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Nanoporous Gold as a Highly Selective and Active Carbon Dioxide Reduction Catalyst

Welch, Alex J. and DuChene, Joseph S. and Tagliabue, Giulia and Davoyan, Artur and Cheng, Wen-Hui and Atwater, Harry A. (2019) Nanoporous Gold as a Highly Selective and Active Carbon Dioxide Reduction Catalyst. ACS Applied Energy Materials, 2 (1). pp. 164-170. ISSN 2574-0962. http://resolver.caltech.edu/CaltechAUTHORS:20190102-092234188

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Abstract

Electrochemical conversion of CO_2 into useful chemicals is a promising approach for transforming CO_2 into sustainably produced fuels and/or chemical feedstocks for industrial synthesis. We report that nanoporous gold (np-Au) films, with pore sizes ranging from 10 to 30 nm, represent promising electrocatalytic architectures for the CO_2 reduction reaction (CO_2RR) due to their large electrochemically active surface area, relative abundance of grain boundaries, and ability to support pH gradients inside the nanoporous network. Electrochemical studies show that np-Au films support partial current densities for the conversion of CO_2 to CO in excess of 6 mA cm^(–2) at a Faradaic efficiency of ∼99% in aqueous electrolytes (50 mM K_2CO_3 saturated with CO_2). Moreover, np-Au films are able to maintain Faradaic efficiency greater than 80% for CO production over prolonged periods of continuous operation (110 h). Electrocatalytic experiments at different electrolyte concentrations demonstrate that the pore diameter of nanoporous cathodes represents a critical parameter for creating and controlling local pH gradients inside the porous network of metal ligaments. These results demonstrate the merits of nanoporous metal films for the CO_2RR and offer an interesting architecture for highly selective electrocatalysis capable of sustaining high catalytic currents over prolonged periods.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsaem.8b01570DOIArticle
https://pubs.acs.org/doi/suppl/10.1021/acsaem.8b01570PublisherSupporting Information
ORCID:
AuthorORCID
DuChene, Joseph S.0000-0002-7145-323X
Tagliabue, Giulia0000-0003-4587-728X
Cheng, Wen-Hui0000-0003-3233-4606
Atwater, Harry A.0000-0001-9435-0201
Additional Information:© 2018 American Chemical Society. This article is made available for a limited time sponsored by ACS under the ACS Free to Read License, which permits copying and redistribution of the article for non-commercial scholarly purposes. Received: September 17, 2018; Accepted: December 26, 2018; Published: December 26, 2018. This work is done within the Joint Center for Artificial Photosynthesis, a Department of Energy (DOE) Energy Innovation Hub, supported through the Office of Science of the U.S. Department of energy under Award Number De-SC0004993. A.J.W. acknowledges support from the National Science Foundation (NSF) Graduate Research Fellowship Program under Base Award No. 1745301. G.T. acknowledges support from the Swiss National Science Foundation through the Advanced Mobility Fellowship, grant n. P300P2_171417. We gratefully acknowledge critical support and infrastructure provided for this work by the Kavli Nanoscience Institute at Caltech. We thank Matthew S. Hunt of the Kavli Nanoscience Institute at Caltech for assistance with SEM, He FIB, and TEM imaging of nanoporous Au films. Any opinions, findings, and conclusions expressed in this material are those of the authors and do not necessary reflect those of DOE or NSF. Author Contributions: A.J.W., J.S.D., G.T., and H.A.A. conceived of the experimental study. A.J.W. and J.S.D. executed all electrochemical experiments and performed the data analysis. W.-H.C. assisted with gas chromatography and high-pressure liquid chromatography. A.J.W., J.S.D., and H.A.A. wrote the paper, and all authors commented on the manuscript. The authors declare no competing financial interest.
Group:JCAP, Kavli Nanoscience Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
NSF Graduate Research FellowshipDGE-1745301
Swiss National Science Foundation (SNSF)P300P2_171417
Subject Keywords:CO_2 reduction, nanoporous cathode, pH gradient, grain boundaries, electrocatalysis
Record Number:CaltechAUTHORS:20190102-092234188
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20190102-092234188
Official Citation:Nanoporous Gold as a Highly Selective and Active Carbon Dioxide Reduction Catalyst. Alex J. Welch, Joseph S. DuChene, Giulia Tagliabue, Artur Davoyan, Wen-Hui Cheng, and Harry A. Atwater. ACS Applied Energy Materials 2019 2 (1), 164-170. DOI: 10.1021/acsaem.8b01570
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:91979
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:02 Jan 2019 18:49
Last Modified:29 Jan 2019 17:52

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