Self-Recovery, Fatigue-Resistant, and Multifunctional Sensor Assembled by a Nanocellulose/Carbon Nanotube Nanocomplex-Mediated Hydrogel

Flexible sensors have attracted great research interest due to their applications in artificial intelligence, wearable electronics, and personal health management. However, due to the inherent brittleness of common hydrogels, preparing a hydrogel-based sensor integrated with excellent flexibility, self-recovery, and antifatigue properties still remains a challenge to date. In this study, a type of physically and chemically dual-cross-linked conductive hydrogels based on 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofiber (TOCN)-carrying carbon nanotubes (CNTs) and polyacrylamide (PAAM) matrix via a facial one-pot free-radical polymerization is developed for multifunctional wearable sensing application. Inside the hierarchical gel network, TOCNs not only serve as the nanoreinforcement with a toughening effect but also efficiently assist the homogeneous distribution of CNTs in the hydrogel matrix. The optimized TOCN-CNT/PAAM hydrogel integrates high compressive (∼2.55 MPa at 60% strain) and tensile (∼0.15 MPa) strength, excellent intrinsic self-recovery property (recovery efficiency >92%), and antifatigue capacity under both cyclic stretching and pressing. The multifunctional sensors assembled by the hydrogel exhibit both high strain sensitivity (gauge factor ≈11.8 at 100-200% strain) and good pressure sensing ability over a large pressure range (0-140 kPa), which can effectively detect the subtle and large-scale human motions through repeatable and stable electrical signals even after 100 loading-unloading cycles. The comprehensive performance of the TOCN-CNT/PAAM hydrogel-based sensor is superior to those of most gel-based sensors previously reported, indicating its potential applications in multifunctional sensing devices for healthcare systems and human motion monitoring.