CaltechAUTHORS
  A Caltech Library Service

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) 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, 857 . Art. No. 113704. ISSN 1572-6657. https://resolver.caltech.edu/CaltechAUTHORS:20191202-112107473

[img] PDF - Accepted Version
See Usage Policy.

4039Kb

Use this Persistent URL to link to this item: https://resolver.caltech.edu/CaltechAUTHORS:20191202-112107473

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.2019.113704DOIArticle
ORCID:
AuthorORCID
Kim, Youn-Geun0000-0002-5936-6520
Additional Information:© 2019 Published by Elsevier B.V. Received 30 September 2019, Revised 20 November 2019, Accepted 26 November 2019, Available online 28 November 2019. 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
Record Number:CaltechAUTHORS:20191202-112107473
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20191202-112107473
Official Citation:Jack H. Baricuatro, Youn-Geun Kim, Chu F. Tsang, Alnald C. Javier, Kyle D. Cummins, John C. Hemminger, 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 857, 2020, 113704, ISSN 1572-6657, https://doi.org/10.1016/j.jelechem.2019.113704. (http://www.sciencedirect.com/science/article/pii/S1572665719309725)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100139
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:02 Dec 2019 20:21
Last Modified:11 Feb 2020 23:55

Repository Staff Only: item control page