Hadi Khani

All‐solid‐state lithium‐metal batteries offer higher energy density and safety than lithium‐ion batteries, but their practical applications have been pushed back by the sluggish Li + transport, unstable electrolyte/electrode interface, and/or difficult processing of their solid‐state electrolytes. Li + ‐conducting composite polymer electrolytes (CPEs) consisting of sub‐micron particles of an oxide solid‐state electrolyte (OSSE) dispersed in a solid, flexible polymer electrolyte (SPE) have shown promises to alleviate the low Li + conductivity of SPE, and the high rigidity and large interfacial impedance of OSSEs. Solution casting has been by far the most widely used procedure for the preparation of CPEs in research laboratories; however, this method imposes several drawbacks including particle aggregation and settlement during a long‐term solvent evaporation step, excessive use of organic solvents, slow production time, and mechanical issues associated with handling of ultra‐thin films of CPEs (<50 µm). To address these challenges, an electrophoretic deposition (EPD) method is developed to in situ deposit ultra‐thin CPEs on lithium‐iron‐phosphate (LFP) cathodes within just a few minutes. EPD‐prepared CPEs have shown better electrochemical performance in the lithium‐metal battery than those CPEs prepared by solution casting due to a better dispersion of OSSE within the SPE matrix and improved CPE contact with LFP cathodes.