Synthesis of poly(acrylic acid)–Fe3+/gelatin/poly(vinyl alcohol) triple‐network supramolecular hydrogels with high toughness, high strength and self‐healing properties

Abstract Hydrogels with good mechanical and self‐healing properties are of great importance for various applications. Poly(acrylic acid)–Fe 3+ /gelatin/poly(vinyl alcohol) (PAA‐Fe 3+ /Gelatin/PVA) triple‐network supramolecular hydrogels were synthesized by a simple one‐pot method of copolymerization, cooling and freezing/thawing. The PAA‐Fe 3+ /Gelatin/PVA triple‐network hydrogels exhibit superior toughness, strength and recovery capacity compared to single‐ and double‐network hydrogels. The mechanical properties of the synthesized hydrogels could be tailored by adjusting the compositions. The PAA‐Fe 3+ /Gelatin/PVA triple‐network hydrogel with 0.20 mmol Fe 3+ , 3% gelatin and 15% PVA could achieve good mechanical properties, the tensile strength and elongation at break being 239.6 kPa and 12.8 mm mm −1 , respectively, and the compression strength reaching 16.7 MPa under a deformation of about 91.5%. The synthesized PAA‐Fe 3+ /Gelatin/PVA triple‐network hydrogels have good self‐healing properties owing to metal coordination between Fe 3+ and carboxylic groups, hydrogen bonding between the gelatin chains and hydrogen bonding between the PVA chains. Healed PAA‐Fe 3+ (0.20)/Gelatin3%/PVA15% triple‐network hydrogels sustain a tensile strength of up to 231.4 kPa, which is around 96.6% of the tensile strength of the original samples. Therefore, the synthesized triple‐network supramolecular hydrogels would provide a new strategy for gel research and expand the potential for their application. © 2019 Society of Chemical Industry