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Literature DB >> 16999397

electrochemical generation of a nonheme oxoiron(IV) complex.

Michael J Collins¹, Kallol Ray, Lawrence Que.

Abstract

The complex [Fe(IV)O(N4Py)]2+ (N4Py = N,N-bis(2-pyridylmethyl)-N-bis(2-pyridyl)methylamine) has been prepared by bulk electrolysis in aqueous CH3CN and CH2Cl2, and its redox properties characterized. Bulk chronocoulometry and spectropotentiometry experiments in CH3CN show that [Fe(II)(N4Py)(NCCH3)]2+ can be oxidized quantitatively to its iron(III) derivative at an applied potential of +0.71 V vs ferrocene and then to the oxoiron(IV) complex (in the presence of added water) at potentials above +1.3 V. The E1/2 value for the Fe(IV/III) couple has been estimated to be +0.90 V from spectropotentiometric titrations in CH3CN and cyclic voltammetric measurements in CH2Cl2.

Entities: Chemical

Mesh：

Substances：

Year: 2006 PMID： 16999397 PMCID： PMC3678529 DOI： 10.1021/ic061263i

Source DB: PubMed Journal: Inorg Chem ISSN： 0020-1669 Impact factor: 5.165

21 in total

Review 1. Dioxygen activation at mononuclear nonheme iron active sites: enzymes, models, and intermediates.

Authors: Miquel Costas; Mark P Mehn; Michael P Jensen; Lawrence Que
Journal: Chem Rev Date: 2004-02 Impact factor: 60.622

Review 2. Reaction mechanisms of mononuclear non-heme iron oxygenases.

Authors: Mahdi M Abu-Omar; Aristobulo Loaiza; Nikos Hontzeas
Journal: Chem Rev Date: 2005-06 Impact factor: 60.622

3. Mechanistic insight into alcohol oxidation by high-valent iron-oxo complexes of heme and nonheme ligands.

Authors: Na Young Oh; Yumi Suh; Mi Joo Park; Mi Sook Seo; Jinheung Kim; Wonwoo Nam
Journal: Angew Chem Int Ed Engl Date: 2005-07-04 Impact factor: 15.336

4. Two-state reactivity in alkane hydroxylation by non-heme iron-oxo complexes.

Authors: Hajime Hirao; Devesh Kumar; Lawrence Que; Sason Shaik
Journal: J Am Chem Soc Date: 2006-07-05 Impact factor: 15.419

5. Oxoiron(IV) complexes of the tris(2-pyridylmethyl)amine ligand family: effect of pyridine alpha-substituents.

Authors: Tapan K Paine; Miquel Costas; József Kaizer; Lawrence Que
Journal: J Biol Inorg Chem Date: 2006-03-11 Impact factor: 3.358

6. Crystallographic and spectroscopic characterization of a nonheme Fe(IV)-O complex.

Authors: Jan-Uwe Rohde; Jun-Hee In; Mi Hee Lim; William W Brennessel; Michael R Bukowski; Audria Stubna; Eckard Münck; Wonwoo Nam; Lawrence Que
Journal: Science Date: 2003-02-14 Impact factor: 47.728

7. Rapid freeze-quench 57Fe Mössbauer spectroscopy: monitoring changes of an iron-containing active site during a biochemical reaction.

Authors: Carsten Krebs; John C Price; Jeffrey Baldwin; Lana Saleh; Michael T Green; J Martin Bollinger
Journal: Inorg Chem Date: 2005-02-21 Impact factor: 5.165

8. An FeIV=O complex of a tetradentate tripodal nonheme ligand.

Authors: Mi Hee Lim; Jan-Uwe Rohde; Audria Stubna; Michael R Bukowski; Miquel Costas; Raymond Y N Ho; Eckard Munck; Wonwoo Nam; Lawrence Que
Journal: Proc Natl Acad Sci U S A Date: 2003-03-18 Impact factor: 11.205

9. Mixed-valent [FeIV(mu-O)(mu-carboxylato)2FeIII]3+ core.

Authors: Leonardo D Slep; Ana Mijovilovich; Wolfram Meyer-Klaucke; Thomas Weyhermüller; Eckhard Bill; Eberhard Bothe; Frank Neese; Karl Wieghardt
Journal: J Am Chem Soc Date: 2003-12-17 Impact factor: 15.419

10. Stabilization of higher-valent states of iron porphyrin by hydroxide and methoxide ligands: electrochemical generation of iron(IV)-oxo porphyrins.

Authors: W A Lee; T S Calderwood; T C Bruice
Journal: Proc Natl Acad Sci U S A Date: 1985-07 Impact factor: 11.205

14 in total

1. Axial ligand tuning of a nonheme iron(IV)-oxo unit for hydrogen atom abstraction.

Authors: Chivukula V Sastri; Jimin Lee; Kyungeun Oh; Yoon Jin Lee; Junghyun Lee; Timothy A Jackson; Kallol Ray; Hajime Hirao; Woonsup Shin; Jason A Halfen; Jinheung Kim; Lawrence Que; Sason Shaik; Wonwoo Nam
Journal: Proc Natl Acad Sci U S A Date: 2007-11-28 Impact factor: 11.205

electrochemical generation of a nonheme oxoiron(IV) complex.

Review 1. Dioxygen activation at mononuclear nonheme iron active sites: enzymes, models, and intermediates.

Review 2. Reaction mechanisms of mononuclear non-heme iron oxygenases.

3. Mechanistic insight into alcohol oxidation by high-valent iron-oxo complexes of heme and nonheme ligands.

4. Two-state reactivity in alkane hydroxylation by non-heme iron-oxo complexes.

5. Oxoiron(IV) complexes of the tris(2-pyridylmethyl)amine ligand family: effect of pyridine alpha-substituents.

6. Crystallographic and spectroscopic characterization of a nonheme Fe(IV)-O complex.

7. Rapid freeze-quench 57Fe Mössbauer spectroscopy: monitoring changes of an iron-containing active site during a biochemical reaction.

8. An FeIV=O complex of a tetradentate tripodal nonheme ligand.

9. Mixed-valent [FeIV(mu-O)(mu-carboxylato)2FeIII]3+ core.

10. Stabilization of higher-valent states of iron porphyrin by hydroxide and methoxide ligands: electrochemical generation of iron(IV)-oxo porphyrins.

1. Axial ligand tuning of a nonheme iron(IV)-oxo unit for hydrogen atom abstraction.

2. A synthetic precedent for the [FeIV2(mu-O)2] diamond core proposed for methane monooxygenase intermediate Q.

3. Redox potential and C-H bond cleaving properties of a nonheme Fe(IV)=O complex in aqueous solution.

Review 4. The biology and chemistry of high-valent iron-oxo and iron-nitrido complexes.

5. An isoelectronic NO dioxygenase reaction using a nonheme iron(III)-peroxo complex and nitrosonium ion.

6. The crystal structure of a high-spin oxoiron(IV) complex and characterization of its self-decay pathway.

Review 7. Proton-Coupled Electron Transfer in Organic Synthesis: Fundamentals, Applications, and Opportunities.

8. Nonheme Oxoiron(IV) Complexes of Pentadentate N5 Ligands: Spectroscopy, Electrochemistry, and Oxidative Reactivity.

9. A diiron(IV) complex that cleaves strong C-H and O-H bonds.

10. Iron-oxidation-state-dependent O-O bond cleavage of meta-chloroperbenzoic acid to form an iron(IV)-oxo complex.