Spectroscopic identification of active sites for the oxygen evolution reaction on iron-cobalt oxides

Rodney D. L. Smith (), Chiara Pasquini, Stefan Loos, Petko Chernev, Katharina Klingan, Paul Kubella, Mohammad Reza Mohammadi, Diego Gonzalez-Flores and Holger Dau ()
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Rodney D. L. Smith: University of Waterloo
Chiara Pasquini: Freie Universität Berlin
Stefan Loos: Freie Universität Berlin
Petko Chernev: Freie Universität Berlin
Katharina Klingan: Freie Universität Berlin
Paul Kubella: Freie Universität Berlin
Mohammad Reza Mohammadi: Freie Universität Berlin
Diego Gonzalez-Flores: Freie Universität Berlin
Holger Dau: Freie Universität Berlin

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract The emergence of disordered metal oxides as electrocatalysts for the oxygen evolution reaction and reports of amorphization of crystalline materials during electrocatalysis reveal a need for robust structural models for this class of materials. Here we apply a combination of low-temperature X-ray absorption spectroscopy and time-resolved in situ X-ray absorption spectroelectrochemistry to analyze the structure and electrochemical properties of a series of disordered iron-cobalt oxides. We identify a composition-dependent distribution of di-μ-oxo bridged cobalt–cobalt, di-μ-oxo bridged cobalt–iron and corner-sharing cobalt structural motifs in the composition series. Comparison of the structural model with (spectro)electrochemical data reveals relationships across the composition series that enable unprecedented assignment of voltammetric redox processes to specific structural motifs. We confirm that oxygen evolution occurs at two distinct reaction sites, di-μ-oxo bridged cobalt–cobalt and di-μ-oxo bridged iron–cobalt sites, and identify direct and indirect modes-of-action for iron ions in the mixed-metal compositions.

Date: 2017
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DOI: 10.1038/s41467-017-01949-8

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