Transient Formation and Reactivity of a High-Valent Nickel(IV) Oxido Complex

A reactive high-valent dinuclear nickel(IV) oxido bridged complex is reported that can be formed at room temperature by reaction of [(L) 2 Ni(II) 2 (μ-X) 3 ]X (X = Cl or Br) with NaOCl in methanol or acetonitrile (where L = 1,4,7-trimethyl-1,4,7-triazacyclononane). The unusual Ni(IV) oxido species i...

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Detalles Bibliográficos
Autores: Padamati, Sandeep K., Angelone, Davide, Draksharapu, Apparao, Primi, Gloria, Martin, David J., Tromp, Moniek, Swart, Marcel, Browne, Wesley R.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2017
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:10256/14724
Acceso en línea:http://hdl.handle.net/10256/14724
Access Level:acceso abierto
Palabra clave:Química -- Proves i reactius
Chemical tests and reagents
Níquel -- Reactivitat
Nickel -- Reactivity
Descripción
Sumario:A reactive high-valent dinuclear nickel(IV) oxido bridged complex is reported that can be formed at room temperature by reaction of [(L) 2 Ni(II) 2 (μ-X) 3 ]X (X = Cl or Br) with NaOCl in methanol or acetonitrile (where L = 1,4,7-trimethyl-1,4,7-triazacyclononane). The unusual Ni(IV) oxido species is stabilized within a dinuclear tris-μ-oxido-bridged structure as [(L) 2 Ni(IV) 2 (μ-O) 3 ] 2+ . Its structure and its reactivity with organic substrates are demonstrated through a combination of UV-vis absorption, resonance Raman, 1 H NMR, EPR, and X-ray absorption (near-edge) spectroscopy, ESI mass spectrometry, and DFT methods. The identification of a Ni(IV)-O species opens opportunities to control the reactivity of NaOCl for selective oxidations