Tannic Acid-Silver Dual Catalysis Induced Rapid Polymerization of Conductive Hydrogel Sensors with Excellent Stretchability, Self-Adhesion, and Strain-Sensitivity Properties

The application of conductive hydrogels in intelligent biomimetic electronics is a hot topic in recent years, but it is still a great challenge to develop the conductive hydrogels through a rapid fabrication process at ambient temperature. In this work, a versatile poly(acrylamide) @cellulose nanocrystal/tannic acid-silver nanocomposite (NC) hydrogel integrated with excellent stretchability, repeatable self-adhesion, high strain sensitivity, and antibacterial property, was synthesized via radical polymerization within 30 s at ambient temperature. Notably, this rapid polymerization was realized through a tannic acid-silver (TA-Ag) mediated dynamic catalysis system that was capable of activating ammonium persulfate and then initiated the free-radical polymerization of the acrylamide monomer. Benefiting from the incorporation of TA-Ag metal ion nanocomplexes and cellulose nanocrystals, which acted as dynamic connecting bridges by hydrogen bonds to efficiently dissipate energy, the obtained NC hydrogels exhibited prominent tensile strain (up to 4000%), flexibility, self-recovery, and antifatigue properties. In addition, the hydrogels showed repeatable adhesiveness to different substrates (e.g., glass, wood, bone, metal, and skin) and significant antibacterial properties, which were merits for the hydrogels to be assembled into a flexible epidermal sensor for long-term human-machine interfacial contact without concerns about the use of external adhesive tapes and bacterial breeding. Moreover, the remarkable conductivity (σ ∼ 5.6 ms cm^-1) and strain sensitivity (gauge factor = 1.02) allowed the flexible epidermal sensors to monitor various human motions in real time, including huge movement of deformations (e.g., wrist, elbow, neck, shoulder) and subtle motions. It is envisioned that this work would provide a promising strategy for the rapid preparation of conductive hydrogels in the application of flexible electronic skin, biomedical devices, and soft robotics.