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Título: | Ammonia-Borane dehydrogenation promoted by an osmium dihydride complex: Kinetics and mechanism |
Autor: | Esteruelas, Miguel A. CSIC ORCID; López, Ana M. CSIC ORCID; Mora, Malka CSIC ORCID; Oñate, Enrique CSIC ORCID | Fecha de publicación: | 2015 | Editor: | American Chemical Society | Citación: | ACS Catalysis 5(1): 187-191 (2015) | Resumen: | Complex 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. | Versión del editor: | http://dx.doi.org/10.1021/cs501536d | URI: | http://hdl.handle.net/10261/118271 | DOI: | 10.1021/cs501536d | ISSN: | 2155-5435 |
Aparece en las colecciones: | (ISQCH) Artículos |
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Ammonia-Boranerevised.pdf | 223,76 kB | Adobe PDF | Visualizar/Abrir |
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