An Antipulverization and High‐Continuity Lithium Metal Anode for High‐Energy Lithium Batteries

Abstract Lithium metal is one of the most promising anode candidates for next‐generation high‐energy batteries. Nevertheless, lithium pulverization and associated loss of electrical contact remain significant challenges. Here, an antipulverization and high‐continuity lithium metal anode comprising a small number of solid‐state electrolyte (SSE) nanoparticles as conformal/sacrificial fillers and a copper (Cu) foil as the supporting current collector is reported. Guiding by the SSE, this new anode facilitates lithium nucleation, contributing to form a roundly shaped, micro‐sized, and dendrite‐free electrode during cycling, which effectively mitigates the lithium dendrite growth. The embedded Cu current collector in the hybrid anode not only reinforces the mechanical strength but also improves the efficient charge transfer among active lithium filaments, affording good electrode structural integrity and electrical continuity. As a result, this antipulverization and high‐continuity lithium anode delivers a high average Coulombic efficiency of ≈99.6% for 300 cycles under a current density of 1 mA cm⁻². Lithium–sulfur batteries (elemental sulfur or sulfurized polyacrylonitrile cathodes) equipped with this anode show high‐capacity retentions in their corresponding ether‐based or carbonate‐based electrolytes, respectively. This new electrode provides important insight into the design of electrodes that may experience large volume variation during operations.