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| Content Provider | World Health Organization (WHO)-Global Index Medicus |
|---|---|
| Author | Carmieli, Ranaan Wasielewski, Michael R. Barnes, Jonathan C. Dyar, Scott M. Stoddart, J. Fraser Giesener, Marc A. Zhu, Zhixue Hartlieb, Karel J. Frasconi, Marco Fahrenbach, Albert C. Liu, Zhichang |
| Description | Author Affiliation: Barnes JC ( Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208-3113, USA.); |
| 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(â ¢+)) diradical dication while the P-BIPY(2+) unit is reduced to its P-BIPY(â ¢+) radical cation. A radical-state co-conformation (RSCC) results from movement of the CBPQT(2(â ¢+)) ring along the dumbbell to surround the P-BIPY(â ¢+) unit. This shuttling event induces IET to occur between the pyridinium redox centers of the P-BIPY(â ¢+) 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(â ¢+)) ring and the radical cation of methyl-phenylene-viologen (MPV(â ¢+)). 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 x 10(7) s(-1)) and activation energy (ΔG( ) = 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. |
| ISSN | 00278424 |
| e-ISSN | 10916490 |
| Journal | Proceedings of the National Academy of Sciences of the United States of America |
| Issue Number | 29 |
| Volume Number | 109 |
| Language | English |
| Publisher | National Academy of Sciences |
| Publisher Date | 2012-07-01 |
| Publisher Place | United States |
| Access Restriction | Open |
| Subject Keyword | Models, Chemical Protein Conformation Rotaxanes Chemistry Chemical Synthesis Electron Spin Resonance Spectroscopy Electron Transport Physiology Kinetics Oxidation-Reduction Spectroscopy, Near-Infrared Thermodynamics Research Support, U.S. Gov't, Non-P.H.S. Multidisciplinary |
| Content Type | Text |
| Resource Type | Article |
| Subject | Multidisciplinary |
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