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Ammonia-Borane dehydrogenation promoted by an osmium dihydride complex: Kinetics and mechanism

AuthorsEsteruelas, Miguel A. ; López, Ana M. ; Mora, Malka ; Oñate, Enrique
Issue Date2015
PublisherAmerican Chemical Society
CitationACS Catalysis 5(1): 187-191 (2015)
AbstractComplex OsH2(CO)(PiPr3)2, generated from OsH2(CO)(η2-CH2═CHEt)(PiPr3)2 by dissociation of the olefin, promotes the release of 1 equiv of H2 from ammonia-borane and the formation of polyaminoborane. The dehydrogenation rate law is of the form d[H2]/dt = k[Os] with activation parameters of ΔH‡ = 19.6 ± 2.5 kcal·mol–1 and ΔS‡ = 6 ± 9 cal·mol–1·K–1. On the basis of kinetic results, spectroscopic NMR observations, and DFT calculations, the dihydride-dihydrogen derivative OsH2(η2-H2)(CO)(PiPr3)2 is proposed as a key intermediate for the dehydrogenation. Its formation involves the concerted BH- and NH-hydrogen transfers from the amine-borane to the metal center and to a hydride ligand, respectively.
Publisher version (URL)http://dx.doi.org/10.1021/cs501536d
Appears in Collections:(ISQCH) Artículos
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