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Nickel−Gallium-Catalyzed Electrochemical Reduction of CO_2 to Highly Reduced Products at Low Overpotentials

Torelli, Daniel A. and Francis, Sonja A. and Crompton, J. Chance and Javier, Alnald and Thompson, Joanthan R. and Brunschwig, Bruce S. and Soriaga, Manuel P. and Lewis, Nathan S. (2016) Nickel−Gallium-Catalyzed Electrochemical Reduction of CO_2 to Highly Reduced Products at Low Overpotentials. ACS Catalysis, 6 (3). pp. 2100-2104. ISSN 2155-5435. doi:10.1021/acscatal.5b02888.

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We report the electrocatalytic reduction of CO_2 to the highly reduced C_2 products, ethylene and ethane, as well as to the fully reduced C_1 product, methane, on three different phases of nickel–gallium (NiGa, Ni_3Ga, and Ni_5Ga_3) films prepared by drop-casting. In aqueous bicarbonate electrolytes at neutral pH, the onset potential for methane, ethylene, and ethane production on all three phases was found to be −0.48 V versus the reversible hydrogen electrode (RHE), among the lowest onset potentials reported to date for the production of C_2 products from CO_2. Similar product distributions and onset potentials were observed for all three nickel–gallium stoichiometries tested. The onset potential for the reduction of CO_2 to C_2 products at low current densities catalyzed by nickel–gallium was >250 mV more positive than that of polycrystalline copper, and approximately equal to that of single crystals of copper, which have some of the lowest overpotentials to date for the reduction of CO_2 to C_2 products and methane. The nickel–gallium films also reduced CO to ethylene, ethane, and methane, consistent with a CO_2 reduction mechanism that first involves the reduction of CO2 to CO. Isotopic labeling experiments with ^(13)CO_2 confirmed that the detected products were produced exclusively by the reduction of CO_2.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Torelli, Daniel A.0000-0002-6222-817X
Javier, Alnald0000-0002-0306-5462
Brunschwig, Bruce S.0000-0002-6135-6727
Soriaga, Manuel P.0000-0002-0077-6226
Lewis, Nathan S.0000-0001-5245-0538
Alternate Title:Nickel−Gallium-Catalyzed Electrochemical Reduction of CO2 to Highly Reduced Products at Low Overpotentials
Additional Information:© 2016 American Chemical Society. Received: December 17, 2015. Publication Date (Web): February 17, 2016. The authors would like to thank Prof. Matthew McDowell for his help with TEM and insightful discussions, Dr. Ivonne Ferrer for her help with GC setup and calibration, and Dr. Kimberly Papadantonakis for help with editing. 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. D.A.T. recognizes a Graduate Research Fellowship from the National Science Foundation for support. S.A.F. acknowledges the Resnick Sustainability Institute at Caltech for a Postdoctoral Fellowship. J.C.C. acknowledges support from the Department of Defense through the National Defense Science & Engineering Graduate Fellowship Program. N.S.L. acknowledges support through the Multidisciplinary University Research Initiative (MURI) under AFOSR Award No. FA9550-10-1-0572. These authors contributed equally (D.A.T. and S.A.F.). The authors declare no competing financial interest.
Group:Resnick Sustainability Institute, JCAP
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
NSF Graduate Research FellowshipUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
National Defense Science and Engineering Graduate (NDSEG) FellowshipUNSPECIFIED
Air Force Office of Scientific Research (AFOSR)FA9550-10-1-0572
Subject Keywords:CO_2 reduction; electrocatalysis; nickel gallium; NiGa; ethane; methane; low overpotential; C_2 production
Issue or Number:3
Record Number:CaltechAUTHORS:20160224-132719916
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Official Citation:Nickel–Gallium-Catalyzed Electrochemical Reduction of CO2 to Highly Reduced Products at Low Overpotentials Daniel A. Torelli, Sonja A. Francis, J. Chance Crompton, Alnald Javier, Jonathan R. Thompson, Bruce S. Brunschwig, Manuel P. Soriaga, and Nathan S. Lewis ACS Catalysis 2016 6 (3), 2100-2104 DOI: 10.1021/acscatal.5b02888
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:64740
Deposited By: Heidi Rusina
Deposited On:24 Feb 2016 21:43
Last Modified:10 Nov 2021 23:34

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