| Summary: | The μ-aminoborane complexes [Rh<sub>2</sub>(L<sup>R</sup>)<sub>2</sub>(μ–H)(μ–H<sub>2</sub>B=NHR')][BAr<sup>F</sup><sub>4</sub>] (L<sup>R</sup> = R<sub>2</sub>P(CH<sub>2</sub>)<sub>3</sub>PR<sub>2</sub>; R = Ph, <sup>i</sup>Pr; R' = H, Me) form by addition of H<sub>3</sub>B·NMeR'H to [Rh(L<sup>Ph</sup>)(η6–C<sub>6</sub>H<sub>5</sub>F)][BAr<sup>F</sup><sub>4</sub>]. DFT calculations demonstrate that the aminoborane interacts with the Rh centers through strong Rh–H and Rh–B interactions. Mechanistic investigations show that these dimers can form via a boronium–mediated route; and are precatalysts for amine–borane dehydropolymerization, suggesting a possible role for bimetallic motifs in catalysis.
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