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J Am Chem Soc. 2015 Aug 12;137(31):9808-11. doi: 10.1021/jacs.5b06227. Epub 2015 Jul 30.

Probing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts.

Author information

1
†Center for Individual Nanoparticle Functionality, Department of Physics, Technical University of Denmark (DTU), Kongens Lyngby, Denmark.
2
‡Department of Chemistry, Stanford University, Stanford, California 94305, United States.
3
§Materials Science Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United States.
4
∥Materials Engineering Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United States.

Abstract

CO electroreduction activity on oxide-derived Cu (OD-Cu) was found to correlate with metastable surface features that bind CO strongly. OD-Cu electrodes prepared by H2 reduction of Cu2O precursors reduce CO to acetate and ethanol with nearly 50% Faradaic efficiency at moderate overpotential. Temperature-programmed desorption of CO on OD-Cu revealed the presence of surface sites with strong CO binding that are distinct from the terraces and stepped sites found on polycrystalline Cu foil. After annealing at 350 °C, the surface-area corrected current density for CO reduction is 44-fold lower and the Faradaic efficiency is less than 5%. These changes are accompanied by a reduction in the proportion of strong CO binding sites. We propose that the active sites for CO reduction on OD-Cu surfaces are strong CO binding sites that are supported by grain boundaries. Uncovering these sites is a first step toward understanding the surface chemistry necessary for efficient CO electroreduction.

PMID:
26196863
DOI:
10.1021/jacs.5b06227

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