Surface-Modified Lithium Enabling High-Performance All-Solid-State Lithium Metal Batteries

Sulfide-based all-solid-state lithium metal batteries (ASSLMBs) are promising next-generation batteries due to their high energy density and safety. However, lithium anodes face challenges like dendrite growth and side reactions at the lithium metal-sulfide electrolyte interface. In this study, we eliminated the resistive native layer on lithium metal and formed a protective layer with high ionic conductivity, mechanical strength, and cohesion by reacting lithium metal with a solution containing nitromethane, dimethoxyethene, and lithium nitrate. The lithium symmetric cell with the surface-modified Li exhibited a high critical current density of 2.8 mA cm–2 and stable cycling over 1000 h at 30 °C. The ASSLMB with surface-modified Li anode, Li6PS5Cl electrolyte, and LiNi0.78Co0.10Mn0.12O2 cathode achieved a high discharge capacity (183.2 mAh g–1) and stable cycling for 300 cycles without short-circuit at 0.3 C and 30 °C, which enabled solving the critical challenging issues of Li metal for the development of ASSLMBs.