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Effects of Surface Roughness on the Electrochemical Reduction of CO₂ over Cu

Jiang, Kun and Huang, Yufeng and Zeng, Guosong and Toma, Francesca M. and Goddard, William A., III and Bell, Alexis T. (2020) Effects of Surface Roughness on the Electrochemical Reduction of CO₂ over Cu. ACS Energy Letters, 5 (4). pp. 1206-1214. ISSN 2380-8195. https://resolver.caltech.edu/CaltechAUTHORS:20200319-124814828

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Abstract

We have investigated the role of surface roughening on the CO₂ reduction reaction (CO₂RR) over Cu. The activity and product selectivity of Cu surfaces roughened by plasma pretreatment in Ar, O₂, or N₂ were compared with that of electrochemically polished Cu samples. Differences in total and product current densities, the ratio of current densities for HER (the hydrogen evolution reaction) to CO₂RR, and the ratio of current densities for C₂₊ to C₁ products depend on the electrochemically active surface and are nearly independent of plasma composition. Theoretical analysis of an electropolished and roughened Cu surface reveals a higher fraction of undercoordinated Cu sites on the roughened surface, sites that bind CO preferentially. Roughened surfaces also contain square sites similar to those on a Cu(100) surface but with neighboring step sites, which adsorb OC–COH, a precursor to C₂₊ products. These findings explain the increases in the formation of oxygenates and hydrocarbons relative to CO and the ratio of oxygenates to hydrocarbons observed with increasing surface roughness.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsenergylett.0c00482DOIArticle
ORCID:
AuthorORCID
Jiang, Kun0000-0003-3148-5058
Huang, Yufeng0000-0002-0373-2210
Toma, Francesca M.0000-0003-2332-0798
Goddard, William A., III0000-0003-0097-5716
Bell, Alexis T.0000-0002-5738-4645
Additional Information:© 2020 American Chemical Society. Received: February 29, 2020; Accepted: March 19, 2020; Published: March 19, 2020. 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. K.J. acknowledges the startup funding from Shanghai Jiao Tong University. We also acknowledge Ms. Lien-Chun Weng, Dr. Zhou Lin, and Prof. Martin Head-Gordon for insightful discussions. Author Contributions: K.J. and Y.H. contributed equally to this work. The authors declare no competing financial interest.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Shanghai Jiao Tong UniversityUNSPECIFIED
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1373
Issue or Number:4
Record Number:CaltechAUTHORS:20200319-124814828
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200319-124814828
Official Citation:Effects of Surface Roughness on the Electrochemical Reduction of CO2 over Cu. Kun Jiang, Yufeng Huang, Guosong Zeng, Francesca M. Toma, William A. Goddard, III, and Alexis T. Bell. ACS Energy Letters 2020 5 (4), 1206-1214; DOI: 10.1021/acsenergylett.0c00482
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:101999
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:19 Mar 2020 19:58
Last Modified:11 Jul 2020 09:07

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