Molecular/Ionic Designs in the Electrolyte and Interphases for Lithium Metal Anode

The undesirable interactions between the charge carriers (Li + ) and various objects in the special microenvironment of batteries would cause uneven lithium (Li) metal deposition behavior, which severely impedes the application of Li metal batteries (LMBs). In recent years, many works focus on optimizing these interactions by functional molecules/ions modification. Nevertheless, related reviews are still absent. Here, this review introduces the regulation methods of Li metal deposition from molecular/ionic designs, which is a new perspective including Li + flux homogenization, the de‐solvation process regulation, optimizing the solid electrolyte interphase (SEI) in conventional solvation structure and anion‐rich solvation structure. Also, the general design principles are studied in each mechanism and some suggestions are proposed in the prospective future directions, aiming to guide the development of molecular/ionic designs and the actual application of LMBs with high energy densities.