Abstract
This report investigates viscoelastic and mechanical behavior of hybrid polyvinyl alcohol (PVA)-cellulose nanocrystals (CNC) hydrogel aggregated with sodium chloride (NaCl) salt. In almost all samples, wide distribution of pores with roughly equal average pore size was observed, denoting that the average porosity is independent from CNC concentration. To assess the dispersion quality of CNCs in CNC-PVA/salt hybrid samples, transmission electron microscopy (TEM) was employed. Small and large amplitude oscillatory shear (SAOS and LAOS) measurements were also performed on CNC-loaded PVA-salt hydrogels to further characterize their microstructure. At CNC loadings near the percolation threshold (15 g/L), a sudden jump in storage modulus was observed, attributing to hybrid polymer-CNC 3D network formation. The appearance of a more dramatic jump in the value of the rheological parameters at higher CNC concentrations (30 g/L) indicates the establishment of a secondary network structure upon formation of direct contacts between individual CNC particles and/or clusters. The viscoelastic behavior of the hydrogels was further investigated via LAOS approach based on Lissajous-Bowditch plots and sequence of physical processes method. In addition, through a wide range of rheological characterizations, we demonstrated successful fabrication of a healable hydrogel, able to regain original strength after disruption of the structure at sufficiently large deformations. Afterward, to explore the interactions between CNC-CNC and PVA-CNC, the Foglar-Tucker model, designed to account for modeling the orientation of particles within a matrix, was fitted on stress-overshoot (start-up) experiments. The present study on PVA-CNC hydrogels opens avenues for further developing advanced materials with tunable microstructures for tissue engineering and regenerative medicine applications.
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