Investigation of the oxygen storage capacity behaviour of Three Way Catalysts using spatio-temporal analysis

Ciaran Coney, Christopher Hardacre, Kevin Morgan, Nancy Artioli, Andrew P. E. York, Paul Millington, Amy Kolpin, Alexandre Goguet

Research output: Contribution to journalArticle

Abstract

A transient lean-rich switching method has been developed in conjunction with the spatially resolved capillary inlet mass spectrometry (SpaciMS) technique using CO oxidation as a probe reaction. This has allowed in-situ spatiotemporal mapping of gaseous species and temperature profiles inside the channels of commercial three way 1%Pd/0.07%Rh/Al2O3/CexZr1-xO2 and 3%Pd/Al2O3 monolith catalysts. The identification of the spatiotemporal reactant conversion, intermediate and product formation, as well as the associated heat evolution, has helped in the elucidation of reaction sequences and furthermore, the postulation of reaction mechanisms, both axially and temporally inside the monolith catalyst. Intriguingly in this work, the SpaciMS technique has provided previously unobserved insights into an apparent excess OSC-like behaviour of the 3%Pd/Al2O3 catalyst, where excess CO conversion is detected under rich CO oxidation conditions in the presence of water. It has been demonstrated that the water gas shift reaction is insufficient to account for the excess CO conversion in this work, therefore a Pd(OH)x surface species is hypothesised to be acting in the same way as an oxygen storage component under rich conditions.
Original languageEnglish
JournalApplied Catalysis B: Environmental
Early online date26 Jul 2019
DOIs
Publication statusEarly online date - 26 Jul 2019

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temporal analysis
Carbon Monoxide
catalyst
Oxygen
oxygen
Catalysts
Mass spectrometry
mass spectrometry
oxidation
Oxidation
Water gas shift
temperature profile
probe
water
gas
Water
Temperature

Cite this

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title = "Investigation of the oxygen storage capacity behaviour of Three Way Catalysts using spatio-temporal analysis",
abstract = "A transient lean-rich switching method has been developed in conjunction with the spatially resolved capillary inlet mass spectrometry (SpaciMS) technique using CO oxidation as a probe reaction. This has allowed in-situ spatiotemporal mapping of gaseous species and temperature profiles inside the channels of commercial three way 1{\%}Pd/0.07{\%}Rh/Al2O3/CexZr1-xO2 and 3{\%}Pd/Al2O3 monolith catalysts. The identification of the spatiotemporal reactant conversion, intermediate and product formation, as well as the associated heat evolution, has helped in the elucidation of reaction sequences and furthermore, the postulation of reaction mechanisms, both axially and temporally inside the monolith catalyst. Intriguingly in this work, the SpaciMS technique has provided previously unobserved insights into an apparent excess OSC-like behaviour of the 3{\%}Pd/Al2O3 catalyst, where excess CO conversion is detected under rich CO oxidation conditions in the presence of water. It has been demonstrated that the water gas shift reaction is insufficient to account for the excess CO conversion in this work, therefore a Pd(OH)x surface species is hypothesised to be acting in the same way as an oxygen storage component under rich conditions.",
author = "Ciaran Coney and Christopher Hardacre and Kevin Morgan and Nancy Artioli and York, {Andrew P. E.} and Paul Millington and Amy Kolpin and Alexandre Goguet",
year = "2019",
month = "7",
day = "26",
doi = "10.1016/j.apcatb.2019.117918",
language = "English",
journal = "Applied Catalysis B: Environmental",
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Investigation of the oxygen storage capacity behaviour of Three Way Catalysts using spatio-temporal analysis. / Coney, Ciaran; Hardacre, Christopher; Morgan, Kevin; Artioli, Nancy; York, Andrew P. E.; Millington, Paul; Kolpin, Amy; Goguet, Alexandre.

In: Applied Catalysis B: Environmental, 26.07.2019.

Research output: Contribution to journalArticle

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AU - Coney, Ciaran

AU - Hardacre, Christopher

AU - Morgan, Kevin

AU - Artioli, Nancy

AU - York, Andrew P. E.

AU - Millington, Paul

AU - Kolpin, Amy

AU - Goguet, Alexandre

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AB - A transient lean-rich switching method has been developed in conjunction with the spatially resolved capillary inlet mass spectrometry (SpaciMS) technique using CO oxidation as a probe reaction. This has allowed in-situ spatiotemporal mapping of gaseous species and temperature profiles inside the channels of commercial three way 1%Pd/0.07%Rh/Al2O3/CexZr1-xO2 and 3%Pd/Al2O3 monolith catalysts. The identification of the spatiotemporal reactant conversion, intermediate and product formation, as well as the associated heat evolution, has helped in the elucidation of reaction sequences and furthermore, the postulation of reaction mechanisms, both axially and temporally inside the monolith catalyst. Intriguingly in this work, the SpaciMS technique has provided previously unobserved insights into an apparent excess OSC-like behaviour of the 3%Pd/Al2O3 catalyst, where excess CO conversion is detected under rich CO oxidation conditions in the presence of water. It has been demonstrated that the water gas shift reaction is insufficient to account for the excess CO conversion in this work, therefore a Pd(OH)x surface species is hypothesised to be acting in the same way as an oxygen storage component under rich conditions.

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