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• W2000359964 abstract "The kinetics and thermodynamics of intramolecular electron transfer (IET) can be subjected to redox control in a bistable [2]rotaxane comprised of a dumbbell component containing an electron-rich 1,5-dioxynaphthalene (DNP) unit and an electron-poor phenylene-bridged bipyridinium (P-BIPY 2+ ) unit and a cyclobis (paraquat- p -phenylene) (CBPQT 4+ ) ring component. The [2]rotaxane exists in the ground-state co-conformation (GSCC) wherein the CBPQT 4+ ring encircles the DNP unit. Reduction of the CBPQT 4+ leads to the CBPQT 2(•+) diradical dication while the P-BIPY 2+ unit is reduced to its P-BIPY •+ radical cation. A radical-state co-conformation (RSCC) results from movement of the CBPQT 2(•+) ring along the dumbbell to surround the P-BIPY •+ unit. This shuttling event induces IET to occur between the pyridinium redox centers of the P-BIPY •+ unit, a property which is absent between these redox centers in the free dumbbell and in the 1∶1 complex formed between the CBPQT 2(•+) ring and the radical cation of methyl-phenylene-viologen (MPV •+ ). Using electron paramagnetic resonance (EPR) spectroscopy, the process of IET was investigated by monitoring the line broadening at varying temperatures and determining the rate constant ( k ET = 1.33 × 10 7 s -1 ) and activation energy (Δ G ‡ = 1.01 kcal mol -1 ) for electron transfer. These values were compared to the corresponding values predicted, using the optical absorption spectra and Marcus–Hush theory." @default.
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• W2000359964 date "2012-06-08" @default.
• W2000359964 modified "2023-10-10" @default.
• W2000359964 title "Mechanically induced intramolecular electron transfer in a mixed-valence molecular shuttle" @default.
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• W2000359964 doi "https://doi.org/10.1073/pnas.1201561109" @default.
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