An in-situ electrochemical IR investigation of solution CO electro-oxidation on a polycrystalline Au surface in an alkaline electrolyte: Identification of active reaction intermediates
Abstract
Here we report an in-situ electrochemical surface enhanced IR reflection absorption spectroscopic (SEIRAS) study of carbon monoxide electro-oxidation reaction (COR) of CO dissolved in alkaline supporting electrolyte (COsol). With judiciously chosen concentration of OH-, we were able to observe for the first time the vibrational band of the weakly adsorbed COw in an alkaline solution and identify it as the active reaction intermediate for the COR of COsol, as in the acidic media. With the help of deuterium labeling, we were also able to confirm spectroscopically, again for the first time, the previously proposed CO-adsorption-promoted-OH-adsorption hypothesis. We proposed a reaction mechanism accordingly that consists of (1) CO-adsorption-promoted OH adsorption, (2) formation of weakly-bound COw from COsol, and (3) the oxidation of COw by a surface-anchored weakly-hydrogen-bound species. We believe that the synergistic actions of these elemental chemical processes are the reasons for the observed unusually high activity of COR of COsol in an alkaline solution.
- Authors:
-
- Georgetown University, Washington, DC (United States)
- Publication Date:
- Research Org.:
- Georgetown Univ., Washington, DC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1533978
- Alternate Identifier(s):
- OSTI ID: 1550515
- Grant/Contract Number:
- FG02-07ER15895
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Electroanalytical Chemistry
- Additional Journal Information:
- Journal Volume: 800; Journal Issue: C; Journal ID: ISSN 1572-6657
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon monoxide electro-oxidation reaction; in situ SEIRAS; weakly-bound CO; CO-adsorption-promoted OH adsorption; alkaline solution
Citation Formats
Chen, De-Jun, and Tong, YuYe J. An in-situ electrochemical IR investigation of solution CO electro-oxidation on a polycrystalline Au surface in an alkaline electrolyte: Identification of active reaction intermediates. United States: N. p., 2017.
Web. doi:10.1016/j.jelechem.2017.04.045.
Chen, De-Jun, & Tong, YuYe J. An in-situ electrochemical IR investigation of solution CO electro-oxidation on a polycrystalline Au surface in an alkaline electrolyte: Identification of active reaction intermediates. United States. https://doi.org/10.1016/j.jelechem.2017.04.045
Chen, De-Jun, and Tong, YuYe J. Wed .
"An in-situ electrochemical IR investigation of solution CO electro-oxidation on a polycrystalline Au surface in an alkaline electrolyte: Identification of active reaction intermediates". United States. https://doi.org/10.1016/j.jelechem.2017.04.045. https://www.osti.gov/servlets/purl/1533978.
@article{osti_1533978,
title = {An in-situ electrochemical IR investigation of solution CO electro-oxidation on a polycrystalline Au surface in an alkaline electrolyte: Identification of active reaction intermediates},
author = {Chen, De-Jun and Tong, YuYe J.},
abstractNote = {Here we report an in-situ electrochemical surface enhanced IR reflection absorption spectroscopic (SEIRAS) study of carbon monoxide electro-oxidation reaction (COR) of CO dissolved in alkaline supporting electrolyte (COsol). With judiciously chosen concentration of OH-, we were able to observe for the first time the vibrational band of the weakly adsorbed COw in an alkaline solution and identify it as the active reaction intermediate for the COR of COsol, as in the acidic media. With the help of deuterium labeling, we were also able to confirm spectroscopically, again for the first time, the previously proposed CO-adsorption-promoted-OH-adsorption hypothesis. We proposed a reaction mechanism accordingly that consists of (1) CO-adsorption-promoted OH adsorption, (2) formation of weakly-bound COw from COsol, and (3) the oxidation of COw by a surface-anchored weakly-hydrogen-bound species. We believe that the synergistic actions of these elemental chemical processes are the reasons for the observed unusually high activity of COR of COsol in an alkaline solution.},
doi = {10.1016/j.jelechem.2017.04.045},
journal = {Journal of Electroanalytical Chemistry},
number = C,
volume = 800,
place = {United States},
year = {Wed Apr 26 00:00:00 EDT 2017},
month = {Wed Apr 26 00:00:00 EDT 2017}
}
Web of Science
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