Impact of salt and fillers on the rheological properties of polymer composites

Abstract Polymer composites with salts or conductive fillers are promising for various solid‐state energy storage applications, where processability is often determined by their rheological properties. This study investigates the effect of lithium salts and conductive fillers on the rheological behavior of polylactic acid (PLA)‐based composites. We specifically examine how these additives influence complex viscosity and the interactions between the salt, fillers, and polymer. Our findings reveal that adding salt to the polymer reduces its viscosity, whereas adding conductive fillers imparts a shear‐thinning property, which is advantageous for thermal processing methods like thermal drawing, injection molding, or 3D printing. The combination of salt and conductive fillers results in multifunctional electrode‐electrolyte composites with enhanced shear‐thinning behavior and improved storage modulus. Characterizations through x‐ray diffraction, electrical measurements, and transmission electron microscopy link the electrical properties and morphology with rheological behavior. The formation of a robust filler network in these composites ensures stable viscoelastic behavior across a range of temperatures and frequencies, indicating their suitability for efficient manufacturing of polymer‐based solid‐state electrode‐electrolyte composites via thermal processing. Highlights Shear‐thinning behavior enhanced by conductive fillers. Viscosity increased with CB and CNT fillers, forming robust networks. Salt reduced viscosity but filler networks dominated flow behavior. Filler combinations led to stable viscoelastic properties across temperatures. Polymer electrolyte–electrode composites improved processability and storage modulus.