Strong, tough, anti-freezing, non-drying and sensitive ionic sensor based on fully physical cross-linked double network hydrogel

Abstract Ionic conductive double network (DN) sensors have attracted increasing attention in wearable electronic devices. However, their low mechanical and sensing properties as well as poor moisture retention and freezing resistance restrict severely their applications. Herein, we synthesized a fully physical cross-linked poly (N-hydroxymethyl acrylamide)/agar/ethylene glycol (PHA/Agar/EG) ionic conductive DN hydrogel exhibiting high strength and toughness, fast self-recovery, good fatigue resistance and good self-healing. Agar could form a physical network via reversible sol-gel transition, and interact with physical cross-linked poly (N-hydroxymethyl acrylamide) and sodium chloride (NaCl) via hydrogen bonds and salting-out effect, respectively. Meanwhile, ethylene glycol and NaCl improved the mechanical properties, long-lasting moisture retention and anti-freezing ability. The PHA/Agar/EG gel-based flexible sensor possessed excellent long-lasting and fatigue resistant sensing properties, and could monitor various human activities stably and sensitively. Therefore, this work would provide a simple and promising strategy to fabricate flexible sensors with integrated high performances for smart wearable devices.