High-Strength, Self-Adhesive, and Strain-Sensitive Chitosan/Poly(acrylic acid) Double-Network Nanocomposite Hydrogels Fabricated by Salt-Soaking Strategy for Flexible Sensors

As a promising functional material, hydrogels have attracted extensive attention, especially in flexible wearable sensor fields, but it remains a great challenge to facilely integrate excellent mechanical properties, self-adhesion, and strain sensitivity into a single hydrogel. In this work, we present high in strength, stretchable, conformable, and self-adhesive chitosan/poly(acrylic acid) double-network nanocomposite hydrogels for application in epidermal strain sensor via in situ polymerization of acrylic acid in chitosan acid aqueous solution with tannic acid-coated cellulose nanocrystal (TA@CNC) acting as nanofillers to reinforce tensile properties, followed by a soaking process in a saturated NaCl solution to cross-link chitosan chains. With addition of a small amount of TA@CNC, the double-network nanocomposite hydrogels became highly adhesive and mechanically compliant, which were critical factors for the development of conformable and resilient wearable epidermal sensors. The salt-soaking process was applied to cross-link chitosan chains by shielded electrostatic repulsions between positively charged amino groups, drastically enhancing the mechanical properties of the hydrogels. The obtained double-network nanocomposite hydrogels exhibited excellent tunable mechanical properties that could be conveniently tailored with fracture stress and fracture strain ranging from 0.39 to 1.2 MPa and 370 to 800%, respectively. Besides, the hydrogels could be tightly attached onto diverse substrates, including wood, glass, plastic, polytetrafluoroethylene, glass, metal, and skin, demonstrating high adhesion strength and compliant adhesion behavior. In addition, benefiting from the abundant free ions from strong electrolytes, the flexible hydrogel sensors demonstrated stable conductivity and strain sensitivity, which could monitor both large human motions and subtle motions. Furthermore, the antibacterial property originating from chitosan made the hydrogels suitable for wearable epidermal sensors. The facile soaking strategy proposed in this work would be promising in fabricating high-strength multifunctional conductive hydrogels used for wearable epidermal devices.