Eutectic‐Based Polymer Electrolyte with the Enhanced Lithium Salt Dissociation for High‐Performance Lithium Metal Batteries

Abstract The deployment of lithium metal anode in solid‐state batteries with polymer electrolytes has been recognized as a promising approach to achieving high‐energy‐density technologies. However, the practical application of the polymer electrolytes is currently constrained by various challenges, including low ionic conductivity, inadequate electrochemical window, and poor interface stability. To address these issues, a novel eutectic‐based polymer electrolyte consisting of succinonitrile (SN) and poly (ethylene glycol) methyl ether acrylate (PEGMEA) is developed. The research results demonstrate that the interactions between SN and PEGMEA promote the dissociation of the lithium difluoro(oxalato) borate (LiDFOB) salt and increase the concentration of free Li + . The well‐designed eutectic‐based PAN 1.2 ‐SPE (PEGMEA: SN=1: 1.2 mass ratio) exhibits high ionic conductivity of 1.30 mS cm −1 at 30 °C and superior interface stability with Li anode. The Li/Li symmetric cell based on PAN 1.2 ‐SPE enables long‐term plating/stripping at 0.3 and 0.5 mA cm −2 , and the Li/LiFePO 4 cell achieves superior long‐term cycling stability (capacity retention of 80.3 % after 1500 cycles). Moreover, Li/LiFePO 4 and Li/LiNi 0.6 Co 0.2 Mn 0.2 O 2 pouch cells employing PAN 1.2 ‐SPE demonstrate excellent cycling and safety characteristics. This study presents a new pathway for designing high‐performance polymer electrolytes and promotes the practical application of high‐stable lithium metal batteries.