Nanocellulose-enhanced organohydrogel with high-strength, conductivity, and anti-freezing properties for wearable strain sensors

The use of ion-conductive hydrogels in strain sensors with high mechanical properties, conductivity, and anti-freezing properties is challenging. Here, high-strength, transparent, conductive, and anti-freezing organohydrogels were fabricated through the radical polymerization of polyacrylamide (PAM)/sodium alginate (SA)/TEMPO-oxidized cellulose nanofibrils (TOCNs) in a dimethyl sulfoxide (DMSO)/water solution, followed by soaking in a CaCl2 solution. The resulting organohydrogels demonstrated a high strength (tensile strength of 1.04 MPa), stretchability (681%), transparency (>84% transmittance), and ionic conductivity (1.25 S m-1). The organohydrogel-based strain sensor showed a high strain sensitivity (GF = 2.1). In addition, due to a synergistic effect between the DMSO/H2O binary solvent and CaCl2, the organohydrogel remained flexible (could bend 180°) and conductive (1.01 S m-1) at -20 °C. Interestingly, the TOCNs exerted a reinforcing effect on both the mechanical properties and ionic conductivity. This research provides a novel strategy to prepare ion-conductive organohydrogels with good mechanical properties, conductivity, and anti-freezing properties for use as flexible electronic materials.