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We perform a joint experimental-theoretical study of the electrochemicaloxidation of CO on copper (Cu) under alkaline conditions. Using cyclicvoltammetry on Cu single crystal surfaces, we demonstrate that both Cu terracesand steps show CO oxidation activity at potentials just slightly positive(0.03-0.14 V) of the thermodynamic equilibrium potential. The overpotentialsare 0.23-0.12 V lower than that of gold (approx. 0.26 V), which up until nowhas been considered to be the most active catalyst for this process. Ourtheoretical calculations suggest that Cu's activity arises from theadvantageous combination of simultaneous *OH adsorption under CO oxidationpotentials and surmountable *CO-*OH coupling barriers. Experimentally observedonset potentials are in agreement with the computed onsets of *OH adsorption.We furthermore show that the onsets of *OH adsorption on steps are moreaffected by *CO-*OH interactions than on terraces due to a stronger competitiveadsorption. Overall, Cu(100) shows the lowest overpotential (0.03 V) of thefacets considered.

Electrochemical oxidation of CO on Cu single crystals under alkaline conditions