Reduction of Aqueous CO2 to 1-Propanol at MoS2 Electrodes

Sonja A. Francis, Jesus M. Velazquez, Ivonne M. Ferrer, Daniel A. Torelli, Dan Guevarra, Matthew T. McDowell, Ke Sun, Xinghao Zhou, Fadl H. Saadi, Jimmy John, Matthias H. Richter, Forrest P. Hyler, Kimberly M. Papadantonakis, Bruce S. Brunschwig, Nathan S. Lewis

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Abstract

Reduction of carbon dioxide in aqueous electrolytes at single-crystal MoS2 or thin-film MoS2 electrodes yields 1-propanol as the major CO2 reduction product, along with hydrogen from water reduction as the predominant reduction process. Lower levels of formate, ethylene glycol, and t-butanol were also produced. At an applied potential of 0.59 V versus a reversible hydrogen electrode, the Faradaic efficiencies for reduction of CO2 to 1-propanol were 3.5% for MoS2 single crystals and 1% for thin films with low edge-site densities. Reduction of CO2 to 1-propanol is a kinetically challenging reaction that requires the overall transfer of 18 e- and 18 H+ in a process that involves the formation of 2 C-C bonds. NMR analyses using 13CO2 showed the production of 13C-labeled 1-propanol. In all cases, the vast majority of the Faradaic current resulted in hydrogen evolution via water reduction. H2S was detected qualitatively when single-crystal MoS2 electrodes were used, indicating that some desulfidization of single crystals occurred under these conditions.

Original languageEnglish
Pages (from-to)4902-4908
Number of pages7
JournalChemistry of Materials
Volume30
Issue number15
DOIs
Publication statusPublished - Aug 14 2018

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ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

Francis, S. A., Velazquez, J. M., Ferrer, I. M., Torelli, D. A., Guevarra, D., McDowell, M. T., Sun, K., Zhou, X., Saadi, F. H., John, J., Richter, M. H., Hyler, F. P., Papadantonakis, K. M., Brunschwig, B. S., & Lewis, N. S. (2018). Reduction of Aqueous CO2 to 1-Propanol at MoS2 Electrodes. Chemistry of Materials, 30(15), 4902-4908. https://doi.org/10.1021/acs.chemmater.7b04428