Reactivity of surface intermediates derived from Al2O3-supported Ru3(CO)12 in the CO + H2 reaction

A. Beck, S. Dobos, L. Guczi

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27 Citations (Scopus)

Abstract

The effect of subcarbonyl surface intermediates resulting from Ru3(CO)12 molecular clusters supported on Al2O3 in the CO hydrogenation has been investigated by using an isotope-labeling technique. It has been established that single ruthenium atoms are stabilized in the form of dicarbonyl species, characterized by 2072- and 2001-cm-1 IR frequencies, when temperature-programmed decomposition (TPDE) is carried out in the temperature range between 473 and 573 K. Despite the presence of RuII(CO)2, free ruthenium sites are responsible for the catalytic activity in the 13CO hydrogenation reaction. The high mobility of the CO ligands in the surface ruthenium dicarbonyl species, demonstrated by CO molecular exchange during the reaction, makes the CO from the dicarbonyl species compete successfully with that chemisorbed from the gas phase labeled in the form of 13CO. An explanation for the stability of the highly dispersed ruthenium particles and detailed mechanisms of the surface reactions are given.

Original languageEnglish
Pages (from-to)3220-3226
Number of pages7
JournalInorganic Chemistry
Volume27
Issue number18
Publication statusPublished - 1988

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Carbon Monoxide
ruthenium
Ruthenium
reactivity
hydrogenation
Hydrogenation
molecular clusters
surface reactions
marking
catalytic activity
isotopes
Surface reactions
vapor phases
decomposition
Isotopes
Labeling
ligands
temperature
Catalyst activity
Gases

ASJC Scopus subject areas

  • Inorganic Chemistry

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Reactivity of surface intermediates derived from Al2O3-supported Ru3(CO)12 in the CO + H2 reaction. / Beck, A.; Dobos, S.; Guczi, L.

In: Inorganic Chemistry, Vol. 27, No. 18, 1988, p. 3220-3226.

Research output: Contribution to journalArticle

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N2 - The effect of subcarbonyl surface intermediates resulting from Ru3(CO)12 molecular clusters supported on Al2O3 in the CO hydrogenation has been investigated by using an isotope-labeling technique. It has been established that single ruthenium atoms are stabilized in the form of dicarbonyl species, characterized by 2072- and 2001-cm-1 IR frequencies, when temperature-programmed decomposition (TPDE) is carried out in the temperature range between 473 and 573 K. Despite the presence of RuII(CO)2, free ruthenium sites are responsible for the catalytic activity in the 13CO hydrogenation reaction. The high mobility of the CO ligands in the surface ruthenium dicarbonyl species, demonstrated by CO molecular exchange during the reaction, makes the CO from the dicarbonyl species compete successfully with that chemisorbed from the gas phase labeled in the form of 13CO. An explanation for the stability of the highly dispersed ruthenium particles and detailed mechanisms of the surface reactions are given.

AB - The effect of subcarbonyl surface intermediates resulting from Ru3(CO)12 molecular clusters supported on Al2O3 in the CO hydrogenation has been investigated by using an isotope-labeling technique. It has been established that single ruthenium atoms are stabilized in the form of dicarbonyl species, characterized by 2072- and 2001-cm-1 IR frequencies, when temperature-programmed decomposition (TPDE) is carried out in the temperature range between 473 and 573 K. Despite the presence of RuII(CO)2, free ruthenium sites are responsible for the catalytic activity in the 13CO hydrogenation reaction. The high mobility of the CO ligands in the surface ruthenium dicarbonyl species, demonstrated by CO molecular exchange during the reaction, makes the CO from the dicarbonyl species compete successfully with that chemisorbed from the gas phase labeled in the form of 13CO. An explanation for the stability of the highly dispersed ruthenium particles and detailed mechanisms of the surface reactions are given.

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