Die intermolekulare Aktivierung vonn-Alkanen durch einen dreikernigen Ru-Pentahydrid-Komplex – Bildung voncloso-Ruthenacyclopentadienkomplexen

Inagaki, Akiko; Takemori, Tamiki; Tanaka, Masako; Suzuki, Hiroharu

doi:10.1002/(sici)1521-3757(20000117)112:2<411::aid-ange411>3.0.co;2-a

Angewandte Chemie

2000

DOI: 10.1002/(sici)1521-3757(20000117)112:2<411::aid-ange411>3.0.co;2-a

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Die intermolekulare Aktivierung vonn-Alkanen durch einen dreikernigen Ru-Pentahydrid-Komplex – Bildung voncloso-Ruthenacyclopentadienkomplexen

Akiko Inagaki

Tamiki Takemori

Masako Tanaka

et al.

Abstract: Durch schrittweise Aktivierung der C‐H‐Bindungen von n‐Alkanen an einem dreikernigen Rutheniumcluster werden insgesamt sechs C‐H‐Bindungen gespalten und es entstehen closo‐Ruthenacyclopentadienkomplexe (siehe Struktur des mit Hexan erhaltenen Komplexes).

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Cited by 12 publications

References 31 publications

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[{(η5-C5Me5)Fe}2(μ-H)4]: A Novel Dinuclear Iron Tetrahydrido Complex

Ohki

Suzuki

2000

Angewandte Chemie

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Transition metal cluster complexes have attracted attention because of their potential ability for cooperative and effective activation of substrates in a multimetallic site. [1] We have used the term ªmultimetallic activationº to refer to a mode of activation achieved as a result of cooperative action of many metal centers. Our research on multimetallic activation began as an attempt to prepare a cluster with bridging hydrido ligands. As a result, we synthesized a new class of ruthenium polyhydrido clusters, 1 and 2, and demonstrated many examples of multimetallic activation through the reaction with unsaturated hydrocarbons, silanes, and phosphanes as well as alkanes. [2] According to the vertical trends associated with the transition elements, the metal ± metal and metal ± ligand bond enthalpies increase down a column and the complexes become more substitutionally inert. The iron analogues of these ruthenium polyhydrido clusters are, therefore, expected to be much more reactive. So far there have been no examples of an iron polyhydrido cluster which has only cyclopentadienyl derivatives (h 5 -C 5 R 5 ) as ancillary ligands. Here we report the first synthesis and brief reaction chemistry of the highly reactive and unstable dinuclear iron tetrahydrido complex [{(h 5 -C 5

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[{(η5-C5Me5)Fe}2(μ-H)4]: A Novel Dinuclear Iron Tetrahydrido Complex

Ohki

Suzuki

2000

Angewandte Chemie

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Alkene C−H Activations at Dinuclear Complexes Promoted by Oxidation

et al. 2002

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Several recent discoveries in the chemistry of transition metal di-and polynuclear complexes have disclosed new methods of hydrocarbon activation and functionalization, favored by polynuclear environments. [1,2] In parallel, considerable progress has been made in understanding the reactivity features resulting from multimetallic reaction sites. [1, 3,4] Together, such advances may contribute to the rational design of new catalysts and applications based on this type of compound. However, the proximity of the metal centers is likely to have significant repercussions for the reactivity, which remain to be determined.In our recent studies on ™open-book∫ d 8 diiridium complexes with N-donor bridges, we have observed a remarkable substrate selectivity in the reactions of these compounds towards oxidative addition reactants. Whereas the d 8 diiridium complexes underwent fast S N 2 oxidative additions with substrates such as halocarbons, [4] the additions of less-polar reactants such as dihydrogen were not observed. The oxidation of these d 8 d 8 diiridium compounds, to species of d 6 d 8 or d 7 d 7 electronic configurations, gave dihydrogen-activating compounds. [5] Here we report that such an oxidation strategy also allows the transformation of nonreactive d 8 d 8 compounds into dinuclear CÀH activating species.The treatment of the diamidonaphthalene ((NH 2 )naphth)bridged diiridium (iii) complex [Ir 2 (m-1,8-(NH) 2 naphth)-(m-H)H 3 (NCCH 3 )(PiPr 3 ) 2 ] (1) with two equivalents of an internal alkyne such as 2-butyne or diphenylacetylene afforded diiridium(i) derivatives of the formula [Ir 2 (m-1,8-(NH) 2 naphth)(h 2 -Z-RHCCHR) 2 (PiPr 3 ) 2 ] (R Me (2), Ph (3)) [Eq. (1)]. The solution NMR spectra of both compounds indicate symmetric C 2 structures with a transoid arrangement of nonrotating Z-alkene ligands. These features have been confirmed by the X-ray crystallographic determination of the structure of 2, [6] (Figure 1). reaction see: M. AlajarÌn, C. Conesa, H. S. Rzepa, J. Chem. Soc.

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A Novel Dinuclear Ruthenium Complex Bridged through a Substituted Phenazine Ligand Formed by Ruthenium-Promoted Oxidative Assembly of 1,3-Diaminobenzene

Majumdar¹,

Falvello²,

Tomás³

et al. 2001

Chem. Eur. J.

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The reaction of [Ru(acac)3] (acac = acetylacetonate) with molten 1,3-diaminobenzene affords the crystalline monometallic compound [Ru(L1)-(acac)21 (1: L1 = N-(3'-aminophenyl)1,2-(3-amino)benzoquinone diimine) along with an unstable dimetallic compound [Ru2(mu-L2)(acac)4] (2: L2=N-4,6-bis(3'-aminophenyl)imino-3,5-diimino-hex-1-ene). Compound 2 transforms to a stable dimetallic compound [Ru2(mu-L3)(acac)4] (3: L3 = 2-amino-6(3'-aminophenyl)imino-9-imino-phenazine) in boiling 2-methoxyethanol. The above compounds are formed by ruthenium-mediated oxidative di- or trimerization of the diamine with the formation of several new C-N bonds. The products have been thoroughly characterized. FAB mass spectra, along with other physicochemical data, were used for their formulations. The compounds 1, 2, and 3 display intense peaks due to their parent molecular ions at m/z 512, 916, and 914, respectively. Final characterization of complex 3 was made by single-crystal X-ray structure determination. The structure of 3 confirmed the formation of three new C-N bonds and the bridging ligand L3 from 1,3-diaminobenzene. The conversion, 2 --> 3 is an oxidative ring-closure reaction, which is associated with dehydrogenation reactions. The monometallic compound 1, showed a reversible metal-based anodic response at 0.35 V. On the other hand, both the compounds 2 and 3 showed a pair of well-resolved metal-based anodic oxidations, for which the separation between the two successive anodic responses were high (>0.4 V). In addition, all of them showed multiple cathodic responses that were in the range -1.0 to -2.0 V.

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Die intermolekulare Aktivierung vonn-Alkanen durch einen dreikernigen Ru-Pentahydrid-Komplex – Bildung voncloso-Ruthenacyclopentadienkomplexen

Abstract: Durch schrittweise Aktivierung der C‐H‐Bindungen von n‐Alkanen an einem dreikernigen Rutheniumcluster werden insgesamt sechs C‐H‐Bindungen gespalten und es entstehen closo‐Ruthenacyclopentadienkomplexe (siehe Struktur des mit Hexan erhaltenen Komplexes).

Cited by 12 publications

References 31 publications

[{(η5-C5Me5)Fe}2(μ-H)4]: A Novel Dinuclear Iron Tetrahydrido Complex

[{(η5-C5Me5)Fe}2(μ-H)4]: A Novel Dinuclear Iron Tetrahydrido Complex

Alkene C−H Activations at Dinuclear Complexes Promoted by Oxidation

A Novel Dinuclear Ruthenium Complex Bridged through a Substituted Phenazine Ligand Formed by Ruthenium-Promoted Oxidative Assembly of 1,3-Diaminobenzene

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