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Reprint of "Selective conversion of CO into ethanol on Cu(511) surface reconstructed from Cu(pc): Operando studies by electrochemical scanning tunneling microscopy, mass spectrometry, quartz crystal nanobalance, and infrared spectroscopy"

Baricuatro, Jack H. and Kim, Youn-Geun and Tsang, Chu F. and Javier, Alnald C. and Cummins, Kyle D. and Hemminger, John C. (2020) Reprint of "Selective conversion of CO into ethanol on Cu(511) surface reconstructed from Cu(pc): Operando studies by electrochemical scanning tunneling microscopy, mass spectrometry, quartz crystal nanobalance, and infrared spectroscopy". Journal of Electroanalytical Chemistry, 875 . Art. No. 114757. ISSN 1572-6657. doi:10.1016/j.jelechem.2020.114757. https://resolver.caltech.edu/CaltechAUTHORS:20201013-154709745

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Abstract

A polycrystalline copper, surface-terminated by a well-defined (511)-oriented facet, was electrochemically generated by a series of step-wise surface reconstruction and iterations of mild oxidative-reductive processes in 0.1 M KOH. The electrochemical reduction of CO on the resultant stepped surface was investigated by four surface-sensitive operando methodologies: electrochemical scanning tunneling microscopy (STM), electrochemical quartz crystal nanobalance (EQCN), differential electrochemical mass spectrometry (DEMS), and polarization-modulation infrared spectroscopy (PMIRS). The stepped surface catalyzed the facile conversion of CO into ethanol, the exclusive alcohol product at a low overpotential of −1.06 V (SHE) or − 0.3 V (RHE). The chemisorption of CO was found to be a necessary prelude to ethanol production; i.e. the surface coverages, rather than solution concentrations, of CO and its surface-bound intermediates primarily dictate the reaction rates (current densities). Contrary to the expected predominance of undercoordinated step-site reactivity over the coordination chemistry of vicinal surfaces, vibrational spectroscopic evidence reveals the involvement of terrace-bound CO adsorbates during the multi-atomic transformations associated with the production of ethanol.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.jelechem.2020.114757DOIReprint
https://resolver.caltech.edu/CaltechAUTHORS:20191202-112107473Related ItemOriginal Article
ORCID:
AuthorORCID
Kim, Youn-Geun0000-0002-5936-6520
Javier, Alnald C.0000-0002-0306-5462
Hemminger, John C.0000-0003-2467-6630
Additional Information:© 2019 Elsevier B.V. Received 30 September 2019, Revised 20 November 2019, Accepted 26 November 2019, Available online 13 October 2020. A publisher's error resulted in this article appearing in the wrong issue. The article is reprinted here for the reader's convenience and for the continuity of the special issue. For citation purposes, please use the original publication details; Volume 857, 15 January 2020, 113704, DOI of original item: 10.1016/j.jelechem.2019.113704. 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. Authors contributions: J.H.B., Y.-G.K., C.F.T., A.C.J., K.D.C. and J.C.H. designed research. J.H.B., Y.-G.K., C.F.T., A.C.J., performed research. J.H.B., Y.-G.K., C.F.T., A.C.J., K.D.C. and J.C.H. analyzed data. J.H.B. wrote the paper. Declaration of interest: None.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Subject Keywords:Electrochemically generated Cu(511) surface; Operando electrode-surface microscopy; Operando molecular vibrational spectroscopy; CO adsorption on Cu vicinal surface; Selective reduction of CO into ethanol
DOI:10.1016/j.jelechem.2020.114757
Record Number:CaltechAUTHORS:20201013-154709745
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20201013-154709745
Official Citation:Jack H. Baricuatro, Youn-Geun Kim, Chu F. Tsang, Alnald C. Javier, Kyle D. Cummins, John C. Hemminger, Reprint of "Selective conversion of CO into ethanol on Cu(511) surface reconstructed from Cu(pc): Operando studies by electrochemical scanning tunneling microscopy, mass spectrometry, quartz crystal nanobalance, and infrared spectroscopy", Journal of Electroanalytical Chemistry, Volume 875, 2020, 114757, ISSN 1572-6657, https://doi.org/10.1016/j.jelechem.2020.114757. (http://www.sciencedirect.com/science/article/pii/S1572665720309851)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:106046
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:14 Oct 2020 15:49
Last Modified:16 Nov 2021 18:49

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