Experimental and computational evidence for the mechanism of intradiol catechol dioxygenation by non-heme iron(III) complexes

Jastrzebski, R., Quesne, Matthew, Weckhuysen, B. M., De visser, S. P. and Bruijinicx, P. C. A. 2014. Experimental and computational evidence for the mechanism of intradiol catechol dioxygenation by non-heme iron(III) complexes. Chemistry - a European Journal 20 (48) , pp. 15686-15691. 10.1002/chem.201404988

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Abstract

Catechol intradiol dioxygenation is a unique reaction catalyzed by iron-dependent enzymes and non-heme iron(III) complexes. The mechanism by which these systems activate dioxygen in this important metabolic process remains controversial. Using a combination of kinetic measurements and computational modelling of multiple iron(III) catecholato complexes, we have elucidated the catechol cleavage mechanism and show that oxygen binds the iron center by partial dissociation of the substrate from the iron complex. The iron(III) superoxide complex that is formed subsequently attacks the carbon atom of the substrate by a rate-determining C[BOND]O bond formation step.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry
Subjects:	Q Science > QD Chemistry
Publisher:	WileyBlackwell
ISSN:	0947-6539
Last Modified:	25 Feb 2019 16:50
URI:	https://orca.cardiff.ac.uk/id/eprint/88599

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