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Role of Surface Oxide Layer during CO2 Reduction at Copper Electrodes

Published online by Cambridge University Press:  11 July 2012

Cheng-Chun Tsai ,
Joel Bugayong  and
Gregory L. Griffin
Cheng-Chun Tsai
Affiliation:
Department of Chemical Engineering, Louisiana State University, Baton Rouge, LA 70803, U.S.A.
Joel Bugayong
Affiliation:
Department of Chemical Engineering, Louisiana State University, Baton Rouge, LA 70803, U.S.A.
Gregory L. Griffin
Affiliation:
Department of Chemical Engineering, Louisiana State University, Baton Rouge, LA 70803, U.S.A.
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Abstract

We have compared the rates of CO formation on Cu and Cu oxide surfaces during the electrochemical reduction of CO2 in aqueous media. On metallic Cu surfaces, H2 formation is the main reaction at potentials less cathodic than –1.16 V(NHE). At this potential the formation of CO becomes significant, while CH4 appears at potentials more cathodic than –1.36 V(NHE). On electrodeposited Cu oxide surfaces there is a complex transient response. During reduction at constant potential (–1.1 V(NHE)), there is a large, transient cathodic current that corresponds to reduction of the oxide layer. After this initial oxide reduction, the current density stabilizes and the formation rates of H2 and CO show a more slowly varying transient behavior. The H2 formation rate is roughly 3x higher than on freshly cleaned Cu foil, but is largely independent of the thickness of the initial oxide layer. In contrast, the CO formation rate is at least one order of magnitude higher on the (reduced) Cu oxide samples than on Cu foil at the same potential. These results are interpreted as evidence that CO formation is enhanced at low-coordination number Cu sites present on freshly nucleated Cu clusters following oxide reduction.

Keywords

Cuelectrochemical synthesisenergy storage
Type
Articles
Information
MRS Online Proceedings Library (OPL) , Volume 1446: Symposium U – Materials for Catalysis in Energy , 2012 , mrss12-1446-u06-02
Copyright
Copyright © Materials Research Society 2012

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References

REFERENCES

1. Bell, A.T., in “Basic Research Needs: Catalysis for Energy”; U.S. Department of Energy, Office of Basic Energy Sciences Workshop August 6-8, 2007; available at: http://science.energy.gov/bes/news-and-resources/reports/basic-research-needs/ Google Scholar
2. Kerr, R. A., Science 331, 1510 (2011).Google Scholar
3. Varghese, O. K., Paulose, M., LaTempa, T. J., and Grimes, C. A., Nano Letters 9(2) 731 (2009).Google Scholar
4. Pan, Y., et al. ., Science 333, 988 (2011).Google Scholar
5. Hori, Y., “Electrochemical CO2 Reduction on Metal Electrodes”, in Modern Aspects of Electrochemistry, 42, edited by Vayenas, C. G., (Springer, 2008) p89–189.Google Scholar
6. Gattrell, M., Gupta, N., and Co, A., Journal of Electroanalytical Chemistry 594, 1 (2006).Google Scholar
7. Karl, W. Frese, Jr., J. Electrochem. Soc., 138 (11) 3338 (1991).Google Scholar
8. Chang, T.-Y., Liang, R.-M., Wu, P.-W., Chen, J.-Y., and Hsieh, Y.-C., Materials Letters 63, 1001 (2009).Google Scholar
9. Le, M., Ren, M., Zhang, Z., Sprunger, P. T., Kurtz, R. L., and Flake, J. C., J. Electrochem. Soc., 158(5), E45 (2011).Google Scholar
10. Hori, Y., Murata, A., and Takahashi, R., JCS Faraday Trans. I, 85 2309 (1989).Google Scholar
11. Whipple, D. T. and Kenis, P. J. A., J. Phys. Chem. Lett. 1 3451 (2010).Google Scholar
12. Peterson, A., Abild-Pederson, F., Studt, F., Rossmeisl, J., and Norskov, J. K., Energy & Environ. Sci. 3 1311 (2010).Google Scholar
13. Asthagiri, A. (private communication)Google Scholar
14. Tang, W., Peterson, A. A., Varela, A. S., Jovanov, Z. P., Bech, L., Durand, W. J., Dahl, S., Nørskov, J. K. and Chorkendorff, I., Phys. Chem. Chem. Phys., 14 76 (2012).Google Scholar