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| Content Provider | Springer Nature Link |
|---|---|
| Author | Rodriguez, J. A. Wang, X. Liu, P. Wen, W. Hanson, J. C. Hrbek, J. Pérez, M. Evans, J. |
| Copyright Year | 2007 |
| Abstract | Synchrotron-based techniques (high-resolution photoemission, in-situ X-ray absorption spectroscopy, and time-resolved X-ray diffraction) have been used to study the destruction of SO$_{2}$ and the water-gas shift (WGS, CO + H$_{2}$O → H$_{2}$ + CO$_{2}$) reaction on a series of gold/ceria systems. The adsorption and chemistry of SO$_{2}$ was investigated on Au/CeO$_{2}$(111) and AuO$_{ x }$/CeO$_{2}$ surfaces. The heat of adsorption of the molecule on Au nanoparticles supported on stoichiometric CeO$_{2}$(111) was 4–7 kcal/mol larger than on Au(111). However, there was negligible dissociation of SO$_{2}$ on the Au/CeO$_{2}$(111) surfaces. The full decomposition of SO$_{2}$ was observed only after introducing O vacancies in the ceria support. AuO$_{ x }$/CeO$_{2}$ surfaces were found to be much less chemically active than Au/CeO$_{2}$(111) or Au/CeO$_{2−x }$(111) surfaces. In a separate set of experiments, in-situ time-resolved X-ray diffraction and X-ray absorption spectroscopy were used to monitor the behavior of nanostructured {Au + AuO$_{ x }$}–CeO$_{2}$ catalysts under the WGS reaction. At temperatures above 250 °C, a complete AuO$_{ x }$ → Au transformation was observed with high catalytic activity. Photoemission results for the oxidation and reduction of Au nanoparticles supported on rough ceria films or a CeO$_{2}$(111) single crystal corroborate that cationic Au$^{δ+}$ species cannot be the key sites responsible for the WGS activity at high temperatures. The active sites in {Au + AuO$_{ x }$}/ceria catalysts should involve pure gold nanoparticles in contact with O vacancies of the oxide. |
| Starting Page | 73 |
| Ending Page | 81 |
| Page Count | 9 |
| File Format | |
| ISSN | 10225528 |
| Journal | Topics in Catalysis |
| Volume Number | 44 |
| Issue Number | 1-2 |
| e-ISSN | 15729028 |
| Language | English |
| Publisher | Kluwer Academic Publishers-Plenum Publishers |
| Publisher Date | 2007-01-01 |
| Publisher Place | New York |
| Access Restriction | One Nation One Subscription (ONOS) |
| Subject Keyword | gold gold oxide ceria sulfur dioxide DeSO$_{ x }$ water-gas shift hydrogen production CO oxidation Catalysis Physical Chemistry Pharmacy Industrial Chemistry/Chemical Engineering Characterization and Evaluation of Materials |
| Content Type | Text |
| Resource Type | Article |
| Subject | Chemistry Catalysis |
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