Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 10, Pages 3663-3668Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b10855
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- US Department of Energy [DE-SC0008686]
- U.S. Department of Energy (DOE) [DE-SC0008686] Funding Source: U.S. Department of Energy (DOE)
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Electroreduction of small molecules in aqueous solution often competes with the hydrogen evolution reaction (HER), especially if the reaction is driven even moderately hard using a large overpotential. Here, the oxygen reduction reaction (ORR) was studied under proton diffusion-limited conditions in slightly acidic electrolytes: a model system to study the relative transport kinetics of protons and reactants to an electrocatalyst and the relationship between transport and catalytic performance. Using dealloyed nanoporous nickel platinum (np-NiPt) electrodes, we find the hydrogen evolution reaction can be completely suppressed even at high overpotentials (-400 mV vs RHE). In addition, the mechanism of oxygen reduction can be changed by using buffered versus unbuffered solutions, suggesting the reaction selectivity is associated with a transient rise (or lack thereof) in the interface pH at the np-NiPt surface. Independently controlling reactant transport to electrocatalyst surfaces at high overpotentials exhibited a surprisingly rich phenomenology that may offer a generalizable strategy to increase activity and selectivity during electroreduction reactions.
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