Isomeric [RuCl2(dmso)2(indazole)2] complexes: Ruthenium(II)-mediated coupling reaction of acetonitrile with 1H-indazole

Erwin Reisner, Vladimir B. Arion, Anna Rufińska, Ion Chiorescu, Wolfgang F. Schmid, Bernhard K. Keppler

    Research output: Contribution to journalArticlepeer-review

    Abstract

    Reaction of the antitumor complex trans-[RuIIICl 4(Hind)2]- (Hind = indazole) with an excess of dimethyl sulfoxide (dmso) in acetone afforded the complex trans,trans,trans- [RuIICl2(dmso)2(Hind)2] (1). Two other isomeric compounds trans,cis,cis-[RuIICl2(dmso) 2(Hind)2] (2) and cis,cis,cis-[RuIICl 2(dmso)2(Hind)2] (3) have been obtained on refluxing cis-[RuIICl2(dmso)4] with 2 equiv. of indazole in ethanol and methanol, respectively. Isomers 1 and 2 react with acetonitrile yielding the complexes trans-[RuIICl2(dmso) (Hind){HN=C(Me)ind}]·CH3CN (4·CH3CN) and trans,cis-[RuIICl2(dmso)2{HN=C(Me)ind}] ·H2O (5·H2O), respectively, containing a cyclic amidine ligand resulting from insertion of the acetonitrile C≡N group in the N1-H bond of the N2-coordinated indazole ligand in the nomenclature used for 1H-indazole. These are the first examples of the metal-assisted iminoacylation of indazole. The products isolated have been characterized by elemental analysis, IR spectroscopy, UV-vis spectroscopy, electrospray mass-spectrometry, thermogravimetry, differential scanning calorimetry, 1H NMR spectroscopy, and solid-state 13C CP MAS NMR spectroscopy. The isomeric structures of 1-3 and the presence of a chelating amidine ligand in 4 and 5 have been confirmed by X-ray crystallography. The electrochemical behavior of 1-5 and the formation of 5 have been studied by cyclic voltammetry. © The Royal Society of Chemistry 2005.
    Original languageEnglish
    Pages (from-to)2355-2364
    Number of pages9
    JournalDalton Transactions
    Issue number14
    DOIs
    Publication statusPublished - 21 Jul 2005

    Keywords

    • Diastereomers (geometric
    • prepn. and crystal structure and optimized geometry and electronic structure and cyclic voltammetry and indazole-acetonitrile coupling reaction of isomeric ruthenium DMSO indazole complexes)
    • Acylation (mechanism
    • metal-assisted iminoacylation of isomeric ruthenium DMSO indazole complexes on reaction with acetonitrile)
    • Crystal structure
    • Molecular structure
    • Oxidation
    • Oxidation potential (of ruthenium DMSO complexes with indazole/amidine)
    • Molecular orbital
    • Total energy (of ruthenium DMSO indazole isomeric complexes)
    • Hydrogen bond (of ruthenium DMSO indazole/amidine complexes)
    • Molecular structure (optimized
    • of ruthenium DMSO indazole isomeric complexes)
    • ruthenium indazole DMSO isomeric complex prepn structure coupling acetonitrile
    • amidine ruthenium DMSO complex prepn structure
    • crystal structure ruthenium DMSO indazole amidine complex
    • geometry optimized ruthenium DMSO indazole isomeric complex
    • electronic structure ruthenium DMSO indazole isomeric complex
    • cyclic voltammetry ruthenium DMSO indazole amidine complex
    • iminoacylation ruthenium DMSO indazole isomeric complex

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