Tungsten-Doped NiFe-Layered Double Hydroxides as Efficient Oxygen Evolution Catalysts

1.
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
2.
Ocean Hydrogen Energy R & D Center, Research Institute of Tsinghua University in Shenzhen, Shenzhen 518071, Guangdong Province, China
3.
China Institute of Nuclear Industry Strategy, Beijing 100048, China
4.
Xinjiang Coal Mine Mechanical and Electrical Engineering Technology Research Center, Xinjiang Institute of Engineering, Urumchi 830023, China
5.
College of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, China

Corresponding author: Yun Kuang, kuangyun@mail.buct.edu.cn Xiaoming Sun, sunxm@mail.buct.edu.cn

Received Date: 30 March 2023
Accepted Date: 25 May 2023
Revised Date: 24 May 2023
Available Online: 15 January 2024
Fund Project:

Abstract: Electrochemical water splitting proves critical to sustainable and clean hydrogen fuel production. However, the anodic water oxidation reaction—the major half-reaction in water splitting—has turned into a bottleneck due to the high energy barrier of the complex and sluggish four-electron transfer process. Nickel-iron layered double hydroxides (NiFe-LDHs) are regarded as promising non-noble metal electrocatalysts for oxygen evolution reaction (OER) catalysis in alkaline conditions. However, the electrocatalytic activity of NiFe-LDH requires improvement because of poor conductivity, a small number of exposed active sites, and weak adsorption of intermediates. As such, tremendous effort has been made to enhance the activity of NiFe-LDH, including introducing defects, doping, exfoliation to obtain single-layer structures, and constructing arrayed structures. In this study, researchers controllably doped NiFe-LDH with tungsten using a simple one-step alcohothermal method to afford nickel-iron-tungsten layered double hydroxides (NiFeW-LDHs). X-ray powder diffraction analysis was used to investigate the structure of NiFeW-LDH. The analysis revealed the presence of the primary diffraction peak corresponding to the perfectly hexagonal-phased NiFe-LDH, with no additional diffraction peaks observed, thereby ruling out the formation of tungsten-based nanoparticles. Furthermore, scanning electron microscopy (SEM) showed that the NiFeW-LDH nanosheets were approximately 500 nm in size and had a flower-like structure that consisted of interconnected nanosheets with smooth surfaces. Additionally, it was observed that NiFeW-LDH had a uniform distribution of Ni, Fe, and W throughout the nanosheets. X-ray photoelectron spectra (XPS) revealed the surface electronic structure of the NiFeW-LDH catalyst. It was determined that the oxidation state of W in NiFeW-LDH was +6 and that the XPS signal of Fe in NiFeW-LDH shifted to a higher oxidation state compared to NiFe-LDH. These results suggest electron redistribution between Fe and W. Simultaneously, the peak area of surface-adsorbed OH increased significantly after W doping, suggesting enhanced OH adsorption on the surface of NiFeW-LDH. Furthermore, density functional theory (DFT) calculations indicated that W(Ⅵ) facilitates the adsorption of H₂O and O^*-intermediates and enhances the activity of Fe sites, which aligns with experimental results. The novel NiFeW-LDH catalyst displayed a low overpotential of 199 and 237 mV at 10 and 100 mA∙cm⁻² in 1 mol∙L⁻¹ KOH, outperforming most NiFe-based colloid catalysts. Furthermore, experimental characterizations and DFT+U calculations suggest that W doping plays an important role through strong electronic interactions with Fe and facilitating the adsorption of important O-containing intermediates.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

钨掺杂镍铁水滑石高效电催化析氧反应

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孙晓明, sunxm@mail.buct.edu.cn

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