcoming electrochemomechanical stability issues that have heretofore limited the performance of solid-state metal batteries. A challenge with the use of metal anodes in batteries is their inability to sustain structural stability, especially at high currents. Here the authors examine electrochemomechanical properties of metal anodes and demonstrate an effective semi-solid electrode approach at practically relevant conditions.