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The Selective Electrochemical Conversion of Preactivated CO_2 to Methane

Luca, Oana R. and McCrory, Charles C. L. and Dalleska, Nathan F. and Koval, Carl A. (2015) The Selective Electrochemical Conversion of Preactivated CO_2 to Methane. Journal of the Electrochemical Society, 162 (7). H473-H476. ISSN 0013-4651. http://resolver.caltech.edu/CaltechAUTHORS:20150622-081748039

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Abstract

This work reports the selective electrochemical conversion of CO_2 to methane, the reverse reaction of fossil fuel combustion. This reaction is facilitated by preactivation of the CO_2 molecule with an N-heterocyclic carbene (NHC) to form a zwitterionic species in the first step. In the presence of Ni(cyclam)^(2+) and CF_3CH_2OH, this species is shown to undergo further electrochemical reduction of the bound-CO_2 fragment at glassy carbon cathodes in dichloromethane electrolyte solution. Labeling studies confirm the origin of the carbon and protons in the methane product are the preactivated CO_2 and trifluoroethanol respectively.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1149/2.0371507jesDOIArticle
http://jes.ecsdl.org/content/162/7/H473PublisherArticle
http://jes.ecsdl.org/content/162/7/H473/suppl/DC1PublisherSupplemental Material
ORCID:
AuthorORCID
Luca, Oana R.0000-0002-2988-4909
McCrory, Charles C. L.0000-0001-9039-7192
Dalleska, Nathan F.0000-0002-2059-1587
Additional Information:© 2015 The Author(s). Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. Manuscript submitted February 9, 2015; revised manuscript received March 24, 2015. Published April 14, 2015. 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 Number DE-SC0004993. The authors thank Professors Jonas Peters, T. Don Tilley, Clifford Kubiak and Nathan Lewis for many insightful discussions. We thank Dr. Slobodan Mitrovic and Natalie Becerra for help with the XPS analyses, Ryan Jones and Katherine Schilling for technical support and Rick Gerhardt for help with the electrochemical cell design. ORL and CCLM performed electrochemical experiments. CCLM analyzed the XPS data, NFD aided in the labeling experiments. CAK advised the research. ORL had the idea for the project. ORL, CCLM, NFD and CAK wrote the manuscript.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Record Number:CaltechAUTHORS:20150622-081748039
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20150622-081748039
Official Citation:Oana R. Luca, Charles C. L. McCrory, Nathan F. Dalleska, and Carl A. Koval The Selective Electrochemical Conversion of Preactivated CO2 to Methane J. Electrochem. Soc. 2015 162(7): H473-H476; doi:10.1149/2.0371507jes
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:58389
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:22 Jun 2015 19:49
Last Modified:11 Apr 2017 16:12

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