Designing dynamic metal-coordinated hydrophobically associated mechanically robust and stretchable hydrogels for versatile, multifunctional applications in strain sensing, actuation and flexible supercapacitors

Combining the synergistic effect of dynamic metal–ligand cross-linking and hydrophobic association along with low density chemical cross-linking, we have developed a mechanically robust and stretchable hydrogel that was synthesized by micellar copolymerization of acrylamide (AM), maleic acid (MA) and butyl acrylate monomer. With optimized composition, this hydrogel showed ∼ 3 MPa tensile strength & ∼ 60 MPa compressive strength. The hydrogel is stretchable ∼ 7 times of its original length. These hydrogel materials are flexible and can be folded, bent, and twisted due to their high toughness (∼10 MJ m−3) and low elastic modulus (0.56 MPa). Because of the dynamic nature of metal–ligand interaction and hydrophobic association, the hydrogel showed high energy dissipation under tensile deformation and quick recovery of the dissipated energy after repeated loading and unloading. This hydrogel showed pH responsive mechanical properties. At lower pH, the mechanical strength and elastic modulus of the hydrogel deteriorated due to the dissociation of metal–ligand interaction. This concept was further used for demonstrating shape memory effect in these materials. Utilizing the colorimetric change in presence of Fe3+ and H+, the hydrogel can be used for data encryption-decryption technology. Combining with a thermoresponsive hydrogel (Poly (N-Isopropyl acrylamide)) layer, our hydrogel showed excellent thermoresponsive reversible actuation effect. Furthermore, because of its high ionic conductivity and strain dependent resistance change, the hydrogel can be used as a flexible strain sensor and as a compressible electrolyte in flexible supercapacitor devices.