Dipole–Dipole and H‐Bonding Interactions Significantly Enhance the Multifaceted Mechanical Properties of Thermoresponsive Shape Memory Hydrogels

Abstract

High strength hydrogels were previously constructed based on dipole–dipole and hydrogen bonding reinforcement. In spite of the high tensile and compressive strengths achieved, the fracture energy of the hydrogels strengthened with sole noncovalent bondings was rather low due to the lack in energy dissipating mechanism. In this study, combined dipole–dipole and hydrogen bonding interactions reinforced (DHIR) hydrogels are synthesized by one‐step copolymerization of three feature monomers, namely acrylonitrile (AN, dipole monomer), acrylamide (AAm, H‐bonding monomer), and 2‐acrylamido‐2‐methyl‐1‐propanesulfonic acid (AMPS, anionic monomer) in the presence of PEGDA575, a hydrophilic crosslinker. The electrostatic repulsion from PAMPS allows the gel network to absorb water readily, and meanwhile the synergistic effect of dipole–dipole and H‐bonding interactions enable the DHIR hydrogel to withstand up to 8.3 MPa tensile stress, 4.8 MPa compressive stress and 140–716% elongation at break with the fracture energy reaching as high as 5500 J/m 2. In addition, this DHIR hydrogel exhibits reversible mechanical properties after undergoing cyclic loading and unloading. Interestingly, the DHIR hydrogels with appropriate compositions demonstrate temperature‐tunable mechanical properties as well as accompanied shape memory effect. The dual noncovalent bonding strengthening mechanism reported here offers a universal strategy for significantly enhancing the comprehensive mechanical properties of hydrogels.