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Time-resolved, in situ DRIFTS/EDE/MS studies on alumina-supported rhodium catalysts: effects of ceriation and zirconiation on rhodium-CO interactions

Time-resolved, in situ DRIFTS/EDE/MS studies on alumina-supported rhodium catalysts: effects of ceriation and zirconiation on rhodium-CO interactions
Time-resolved, in situ DRIFTS/EDE/MS studies on alumina-supported rhodium catalysts: effects of ceriation and zirconiation on rhodium-CO interactions
The effects of ceria and zirconia on the structure-function properties of supported rhodium catalysts (1.6 and 4 wt?% Rh/?-Al2 O3 ) during CO exposure are described. Ceria and zirconia are introduced through two preparation methods: 1) ceria is deposited on ?-Al2 O3 from [Ce(acac)3 ] and rhodium metal is subsequently added, and 2) through the controlled surface modification (CSM) technique, which involves the decomposition of [M(acac)x ] (M=Ce, x=3; M=Zr, x=4) on Rh/?-Al2 O3 . The structure-function correlations of ceria and/or zirconia-doped rhodium catalysts are investigated by diffuse reflectance infrared Fourier-transform spectroscopy/energy-dispersive extended X-ray absorption spectroscopy/mass spectrometry (DRIFTS/EDE/MS) under time-resolved, in situ conditions. CeOx and ZrO2 facilitate the protection of Rh particles against extensive oxidation in air and CO. Larger Rh core particles of ceriated and zirconiated Rh catalysts prepared by CSM are observed and compared with Rh/?-Al2 O3 samples, whereas supported Rh particles are easily disrupted by CO forming mononuclear Rh geminal dicarbonyl species. DRIFTS results indicate that, through the interaction of CO with ceriated Rh particles, a significantly larger amount of linear CO species form; this suggests the predominance of a metallic Rh phase.
1439-4235
3049-3059
Kroner, Anna B.
e0f05400-c002-4d09-83c0-70d91edb52c2
Newton, Mark A.
73aab2af-4641-47f3-89ad-3b7d3026164f
Tromp, Moniek
48c1ebbb-579c-42b6-83bb-7188c668b322
Roscioni, Otello M.
6a9e222d-d8f6-490b-ad64-bc13b0b26d2c
Russell, Andrea E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169
Dent, Andrew J.
24c2a218-cb0e-4193-af0b-3ff1dc42b552
Prestipino, Carmelo
cd7a8043-6441-4c42-86a8-dcc4e526b86f
Evans, John
05890433-0155-49fe-a65d-38c90ea25c69
Kroner, Anna B.
e0f05400-c002-4d09-83c0-70d91edb52c2
Newton, Mark A.
73aab2af-4641-47f3-89ad-3b7d3026164f
Tromp, Moniek
48c1ebbb-579c-42b6-83bb-7188c668b322
Roscioni, Otello M.
6a9e222d-d8f6-490b-ad64-bc13b0b26d2c
Russell, Andrea E.
b6b7c748-efc1-4d5d-8a7a-8e4b69396169
Dent, Andrew J.
24c2a218-cb0e-4193-af0b-3ff1dc42b552
Prestipino, Carmelo
cd7a8043-6441-4c42-86a8-dcc4e526b86f
Evans, John
05890433-0155-49fe-a65d-38c90ea25c69

Kroner, Anna B., Newton, Mark A., Tromp, Moniek, Roscioni, Otello M., Russell, Andrea E., Dent, Andrew J., Prestipino, Carmelo and Evans, John (2014) Time-resolved, in situ DRIFTS/EDE/MS studies on alumina-supported rhodium catalysts: effects of ceriation and zirconiation on rhodium-CO interactions. ChemPhysChem, 15 (14), 3049-3059. (doi:10.1002/cphc.201402122). (PMID:25044889)

Record type: Article

Abstract

The effects of ceria and zirconia on the structure-function properties of supported rhodium catalysts (1.6 and 4 wt?% Rh/?-Al2 O3 ) during CO exposure are described. Ceria and zirconia are introduced through two preparation methods: 1) ceria is deposited on ?-Al2 O3 from [Ce(acac)3 ] and rhodium metal is subsequently added, and 2) through the controlled surface modification (CSM) technique, which involves the decomposition of [M(acac)x ] (M=Ce, x=3; M=Zr, x=4) on Rh/?-Al2 O3 . The structure-function correlations of ceria and/or zirconia-doped rhodium catalysts are investigated by diffuse reflectance infrared Fourier-transform spectroscopy/energy-dispersive extended X-ray absorption spectroscopy/mass spectrometry (DRIFTS/EDE/MS) under time-resolved, in situ conditions. CeOx and ZrO2 facilitate the protection of Rh particles against extensive oxidation in air and CO. Larger Rh core particles of ceriated and zirconiated Rh catalysts prepared by CSM are observed and compared with Rh/?-Al2 O3 samples, whereas supported Rh particles are easily disrupted by CO forming mononuclear Rh geminal dicarbonyl species. DRIFTS results indicate that, through the interaction of CO with ceriated Rh particles, a significantly larger amount of linear CO species form; this suggests the predominance of a metallic Rh phase.

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Published date: 18 July 2014
Organisations: Chemistry, Faculty of Natural and Environmental Sciences, Electrochemistry

Identifiers

Local EPrints ID: 369821
URI: http://eprints.soton.ac.uk/id/eprint/369821
ISSN: 1439-4235
PURE UUID: af73dfbd-2b67-463b-92ca-7fd17383b8f6
ORCID for Andrea E. Russell: ORCID iD orcid.org/0000-0002-8382-6443

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Date deposited: 13 Oct 2014 13:01
Last modified: 31 Jul 2019 00:48

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