Flexible Strain-Sensitive Sensors Assembled from Mussel-inspired Hydrogel with Tunable Mechanical Properties and Wide Temperature Tolerance in Multiple Application Scenarios

Conductive hydrogels, exhibiting wide applications in electronic skins and soft wearable sensors, often require maturely regulating of the hydrogel mechanical properties to meet specific demands and work for a long-term or under extreme environment. However, in situ regulation of the mechanical properties of hydrogels is still a challenge, and regular conductive hydrogels will inevitably freeze at subzero temperature and easily dehydrate, which leads to a short service life. Herein, a novel adhesive hydrogel (PAA-Dopa-Zr⁴⁺) capable of strain sensing is proposed with antifreezing, nondrying, strong surface adhesion, and tunable mechanical properties. 3,4-Dihydroxy­phenyl-l-alanine (l-Dopa)-grafted poly­(acrylic acid) (PAA) and Zr⁴⁺ ion are introduced into the hydrogel, which broadly alters the mechanical properties via tuning the in situ aggregation state of polymer chains by ions based on the complexation effect. The catechol groups of l-Dopa and viscous glucose endow the hydrogel with high adhesiveness for skin and device interface (including humid and dry environments) and exhibit an outstanding temperature tolerance under extreme wide temperature spectrum (−35 to 65 °C) or long-lasting moisture retention (60 days). Furthermore, this PAA-Dopa-Zr⁴⁺ can be assembled as a flexible strain-sensitive sensor to detect human motions based on specific mechanical properties requirements. This work, enabling superior adhesive and temperature tolerance performance and broad mechanical tenability, presents a new paradigm for numerous applications to wearable sensing and personalized healthcare monitoring.