Autor segons l'article: Álvarez-Ruiz E; Carbó JJ; Gómez M; Hernández-Prieto C; Hernán-Gómez A; Martín A; Mena M; Ricart JM; Salom-Català A; Santamaría C
Departament: Química Física i Inorgànica
Autor/s de la URV: Carbó Martin, Jorge Juan / Ricart Pla, Jose Manuel
Paraules clau: Early transition-metals potential basis-sets polarization functions nitrogen molecular-orbital methods hydrogenation effective core potentials dinitrogen activation crystal-structure coordination basis-sets azobenzene ab-initio
Resum: The reaction of [TaCpRX4] (CpR = ?5-C5Me5, ?5-C5H4SiMe3, ?5-C5HMe4; X = Cl, Br) with SiH3Ph resulted in the formation of the dinuclear hydride tantalum(IV) compounds [(TaCpRX2)2(?-H)2], structurally identified by single-crystal X-ray analyses. These species react with azobenzene to give the mononuclear imide complex [TaCpRX2(NPh)] along with the release of molecular hydrogen. Analogous reactions between the [{Ta(?5-C5Me5)X2}2(?-H)2] derivatives and the cyclic diazo reagent benzo[c]cinnoline afford the biphenyl-bridged (phenylimido)tantalum complexes [{Ta(?5-C5Me5)X2}2(?-NC6H4C6H4N)] along with the release of molecular hydrogen. When the compounds [(TaCpRX2)2(?-H)2] (CpR = ?5-C5H4SiMe3, ?5-C5HMe4; X = Cl, Br) were employed, we were able to trap the side-on-bound diazo derivatives [(TaCpRX)2{?-(?2,?2-NC6H4C6H4N)}] (CpR = ?5-C5H4SiMe3, ?5-C5HMe4; X = Cl, Br) as intermediates in the N=N bond cleavage process. DFT calculations provide insights into the N=N cleavage mechanism, in which the ditantalum(IV) fragment can promote two-electron reductions of the N=N bond at two different metal-metal bond splitting stages. © 2021 The Authors. Published by American Chemical Society.
Àrees temàtiques: Química Physical and theoretical chemistry Medicina i Materiais Interdisciplinar Inorganic chemistry General medicine Farmacia Engenharias iii Engenharias ii Engenharias i Ciências biológicas iii Ciências biológicas ii Ciências biológicas i Ciências agrárias i Chemistry, inorganic & nuclear Chemistry (miscellaneous) Biotecnología Astronomia / física
Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
Adreça de correu electrònic de l'autor: josep.ricart@urv.cat j.carbo@urv.cat
Identificador de l'autor: 0000-0002-2610-5535 0000-0002-3945-6721
Data d'alta del registre: 2023-10-21
Versió de l'article dipositat: info:eu-repo/semantics/publishedVersion
Enllaç font original: https://pubs.acs.org/doi/10.1021/acs.inorgchem.1c03152
URL Document de llicència: http://repositori.urv.cat/ca/proteccio-de-dades/
Referència a l'article segons font original: Inorganic Chemistry. 61 (1): 474-485
Referència de l'ítem segons les normes APA: Álvarez-Ruiz E; Carbó JJ; Gómez M; Hernández-Prieto C; Hernán-Gómez A; Martín A; Mena M; Ricart JM; Salom-Català A; Santamaría C (2022). N=N Bond Cleavage by Tantalum Hydride Complexes: Mechanistic Insights and Reactivity. Inorganic Chemistry, 61(1), 474-485. DOI: 10.1021/acs.inorgchem.1c03152
DOI de l'article: 10.1021/acs.inorgchem.1c03152
Entitat: Universitat Rovira i Virgili
Any de publicació de la revista: 2022
Tipus de publicació: Journal Publications
Repositori URV