Controlled Synthesis of Flower-like Hierarchical NiCo-Layered Double Hydroxide Integrated with Metal–Organic Framework-Derived Co@C for Supercapacitors

Layered double hydroxides (LDHs) have come to the foreground recently, considering their unique layered structure and short ion channels when they act as electrode materials for supercapacitors (SCs). However, due to their poor rate and cycle performance, they are not highly sought after in the market. Therefore, a flower-like hierarchical NiCo-LDH@C nanostructure with flake NiCo-LDH anchored on the carbon skeleton has emerged here, which is constructed by calcination and hydrothermal reaction and applying flake ZIF-67 as a precursor. In this structure, NiCo-LDH grows outward with abundant and homogeneously distributed Co nanoparticles on Co@C as nucleation sites, forming a hierarchical structure that is combined tightly with the carbon skeleton. The flower-like hierarchical nanostructures formed by the composite of metal-organic frameworks (MOFs) and LDHs have successfully enhanced the cycle and rate performance of LDH materials on the strength of strong structural stability, large specific surface area, and unique cooperative effect. The NiCo-LDH@C electrode displays superb electrochemical performance, with a specific capacitance of 2210.6 F g^-1 at 1 A g^-1 and 88.8% capacitance retention at 10 A g^-1. Furthermore, the asymmetric supercapacitor (ASC) constructed with NiCo-LDH@C//RGO reveals a remarkable energy density of 45.02 W h kg^-1 with a power density of 799.96 W kg^-1. This project aims to propose a novel avenue to exploit NiCo-LDH electrode materials and provide theory and methodological guidance for deriving complex structures from MOF derivatives.