Synthesis and Redox Chemistry of a Tantalum Alkylidene Complex Bearing a Metallaimidazole Ring

Benjamin M. Kriegel, Nikolas Kaltsoyannis, Ruchira Chatterjee, Robert G Bergman, John Arnold

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    Abstract

    The cyclometalated tantalum(V) terminal hydride complex {ArNC(Me)CHC(Me)N[2-(CHMeCH2)-6-iPr-C6H3]}(η2-N(Xyl)CH)Ta(NtBu) reacts cleanly with 2 equiv of 2,6-dimethylphenyl isocyanide via migratory insertion to give a product containing a unique metallaimidazole ring. This complex can be reversibly oxidized by one electron, either electrochemically or chemically, to give a tantalum radical cation species. DFT calculations, as well as X-ray crystallographic and EPR spectroscopic data, are consistent with the electron being removed from an orbital primarily composed of Ta–C π-bonding character but also delocalized over the tantalaimidazole ring.
    Original languageEnglish
    Pages (from-to)3520–3529
    JournalOrganometallics
    Volume36
    Early online date21 Aug 2017
    DOIs
    Publication statusPublished - 2017

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