Mechanistic implications of the active species involved in the oxidation of hydrocarbons by iron complexes of pyrazine-2-carboxylic acid |
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Authors: | Tanase Stefania Marques-Gallego Patricia Browne Wesley R Hage Ronald Bouwman Elisabeth Feringa Ben L Reedijk Jan |
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Institution: | Leiden Institute of Chemistry, Gorlaeus Laboratories, Leiden University, PO Box 9502, 2300, RA Leiden, The Netherlands. |
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Abstract: | The reactivity towards H(2)O(2) of the complexes Fe(pca)(2)(py)(2)].py (1) and Na(2){Fe(pca(3))](2)O}.2H(2)O.CH(3)CN (2) (where pca(-) is pyrazine-2-carboxylate) and their catalytic activity in the oxidation of hydrocarbons is reported. Addition of H(2)O(2) to 1 results in the formation of a dinuclear Fe(III)-(mu-O)-Fe(III) species characterized spectroscopically and by cyclic voltammetry. By contrast, treatment of 2 with H(2)O(2) results in the formation of mononuclear iron(II) complexes, Fe(pca)(2)(solvent)(2)]. The experimental results indicate that the catalytic activity of the starting complexes 1 and 2 is strongly dependent on the species formed in solution. |
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