Physically Crosslinked Poly(methacrylic acid)/Gelatin Hydrogels with Excellent Fatigue Resistance and Shape Memory Properties

Hydrogels endure various dynamic stresses, demanding robust mechanical properties. Despite significant advancements, matching hydrogels' strength to biological tissues and plastics is often challenging without applying potentially harmful crosslinkers. Using hydrogen bonds as sacrificial bonds offers a promising strategy to produce tough, versatile hydrogels for biomedical and industrial applications. Poly(methacrylic acid) (PMA)/gelatin hydrogels were synthesized by thermally induced free-radical polymerization and crosslinked only by physical bonds, without adding any chemical crosslinker. The addition of gelatin increased the formation of hydrophobic domains in the structure of the hydrogels, which acted as permanent crosslinking points. The increase in PMA and gelatin contents generally led to a lower equilibrium water content (WC), higher thermal stability and better mechanical properties. The values of tensile strength and toughness reached up to 1.44 +/- 0.17 MPa and 4.91 +/- 0.51 MJ m-3, respectively, while the compressive modulus and strength reached up to 0.75 +/- 0.06 MPa and 24.81 +/- 5.85 MPa, respectively, with the WC being higher than 50 wt.%. The obtained values for compressive mechanical properties are comparable with super-strong hydrogels reported in the literature. In addition, hydrogels exhibited excellent fatigue resistance and biocompatibility, as well as great shape memory properties, which make them prominent candidates for a wide range of biomedical applications.