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DOI10.1039/d0ee01609h
Capturing the active sites of multimetallic (oxy)hydroxides for the oxygen evolution reaction
Bo X.; Hocking R.K.; Zhou S.; Li Y.; Chen X.; Zhuang J.; Du Y.; Zhao C.
发表日期2020
ISSN17545692
起始页码4225
结束页码4237
卷号13期号:11
英文摘要Efficient generation of H2via water-splitting is an underpinning technology for realizing the hydrogen economy. However, the sluggish anodic oxygen evolution reaction (OER) requires a large energy input. Low-cost, transition metals such as NiFe oxides/hydroxides have been regarded as one of the most efficient catalysts for the OER in alkaline media, although the detailed mechanisms remain debated due to the lack of direct evidence for the proposed active sites during the catalytic processes. Herein, we show a NiFe (oxy)hydroxide catalyst doped with a third metal Cr prepared by facile electrodeposition to achieve further enhanced activity for the OER. Operando Raman and X-ray absorption spectroscopy (XAS) characterisation were employed to detect the formation of active intermediates and M-O bonds on active sites during the OER process. For the host NiFe (oxy)hydroxide catalyst, the shorter Fe-O in the Fe-substituted-β-NiOOH intermediate is observed as active sites for the OER. A Cr, Fe-substituted-β-NiOOH intermediate is detected in the enhanced NiFeCr (oxy)hydroxide catalyst where Cr is oxidized into the 6+ valence state with optimal Cr-O bonds, adding new active sites to boost the OER. Density functional theory (DFT) calculations support the operando spectroscopic observations and reveal the lower overpotential at the Cr6+ sites in the NiFeCr oxyhydroxide intermediate than the Fe3+ sites in the NiFe oxyhydroxide intermediate. This study demonstrates a strategy for designing highly active OER catalysts by introducing high valence metals into oxides/hydroxides to further enhance the kinetics of water oxidation. © The Royal Society of Chemistry.
英文关键词Binary alloys; Catalyst activity; Density functional theory; Hydrogen economy; Oxygen; Oxygen evolution reaction; Ternary alloys; Transition metal compounds; X ray absorption spectroscopy; Active intermediates; Catalytic process; Efficient catalysts; Fe-substituted; Oxygen evolution reaction (oer); Valence metals; Water oxidation; Water splitting; Chromium; atomic absorption spectroscopy; catalysis; catalyst; efficiency measurement; hydrogen; oxygen; reaction kinetics
语种英语
来源期刊Energy & Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/189484
作者单位School of Chemistry, University of New South Wales, Sydney, 2052, Australia; Department of Chemistry and Biotechnology and Centre for Translational Atomaterials, CTAM, Swinburne University of Technology, Hawthorn, VIC 3122, Australia; Institute for Superconducting and Electronic Materials (ISEM), Australian Institute for Innovative Materials (AIIM), University of Wollongong, Wollongong, NSW 2522, Australia; Key Laboratory of Materials Modification by Laser, Ion and Electron Beams Dalian University of Technology, Dalian, 116024, China; BUAA-UOW Joint Research Center, School of Physics, Beihang University, Beijing, 100191, China
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Bo X.,Hocking R.K.,Zhou S.,et al. Capturing the active sites of multimetallic (oxy)hydroxides for the oxygen evolution reaction[J],2020,13(11).
APA Bo X..,Hocking R.K..,Zhou S..,Li Y..,Chen X..,...&Zhao C..(2020).Capturing the active sites of multimetallic (oxy)hydroxides for the oxygen evolution reaction.Energy & Environmental Science,13(11).
MLA Bo X.,et al."Capturing the active sites of multimetallic (oxy)hydroxides for the oxygen evolution reaction".Energy & Environmental Science 13.11(2020).
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