Rheological, electrochemical, and microstructural properties of graphene oxides as flowable electrodes for energy storage applications

Interest in novel energy storage and conversion methods has prompted a broad interest in potential applications of conductive, complex materials such as graphene oxide slurries. Investigating the complex rheological, material, and chemical properties of chemically exfoliated graphene oxide suspensions is a potential means to address that interest. The morphological size and clustering, rheology, and electronic conductivity are determined to characterize the properties of graphene oxide (GO) suspensions from variable centrifugation speeds. The evolution of viscosity is then analyzed under oscillatory shear, steady shear, and transient shear characteristics. The resulting microstructure is then analyzed <i>via</i> neutron scattering analysis and imaged with scanning electron microscopy. Small-Angle Neutron Scattering (SANS) of a 500<i>g</i> centrifuged GO suspension determined that particle structure is locally flat sheet-like at lengths below 100 nm, crumpled aggregates of GO sheets with surface roughness at length scales from 200 nm to 2 μm, and a dense mass fractal of overlapping GO sheets extending up to length scales of 20 μm. Increased centrifugation force of the 1000<i>g</i> GO suspension corresponded with lower zero-shear viscosity, yield stress, and less pronounced thixotropic behavior. Rheo-dielectric measurements were conducted on 1000<i>g</i> and 500<i>g</i> GO suspensions to determine the ohmic resistance, electronic conductivity, and specific capacitance. The more fluid-like microstructure of 1000<i>g</i> with smaller monodispered thinning GO sheets in suspension had lower ohmic resistance and higher electronic conductivity compared to the 500<i>g</i> GO suspension with more polydispersed larger aggregates. The 1000<i>g</i> GO suspension had the highest specific capacitance of 4.63 mF cm^-2 at the highest shear rate of 700 s^-1 due to the higher frequency of particle-particle collisions during shear within the network of smaller and more intrinsically conductive GO sheets to store charge. Therefore, the results of this study have implications for future studies in flowable carbon nanomaterials in flow battery and flow capacitor technologies.