Polymerization-Driven Self-Wrinkling on a Frozen Hydrogel Surface toward Ultra-Stretchable Polypyrrole-Based Supercapacitors

The construction of ultra-stretchable and smart supercapacitors with a large deformation-tolerance range and highly efficient self-healability is fully desired for next-generation wearable electronics. Herein, a sandwich-structured self-wrinkling hydrogel film (SSHF) is fabricated by freezing-constrained polymerization-driven self-wrinkling. Polypyrrole layers are first polymerized on a frozen pre-stretching hydrogel surface and subsequently self-wrinkled upon releasing the pre-strain. The SSHF with two polypyrrole electrode layers sandwiched with a hydrogel electrolytic layer is finally achieved by cutting four edges, and the all-in-one integrated structure creatively avoids the delamination between the electrodes and the electrolyte. The as-obtained SSHF can be directly used as an integrated all-in-one supercapacitor demonstrating high specific capacitance (79.5 F g–1 at 0.5 A g–1), large stretchability (>500%), and reliable room temperature self-healability. The freezing-constrained polymerization-driven self-wrinkling strategy might provide a unique self-wrinkling procedure to fabricate self-healable conducting polymer-based hydrogels for ultra-stretchable smart supercapacitors.