Controlling the Lithium-Metal Growth To Enable Low-Lithium-Metal-Excess All-Solid-State Lithium-Metal Batteries

Abstract Solid-state lithium-metal batteries are considered to be promising candidates for next-generation high-energy density storage devices to power electrical vehicles. Critical challenges for solid-state lithium-metal batteries include the large morphological changes associated with the plating and stripping of lithium metal and decomposition of the solid electrolyte, because of the reductive nature of the lithium metal, both increasing the lithium metal–solid electrolyte interface resistance. This is especially challenging when starting in the discharged state with a bare anode or “anode-less” current collector facing the solid electrolyte. To overcome this, a 100-nm thin layer of ZnO is deposited on the copper current collector with atomic layer deposition (ALD). During the first charge, this results in more homogeneous lithium-metal growth, rationalized by the formation of a Zn–Li alloy that acts as seed crystals for the lithium metal. The resulting more homogeneous lithium-metal growth maintains better contact with the solid electrolyte, leading to more reversible cycling of lithium metal. Minor prelithiating of the ZnO/Cu anode with 1 mAh/cm2 further improves the cycling performance, as demonstrated in a full all-solid-state cell using LiFePO4 as a cathode, resulting in an average Coulombic efficiency of >95%. These findings mark the first steps in an interface strategy to overcome the challenges at the solid electrolyte/lithium-metal interface in solid-state lithium-metal batteries.