Understanding the self-assembly of cellulose nanocrystals dispersions comprising stimuli-responsive polymers

Cellulose nanocrystals (CNCs) are high-aspect ratio colloids that self-organize into liquid crystalline phases in solution. Taking advantage of this self- organization behaviour, we strive to develop soft CNC-based artificial muscles capable of directional (anisotropic) actuation. To this end, we decorate the CNCs with temperature-responsive polymer chains and we subsequently align and cross-link these building blocks to form colloidal hydrogels. To achieve directional actuation, the polymer-grafted CNCs must align along a common direction throughout the entire material. This configuration is extremely challenging to obtain and typically requires the use of external orienting fields such as magnetic fields. Using a combination of small- and wide-angle X-ray scattering (SAXS/WAXS) we aim at unravelling the self-organization of these polymer-grafted CNCs and use the acquired knowledge to realize macroscopically aligned nano composite artificial muscles.