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

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

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.

Dehydrogenation, Inelastic neutron scattering spectroscopy, Infrared spectroscopy, Molybdenum oxide, Propane, Raman spectroscopy, XANES
2073-4344
1-13
Matam, Santhosh K.
b75aaeab-adb8-4d57-857f-4c6ef4f7de63
Moffat, Caitlin
95797d2c-2fe9-4707-a3a3-1ff11859962e
Hellier, Pip
c3bd090a-2f8d-45ec-8ee6-781c034eb9b9
Bowker, Michael
c9ab10a5-d144-4533-bf6d-2fa16b669565
Silverwood, Ian P.
82866f8b-db54-4b52-ae0e-20ac70e21b9e
Catlow, C. Richard A.
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David Jackson, S.
84c9250a-4e50-47c5-bb0a-c159cd1ff595
Craswell, James
7b33adf1-723e-44bf-8bb6-1134e1114d1f
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266
Parker, Stewart F.
fa284f3b-cd03-4981-b968-0335285a7aec
Gibson, Emma K.
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Matam, Santhosh K.
b75aaeab-adb8-4d57-857f-4c6ef4f7de63
Moffat, Caitlin
95797d2c-2fe9-4707-a3a3-1ff11859962e
Hellier, Pip
c3bd090a-2f8d-45ec-8ee6-781c034eb9b9
Bowker, Michael
c9ab10a5-d144-4533-bf6d-2fa16b669565
Silverwood, Ian P.
82866f8b-db54-4b52-ae0e-20ac70e21b9e
Catlow, C. Richard A.
50b88125-9415-4b37-9146-af6783e42510
David Jackson, S.
84c9250a-4e50-47c5-bb0a-c159cd1ff595
Craswell, James
7b33adf1-723e-44bf-8bb6-1134e1114d1f
Wells, Peter P.
bc4fdc2d-a490-41bf-86cc-400edecf2266
Parker, Stewart F.
fa284f3b-cd03-4981-b968-0335285a7aec
Gibson, Emma K.
738c74e4-ab68-42fe-bda8-9d4a43669b31

Matam, Santhosh K., Moffat, Caitlin, Hellier, Pip, Bowker, Michael, Silverwood, Ian P., Catlow, C. Richard A., David Jackson, S., 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), 1-13, [1370]. (doi:10.3390/catal10121370).

Record type: Article

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.

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More information

Accepted/In Press date: 22 November 2020
e-pub ahead of print date: 24 November 2020
Keywords: Dehydrogenation, Inelastic neutron scattering spectroscopy, Infrared spectroscopy, Molybdenum oxide, Propane, Raman spectroscopy, XANES

Identifiers

Local EPrints ID: 446630
URI: http://eprints.soton.ac.uk/id/eprint/446630
ISSN: 2073-4344
PURE UUID: afc10ff9-32b9-469b-85fa-cac0423f32d3
ORCID for Peter P. Wells: ORCID iD orcid.org/0000-0002-0859-9172

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Date deposited: 16 Feb 2021 17:35
Last modified: 18 Feb 2021 17:05

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Contributors

Author: Santhosh K. Matam
Author: Caitlin Moffat
Author: Pip Hellier
Author: Michael Bowker
Author: Ian P. Silverwood
Author: C. Richard A. Catlow
Author: S. David Jackson
Author: James Craswell
Author: Peter P. Wells ORCID iD
Author: Stewart F. Parker
Author: Emma K. Gibson

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