Rapid Recovery Double Cross-Linking Hydrogel with Stable Mechanical Properties and High Resilience Triggered by Visible Light

The designed tough hydrogels, depending on energy dissipation mechanism, possess excellent biocompatibility, stimuli-responsiveness, and outstanding mechanical properties. However, the application of hydrogels is greatly limited in actuators and sensors for the lack of instantaneous recovery and resilience. In this work, we synthesized a double cross-linking poly­(acrylic acid) hydrogel via a simple, one-pot, visible-light-trigger polymerization, with carboxymethyl cellulose as initiator and the first cross-linker, N,N′-methylene bis­(acrylamide) (MBA) as the second cross-linker. The tensile strength and elastic modulus are in the range of 724–352 kPa and 115–307 kPa, respectively, depending on the MBA content. The swelling ratio of hydrogels dramatically decreased with increasing the MBA content. DMA results indicate that the internal friction between molecules within the hydrogel decreases with the increase of MBA content. Cyclic tensile tests show that after the structure stabilizes, the resilience, maximum stress, and residual strain of Gel-2 maintains over 93% (95% for successive cyclic tensile test), 115 kPa and less than 3%, respectively, at a strain of 125%. The values of resilience and residual strain are almost constant in both successive and intermittent cyclic tensile tests. Moreover, the swollen hydrogel has higher resilience and lower residual strain than the same hydrogel in the as-prepared state.