Fully Polymeric Conductive Hydrogels with Low Hysteresis and High Toughness as Multi‐Responsive and Self‐Powered Wearable Sensors

Abstract High mechanical strength, excellent toughness, low hysteresis, and robust resilience are of great importance for stretchable conductive hydrogels (CHs) to heighten their reliabilities for self‐powered sensing applications. However, it still remains challenging to simultaneously obtain the mutually exclusive performances. Herein, an intrinsically conductive and adhesive hydrogel is fabricated by one‐step radical polymerization of acrylamide (AAm), three hydroxy groups together clustered‐N‐[tris(hydroxymethyl)methyl]acrylamide (THMA), and cationic 1‐Butyl‐3‐Vinylimidazolium Bromide (ILs) dissolved in core‐shell structurally dispersed PEDOT:PSS (PP) solution. Owing to abundant clustered hydrogen bonds, electrostatic interactions between PILs chains and anionic PSS shells, and polymer chain entanglements, the CHs feature superior mechanical properties with a high tensile strength (0.25 MPa), fracture strain (1015%), fracture toughness (1.22 MJ m ‐3 ), fracture energy of 36.5 kJ m ‐2 and extremely low hysteresis (5%), and display excellent resilience and fatigue resistance. As a result, the CHs indicate excellent sensing properties with a gauge factor up to 10.46, a broad sensing range of strain (1‐900%) and pressure (0.05‐100 kPa), and fast responsive rate, thus qualifying for monitoring reliably and accurately large and tiny human movements in daily life. Moreover, the hydrogel‐assembled triboelectric nanogenerators (TENGs) exhibit excellent and stable electrical output performances, which are greatly promising in self‐powered flexible wearable electronics.