High-throughput screening of protective layers to stabilize the electrolyte-anode interface in solid-state Li-metal batteries

Solid-state Li-metal batteries have attracted growing interest over the years as a promising candidate for next-generation energy storage. Yet, the Li metal not only spontaneously reacts with most solid-state electrolytes (SSEs), but also triggers Li dendrite growth in the SSEs at a lower current density than traditional liquid electrolytes. Buffering the electrolyte-anode interface with a protective layer could be a viable solution to this problem. Herein, we search for candidate protective-layer materials from 2316 experimentally known Li-containing compounds using high-throughput first principles calculations. Tiered screening of both stability and electronic structure allows the identification of 5, 28 and 7 materials as suitable for protecting Li7La3Zr2O12, Li3PS4 and LiTi2(PO4)3, respectively. We demonstrate that electron transfer from Li metal to SSE is successfully blocked by the protective layer to restrain the dendrite growth. This work enables a significant reduction of search space for materials discoveries in protective layer for solid-state Li-metal batteries.