High-Performance Stretchable Supercapacitors Based on Centrifugal Electrospinning-Directed Hetero-structured Graphene–Polyaniline Hierarchical Fabric

Stretchable supercapacitors (S-SCs) are of considerable interest as prospective energy-storage devices for wearable electronics and smart products. However, achieving high energy density and stable output under large deformations remains an urgent challenge. Here, we develop a high-performance S-SC based on a robust heterostructured graphene–polyaniline (G-PANI) anchored hierarchical fabric (G-PANI@pcPU). By precisely manipulating centrifugal electrospinning and PANI-induced two-step self-assembly process, the G-PANI@pcPU features an inter-linkage porous backbone, which open ions migration/intercalation pathways, high mechanical flexibility (elongation: 400%), and large production area (> 90 cm 2 ). The resultant G-PANI@pcPU presents ultra-large specific areal capacitance ( C areal ) of 5093.7 mF cm −2 (about 35 mg cm −2 mass loading of G-PANI) and redox reversibility in 1 M H 2 SO 4 electrolyte. Additionally, the G-PANI@pcPU fabric-based solid-state S-SCs show a high energy density of 69.2 μWh cm −2 and capacitance of 3113.7 mF cm −2 . More importantly, the superior stretchable stability (84.1% capacitance retentions after 5000 cycles) and foldable performance (86.7% capacitance retentions after 5000 cycles) of S-SCs are impressively achieved. Finally, the S-SCs realize potential applications of steady powering light-emitting diode (LED) lights at 100% strain, smart watch at bending deformation, toy car, and lamp. This work can offer an overwhelming foundation for designing advanced flexible electrodes toward new energy and smart wearable applications. Graphical Abstract