New example of a non-heme mononuclear iron(IV) oxo complex. Spectroscopic data and oxidation activity |
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Authors: | Martinho Marlène Banse Frédéric Bartoli Jean-François Mattioli Tony A Battioni Pierrette Horner Olivier Bourcier Sophie Girerd Jean-Jacques |
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Institution: | Laboratoire de Chimie Inorganique, UMR 8613, Institut de Chimie Moléculaire et des Matériaux d'Orsay, Université Paris Sud, 91405 Orsay Cedex, France. |
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Abstract: | The green complex S=1 (TPEN)FeO]2+ TPEN=N,N,N',N'-tetrakis(2-pyridylmethyl)ethane-1,2-diamine] has been obtained by treating the (TPEN)Fe]2+ precursor with meta-chloroperoxybenzoic acid (m-CPBA). This high-valent complex belongs to the emerging family of synthetic models of Fe(IV)=O intermediates invoked during the catalytic cycle of biological systems. This complex exhibits spectroscopic characteristics that are similar to those of other models reported recently with a similar amine/pyridine environment. Thanks to its relative stability, vibrational data in solution have been obtained by Fourier transform infrared. A comparison of the Fe=O and Fe=(18)O wavenumbers reveals that the Fe-oxo vibration is not a pure one. The ability of the green complex to oxidize small organic molecules has been studied. Mixtures of oxygenated products derived from two- or four-electron oxidations are obtained. The reactivity of this FeO]2+ complex is then not straightforward, and different mechanisms may be involved. |
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