Fischer Tropsch synthesis: Deuterium isotopic study for the formation of oxygenates over CeO 2 supported Pt-Co catalysts

Muthu Kumaran Gnanamani; Gary Jacobs; Wilson D. Shafer; Mauro C. Ribeiro; Venkat Ramana Rao Pendyala; Wenping Ma; Burtron H. Davis

doi:10.1016/j.catcom.2012.03.028

Fischer Tropsch synthesis: Deuterium isotopic study for the formation of oxygenates over CeO ₂ supported Pt-Co catalysts

Muthu Kumaran Gnanamani, Gary Jacobs, Wilson D. Shafer, Mauro C. Ribeiro, Venkat Ramana Rao Pendyala, Wenping Ma, Burtron H. Davis

Center for Applied Energy Research (CAER)

Research output: Contribution to journal › Article › peer-review

23 Scopus citations

Abstract

The effect of deuterium on Fischer-Tropsch (FT) synthesis was investigated over a Pt promoted Co/CeO ₂ catalyst. CeO ₂ supported Pt-Co catalyst is more selective towards methane and oxygenates. H ₂-D ₂-H ₂ switching experiments suggest that the hydrogenation of CO is involved in the rate determining step (inverse isotope effect). The suppression of oxygenate formation with deuterium leads to the conclusion that common FT intermediates are responsible for the observed shift in the product spectrum. The deuterium isotopic study supports our previously proposed mechanism for the formation of alcohols in that the Co-CeO ₂ interface is involved in the catalysis, such that termination of chain growth occurs at the metal-oxide junction and involves bridging OH groups on partially reduced ceria.

Original language	English
Pages (from-to)	12-17
Number of pages	6
Journal	Catalysis Communications
Volume	25
DOIs	https://doi.org/10.1016/j.catcom.2012.03.028
State	Published - Aug 5 2012

Keywords

Ceria
Cobalt catalyst
Deuterium isotope effect
Fischer-Tropsch synthesis
Oxygenates

ASJC Scopus subject areas

Catalysis
Chemistry (all)
Process Chemistry and Technology

Access to Document

10.1016/j.catcom.2012.03.028

Cite this

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title = "Fischer Tropsch synthesis: Deuterium isotopic study for the formation of oxygenates over CeO 2 supported Pt-Co catalysts",

abstract = "The effect of deuterium on Fischer-Tropsch (FT) synthesis was investigated over a Pt promoted Co/CeO 2 catalyst. CeO 2 supported Pt-Co catalyst is more selective towards methane and oxygenates. H 2-D 2-H 2 switching experiments suggest that the hydrogenation of CO is involved in the rate determining step (inverse isotope effect). The suppression of oxygenate formation with deuterium leads to the conclusion that common FT intermediates are responsible for the observed shift in the product spectrum. The deuterium isotopic study supports our previously proposed mechanism for the formation of alcohols in that the Co-CeO 2 interface is involved in the catalysis, such that termination of chain growth occurs at the metal-oxide junction and involves bridging OH groups on partially reduced ceria.",

keywords = "Ceria, Cobalt catalyst, Deuterium isotope effect, Fischer-Tropsch synthesis, Oxygenates",

author = "Gnanamani, {Muthu Kumaran} and Gary Jacobs and Shafer, {Wilson D.} and Ribeiro, {Mauro C.} and Pendyala, {Venkat Ramana Rao} and Wenping Ma and Davis, {Burtron H.}",

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doi = "10.1016/j.catcom.2012.03.028",

language = "English",

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T2 - Deuterium isotopic study for the formation of oxygenates over CeO 2 supported Pt-Co catalysts

AU - Gnanamani, Muthu Kumaran

AU - Jacobs, Gary

AU - Shafer, Wilson D.

AU - Ribeiro, Mauro C.

AU - Pendyala, Venkat Ramana Rao

AU - Ma, Wenping

AU - Davis, Burtron H.

PY - 2012/8/5

Y1 - 2012/8/5

N2 - The effect of deuterium on Fischer-Tropsch (FT) synthesis was investigated over a Pt promoted Co/CeO 2 catalyst. CeO 2 supported Pt-Co catalyst is more selective towards methane and oxygenates. H 2-D 2-H 2 switching experiments suggest that the hydrogenation of CO is involved in the rate determining step (inverse isotope effect). The suppression of oxygenate formation with deuterium leads to the conclusion that common FT intermediates are responsible for the observed shift in the product spectrum. The deuterium isotopic study supports our previously proposed mechanism for the formation of alcohols in that the Co-CeO 2 interface is involved in the catalysis, such that termination of chain growth occurs at the metal-oxide junction and involves bridging OH groups on partially reduced ceria.

AB - The effect of deuterium on Fischer-Tropsch (FT) synthesis was investigated over a Pt promoted Co/CeO 2 catalyst. CeO 2 supported Pt-Co catalyst is more selective towards methane and oxygenates. H 2-D 2-H 2 switching experiments suggest that the hydrogenation of CO is involved in the rate determining step (inverse isotope effect). The suppression of oxygenate formation with deuterium leads to the conclusion that common FT intermediates are responsible for the observed shift in the product spectrum. The deuterium isotopic study supports our previously proposed mechanism for the formation of alcohols in that the Co-CeO 2 interface is involved in the catalysis, such that termination of chain growth occurs at the metal-oxide junction and involves bridging OH groups on partially reduced ceria.

KW - Ceria

KW - Cobalt catalyst

KW - Deuterium isotope effect

KW - Fischer-Tropsch synthesis

KW - Oxygenates

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