Mapping of composition‐rheology relationships in polymer composite‐type precursors

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. Highlights Rheology 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.