Abstract
Stretchable ionic skins are intriguing in mimicking the versatile sensations of natural skins. However, for their applications in advanced electronics, good elastic recovery, self-healing, and more importantly, skin-like nonlinear mechanoresponse (strain-stiffening) are essential but can be rarely met in one material. Here we demonstrate a robust proton-conductive ionic skin design via introducing an entropy-driven supramolecular zwitterionic reorganizable network to the hydrogen-bonded polycarboxylic acid network. The design allows two dynamic networks with distinct interacting strength to sequentially debond with stretch, and the conflict among elasticity, self-healing, and strain-stiffening can be thus defeated. The representative polyacrylic acid/betaine elastomer exhibits high stretchability (1600% elongation), immense strain-stiffening (24-fold modulus enhancement), ~100% self-healing, excellent elasticity (97.9 ± 1.1% recovery ratio, <14% hysteresis), high transparency (99.7 ± 0.1%), moisture-preserving, anti-freezing (elastic at -40 °C), water reprocessibility, as well as easy-to-peel adhesion. The combined advantages make the present ionic elastomer very promising in wearable iontronic sensors for human-machine interfacing.