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Tracking the Prelude of the Electroreduction of Carbon Monoxide Via its Interaction With Cu(100): Studies by Operando Scanning Tunneling Microscopy and Infrared Spectroscopy

Baricuatro, Jack H. and Kim, Youn-Geun and Korzeniewski, Carol L. and Soriaga, Manuel P. (2020) Tracking the Prelude of the Electroreduction of Carbon Monoxide Via its Interaction With Cu(100): Studies by Operando Scanning Tunneling Microscopy and Infrared Spectroscopy. Catalysis Today . ISSN 0920-5861. (In Press) https://resolver.caltech.edu/CaltechAUTHORS:20200124-132304036

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Abstract

The first isolable intermediate in the electrochemical reduction of carbon dioxide is carbon monoxide. This species, or its hydrated form, formic acid, is also the primary end product from all but a handful of metallic electrodes; with the latter, hydrogen gas is generated, but it emanates from the reduction of water and not from CO₂. Only one electrode material, zerovalent copper, can spawn, in greater-than-trace quantities, a variety of species that are more highly reduced than CO. Hence, if the aim is to extract a reaction trail of the reduction of CO₂ to products other than CO, it would be both logical and expedient to track the electrocatalytic reaction of CO itself. Heterogeneous electrocatalysis is a surface phenomenon; it transpires only when the reactant, CO in this case, chemisorbs on, or chemically interacts with, the Cu electrode surface. There is no electrocatalytic reaction if there is no CO adsorption. In ultrahigh vacuum, no CO resides on the Cu(100) surface at temperatures higher than 200 K. However, under electrochemical conditions, CO is chemisorbed on Cu at ambient temperatures at a given potential. We thus paired, in seriatim fashion, scanning tunneling microscopy (STM) and polarization-modulation IR reflection-absorption spectroscopy (PMIRS) to document the influence of applied potential on the coverage, the molecular orientation, and the adlattice structure of CO adsorbed on Cu(100) in alkaline solutions; the results are described in this paper.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.cattod.2020.01.028DOIArticle
ORCID:
AuthorORCID
Kim, Youn-Geun0000-0002-5936-6520
Soriaga, Manuel P.0000-0002-0077-6226
Additional Information:© 2020 Published by Elsevier B.V. Received 11 March 2019, Revised 21 January 2020, Accepted 23 January 2020, Available online 24 January 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 No. DE-SC0004993.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Subject Keywords:Seriatim STM-PMIRS; Operando electrode-surface microscopy; Operando molecular vibrational spectroscopy; Potential-dependent CO adsorption on Cu(100)
Record Number:CaltechAUTHORS:20200124-132304036
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200124-132304036
Official Citation:Jack H. Baricuatro, Youn-Geun Kim, Carol L. Korzeniewski, Manuel P. Soriaga, Tracking the Prelude of the Electroreduction of Carbon Monoxide Via its Interaction With Cu(100): Studies by Operando Scanning Tunneling Microscopy and Infrared Spectroscopy, Catalysis Today, 2020, ISSN 0920-5861, https://doi.org/10.1016/j.cattod.2020.01.028. (http://www.sciencedirect.com/science/article/pii/S0920586120300328)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100901
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:25 Jan 2020 03:35
Last Modified:25 Jan 2020 03:35

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