New insights into the flow and microstructural relaxation behavior of biphasic cellulose nanocrystal dispersions from RheoSANS

Cellulose nanocrystals (CNC) have been studied as nanostructured building blocks for functional materials and function as a model nanomaterial mesogen for cholesteric (chiral nematic) liquid crystalline phases. In this study, both rheology and small angle neutron scattering (RheoSANS) were used to measure changes in flow-oriented order parameter and viscosity as a function of shear rate for isotropic, biphasic, liquid crystalline, and gel dispersions of CNC in deuterium oxide (D2O). In contrast to plots of viscosity versus shear rate, the order parameter trends showed three distinct rheological regions over a range of concentrations. This finding is significant because the existence of three rheological regions as a function of shear rate is a long-standing signature of liquid crystalline phases composed of rod-like polymers, but observing this trend has been elusive for high-concentration dispersions of anisotropic nanomaterials. The results of this work are valuable for guiding the development of processing methodologies for producing ordered materials from CNC dispersions and the broader class of chiral nanomaterial mesogens.