Atomic-scale cation dynamics in a monolayer VOX/α-Fe2O3 catalyst
Abstract
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 α-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.
- Authors:
-
[1];
- Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Science and Technology of China, Hefei (China)
- Argonne National Lab. (ANL), Lemont, IL (United States); Xi'an Modern Chemistry Research Inst., Shaanxi (China)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Institute for Atom-efficient Chemical Transformations (IACT); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- E. I. duPont de Nemours & Co.; Northwestern University; Dow Chemical Co.; State of Illinois; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1370178
- Grant/Contract Number:
- AC02-06CH11357; FG02-03ER15457; DMR-1121262
- Resource Type:
- Accepted Manuscript
- Journal Name:
- RSC Advances
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 126; Related Information: IACT partners with Argonne National Laboratory (lead); Brookhaven National Laboratory; Northwestern University; Purdue University; University of Wisconsin at Madison; Journal ID: ISSN 2046-2069
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Feng, Z., Ma, Q., Lu, J., Feng, H., Elam, J. W., Stair, P. C., and Bedzyk, M. J. Atomic-scale cation dynamics in a monolayer VOX/α-Fe2O3 catalyst. United States: N. p., 2015.
Web. doi:10.1039/c5ra18404e.
Feng, Z., Ma, Q., Lu, J., Feng, H., Elam, J. W., Stair, P. C., & Bedzyk, M. J. Atomic-scale cation dynamics in a monolayer VOX/α-Fe2O3 catalyst. United States. https://doi.org/10.1039/c5ra18404e
Feng, Z., Ma, Q., Lu, J., Feng, H., Elam, J. W., Stair, P. C., and Bedzyk, M. J. Wed .
"Atomic-scale cation dynamics in a monolayer VOX/α-Fe2O3 catalyst". United States. https://doi.org/10.1039/c5ra18404e. https://www.osti.gov/servlets/purl/1370178.
@article{osti_1370178,
title = {Atomic-scale cation dynamics in a monolayer VOX/α-Fe2O3 catalyst},
author = {Feng, Z. and Ma, Q. and Lu, J. and Feng, H. and Elam, J. W. and Stair, P. C. and Bedzyk, M. J.},
abstractNote = {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 α-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.},
doi = {10.1039/c5ra18404e},
journal = {RSC Advances},
number = 126,
volume = 5,
place = {United States},
year = {Wed Nov 18 00:00:00 EST 2015},
month = {Wed Nov 18 00:00:00 EST 2015}
}
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