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SpaciMS:spatial and temporal operando resolution of reactions within catalytic monoliths

Sá, Jacinto and Fernandes, Daniel Luis Abreu and Aiouache, Farid and Goguet, Alexandre and Hardacre, Christopher and Lundie, David and Naeem, Wasif and Partridge, William P and Stere, Cristina (2010) SpaciMS:spatial and temporal operando resolution of reactions within catalytic monoliths. Analyst, 135 (9). pp. 2260-2272. ISSN 1364-5528

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Abstract

Monolithic catalysts are widely used as structured catalysts, especially in the abatement of pollutants. Probing what happens inside these monoliths during operation is, therefore, vital for modelling and prediction of the catalyst behavior. SpaciMS is a spatially resolved capillary-inlet mass spectroscopy system allowing for the generation of spatially resolved maps of the reactions within monoliths. In this study SpaciMS results combined with 3D CFD modelling demonstrate that SpaciMS is a highly sensitive and minimally invasive technique that can provide reaction maps as well as catalytic temporal behavior. Herein we illustrate this by examining kinetic oscillations during a CO oxidation reaction over a Pt/Rh on alumina catalyst supported on a cordierite monolith. These oscillations were only observed within the monolith by SpaciMS between 30 and 90% CO conversion. Equivalent experiments performed in a plug-flow reactor using this catalyst in a crushed form over a similar range of reaction conditions did not display any oscillations demonstrating the importance of intra monolith analysis. This work demonstrates that the SpaciMS offers an accurate and comprehensive picture of structured catalysts under operation.

Item Type: Article
Journal or Publication Title: Analyst
Subjects:
Departments: Faculty of Science and Technology > Engineering
ID Code: 60671
Deposited By: ep_importer_pure
Deposited On: 13 Dec 2012 15:58
Refereed?: Yes
Published?: Published
Last Modified: 19 Nov 2017 12:08
Identification Number:
URI: http://eprints.lancs.ac.uk/id/eprint/60671

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