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- W1978018874 abstract "Abstract A series of binuclear donor-acceptor complexes with helical polyproline bridges [(bpy) 2 Ru II L-(Pro) n -apy-Ru III (NH 3 ) 5 ] 5+ , n = 6, 7, 9, where L = 4-carboxy-4′-methyl-2,2′-bipyridine, bpy = 4,4′-bipyridine, and apy = 4-aminopyridine, were synthesized and characterized by absorption spectra, electrochemistry and HPLC. The CD spectra of the complexes confirm that they exist in the helical polyproline II structure. Intramolecular electron transfer within these complexes was studied by generating the [(bpy) 2 Ru I L · -(Pro) n -apy-Ru III (NH 3 ) 5 ] intermediate from the reaction of e aq (from pulse radiolysis) with the [(bpy) 2 Ru II L-(Pro) n -apy-Ru III (NH 3 ) 5 ] species in aqueous solution. The driving force for this reaction is estimated to be |Δ G 0 | ≈ 1.5 V. The rates ( k , 25°C) and activation parameters (Δ H ‡ (kcal/mol), Δ S ‡ (eu)) for the intra molecular electron transfer were found to be: 1.08×10 5 s −1 , 5.6, −17; 6.40 × 10 4 s −1 , 5.1, −19; 1.91 × 10 4 s −1 , 4.0, and −26 for n = 6, 7, 9 respectively. The rate ( k , 25°C) and activation parameters (Δ H ‡ (kcal/mol), Δ S ‡ (eu)) for the inter molecular reaction between [(bpy) 2 Ru I L · ] and [(NH 3 ) 5 Ru III -apy-Pro] were found to be 2.1 × 10 9 M −1 s −1 , 3.3 and −5. This series extends our studies of the distance dependence of rate versus the number of helical prolines bridging a donor and acceptor ruthenium site to a metal-to-metal distance ≈ 40 A. The weak dependence of rate versus the number of prolines observed for n = 6, 7, and 9 is very similar to that observed earlier for [(bpy) 2 Ru II L-(Pro) n -Co III (NH 3 ) 5 ], n = 4–6. The rapid rates observed at these long distances show that long range electron transfer can be observed between an appropriate donor and acceptor directly connected to the proline bridge via peptide bonds at distances similar to the diameter of a small protein." @default.
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- W1978018874 date "1993-10-01" @default.
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- W1978018874 title "Long range electron transfer in helical polyproline II oligopeptides" @default.
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- W1978018874 doi "https://doi.org/10.1016/0301-0104(93)80263-9" @default.
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