Experimental and Computational Evidence of Highly Active Fe Impurity Sites on the Surface of Oxidized Au for the Electrocatalytic Oxidation of Water in Basic Media
Addition of Fe to Ni- and Co-based (oxy)hydroxides has been shown to enhance the activity of these materials for electrochemical oxygen evolution. Here we show that Fe cations bound to the surface of oxidized Au exhibit enhanced oxygen evolution reaction (OER) activity. We find that the OER activity increases with increasing surface concentration of Fe. Density functional theory analysis of the OER energetics reveals that oxygen evolution over Fe cations bound to a hydroxyl-terminated oxidized Au (Fe-Au2O3) occurs at an overpotential ∼0.3V lower than over hydroxylated Au2O3 (0.82V). This finding agrees well with experimental observations and is a consequence of the more optimal binding energetics of OER reaction intermediates at Fe cations bound to the surface of Au2O3. These findings suggest that the enhanced OER activity reported recently upon low-potential cycling of Au may be due to surface Fe impurities rather than to "superactive" AuIII surfaquo species.
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- 3406 Physical chemistry
- 3405 Organic chemistry
- 3403 Macromolecular and materials chemistry
- 0399 Other Chemical Sciences
- 0306 Physical Chemistry (incl. Structural)
- 0301 Analytical Chemistry
Citation
Published In
DOI
EISSN
Publication Date
Volume
Issue
Start / End Page
Related Subject Headings
- 3406 Physical chemistry
- 3405 Organic chemistry
- 3403 Macromolecular and materials chemistry
- 0399 Other Chemical Sciences
- 0306 Physical Chemistry (incl. Structural)
- 0301 Analytical Chemistry