Fabrication of Li-Polymer/Silica Aerogel Nanocomposite Electrolyte for an All-Solid-State Lithium Battery

The demand for solid-state lithium ion electrolytes has increased owing to the safety concerns regarding the use of lithium ion batteries, which contain flammable organic solvent electrolytes. The liquid electrolyte can give rise to serious problems such as leakage and gas explosions when the operating temperature rises. The use of an organic or inorganic solid electrolyte not only results in improved safety, but also facilitates the fabrication of miniature batteries using thin films. A solid electrolyte is required to have high lithium ion conductivity, mechanical strength, and transference number for lithium ions as well as good thermal/electrochemical stability and compatibility with the electrodes. Recently, polymer-based solid electrolytes have been widely studied for a possible replacement for liquid electrolytes. Various types of polymer-based solid electrolytes for lithium ion batteries exist, such as polyethylene oxide (PEO), polyacrylonitrile (PAN), polymethyl methacrylate (PMMA), polyvinyl chloride (PVC), and polyvinylidene fluoride (PVDF). Among them, the PEO-based polymer has attracted considerable attention, owing to its flexible skeleton and good interfacial stability with lithium electrodes. The mechanism of lithium ion conduction in the PEO-based solid-polymer electrolyte involves the coordination of the lithium ion from the Li-salt by the ether oxygen from the PEO, which moves according to the polymer segmental motion. In this study, a polymer blend of PEO and PVDF, containing fluorine as a polar element, was fabricated to improve the dissociation degree of the Li-salt. In addition, we anticipate that the addition of ultra-porous silica aerogels, which has a high porosity and specific surface area, would increase the lithium ion conductivity. The silica aerogel was fabricated from water glass using the emulsion polymerization method, as was previously described by our research group. We also investigated the effects of the PEO:PVDF molar ratio, polymer:Li-salt molar ratio, and silica aerogel content on the structural, thermal, and electrical properties.