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| Content Provider | World Health Organization (WHO)-Global Index Medicus |
|---|---|
| Author | Kuss-petermann, Martin Chen, Jing Wenger, Oliver S. |
| Description | Author Affiliation: Chen J ( Department of Chemistry, University of Basel, St. Johanns-Ring 19, 4056 Basel (Switzerland), Fax: (+41) 61-267-09-76.) |
| Abstract | Proton-coupled electron transfer (PCET) was investigated in three covalent donor–bridge–acceptor molecules with different bridge lengths. Upon photoexcitation of their $Ru(bpy)_{3}^{2+}$ (bpy=2,2′-bipyridine) photosensitizer in acetonitrile, intramolecular long-range electron transfer from a phenolic unit to $Ru(bpy)_{3}^{2+}$ occurs in concert with release of the phenolic proton to pyrrolidine base. The kinetics of this bidirectional concerted proton–electron transfer (CPET) reaction were studied as a function of $phenol–Ru(bpy)_{3}^{2+}$ distance by increasing the number of bridging p-xylene units. A distance decay constant (β) of $0.67±0.23 Å^{−1}$ was determined. The distance dependence of the rates for CPET is thus not significantly steeper than that for ordinary (i.e., not proton coupled) electron transfer across the same bridges, despite the concerted motion of oppositely charged particles into different directions. Long-range bidirectional CPET is an important reaction in many proteins and plays a key role in photosynthesis; our results are relevant in the context of photoinduced separation of protons and electrons as a means of light-to-chemical energy conversion. This is the first determination of β for a bidirectional CPET reaction. |
| ISSN | 09476539 |
| e-ISSN | 15213765 |
| Journal | Chemistry - A European Journal |
| Issue Number | 14 |
| Volume Number | 20 |
| Language | English |
| Publisher | Wiley-VCH;ChemPubSoc Europe |
| Publisher Date | 2014-04-01 |
| Publisher Place | Germany |
| Access Restriction | Open |
| Subject Keyword | Phenols Chemistry Electron Transport Electrons Kinetics Protons Thermodynamics Research Support, Non-U.S. Gov't |
| Content Type | Text |
| Resource Type | Article |
| Subject | Organic Chemistry Catalysis |
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