skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

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.

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [1];  [4];  [1]
  1. Queen's University, Belfast
  2. University of Aveiro, Portugal
  3. Hiden Analytical Ltd
  4. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Fuels, Engines and Emissions Research Center (FEERC)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
986836
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Analyst, The
Additional Journal Information:
Journal Volume: 135; Journal Issue: 9; Journal ID: ISSN 0003-2654
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CATALYSTS; CATALYSIS; MASS SPECTROMETERS; PERFORMANCE; PLATINUM; RHODIUM; CARBON MONOXIDE; OXIDATION

Citation Formats

Sa, Jacinto, Fernandes, Daniel, Aiouache, Farid, Goguet, Alexandre, Hardacdre, Christopher, Lundie, David, Naeem, Wasif, Partridge, Jr, William P, and Stere, Cristina. SpaciMS: spatial and temporal operando resolution of reactions within catalytic monoliths. United States: N. p., 2010. Web. doi:10.1039/c0an00303d.
Sa, Jacinto, Fernandes, Daniel, Aiouache, Farid, Goguet, Alexandre, Hardacdre, Christopher, Lundie, David, Naeem, Wasif, Partridge, Jr, William P, & Stere, Cristina. SpaciMS: spatial and temporal operando resolution of reactions within catalytic monoliths. United States. https://doi.org/10.1039/c0an00303d
Sa, Jacinto, Fernandes, Daniel, Aiouache, Farid, Goguet, Alexandre, Hardacdre, Christopher, Lundie, David, Naeem, Wasif, Partridge, Jr, William P, and Stere, Cristina. 2010. "SpaciMS: spatial and temporal operando resolution of reactions within catalytic monoliths". United States. https://doi.org/10.1039/c0an00303d.
@article{osti_986836,
title = {SpaciMS: spatial and temporal operando resolution of reactions within catalytic monoliths},
author = {Sa, Jacinto and Fernandes, Daniel and Aiouache, Farid and Goguet, Alexandre and Hardacdre, Christopher and Lundie, David and Naeem, Wasif and Partridge, Jr, William P and Stere, Cristina},
abstractNote = {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.},
doi = {10.1039/c0an00303d},
url = {https://www.osti.gov/biblio/986836}, journal = {Analyst, The},
issn = {0003-2654},
number = 9,
volume = 135,
place = {United States},
year = {Fri Jan 01 00:00:00 EST 2010},
month = {Fri Jan 01 00:00:00 EST 2010}
}