In situ X-ray studies of crotyl alcohol selective oxidation over Au/Pd(1 1 1) surface alloys

Adam F. Lee; Simon F.J. Hackett; Graham J. Hutchings; Silvano Lizzit; James Naughton; Karen Wilson

doi:10.1016/j.cattod.2008.10.034

In situ X-ray studies of crotyl alcohol selective oxidation over Au/Pd(1 1 1) surface alloys

Adam F. Lee, Simon F.J. Hackett, Graham J. Hutchings, Silvano Lizzit, James Naughton, Karen Wilson

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

Abstract

The selective oxidation of crotyl alcohol to crotonaldehyde over ultrathin Au overlayers on Pd(1 1 1) and Au/Pd(1 1 1) surface alloys has been investigated by time-resolved X-ray photoelectron spectroscopy (XPS) and mass spectrometry. Pure gold is catalytically inert towards crotyl alcohol which undergoes reversible adsorption. In contrast, thermal processing of a 3.9 monolayer (ML) gold overlayer allows access to a range of AuPd surface alloy compositions, which are extremely selective towards crotonaldehyde production, and greatly reduce the extent of hydrocarbon decomposition and eventual carbon laydown compared with base Pd(1 1 1). XPS and CO titrations suggest that palladium-rich surface alloys offer the optimal balance between alcohol oxidative dehydrogenation activity while minimising competitive decomposition pathways, and that Pd monomers are not the active surface ensemble for such selox chemistry over AuPd alloys. Crown

Original language	English
Pages (from-to)	251-257
Number of pages	7
Journal	Catalysis Today
Volume	145
Issue number	3-4
Early online date	13 Dec 2008
DOIs	https://doi.org/10.1016/j.cattod.2008.10.034
Publication status	Published - 30 Jul 2009

Bibliographical note

We thank the EPSRC (EP/D038359/1 and EP/E046754/1), and acknowledge support by the EC-Research Infrastructure Action under the FP6 ‘‘Structuring the European Research Area’’ Programme (through the Integrated Infrastructure Initiative ‘‘Integrating Activity on Synchrotron and Free Electron Laser Science’’). SFJH and JN thank the EPSRC for the award of studentships.

Keywords

alcohol
gold
oxidation
palladium
XPS

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10.1016/j.cattod.2008.10.034

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title = "In situ X-ray studies of crotyl alcohol selective oxidation over Au/Pd(1 1 1) surface alloys",

abstract = "The selective oxidation of crotyl alcohol to crotonaldehyde over ultrathin Au overlayers on Pd(1 1 1) and Au/Pd(1 1 1) surface alloys has been investigated by time-resolved X-ray photoelectron spectroscopy (XPS) and mass spectrometry. Pure gold is catalytically inert towards crotyl alcohol which undergoes reversible adsorption. In contrast, thermal processing of a 3.9 monolayer (ML) gold overlayer allows access to a range of AuPd surface alloy compositions, which are extremely selective towards crotonaldehyde production, and greatly reduce the extent of hydrocarbon decomposition and eventual carbon laydown compared with base Pd(1 1 1). XPS and CO titrations suggest that palladium-rich surface alloys offer the optimal balance between alcohol oxidative dehydrogenation activity while minimising competitive decomposition pathways, and that Pd monomers are not the active surface ensemble for such selox chemistry over AuPd alloys. Crown",

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author = "Lee, {Adam F.} and Hackett, {Simon F.J.} and Hutchings, {Graham J.} and Silvano Lizzit and James Naughton and Karen Wilson",

note = "We thank the EPSRC (EP/D038359/1 and EP/E046754/1), and acknowledge support by the EC-Research Infrastructure Action under the FP6 {\textquoteleft}{\textquoteleft}Structuring the European Research Area{\textquoteright}{\textquoteright} Programme (through the Integrated Infrastructure Initiative {\textquoteleft}{\textquoteleft}Integrating Activity on Synchrotron and Free Electron Laser Science{\textquoteright}{\textquoteright}). SFJH and JN thank the EPSRC for the award of studentships.",

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AU - Lee, Adam F.

AU - Hackett, Simon F.J.

AU - Hutchings, Graham J.

AU - Lizzit, Silvano

AU - Naughton, James

AU - Wilson, Karen

N1 - We thank the EPSRC (EP/D038359/1 and EP/E046754/1), and acknowledge support by the EC-Research Infrastructure Action under the FP6 ‘‘Structuring the European Research Area’’ Programme (through the Integrated Infrastructure Initiative ‘‘Integrating Activity on Synchrotron and Free Electron Laser Science’’). SFJH and JN thank the EPSRC for the award of studentships.

PY - 2009/7/30

Y1 - 2009/7/30

N2 - The selective oxidation of crotyl alcohol to crotonaldehyde over ultrathin Au overlayers on Pd(1 1 1) and Au/Pd(1 1 1) surface alloys has been investigated by time-resolved X-ray photoelectron spectroscopy (XPS) and mass spectrometry. Pure gold is catalytically inert towards crotyl alcohol which undergoes reversible adsorption. In contrast, thermal processing of a 3.9 monolayer (ML) gold overlayer allows access to a range of AuPd surface alloy compositions, which are extremely selective towards crotonaldehyde production, and greatly reduce the extent of hydrocarbon decomposition and eventual carbon laydown compared with base Pd(1 1 1). XPS and CO titrations suggest that palladium-rich surface alloys offer the optimal balance between alcohol oxidative dehydrogenation activity while minimising competitive decomposition pathways, and that Pd monomers are not the active surface ensemble for such selox chemistry over AuPd alloys. Crown

AB - The selective oxidation of crotyl alcohol to crotonaldehyde over ultrathin Au overlayers on Pd(1 1 1) and Au/Pd(1 1 1) surface alloys has been investigated by time-resolved X-ray photoelectron spectroscopy (XPS) and mass spectrometry. Pure gold is catalytically inert towards crotyl alcohol which undergoes reversible adsorption. In contrast, thermal processing of a 3.9 monolayer (ML) gold overlayer allows access to a range of AuPd surface alloy compositions, which are extremely selective towards crotonaldehyde production, and greatly reduce the extent of hydrocarbon decomposition and eventual carbon laydown compared with base Pd(1 1 1). XPS and CO titrations suggest that palladium-rich surface alloys offer the optimal balance between alcohol oxidative dehydrogenation activity while minimising competitive decomposition pathways, and that Pd monomers are not the active surface ensemble for such selox chemistry over AuPd alloys. Crown

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In situ X-ray studies of crotyl alcohol selective oxidation over Au/Pd(1 1 1) surface alloys

Abstract

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Keywords

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