New Synthesis of Carbonaceous Lithium Hosts for High-Performance Lithium Metal Batteries

Lithium metal is a highly promising anode material for next-generation lithium batteries. However, challenges such as non-uniform lithium nucleation, dendritic growth, and significant volume changes lead to rapid cell failure, limiting its practical application. In this study, we present a defective graphene shell grown on a carbon matrix as a stable host for lithium metal, produced via carbide-mediated catalytic hydrogenolysis. This structure features numerous nano-channels with defective graphene shells on its surface, effectively guiding dendrite-free lithium deposition and accommodating a substantial amount of metallic lithium with minimal volume change. As a result, this host demonstrates excellent cycle stability (87.2% capacity retention after 500 cycles) and low dimensional variation (9 μm) in carbonate electrolyte full-cell evaluations. Additionally, when used as a lithium-ion flux-regulating interlayer, our versatile lithium host enhances cycling performance in argyrodite Li₆PS₅Cl-based high energy density all-solid-state battery full-cell configurations.