Highly Conductive Single-Ion Polymeric Electrolyte for Long-Cycle-Life Lithium Metal Batteries

Considerable research has been conducted on single-ion conductive polymeric electrolytes with high lithium ion transference numbers. However, low ionic conductivity is a long-standing challenge for lithium metal batteries, hindering the development of extending their cycle life. In this study, we synthesized a novel fluorine-containing single-ion polymeric electrolyte, LiP(VDF-co-MAF)BB (Polyvinylidene fluoride trifluoromethyl acrylate lithium borate polymer; subsequently referred to as PPMBB), exhibiting a room temperature conductivity of 1.03 × 10−3 S/cm. This electrolyte demonstrates a high lithium ion transference number of 0.7901 and an extended electrochemical stability window of 5.5 V. Under a 2 C discharge rate, it manifests a remarkable discharge specific capacity of 146.8 mAh/g. Moreover, even after 364 cycles, the capacity retention remains at 76%. The single-ion polymeric gel electrolyte designed in this work provides a promising strategy for the prolonged cycling performance of lithium metal batteries.