Self-Healing and Highly Stretchable Hydrogel for Interfacial Compatible Flexible Paper-Based Micro-Supercapacitor

Most reported wearable electronic devices lack self-healing chemistry and flexible function to maintain stable energy output while irreversible damages and complex deformations. In this work, we report a dual-dynamic network electrolyte synthesized by micellar elastomers introduced into strong hydrogel matrix. The gel electrolyte is fabricated by physically cross-linking the borax-polyvinyl alcohol (B-PVA) network as tough matrix and poly (ethylene oxide) (PEO)-poly (propylene oxide) (PPO)-poly (ethylene oxide) (Pluronic) to frame elastic network, followed by immersion in potassium chloride solution. Under the action of dynamic borate ester bond and multi-network hydrogen bond, the as-prepared electrolyte exhibits high stretchability (1535%) and good self-healing efficiency. Based on the electrolyte, we assemble the interfacial compatible micro-supercapacitor (MSC) by multi-walled carbon nanotubes (MWCNT) interdigital electrode printed on cellulosic paper by direct ink writing (DIW) technique. Thanks to the large specific area and compressive deformation resistance of cellulosic paper, the MSC with tightly interfacial contact achieves high volumetric capacitance of 801.9 mF cm(−3) at the current density of 20 μA cm(−2). In the absence of stimulation of the external environment, the self-healing MSC demonstrates an ideal capacity retention (90.43%) after five physical damaged/healing cycles. Our research provides a clean and effective strategy to construct wearable MSC.