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

Abstract

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″-Al O electrolyte) that exceed 15 mA cm . Second, introducing a wetting interfacial film of Na–K liquid between Li metal and Li La Zr Ta O solid electrolyte doubles the critical current density and permits cycling at areal capacities that exceed 3.5 mAh cm . These design approaches hold promise for overcoming electrochemomechanical stability issues that have heretofore limited the performance of solid-state metal batteries. + ‒2 ‒2 2 3 6.75 3 1.75 0.25 12