Electrochemical Oxidation of CO on Cu Single Crystals under Alkaline Conditions

Aarti Tiwari, Hendrik H. Heenen, Anton Simon Bjørnlund, Degenhart Hochfilzer, Karen Chan*, Sebastian Horch*

*Corresponding author for this work

Research output: Contribution to journalLetterResearchpeer-review

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Abstract

We perform a joint experimental–theoretical study of the electrochemical oxidation of CO on copper (Cu) under alkaline conditions. Using cyclic voltammetry on Cu single-crystal surfaces, we demonstrate that both Cu terraces and steps show CO oxidation activity at potentials just slightly positive (0.03–0.14 V) of the thermodynamic equilibrium potential. The overpotentials are 0.23–0.12 V lower than that of gold (≈0.26 V), which until now has been considered to be the most active catalyst for this process. Our theoretical calculations suggest that Cu’s activity arises from the advantageous combination of simultaneous *CO and *OH adsorption under CO oxidation potentials and surmountable *CO–*OH coupling barriers. Experimentally observed onset potentials are in agreement with the computed onsets of *OH adsorption. We furthermore show that the onsets of *OH adsorption on steps are more affected by *CO–*OH interactions than on terraces due to a stronger competitive adsorption. Overall, Cu(100) shows the lowest overpotential (0.03 V) of the facets considered.
Original languageEnglish
JournalACS Energy Letters
Volume5
Pages (from-to)3437-3442
Number of pages6
ISSN2380-8195
DOIs
Publication statusPublished - 2020

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