Ultrastretchable, Adhesive, Fast Self-Healable, and Three-Dimensional Printable Photoluminescent Ionic Skin Based on Hybrid Network Ionogels

Developing multifunctional stretchable ionic skin (I-Skin) to mimic the sensations of the human skin is of great interest and shows promising potential in wearable sensors and human–machine interfaces (HMIs). However, common ionogels prepared with small-molecule cross-linkers and single networks can hardly satisfy the requirements of adjustable mechanical properties, strong adhesion, fast self-healability, and good stability in extreme environments. Herein, an ultrastretchable (>10,000%), ultrastrong adhesive (>6.8 MPa), ultrafast self-healable (10 s), high thermally stable (−60 to 250 °C), and three-dimensional (3D)-printable photoluminescent ionogel with shape memory properties has been designed. The ionogel consists of hyperbranched polymer covalent-cross-linked poly­(zwitterionic ionic liquid)-co-poly­(acrylic acid) and multiple dynamic bonding cross-linked networks. The excellent performance of the ionogel-based high-stretchable strain sensor and the triboelectric nanogenerator (TENG)-based self-powered touch sensor is further demonstrated over a wide temperature range (−40 to 150 °C). More importantly, ionogel-based I-Skin can work as an HMI for human gesture recognition and real-time wireless control of robots under extreme vacuum conditions and can also self-heal immediately along with function recovery after mechanical damage.