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Molecules that associate to form cross-links by hydrophobic association are designed and synthesised. Hydrogels, based on cellulose nanowhiskers (CNWs), acrylamide (AM), and stearyl methacrylate (C18), were synthesised by micellar copolymerisation, using ammonium peroxydisulfate as an initiator. CNWs composite hydrogels were characterised by Fourier transform infrared spectroscopy (FTIR) and their morphologies were investigated by scanning electron microscope (SEM). The system shows the original extensibility up to about 2500%: the tensile strength and compressive strength have maximum values of 1.338 MPa and 2.835 MPa, respectively. Besides excellent mechanical properties, CNWs composite hydrogels also have the ability to self-heal and remould: this is mainly attributed to the dissociation and reassociation of the associated micelles. In contrast to conventional cellulose hydrogels, these systems, when broken or cut, can be simply repaired by bringing together fractured surfaces to self-heal at room temperature.

Cellulose possessingβ-cyclodextrin (β-CD) was used as a host molecule and cellulose possessing ferrocene (Fc) as a guest polymer. Infrared spectra, differential scanning calorimetry (DSC), ultraviolet spectroscopy (UV), and contact angle analysis were used to characterise the material structure and the inclusion behaviour. The results showed that theβ-CD-cellulose and the Fc-cellulose can form inclusion complexes. Moreover, ferrocene oxidation, and reduction of state can be adjusted by sodium hypochlorite (NaClO) as an oxidant and glutathione (GSH) as a reductant. In this study, a physical gel based onβ-CD-cellulose/Fc-cellulose was formed under mild conditions in which autonomous healing between cut surfaces occurred after 24 hours. The physical gel can be controlled in the sol-gel transition. The compressive strength of the Fc-cellulose/β-CD-cellulose gel increased with increased cellulose concentration. The host-guest interaction between the side chains of cellulose could strengthen the gel. The cellulose physical gel may eventually be used as a stimulus-responsive, healing material in biomedical applications.