Identification of highly active Fe sites in (Ni,Fe)OOH for electrocatalytic water splitting

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

Research output: Contribution to journalArticlepeer-review

1174 Citations (Scopus)

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 (Ni1-xFexOOH) 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 Ni1-xFexOOH 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 Ni1-xFexOOH are not active sites for the oxidation of water. (Graph Presented).

Original languageEnglish
Pages (from-to)1305-1313
Number of pages9
JournalJournal of the American Chemical Society
Volume137
Issue number3
DOIs
Publication statusPublished - 2015 Jan 28

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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