Hierarchical Nickel–Cobalt Hydroxide Composite Nanosheets-Incorporated Nitrogen-Doped Carbon Nanotubes Embedded with Nickel–Cobalt Alloy Nanoparticles for Driving a 2 V Asymmetric Supercapacitor

A class of electrode materials with favorable structures and compositions and powerful electrochemical (EC) properties are needed to boost the supercapacitor capacity significantly. In this study, an inventive technique was established to produce a well-aligned nickel-cobalt alloy nanoparticles-encapsulated N-doped carbon nanotubes with porous structure and good conductivity on carbon cloth (NiCo@NCNTs/CC) as a substrate. Then, nanosheets of nickel-cobalt layered double hydroxide (NiCo-LDH) were grown on NiCo@NCNTs/CC via a simple EC deposition method to construct a self-supported monolithic hierarchical nanosheets/nanotubes composite electrode of NiCo-LDH/NiCo@NCNTs/CC. In such a composite electrode, the NiCo@NCNTs can act as a good conductor and structural scaffold to grow NiCo-LDH nanosheets with a three-dimensional open and porous structure, which helps to improve the electron/ion-transfer performance, increase the number of exposed reactive sites, and inhibit the aggregation of NiCo-LDH nanosheets, thereby boosting the capacitance and stability. As a positive electrode, the NiCo-LDH/NiCo@NCNTs/CC hierarchical nanosheets/nanotubes electrode displays 1898 mF cm^-2 (1262 A g^-1) of high capacitance, long-term stability with a capacitance retention of around 100% after 8000 cycles, and nearly 103% Coulombic efficiency. After assembling into an asymmetric supercapacitor with a Co(OH)₂/NiCo@NCNTs/CC negative electrode, 2 V of operating voltage with 73.1 μW h cm^-2 (52.8 W h kg^-1) of energy density was achieved. Our investigation gives a potential approach for constructing the integrated composite electrode of transition-metal compounds-carbon materials for high-performance supercapacitors.