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N-Heterocyclic Carbene Stabilized trans-Dihydrido Aqua and Ethanol Complexes of Ruthenium: Precursors to Complexes with Ru-Heteroatom Bonds


Reference:

Jazzar, R. F. R., Bhatia, P. H., Mahon, M. F. and Whittlesey, M. K., 2003. N-Heterocyclic Carbene Stabilized trans-Dihydrido Aqua and Ethanol Complexes of Ruthenium: Precursors to Complexes with Ru-Heteroatom Bonds. Organometallics, 22 (4), pp. 670-683.

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Abstract

Attempts to isolate the bis-N-heterocyclic carbene complex Ru(AsPh3)(IMes)2(CO)H2 (IMes = bis(1,3-(2,4,6-trimethylphenyl)imidazol-2-ylidene)) by crystn. with either ethanol or hexane yields instead the ethanol and water complexes Ru(IMes)2(CO)(EtOH)H2 (1) and Ru(IMes)2(CO)(H2O)H2 (2), resp. Both multinuclear NMR spectroscopy and x-ray crystallog. demonstrate that these two compds. are isostructural with a trans arrangement of the hydride ligands. Thermolysis of 1 results in decarbonylation of the bound ethanol ligand to yield Ru(IMes)2(CO)2H2 (3). Substitution of the coordinated solvent ligands in 1 or 2 occurs readily with p-ethoxyphenol to give Ru(IMes)2(CO)(HOC6H4-p-OEt)H2 (4), while treatment of 2 with 1-propanethiol affords the thiol complex Ru(IMes)2(CO)(HSCH2CH2CH3)H2 (8). Reaction of 8 with CO gives the thiolate hydride species Ru(IMes)2(CO)2(SCH2CH2CH3)H (9), whereas addn. of CO to either 1 or 2 affords Ru(IMes)2(CO)3 (5). The hydroxy hydride complex Ru(IMes)2(CO)2(OH)H (6) has been isolated as an intermediate on the pathway from 2 to 5. Addn. of CO2 or p-HO2CC5H4N to solns. of 2 yields the bicarbonate complex Ru(IMes)2(CO)(k2-O2COH)H (10) and the isonicotinate species Ru(IMes)2(CO)(k2-O2CC5H4N)H (11), resp. Addn. of CO to 10 affords Ru(IMes)2(CO)2(h1-O2COH)H (7). Treatment of complex 2 with excess acetonitrile yields the N-imidoylimidato complex Ru(IMes)2(CO)(NH:C(CH3)N:C(CH3)O)H (12), which arises from the formal addn. of two mols. of acetonitrile in head-to-tail fashion across the RuO-H bond. Compds. 1, 2, 6, 7, 8, 9, 11, and 12 have been structurally characterized by single-crystal x-ray diffraction.

Details

Item Type Articles
CreatorsJazzar, R. F. R., Bhatia, P. H., Mahon, M. F. and Whittlesey, M. K.
Uncontrolled Keywordsprep (preparation), ethanol, crystal structure, ract (reactant or reagent) (prepn. and structures of nitrogen heterocyclic carbene stabilized trans-dihydrido aqua and ethanol complexes of ruthen, nitrogen heterocyclic carbene stabilized trans dihydrido aqua ethanol ruthenium, molecular structure (of nitrogen heterocyclic carbene stabilized trans-dihydrido aqua, prp (properties), carbene complexes role, and related complexes of ruthenium), crystal mol structure nitrogen heterocyclic carbene stabilized ruthenium complex, spn (synthetic preparation), rct (reactant)
DepartmentsFaculty of Science > Chemistry
RefereedYes
StatusPublished
ID Code5010

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