High-performance supercapacitors based on coarse nanofiber bundle and ordered network hydrogels

Most of the developed flexible hydrogel supercapacitors struggle to maintain their electrochemical stability and structural integrity under tensile strain. Therefore, developing a flexible supercapacitor with excellent mechanical properties and stable electrochemical performance under different strains remains a challenge. Based on the previous cartilage-like structure, we designed a new coarse nanofiber bundle and ordered network. A coarse nanofiber bundle and ordered network skeleton was constructed by directional freezing and filled with polyvinyl alcohol (PVA) to serve as a soft matrix to prepare PVA-SNF-CNTs-PPy-3 hydrogel electrode, which has high tensile strength (6.22 MPa) and fatigue threshold (8759.8 J/m²). In addition, the loading of carbon nanotubes and polypyrrole onto the SNF-ordered network enabled the conductive material to form an ordered conductive energy storage network along the skeleton, providing an area-specific capacitance of up to 23.96 F/cm². The coarse nanofiber bundle and ordered network provided supercapacitors with the least capacitance consumption under 150 % deformation, and the capacitance retention was >98.2 %. After repeated stretching (3000 times), the capacitance remained >91.45 %. This study provides new ideas for the development of flexible supercapacitors with high capacitance and high mechanical reliability.