Optimizing Current Collector Interfaces for Efficient “Anode‐Free” Lithium Metal Batteries

Abstract Current lithium (Li)‐metal anodes are not sustainable for the mass production of future energy storage devices because they are inherently unsafe, expensive, and environmentally unfriendly. The anode‐free concept, in which a current collector (CC) is directly used as the host to plate Li‐metal, by using only the Li content coming from the positive electrode, could unlock the development of highly energy‐dense and low‐cost rechargeable batteries. Unfortunately, dead Li‐metal forms during cycling, leading to a progressive and fast capacity loss. Therefore, the optimization of the CC/electrolyte interface and modifications of CC designs are key to producing highly efficient anode‐free batteries with liquid and solid‐state electrolytes. Lithiophilicity and electronic conductivity must be tuned to optimize the plating process of Li‐metal. This review summarizes the recent progress and key findings in the CC design (e.g. 3D structures) and its interaction with electrolytes.