期刊
RSC ADVANCES
卷 5, 期 126, 页码 103834-103840出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5ra18404e
关键词
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资金
- Institute for Catalysis in Energy Processes (DOE) [DE-FG02-03ER15457]
- DOE [DE-AC02-06CH11357]
- E. I. duPont de Nemours Co.
- Northwestern University
- Dow Chemical Co.
- State of Illinois through the Department of Commerce and the Board of Education (HECA)
- US National Science Foundation
- Institute for Atom-efficient Chemical Transformations, an Energy Frontier Research Center - DOE, Office of Science, Office of Basic Energy Sciences
- MRSEC through NSF [DMR-1121262]
Catalytic reactions are associated with dynamical changes in the catalyst that include the oxidation state and local structural variations. The understanding of such dynamics, particularly at the atomic-scale, is of great importance for revealing the activity and selectivity of the catalyst in numerous reactions. Combining in situ X-ray absorption spectroscopy with in situ diffuse reflectance infrared Fourier transform spectroscopy, we studied the redox-induced dynamical changes for a VOX monolayer catalyst supported on a alpha-Fe2O3 powder. The results show that several co-existing VOX species reversibly change their V oxidation states between +5 and +4, in concurrence with a structural change from two-dimensional chains to well connected V-O-V networks. These changes are also associated with the breaking and formation of the V = O vanadyl group. This combined study provides new insight into how VOX species change during catalytic reactions, which leads to proposed atomic-scale models for the redox-induced dynamics of the catalyst.
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