Tough, Resilient, Adhesive, and Anti-Freezing Hydrogels Cross-Linked with a Macromolecular Cross-Linker for Wearable Strain Sensors

Ideal conductive hydrogels for flexible, wearable strain sensors should be tough, highly resilient, adhesive, and anti-freezing. However, such hydrogels are difficult to design. Herein, a multifunctional macromolecular cross-linker (MC) based on poly­(hydroxyethyl-l-glutamine) was designed and used to synthesize the hydrogels. Cross-linking with the MC leads to a reduced inhomogeneity of the gel network. Therefore, the mechanical properties of the gels are significantly improved compared with the ordinary hydrogels cross-linked with the conventional cross-linker N,N-methylenebisacrylamide (BIS). The MC-cross-linked gels also exhibit high resilience. At the same time, replacing BIS with MC significantly improves the adhesive properties of the gel, which is attributed to the introduction of a large amount of adhesive groups with the MC. The gels can stick to various substrates including skin. The good tissue adhesiveness of the gel allows it to stick to skin by itself without using any straps or adhesive tapes when used as a flexible wearable strain sensor. Both large and subtle human movements were successfully monitored using the sensor. The signals are highly stable and reliable, thanks to the high resilience of the gel. The introduction of the polar groups also improved dramatically the anti-freezing properties of the gels. Even at −20 °C, the gels still remained highly flexible and stretchable, therefore allowing the gel-based sensor to work at sub-zero temperatures. The excellent toughness, resilience, tissue-adhesiveness, and anti-freezing properties of the gel make it a good choice for a flexible wearable sensor.