Six-, Five-, and Four-Coordinate Ruthenium(II) Hydride Complexes Supported by N-Heterocyclic Carbene Ligands: Synthesis, Characterization, Fundamental Reactivity, and Catalytic Hydrogenation of Olefins, Aldehydes, and Ketones

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This article discusses six-, five-, and four-coordinate ruthenium(II) hydride complexes.

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18 p.

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Lee, John P.; Ke, Zhuofeng; Ramírez, Magaly A.; Gunnoe, T. Brent; Cundari, Thomas R., 1964-; Boyle, Paul D. et al. February 20, 2009.

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This article discusses six-, five-, and four-coordinate ruthenium(II) hydride complexes.

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18 p.

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Reprinted with permission from Organometallics. Copyright 2009 American Chemical Society.

Abstract: The Ru(II) hydride complex (IMes)2Ru(Cl)(H)(CO) (1) {IMes = 1,3-bis-(2,4,6-trimethylphenyl)imidazol-2-ylidene} was synthesized from [Ru(CO)2Cl2]n and free IMes. Complex 1 rapidly reacts with CO to produce the cis-dicarbonyl Ru(II) complex (IMes)2Ru(Cl)(H)(CO)2 (2). The reaction of 1 with NaBAr'4 {Ar' = 3,5-(CF3)C6H3} produces the four-coordinate Ru(II) cationic complex [(IMes)2Ru(H)(CO)][BAr'4] (4), which can be trapped by two equivalents of tert-butylisonitrile to produce [(IMes)2Ru(H)(CO)(CNtBu)2][BAr'4] (5). Experimental and computational studies suggest that complex 4 is a diamagnetic system that adopts a sawhorse structure. The hydride ligand of complex 2 is readily displaced as dihydrogen upon reaction with HCI to produce (IMes)2Ru(CI)2(CO)2 (3). Both complex 1 and 4 were found to react with D2 (30 psi) at room temperature to produce the isotopomers (IMes)2Ru(CI)(D)(CO) (1-d1) and [(IMes)2Ru(D)(CO)][BAr'4] (4-d1), respectively, with the rate of formation of 4-d1 at least 28 times faster than the conversion of 1/D2 to 1-d1. In the presence of excess D2 complex 4 reversibly incorporates deuterium into the ortho methyl groups of the IMes ligands, whereas complex 1 does not show evidence of H/D exchange with the IMes ligands. Both 1 and 4 were found to catalyze the hydrogenation of olefins, ketones, and aldehydes.

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  • Organometallics, 2009, Washington DC: American Chemical Society, pp. 1758-1775

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  • Publication Title: Organometallics
  • Volume: 28
  • Page Start: 1758
  • Page End: 1775
  • Pages: 18
  • Peer Reviewed: Yes

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  • February 20, 2009

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  • March 9, 2012, 2:17 p.m.

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Lee, John P.; Ke, Zhuofeng; Ramírez, Magaly A.; Gunnoe, T. Brent; Cundari, Thomas R., 1964-; Boyle, Paul D. et al. Six-, Five-, and Four-Coordinate Ruthenium(II) Hydride Complexes Supported by N-Heterocyclic Carbene Ligands: Synthesis, Characterization, Fundamental Reactivity, and Catalytic Hydrogenation of Olefins, Aldehydes, and Ketones, article, February 20, 2009; [Washington, D.C.]. (https://digital.library.unt.edu/ark:/67531/metadc77193/: accessed February 12, 2025), University of North Texas Libraries, UNT Digital Library, https://digital.library.unt.edu; crediting UNT College of Arts and Sciences.

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