Solution-Processable Conductive Composite Hydrogels with Multiple Synergetic Networks toward Wearable Pressure/Strain Sensors

A biocompatible, flexible, yet robust conductive composite hydrogel (CCH) for wearable pressure/strain sensors has been achieved by an all-solution-based approach. The CCH is rationally constructed by in situ polymerization of aniline (An) monomers in the polyvinyl alcohol (PVA) matrix, followed by the cross-linking of PVA with glutaraldehyde (GA) as the cross-linker. The unique multiple synergetic networks in the CCH including strong chemical covalent bonds and abundance of weak physical cross-links, i.e., hydrogen bondings and electrostatic interactions, impart excellent mechanical strength (a fracture tensile strength of 1200 kPa), superior compressibility (ε = 80%@400 kPa), outstanding stretchability (a fracture strain of 670%), high sensitivity (0.62 kPa^–1 at a pressure range of 0–1.0 kPa for pressure sensing and a gauge factor of 3.4 at a strain range of 0–300% for strain sensing, respectively), and prominent fatigue resistance (1500 cycling). As the flexible wearable sensor, the CCH is able to monitor different types of human motion and diagnostically distinguish speaking. As a proof of concept, a sensing device has been designed for the real-time detection of 2D distribution of weight or pressure, suggesting its promising potentials for electronic skin, human–machine interaction, and soft robot applications.