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Particle size effects in Rh/Al2O3 catalysts as viewed from a structural, functional, and reactive perspective: the case of the reactive adsorption of NO

Particle size effects in Rh/Al2O3 catalysts as viewed from a structural, functional, and reactive perspective: the case of the reactive adsorption of NO
Particle size effects in Rh/Al2O3 catalysts as viewed from a structural, functional, and reactive perspective: the case of the reactive adsorption of NO
The structural-dynamic behaviour of ?-Al2O3 supported Rh nanoparticles under He, H2/He, and NO/He has been investigated using a newly developed methodology that permits dispersive EXAFS (EDE), diffuse reflectance infra red spectroscopy (DRIFTS), and mass spectrometry (MS) to be applied simultaneously to the study of gas-solid interactions. This reveals a considerably variability in nanoparticle habit (for 11 Å diameter nanoparticles as a function of temperature), and between 8 Å and 11 Å particles in their response to NO. The selectivity (N2/(N2 + N2O)) of the reactive interaction between NO and the supported Rh shows essentially no particle size dependence above 473 K: it is apparent, however, that considerable differences in some aspects of the structural behaviour of the 8 Å and 11 Å Rh particles do nonetheless, exist. At 373 < T < 473 K a clear divergence in structural, functional, and reactive response of the different sized supported Rh nanoparticles toward NO is observed. These observations are discussed in terms of the ability of different sized Rh particles to change structure in response to the reactive environment, the subsequent effect this has on the nitrosyl functionality that different phases may support, and the reactive pathways for NO conversion that may therefore arise.
0022-2461
3288-3298
Newton, Mark A.
73aab2af-4641-47f3-89ad-3b7d3026164f
Dent, Andrew J.
24c2a218-cb0e-4193-af0b-3ff1dc42b552
Fiddy, Steven G.
f6c255cf-6aa1-4798-85ca-1a2ccdaa1186
Jyoti, Bhrat
9e00e347-0864-48fa-9bb8-f44f98161fd0
Evans, John
05890433-0155-49fe-a65d-38c90ea25c69
Newton, Mark A.
73aab2af-4641-47f3-89ad-3b7d3026164f
Dent, Andrew J.
24c2a218-cb0e-4193-af0b-3ff1dc42b552
Fiddy, Steven G.
f6c255cf-6aa1-4798-85ca-1a2ccdaa1186
Jyoti, Bhrat
9e00e347-0864-48fa-9bb8-f44f98161fd0
Evans, John
05890433-0155-49fe-a65d-38c90ea25c69

Newton, Mark A., Dent, Andrew J., Fiddy, Steven G., Jyoti, Bhrat and Evans, John (2007) Particle size effects in Rh/Al2O3 catalysts as viewed from a structural, functional, and reactive perspective: the case of the reactive adsorption of NO. Journal of Materials Science, 42 (10), 3288-3298. (doi:10.1007/s10853-006-0751-y).

Record type: Article

Abstract

The structural-dynamic behaviour of ?-Al2O3 supported Rh nanoparticles under He, H2/He, and NO/He has been investigated using a newly developed methodology that permits dispersive EXAFS (EDE), diffuse reflectance infra red spectroscopy (DRIFTS), and mass spectrometry (MS) to be applied simultaneously to the study of gas-solid interactions. This reveals a considerably variability in nanoparticle habit (for 11 Å diameter nanoparticles as a function of temperature), and between 8 Å and 11 Å particles in their response to NO. The selectivity (N2/(N2 + N2O)) of the reactive interaction between NO and the supported Rh shows essentially no particle size dependence above 473 K: it is apparent, however, that considerable differences in some aspects of the structural behaviour of the 8 Å and 11 Å Rh particles do nonetheless, exist. At 373 < T < 473 K a clear divergence in structural, functional, and reactive response of the different sized supported Rh nanoparticles toward NO is observed. These observations are discussed in terms of the ability of different sized Rh particles to change structure in response to the reactive environment, the subsequent effect this has on the nitrosyl functionality that different phases may support, and the reactive pathways for NO conversion that may therefore arise.

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Published date: May 2007

Identifiers

Local EPrints ID: 147891
URI: http://eprints.soton.ac.uk/id/eprint/147891
ISSN: 0022-2461
PURE UUID: d43b8077-604a-4f2d-8816-0f03d9c676c8

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Date deposited: 03 Jun 2010 13:46
Last modified: 14 Mar 2024 01:00

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Contributors

Author: Mark A. Newton
Author: Andrew J. Dent
Author: Steven G. Fiddy
Author: Bhrat Jyoti
Author: John Evans

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