Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage
Abstract
In this study, scanning tunnelling microscopy has been used to study the morphology of an overlayer of ceria in contact with a TiO2(110) substrate. Two types of domains were observed after ceria deposition. An ordered ceria film covered half of the surface and high-resolution imaging suggested a near-c(6 × 2) relationship to the underlying TiO2(110)-(1 × 1). The other half of the surface comprised CeOx nanoparticles and reconstructed TiOx supported on TiO2(110)-(1 × 1). Exposure to a small amount of gold resulted in the formation of isolated gold atoms and small clusters on the ordered ceria film and TiO2(110)-(1 × 1) areas, which exhibited significant sintering at 500 K and showed strong interaction between the sintered gold clusters and the domain boundaries of the ceria film. The Au/CeOx/TiO2(110) model system proved to be a good catalyst for the water–gas shift (WGS) exhibiting much higher turnover frequencies (TOFs) than Cu(111) and Pt(111) benchmarks, or the individual Au/TiO2(110) and Au/CeO2(111) systems. For Au/CeOx/TiO2(110) catalysts, there was a decrease in catalytic activity with increasing ceria coverage that correlates with a reduction in the concentration of Ce3+ formed during WGS reaction conditions.
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Central Univ. of Venezuela, Caracas (Venezuela)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1303023
- Alternate Identifier(s):
- OSTI ID: 1333203; OSTI ID: 1373613
- Report Number(s):
- BNL-112519-2016-JA; BNL-113208-2016-JA
Journal ID: ISSN 0039-6028; R&D Project: CO009; KC0302010
- Grant/Contract Number:
- SC00112704; SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Surface Science
- Additional Journal Information:
- Journal Volume: 650; 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; STM; TiO2 (110); CeO2; gold; water-gas shift; TiO2(110); water–gas shift
Citation Formats
Grinter, D. C., Park, J. B., Agnoli, S., Evans, J., Hrbek, J., Stacchiola, D. J., Senanayake, S. D., and Rodriguez, J. A. Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage. United States: N. p., 2016.
Web. doi:10.1016/j.susc.2015.10.002.
Grinter, D. C., Park, J. B., Agnoli, S., Evans, J., Hrbek, J., Stacchiola, D. J., Senanayake, S. D., & Rodriguez, J. A. Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage. United States. https://doi.org/10.1016/j.susc.2015.10.002
Grinter, D. C., Park, J. B., Agnoli, S., Evans, J., Hrbek, J., Stacchiola, D. J., Senanayake, S. D., and Rodriguez, J. A. Mon .
"Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage". United States. https://doi.org/10.1016/j.susc.2015.10.002. https://www.osti.gov/servlets/purl/1303023.
@article{osti_1303023,
title = {Water–gas shift reaction over gold nanoparticles dispersed on nanostructured CeOx–TiO2(110) surfaces: Effects of high ceria coverage},
author = {Grinter, D. C. and Park, J. B. and Agnoli, S. and Evans, J. and Hrbek, J. and Stacchiola, D. J. and Senanayake, S. D. and Rodriguez, J. A.},
abstractNote = {In this study, scanning tunnelling microscopy has been used to study the morphology of an overlayer of ceria in contact with a TiO2(110) substrate. Two types of domains were observed after ceria deposition. An ordered ceria film covered half of the surface and high-resolution imaging suggested a near-c(6 × 2) relationship to the underlying TiO2(110)-(1 × 1). The other half of the surface comprised CeOx nanoparticles and reconstructed TiOx supported on TiO2(110)-(1 × 1). Exposure to a small amount of gold resulted in the formation of isolated gold atoms and small clusters on the ordered ceria film and TiO2(110)-(1 × 1) areas, which exhibited significant sintering at 500 K and showed strong interaction between the sintered gold clusters and the domain boundaries of the ceria film. The Au/CeOx/TiO2(110) model system proved to be a good catalyst for the water–gas shift (WGS) exhibiting much higher turnover frequencies (TOFs) than Cu(111) and Pt(111) benchmarks, or the individual Au/TiO2(110) and Au/CeO2(111) systems. For Au/CeOx/TiO2(110) catalysts, there was a decrease in catalytic activity with increasing ceria coverage that correlates with a reduction in the concentration of Ce3+ formed during WGS reaction conditions.},
doi = {10.1016/j.susc.2015.10.002},
journal = {Surface Science},
number = C,
volume = 650,
place = {United States},
year = {Mon Aug 01 00:00:00 EDT 2016},
month = {Mon Aug 01 00:00:00 EDT 2016}
}
Web of Science
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