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Investigation of MoOx/Al2O3 under cyclic operation for oxidative and non-oxidative dehydrogenation of propane

Matam, Santhosh K., Moffat, Caitlin, Hellier, Pip, Bowker, Michael, Silverwood, Ian P., Catlow, C. Richard A., Jackson, S. David, Craswell, James, Wells, Peter P., Parker, Stewart F. and Gibson, Emma K. 2020. Investigation of MoOx/Al2O3 under cyclic operation for oxidative and non-oxidative dehydrogenation of propane. Catalysts 10 (12) , 1370. 10.3390/catal10121370

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Abstract

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: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Additional Information: This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited
Publisher: MDPI
ISSN: 2073-4344
Funders: EPSRC
Date of First Compliant Deposit: 3 December 2020
Date of Acceptance: 22 November 2020
Last Modified: 04 Dec 2020 14:15
URI: http://orca.cf.ac.uk/id/eprint/136769

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