Mechanisms of the Accelerated Li+ Conduction in MOF‐Based Solid‐State Polymer Electrolytes for All‐Solid‐State Lithium Metal Batteries

Abstract Solid polymer electrolytes (SPEs) for lithium metal batteries have garnered considerable interests owing to their low cost, flexibility, lightweight, and favorable interfacial compatibility with battery electrodes. Their soft mechanical nature compared to solid inorganic electrolytes give them a large advantage to be used in low pressure solid‐state lithium metal batteries, which can avoid the cost and weight of the pressure cages. However, the application of SPEs is hindered by their relatively low ionic conductivity. In addressing this limitation, enormous efforts are devoted to the experimental investigation and theoretical calculations/simulation of new polymer classes. Recently, metal–organic frameworks (MOFs) have been shown to be effective in enhancing ion transport in SPEs. However, the mechanisms in enhancing Li + conductivity have rarely been systematically and comprehensively analyzed. Therefore, this review provides an in‐depth summary of the mechanisms of MOF‐enhanced Li + transport in MOF‐based solid polymer electrolytes (MSPEs) in terms of polymer, MOF, MOF/polymer interface, and solid electrolyte interface aspects, respectively. Moreover, the understanding of Li + conduction mechanisms through employing advanced characterization tools, theoretical calculations, and simulations are also reviewed in this review. Finally, the main challenges in developing MSPEs are deeply analyzed and the corresponding future research directions are also proposed.