A Skin-Inspired Stretchable, Self-Healing and Electro-Conductive Hydrogel with a Synergistic Triple Network for Wearable Strain Sensors Applied in Human-Motion Detection

Hydrogel-based strain sensors inspired by nature have attracted tremendous attention for their promising applications in advanced wearable electronics. Nevertheless, achieving a skin-like stretchable conductive hydrogel with synergistic characteristics, such as ideal stretchability, excellent sensing performance and high self-healing efficiency, remains challenging. Herein, a highly stretchable, self-healing and electro-conductive hydrogel with a hierarchically triple-network structure was developed through a facile two-step preparation process. Firstly, 2, 2, 6, 6-tetrametylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibrils were homogeneously dispersed into polyacrylic acid hydrogel, with the presence of ferric ions as an ionic crosslinker to synthesize TEMPO-oxidized cellulose nanofibrils/polyacrylic acid hydrogel via a one-pot free radical polymerization. A polypyrrole conductive network was then incorporated into the synthetic hydrogel matrix as the third-level gel network by polymerizing pyrrole monomers. The hierarchical 3D network was mutually interlocked through hydrogen bonds, ionic coordination interactions and physical entanglements of polymer chains to achieve the target composite hydrogels with a homogeneous texture, enhanced mechanical stretchability (elongation at break of 890%), high viscoelasticity (maximum storage modulus of 27.1 kPa), intrinsic self-healing ability (electrical and mechanical healing efficiencies of 99.4% and 98.3%) and ideal electro-conductibility (3.9 S m(-1)). The strain sensor assembled by the hybrid hydrogel, with a desired gauge factor of 7.3, exhibits a sensitive, fast and stable current response for monitoring small/large-scale human movements in real-time, demonstrating promising applications in damage-free wearable electronics.