Hydrogels are important for stretchable and wearable multifunctional sensors, but their application is limited by their low mechanical strength and poor long-term stability. Herein, a conductive organohydrogel with a 3D honeycomb structure was prepared by integrating carbon nanotubes (CNTs) and carbon black (CB) into a poly(vinyl alcohol)/glycerol (PVA/Gly) organohydrogel. Such a nanocomposite organohydrogel is built on a physical cross-linking network formed by the hydrogen bonds among PVA, glycerol, and water. CNTs and CB had an add-in synergistic impact on the mechanical and electrical performances of the PVA/Gly organohydrogel because of the distinct aspect ratios and geometric shapes. The prepared organohydrogel integrated with a tensile strength of 4.8 MPa, a toughness of 15.93 MJ m-3, and flexibility with an elongation at break up to 640%. The organohydrogels also showed good antifreezing feature, long-term moisture retention, self-healing, and thermoplasticity. Sensors designed from these organohydrogels displayed high stretching sensitivity to tensile strain and temperature, with a gauge factor of 2.1 within a relatively broad strain range (up to ∼600% strain), a temperature coefficient of resistance of -0.935%·°C-1, and long-term durability. The sensors could detect full-range human physiological signals and respond to the change in temperature, which are highly desired for multifunctional wearable electronic devices.
Keywords: antifreezing; hydrogel electrolyte; sensor; thermoplasticity; toughness.