Addressing Manufacturability and Processability in Polymer Gel Electrolytes for Li/Na Batteries.

Gel electrolytes are prepared with Ultra High Molecular Weight (UHMW) polyethylene oxide (PEO) in a concentration ranging from 5 to 30 wt.% and Li- and Na-doped 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide (PYR14-TFSI) by a simple procedure consisting of dissolving PEO by melting it directly in the liquid electrolyte while stirring the blend. This procedure is fast, reproducible and needs no auxiliary solvents, which makes it sustainable and potentially easy to scale up for mass production. The viability of the up-scaling by extrusion has been studied. Extrusion has been chosen because it is a processing method commonly employed in the plastics industry. The structure and morphology of the gel electrolytes prepared by both methods have been studied by DSC and FTIR, showing small differences among the two methods. Composite gels incorporation high concentrations of surface modified sepiolite fibers have been successfully prepared by extrusion. The rheological behavior and ionic conductivity of the gels have been characterized, and very similar performance of the extruded and manually mixed gels is detected. Ionic conductivity of all the gels, including the composites, are at or over 0.4 mS cm at 25 °C, being at the same time thermoreversible and self-healing gels, tough, sticky, transparent and stretchable. This combination of properties, together with the viability of their industrial up-scaling, makes these gel electrolyte families very attractive for their application in energy storage devices.