Dynamic Metal-Coordinated Adhesive and Self-Healable Antifreezing Hydrogels for Strain Sensing, Flexible Supercapacitors, and EMI Shielding Applications.

Dynamic metal-coordinated adhesive and self-healable hydrogel materials have garnered significant attention in recent years due to their potential applications in various fields. These hydrogels can form reversible metal-ligand bonds, resulting in a network structure that can be easily broken and reformed, leading to self-healing capabilities. In addition, these hydrogels possess excellent mechanical strength and flexibility, making them suitable for strain-sensing applications. In this work, we have developed a mechanically robust, highly stretchable, self-healing, and adhesive hydrogel by incorporating Ca-dicarboxylate dynamic metal-ligand cross-links in combination with low density chemical cross-links into a poly(acrylamide--maleic acid) copolymer structure. Utilizing the reversible nature of the Ca-dicarboxylate bond, the hydrogel exhibited a tensile strength of up to ∼250 kPa and was able to stretch to 15-16 times its original length. The hydrogel exhibited a high fracture energy of ∼1500 J m, similar to that of cartilage. Furthermore, the hydrogel showed good recovery, fatigue resistance, and fast self-healing properties due to the reversible Ca-dicarboxylate cross-links. The presence of Ca resulted in a highly conductive hydrogel, which was utilized to design a flexible resistive strain sensor. This hydrogel can strongly adhere to different substrates, making it advantageous for applications in flexible electronic devices. When adhered to human body parts, the hydrogel can efficiently detect limb movements. The hydrogel also exhibited excellent performance as a solid electrolyte for flexible supercapacitors, with a capacitance of ∼260 F/g at 0.5 A/g current density. Due to its antifreezing and antidehydration properties, this hydrogel retains its flexibility at subzero temperatures for an extended period. Additionally, the porous network and high water content of the hydrogel impart remarkable electromagnetic attenuation properties, with a value of ∼38 dB in the 14.5-20.5 GHz frequency range, which is higher than any other hydrogel without conducting fillers. Overall, the hydrogel reported in this study exhibits diverse applications as a strain sensor, solid electrolyte for flexible supercapacitors, and efficient material for electromagnetic attenuation. Its multifunctional properties make it a promising candidate for use in various fields as a state-of-the-art material.