Iron(III) complexes with a tripodal N3O ligand containing an internal base as a model for catechol intradiol-cleaving dioxygenases.

Iron(III) complexes with a tripodal N3O ligand containing an internal base as a model for catechol intradiol-cleaving dioxygenases. Research Abstract Details 

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Iron(III) complexes with a tripodal N3O ligand containing an internal base as a model for catechol intradiol-cleaving dioxygenases. Abstract Text:

Fei Li,Mei Wang,Ping Li,Tingting Zhang,Licheng Sun,Fei Li,Mei Wang,Ping Li,Tingting Zhang,Licheng Sun,

A bis(mu-alkoxo)-bridged dinuclear iron(III) complex [Fe(L)(NO3)]2(NO3)2 [1; HL = N,N-bis(2-pyridylmethyl)-N-(2-hydroxyethyl)amine] of the tripodal N3O ligand was prepared as a biomimetic model for the intradiol-cleaving dioxygenase enzymes. The reaction of 1 and catechol in the presence of excess triethylamine gave the catecholate (CAT) chelate bis(mu-alkoxo)-bridged dinuclear iron(III) complex [Fe(L)(CAT)]2 (2). The molecular structures of complexes 1 and 2 were determined by X-ray crystallography. Diiron complexes 1 and 2 contain the same bis(mu-alkoxo)diiron diamond core. All heteroatoms (N3O) of the ligand are coordinated to the iron center in complex 1 with two pyridine nitrogen atoms on the axial bonds, while one of the pyridyl arms of the ligand is left uncoordinated in complex 2. The interaction of the diiron complex 1 and 3,5-di-tert-butylcatechol (H2DBC) was investigated by electronic and mass spectroscopy. Complex 1 displays the intradiol-cleaving dioxygenase activity, and the coordinate ethoxyl arm of the ligand is capable of accepting the proton from catechol, which mimics the function of Tyr447 in the protocatechuate 3,4-dioxygenase as an internal base. The spectrophotometric titration experiment indicates the relatively low demand of the external base (0.8 equiv based on Fe(3+)) for attaining the highest dioxygenase activity of complex 1. The reaction rate of the reactive intermediate [Fe(HL)(DBC)]+ with dioxygen is 0.38 M(-1) s(-1) determined by kinetic studies.

Iron(III) complexes with a tripodal N3O ligand containing an internal base as a model for catechol intradiol-cleaving dioxygenases. Publishing Authors By Initials

F Li,M Wang,P Li,T Zhang,L Sun,F Li,M Wang,P Li,T Zhang,L Sun,

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Iron(III) complexes with a tripodal N3O ligand containing an internal base as a model for catechol intradiol-cleaving dioxygenases. Journal Published:

PUBLICATION TYPE: Research Support, Non-U.S. Gov

Journal: Inorganic chemistry

VOLUME: 46

Page Numbers: 9364-71

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ISSN: 0020-1669

DAY: 5

MONTH: 10

YEAR: 2007

Iron(III) complexes with a tripodal N3O ligand containing an internal base as a model for catechol intradiol-cleaving dioxygenases. Information

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LANGUAGE: eng

NlmUniqueID: 366543

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Grant and Affiliation Information for Iron(III) complexes with a tripodal N3O ligand containing an internal base as a model for catechol intradiol-cleaving dioxygenases.

AFFILIATION: State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Dalian 116012, China.

Country: United States

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MEDLINETA: Inorg Chem

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