Hierarchical Nanocages Assembled by NiCo-Layered Double Hydroxide Nanosheets for a High-Performance Hybrid Supercapacitor

Layered double hydroxides (LDHs) have attracted broad attention as cathode materials for hybrid supercapacitors (HSCs) because of their ultrahigh theoretical specific capacitance, high compositional flexibility, and adjustable interlayer spacing. However, as reported, specific capacitance of LDHs is still far below the theoretical value, inspiring countless efforts to these ongoing challenges. Herein, a hierarchical nanocage structure assembled by NiCo-LDH nanosheet arrays was rationally designed and fabricated via a facile solvothermal method assisted by the ZIF-67 template. The transformation from the ZIF-67 template to this hollow structure is achieved by a synergistic effect involving the Kirkendall effect and the Ostwald ripening process. The enlarged specific surface area co-occurred with broadened interlayer spacing of LDH nanosheets by finely increasing the Ni concentration, leading to synchronous improvement of electron/ion transfer kinetics. The optimized NiCo-LDH-210 electrode displays a maximum specific capacitance of 2203.6 F g^-1 at 2 A g^-1, excellent rate capability, and satisfactory cycling stability because of the highly exposed active sites and shortened ion transport paths provided by vertically aligned LDH nanosheets together with the cavity. Furthermore, the assembled HSC device achieves a superior energy density of 57.3 Wh kg^-1 with prominent cycling stability. Impressively, the design concept of complex construction derived from metal-organic frameworks (MOF) derivatives shows tremendous potential for use in energy storage systems.