Advanced Carbon–Nickel Sulfide Hybrid Nanostructures: Extending the Limits of Battery-Type Electrodes for Redox-Based Supercapacitor Applications

[Image: see text] Transition-metal sulfides combined with conductive carbon nanostructures are considered promising electrode materials for redox-based supercapacitors due to their high specific capacity. However, the low rate capability of these electrodes, still considered “battery-type” electrodes, presents an obstacle for general use. In this work, we demonstrate a successful and fast fabrication process of metal sulfide–carbon nanostructures ideal for charge-storage electrodes with ultra-high capacity and outstanding rate capability. The novel hybrid binder-free electrode material consists of a vertically aligned carbon nanotube (VCN), terminated by a nanosized single-crystal metallic Ni grain; Ni is covered by a nickel nitride (Ni(3)N) interlayer and topped by trinickel disulfide (Ni(3)S(2), heazlewoodite). Thus, the electrode is formed by a Ni(3)S(2)/Ni(3)N/Ni@NVCN architecture with a unique broccoli-like morphology. Electrochemical measurements show that these hybrid binder-free electrodes exhibit one of the best electrochemical performances compared to the other reported Ni(3)S(2)-based electrodes, evidencing an ultra-high specific capacity (856.3 C g(–1) at 3 A g(–1)), outstanding rate capability (77.2% retention at 13 A g(–1)), and excellent cycling stability (83% retention after 4000 cycles at 13 A g(–1)). The remarkable electrochemical performance of the binder-free Ni(3)S(2)/Ni(3)N/Ni@NVCN electrodes is a significant step forward, improving rate capability and capacity for redox-based supercapacitor applications.