3D Hierarchically Structured Tin Oxide and Iron Oxide-Embedded Carbon Nanofiber with Outermost Polypyrrole Layer for High-Performance Asymmetric Supercapacitor

Abstract

Herein, unique three-dimensional (3D) hierarchically structured carbon nanofiber (CNF)/metal oxide/conducting polymer composite materials were successfully synthesized by combinations of various experimental methods. Firstly, base CNFs were synthesized by carbonization of electrospun PAN/PVP fibers to attain electric double-layer capacitor (EDLC) characteristics. To further enhance the capacitance, tin oxide (SnO₂) and iron oxide (Fe₂O₃) were coated onto the CNFs via facile hydrothermal treatment. Finally, polypyrrole (PPy) was introduced as the outermost layer by a dispersion polymerization method under static condition to obtain 3D-structured CNF/SnO₂/PPy and CNF/Fe₂O₃/PPy materials. With each synthesis step, the morphology and dimension of materials were transformed, which also added the benign characteristic for supercapacitor application. For the practical application, as-synthesized CNF/SnO₂/PPy and CNF/Fe₂O₃/PPy were applied as active materials for supercapacitor electrodes, and superb specific capacitances of 508.1 and 426.8 F g^-1 (at 1 A g^-1) were obtained (three-electrode system). Furthermore, an asymmetric supercapacitor (ASC) device was assembled using CNF/SnO₂/PPy as the positive electrode and CNF/Fe₂O₃/PPy as the negative electrode. The resulting CNF/SnO₂/PPy//CNF/Fe₂O₃/PPy device exhibited excellent specific capacitance of 101.2 F g^-1 (at 1 A g^-1). Notably, the ASC device displayed a long-term cyclability (at 2000 cycles) with a retention rate of 81.1%, compared to a CNF/SnO₂//CNF/Fe₂O₃ device of 70.3% without an outermost PPy layer. By introducing the outermost PPy layer, metal oxide detachment from CNFs were prevented to facilitate long-term cyclability of electrodes. Accordingly, this study provides an effective method for manufacturing a high-performance and stable supercapacitor by utilizing unique 3D hierarchical materials, comprised of CNF, metal oxide, and conducting polymer.