Highly Adhesive, Stretchable, and Antifreezing Hydrogel with Excellent Mechanical Properties for Sensitive Motion Sensors and Temperature-/Humidity-Driven Actuators

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Abstract

Conductive hydrogels as flexible wearable devices have attracted considerable attention due to their mechanical flexibility and intelligent sensing. How to endow more and better performance, such as high self-adhesion, stretchability, and wide application temperature range for traditional hydrogels and flexible sensors is a challenge. Herein, a stretchable, self-adhesive, and antifreezing conductive hydrogel with multiple networks and excellent mechanical properties was prepared by a two-step method for its application in sensitive motion sensors and temperature-/humidity-driven actuators. First, quaternary chitosan (QCS) was introduced into the network of an acrylamide (AM) and 1-vinyl imidazole (VI) copolymer initiated by UV-photoinitiated radical polymerization. Then, the double-network hydrogel was immersed in a FeCl₃ solution to fabricate the P(AAm-co-VI)/QCS-Fe3+ ionic hydrogel with multiple physical networks. The properties of the hydrogel were controllable and adjustable. The toughness of the ionic hydrogel could reach up to 654.4 kJ/m3, the fracture strength could reach 253.1 kPa, and the compressive strength reached 8.4 MPa at an 80% compression strain. The multiple physical networks improved the mechanical properties and the quick resilience of the hydrogel. A large amount of FeCl₃ in the network greatly enhanced the ionic conductivity. Meanwhile, hydrogen bonds with water molecules inhibit the formation of ice crystals between zero water molecules and enhance the freezing resistance of P(Aam-co-VI)/QCS hydrogels. The active group on the QCS chain provided adhesiveness to various substrates for hydrogels. The P(AAm-co-VI)/QCS-Fe3+ hydrogel-based sensor showed high sensitivity, which can detect human movement and pulse, with a gauge factor of 2.37. Finally, due to the different dehydration rates of the P(AAm-co-VI)/QCS-Fe3+ and P(AAm-co-VI)/QCS hydrogel, a double-layer temperature/humidity-driven actuator was fabricated, expanding the application of conductive hydrogels.

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