Tough, Healable, and Sensitive Strain Sensor Based on Multiphysically Cross-Linked Hydrogel for Ionic Skin

Ion conductive hydrogels (ICHs) have attracted great interest in the application of ionic skin because of their superior characteristics. However, it remains a challenge for ICHs to achieve balanced properties of high strength, large fracture strain, self-healing and freezing tolerance. In this study, a strong, stretchable, self-healing and antifreezing ICH was demonstrated by rationally designing a multiphysically cross-linked network structure consisting of the hydrophobic association, metal-ion coordination and chain entanglement among poly(acrylic acid) (PAA) polymer chains. The deliberately designed Brij S 100 acrylate (Brij-100A) micelle cross-linker can effectively dissipate energy and endow hydrogels with desirable stretchability. The self-healing ability of hydrogels originates from the reversible hydrophobic association in micelles and Fe³⁺-COO^- coordination. After the addition of NaCl, the chain-entangled physical network caused by the salting-out effect can both enhance mechanical strength and promote electron transport. With the synergy of hydrophobic association, mental-ligand coordination and chain entanglement, the PAA/Brij-100A/Fe³⁺/NaCl (PAA/BA/Fe³⁺/NaCl) hydrogels exhibited a high tensile strain of 1140%, a tensile strength of 0.93 MPa and a toughness of 3.48 MJ m^-3. Besides, the PAA/BA/Fe³⁺/NaCl hydrogels exhibited a high conductivity of 0.43 S m^-1 and good freezing resistance. The ionic skin based on the PAA/BA/Fe³⁺/NaCl hydrogels showed high sensitivity (GF = 5.29), wide strain range (0-950%), fast response time (220 ms) and good stability. Also, the self-healing ability of the ionic skin can significantly prolong its service time, and the antifreezing property can broaden its applicable temperature. This study offers new insight into the design of multifunctional ionic skin for wearable electronics.