Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 22, Issue 9, Pages 3000-3008Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201504439
Keywords
hydroamination; metallacycles; solid-state NMR spectroscopy; supported catalysts; tantalum
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Funding
- King Abdullah University of Science and Technology
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Single-site, well-defined, silica-supported tantallaaziridine intermediates [Si-O-Ta((2)-NRCH2)(NMe2)(2)] [R=Me (2), Ph (3)] were prepared from silica-supported tetrakis(dimethylamido)tantalum [Si-O-Ta(NMe2)(4)] (1) and fully characterized by FTIR spectroscopy, elemental analysis, and H-1,C-13 HETCOR and DQ TQ solid-state (SS) NMR spectroscopy. The formation mechanism, by -H abstraction, was investigated by SS NMR spectroscopy and supported by DFT calculations. The C-H activation of the dimethylamide ligand is favored for R=Ph. The results from catalytic testing in the hydroaminoalkylation of alkenes were consistent with the N-alkyl aryl amine substrates being more efficient than N-dialkyl amines.
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