Optimization of a Solvent Exchange Method Enabling the Use of Dehydrated Cellulose Nanofibers as the Thickener in Lubricating Oleogels

A method that enabled the formulation of lubricating oleogels using dried cellulose nanofibers (CNFs) as an eco-friendly thickener in castor oil was studied. In their dehydrated state, strong hydrogen bonding between nanofibers and high hydrophilicity are the main obstacles to their dispersion in oil. Hence, clusters of dried CNFs had to be previously detached by their dispersion in water. The resulting hydrogels were then subjected to methanol washes to displace the water from the nanofibers. After centrifugation, the methanol-wetted precipitate was readily dispersed in castor oil, forming an oleogel once the methanol was removed. Optimization was conducted in terms of the following variables: (a) hydrogel processing method; (b) hydrogel pH; (c) methanol/hydrogel ratio; (d) number of washes; and (e) oleogel CNF concentration. Their effect on the oleogel linear viscoelastic behavior was analyzed. In general, they demonstrated a prevailing elastic behavior denoted by a well-developed plateau region. The CNF concentration was found to have a more remarkable impact on the oleogels' rheological behavior than any other variable studied. Hence, substantial differences were observed between 1 and 2 wt.%. The CNFs exhibited a very remarkable thickening capacity in castor oil, achieving a plateau modulus of ca. 700 Pa with just 2 wt.%. Moreover, the resulting oleogels maintained a uniform texture even after one year of storage. This indicates that the oleogels were both homogeneous and storage stable, effectively overcoming the stability issues associated with direct dispersion of dried CNFs in castor oil.