Linear free-energy relationship for electron-transfer processes of pyrrolidinofullerenes with tetrakis(dimethylamino)ethylene in ground and excited states
作者： Chuping Luo , Mamoru Fujitsuka , Chun-Hui Huang , Osamu Ito
DOI: 10.1039/A901837I
关键词:
摘要: Systematic studies of electron-transfer processes in the ground states and excited triplet pyrrolidinofullerenes {C60(C3H6N)R [R=H (1), p-C6H4NO2 (2), p-C6H4CHO (3), p-C6H5 (4), p-C6H4OMe (5), p-C6H4NMe2 (6)]} with tetrakis(dimethylamino)ethylene (TDAE) have been carried out by steady-state transient absorption measurements visible–NIR region. Analyses equilibria indicate that free ion radicals are produced polar solvents. Photoinduced viaT(C60(C3H6N)R)* were observed applying a perturbation to reactions laser flash photolysis. Based on relationship thermodynamic data kinetic data, rate constants (ketG) can be evaluated. The ketG values affected substituents smaller extent compared equilibrium (K) solvents; α=0.6 Δ log ketG=α K. This α value indicates activation energies forward electron transfer vary moderately stabilities (C60(C3H6N)R)-. Electron-transfer viaT(C60(C3H6N)R)*, which close diffusion-controlled limit, do not show large substituent effect (α′=0), because their highly exothermic processes. Such linear free-energy extended other systems such as T(C60(C3H6N)R)*/N,N-dimethylaniline, from valuable information for obtained.
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