Highly viscoelastic, stretchable, conductive, and self-healing strain sensors based on cellulose nanofiber-reinforced polyacrylic acid hydrogel

Conductive and self-healing hydrogels are among the emerging materials that mimic the human skin and are important due to their probable prospects in soft robots and wearable electronics. However, the mechanical properties of the hydrogel matrix limit their applications. In this study, we developed a physicochemically dual cross-linked chemically modified-cellulose nanofibers-carbon nanotubes/polyacrylic acid (TOCNF-CNTs/PAA) hydrogel. The TOCNFs acted both as a nanofiller and dispersant to increase the mechanical strength of the PAA matrix and break the agglomerates of the CNTs. The final self-healing and conductive TOCNF-CNTs/PAA-0.7 (mass ratio of CNTs to AA) hydrogel with a uniform texture exhibited highly intrinsic stretchability (breaking elongation to ca. 850%), enhanced tensile properties (ca. 59 kPa), ideal conductivity (ca. 2.88 S m− 1) and pressure sensitivity. Besides, the composite hydrogels achieved up to approximately 98.36% and 99.99% self-healing efficiency for mechanical and electrical properties, respectively, without any external stimuli. Therefore, the as-designed multi-functional self-healing hydrogels, combined with stretching, sensitivity, and repeatability, possess the ability to monitor human activity and develop multifunctional, advanced, and commercial products such as wearable strain sensors, health monitors, and smart robots.