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• W2067828265 abstract "Two heterobimetallic complexes of [Fc(4-Py)Ru(NH3)5](PF6)2 (1) and [Fc(3-Py)Ru(NH3)5](PF6)2 (2) (Fc(4-Py) = 4-ferrocenylpyridine, Fc(3-Py) = 3-ferrocenylpyridine) have been synthesized and characterized for the purpose of investigating optical and thermal electron transfer. The mixed-valence species generated in situ using ferrocenium hexafluorophosphate as the oxidant show Robin and Day class II behavior, and the oxidized sites are ruthenium centered. ΔE1/2°, E1/2°(FeIII/FeII) − E1/2°(RuIII/RuII), an estimate of ΔEo that is an energetic difference between the donor and acceptor sites, changes sharply with variation of solvents. Good linear relationship exists between ΔE1/2° and Gutmann solvent donor number (DN) and ΔE1/2° versus DN plots yield a slope of 20.4 ± 1.6 mV/DN for [Fc(4-Py)Ru(NH3)5]2+/3+/4+ and a slope of 21.1 ± 2.2 mV/DN for [Fc(3-Py)Ru(NH3)5]2+/3+/4+. The solvent-dependent IT bands were found to vary almost exclusively with ΔE1/2°. The continuum dielectric approximation is found to be adequate, and the (Eop − ΔEo) versus (1/εop − 1/εs) plot yields a straight line with a slope of 3848 ± 1444 and an intercept of 4265 ± 227 cm-1 for [Fc(4-Py)Ru(NH3)5]3+. The corresponding values for [Fc(3-Py)Ru(NH3)5]3+are 2328 ± 1560 and 6712 ± 100 cm-1. The thermal electron transfer (the reverse of the optical process, viz., RuII → FeIII electron transfer) is adiabatic for [Fc(4-Py)Ru(NH3)5]3+ but somewhat nonadiabatic (κ ≈ 0.6) for [Fc(3-Py)Ru(NH3)5]3+. The thermal transfer rate constants of both complexes decrease exponentially with increasing solvent donor number and show close magnitude in all solvents despite [Fc(3-Py)Ru(NH3)5]3+ having apparently a shorter through-space distance and lower activation energies. However, these calculated kth values should be used with caution because no experimental data as measured by flash photolysis techniques are available." @default.
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• W2067828265 date "1999-02-02" @default.
• W2067828265 modified "2023-10-14" @default.
• W2067828265 title "Solvent-Dependent Studies of Intervalence Transfer of Mixed-Valence Complexes Containing Ferrocenylpyridine and Rutheniumammines" @default.
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• W2067828265 doi "https://doi.org/10.1021/ic9713341" @default.
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