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Electron density modulation of NiCo2S4 nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis.

ABSTRACT: Metal sulfides for hydrogen evolution catalysis typically suffer from unfavorable hydrogen desorption properties due to the strong interaction between the adsorbed H and the intensely electronegative sulfur. Here, we demonstrate a general strategy to improve the hydrogen evolution catalysis of metal sulfides by modulating the surface electron densities. The N modulated NiCo2S4 nanowire arrays exhibit an overpotential of 41?mV at 10?mA?cm-2 and a Tafel slope of 37?mV?dec-1, which are very close to the performance of the benchmark Pt/C in alkaline condition. X-ray photoelectron spectroscopy, synchrotron-based X-ray absorption spectroscopy, and density functional theory studies consistently confirm the surface electron densities of NiCo2S4 have been effectively manipulated by N doping. The capability to modulate the electron densities of the catalytic sites could provide valuable insights for the rational design of highly efficient catalysts for hydrogen evolution and beyond.

SUBMITTER: Wu Y

PROVIDER: S-EPMC5897358 | biostudies-literature | 2018 Apr

REPOSITORIES: biostudies-literature

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Electron density modulation of NiCo2S4 nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis.

Wu Yishang Y Liu Xiaojing X Han Dongdong D Song Xianyin X Shi Lei L Song Yao Y Niu Shuwen S Xie Yufang Y Cai Jinyan J Wu Shaoyang S Kang Jian J Zhou Jianbin J Chen Zhiyan Z Zheng Xusheng X Xiao Xiangheng X Wang Gongming G

Nature communications 20180412 1

Metal sulfides for hydrogen evolution catalysis typically suffer from unfavorable hydrogen desorption properties due to the strong interaction between the adsorbed H and the intensely electronegative sulfur. Here, we demonstrate a general strategy to improve the hydrogen evolution catalysis of metal sulfides by modulating the surface electron densities. The N modulated NiCo2S4 nanowire arrays exhibit an overpotential of 41 mV at 10 mA cm-2 and a Tafel slope of 37 ...[more]

PMID: 29651037

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Project description:There are many challenges associated with the fabrication of efficient, inexpensive, durable and very stable nonprecious metal catalysts for the hydrogen evolution reaction (HER). In this study, we have designed a facile strategy by tailoring the concentration of precursors to successfully obtain nickel-cobalt bimetallic sulfide (NiCo2S4) using a simple hydrothermal method. The morphology of the newly prepared NiCo2S4 comprised a mixture of microparticles and nanorods, which were few microns in dimension. The crystallinity of the composite sample was found to be excellent with a cubic phase. The sample that contained a higher amount of cobalt compared to nickel and produced single-phase NiCo2S4 exhibited considerably improved HER performance. The variation in the salt precursor concentration during the synthesis of a material is a simple methodology to produce a scalable platinum-free catalyst for HER. The advantageous features of the multiple active sites of cobalt in the CN-21 sample as compared to that for pristine CoS and NiS laid the foundation for the provision of abundant active edges for HER. The composite sample produced a current density of 10 mA cm-2 at an overpotential of 345 mV. Also, it exhibited a Tafel value of 60 mV dec-1, which predominantly ensured rapid charge transfer kinetics during HER. CN-21 was highly durable and stable for 30 hours. Electrochemical impedance spectroscopy showed that the charge transfer resistance was 21.88 ohms, which further validated the HER polarization curves and Tafel results. CN-21 exhibited a double layer capacitance of 4.69 μF cm-2 and a significant electrochemically active surface area of 134.0 cm2, which again supported the robust efficiency for HER. The obtained results reveal that our developed NiCo2S4 catalyst has a high density of active edges, and it is a non-noble metal catalyst for the hydrogen evolution reaction. The present findings provide an alternative strategy and an active nonprecious material for the development of energy-related applications.

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Electron density modulation of NiCo2S4 nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis.

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Electron density modulation of NiCo<sub>2</sub>S<sub>4</sub> nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis.

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