High-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility

Abstract Lithium metal batteries using solid electrolytes are considered to be the next-generation lithium batteries due to their enhanced energy density and safety. However, interfacial instabilities between Li-metal and solid electrolytes limit their implementation in practical batteries. Herein, Li-metal batteries using tailored garnet-type Li 7-x La 3-a Zr 2-b O 12 (LLZO) solid electrolytes is reported, which shows remarkable stability and energy density, meeting the lifespan requirements of commercial applications. We demonstrate that the compatibility between LLZO and lithium metal is crucial for long-term stability, which is accomplished by bulk dopant regulating and dopant-specific interfacial treatment using protonation/etching. An all-solid-state with 5 mAh cm −2 cathode delivers a cumulative capacity of over 4000 mAh cm −2 at 3 mA cm −2 , which to the best of our knowledge, is…