Quantitative Insights into the Effects of Post-Cross-Linking on Physical Performance Improvement and Surface-Cracking Healing of a Hydrogel

We report a post-cross-linking protocol that can improve the mechanical properties, freezing resistance, and fracture energies of a covalent cross-linking hydrogel and can also enable its surface-cracking healing. We design a covalent cross-linking reaction based on 3-(methacryloylamino) propyl-trimethylammonium chloride (MPTC) and sodium acrylate (SA) to give rise to a PMPTC@PSA model hydrogel. After post-cross-linking treatment, the mechanical stress is improved by 9.0-fold, accompanied by a 3.5-fold improvement in elongation; the freezing resistance is increased by 2.5-fold, which is reflected by the stretchability improvement at −35 °C. In addition, the fracture energy increased from 266 to 4686 J/m², an ∼17-fold improvement. Importantly, a surface-cracking hydrogel can be healed through the post-cross-linking treatment that enables the healing efficiency to approach 100% in terms of mechanical modulus and >81% in terms of maximum mechanical stress. This protocol is expected to provide a new option for physical performance improvement and crack healing of hydrogels in soft actuator, sensing device, and robotic applications.