Strongly Metal-Adhesive and Self-Healing Gelatin@Polydopamine-Based Hydrogels with Long-Term Antioxidant Activity

Bioinspired adhesives have been increasingly developed, especially towards a biomedical application. Therefore, in this study, dopamine (DA) was oxidized into polydopamine (PDA) in a gelatin mixture via titration with NaIO₄ as a strong oxidant to easily obtain an adhesive antioxidant and self-healing PDA-gelatin hydrogel. Rheology experiments show a stiffness in the order of kPa and a thermal resistance above 50 °C, much above the gel-sol transition temperature of pristine gelatin. After heating at 55 °C, the gel is self-healing. In addition, just after formulation, it shows strong peeling-rate-dependent adhesion to steel with a tensile work per unit area (W) of up to 100 ± 39 J/m², which is 2.5 times higher than that of the same gel without PDA at a peeling rate of 1000 µm/s. The increase in W between peeling rates of 10 and 1000 µm/s was studied and interpreted in terms of the gels' viscoelasticity. Moreover, this hydrogel offers significant antioxidant activity (measured by DPPH scavenging) that lasts with storage for at least over 15 days, this being then prolonged for 2 additional days, which seems particularly relevant considering the importance of reactive oxygen species (ROS) in wound healing. To summarize, PDA-gelatin gel is a promising strong and antioxidant adhesive.