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| Content Provider | World Health Organization (WHO)-Global Index Medicus |
|---|---|
| Author | Torres-alacan, Joel Neese, Frank Vöhringer, Peter Krahe, Oliver Filippou, Alexander C. Schwarzer, Dirk |
| Description | Author Affiliation: Torres-Alacan J ( Institut für Physikalische und Theoretische Chemie, Rheinische Friedrich-Wilhelms Universität, Wegelerstraße 12, 53115 Bonn, Germany.) |
| Abstract | The photochemistry of iron azido complexes is quite challenging and poorly understood. For example, the photochemical decomposition of $[Fe^{III}N_{3}(cyclam-ac)]PF_{6}$ $([1]PF_{6}),$ where cyclam-ac represents the 1,4,8,11-tetraazacyclotetradecane-1-acetate ligand, has been shown to be wavelength-dependent, leading either to the rare high-valent iron(V) nitrido complex $[Fe^{V}N(cyclam-ac)]PF_{6}$ $([3]PF_{6})$ after cleavage of the azide $N_{α}N_{β}$ bond, or to a photoreduced $Fe^{II}$ species after $FeN_{azide}$ bond homolysis. The mechanistic details of this intriguing reactivity have never been studied in detail. Here, the photochemistry of 1 in acetonitrile solution at room temperature has been investigated using step-scan and rapid-scan time-resolved Fourier transform infrared (FTIR) spectroscopy following a 266 nm, 10 ns pulsed laser excitation. Using carbon monoxide as a quencher for the primary iron-containing photochemical product, it is shown that 266 nm excitation of 1 results exclusively in the cleavage of the $FeN_{azide}$ bond, as was suspected from earlier steady-state irradiation studies. In argon-purged solutions of $[1]PF_{6},$ the solvent-stabilized complex cation $[Fe^{II}(CH_{3}CN)(cyclam-ac)]^{+}$ (2 red) together with the azide radical $(N_{3}^{.})$ is formed with a relative yield of 80 %, as evidenced by the appearance of their characteristic vibrational resonances. Strikingly, step-scan experiments with a higher time resolution reveal the formation of azide anions $(N_{3}^{−})$ during the first 500 ns after photolysis, with a yield of 20 %. These azide ions can subsequently react thermally with 2 red to form $[Fe^{II}N_{3}(cyclam-ac)]$ (1 red) as a secondary product of the photochemical decomposition of 1. Molecular oxygen was further used to quench 1 red and 2 red to form what seems to be the elusive complex $[Fe(O_{2})(cyclam-ac)]^{+}$ (6). |
| ISSN | 09476539 |
| e-ISSN | 15213765 |
| Journal | Chemistry - A European Journal |
| Issue Number | 10 |
| Volume Number | 18 |
| Language | English |
| Publisher | Wiley-VCH;ChemPubSoc Europe |
| Publisher Date | 2012-03-05 |
| Publisher Place | Germany |
| Access Restriction | Open |
| Subject Keyword | Ferric Compounds Chemistry Heterocyclic Compounds Photochemistry Crystallography, X-Ray Models, Molecular Molecular Conformation Molecular Structure Spectroscopy, Fourier Transform Infrared Research Support, Non-U.S. Gov't |
| Content Type | Text |
| Resource Type | Article |
| Subject | Organic Chemistry Catalysis |
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