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Regulating the Product Distribution of CO Reduction by the Atomic-Level Structural Modification of the Cu Electrode Surface

Kim, Youn-Geun and Javier, Alnald and Baricuatro, Jack H. and Soriaga, Manuel P. (2016) Regulating the Product Distribution of CO Reduction by the Atomic-Level Structural Modification of the Cu Electrode Surface. Electrocatalysis, 7 (5). pp. 391-399. ISSN 1868-2529. https://resolver.caltech.edu/CaltechAUTHORS:20160620-134104006

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Abstract

Cu catalyzes the electrochemical reduction of CO_2 or CO to an assortment of products, a behavior that is a detriment when only one reduced compound is desired. The present article provides an example in which, through the atomic-level control of the structure of the Cu electrode surface, the yield distribution is regulated to generate only one product. The reaction investigated was the preferential reduction of CO to C_2H_5OH on Cu at a low overpotential in alkaline solution. Experimental measurements combined electrochemical scanning tunneling microscopy (ECSTM) and differential electrochemical mass spectrometry (DEMS). An atomically ordered Cu(100) surface, prepared from either a single crystal or by Cu(pc)-to-Cu(100) reconstruction, did not produce ethanol. When the surfaces were subjected to monolayer-limited Cu↔Cu_2O cycles, only the reconstructed surface underwent an additional structural transformation that spawned the selective production of ethanol at a potential 645 mV lower than that which generates multiple products. Quasi-operando ECSTM indicated transformation to an ordered stepped surface, Cu(S) − [3(100) × (111)], or Cu(511). The non-selective, multiple-product Cu-catalyzed reduction of CO had thus been regulated to yield only one liquid fuel by an atomic-level structural modification of the electrode surface.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1007/s12678-016-0314-1DOIArticle
http://link.springer.com/article/10.1007%2Fs12678-016-0314-1PublisherArticle
http://rdcu.be/raUlPublisherFree ReadCube access
ORCID:
AuthorORCID
Kim, Youn-Geun0000-0002-5936-6520
Javier, Alnald0000-0002-0306-5462
Soriaga, Manuel P.0000-0002-0077-6226
Additional Information:© 2016 Springer Science+Business Media New York. Published online: 7 June 2016. 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 No. DE-SC0004993.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Subject Keywords:Selective reduction of CO to ethanol on Cu(511) in alkaline solution at low overpotential; Operando generation of Cu(511) electrode surface from polycrystalline Cu; Operando electrochemical scanning tunneling microscopy (OECSTM); Differential electrochemical mass spectrometry (DEMS); Seriatim OECSTM-DEMS
Issue or Number:5
Record Number:CaltechAUTHORS:20160620-134104006
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20160620-134104006
Official Citation:Kim, YG., Javier, A., Baricuatro, J.H. et al. Electrocatalysis (2016) 7: 391. doi:10.1007/s12678-016-0314-1
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:68537
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:21 Jun 2016 23:51
Last Modified:09 Mar 2020 13:18

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