Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 3, Issue 19, Pages 2845-2850Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz3011546
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Funding
- Institute for Catalysis and Energy Processes (U.S. Department of Energy (DOE)) [DE-FG02-03ER15457]
- DOE, Office of Science, BES [DE-AC02-06CH11357]
- DOE Office of Biological and Environmental Research
- DuPont
- Northwestern University
- Dow Chemical
- NSF [DMR-1121262]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1121262] Funding Source: National Science Foundation
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The activity of supported catalysts is strongly linked to the structure of the surface species. However, direct in situ structural measurements of submonolayer catalysts are lacking. Using in situ X-ray standing wave analysis combined with ex situ X-ray photoelectron spectroscopy and atomic force microscopy, we observed reversible redox-induced surface cation dynamics for three-fourths of a monolayer of vanadia grown by atomic-layer deposition on an alpha-TiO2(110) surface. On the basis of first-principles density functional theory calculations, we propose vanadia submonolayer structures that agree with and suggest explanations for the observed redox-induced structural changes. Under oxidation conditions, the correlated submonolayer structure is a 2D trimer-decorated polymeric chain along the rutile [-1 1 0] direction; under reducing conditions, the more stable polymeric chain remains unreduced, whereas the less stable decorating trimers become reduced and uncorrelated with the support lattice. These results show that a large fraction of V sites retains redox activity at submonolayer V coverages.
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