Strong, conductive, and freezing-tolerant polyacrylamide/PEDOT:PSS/cellulose nanofibrils hydrogels for wearable strain sensors

Hydrogels with prominent flexibility, versatility, and high sensitivity play an important role in the design and fabrication of wearable sensors. In particular, these flexible conductive hydrogels exhibit elastic modulus that is highly compatible with human skin, demonstrating the great potential for flexible sensing. However, the preparation of high-performance hydrogel-based sensors that can restrain extreme cold conditions is still challenging. Herein, a novel anti-freezing composite hydrogel with superior conductivity based on polyacrylamide (PAM), LiCl, and PEDOT:PSS coated cellulose nanofibrils (PAM/PEDOT:PSS/CNF) is constructed. The addition of CNF increased the hydrogen bonding sites of the molecular chains in the micro, thus improving the mechanical strength and the conductivity of the hydrogel in the macro. The hydrogels achieve a high tensile strength of 0.19 MPa, compressive strength of 0.92 MPa, and dissipation energy of 41.9 kJ/m3. Otherwise, LiCl increases the interactions between the colloidal phase and water molecules, endowing the hydrogels with excellent freezing tolerance. Specifically, the optimized hydrogel of 45 % LiCl exhibited stable mechanical properties at -40 °C. Finally, the composite hydrogel was used to assemble flexible sensors with high sensitivity of 10.3 MPa-1, which can detect a wide range of human movements and physiological activities.