Charge-Transfer Effects in Ni–Fe and Ni–Fe–Co Mixed-Metal Oxides for the Alkaline Oxygen Evolution Reaction

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Northeastern University Center for Renewable Energy Technology (NUCRET), Department of Chemistry and Chemical Biology, Northeastern University, 317 Egan Research Center, 360 Huntington Avenue, Boston, Massachusetts 02115, United States
*E-mail for S.M.: [email protected]
Cite this: ACS Catal. 2016, 6, 1, 155–161
Publication Date (Web):November 20, 2015
Copyright © 2015 American Chemical Society
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Ni–Fe and Ni–Fe–Co mixed-metal oxide (MMO) films were investigated as electrocatalysts for the oxygen evolution reaction (OER) in 0.1 M KOH. In an effort to optimize MMO morphology, aniline was used as a capping agent to produce high-surface-area Ni–Fe–Co films on Raney nickel supports. This catalyst exhibits enhanced mass activity in comparison to the Ni–Fe OER electrocatalysts reported to date. Cyclic voltammetry shows changes in the potential of the Ni2+/3+ transitions in Fe- or Co-containing MMO films. In situ X-ray absorption spectroscopy (XAS) analysis confirms that Fe acts to stabilize Ni in the 2+ oxidation state, while Co facilitates oxidation to the 3+ state. The results of this study support the recent claims that Fe (not Ni) is the OER active site. The OER enhancement of the ternary Ni–Fe–Co catalyst results from two effects: (1) the charge-transfer effects of Co result in the formation of the conductive NiIIIOOH phase at lower overpotential, thus activating the Fe sites which are otherwise inaccessible to electron transfer in the nonconductive NiII(OH)2 host lattice, and (2) XAS analysis shows that the presence of Co effectively “shrinks” the Ni and Fe local geometry, likely resulting in an optimized Fe–OH/OOH bond strength. In addition, analysis of heat-treatment effects indicates that calcination at 400 °C improves the OER activity of Ni–Fe–Co but deactivates Ni–Fe. Annealing studies under argon show that MMO surfaces with a hydrated Ni(OH)2 phase and a crystalline NiO phase exhibit nearly identical OER activities. Finally, the morphology of the MMO catalyst film on Raney Ni support provides excellent catalyst dispersion and should result in high active-site utilization for use in technologically relevant gas-diffusion electrodes.

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