Orthogonality between cellulose nanocrystals and a low-molecular weight gelator

The development of multicomponent hydrogels has gained a lot of attention in the field of soft matter, as precise tuning of the chemical nature and colloidal properties of each component brings mechanical and functional benefits compared to one-component gels. Within the field, orthogonality between a self-assembled low-molecular weight gelator (LMWG) and a colloid is a domain that has received little attention. In this study, orthogonal LMWG-colloid hydrogels were developed with the additional constraint of sustainability: a bolaamphiphile glycolipid (G-C18:1) is selected as LMWG while cellulose nanocrystals (CNCs) as colloid. These compounds are chosen for their dual role. G-C18:1 is a LMWG but it can also be used, at lower concentrations, as surface stabilizer for CNCs and tune its aggregative properties. On the other hand, tuning surface properties of CNCs drives its bulk behavior: uncharged CNCs locally aggregate and act as reinforcing agent for the LMWG gel, while negatively-charged CNCs, cross-linked with Ca²⁺, naturally form a hydrogel, which can interpenetrate with the LMWG network. By means of rheometry, small-angle X-ray scattering (SAXS) and rheo-SAXS, it is shown here how the aggregative behavior of CNCs enhances the mechanical properties of G-C18:1 hydrogels, while G-C18:1 imparts pH and temperature responsiveness to CNC hydrogels.