Fine Tuning of MLCT States in New Mononuclear Complexes of Ruthenium(II) Containing Tris(1-pyrazolyl)methane, 2,2 -Bipyridine and Aromatic Nitrogen Heterocycles

The syntheses of new mononuclear ruthenium(II) complexes of the type: [Ru(bpy)(L)(tpm)](PF6)2 {tpm = tris(1-pyrazolyl)methane; bpy = 2,2′-bipyridine; L = pz (pyrazine; 1), 4,4′-bpy (4,4′-bipyridine; 2), and bpe [trans-1,2-bis(4-pyridyl)ethylene; 3]} are described, together with their spectroscopic,...

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Detalles Bibliográficos
Autores: Katz, Néstor E., Romero García, Isabel, Llobet Dalmases, Antoni, Parella Coll, Teodor, Benet Buchholz, Jordi
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2005
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:10256/13088
Acceso en línea:http://hdl.handle.net/10256/13088
Access Level:acceso embargado
Palabra clave:Ruteni -- Compostos
Ruthenium compounds
Descripción
Sumario:The syntheses of new mononuclear ruthenium(II) complexes of the type: [Ru(bpy)(L)(tpm)](PF6)2 {tpm = tris(1-pyrazolyl)methane; bpy = 2,2′-bipyridine; L = pz (pyrazine; 1), 4,4′-bpy (4,4′-bipyridine; 2), and bpe [trans-1,2-bis(4-pyridyl)ethylene; 3]} are described, together with their spectroscopic, electrochemical, and photophysical properties. A complete assignment of the NMR resonances of the three species could be made in CD3CN by bidimensional techniques. A fine tuning of the energies of MLCT (metal-to-ligand charge transfer) states in these complexes is disclosed when comparing, in CH3CN, the values of their maximum absorption wavelengths for the most intense visible bands (λmax) and their redox potentials for the RuIII/RuII couples; this effect, relevant to the design of efficient photocatalysts, can be attributed to a decreasing order of dπ(Ru) → π*(2,2′-bpy) backbonding when decreasing the distance between both N atoms in the aromatic nitrogen heterocycle L that acts in a monodentate manner. Only the species with L = bpe emits at room temperature, pointing to the conclusion that MLCT excited states in this series become higher in energy than dd excited states when the value of λmax is lower than 400 nm. These species are also useful building blocks for new dinuclear mixed-valent complexes