Carbide-Mediated Catalytic Hydrogenolysis: Defective Carbonaceous Lithium Host for Liquid-Electrolyte and All-Solid-State Lithium Metal Batteries

Commercial lithium-ion batteries based on intercalation carbonaceous anodes are reaching their limit in energy density due to the limitation of theoretical capacity of electrode materials. In this regard, lithium metal is an ideal anode owing to its high specific capacity. However, the practical use of the Li metal is still challenging. The Li metal anode suffers from dendrite formation, volume change, and severe side reactions, which lead to fatal safety issues and cell degradation.<br/>Here, we propose a defective graphene shell grown on a carbon matrix as a stable lithium metal host via carbide-mediated catalytic hydrogenolysis. Unlike conventional carbon hydrogenolysis, the carbide-mediated hydrogenolysis provides not only channelling reaction but also the graphene shell with defects. These defects and nano-channels effectively mitigate the Li nucleation overpotential and achieve a stable cycle life with a comparable volume change with that of commercial graphite. Due to these features, the host exhibits good cycle stability (87.2% after 500 cycles) and low dimension variation (9 μm) in carbonate electrolyte full-cell evaluations. In addition to its good performances in the carbonate electrolyte, our versatile Li host, acting as a Li-ion flux regulating interlayer, also achieves an improved cycling performance in the argyrodite Li₆PS₅Cl based high energy density all-solid-state battery full-cell configuration.