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- W3169492090 abstract "We demonstrate the formation of a diverse array of organic and organometallic products containing newly formed C-C bonds via successive methyl transfers from di-, tri-, and tetramethyl Ta(V) precursors to unsaturated small molecule substrates under mild conditions. The reactions of Ta(V) methyl complexes 1-X [H2B(MesIm)2]TaMe3X (X = Me, Cl; Im = imidazole, Mes = 2,4,6-trimethylphenyl) with CO led to oxo enolate Ta(V) products, in which the enolate ligands were constructed from Ta-Me groups and two equivalents of CO. Similarly, the reaction of 1-Me with CNXyl yielded an imido enamine Ta(V) product. Surprisingly, 1-Cl reacted with CNXyl (1 equiv) at the borate backbone of the [H2B(MesIm)2] ligand with concomitant methyl transfer from the metal center to form a new, dianionic scorpionate ligand that supported a Ta(V) dimethyl chloro complex (6). Treatment of 1-Cl with further CNXyl led to an azaallyl scorpionate complex, and an imido isocyanide scorpionate complex, along with propene and xylyl ketenimine. Complex 6 reacted with CO to yield a pinacol scorpionate complex 10-a new reaction pathway in early transition metal chemistry. Mechanistic studies revealed that this proceeded via migratory insertion of CO into a Ta-Me group, followed by methyl transfer to form an η2-acetone intermediate. Elimination of acetone furnished a CO-stabilized Ta(III) intermediate capable of rebinding and subsequently coupling two equivalents of CO-derived acetone to form the pinacol ligand in 10." @default.
- W3169492090 created "2021-06-22" @default.
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- W3169492090 date "2021-06-14" @default.
- W3169492090 modified "2023-10-14" @default.
- W3169492090 title "A Diverse Array of C–C Bonds Formed at a Tantalum Metal Center" @default.
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- W3169492090 doi "https://doi.org/10.1021/acs.inorgchem.1c01159" @default.
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- W3169492090 hasPublicationYear "2021" @default.
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