Unraveling the H2 promotional effect on the Palladium catalysed CO oxidation using a combination of temporally and spatially resolved investigations

Caomhan Stewart, Emma K Gibson, Kevin Morgan, Giannantonio Cibin, Andrew Dent, Christopher Hardacre, Evgenii V. Kondratenko, Vita Kondratenko, Colin McManus, Scott Rogers, Cristina-Elena Stere, Sarayute Chansai, Yi-Chi Wang, Sarah Haigh, Peter Wells, Alexandre Goguet

Research output: Contribution to journalArticle

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Abstract

The promotional effect of H2 on the oxidation of CO is of topical interest and there is debate over whether this promotion is due to either thermal or chemical effects. As yet there is no definitive consensus in the literature. Combining spatially resolved mass spectrometry and X-ray absorption spectroscopy (XAS) we observe a specific environment of the active catalyst during CO oxidation, having the same specific local coordination of the Pd in both the absence and presence of H2. In combination with Temporal Analysis of Products (TAP), performed under isothermal conditions, a mechanistic insight into the promotional effect of H2 was found, providing clear evidence of non-thermal effects in the hydrogen promoted of oxidation of carbon monoxide. We have identified that H2 promotes the Langmuir Hinshelwood mechanism and we propose this is linked to the increased interaction of O with the Pd surface in the presence of H2. This combination of spatially resolved MS and XAS and TAP studies has provided previously unobserved insights into the nature of this promotional effect.
LanguageEnglish
Pages8255-8262
Number of pages8
JournalACS Catalysis
Early online date26 Jul 2018
DOIs
Publication statusPublished - 07 Sep 2018

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Palladium
Carbon Monoxide
X ray absorption spectroscopy
Oxidation
Carbon monoxide
Mass spectrometry
Hydrogen
Catalysts

Cite this

Stewart, Caomhan ; Gibson, Emma K ; Morgan, Kevin ; Cibin, Giannantonio ; Dent, Andrew ; Hardacre, Christopher ; Kondratenko, Evgenii V. ; Kondratenko, Vita ; McManus, Colin ; Rogers, Scott ; Stere, Cristina-Elena ; Chansai, Sarayute ; Wang, Yi-Chi ; Haigh, Sarah ; Wells, Peter ; Goguet, Alexandre. / Unraveling the H2 promotional effect on the Palladium catalysed CO oxidation using a combination of temporally and spatially resolved investigations. In: ACS Catalysis. 2018 ; pp. 8255-8262.
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abstract = "The promotional effect of H2 on the oxidation of CO is of topical interest and there is debate over whether this promotion is due to either thermal or chemical effects. As yet there is no definitive consensus in the literature. Combining spatially resolved mass spectrometry and X-ray absorption spectroscopy (XAS) we observe a specific environment of the active catalyst during CO oxidation, having the same specific local coordination of the Pd in both the absence and presence of H2. In combination with Temporal Analysis of Products (TAP), performed under isothermal conditions, a mechanistic insight into the promotional effect of H2 was found, providing clear evidence of non-thermal effects in the hydrogen promoted of oxidation of carbon monoxide. We have identified that H2 promotes the Langmuir Hinshelwood mechanism and we propose this is linked to the increased interaction of O with the Pd surface in the presence of H2. This combination of spatially resolved MS and XAS and TAP studies has provided previously unobserved insights into the nature of this promotional effect.",
author = "Caomhan Stewart and Gibson, {Emma K} and Kevin Morgan and Giannantonio Cibin and Andrew Dent and Christopher Hardacre and Kondratenko, {Evgenii V.} and Vita Kondratenko and Colin McManus and Scott Rogers and Cristina-Elena Stere and Sarayute Chansai and Yi-Chi Wang and Sarah Haigh and Peter Wells and Alexandre Goguet",
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Stewart, C, Gibson, EK, Morgan, K, Cibin, G, Dent, A, Hardacre, C, Kondratenko, EV, Kondratenko, V, McManus, C, Rogers, S, Stere, C-E, Chansai, S, Wang, Y-C, Haigh, S, Wells, P & Goguet, A 2018, 'Unraveling the H2 promotional effect on the Palladium catalysed CO oxidation using a combination of temporally and spatially resolved investigations', ACS Catalysis, pp. 8255-8262. https://doi.org/10.1021/acscatal.8b01509

Unraveling the H2 promotional effect on the Palladium catalysed CO oxidation using a combination of temporally and spatially resolved investigations. / Stewart, Caomhan; Gibson, Emma K; Morgan, Kevin; Cibin, Giannantonio; Dent, Andrew; Hardacre, Christopher; Kondratenko, Evgenii V.; Kondratenko, Vita; McManus, Colin; Rogers, Scott; Stere, Cristina-Elena; Chansai, Sarayute; Wang, Yi-Chi; Haigh, Sarah; Wells, Peter; Goguet, Alexandre.

In: ACS Catalysis, 07.09.2018, p. 8255-8262.

Research output: Contribution to journalArticle

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AU - Stewart, Caomhan

AU - Gibson, Emma K

AU - Morgan, Kevin

AU - Cibin, Giannantonio

AU - Dent, Andrew

AU - Hardacre, Christopher

AU - Kondratenko, Evgenii V.

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AU - McManus, Colin

AU - Rogers, Scott

AU - Stere, Cristina-Elena

AU - Chansai, Sarayute

AU - Wang, Yi-Chi

AU - Haigh, Sarah

AU - Wells, Peter

AU - Goguet, Alexandre

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