Freeze–Thaw Gelation of Cellulose Nanocrystals

Gels are attractive for applications in drug delivery, tissue engineering, and 3D printing. Here, physical colloidal gels were prepared by freeze–thaw (FT) cycling of cellulose nanocrystal (CNC) suspensions. The aggregation of CNCs was driven by the physical confinement of CNCs between growing ice crystal domains. FT cycling was employed to form larger aggregates of CNCs without changing the surface chemistry or ionic strength of the suspensions. Gelation of CNC suspensions by FT cycling was demonstrated in water and other polar solvents. The mechanical and structural properties of the gels were investigated using rheometry, electron microscopy, X-ray diffraction, and dynamic light scattering. We found that the rheology could be tuned by varying the freezing time, the number of FT cycles, and concentration of CNCs in suspension