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Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting

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Friebel, Daniel, Louie, Mary W., Bajdich, Michal, Sanwald, Kai E., Cai, Yun, Wise, Anna M., Cheng, Mu-Jeng, Sokaras, Dimosthenis, Weng, Tsu-Chien, Alonso-Mori, Roberto, Davis, Ryan C., Bargar, John R., Nørskov, Jens K., Nilsson, Anders, Bell, Alexis T.·2015·Journal of the American Chemical Society

DOI 10.1021/ja511559d

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Abstract

Highly active catalysts for the oxygen evolution reaction (OER) are required for the development of photoelectrochemical devices that generate hydrogen efficiently from water using solar energy. Here, we identify the origin of a 500-fold OER activity enhancement that can be achieved with mixed (Ni,Fe)oxyhydroxides (Ni(1-x)Fe(x)OOH) over their pure Ni and Fe parent compounds, resulting in one of the most active currently known OER catalysts in alkaline electrolyte. Operando X-ray absorption spectroscopy (XAS) using high energy resolution fluorescence detection (HERFD) reveals that Fe(3+) in Ni(1-x)Fe(x)OOH occupies octahedral sites with unusually short Fe-O bond distances, induced by edge-sharing with surrounding [NiO6] octahedra. Using computational methods, we establish that this structural motif results in near optimal adsorption energies of OER intermediates and low overpotentials at Fe sites. By contrast, Ni sites in Ni(1-x)Fe(x)OOH are not active sites for the oxidation of water.

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Authors: Friebel, D., Louie, M. W., Bajdich, M., Sanwald, K. E., Cai, Y., Wise, A. M., Cheng, M.-J., Sokaras, D., Weng, T.-C., Alonso-Mori, R., Davis, R. C., Bargar, J. R., Nørskov, J. K., Nilsson, A., & Bell, A. T.
Venue: Journal of the American Chemical Society
Publisher: American Chemical Society (ACS)
Published: 2015-01-16
Volume: 137
Issue: 3
Pages: 1305-1313
ISSN: 0002-7863 (ISSN-L)
1520-5126
DOI: 10.1021/ja511559d
OpenAlex: W2323275360
Cited by: 2,732
References: 3
FWCI: 61.68
Type: journal article
Language: en
Open access: green

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Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting

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