Temperature Dependent CO Oxidation Mechanisms on Size-Selected Clusters

Sebastian Kunz; Florian F. Schweinberger; Vahideh Habibpour; Martin Roettgen; Christopher Harding; Matthias Arenz; Ulrich Heiz

doi:10.1021/jp911269z

Temperature Dependent CO Oxidation Mechanisms on Size-Selected Clusters

Sebastian Kunz, Florian F. Schweinberger, Vahideh Habibpour, Martin Roettgen, Christopher Harding, Matthias Arenz, Ulrich Heiz

Department of Chemistry

65 Citations (Scopus)

Abstract

Using p-MBRS experiments and TPR as well as FTIR measurements, it could be shown that dissociative oxygen activation occurs in the same temperature range for small clusters in comparison to faceted nanoparticles (NPs) and Pd single crystals. Surprisingly, CO poisoning does not take place on small Pd clusters at temperatures above 300 K. Furthermore, an oxygen activation has been found in this low temperature range which differs from the normal dissociative activation since it occurs only if CO is already adsorbed, before O₂ adsorbs. Hence, the reactivity is promoted by CO under these conditions. This is in contrast to the normal Langmuir-Hinshelwood mechanism which has previously been observed for single crystals and facted NPs. Cooperative effects in the adsorption of the reactants are most likely responsible for such unordinary behaviors.

Original language	English
Journal	Journal of Physical Chemistry Part C: Nanomaterials and Interfaces
Volume	114
Issue number	3
Pages (from-to)	1651-1654
ISSN	1932-7447
DOIs	https://doi.org/10.1021/jp911269z
Publication status	Published - 28 Jan 2010

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title = "Temperature Dependent CO Oxidation Mechanisms on Size-Selected Clusters",

abstract = "Using p-MBRS experiments and TPR as well as FTIR measurements, it could be shown that dissociative oxygen activation occurs in the same temperature range for small clusters in comparison to faceted nanoparticles (NPs) and Pd single crystals. Surprisingly, CO poisoning does not take place on small Pd clusters at temperatures above 300 K. Furthermore, an oxygen activation has been found in this low temperature range which differs from the normal dissociative activation since it occurs only if CO is already adsorbed, before O2 adsorbs. Hence, the reactivity is promoted by CO under these conditions. This is in contrast to the normal Langmuir-Hinshelwood mechanism which has previously been observed for single crystals and facted NPs. Cooperative effects in the adsorption of the reactants are most likely responsible for such unordinary behaviors.",

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T1 - Temperature Dependent CO Oxidation Mechanisms on Size-Selected Clusters

AU - Kunz, Sebastian

AU - Schweinberger, Florian F.

AU - Habibpour, Vahideh

AU - Roettgen, Martin

AU - Harding, Christopher

AU - Arenz, Matthias

AU - Heiz, Ulrich

PY - 2010/1/28

Y1 - 2010/1/28

N2 - Using p-MBRS experiments and TPR as well as FTIR measurements, it could be shown that dissociative oxygen activation occurs in the same temperature range for small clusters in comparison to faceted nanoparticles (NPs) and Pd single crystals. Surprisingly, CO poisoning does not take place on small Pd clusters at temperatures above 300 K. Furthermore, an oxygen activation has been found in this low temperature range which differs from the normal dissociative activation since it occurs only if CO is already adsorbed, before O2 adsorbs. Hence, the reactivity is promoted by CO under these conditions. This is in contrast to the normal Langmuir-Hinshelwood mechanism which has previously been observed for single crystals and facted NPs. Cooperative effects in the adsorption of the reactants are most likely responsible for such unordinary behaviors.

AB - Using p-MBRS experiments and TPR as well as FTIR measurements, it could be shown that dissociative oxygen activation occurs in the same temperature range for small clusters in comparison to faceted nanoparticles (NPs) and Pd single crystals. Surprisingly, CO poisoning does not take place on small Pd clusters at temperatures above 300 K. Furthermore, an oxygen activation has been found in this low temperature range which differs from the normal dissociative activation since it occurs only if CO is already adsorbed, before O2 adsorbs. Hence, the reactivity is promoted by CO under these conditions. This is in contrast to the normal Langmuir-Hinshelwood mechanism which has previously been observed for single crystals and facted NPs. Cooperative effects in the adsorption of the reactants are most likely responsible for such unordinary behaviors.

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DO - 10.1021/jp911269z

M3 - Journal article

SN - 1932-7447

VL - 114

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EP - 1654

JO - Journal of Physical Chemistry Part C: Nanomaterials and Interfaces

JF - Journal of Physical Chemistry Part C: Nanomaterials and Interfaces

IS - 3

ER -

Temperature Dependent CO Oxidation Mechanisms on Size-Selected Clusters

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