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Investigation of MoOx/Al2O3 under Cyclic Operation for Oxidative and Non-Oxidative Dehydrogenation of Propane

Matam, SK; Moffat, C; Hellier, P; Bowker, M; Silverwood, IP; Catlow, CRA; Jackson, SD; ... Gibson, EK; + view all (2020) Investigation of MoOx/Al2O3 under Cyclic Operation for Oxidative and Non-Oxidative Dehydrogenation of Propane. Catalysts , 10 (12) , Article 1370. 10.3390/catal10121370. Green open access

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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.

Type: Article
Title: Investigation of MoOx/Al2O3 under Cyclic Operation for Oxidative and Non-Oxidative Dehydrogenation of Propane
Open access status: An open access version is available from UCL Discovery
DOI: 10.3390/catal10121370
Publisher version: https://doi.org/10.3390/catal10121370
Language: English
Additional information: This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
Keywords: Science & Technology, Physical Sciences, Chemistry, Physical, Chemistry, propane, dehydrogenation, molybdenum oxide, XANES, Raman spectroscopy, inelastic neutron scattering spectroscopy, infrared spectroscopy, MOLYBDENUM OXIDE CATALYSTS, SUPPORTED METAL-OXIDE, RAY-ABSORPTION SPECTROSCOPY, NEUTRON-SCATTERING, MO/AL2O3 CATALYST, MIXED OXIDES, RAMAN, SURFACE, ETHANE, MO
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10119512
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