Mechanically Robust, Elastic, and Healable Ionogels for Highly Sensitive Ultra‐Durable Ionic Skins

The fabrication of highly durable skin-mimicking sensors remains challenging because of the unavoidable fatigue and physical damage that sensors are subjected to in practical applications. In this study, ultra-durable ionic skins (I-skins) with excellent healability and high sensitivity are fabricated by impregnating ionic liquids (ILs) into a mechanically robust poly(urea-urethane) (PU) network. The PU network is composed of crystallized poly(ε-caprolactone) and flexible poly(ethylene glycol) that are dynamically cross-linked with hindered urea bonds and hydrogen bonds. Such a design endows the resultant ionogels with high mechanical strength, good elasticity, Young's modulus similar to that of natural skin, and excellent healability. The ionogel-based I-skins exhibit a high sensitivity to a wide range of strains (0.1-300%) and pressures (0.1-20 kPa). Importantly, the I-skins show a highly reproducible electrical response over 10 000 uninterrupted strain cycles. The sensing performance of the I-skins stored in open air for 200 days is almost the same as that of the freshly prepared I-skin. The fractured I-skins can be easily healed by heating at 65 °C that restores their original ultra-durable sensing performance. The long-term durability of the I-skins is attributed to the combination of non-volatility of the ILs, excellent healability, and well-designed mechanical properties.