Rhodium amine-borane sigma-complexes of H3BNHMe2 have been isolated which are potential intermediates in the catalytic dehydrogenation of H3B.NHMe2.
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A d Ag(i) amine-borane σ-complex and comparison with a d Rh(i) analogue: structures on the η to η:η continuum.
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Chemistry Research Laboratories, Department of Chemistry, University of Oxford, Oxford, OX1 3TA, UK.
H3B·NMe3 σ-complexes of d8 [(L1)Rh][BArF4] and d10 [(L1)Ag][BArF4] (where L1 = 2,6-bis-[1-(2,6-diisopropylphenylimino)ethyl]pyridine) have been prepared and structurally characterised. Analysis of the molecular and electronic structures reveal important but subtle differences in the nature of the bonding in these σ-complexes, which differ only by the identity of the metal centre and the d-electron count. With Rh the amine-borane binds in an η2:η2 fashion, whereas at Ag the unsymmetrical {AgH3B·NMe3} unit suggests a structure lying between the η2:η2 and η1 extremes.
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Department of Chemistry, University of Oxford, Mansfield Road, Oxford, OX1 3TA (UK).
The coordination chemistry of the 1,2-BN-cyclohexanes 2,2-R2 -1,2-B,N-C4 H10 (R2 =HH, MeH, Me2 ) with Ir and Rh metal fragments has been studied. This led to the solution (NMR spectroscopy) and solid-state (X-ray diffraction) characterization of [Ir(PCy3 )2 (H)2 (η(2) η(2) -H2 BNR2 C4 H8 )][BAr(F) 4 ] (NR2 =NH2 , NMeH) and [Rh(iPr2 PCH2 CH2 CH2 PiPr2 )(η(2) η(2) -H2 BNR2 C4 H8 )][BAr(F) 4 ] (NR2 =NH2 , NMeH, NMe2 ). For NR2 =NH2 subsequent metal-promoted, dehydrocoupling shows the eventual formation of the cyclic tricyclic borazine [BNC4 H8 ]3 , via amino-borane and, tentatively characterized using DFT/GIAO chemical shift calculations, cycloborazane intermediates.
View Article and Find Full Text PDFMonomeric and oligomeric amine-borane sigma-complexes of rhodium. intermediates in the catalytic dehydrogenation of amine-boranes.
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Department of Chemistry, Inorganic Chemisty Laboratories, University of Oxford, Oxford OX1 3QR, UK.
A combined experimental/quantum chemical investigation of the transition metal-mediated dehydrocoupling reaction of H(3)B.NMe(2)H to ultimately give the cyclic dimer [H(2)BNMe(2)](2) is reported. Intermediates and model complexes have been isolated, including examples of amine-borane sigma-complexes of Rh(I) and Rh(III).
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CNRS, Laboratoire de Chimie de Coordination, 205 route de Narbonne, F-31077 Toulouse, France.
Hydrogen, the simplest element in the periodic table, plays a tremendous role in organic and inorganic chemistry. For years, it was inconceivable that dihydrogen could be bound to a metal center without breaking the H-H bond. Thus, oxidative addition of H(2) was universally recognized as a key elementary step in hydrogenation processes.
View Article and Find Full Text PDFAmine-borane sigma-complexes of rhodium. relevance to the catalytic dehydrogenation of amine-boranes.
J Am Chem Soc
November 2008
Department of Chemistry, Inorganic Chemistry Laboratories, University of Oxford, UK.
Rhodium amine-borane sigma-complexes of H3BNHMe2 have been isolated which are potential intermediates in the catalytic dehydrogenation of H3B.NHMe2.
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