Facile Preparation of Polymerizable Deep Eutectic Solvents Under Mild Conditions for Multisensory Ionic Skins

Abstract Polymerizable deep eutectic solvents (PDESs) have emerged as promising building blocks for next‐generation eutectic gels, offering new opportunities for the development of advanced electronic devices. Traditional PDES fabrication typically involves heating and extended processing time. In this study, a facile method where a solid‐solid mixture of lithium bis(trifluoromethane) sulfonimide (LiTFSI) and acrylamide (AAm) rapidly forms a PDES at room temperature, significantly simplifying the ionogel preparation is presented. By combining this PDES with another system, comprising 3‐[dimethyl‐[2‐(2‐methylprop‐2‐enoyloxy)ethyl]azaniumyl]propane‐1‐sulfonate (SBMA) and ethylene glycol (EG), an eutectic gel is successfully fabricated with exceptional mechanical and conductive properties. This gel exhibits a fracture stress of 0.8 MPa, fracture energy of 3.7 kJ m −2 , adhesion strength of 60 kPa, transmittance over 90%, high conductivity (0.113 S m −1 ), and an outstanding temperature tolerance ranged from ‐50 to 50 °C. Notably, the absence of chemical crosslinkers and the presence of reversible interactions such as hydrogen bonding and ion‐dipole electrostatic forces impart excellent self‐healing capabilities. These combined features position the gel a promising candidate for multisensory ionic skins, capable of detecting pressure, temperature, humidity, and sweat. This work pioneers the rapid, mild‐condition synthesis of PDESs, paving the way for new techniques in ionic skin development.