Scanning Tunneling Microscopy Evidence for the Dissociation of Carbon Monoxide on Ruthenium Steps

Yann Tison, Kenneth Nielsen, Duncan J. Mowbray, Lone Bech, Christian Holse, Federico Calle Vallejo, Kirsten Andersen, Jens J. Mortensen, Karsten W. Jacobsen, Jane H. Nielsen

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

In heterogeneous catalysis, identifying the active site for key reaction steps is an important contribution for the optimization of industrial synthesis. The structure sensitivity of CO dissociation on a metal catalyst, which is the rate-limiting step for the methanation and the Fischer–Tropsch processes under certain conditions, has been debated for years. Here, scanning tunneling microscopy (STM) and density functional theory (DFT) are used to clarify the role of monatomic steps in the splitting of CO on a stepped Ru(0 1 54) crystal, which displays alternating steps with either 4-fold or 3-fold symmetry. After CO doses at elevated temperatures, the STM images reveal step decorations characteristic of atomic oxygen resulting from CO dissociation on every second step. The comparison of the STM images with the results of DFT calculations shows that the step decoration occurs on the steps displaying the 4-fold symmetry. We conclude that the active sites for CO dissociation on ruthenium are located on the 4-fold symmetry monatomic steps.
Original languageEnglish
JournalThe Journal of Physical Chemistry Part C
Volume116
Issue number27
Pages (from-to)14350-14359
ISSN1932-7447
DOIs
Publication statusPublished - 2012

Cite this

Tison, Yann ; Nielsen, Kenneth ; Mowbray, Duncan J. ; Bech, Lone ; Holse, Christian ; Vallejo, Federico Calle ; Andersen, Kirsten ; Mortensen, Jens J. ; Jacobsen, Karsten W. ; Nielsen, Jane H. / Scanning Tunneling Microscopy Evidence for the Dissociation of Carbon Monoxide on Ruthenium Steps. In: The Journal of Physical Chemistry Part C. 2012 ; Vol. 116, No. 27. pp. 14350-14359.
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title = "Scanning Tunneling Microscopy Evidence for the Dissociation of Carbon Monoxide on Ruthenium Steps",
abstract = "In heterogeneous catalysis, identifying the active site for key reaction steps is an important contribution for the optimization of industrial synthesis. The structure sensitivity of CO dissociation on a metal catalyst, which is the rate-limiting step for the methanation and the Fischer–Tropsch processes under certain conditions, has been debated for years. Here, scanning tunneling microscopy (STM) and density functional theory (DFT) are used to clarify the role of monatomic steps in the splitting of CO on a stepped Ru(0 1 54) crystal, which displays alternating steps with either 4-fold or 3-fold symmetry. After CO doses at elevated temperatures, the STM images reveal step decorations characteristic of atomic oxygen resulting from CO dissociation on every second step. The comparison of the STM images with the results of DFT calculations shows that the step decoration occurs on the steps displaying the 4-fold symmetry. We conclude that the active sites for CO dissociation on ruthenium are located on the 4-fold symmetry monatomic steps.",
author = "Yann Tison and Kenneth Nielsen and Mowbray, {Duncan J.} and Lone Bech and Christian Holse and Vallejo, {Federico Calle} and Kirsten Andersen and Mortensen, {Jens J.} and Jacobsen, {Karsten W.} and Nielsen, {Jane H.}",
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language = "English",
volume = "116",
pages = "14350--14359",
journal = "The Journal of Physical Chemistry Part C",
issn = "1932-7447",
publisher = "American Chemical Society",
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Scanning Tunneling Microscopy Evidence for the Dissociation of Carbon Monoxide on Ruthenium Steps. / Tison, Yann; Nielsen, Kenneth; Mowbray, Duncan J.; Bech, Lone; Holse, Christian; Vallejo, Federico Calle; Andersen, Kirsten; Mortensen, Jens J.; Jacobsen, Karsten W.; Nielsen, Jane H.

In: The Journal of Physical Chemistry Part C, Vol. 116, No. 27, 2012, p. 14350-14359.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Scanning Tunneling Microscopy Evidence for the Dissociation of Carbon Monoxide on Ruthenium Steps

AU - Tison, Yann

AU - Nielsen, Kenneth

AU - Mowbray, Duncan J.

AU - Bech, Lone

AU - Holse, Christian

AU - Vallejo, Federico Calle

AU - Andersen, Kirsten

AU - Mortensen, Jens J.

AU - Jacobsen, Karsten W.

AU - Nielsen, Jane H.

PY - 2012

Y1 - 2012

N2 - In heterogeneous catalysis, identifying the active site for key reaction steps is an important contribution for the optimization of industrial synthesis. The structure sensitivity of CO dissociation on a metal catalyst, which is the rate-limiting step for the methanation and the Fischer–Tropsch processes under certain conditions, has been debated for years. Here, scanning tunneling microscopy (STM) and density functional theory (DFT) are used to clarify the role of monatomic steps in the splitting of CO on a stepped Ru(0 1 54) crystal, which displays alternating steps with either 4-fold or 3-fold symmetry. After CO doses at elevated temperatures, the STM images reveal step decorations characteristic of atomic oxygen resulting from CO dissociation on every second step. The comparison of the STM images with the results of DFT calculations shows that the step decoration occurs on the steps displaying the 4-fold symmetry. We conclude that the active sites for CO dissociation on ruthenium are located on the 4-fold symmetry monatomic steps.

AB - In heterogeneous catalysis, identifying the active site for key reaction steps is an important contribution for the optimization of industrial synthesis. The structure sensitivity of CO dissociation on a metal catalyst, which is the rate-limiting step for the methanation and the Fischer–Tropsch processes under certain conditions, has been debated for years. Here, scanning tunneling microscopy (STM) and density functional theory (DFT) are used to clarify the role of monatomic steps in the splitting of CO on a stepped Ru(0 1 54) crystal, which displays alternating steps with either 4-fold or 3-fold symmetry. After CO doses at elevated temperatures, the STM images reveal step decorations characteristic of atomic oxygen resulting from CO dissociation on every second step. The comparison of the STM images with the results of DFT calculations shows that the step decoration occurs on the steps displaying the 4-fold symmetry. We conclude that the active sites for CO dissociation on ruthenium are located on the 4-fold symmetry monatomic steps.

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