Inducing Nematic Ordering of Cellulose Nanofibers using Osmotic Dehydration

The formation and characterization of nematically-ordered CNF materials (maximum order parameter f ≈ 0.8) has been studied by polarized optical microscopy, small angle x-ray scattering (SAXS), and rheological measurements as a function of CNF concentration. The wide range of CNF concentrations, from 0.5 wt% to 4.9 wt%, is obtained using osmotic dehydration with PEG. At concentrations >1.05 wt% the CNF suspension crosses an isotropic-anisotropic transition that is accompanied by a dramatic increase of the optical birefringence. The resulting nanostructures are depicted by a hierarchical model with mass fractal structures that converge into co-existing nematically-ordered regions and network-like regions, in which the correlation distances decrease upon increasing concentration. The use of rapid, upscaleble osmotic dehydration is an effective method to increase the concentration of CNF suspensions while partly circumventing the gel formation. The facile formation of highly ordered fibers can result in materials with interesting macroscopic properties.