Nickel–Gallium-Catalyzed Electrochemical Reduction of CO2 to Highly Reduced Products at Low Overpotentials

Torelli, Daniel A.; Francis, Sonja A.; Crompton, J. Chance; Javier, Alnald; Thompson, Jonathan R.; Brunschwig, Bruce S.; Soriaga, Manuel P.; Lewis, Nathan S.

doi:10.1021/acscatal.5b02888

Cited by 306CO2 Reduction Techniques and CatalystsCatalysts for Methane ReformingCarbon dioxide utilization in catalysis

Nickel–Gallium-Catalyzed Electrochemical Reduction of CO2 to Highly Reduced Products at Low Overpotentials

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Torelli, Daniel A., Francis, Sonja A., Crompton, J. Chance, Javier, Alnald, Thompson, Jonathan R., Brunschwig, Bruce S., Soriaga, Manuel P., Lewis, Nathan S.·2016·ACS Catalysis

DOI 10.1021/acscatal.5b02888

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Abstract

We report the electrocatalytic reduction of CO2 to the highly reduced C2 products, ethylene and ethane, as well as to the fully reduced C1 product, methane, on three different phases of nickel–gallium (NiGa, Ni3Ga, and Ni5Ga3) 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 C2 products from CO2. Similar product distributions and onset potentials were observed for all three nickel–gallium stoichiometries tested. The onset potential for the reduction of CO2 to C2 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 CO2 to C2 products and methane. The nickel–gallium films also reduced CO to ethylene, ethane, and methane, consistent with a CO2 reduction mechanism that first involves the reduction of CO2 to CO. Isotopic labeling experiments with 13CO2 confirmed that the detected products were produced exclusively by the reduction of CO2.

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The predicted theoretical limiting potential for CH3OH production using Pt@dv-Gr is significantly less negative than any catalysts that produce CH4 or CH3OH in the literature, whether synthesized (-0.5 to -1.0 V) or predicted (-0.3 to -1.0 V).
“In particular, as in the free energy diagram shown in Fig. 4 in detail, the predicted theoretical limiting potential (U L) for CH3OH production using Pt@dv-Gr is significantly less negative than any catalysts that produce CH4 or CH3OH in the literature, synthesized (–0.5 to –1.0 V)35,37,38 or predicted (–0.3 V to –1.0 V).4,6,39,40”
From Single-atom catalysts for CO 2 electroreduction with significant activity and selectivity improvements (2017) · cites this paper as [38]

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Self-citation

Authors: Torelli, D. A., Francis, S. A., Crompton, J. C., Javier, A., Thompson, J. R., Brunschwig, B. S., Soriaga, M. P., & Lewis, N. S.
Affiliations: California Institute of Technology (US)
Corresponding author: Lewis, Nathan S.
ORCID: Torelli, Daniel A.
Javier, Alnald
Thompson, Jonathan R.
Brunschwig, Bruce S.
Soriaga, Manuel P.
Lewis, Nathan S.
Venue: ACS Catalysis
Publisher: American Chemical Society (ACS)
Published: 2016-02-17
Volume: 6
Issue: 3
Pages: 2100-2104
ISSN: 2155-5435 (ISSN-L)
DOI: 10.1021/acscatal.5b02888
OpenAlex: W2282681552
Cited by: 306
References: 46
Citations by year: 2026: 16 · 2025: 25 · 2024: 28 · 2023: 25 · 2022: 33 · 2021: 33 · 2020: 37 · 2019: 36 · 2018: 33 · 2017: 33 · 2016: 7
FWCI: 9.86
Type: journal article
Language: en
Open access: hybrid
doi.org
Licence: other-oa
pubs.acs.org/page/policy/authorchoice_termsofuse.html (vor, 579 d)
Locations: ACS Catalysis (publishedVersion, other-oa)
CaltechAUTHORS (California Institute of Technology) (submittedVersion)
OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
Funders: National Science Foundation (NA)
U.S. Department of Defense (NA)
Air Force Office of Scientific Research (FA9550-10-1-0572)
Office of Science (DE-SC0004993)
Resnick Sustainability Institute for Science, Energy and Sustainability, California Institute of Technology (NA)
Beckman Institute, California Institute of Technology (NA)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
Physical Sciences › Chemical Engineering › Process Chemistry and Technology › Carbon dioxide utilization in catalysis
Keywords: electrochemical CO2 reduction, Ni3Ga, methane production, ethylene production, ethane production, low overpotential, turn-on voltage, bicarbonate electrolyte, isotopic labeling, 13CO2, copper comparison, drop-cast films

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Nickel–Gallium-Catalyzed Electrochemical Reduction of CO2 to Highly Reduced Products at Low Overpotentials

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