Self-healing, piezoresistive and temperature responsive behaviour of chitosan/polyacrylic acid dynamic hydrogels

Flexible electronics have introduced new challenges for efficient human-machine interactions. Hydrogels have emerged as prominent materials for electronic wearable applications due to their exceptional mechanical deformability and lightweight characteristics combined in some cases with conductive properties, and softness. Additionally, bio-interphases require multisensory response to stress, strain, temperature, and self-healing capacity. To mimic these properties, this work developed interpenetrated hydrogel networks composed of chitosan (CHI) and polyacrylic acid (PAA), combined with Fe (III) ions and varying amounts of NMBA (0-0.25 %), to achieve tailored conductivity (0.8-2.5 mS/cm), self-healing, self-standing and mechanical properties (E = 11.7-110 Pa and fracture strain = 64.9-1923 %) suitable for strain sensor applications. The results revealed a significant influence of the restrictive effect on the mobility of uncrosslinked chain segments, caused by Fe ions and NMBA, on the piezoresistance (GF 2.1-1.3) and self-healing capability of the gels. Interestingly, a transparent/turbid transition, driven by microphase separation that is characteristic of systems with high dynamic interactions, was encountered for the first time in these hydrogels. This transition was analyzed in relation to external temperature, water content, pH, and the influence of Fe ions and NMBA. The simultaneous sensitivity of these materials to temperature and pH, along with their piezoresistive and self-healing behaviour, can be highly valuable for multifunctional sensors in a wide range of applications.