Abstract
Two novel mixed-valent ruthenium complexes, of formulae [(tpy)(bpy)Ru II(pz)Ru III(edta)] + and [(CN) 4Ru II(bpz)Ru III(edta)] 3− (where tpy=2,2′:6′,2″-terpyridine, bpy=2,2′-bipyridine, pz=pyrazine, bpz=2,2′-bipyrazine, edta=ethylenediaminetetraacetate), were prepared and spectroscopically characterized in aqueous solutions and as solid salts with suitable counterions. For comparison purposes, two new ruthenium complexes: a dinuclear species, of formula [(CN) 4Ru II(bpz)Ru II(NH 3) 5], and a trinuclear species, of formula {(CN) 4Ru II(bpz)[Ru II(NH 3) 5] 2} 2+, were also prepared and characterized in aqueous solutions. From spectral data of metal-to-metal charge transfer (MMCT) absorption bands, a Hush analysis was made, and the reorganization energies for the intramolecular electron transfers were calculated. A dramatic change in these values was disclosed when comparing both mixed-valent species, which can be explained on the basis of the influence exerted by the ‘innocent’ co-ligands (polypyridines or cyanides) bonded to the ruthenium centers. This tuning is an important factor in devising molecular devices for energy conversion.
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