Insights into the Low Overpotential Electroreduction of CO2 to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer
Abstract
Cost competitive electroreduction of CO 2 to CO requires electrochemical systems that exhibit partial current density ( j CO ) exceeding 150 mA cm –2 at cell overpotentials (|η cell |) less than 1 V. However, achieving such benchmarks remains difficult. Here, we report the electroreduction of CO 2 on a supported gold catalyst in an alkaline flow electrolyzer with performance levels close to the economic viability criteria. Onset of CO production occurred at cell and cathode overpotentials of just −0.25 and −0.02 V, respectively. High j CO (∼99, 158 mA cm –2 ) was obtained at low |η cell | (∼0.70, 0.94 V) and high CO energetic efficiency (∼63.8, 49.4%). The performance was stable for at least 8 h. Additionally, the onset cathode potentials, kinetic isotope effect, and Tafel slopes indicate the low overpotential production of CO in alkaline media to be the result of a pH-independent rate-determining step (i.e., electron transfer) in contrast to a pH-dependent overall process.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
Claims other papers make about this one
Each is checked against this paper’s own text: does it say what the citing paper says it does?
For catalysts producing CO (Au, Ag, etc.) or formate (Sn, Pb, etc.), elevated pressures do not greatly influence selectivity, but reduce cathodic overpotentials.
“For catalysts producing CO (Au, Ag, etc.) or formate (Sn, Pb, etc.), elevated pressures do not greatly influence selectivity, [139,143,202,220,221,[223][224][225][226] but reduce cathodic overpotentials.[131,143,221,224,225]”
From Electrochemical CO <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [143]
Some catalysts (Fe, Co, Rh, Ni, Pd, Pt, and C) with predominantly H2 selectivity at 1 atm can generate CO or HCOOH when pressurized.
“In addition, some catalysts (Fe, Co, Rh, Ni, Pd, Pt, and C) with predominantly H2 selectivity at 1 atm can generate CO or HCOOH when pressurized.[140,141,143,223,[227][228][229]”
From Electrochemical CO <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [143]
Cites
Opportunities and challenges for a sustainable energy future
Chu, S., & Majumdar, A. (2012) · Nature · doi:10.1038/nature11475 · Cited by 12,550 · see citing works
Carbon dioxide in water and seawater: the solubility of a non-ideal gas
Weiss, R. F. (1974) · Marine Chemistry · doi:10.1016/0304-4203(74)90015-2 · Cited by 3,373 · see citing works
A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels
Qiao, J., Liu, Y., Hong, F., & Zhang, J. (2014) · Chem. Soc. Rev. · doi:10.1039/c3cs60323g · Cited by 2,990 · see citing works
Hori, Y., Wakebe, H., Tsukamoto, T., & Koga, O. (1994) · Electrochimica Acta · doi:10.1016/0013-4686(94)85172-7 · Cited by 2,140 · see citing works
Electrochemical CO2 Reduction on Metal Electrodes
Hori, Y. (2008) · Springer eBooks · doi:10.1007/978-0-387-49489-0_3 · Cited by 1,904 · see citing works
Aqueous CO 2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles
Chen, Y., Li, C. W., & Kanan, M. W. (2012) · Journal of the American Chemical Society · doi:10.1021/ja309317u · Cited by 1,661 · see citing works
Ionic Liquid–Mediated Selective Conversion of CO <sub>2</sub> to CO at Low Overpotentials
Rosen, B. A., Salehi-Khojin, A., Thorson, M. R., Zhu, W., Whipple, D. T., Kenis, P. J. A., & Masel, R. I. (2011) · Science · doi:10.1126/science.1209786 · Cited by 1,558 · see citing works
Self-citationA selective and efficient electrocatalyst for carbon dioxide reduction
Lu, Q., Rosen, J., Zhou, Y., Hutchings, G. S., Kimmel, Y. C., Chen, J. G., & Jiao, F. (2014) · Nature Communications · doi:10.1038/ncomms4242 · Cited by 1,474 · see citing works
Monodisperse Au Nanoparticles for Selective Electrocatalytic Reduction of CO 2 to CO
Zhu, W., Michalsky, R., Metin, Ö., Lv, H., Guo, S., Wright, C. J., Sun, X., Peterson, A. A., & Sun, S. (2013) · Journal of the American Chemical Society · doi:10.1021/ja409445p · Cited by 1,379 · see citing works
Singh, M. R., Kwon, Y., Lum, Y., Ager, J. W., & Bell, A. T. (2016) · Journal of the American Chemical Society · doi:10.1021/jacs.6b07612 · Cited by 985 · see citing works
Theory of multiple proton–electron transfer reactions and its implications for electrocatalysis
Koper, M. T. M. (2013) · Chemical Science · doi:10.1039/c3sc50205h · Cited by 908 · see citing works
Kinetic Isotope Effects in the Study of Organometallic Reaction Mechanisms
Gómez‐Gallego, M., & Sierra, M. Á. (2011) · Chemical Reviews · doi:10.1021/cr100436k · Cited by 842 · see citing works
Jhong, H. “., Ma, S., & Kenis, P. J. A. (2013) · Current Opinion in Chemical Engineering · doi:10.1016/j.coche.2013.03.005 · Cited by 824 · see citing works
Self-citationElectrochemical CO2 reduction: Electrocatalyst, reaction mechanism, and process engineering
Lu, Q., & Jiao, F. (2016) · Nano Energy · doi:10.1016/j.nanoen.2016.04.009 · Cited by 817 · see citing works
Mistry, H., Reske, R., Zeng, Z., Zhao, Z.-J., Greeley, J., Strasser, P., & Cuenya, B. R. (2014) · Journal of the American Chemical Society · doi:10.1021/ja508879j · Cited by 690 · see citing works
Hansen, J. E., Kharecha, P. A., Sato, M., Masson‐Delmotte, V., Ackerman, F., Beerling, D. J., Hearty, P. J., Hoegh‐Guldberg, O., Hsu, S.-L., Parmesan, C., et al. (2013) · PLoS ONE · doi:10.1371/journal.pone.0081648 · Cited by 676 · see citing works
Verma, S., Kim, B., Jhong, H. “., Ma, S., & Kenis, P. J. A. (2016) · ChemSusChem · doi:10.1002/cssc.201600394 · Cited by 655 · see citing works
Self-citationInsights into the electrocatalytic reduction of CO 2 on metallic silver surfaces
Hatsukade, T., Kuhl, K. P., Cave, E. R., Abram, D. N., & Jaramillo, T. F. (2014) · Physical Chemistry Chemical Physics · doi:10.1039/c4cp00692e · Cited by 576 · see citing works
Reduction potentials of CO2- and the alcohol radicals
Schwarz, H., & Dodson, R. W. (1989) · The Journal of Physical Chemistry · doi:10.1021/j100338a079 · Cited by 530 · see citing works
Ma, M., Trześniewski, B. J., Xie, J., & Smith, W. A. (2016) · Angewandte Chemie International Edition · doi:10.1002/anie.201604654 · Cited by 530 · see citing works
Verma, S., Lu, X., Ma, S., Masel, R. I., & Kenis, P. J. A. (2016) · Physical Chemistry Chemical Physics · doi:10.1039/c5cp05665a · Cited by 497 · see citing works
Self-citationNanoparticle Silver Catalysts That Show Enhanced Activity for Carbon Dioxide Electrolysis
Salehi‐Khojin, A., Jhong, H. “., Rosen, B. A., Zhu, W. D., Ma, S., Kenis, P. J. A., & Masel, R. I. (2012) · The Journal of Physical Chemistry C · doi:10.1021/jp310509z · Cited by 432 · see citing works
Self-citationCao, Z. M., Kim, D., Hong, D., Yu, Y., Xu, J., Lin, S., Wen, X., Nichols, E. M., Jeong, K., Reimer, J. A., et al. (2016) · Journal of the American Chemical Society · doi:10.1021/jacs.6b02878 · Cited by 430 · see citing works
Inhibited proton transfer enhances Au-catalyzed CO 2 -to-fuels selectivity
Wuttig, A., Yaguchi, M., Motobayashi, K., Osawa, M., & Surendranath, Y. (2016) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1602984113 · Cited by 416 · see citing works
Continuous-flow electroreduction of carbon dioxide
Endrődi, B., Bencsik, G., Darvas, F., Jones, R. V., Rajeshwar, K., & Janáky, C. (2017) · Progress in Energy and Combustion Science · doi:10.1016/j.pecs.2017.05.005 · Cited by 383 · see citing works
Microfluidic Reactor for the Electrochemical Reduction of Carbon Dioxide: The Effect of pH
Whipple, D. T., Finke, E. C., & Kenis, P. J. A. (2010) · Electrochemical and Solid-State Letters · doi:10.1149/1.3456590 · Cited by 375 · see citing works
Self-citationHernández, S., Farkhondehfal, M. A., Sastre, F., Makkee, M., Saracco, G., & Russo, N. (2017) · Green Chemistry · doi:10.1039/c7gc00398f · Cited by 372 · see citing works
Martín, A. J., Larrazábal, G. O., & Pérez‐Ramírez, J. (2015) · Green Chemistry · doi:10.1039/c5gc01893e · Cited by 361 · see citing works
Effect of Cations on the Electrochemical Conversion of CO2to CO
Thorson, M. R., Siil, K. I., & Kenis, P. J. A. (2012) · Journal of The Electrochemical Society · doi:10.1149/2.052301jes · Cited by 354 · see citing works
Self-citationA general framework for the assessment of solar fuel technologies
Herron, J. A., Kim, J., Upadhye, A. A., Huber, G. W., & Maravelias, C. T. (2014) · Energy & Environmental Science · doi:10.1039/c4ee01958j · Cited by 350 · see citing works
New trends in the development of heterogeneous catalysts for electrochemical CO 2 reduction
Kumar, B., Brian, J. P., Atla, V., Kumari, S., Bertram, K. A., White, R. T., & Spurgeon, J. M. (2016) · Catalysis Today · doi:10.1016/j.cattod.2016.02.006 · Cited by 313 · see citing works
Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels
Yoon, Y., Hall, A. S., & Surendranath, Y. (2016) · Angewandte Chemie International Edition · doi:10.1002/anie.201607942 · Cited by 310 · see citing works
Comprehensive Treatise of Electrochemistry
Bockris, J. O., Conway, B. E., Yeager, E. B., et al. (1981) · Springer eBooks · doi:10.1007/978-1-4615-6687-8 · Cited by 303 · see citing works
The Effects of Catalyst Layer Deposition Methodology on Electrode Performance
Jhong, H. “., Brushett, F. R., & Kenis, P. J. A. (2013) · Advanced Energy Materials · doi:10.1002/aenm.201200759 · Cited by 244 · see citing works
Self-citationKim, B., Ma, S., Molly Jhong, H.-R., & Kenis, P. J. A. (2015) · Electrochimica Acta · doi:10.1016/j.electacta.2015.03.064 · Cited by 243 · see citing works
Self-citationSilver Supported on Titania as an Active Catalyst for Electrochemical Carbon Dioxide Reduction
Ma, S., Lan, Y., Perez, G. M. J., Moniri, S., & Kenis, P. J. A. (2014) · ChemSusChem · doi:10.1002/cssc.201300934 · Cited by 222 · see citing works
Self-citationMa, S., Luo, R., Gold, J. I., Yu, A. Z., Kim, B., & Kenis, P. J. A. (2016) · Journal of Materials Chemistry A · doi:10.1039/c6ta00427j · Cited by 209 · see citing works
Self-citationModern Aspects Of Electrochemistry
Vayenas, C. G. (2007) · Modern aspects of electrochemistry · doi:10.1007/978-0-387-46108-3 · Cited by 199 · see citing works
Barriers of Electrochemical CO2 Reduction on Transition Metals
Shi, C., Chan, K., Yoo, J. S., & Nørskov, J. K. (2016) · Organic Process Research & Development · doi:10.1021/acs.oprd.6b00103 · Cited by 186 · see citing works
Fuel Cell Electrocatalyst Using Polybenzimidazole‐Modified Carbon Nanotubes As Support Materials
Fujigaya, T., & Nakashima, N. (2013) · Advanced Materials · doi:10.1002/adma.201204461 · Cited by 176 · see citing works
Self-citationCarbon Sequestration for Climate Change Mitigation and Adaptation
Ussiri, D. A. N., & Lal, R. (2017) · Springer eBooks · doi:10.1007/978-3-319-53845-7 · Cited by 118 · see citing works
Chandrasekaran, K., & Bockris, L. O. (1987) · Surface Science · doi:10.1016/s0039-6028(87)80173-5 · Cited by 116 · see citing works
Observation of an Inverse Kinetic Isotope Effect in Oxygen Evolution Electrochemistry
Tse, E. C. M., Hoang, T. T. H., Varnell, J. A., & Gewirth, A. A. (2016) · ACS Catalysis · doi:10.1021/acscatal.6b01170 · Cited by 101 · see citing works
Self-citationKatsounaros, I., Chen, T., Gewirth, A. A., Marković, N. M., & Koper, M. T. M. (2016) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.5b02556 · Cited by 93 · see citing works
Self-citationEfficient Electrochemical Flow System with Improved Anode for the Conversion of CO2to CO
Ma, S., Luo, R., Moniri, S., Lan, Y., & Kenis, P. J. A. (2014) · Journal of The Electrochemical Society · doi:10.1149/2.1201410jes · Cited by 86 · see citing works
Self-citationJhong, H. “., Tornow, C. E., Kim, C., Verma, S., Oberst, J. L., Anderson, P. S., Gewirth, A. A., Fujigaya, T., Nakashima, N., & Kenis, P. J. A. (2017) · ChemPhysChem · doi:10.1002/cphc.201700815 · Cited by 70 · see citing works
Self-citationHafez, I. H., Berber, M. R., Fujigaya, T., & Nakashima, N. (2014) · Scientific Reports · doi:10.1038/srep06295 · Cited by 59 · see citing works
Self-citationHuan, T. N., Prakash, P., Simon, P., Rousse, G., Xu, X., Artero, V., Gravel, E., Doris, E., & Fontecave, M. (2016) · ChemSusChem · doi:10.1002/cssc.201600597 · Cited by 55 · see citing works
Studies on the Hydrogen Evolution Reaction Down to —150°C and the Role of Proton Tunneling
Conway, B. E., & Salomon, M. (1964) · The Journal of Chemical Physics · doi:10.1063/1.1725692 · Cited by 55 · see citing works
Kinetic isotope effect in the hydrogen evolution reaction
Krishtalik, L. I. (2001) · Electrochimica Acta · doi:10.1016/s0013-4686(01)00526-6 · Cited by 49 · see citing works
Fujigaya, T., Kim, C., Hamasaki, Y., et al. (2016) · Scientific Reports · doi:10.1038/srep21314 · Cited by 42 · see citing works
Self-citationIntroduction to Global Carbon Cycling: An Overview of the Global Carbon Cycle
Ussiri, D. A. N., & Lal, R. (2017) · Springer eBooks · doi:10.1007/978-3-319-53845-7_3 · Cited by 15 · see citing works
Flagged first, then by citations
Cited by
Sorted by citations
What would it take for renewably powered electrosynthesis to displace petrochemical processes?
De Luna, P., Hahn, C., Higgins, D., Jaffer, S. A., Jaramillo, T. F., & Sargent, E. H. (2019) · Science · doi:10.1126/science.aav3506 · Cited by 3,052 · see citing works
CO <sub>2</sub> electrolysis to multicarbon products in strong acid
Huang, J. E., Li, F., Ozden, A., Sedighian Rasouli, A., García de Arquer, F. P., Liu, S., Zhang, S., Luo, M., Wang, X., Lum, Y., et al. (2021) · Science · doi:10.1126/science.abg6582 · Cited by 1,359 · see citing works
Kibria, M. G., Edwards, J. P., Gabardo, C. M., Dinh, C., Seifitokaldani, A., Sinton, D., & Sargent, E. H. (2019) · Advanced Materials · doi:10.1002/adma.201807166 · Cited by 1,331 · see citing works
Designing materials for electrochemical carbon dioxide recycling
Ross, M. B., De Luna, P., Li, Y., Dinh, C.-T., Kim, D., Yang, P., & Sargent, E. H. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0306-7 · Cited by 1,302 · see citing works
Electrocatalysis for CO <sub>2</sub> conversion: from fundamentals to value-added products
Wang, G., Chen, J., Ding, Y., Cai, P., Yi, L., Li, Y., Tu, C., Hou, Y., Wen, Z., & Dai, L. (2021) · Chemical Society Reviews · doi:10.1039/d0cs00071j · Cited by 1,295 · see citing works
Xia, C., Zhu, P., Jiang, Q., Pan, Y., Liang, W., Stavitski, E., Alshareef, H. N., & Wang, H. (2019) · Nature Energy · doi:10.1038/s41560-019-0451-x · Cited by 782 · see citing works
Wen, G., Ren, B., Park, M. G., Yang, J., Dou, H., Zhang, Z., Deng, Y., Bai, Z., Yang, L., Gostick, J., et al. (2020) · Angewandte Chemie International Edition · doi:10.1002/anie.202004149 · Cited by 97 · see citing works
- Authors
- Verma, S., Hamasaki, Y., Kim, C., Huang, W., Lu, S., Jhong, H.-R. M., Gewirth, A. A., Fujigaya, T., Nakashima, N., & Kenis, P. J. A.
- Affiliations
- Kyushu University (JP)
- University of Illinois Urbana-Champaign (US)
- Corresponding author
- Fujigaya, Tsuyohiko
- Nakashima, Naotoshi
- Kenis, Paul J. A.
- ORCID
- Venue
- ACS Energy Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-12-18
- Volume
- 3
- Issue
- 1
- Pages
- 193-198
- ISSN
- 2380-8195 (ISSN-L)
- OpenAlex
- W2776913936
- Cited by
- 521
- References
- 52
- Citations by year
- 2026: 44 · 2025: 44 · 2024: 56 · 2023: 69 · 2022: 76 · 2021: 83 · 2020: 71 · 2019: 61 · 2018: 17
- FWCI
- 10.90
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- ACS Energy Letters (publishedVersion)
- Funders
- Ministry of Education, Culture, Sports, Science and Technology
- Dow Chemical Company
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
- Keywords
- electrochemical CO2 reduction, co-production, supported gold catalysts, low overpotential, kinetic isotope effects, Tafel slope, rate-determining step, electron transfer, energy efficiency, electrocatalyst stability
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
