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

Jacinto Sá, Daniel Luis Abreu Fernandes, Farid Aiouache, Alexandre Goguet, Christopher Hardacre, David Lundie, Wasif Naeem, William P. Partridge, Cristina Stere

Research output: Contribution to journalArticle

51 Citations (Scopus)

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.
Original languageEnglish
Pages (from-to)2260-2272
Number of pages13
JournalAnalyst
Volume135
Issue number9
Early online date09 Aug 2010
DOIs
Publication statusPublished - 01 Sep 2010

ASJC Scopus subject areas

  • Biochemistry
  • Analytical Chemistry
  • Electrochemistry
  • Spectroscopy
  • Environmental Chemistry

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    Sá, J., Fernandes, D. L. A., Aiouache, F., Goguet, A., Hardacre, C., Lundie, D., Naeem, W., Partridge, W. P., & Stere, C. (2010). SpaciMS: spatial and temporal operando resolution of reactions within catalytic monoliths. Analyst, 135(9), 2260-2272. https://doi.org/10.1039/c0an00303d