Kinetics Aspects of the Reversible Assembly of Copper in Heterometallic Mo3CuS4 Clusters with 4,4′-Di-tert-butyl-2,2′-bipyridine
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Otros documentos de la autoría: Pino Chamorro, Jose Angel; Laricheva, Yuliya A.; Guillamón, Eva; Fernández-Trujillo, M. Jesús; Algarra, Andrés G.; Gushchin, Artem L.; Abramov, Pavel A.; Bustelo, Emilio; Llusar, Rosa; Sokolov, Maxim; García Basallote, Manuel
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Título
Kinetics Aspects of the Reversible Assembly of Copper in Heterometallic Mo3CuS4 Clusters with 4,4′-Di-tert-butyl-2,2′-bipyridineAutoría
Fecha de publicación
2016Editor
American Chemical SocietyISSN
0020-1669; 1520-510XCita bibliográfica
PINO-CHAMORRO, Jose Ángel, et al. Kinetics Aspects of the Reversible Assembly of Copper in Heterometallic Mo3CuS4 Clusters with 4, 4′-Di-tert-butyl-2, 2′-bipyridine. Inorganic Chemistry, 2016.Tipo de documento
info:eu-repo/semantics/articleVersión de la editorial
http://bs8lz6ys5q.search.serialssolutions.com/?ctx_ver=Z39.88-2004&ctx_enc=info% ...Versión
info:eu-repo/semantics/publishedVersionPalabras clave / Materias
Resumen
Treatment of the triangular [Mo3S4Cl3(dbbpy)3]Cl cluster ([1]Cl) with CuCl produces a novel tetrametallic cuboidal cluster [Mo3(CuCl)S4Cl3(dbbpy)3][CuCl2] ([2][CuCl2]), whose crystal structure was determined by X-ray ... [+]
Treatment of the triangular [Mo3S4Cl3(dbbpy)3]Cl cluster ([1]Cl) with CuCl produces a novel tetrametallic cuboidal cluster [Mo3(CuCl)S4Cl3(dbbpy)3][CuCl2] ([2][CuCl2]), whose crystal structure was determined by X-ray diffraction (dbbpy = 4,4′-di-tert-butyl-2,2′-bipyridine). This species, which contains two distinct types of Cu(I), is the first example of a diimine-functionalized heterometallic M3M′S4 cluster. Kinetics studies on both the formation of the cubane from the parent trinuclear cluster and its dissociation after treatment with halides, supported by NMR, electrospray ionization mass spectrometry, cyclic voltammetry, and density functional theory calculations, are provided. On the one hand, the results indicate that addition of Cu(I) to [1]+ is so fast that its kinetics can be monitored only by cryo-stopped flow at −85 °C. On the other hand, the release of the CuCl unit in [2]+ is also a fast process, which is unexpectedly assisted by the CuCl2– counteranion in a process triggered by halide (X–) anions. The whole set of results provide a detailed picture of the assembly–disassembly processes in this kind of cluster. Interconversion between trinuclear M3S4 clusters and their heterometallic M3M′S4 derivatives can be a fast process occurring readily under the conditions employed during reactivity and catalytic studies, so their occurrence is a possibility that must be taken into account in future studies. [-]
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Inorganic Chemistry, 2016, vol. 55, núm. 19Derechos de acceso
© 2016 American Chemical Society
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