5 years ago

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

Synthesis and Redox Chemistry of a Tantalum Alkylidene Complex Bearing a Metallaimidazole Ring
John Arnold, Ruchira Chatterjee, Nikolas Kaltsoyannis, Robert G. Bergman, Benjamin M. Kriegel
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.

Publisher URL: http://dx.doi.org/10.1021/acs.organomet.7b00448

DOI: 10.1021/acs.organomet.7b00448

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