Tough, Stretchable, Compressive Novel Polymer/Graphene Oxide Nanocomposite Hydrogels with Excellent Self-Healing Performance

Designing hydrogels with high mechanical properties without sacrificing their self-healing efficiencies remains great challenges. We have fabricated cationic polyacrylamide/graphene oxide (GO) hydrogels by free-radical polymerization of acrylamide (AM) and 2-(dimethylamino)­ethylacrylatemethochloride (DAC) in the presence of GO. The mechanical properties and self-healing ability can be tuned by the GO content and the mass ratio of AM and DAC. The ionic bonds between DAC and GO and the hydrogen bonds between AM and GO can efficiently dissipate energy and rebuild the networks. The resulting composite hydrogels possess high stiffness (Young’s modulus: ∼1.1 MPa), high toughness (∼9.3 MJ m^–3), and high fatigue resistance, as well as high self-healing efficiency (>92% of tensile strength, >99% of tensile strain and >93% of toughness). In addition, the completely dried hydrogels can recover their original mechanical values by spraying water and still possess outstanding self-healing efficiency. Our design can provide better fundamental understanding of physical properties of hydrogels and should enable the development of tough, self-healing hydrogels for practical applications.