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    Por favor, use este identificador para citar o enlazar este ítem:http://uvadoc.uva.es/handle/10324/21756

    Título
    Some Singular Features of Gold Catalysis: Protection of AuI Catalysts by Substoichiometric Agents, and Associated Phenomena
    Autor
    Bartolomé Albistegui, María del CaminoAutoridad UVA Orcid
    Ramiro Mangas, Zoraida Rosa
    Peñas de Frutos, Marconi NicolásAutoridad UVA Orcid
    Espinet Rubio, PabloAutoridad UVA Orcid
    Año del Documento
    2016
    Editorial
    American Chemical Society
    Descripción
    Producción Científica
    Documento Fuente
    ACS Catalysis 2016, 6 (10), pp 6537–6545
    Zusammenfassung
    This study deals with two striking phenomena: the complete protection against decomposition of hypothetically monocoordinated AuI intermediates [AuL]Y (L = strongly coordinating ligand; Y– = poorly coordinating anion) by addition of small substoichiometric amounts (5 mol% relative to Au) of not strongly coordinating ligands (e.g. AsPh3), and the fact that, in contrast, strongly coordinating ligands cannot provide this substoichiometric protection. The two phenomena are explained considering that: i) the existence of real monocoordinated [AuL]Y is negligible in condensed phases, and the kinetically efficient existing species are dicoordinated [AuL(W)]Y (W = any very weekly coordinating ligand existing in solution, including OH2, the solvent, or the Y– anion); and ii) these [AuL(W)]Y intermediates give rise to decomposition by a disproportionation mechanism, via polynuclear intermediates formed by associative oligomerization with release of some W ligands. It is also shown that very small concentrations of [AuL(W)]Y are still catalytically efficient, and can be stabilized by overstoichiometric adventitious water, so that full decomposition of the catalyst is hardly reached although eventually the stabilized concentration can result kinetically inefficient for the catalysis. These results suggest that, in cases of gold catalysis requiring the use of a significant quantity of gold catalyst, the turnover numbers can be increased, or the concentration of gold catalyst widely reduced, using substoichiometric protection properly tuned to the case.
    Materias (normalizadas)
    Catalyst Protection
    ISSN
    2155-5435
    Revisión por pares
    SI
    DOI
    10.1021/acscatal.6b01825
    Patrocinador
    Ministerio de Economía, Industria y Competitividad (CTQ2014-52796-P)
    Ministerio de Economía, Industria y Competitividad (CTQ2013-48406-P)
    Junta de Castilla y León (programa de apoyo a proyectos de investigación – GR 169 and project VA256U13)
    Idioma
    eng
    URI
    http://uvadoc.uva.es/handle/10324/21756
    Derechos
    openAccess
    Aparece en las colecciones
    • DEP63 - Artículos de revista [322]
    • CINQUIMA - Artículos de revista [162]
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    Nombre:
    ACScatal-Some-Singular-Feature.pdf
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    Universidad de Valladolid

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