Spectroelectrochemical study of water oxidation on nickel and iron oxyhydroxide electrocatalysts

Laia Francàs (), Sacha Corby, Shababa Selim, Dongho Lee, Camilo A. Mesa, Robert Godin, Ernest Pastor, Ifan E. L. Stephens, Kyoung-Shin Choi and James R. Durrant ()
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Laia Francàs: Imperial College London
Sacha Corby: Imperial College London
Shababa Selim: Imperial College London
Dongho Lee: University of Wisconsin-Madison
Camilo A. Mesa: Imperial College London
Robert Godin: Imperial College London
Ernest Pastor: Imperial College London
Ifan E. L. Stephens: Imperial College London
Kyoung-Shin Choi: University of Wisconsin-Madison
James R. Durrant: Imperial College London

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Ni/Fe oxyhydroxides are the best performing Earth-abundant electrocatalysts for water oxidation. However, the origin of their remarkable performance is not well understood. Herein, we employ spectroelectrochemical techniques to analyse the kinetics of water oxidation on a series of Ni/Fe oxyhydroxide films: FeOOH, FeOOHNiOOH, and Ni(Fe)OOH (5% Fe). The concentrations and reaction rates of the oxidised states accumulated during catalysis are determined. Ni(Fe)OOH is found to exhibit the fastest reaction kinetics but accumulates fewer states, resulting in a similar performance to FeOOHNiOOH. The later catalytic onset in FeOOH is attributed to an anodic shift in the accumulation of oxidised states. Rate law analyses reveal that the rate limiting step for each catalyst involves the accumulation of four oxidised states, Ni-centred for Ni(Fe)OOH but Fe-centred for FeOOH and FeOOHNiOOH. We conclude by highlighting the importance of equilibria between these accumulated species and reactive intermediates in determining the activity of these materials.

Date: 2019
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DOI: 10.1038/s41467-019-13061-0

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