Shape-recovering nanocellulose networks: Preparation, characterization and modeling

Development of strong cellulose nanofibril (CNF) networks for advanced applications, such as in the biomedical field, is of high importance owing to the biocompatible nature and plant-based origin of cellulose nanofibrils. Nevertheless, lack of mechanical strength and complex synthesis methods hinder the application of these materials in areas where both toughness and manufacturing simplicity are required. In this work, we introduce a facile method for the synthesis of a low solid content (< 2 wt%), covalently crosslinked CNF hydrogel where Poly (N-isopropylacrylamide) (NIPAM) chains are utilized as crosslinks between the nanofibrils. The resulting networks have the capability to fully recover the shape in which they were formed after various drying and rewetting cycles. Characterization of the hydrogel and its constitutive components was performed using X-ray scattering, rheological investigations and uniaxial testing in compression. Influence of covalent crosslinks was compared with networks crosslinked by the addition of CaCl₂. Among other things the results show that the mechanical properties of the hydrogels can be tuned by controlling the ionic strength of the surrounding medium. Finally, a mathematical model was developed based on the experimental results, which describes and predicts to a decent degree the large-deformation, elastoplastic behavior, and fracture of these networks.