Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 56, Issue 47, Pages 15025-15029Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201709455
Keywords
cation co-adsorption; hydrogen adsorption; non-Nernstian potential shift; pH dependence; stepped platinum single crystals
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Funding
- China Scholarship Council [201506220154]
- National Science Foundation NRT [1449785]
- Direct For Education and Human Resources
- Division Of Graduate Education [1449785] Funding Source: National Science Foundation
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The successful deployment of advanced energy-conversion systems depends critically on our understanding of the fundamental interactions of the key adsorbed intermediates (hydrogen *H and hydroxyl *OH) at electrified metal-aqueous electrolyte interfaces. The effect of alkali metal cations (Li+, Na+, K+, Cs+) on the non-Nernstian pH shift of the step-related voltammetric peak of the Pt(553) electrode is investigated over a wide pH window (1 to 13) by means of experimental and computational methods. The co-adsorbed alkali cations along the step weaken the OH adsorption at the step sites, causing a positive shift of the potential of the step-related peak on Pt(553). Density functional calculations explain the observations on the identity and concentration of alkali cations on the non-Nernstian pH shift, and demonstrate that cation-hydroxyl co-adsorption causes the apparent pH dependence of hydrogen adsorption in the step sites of platinum electrodes.
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