Detection of high-valent iron species in alloyed oxidic cobaltates for catalysing the oxygen evolution reaction

Nancy Li, Ryan G. Hadt (), Dugan Hayes (), Lin X. Chen and Daniel G. Nocera ()
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Nancy Li: Harvard University
Ryan G. Hadt: Argonne National Laboratory
Dugan Hayes: Argonne National Laboratory
Lin X. Chen: Argonne National Laboratory
Daniel G. Nocera: Harvard University

Nature Communications, 2021, vol. 12, issue 1, 1-6

Abstract: Abstract Iron alloying of oxidic cobaltate catalysts results in catalytic activity for oxygen evolution on par with Ni-Fe oxides in base but at much higher alloying compositions. Zero-field 57Fe Mössbauer spectroscopy and X-ray absorption spectroscopy (XAS) are able to clearly identify Fe4+ in mixed-metal Co-Fe oxides. The highest Fe4+ population is obtained in the 40–60% Fe alloying range, and XAS identifies the ion residing in an octahedral oxide ligand field. The oxygen evolution reaction (OER) activity, as reflected in Tafel analysis of CoFeOx films in 1 M KOH, tracks the absolute concentration of Fe4+. The results reported herein suggest an important role for the formation of the Fe4+ redox state in activating cobaltate OER catalysts at high iron loadings.

Date: 2021
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DOI: 10.1038/s41467-021-24453-6

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