“Casein micelle -nanoparticle double cross-linking” triggered stable adhesive, tough CA/MWCNT/PAAm hydrogel wearable strain sensors, for human motion monitoring

Flexible hydrogels have emerged as highly-desirable materials for wearable strain sensors. However, pristine biomass hydrogel systems are limited by their lack of stretchability, self-adhesion, and sensitivity. Here, a novel CA/MWCNT/PAAm double-network conductive hydrogel was developed through integrating casein (CA) micelles and multi-walled carbon nanotubes (MWCNT) into the polyacrylamide (PAAm) network. The resulting hydrogel displayed desired properties such as adhesiveness, toughness, self-healing, and near-infrared photothermal response. In this hybrid system, MWCNT were uniformly dispersed in the presence of casein micelles through hydrogen bonding and electrostatic interactions, favoring its role of nano reinforcement. Moreover, based on the "casein micelle-nanoparticle double cross-linking" mechanism and its double network structure, the prepared hydrogel showed high extensibility (2288 % ± 63 %), fast responsiveness (273 ± 5.13 ms), high sensitivity (GF = 12.46 ± 0.35), and a wide strain range (1-1000 %). Through consistent and repeated electrical inputs, this hydrogel was able to detect including large and small human movements, such as hand, leg, and swallowing motions. The results from this study provide a new way to fabricate bio-based hydrogel sensors with excellent mechanical and electrical properties.