Recent Progress of Advanced Functional Separators in Lithium Metal Batteries

As a representative in the post‐lithium‐ion batteries (LIBs) landscape, lithium metal batteries (LMBs) exhibit high‐energy densities but suffer from low coulombic efficiencies and short cycling lifetimes due to dendrite formation and complex side reactions. Separator modification holds the most promise in overcoming these challenges because it utilizes the original elements of LMBs. In this review, separators designed to address critical issues in LMBs that are fatal to their destiny according to the target electrodes are focused on. On the lithium anode side, functional separators reduce dendrite propagation with a conductive lithiophilic layer and a uniform Li‐ion channel or form a stable solid electrolyte interphase layer through the continuous release of active agents. The classification of functional separators solving the degradation stemming from the cathodes, which has often been overlooked, is summarized. Structural deterioration and the resulting leakage from cathode materials are suppressed by acidic impurity scavenging, transition metal ion capture, and polysulfide shuttle effect inhibition from functional separators. Furthermore, flame‐retardant separators for preventing LMB safety issues and multifunctional separators are discussed. Further expansion of functional separators can be effectively utilized in other types of batteries, indicating that intensive and extensive research on functional separators is expected to continue in LIBs. This review summarizes various types of functional separators designed to address challenges and enhance the performance of lithium metal batteries (LMBs), with a specific focus on the target electrode in need of improvement. Additionally, the review introduces functional separators designed to address safety issues in LMBs, along with multifunctional separators.