Design of an Internal/External Bicontinuous Conductive Network for High-Performance Asymmetrical Supercapacitors

High-energy density supercapacitors have attracted extensive attention due to their electrode structure design. A synergistic effect related to core–shell structure can improve the energy storage capacity and power density of electrode materials. The Ni-foam (NF) substrate coupled with polypyrrole (PPy) conductive coating can serve as an internal/external bicontinuous conductive network. In this work, the distinctive PPy@FeNi₂S₄@NF and PPy@NiCo₂S₄@NF materials were prepared by a simple two-step hydrothermal synthesis with a subsequent in situ polymerization method. PPy@FeNi₂S₄@NF and PPy@NiCo₂S₄@NF could deliver ultrahigh specific capacitances of 3870.3 and 5771.4 F·g⁻¹ at 1 A·g⁻¹ and marvelous cycling capability performances of 81.39% and 93.02% after 5000 cycles. The asymmetric supercapacitors composed of the prepared materials provided a high-energy density of over 47.2 Wh·kg⁻¹ at 699.9 W·kg⁻¹ power density and 67.11 Wh·kg⁻¹ at 800 W·kg⁻¹ power density. Therefore, the self-assembled core–shell structure can effectively improve the electrochemical performance and will have an effective service in advanced energy-storage devices.