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Designing a Zn–Ag Catalyst Matrix and Electrolyzer System for CO₂ Conversion to CO and Beyond

Lamaison, Sarah and Wakerley, David and Kracke, Frauke and Moore, Thomas and Zhou, Lan and Lee, Dong Un and Wang, Lei and Hubert, McKenzie A. and Aviles Acosta, Jaime E. and Gregoire, John M. and Duoss, Eric B. and Baker, Sarah and Beck, Victor A. and Spormann, Alfred M. and Fontecave, Marc and Hahn, Christopher and Jaramillo, Thomas F. (2022) Designing a Zn–Ag Catalyst Matrix and Electrolyzer System for CO₂ Conversion to CO and Beyond. Advanced Materials, 34 (1). Art. No. 2103963. ISSN 0935-9648. doi:10.1002/adma.202103963.

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CO₂ emissions can be transformed into high-added-value commodities through CO₂ electrocatalysis; however, efficient low-cost electrocatalysts are needed for global scale-up. Inspired by other emerging technologies, the authors report the development of a gas diffusion electrode containing highly dispersed Ag sites in a low-cost Zn matrix. This catalyst shows unprecedented Ag mass activity for CO production: −614 mA cm⁻² at 0.17 mg of Ag. Subsequent electrolyte engineering demonstrates that halide anions can further improve stability and activity of the Zn–Ag catalyst, outperforming pure Ag and Au. Membrane electrode assemblies are constructed and coupled to a microbial process that converts the CO to acetate and ethanol. Combined, these concepts present pathways to design catalysts and systems for CO₂ conversion toward sought-after products.

Item Type:Article
Related URLs:
URLURL TypeDescription
Lee, Dong Un0000-0001-7591-5350
Hubert, McKenzie A.0000-0002-9987-0748
Gregoire, John M.0000-0002-2863-5265
Beck, Victor A.0000-0002-0625-9545
Spormann, Alfred M.0000-0001-5103-9704
Jaramillo, Thomas F.0000-0001-9900-0622
Alternate Title:Designing a Zn–Ag Catalyst Matrix and Electrolyzer System for CO2 Conversion to CO and Beyond
Additional Information:© 2021 Wiley-VCH GmbH. Issue Online: 07 January 2022; Version of Record online: 21 October 2021; Manuscript revised: 24 July 2021; Manuscript received: 25 May 2021. S.L. and D.W. contributed equally to this work. This research was supported by a cooperative research and development agreement with TOTAL American Services, Inc. (affiliate of TOTAL SE, France) and Department of Energy under agreement number TC02307. T.M., E.B.D., S.B., and V.B. contributed under the auspices of the US Department of Energy under Contract DE-AC52-07-NA27344 and were supported by the LLNL-LDRD program under project number 19-SI-005, LLNL Release Number LLNL-JRNL-817428. The synthesis and composition characterization of sputtered thin film electrodes carried out by L.Z. and J.M.G. was supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award Number DE-SC0004993. F.K. and A.S. were supported by the Global Climate and Energy Project. S.L. was funded by the Corps des Ponts, des Eaux et des Forêts (Division of the French Ministry of Ecological Transition). D.W. was supported by a Lindemann Trust Fellowship (English-Speaking Union, UK). The authors acknowledge assistance from Juliet Jamtgaard for assistance in acquiring XPS samples and Guangchao Li for carrying out ICP measurements. The authors would also like to thank Dr. Alessandro Gallo and Dr. Joel Sanchez for fruitful spectroscopy discussions. The authors declare no conflict of interest. Data Availability Statement: The data that supports the findings of this study are available in the Supporting Information of this article, and from the corresponding author upon reasonable request.
Funding AgencyGrant Number
TOTAL American Services, Inc.UNSPECIFIED
Department of Energy (DOE)TC02307
Department of Energy (DOE)DE-AC52-07-NA27344
Lawrence Livermore National Laboratory19-SI-005
Department of Energy (DOE)DE-SC0004993
Global Climate and Energy Project (GCEP)UNSPECIFIED
Ministry of Ecological Transition (France)UNSPECIFIED
Lindemann Trust FellowshipUNSPECIFIED
Subject Keywords:carbon dioxide conversion; carbon monoxide; gas diffusion electrodes; mass activities; membrane electrode assemblies; microbial coupling; multiphysics models
Issue or Number:1
Record Number:CaltechAUTHORS:20211130-202117453
Persistent URL:
Official Citation:Lamaison, S., Wakerley, D., Kracke, F., Moore, T., Zhou, L., Lee, D. U., Wang, L., Hubert, M. A., Aviles, J. E., Gregoire, J. M., Duoss, E. B., Baker, S., Beck, V. A., Spormann, A. M., Fontecave, M., Hahn, C., Jaramillo, T. F., Designing a Zn–Ag Catalyst Matrix and Electrolyzer System for CO2 Conversion to CO and Beyond. Adv. Mater. 2022, 34, 2103963.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:112091
Deposited By: Tony Diaz
Deposited On:30 Nov 2021 21:30
Last Modified:11 Jan 2022 19:01

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