Investigation of MoO x/Al 2 O 3 under cyclic operation for oxidative and non-oxidative dehydrogenation of propane

Matam, S. K. et al. (2020) Investigation of MoO x/Al 2 O 3 under cyclic operation for oxidative and non-oxidative dehydrogenation of propane. Catalysts, 10(12), 1370. (doi: 10.3390/catal10121370)

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A MoOx/Al2O3 catalyst was synthesised and tested for oxidative (ODP) and non-oxidative (DP) dehydrogenation of propane in a reaction cycle of ODP followed by DP and a second ODP run. Characterisation results show that the fresh catalyst contains highly dispersed Mo oxide species in the +6 oxidation state with tetrahedral coordination as [MoVIO4]2− moieties. In situ X-ray Absorption Spectroscopy (XAS) shows that [MoVIO4]2− is present during the first ODP run of the reaction cycle and is reduced to MoIVO2 in the following DP run. The reduced species are partly re-oxidised in the subsequent second ODP run of the reaction cycle. The partly re-oxidised species exhibit oxidation and coordination states that are lower than 6 but higher than 4 and are referred to as MoxOy. These species significantly improved propene formation (relatively 27% higher) in the second ODP run at similar propane conversion activity. Accordingly, the initial tetrahedral [MoVIO4]2− present during the first ODP run of the reaction cycle is active for propane conversion; however, it is unselective for propene. The reduced MoIVO2 species are relatively less active and selective for DP. It is suggested that the MoxOy species generated by the reaction cycle are active and selective for ODP. The vibrational spectroscopic data indicate that the retained surface species are amorphous carbon deposits with a higher proportion of aromatic/olefinic like species.

Item Type:Articles
Additional Information:This research was funded by the Engineering and Physical Sciences Research Council (EPSRC) through grants: EP/I038748/1, EP/I019693/1, EP/K014706/1, EP/K014668/1, EP/K014854/1, EP/K014714/1 and EP/M013219/1.
Keywords:Propane, dehydrogenation, molybdenum oxide, XANES, Raman spectroscopy, inelastic neutron scattering spectroscopy, infrared spectroscopy.
Glasgow Author(s) Enlighten ID:Parker, Dr Stewart and Gibson, Dr Emma and Jackson, Professor David and Moffat, Caitlin
Creator Roles:
Moffat, C.Formal analysis, Writing – original draft
Jackson, S. D.Validation, Supervision
Parker, S. F.Conceptualization, Methodology, Formal analysis, Writing – review and editing
Gibson, E. K.Conceptualization, Methodology, Formal analysis, Investigation, Writing – review and editing, Supervision, Funding acquisition
Authors: Matam, S. K., Moffat, C., Hellier, P., Bowker, M., Silverwood, I. P., Catlow, C. R. A., Jackson, S. D., Craswell, J., Wells, P. P., Parker, S. F., and Gibson, E. K.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Catalysts
ISSN (Online):2073-4344
Published Online:24 November 2020
Copyright Holders:Copyright © 2020 The Authors
First Published:First published in Catalysts 10(12): 1370
Publisher Policy:Reproduced under a Creative Commons License
Data DOI:10.5525/gla.researchdata.1092

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
169321Catalytic HDO : Queen's University of Belfast ref R1188CCESamuel JacksonEngineering and Physical Sciences Research Council (EPSRC)EP/K014706/1Chemistry