Formation of an aqueous oxoiron(IV) complex at pH 2-6 from a nonheme iron(II) complex and H2O2

被引：92
作者：
Bautz, Jochen
Bukowski, Michael R.
Kerscher, Marion
Stubna, Audria
Comba, Peter
Lienke, Achim
Munck, Eckard
Que, Lawrence, Jr.
机构：
[1] Univ Heidelberg, Anorgan Chem Inst, D-69120 Heidelberg, Germany
[2] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA
[3] Univ Minnesota, Ctr Met & Biocatalysis, Minneapolis, MN 55455 USA
[4] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA
[5] Unilever Res & Dev, NL-3133 AT Vlaardingen, Netherlands
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2006年 / 45卷 / 34期
关键词：
coordination modes; iron; N ligands; oxidation; oxo ligands;
D O I：
10.1002/anie.200601134
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
(Chemical Equation Presented) A ferryl cation in water: Iron(II) coordinated by the pentadentate ligand L reacts with H2O2 to form a low-spin FeIV=O complex with S = 1 (2 in scheme) under conditions similar to those of the classical Fenton reaction. Complex 2 differs from a recently obtained high-spin aquated oxoiron(IV) species and demonstrates the role of the supporting polydentate ligand in controlling spin state and product formation. © 2006 Wiley-VCH Verlag GmbH & Co. KGaA.
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页码：5681 / 5684
页数：4
相关论文
共 32 条
[1]   THE REACTIVITY OF SPECTROSCOPICALLY DETECTED PEROXY COMPLEXES OF IRON PORPHYRINS [J].
BALCH, AL .
INORGANICA CHIMICA ACTA, 1992, 198 :297-307
[2]   Spectroscopic characterization of an FeIV intermediate generated by reaction of XO- (X = Cl, Br) with an FeII complex bearing a pentadentate non-porphyrinic ligand -: Hydroxylation and epoxidation activity [J].
Balland, V ;
Charlot, MF ;
Banse, F ;
Girerd, JJ ;
Mattioli, TA ;
Bill, E ;
Bartoli, JF ;
Battioni, P ;
Mansuy, D .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2004, (02) :301-308
[3]   Mechanism of aromatic hydroxylation by an activated feIV=O core in tetrahydrobiopterin-dependent hydroxylases [J].
Bassan, A ;
Blomberg, MRA ;
Siegbahn, PEM .
CHEMISTRY-A EUROPEAN JOURNAL, 2003, 9 (17) :4055-4067
[4]   Quantum chemical studies of dioxygen activation by mononuclear non-heme iron enzymes with the 2-His-1-carboxylate facial triad [J].
Bassan, A ;
Borowski, T ;
Siegbahn, PEM .
DALTON TRANSACTIONS, 2004, (20) :3153-3162
[5]   Mechanism of taurine:: α-ketoglutarate dioxygenase (TauD) from Escherichia coli [J].
Bollinger, JM ;
Price, JC ;
Hoffart, LM ;
Barr, EW ;
Krebs, C .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2005, (21) :4245-4254
[6]   Mechanism of dioxygen activation in 2-oxoglutarate-dependent enzymes: A hybrid DFT study [J].
Borowski, T ;
Bassan, A ;
Siegbahn, PEM .
CHEMISTRY-A EUROPEAN JOURNAL, 2004, 10 (04) :1031-1041
[7]   Iron coordination chemistry with tetra-, penta- and hexadentate bispidine-type ligands [J].
Börzel, H ;
Comba, P ;
Hagen, KS ;
Lampeka, YD ;
Lienke, A ;
Linti, G ;
Merz, M ;
Pritzkow, H ;
Tsymbal, LV .
INORGANICA CHIMICA ACTA, 2002, 337 :407-419
[8]   Ferryl ion, a compound of tetravalent iron [J].
Bray, WC ;
Gorin, MH .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1932, 54 :2124-2125
[9]  
Buda F, 2001, CHEM-EUR J, V7, P2775, DOI 10.1002/1521-3765(20010702)7:13<2775::AID-CHEM2775>3.0.CO
[10]  
2-6
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