Highly Stretchable, Fast Self-Healing, and Waterproof Fluorinated Copolymer Ionogels with Selectively Enriched Ionic Liquids for Human-Motion Detection

The development of waterproof ionogels with high stretchability and fast self-healing performance is essential for stretchable ionic conductors in sophisticated skin-inspired wearable sensors but can be rarely met in one material. Herein, a semicrystalline fluorinated copolymer ionogel (SFCI) with extremely high stretchability, underwater stability, and fast self-healability was fabricated, among which hydrophobic ionic liquids ([BMIM][TFSI]) were selectively enriched in fluoroacrylate segment domains of the fluorinated copolymer matrix through unique ion-dipole interactions. Benefiting from the reversible ion-dipole interactions between the [BMIM][TFSI] and fluoroacrylate segment domains as well as the physical cross-linking effects of semicrystalline oligoethylene glycol domains, the SFCI exhibited ultrastretchability (>6000%), fast room-temperature self-healability (>96% healing efficiency after cutting and self-healing for 30 min), and outstanding elasticity. In addition, the representative SFCI also exhibited high-temperature tolerance up to 300 °C, antifreezing performance as low as -35 °C, and high transparency (>93% visible-light transmittance). As a result, the as-obtained SFCI can readily be used as a highly stretchable ionic conductor in skin-inspired wearable sensors with waterproof performance for real-time detecting physiological human activities. These attractive features illustrate that the developed ultrastretchable and rapidly self-healable ionogels with unique waterproofness are promising candidates especially for sophisticated wearable strain sensing applications in complex and extreme environments.