Abstract Considering their simplicity, processibility, and tunable rheological properties, polymer composite‐type precursors hold exceptional promise in the processing of polymers, ceramics, metals, and their composites. This large variety of precursors used in many different applications cover a large compositional space with dramatically varying rheological properties. Understanding how precursor composition influences their rheological properties is a key need towards streamlining the design and implementation of these precursors. With regard to this design advancement, this study elucidates the composition‐rheology relationships of graphene‐poly(ethylene) oxide (PEO) composite inks as a sample polymer composite‐type precursor. To this end, shear and extensional rheology of numerous compositions were studied across a wide compositional space, which varied graphene concentration, total solid concentration, and binder molecular weight. These studies showed that composition greatly affected various rheological parameters, such as the overall presence of yielding behavior. Specifically, this study illustrated the influence of (i) binder structure, (ii) total solid loading, and (iii) binder‐filler interactions on ink rheology. Extensional rheology was studied to examine how relaxation behaviors were dependent on composition and explicate how relaxation behaviors coincide with responses to shear forces. In tandem, our results illuminate significant composition‐rheology relationships in polymer composite‐type precursors. HighlightsRheology of polyethylene oxide‐graphene composite precursors were studied.Shear and extensional rheology, and their correlations were investigated.Composition‐binder molecular weight‐yielding relationships were elucidated.Extensional relaxation regimes were identified with respect to composition.Results can be used to determine compositional ranges for different processes. 
                        more » 
                        « less   
                    This content will become publicly available on December 20, 2025
                            
                            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. HighlightsShear‐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. 
        more » 
        « less   
        
    
    
                            - PAR ID:
- 10643779
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Polymer Composites
- Volume:
- 46
- Issue:
- 8
- ISSN:
- 0272-8397
- Format(s):
- Medium: X Size: p. 6998-7011
- Size(s):
- p. 6998-7011
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            Stretchable conductive composites (SCCs) are generally elastomer matrices filled with conductive fillers. They combine the conductivity of metals and carbon materials with the flexibility of polymers, which are attractive properties for applications such as stretchable electronics, wearable devices, and flexible sensors. Most conventional conductive composites that are filled with only one type of conductive filler face issues in mechanical and electrical properties. Recently, some studies introduced secondary fillers to create hybrid‐filler SCCs to solve these problems. The secondary fillers produce a synergistic effect with the primary fillers to enhance the electrical conductivity of the composites. They also improve the thermal conductivity and mechanical properties or impart composites with special functions like catalysis and self‐healing. Herein, the fabrication methods, stretchability enhancement strategies, and piezoresistivity of SCCs are analyzed, and their latest applications in stretchable electronics are introduced. Finally, the challenges and prospects of their development are discussed.more » « less
- 
            To push upper boundaries of thermal conductivity in polymer composites, understanding of thermal transport mechanisms is crucial. Despite extensive simulations, systematic experimental investigation on thermal transport in polymer composites is limited. To better understand thermal transport processes, we design polymer composites with perfect fillers (graphite) and defective fillers (graphite oxide), using polyvinyl alcohol (PVA) as a matrix model. Measured thermal conductivities of ~1.38 ± 0.22 W m−1K−1in PVA/defective filler composites is higher than those of ~0.86 ± 0.21 W m−1K−1in PVA/perfect filler composites, while measured thermal conductivities in defective fillers are lower than those of perfect fillers. We identify how thermal transport occurs across heterogeneous interfaces. Thermal transport measurements, neutron scattering, quantum mechanical modeling, and molecular dynamics simulations reveal that vibrational coupling between PVA and defective fillers at PVA/filler interfaces enhances thermal conductivity, suggesting that defects in polymer composites improve thermal transport by promoting this vibrational coupling.more » « less
- 
            Three-dimensional printing (3DP) of functional materials is increasingly important for advanced applications requiring objects with complex or custom geometries or prints with gradients or zones with different properties. A common 3DP technique is direct ink writing (DIW), in which printable inks are comprised of a fluid matrix filled with solid particles, the latter of which can serve a dual purpose of rheology modifiers to enable extrusion and functional fillers for performance-related properties. Although the relationship between filler loading and viscosity has been described for many polymeric systems, a thorough description of the rheological properties of three-dimensional (3D) printable composites is needed to expedite the creation of new materials. In this manuscript, the relationship between filler loading and printability is studied using model paraffin/photopolymer composite inks containing between 0 and 73 vol. % paraffin microbeads. The liquid photopolymer resin is a Newtonian fluid, and incorporating paraffin microbeads increases the ink viscosity and imparts shear-thinning behavior, viscoelasticity, and thixotropy, as established by parallel plate rheometry experiments. Using Einstein and Batchelor's work on colloidal suspension rheology, models were developed to describe the thixotropic behavior of inks, having good agreement with experimental results. Each of these properties contributes to the printability of highly filled ([Formula: see text]43 vol. % paraffin) paraffin/photopolymer composite inks. Through this work, the ability to quantify the ideal rheological properties of a DIW ink and to selectively control and predict its rheological performance will facilitate the development of 3D printed materials with tunable functionalities, thus, advancing 3DP technology beyond current capabilities.more » « less
- 
            null (Ed.)Carbon fiber (CF)-reinforced thermoplastic composites have been widely used in different structural applications due to their superior thermal and mechanical properties. The big area additive manufacturing (BAAM) system, developed at Oak Ridge National Laboratory’s Manufacturing Demonstration Facility, has been used to manufacture several composite components, demonstration vehicles, molds, and dies. These components have been designed and fabricated using various CF-reinforced thermoplastics. In this study, the dynamic rheological and mechanical properties of a material commonly used in additive manufacturing, 20 wt% CF-acrylonitrile butadiene styrene (ABS), as well as three CF-reinforced high-temperature polymers, 25 wt% CF-polyphenylsulfone (PPSU), 35 wt% CF-polyethersulfone (PES), and 40 wt% CF-polyphenylene sulfide (PPS), used to print molds were investigated. The viscoelastic properties, namely storage modulus, loss modulus, tan delta, and complex viscosity, of these composites were studied, and the rheological behavior was related to the BAAM extrusion and bead formation process. The results showed 20 wt% CF-ABS and 40 wt% CF-PPS to display a more dominant elastic component at all frequencies tested while 25 wt% CF-PPSU and 35 wt% CF-PES have a more dominant viscous component. This viscoelastic behavior is then used to inform the deposition and bead formation process during extrusion on the BAAM system.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
