Rational design of sulfur vacancy-rich NiCo2S4/C nanostructure for high-performance hybrid supercapacitors

Nickel-cobalt sulfides (NiCo2S4) with abundant valence states are promising electrode materials for multiple faradaic reactions in hybrid supercapacitors. However, the slow electron transfer kinetics and lack of active sites restrict its electrochemical activity. Herein, an effective synthesis strategy was proposed to synergistically improve the electrochemical performance of NiCo2S4 through one-step in-situ carbonization-vulcanization method of metal-organic frameworks (MOF). Through rational selection and optimization of the Ni:Co ratio, the fibre-assembled urchin-like 3D nanoflowers (denoted as NCSC) possess abundant sulfur vacancies and appropriate porosity. Interestingly, the S vacancies can expose more redox active sites, while the expandable 3D carbon conductive network can accelerate electron transport. Furthermore, the electrical conductivity and interfacial activity is synergistically enhanced by strong electronic coupling effects. Experimental results reveal that the NiCo2S4/C exhibit excellent electrochemical performance as a battery-type electrode material. The specific capacitance is 1934 F·g-1 (967C·g-1) at 1A·g-1 and the capacitance retention is 93.2% after 5000 cycles at 5A·g-1. The assembled hybrid supercapacitor device (NiCo2S4/C//AC) exhibits an exceptionally high energy density of 50.24Wh·kg-1 at power density of 800W·kg-1. These results have significant implications for the optimization of the transition metal compounds for electrochemical energy-storage devices.