Mechanistic tuning of hydrocarbon oxidations with H2O 2, catalyzed by hexacoordinate ferrous complexes

Yasmina Mekmouche, Stéphane Ménage*, Jacques Pécaut, Colette Lebrun, Lee Reilly, Volker Schuenemann, Alfred Trautwein, Marc Fontecave

*Corresponding author for this work
25 Citations (Scopus)

Abstract

A comparison of the catalytic properties of a series of FeIILXY complexes on oxidation reactions with H2O2, [L = N,N′-bis(pyridin-2-yl-methyl)-N,N′-bis(3,4,5-trimethoxybenzyl) -ethane-1,2-diamine] indicates that the lability of the X and Y ligands (Cl - or CH3CN) determines the nature of the oxidation pathway. The absence of a labile site in the complex, i.e. when X = Y= Cl -, causes the reaction to proceed via a Fenton pathway (generation of hydroxyl radicals, exclusively). The presence of two labile CH3CN ligands (X = Y = CH3CN) allows the catalysis to proceed through a metal-based mechanism, whereas in the case of a complex with only one labile ligand (X = Cl- and Y = CH3CN), the reaction is less controlled by the metal. We wish to emphasize that the cleavage of the O-O bond in the Fe-OOH moeity, a key intermediate in the reaction, is different in the last two cases.

Original languageEnglish
JournalEuropean Journal of Inorganic Chemistry
Issue number15
Pages (from-to)3163-3171
Number of pages9
ISSN1434-1948
DOIs
Publication statusPublished - 06.08.2004

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