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

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.

doi:10.1021/ja511559d

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

Journal Article · Mon Jan 05 00:00:00 EST 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/ja511559d· OSTI ID:1571037

Friebel, Daniel ^[1]; Louie, Mary W. ^[2]; Bajdich, Michal ^[3]; Sanwald, Kai E. ^[4]; Cai, Yun ^[2]; Wise, Anna M. ^[5]; Cheng, Mu-Jeng ^[2]; Sokaras, Dimosthenis ^[5]; Weng, Tsu-Chien ^[5]; Alonso-Mori, Roberto ^[6]; Davis, Ryan C. ^[5]; Bargar, John R. ^[5]; Nørskov, Jens K. ^[3]; Nilsson, Anders ^[7]; Bell, Alexis T. ^[2]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis; SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; Technische Univ. München, Garching (Germany). Dept. of Chemistry
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Lightsource
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis; SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource

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. In this study, we identify the origin of a 500-fold OER activity enhancement that can be achieved with mixed (Ni,Fe)oxyhydroxides (Ni_1-xFe_xOOH) 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 Fe³⁺ in Ni_1-xFe_xOOH 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-xFe_xOOH are not active sites for the oxidation of water. (Graph Presented).

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1571037

Alternate ID(s):: OSTI ID: 1255581

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 3 Vol. 137; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Practical Cluster Models for a Layered β-NiOOH Material Butera, Valeria; Toroker, Maytal Caspary Materials, Vol. 10, Issue 5 https://doi.org/10.3390/ma10050480	journal	April 2017
FeS2/C Nanowires as an Effective Catalyst for Oxygen Evolution Reaction by Electrolytic Water Splitting Pan, Kefeng; Zhai, Yingying; Zhang, Jiawei Materials, Vol. 12, Issue 20 https://doi.org/10.3390/ma12203364	journal	October 2019
Iron Is the Active Site in Nickel/Iron Water Oxidation Electrocatalysts Hunter, Bryan; Winkler, Jay; Gray, Harry Molecules, Vol. 23, Issue 4 https://doi.org/10.3390/molecules23040903	journal	April 2018

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