Abstract
AbstractThe μ‐amino–borane complexes [Rh2(LR)2(μ‐H)(μ‐H2B=NHR′)][BArF4] (LR=R2P(CH2)3PR2; R=Ph, iPr; R′=H, Me) form by addition of H3B⋅NMeR′H2 to [Rh(LR)(η6‐C6H5F)][BArF4]. DFT calculations demonstrate that the amino–borane interacts with the Rh centers through strong Rh‐H and Rh‐B interactions. Mechanistic investigations show that these dimers can form by a boronium‐mediated route, and are pre‐catalysts for amine‐borane dehydropolymerization, suggesting a possible role for bimetallic motifs in catalysis.
Highlights
Polyamino-boranes ([H2BNRH]n) are potentially exciting new materials that are isoelectronic with technologically pervasive polyolefins, but are chemically distinct because ofHBÀNH(d +) polarization
There is recent evidence that these processes occur at a metal center in which the catalyst needs to perform two roles: 1) formal dehydrogenation of amine-borane to form a latent source of amino-borane (H2B=NRH), and 2) subsequent BÀN bond formation.[2,3,4,5,6]
We report that H2B=NH2 can be trapped by a bimetallic [Rh2(R2PCH2CH2CH2PR2)2]2+ fragment to give a novel bridging amino-borane bonding motif
Summary
Polyamino-boranes ([H2BNRH]n) are potentially exciting new materials that are isoelectronic with technologically pervasive polyolefins, but are chemically distinct because of (dÀ)HBÀNH(d +) polarization. This motif, which is similar to that observed for D, is fully consistent with the low temperature NMR data, and are recreated well in the DFT calculated structure (Supporting Information, Figures S24–26).
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