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Título: | Preparation and degradation of rhodium and iridium diolefin catalysts for the acceptorless and base-free dehydrogenation of secondary alcohols |
Autor: | Buil, María L. CSIC ORCID; Collado, Alba CSIC ORCID; Esteruelas, Miguel A. CSIC ORCID; Gómez-Gallego, Mar; Izquierdo, Susana CSIC ORCID; Nicasio, Antonio I. CSIC ORCID; Oñate, Enrique CSIC ORCID; Sierra, Miguel A. CSIC ORCID | Fecha de publicación: | 2021 | Editor: | American Chemical Society | Citación: | Organometallics 40(7): 989-1003 (2021) | Resumen: | Rhodium and iridium diolefin catalysts for the acceptorless and base-free dehydrogenation of secondary alcohols have been prepared, and their degradation has been investigated, during the study of the reactivity of the dimers [M(μ-Cl)(η4-C8H12)]2 (M = Rh (1), Ir (2)) and [M(μ-OH)(η4-C8H12)]2 (M = Rh (3), Ir (4)) with 1,3-bis(6′-methyl-2′-pyridylimino)isoindoline (HBMePHI). Complex 1 reacts with HBMePHI, in dichloromethane, to afford equilibrium mixtures of 1, the mononuclear derivative RhCl(η4-C8H12){κ1-Npy-(HBMePHI)} (5), and the binuclear species [RhCl(η4-C8H12)]2{μ-Npy,Npy-(HBMePHI)} (6). Under the same conditions, complex 2 affords the iridium counterparts IrCl(η4-C8H12){κ1-Npy-(HBMePHI)} (7) and [IrCl(η4-C8H12)]2{μ-Npy,Npy-(HBMePHI)} (8). In contrast to chloride, one of the hydroxide groups of 3 and 4 promotes the deprotonation of HBMePHI to give [M(η4-C8H12)]2(μ-OH){μ-Npy,Niso-(BMePHI)} (M = Rh (9), Ir (10)), which are efficient precatalysts for the acceptorless and base-free dehydrogenation of secondary alcohols. In the presence of KOtBu, the [BMePHI]− ligand undergoes three different degradations: alcoholysis of an exocyclic isoindoline-N double bond, alcoholysis of a pyridyl-N bond, and opening of the five-membered ring of the isoindoline core. | Versión del editor: | https://doi.org/10.1021/acs.organomet.1c00068 | URI: | http://hdl.handle.net/10261/237746 | DOI: | 10.1021/acs.organomet.1c00068 | E-ISSN: | 1520-6041 |
Aparece en las colecciones: | (ISQCH) Artículos |
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