Decomposition pathways of C2 oxygenates on Rh-modified tungsten carbide surfaces
Abstract
Ethanol decomposition on tungsten monocarbide (WC) and Rh-modified WC was investigated using ultrahigh vacuum (UHV) surface science experiments and density functional theory (DFT) calculations. DFT calculations indicated that the binding energies of ethanol and its decomposition intermediates on WC(0001) were modified by Rh, with Rh/WC(0001) showing similar values to those on Rh(111). Through temperature-programmed desorption (TPD) experiments on polycrystalline WC and Rh-modified WC, it was shown that the selectivity for ethanol decomposition was different on these surfaces. On WC, the C-O bond of ethanol was preferentially broken to produce ethylene; on Rh-modified WC, the C-C bond was broken to produce carbon monoxide and methane. In addition, high-resolution electron energy loss spectroscopy (HREELS) was used to determine likely surface intermediates. On Rh-modified WC, ethanol first formed ethoxy through O-H scission, then reacted through an aldehyde intermediate to form the C1 products.
- Authors:
-
- Univ. of Delaware, Newark, DE (United States)
- Columbia Univ., New York, NY (United States); Brookhaven National Lab., Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1224193
- Alternate Identifier(s):
- OSTI ID: 1244750
- Report Number(s):
- BNL-108465-2015-JA
Journal ID: ISSN 0039-6028; R&D Project: CO009; KC0302010
- Grant/Contract Number:
- SC00112704; 13-038
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Surface Science
- Additional Journal Information:
- Journal Volume: 640; Journal Issue: C; Journal ID: ISSN 0039-6028
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ethanol; acetaldehyde; tungsten carbide; Rh-modified tungsten carbide
Citation Formats
Kelly, Thomas G., Ren, Hui, and Chen, Jingguang G. Decomposition pathways of C2 oxygenates on Rh-modified tungsten carbide surfaces. United States: N. p., 2015.
Web. doi:10.1016/j.susc.2015.03.008.
Kelly, Thomas G., Ren, Hui, & Chen, Jingguang G. Decomposition pathways of C2 oxygenates on Rh-modified tungsten carbide surfaces. United States. https://doi.org/10.1016/j.susc.2015.03.008
Kelly, Thomas G., Ren, Hui, and Chen, Jingguang G. Fri .
"Decomposition pathways of C2 oxygenates on Rh-modified tungsten carbide surfaces". United States. https://doi.org/10.1016/j.susc.2015.03.008. https://www.osti.gov/servlets/purl/1224193.
@article{osti_1224193,
title = {Decomposition pathways of C2 oxygenates on Rh-modified tungsten carbide surfaces},
author = {Kelly, Thomas G. and Ren, Hui and Chen, Jingguang G.},
abstractNote = {Ethanol decomposition on tungsten monocarbide (WC) and Rh-modified WC was investigated using ultrahigh vacuum (UHV) surface science experiments and density functional theory (DFT) calculations. DFT calculations indicated that the binding energies of ethanol and its decomposition intermediates on WC(0001) were modified by Rh, with Rh/WC(0001) showing similar values to those on Rh(111). Through temperature-programmed desorption (TPD) experiments on polycrystalline WC and Rh-modified WC, it was shown that the selectivity for ethanol decomposition was different on these surfaces. On WC, the C-O bond of ethanol was preferentially broken to produce ethylene; on Rh-modified WC, the C-C bond was broken to produce carbon monoxide and methane. In addition, high-resolution electron energy loss spectroscopy (HREELS) was used to determine likely surface intermediates. On Rh-modified WC, ethanol first formed ethoxy through O-H scission, then reacted through an aldehyde intermediate to form the C1 products.},
doi = {10.1016/j.susc.2015.03.008},
journal = {Surface Science},
number = C,
volume = 640,
place = {United States},
year = {Fri Mar 27 00:00:00 EDT 2015},
month = {Fri Mar 27 00:00:00 EDT 2015}
}
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Works referencing / citing this record:
Differentiation of the C–O and C–C bond scission mechanisms of 1-hexadecanol on Pt(111) and Ru(0001): a first principles analysis
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