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- Transition metal sulfides have been investigated as promising bifunctional materials for catalytic energy generation and energy storage applications. Although various strategies such as tuning the size, phase or defects and composition engineering have led to catalytic enhancement, there still remains the requirement for better performance for practical applications. In this study, we have used a potentially scalable solventless route for phase selective synthesis of α-NiS or β-NiS. Both phases were doped with different transition metals (Cu, Co and Fe) for enhanced catalytic performance. Interestingly, besides commonly observed thermal assisted phase transition, dopant (Co, Cu, and Fe) induced α- to β-phase transition or vice versa was also observed which has rarely been reported for NiS. The effect of dopants on the crystal structure and electrocatalytic activity has been investigated. The best supercapacitive behavior was observed for Co-doped α-NiS which showed a specific capacitance of 1586 F g−1 at a current density of 0.5 A g−1 and a high rate capability. On the other hand, Fe-doped α-NiS displayed the best electrocatalytic activity for both the OER (266 mV at 10 mA cm−2) and the HER (146 mV at 10 mA cm−2), with Tafel slopes of 79 and 113 mV dec−1 respectively. The Fe-doped α-NiS catalyst was also used as both the anode and cathode in an electrolyzer, in which an overpotential of about 410 mV at 10 mA cm−2 was observed. The prepared electrodes demonstrate outstanding stability and flexibility.
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- Nickel sulfide is regarded as a material with tremendous potential for energy storage and conversion applications. However, it exists in a variety of stable compositions and obtaining a pure phase is a challenge. This study demonstrates a potentially scalable, solvent free and phase selective synthesis of uncapped α-NiS, β-NiS and α-β-NiS composites using nickel alkyl (ethyl, octyl) xanthate precursors. Phase transformation and morphology were observed by powder-X-ray diffraction (p-XRD), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The comparative efficiency of the synthesized samples was investigated for energy storage and generation applications, in which superior performance was observed for the NiS synthesized from the short chain xanthate complex. A high specific capacitance of 1,940F/g, 2,150F/g and 2,250F/g was observed at 2mV/s for bare α-NiS, β-NiS and α-β-NiS composite respectively. At high current density of 1A/g, α-NiS showed the highest capacitance of 1,287F/g, with 100% of Coulombic efficiency and 79% of capacitance retention. In the case of the oxygen evolution reaction (OER), β-NiS showed an overpotential of 139mV at a current density of 10mA/cm2, with a Tafel slope of only 32mV/dec, showing a fast and efficient process. It was observed that the increase in carbon chain of the synthesized self-capped nickel sulfide nanoparticles decreased the overall efficiency, both for energy storage and energy generation applications.
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- Ternary metal sulfides are currently in the spotlight as promising electroactive materials for high-performance energy storage and/or conversion technologies. Extensive research on metal sulfides has indicated that, amongst other factors, the electrochemical properties of the materials are strongly influenced by the synthetic protocol employed. Herein, we report the electrochemical performance of uncapped NiCo2S4 and CuCo2S4 ternary systems prepared via solventless thermolysis of the respective metal ethyl xanthate precursors at 200 and 300 °C. The structural, morphological and compositional properties of the synthesized nanoparticles were examined by powder X-ray diffraction (p-XRD), transmission electron microscopy (TEM), high-resolution TEM, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDX) techniques. Electrochemical studies indicate that NiCo2S4 nanoparticles synthesized at 300 °C exhibit superior energy storage characteristics with a high specific capacitance of ca. 2650 F g−1 at 1 mV s−1, as compared to CuCo2S4 nanoparticles, which showcased a specific capacitance of ca. 1700 F g−1 at the same scan rate. At a current density of 0.5 A g−1, NiCo2S4 and CuCo2S4 nanoparticles displayed specific capacitances of 1201 and 475 F g−1, respectively. In contrast, CuCo2S4 nanoparticles presented a higher electrocatalytic activity with low overpotentials of 269 mV for oxygen evolution reaction (OER), and 224 mV for the hydrogen evolution reaction (HER), at 10 mA cm−2. The stability of the catalysts was examined for 2000 cycles in which a negligible change in both OER and HER activities was observed.
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