Facile hydrogenation of acenapthylenes and azulenes on the face of a triruthenium carbonyl moiety: Discovery of specific reactions on the cluster framework providing unique insight for cluster catalysis

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Abstract

Activation of molecular hydrogen by triruthenium carbonyl clusters bearing acenaphthylene or aceanthrylene as the face-capping ligand results in partial hydrogenation of these polyaromatic ligands, giving the corresponding hydride carbonyl clusters bound to hydrogenated acenaphthylene or aceanthrylene. The first isolation of 4,5-dihydroacenaphthylene or 4,5-dihydroaceanthrylene was achieved by treatment of the resulting hydride carbonyl clusters with CO. Similarly, triruthenium carbonyl species bearing substituted azulenes as the face-capping moiety gives the corresponding hydride carbonyl cluster bearing partially hydrogenated azulenes at room temperature; the corresponding partial hydrogenation of azulenes does not occur with di-or tetraruthenium homologues. Hydrogenation of di-, tri-, and tetraruthenium carbonyl clusters bearing substituted azulenes at elevated temperatures furnishes hydrogenative cluster fragmentation to mononuclear ruthenium hydrides; the stereochemistry of these complexes suggests that the reaction takes place through the activation of H 2 by the multinuclear species. The roles of the acenaphthylene or azulene ligands as hemilabile μ 3 -ligands for triruthenium carbonyl clusters are discussed.

Original languageEnglish
Pages (from-to)1225-1239
Number of pages15
JournalMonatshefte fur Chemie
Volume131
Issue number12
DOIs
Publication statusPublished - Jan 1 2000

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Azulenes
Bearings (structural)
Hydrides
Catalysis
Hydrogenation
Ligands
Chemical activation
Stereochemistry
Ruthenium
Carbon Monoxide
Hydrogen
Temperature
acenaphthylene

All Science Journal Classification (ASJC) codes

  • Chemistry(all)

Cite this

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abstract = "Activation of molecular hydrogen by triruthenium carbonyl clusters bearing acenaphthylene or aceanthrylene as the face-capping ligand results in partial hydrogenation of these polyaromatic ligands, giving the corresponding hydride carbonyl clusters bound to hydrogenated acenaphthylene or aceanthrylene. The first isolation of 4,5-dihydroacenaphthylene or 4,5-dihydroaceanthrylene was achieved by treatment of the resulting hydride carbonyl clusters with CO. Similarly, triruthenium carbonyl species bearing substituted azulenes as the face-capping moiety gives the corresponding hydride carbonyl cluster bearing partially hydrogenated azulenes at room temperature; the corresponding partial hydrogenation of azulenes does not occur with di-or tetraruthenium homologues. Hydrogenation of di-, tri-, and tetraruthenium carbonyl clusters bearing substituted azulenes at elevated temperatures furnishes hydrogenative cluster fragmentation to mononuclear ruthenium hydrides; the stereochemistry of these complexes suggests that the reaction takes place through the activation of H 2 by the multinuclear species. The roles of the acenaphthylene or azulene ligands as hemilabile μ 3 -ligands for triruthenium carbonyl clusters are discussed.",
author = "Hideo Nagashima",
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N2 - Activation of molecular hydrogen by triruthenium carbonyl clusters bearing acenaphthylene or aceanthrylene as the face-capping ligand results in partial hydrogenation of these polyaromatic ligands, giving the corresponding hydride carbonyl clusters bound to hydrogenated acenaphthylene or aceanthrylene. The first isolation of 4,5-dihydroacenaphthylene or 4,5-dihydroaceanthrylene was achieved by treatment of the resulting hydride carbonyl clusters with CO. Similarly, triruthenium carbonyl species bearing substituted azulenes as the face-capping moiety gives the corresponding hydride carbonyl cluster bearing partially hydrogenated azulenes at room temperature; the corresponding partial hydrogenation of azulenes does not occur with di-or tetraruthenium homologues. Hydrogenation of di-, tri-, and tetraruthenium carbonyl clusters bearing substituted azulenes at elevated temperatures furnishes hydrogenative cluster fragmentation to mononuclear ruthenium hydrides; the stereochemistry of these complexes suggests that the reaction takes place through the activation of H 2 by the multinuclear species. The roles of the acenaphthylene or azulene ligands as hemilabile μ 3 -ligands for triruthenium carbonyl clusters are discussed.

AB - Activation of molecular hydrogen by triruthenium carbonyl clusters bearing acenaphthylene or aceanthrylene as the face-capping ligand results in partial hydrogenation of these polyaromatic ligands, giving the corresponding hydride carbonyl clusters bound to hydrogenated acenaphthylene or aceanthrylene. The first isolation of 4,5-dihydroacenaphthylene or 4,5-dihydroaceanthrylene was achieved by treatment of the resulting hydride carbonyl clusters with CO. Similarly, triruthenium carbonyl species bearing substituted azulenes as the face-capping moiety gives the corresponding hydride carbonyl cluster bearing partially hydrogenated azulenes at room temperature; the corresponding partial hydrogenation of azulenes does not occur with di-or tetraruthenium homologues. Hydrogenation of di-, tri-, and tetraruthenium carbonyl clusters bearing substituted azulenes at elevated temperatures furnishes hydrogenative cluster fragmentation to mononuclear ruthenium hydrides; the stereochemistry of these complexes suggests that the reaction takes place through the activation of H 2 by the multinuclear species. The roles of the acenaphthylene or azulene ligands as hemilabile μ 3 -ligands for triruthenium carbonyl clusters are discussed.

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