Highly Transparent, Stretchable, and Conductive Supramolecular Ionogels Integrated with Three-Dimensional Printable, Adhesive, Healable, and Recyclable Character

In this work, we report the easy fabrication of highly transparent (optical transmittance above 93%), stretchable (1500–2500% elongation at break), and conductive (up to 2.25 S m–1 at 25 °C) supramolecular ionogels that simultaneously integrate with three-dimensional (3D) printable, healable, adhesive, and recyclable character. The supramolecular ionogel is designed using a linear amphiphilic poly(urethane-urea) (PUU) copolymer and ionic liquid (IL) as the elastic scaffold and electrolyte, respectively, via a simple cosolvent method. Intriguingly, the 3D-printed highly conductive (2.25 S m–1 at 25 °C) supramolecular ionogel structure shows record-high mechanical performance with a breaking tensile strain and stress of 945% and 1.51 MPa, respectively, and is able to lift 3400× or bear 10000× its weight without fracture. Furthermore, both the solution casting and 3D-printed ionogel films show high sensitivity and reliability for sensing a wide range of strains, including various human motions. The results present some new insights into the structural, mechanical, and functional design of novel multifunctional ionogels with distinguished mechanical performance and tractable processability, which will extend them to a wide range of flexible electronic applications, including artificial intelligence, wearable/conformable electronics, human/machine interactions, soft robotics, etc.