A facile method to fabricate tough hydrogel with ultra-wide adjustable stiffness, stress, and fast recoverability

In this article, we report a synergistic strategy to develop dual physically cross-linked tough hydrogels via one-pot bulk copolymerization of N-vinyl-2-pyrrolidone, acrylic acid, and stearyl methylacrylate (SMA) without any adscititious surfactant. Due to synergic effects of hydrogen bonding and hydrophobic association, the resulted dual physically cross-linked hydrogels (DP Gel) with ultra-wide range adjustable Young's modulus (0.08–45.6 MPa), tensile stress (0.7–6.9 MPa), and toughness (3.3–23.1 MJ m −3 ). Stretching to 300%, DP Gel exhibited fast recoverability that remained ~95% of initial dissipated energy after resting in 60 °C for 3 min. Finally, scanning electron microscopy revealed that the microstructure of hydrogel changed from phase separation structure to micro phase separation as SMA added, which accounted for excellent performance of DP Gel. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018 , 56 , 1469–1474