Self-Healing Poly(acrylic acid) Hydrogels with Shape Memory Behavior of High Mechanical Strength

A promising strategy to design synthetic hydrogels with the ability to self-heal is to substitute the covalently cross-linked polymer chains by supramolecular ones. Although supramolecular hydrogels generally exhibit rapid self-healing without the need for any stimulus, they suffer from low mechanical strength which prevents them from any stress-bearing applications. Here, we describe a novel way for the production of self-healing hydrogels with shape memory behavior of high tensile strength (0.7–1.7 MPa) and stretch at break (800–900%). Hydrophobically modified poly(acrylic acid) (PAAc) chains with cetyltrimethylammonium (CTA) counterions form the physical network of such hydrogels. They were prepared via micellar copolymerization of acrylic acid with 2 mol % stearyl methacrylate (C18) as the hydrophobic comonomer in an aqueous NaBr solution of cetyltrimethylammonium bromide (CTAB). Extraction of free CTAB micelles from the physical gels results in a drastic increase in their Young’s moduli (from 8–30 to...

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