Hierarchically Structured Porous Electro-Conductive Aerogels for All-Solid-State Flexible Planar Supercapacitors with Cyclic Stability

Flexible supercapacitors have attracted significant attention as promising power sources for portable and wearable electronic devices. However, achieving simultaneous high power density, energy density and long-term cyclic stability in a simple device configuration remains a critical challenge. Herein, we report an all-solid-state flexible planar supercapacitor based on hierarchically structured cellulose nanofiber-carbon nanotube@manganese dioxide (CNF-CNT@MnO2) composite aerogels. The electrode architecture is rationally designed by first dispersing CNTs within a hydrophilic CNF scaffold to form a conductive three-dimensional network, followed by in situ oxidative polymerization of MnO2 onto the CNF-CNT fibrous skeleton. The hydrophilic CNFs network ensures thorough electrolyte penetration, the interconnected CNTs facilitate rapid electron transport, and the uniformly coated MnO2 layer provides substantial pseudocapacitance. The aerogel electrode with a low density of 14.6 mg cm−3 and a high specific surface area of 214.4 m2 g−1 delivers a specific capacitance of 273.0 F g−1 at 0.4 A g−1. The assembled planar supercapacitor, incorporating gel electrolyte and a flexible hydrogel substrate, achieves an impressive areal capacitance of 885.0 mF cm−2 at 2 mA cm−2, energy density of 122.9 μWh cm−2 and corresponding power density of 1000.0 μW cm−2. The device exhibits excellent electrochemical stability, retaining 83.3% capacitance after 2500 charge–discharge cycles, and outstanding mechanical flexibility, with 96.3% capacitance retention after 200 repeated bending cycles. Furthermore, multiple devices can be connected in series or parallel to proportionally increase output voltage or current, meeting the practical power requirements of electronic applications. This work offers a viable pathway toward high-performance, durable energy storage solutions for next-generation wearable electronics.