Design of Poly(Acrylonitrile)-Based Gel Electrolytes for High-Performance Lithium Ion Batteries

The use of polyacrylonitrile (PAN) as a host for gel polymer electrolytes (GPEs) commonly produces a strong dipole–dipole interaction with the polymer. This study presents a strategy for the application of PAN in GPEs for the production of high performance lithium ion batteries. The resulting gel electrolyte GPE-AVM comprises a poly­(acrylonitrile-co-vinyl acetate) copolymer blending poly­(methyl methacrylate) as a host, which is swelled using a liquid electrolyte (LE) of 1 M LiPF6 in carbonate solvent. Vinyl acetate and methacrylate groups segregate the PAN chains in the GPE, which produces high ionic conductivity (3.5 × 10 –3 S cm–1 at 30 °C) and a wide electrochemical voltage range (>6.5 V) as well as an excellent Li+ transference number of 0.6. This study includes GPE-AVM in a full-cell battery comprising a LiFePO4 cathode and graphite anode to promote ion motion, which reduced resistance in the battery by 39% and increased the specific power by 110%, relative to the performance of batteries based on LE. The proposed GPE-based battery has a capacity of 140 mAh g–1 at a discharge rate of 0.1 C and is able to deliver 67 mAh g–1 of electricity at 17 C. The proposed GPE-AVM provides a robust interface with the electrodes in full-cell batteries, resulting in 93% capacity retention after 100 charge–discharge cycles at 17 C and 63% retention after 1000 cycles.