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In situ spectroscopic investigations of MoOx/Fe2O3catalysts for the selective oxidation of methanol

In situ spectroscopic investigations of MoOx/Fe2O3catalysts for the selective oxidation of methanol
In situ spectroscopic investigations of MoOx/Fe2O3catalysts for the selective oxidation of methanol
Multicomponent oxide shell@core catalysts have been prepared, affording overlayers of MoOx on Fe2O3. This design approach allows bulk characterization techniques, such as X-ray Absorption Fine Structure (XAFS), to provide surface sensitive information. Coupling this approach with in situ methodologies provides insights during crucial catalytic processes. Calcination studies were followed by a combination of XAFS and Raman, and demonstrate that amorphous multi-layers of MoOx are first converted to MoO3 before formation of Fe2(MoO4)3. However, a single overlayer of Oh Mo units remains at the surface at all times. In situ catalysis studies during formaldehyde production identified that Mo6+ was present throughout, confirming that gas phase oxygen transfer to molybdenum is rapid under reaction conditions. Reduction studies in the presence of MeOH resulted in the formation of reduced Mo–Mo clusters with a bonding distance of 2.6 Å. It is proposed that the presence of the clusters indicates that the selective conversion of MeOH to formaldehyde requires multiple Mo sites
2044-4753
722-730
Brookes, Catherine
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Bowker, Michael
c9ab10a5-d144-4533-bf6d-2fa16b669565
Gibson, Emma K.
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Gianolio, Diego
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Mohammed, Khaled M.H.
0cace598-da8f-458a-ba97-93f575a1bea7
Parry, Stephen
1ebd8f37-abf4-4dfd-974e-fe18fb33785f
Rogers, Scott M.
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Silverwood, Ian P.
82866f8b-db54-4b52-ae0e-20ac70e21b9e
Wells, Peter
bc4fdc2d-a490-41bf-86cc-400edecf2266
Brookes, Catherine
fcbf76ed-9e86-4aea-b8f5-174607bae342
Bowker, Michael
c9ab10a5-d144-4533-bf6d-2fa16b669565
Gibson, Emma K.
738c74e4-ab68-42fe-bda8-9d4a43669b31
Gianolio, Diego
5b316f7d-f314-4337-954e-8c0ce8e38223
Mohammed, Khaled M.H.
0cace598-da8f-458a-ba97-93f575a1bea7
Parry, Stephen
1ebd8f37-abf4-4dfd-974e-fe18fb33785f
Rogers, Scott M.
81804d0d-1f08-4a12-b6c8-56d7d45a039b
Silverwood, Ian P.
82866f8b-db54-4b52-ae0e-20ac70e21b9e
Wells, Peter
bc4fdc2d-a490-41bf-86cc-400edecf2266

Brookes, Catherine, Bowker, Michael, Gibson, Emma K., Gianolio, Diego, Mohammed, Khaled M.H., Parry, Stephen, Rogers, Scott M., Silverwood, Ian P. and Wells, Peter (2016) In situ spectroscopic investigations of MoOx/Fe2O3catalysts for the selective oxidation of methanol. Catalysis Science & Technology, 6 (3), 722-730. (doi:10.1039/C5CY01175B).

Record type: Article

Abstract

Multicomponent oxide shell@core catalysts have been prepared, affording overlayers of MoOx on Fe2O3. This design approach allows bulk characterization techniques, such as X-ray Absorption Fine Structure (XAFS), to provide surface sensitive information. Coupling this approach with in situ methodologies provides insights during crucial catalytic processes. Calcination studies were followed by a combination of XAFS and Raman, and demonstrate that amorphous multi-layers of MoOx are first converted to MoO3 before formation of Fe2(MoO4)3. However, a single overlayer of Oh Mo units remains at the surface at all times. In situ catalysis studies during formaldehyde production identified that Mo6+ was present throughout, confirming that gas phase oxygen transfer to molybdenum is rapid under reaction conditions. Reduction studies in the presence of MeOH resulted in the formation of reduced Mo–Mo clusters with a bonding distance of 2.6 Å. It is proposed that the presence of the clusters indicates that the selective conversion of MeOH to formaldehyde requires multiple Mo sites

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More information

Accepted/In Press date: 21 August 2015
Published date: 7 February 2016
Organisations: Organic Chemistry: SCF

Identifiers

Local EPrints ID: 400532
URI: https://eprints.soton.ac.uk/id/eprint/400532
ISSN: 2044-4753
PURE UUID: 3e60cbf1-99c9-4a2f-bbf4-8be3d2a2c290
ORCID for Peter Wells: ORCID iD orcid.org/0000-0002-0859-9172

Catalogue record

Date deposited: 16 Sep 2016 15:33
Last modified: 14 Jul 2018 00:33

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