Welcome to the new version of CaltechAUTHORS. Login is currently restricted to library staff. If you notice any issues, please email coda@library.caltech.edu
Published April 14, 2015 | Published + Supplemental Material
Journal Article Open

The Selective Electrochemical Conversion of Preactivated CO_2 to Methane

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.

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.

Attached Files

Published - J._Electrochem._Soc.-2015-Luca-H473-6.pdf

Supplemental Material - 14874_1_supp_0_nlrxfz.txt

Supplemental Material - 14874_1_supp_217874_nlqd0x.pdf

Files

14874_1_supp_0_nlrxfz.txt
Files (665.8 kB)
Name Size Download all
md5:a66b327e3ad0a5dba1b3387c1a39a8ba
1.1 kB Preview Download
md5:4ab6f37961a4761545e05a44faa59eb3
357.8 kB Preview Download
md5:148d66c6304ed96477c3f20922e7bff8
306.9 kB Preview Download

Additional details

Created:
August 20, 2023
Modified:
October 23, 2023