A Rechargeable Li-Air Fuel Cell Battery Based on Garnet Solid Electrolytes

Non-aqueous Li-air batteries have been intensively studied in the past few years for their theoretically super-high energy density. However, they cannot operate properly in real air because they contain highly unstable and volatile electrolytes. Here, we report the fabrication of solid-state Li-air batteries using garnet (i.e., Li_6.4La₃Zr_1.4Ta_0.6O₁₂, LLZTO) ceramic disks with high density and ionic conductivity as the electrolytes and composite cathodes consisting of garnet powder, Li salts (LiTFSI) and active carbon. These batteries run in real air based on the formation and decomposition at least partially of Li₂CO₃. Batteries with LiTFSI mixed with polyimide (PI:LiTFSI) as a binder show rechargeability at 200 °C with a specific capacity of 2184 mAh g^-1_carbon at 20 μA cm^-2. Replacement of PI:LiTFSI with LiTFSI dissolved in polypropylene carbonate (PPC:LiTFSI) reduces interfacial resistance, and the resulting batteries show a greatly increased discharge capacity of approximately 20300 mAh g^-1_carbon and cycle 50 times while maintaining a cutoff capacity of 1000 mAh g^-1_carbon at 20 μA cm^-2 and 80 °C. These results demonstrate that the use of LLZTO ceramic electrolytes enables operation of the Li-air battery in real air at medium temperatures, leading to a novel type of Li-air fuel cell battery for energy storage.