Journal
ACS CATALYSIS
Volume 7, Issue 2, Pages 1248-1258Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b03126
Keywords
oxygen evolution reaction (OER); transiton metal oxides; operando techniques; ambient pressure; catalytic conditions; synchrotron radiation; electron spectroscopies
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Funding
- Office of Science of the U.S. Department of Energy [DE-SC0004993]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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The oxygen evolution reaction (OER) is a critical component of industrial processes such as electrowinning of metals and the chlor-alkali process. It also plays a central role in the development of a renewable energy field for generation a solar fuels by providing both the protons and electrons needed to generate fuels such as H-2 or reduced hydrocarbons from CO2. To improve these processes, it is necessary to expand the fundamental understanding of catalytically active species at low overpotential, which will further the development of electrocatalysts with high activity and durability. In this context, performing experimental investigations of the electrocatalysts under realistic working regimes (i.e., under operando conditions) is of crucial importance. Here, we study a highly active quinary transition-metal-oxide-based OER electrocatalyst by means of operando ambient-pressure X-ray photoelectron spectroscopy and X-ray absorption spectroscopy performed at the solid/liquid interface. We observe that the catalyst undergoes a clear chemical-structural evolution as a function of the applied potential with Ni, Fe, and Co oxyhydroxides comprising the active catalytic species. While CeO2 is redox inactive under catalytic conditions, its influence on the redox processes of the transition metals boosts the catalytic activity at low overpotentials, introducing an important design principle for the optimization of electrocatalysts and tailoring of high-performance materials.
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