In this investigation, we report a non-covalent (ionic interlocking and hydrogen bonding) strategy of self-healing in a covalently crosslinked organic-inorganic hybrid nanocomposite hydrogel, with specific emphasis on tuning its properties fitting into a muscle mimetic material. The hydrogel was prepared via an in situ free radical polymerization of sodium acrylate (SA) and successive crosslinking in the presence of starch grafted with poly(2-(methacryloyloxy)ethyl trimethyl ammonium chloride) (PMTAC) and montmorillonite modified with cetyl ammonium bromide (OMMT). This hydrogel shows stimuli triggered self-healing following damage in both neutral and acidic solutions (pH = 7.4 and pH = 1.2). This behavior was reported using stress-strain experiments and rheological analyses of the hydrogel segments joined at their fracture points. The hydrogel was also able to display shape memory properties in the presence of water as well as stimuli (salt, acid and electric impulse) driven actuation behavior. It was observed that the ultimate tensile strength (UTS) of the self-healed hydrogel at pH = 7.4 was comparable to the extensor digitorum longus (EDL) muscle of a New Zealand white rabbit and the as synthesized self-healable hydrogel was found to be non-cytotoxic against NIH 3T3 fibroblast cells.
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