Tunable viscoelastic features of aqueous mixtures of thermosensitive ethyl(hydroxyethyl)cellulose and cellulose nanowhiskers

Ethyl(hydroxyethyl) cellulose (EHEC) is known to form reversible hydrogels in water at elevated temperatures in the presence of an ionic surfactant. However, the toxicity of common ionic surfactants (like SDS and CTAB) hampers pharmaceutical and biomedical applications of EHEC-based thermogels. Addition of a nature-based material to EHEC solutions - in the form of negatively charged cellulose nanowhiskers (CNWs) - will introduce an internal electrostatic repulsion that could also produce the balanced swelling necessary for forming a stable gel at elevated temperatures (ca. 37 °C). This may therefore be an alternative way of designing low toxicity thermoresponsive hydrogels of high mechanical strength for pharmaceutical and biomedical applications without the use of ionic surfactants. The properties of the temperature-induced gelling systems (EHEC/CNW and EHEC/SDS/CNW) were characterized by rheological methods and rheo-small angle light scattering (rheo-SALS), whereas the structure and morphology of CNWs were examined by transmission electron microscope (TEM) and small angle neutron scattering (SANS). Oscillatory shear results for the EHEC/CNW system showed that the gel temperature (ca. 37 °C) was virtually unaffected by the amount of added CNWs, while the fractal dimension values (2.2–2.3) suggested the evolution of a tighter incipient gel network with increasing level of added CNWs. Furthermore, a threefold increase of the gel strength parameter was observed with increasing concentration of CNWs. For the EHEC/CNW/SDS system, a more open network evolved with increasing amount of CNWs, and for this system, higher values of the gel strength parameter were found. Pronounced shear-thinning, even at very low shear rates, was observed for the EHEC/CNW system at all levels of CNW addition, whereas for the EHEC/CNW/SDS system, Newtonian-like behavior was detected at low shear rates.