Mussel-inspired self-adhesive hydrogels by conducting free radical polymerization in both aqueous phase and micelle phase and their applications in flexible sensors

Polydopamine (PDA)-based self-adhesive hydrogel sensors are extensively explored but it is still a challenge to construct PDA-based hydrogels by free radical polymerization. Herein, a new approach to construct self-adhesive hydrogels by conducting free radical polymerization in both aqueous phase and micelle phase is developed. The following two-phase polymerization processes account for the formation of the self-adhesive hydrogels. The first one is the polymerization of acrylamide (AM) and dopamine (DA) in aqueous phase to form adhesive component PAM-PDA (PAM, polyacrylamide; PDA, polydopamine). The second one is the polymerization of hydrophobic monomer 2-methoxyethyl acrylate (MEA) in micelles of an amphiphilic block copolymer Pluronic F127 diacrylate (F127DA). The poly(2-methoxyethyl acrylate) (PMEA) networks help to maintain the high robustness of the hydrogel. Because PMEA and PDA form in relatively separated phases, the inhibition effect of PDA on the free radical polymerization process of PMEA is weakened. Based on this mechanism, mechanically strong and adhesive hydrogels are achieved. The introduced ions during preparation process, such as Na⁺, OH^- and K⁺, endow the resulting hydrogels ionic conductivity. Resistive strain sensor of the hydrogel achieves a high gauge factor (GF) of 5.26, a response time of 0.25 s and high sensing stability. Because of the adhesiveness, such hydrogel sensor can be applied as wearable sensors in monitoring various human motions. To further address the freezing and drying problems of the hydrogels, organohydrogels are constructed in glycerol-water mixed solvent. The organohydrogels exhibit outstanding anti-freezing property and moisture retention ability, and their adhesiveness is well maintained in subzero conditions. Capacitive pressure sensors of the organohydrogels possessing a GF of 2.05 kPa^-1, high sensing stability and reversibility, are demonstrated and explored in monitoring diverse human motions.