Atomic-scale cation dynamics in a monolayer VOX/α-Fe2O3 catalyst

Feng, Z.; Ma, Q.; Lu, J.; Feng, H.; Elam, J. W.; Stair, P. C.; Bedzyk, M. J.

doi:10.1039/c5ra18404e

Atomic-scale cation dynamics in a monolayer VO_X/α-Fe₂O₃ catalyst

Journal Article · Tue Nov 17 23:00:00 EST 2015 · RSC Advances

DOI:https://doi.org/10.1039/c5ra18404e· OSTI ID:1370178

^[1]; Ma, Q. ^[2]; Lu, J. ^[3]; Feng, H. ^[4]; Elam, J. W. ^[5]; Stair, P. C. ^[2]; Bedzyk, M. J. ^[2]

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)

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 VO_X monolayer catalyst supported on a α-Fe₂O₃ powder. The results show that several co-existing VO_X 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 VO_X species change during catalytic reactions, which leads to proposed atomic-scale models for the redox-induced dynamics of the catalyst.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Institute for Atom-efficient Chemical Transformations (IACT); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: 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)

Grant/Contract Number:: AC02-06CH11357; FG02-03ER15457; AC02-06CH11357

OSTI ID:: 1370178

Journal Information:: RSC Advances, Journal Name: RSC Advances Journal Issue: 126 Vol. 5; ISSN 2046-2069; ISSN RSCACL

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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