Polyvinylidene Fluoride-Based Gel Polymer Electrolytes for Calcium Ion Conduction: A Study of the Influence of Salt Concentration and Drying Temperature on Coordination Environment and Ionic Conductivity

Calcium-ion batteries emerged as a potential sustainable alternative energy storage system; however, there remains the need to further develop electrolytes to improve their performance. We report a gel polymer electrolyte (GPE)-based on polyvinylidene fluoride (PVDF) for calcium ion conduction. The gel electrolyte was synthesized by combining a PVDF polymer host, Ca(TFSI)2 salt, and N-methyl-2-pyrrolidone (NMP) solvent. Using Fourier transform infrared spectroscopy, we analyze the effect of salt concentration and drying temperature on the degree of salt dissociation in the electrolyte. Our results show that the concentration of free cations in the electrolyte is primarily coordinated with NMP as well as PVDF, generating a suitable network for ion transport, i.e., a liquid electrolyte encompassed within a polymer matrix. We find that processing conditions such as drying temperature, which varies solvent content, play a critical role in developing polymer electrolytes that demonstrate optimal electrochemical performance. The GPEs are semicrystalline and stable up to 120 °C, which is critical for their use in applications such as in electric vehicles and renewable energy storage systems. The ionic conductivity of the GPEs exhibit Arrhenius-type behavior, and the total ionic conductivity at room temperature is suitable for applications, with values of 0.85 × 10-4 S/cm for 0.5 M and 3.56 × 10-4 S/cm for 1.0 M concentrations. The results indicate that the GPE exhibits high conductivity and good stability, making it a promising candidate for use in high-performance calcium ion batteries.