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Reduction of aqueous CO_2 to 1-Propanol at MoS_2 electrodes

Francis, Sonja A. and Velazquez, Jesus M. and Ferrer, Ivonne M. and Torelli, Daniel A. and Guevarra, Dan and McDowell, Matthew T. and Sun, Ke and Zhou, Xinghao and Saadi, Fadl H. and John, Jimmy and Richter, Matthias H. and Hyler, Forrest P. and Papadantonakis, Kimberly M. and Brunschwig, Bruce S. and Lewis, Nathan S. (2018) Reduction of aqueous CO_2 to 1-Propanol at MoS_2 electrodes. Chemistry of Materials, 30 (15). pp. 4902-4908. ISSN 0897-4756. http://resolver.caltech.edu/CaltechAUTHORS:20180613-162202390

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Abstract

Reduction of carbon dioxide in aqueous electrolytes at single-crystal MoS_2 or thin-film MoS_2 electrodes yields 1-propanol as the major CO_2 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 CO_2 to 1-propanol were ∼3.5% for MoS2single crystals and ∼1% for thin films with low edge-site densities. Reduction of CO_2 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 ^(13)CO_2 showed the production of ^(13)C-labeled 1-propanol. In all cases, the vast majority of the Faradaic current resulted in hydrogen evolution via water reduction. H_2S was detected qualitatively when single-crystal MoS_2 electrodes were used, indicating that some desulfidization of single crystals occurred under these conditions.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://dx.doi.org/10.1021/acs.chemmater.7b04428DOIArticle
https://pubs.acs.org/doi/suppl/10.1021/acs.chemmater.7b04428PublisherSupporting Information
ORCID:
AuthorORCID
Torelli, Daniel A.0000-0002-6222-817X
Sun, Ke0000-0001-8209-364X
Zhou, Xinghao0000-0001-9229-7670
Saadi, Fadl H.0000-0003-3941-0464
John, Jimmy0000-0002-8772-8939
Papadantonakis, Kimberly M.0000-0002-9900-5500
Brunschwig, Bruce S.0000-0002-6135-6727
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2018 American Chemical Society. Received: October 20, 2017; Revised: June 12, 2018; Published: June 13, 2018. We thank Dr. Nathan Dalleska and Dr. David VanderVelde of the Environmental Analysis Center and High Resolution NMR Facility, respectively, for many useful discussions and instrumental access and assistance. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award DE-SC0004993. S.A.F. acknowledges the Resnick Sustainability Institute at Caltech for a Postdoctoral Fellowship. J.M.V. acknowledges support through an NRC Ford Foundation Postdoctoral Fellowship and UC Davis startup funds. D.A.T. acknowledges support through a Graduate Research Fellowship from the National Science Foundation. Author Contributions: S.A.F. and J.M.V. contributed equally. The authors declare no competing financial interest.
Group:JCAP, Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Resnick Sustainability InstituteUNSPECIFIED
National Research CouncilUNSPECIFIED
Ford FoundationUNSPECIFIED
University of California, DavisUNSPECIFIED
NSF Graduate Research FellowshipUNSPECIFIED
Record Number:CaltechAUTHORS:20180613-162202390
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20180613-162202390
Official Citation: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, and Nathan S. Lewis Chemistry of Materials 2018 30 (15), 4902-4908 DOI: 10.1021/acs.chemmater.7b04428
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:87092
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:14 Jun 2018 14:39
Last Modified:20 Aug 2018 16:07

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