Resilient and Self-Healing Hyaluronic Acid/Chitosan Hydrogel With Ion Conductivity, Low Water Loss, and Freeze-Tolerance for Flexible and Wearable Strain Sensor

Conductive hydrogel is a vital candidate for the fabrication of flexible and wearable electric sensors due to its good designability and biocompatibility. These well-designed conductive hydrogel–based flexible strain sensors show great potential in human motion monitoring, artificial skin, brain computer interface (BCI), and so on. However, easy drying and freezing of conductive hydrogels with high water content greatly limited their further application. Herein, we proposed a natural polymer-based conductive hydrogel with excellent mechanical property, low water loss, and freeze-tolerance. The main hydrogel network was formed by the Schiff base reaction between the hydrazide-grafted hyaluronic acid and the oxidized chitosan, and the added KCl worked as the conductive filler. The reversible crosslinking in the prepared hydrogel resulted in its resilience and self-healing feature. At the same time, the synthetic effect of KCl and glycerol endowed our hydrogel with outstanding anti-freezing property, while glycerol also endowed this hydrogel with anti-drying property. When this hydrogel was assembled as a flexible strain sensor, it showed good sensitivity (GF = 2.64), durability, and stability even under cold condition (−37°C).