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• W2014903377 endingPage "6386" @default.
• W2014903377 startingPage "6378" @default.
• W2014903377 abstract "Use of 1,4,7,10-tetraazacyclododecane (cyclen) as a capping ligand and 4,4‘-bipyridine (4,4‘-bpy) as a bridging ligand enables assembly of redox-active Ru3 triangle and Ru4 square complexes. The former is produced by reacting [(cyclen)Ru(DMSO)Cl]Cl with 4,4‘-bpy in a 3:1 ethanol:water mixture to precipitate [(cyclen)3Ru3(4,4‘-bpy)3]Cl6·18H2O·THF (4), whereas the latter is generated as [(cyclen)4Ru4(4,4‘-bpy)4](CF3SO3)8·2CF3SO3H·5MeOH (7) by reacting (cyclen)Ru(CF3SO3)3 with 4,4‘-bpy in methanol. The crystal structure of 4·11H2O reveals an equilateral triangle in which the 4,4‘-bpy bridges are bowed outward, such that the pyridine rings are all forced to be perpendicular to the Ru3 triangle. Consequently, adjacent pyridine rings are essentially coplanar, and the cyclic voltammogram of [(cyclen)3Ru3(4,4‘-bpy)3]6+ in acetonitrile displays three distinct one-electron oxidation events. Cyclic voltammetry measurements reveal redox processes centered at E1/2 = 0.207, 0.342, and 0.434 V versus Cp2Fe0/+ that are assigned to 6+/7+, 7+/8+, and 8+/9+ couples of the [(cyclen)3Ru3(4,4‘-bpy)3]n+ triangle, respectively. In contrast, the structure of [(cyclen)4Ru4(4,4‘-bpy)4]8+ features a regular square geometry wherein the rings of the bridging 4,4‘-bpy ligands are free to rotate, leading to just one four-electron oxidation couple centered at 0.430 V. Density functional theory calculations performed on [(cyclen)3Ru3(4,4‘-bpy)3]6+ reveal metal-based orbitals with contributions from the π system of the bridging 4,4‘-bpy ligands, providing a likely pathway for electron transfer." @default.
• W2014903377 created "2016-06-24" @default.
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• W2014903377 date "2006-07-08" @default.
• W2014903377 modified "2023-09-29" @default.
• W2014903377 title "Angle-Dependent Electronic Effects in 4,4‘-Bipyridine-Bridged Ru₃ Triangle and Ru₄ Square Complexes" @default.
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• W2014903377 doi "https://doi.org/10.1021/ic060570l" @default.
• W2014903377 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/16878949" @default.
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