Literature DB >> 23432330

Factors affecting the carboxylate shift upon formation of nonheme diiron-O2 adducts.

Jonathan R Frisch1, Ryan McDonnell, Elena V Rybak-Akimova, Lawrence Que.   

Abstract

Several [Fe(II)2(N-EtHPTB)(μ-n class="Chemical">O2X)](2+) complexes (1·O2X) have been synthesized, where N-EtHPTB is the anion of N,N,N'N'-tetrakis(2-benzimidazolylmethyl)-2-hydroxy-1,3-diaminopropane and O2X is an oxyanion bridge. Crystal structures reveal five-coordinate (μ-alkoxo)diiron(II) cores. These diiron(II) complexes react with O2 at low temperatures in CH2Cl2 (-90 °C) to form blue-green O2 adducts that are best described as triply bridged (μ-η(1):η(1)-peroxo)diiron(III) species (2·O2X). With one exception, all 2·O2X intermediates convert irreversibly to doubly bridged, blue (μ-η(1):η(1)-peroxo)diiron(III) species (3·O2X). Where possible, 2·O2X and 3·O2X intermediates were characterized using resonance Raman spectroscopy, showing respective νO-O values of ∼850 and ∼900 cm(-1). How the steric and electronic properties of O2X affect conversion of 2·O2X to 3·O2X was examined. Stopped-flow analysis reveals that oxygenation kinetics of 1·O2X is unaffected by the nature of O2X, and for the first time, the benzoate analog of 2·O2X (2·O2CPh) is observed.

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Year:  2013        PMID: 23432330      PMCID: PMC3678525          DOI: 10.1021/ic302543n

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


  29 in total

1.  Dioxygen Activation by Enzymes Containing Binuclear Non-Heme Iron Clusters.

Authors:  Bradley J. Wallar; John D. Lipscomb
Journal:  Chem Rev       Date:  1996-11-07       Impact factor: 60.622

2.  Dioxygen activation at non-heme diiron centers: characterization of intermediates in a mutant form of toluene/o-xylene monooxygenase hydroxylase.

Authors:  Leslie J Murray; Ricardo García-Serres; Sunil Naik; Boi Hanh Huynh; Stephen J Lippard
Journal:  J Am Chem Soc       Date:  2006-06-14       Impact factor: 15.419

3.  (Mu-1,2-peroxo)diiron(III/III) complex as a precursor to the diiron(III/IV) intermediate X in the assembly of the iron-radical cofactor of ribonucleotide reductase from mouse.

Authors:  Danny Yun; Ricardo García-Serres; Brandon M Chicalese; Young H An; Boi Hanh Huynh; J Martin Bollinger
Journal:  Biochemistry       Date:  2007-01-27       Impact factor: 3.162

4.  Mechanistic Studies of the Formation and Decay of Diiron(III) Peroxo Complexes in the Reaction of Diiron(II) Precursors with Dioxygen.

Authors:  Andrew L. Feig; Michael Becker; Siegfried Schindler; Rudi van Eldik; Stephen J. Lippard
Journal:  Inorg Chem       Date:  1996-04-24       Impact factor: 5.165

5.  Diiron(II) mu-aqua-mu-hydroxo model for non-heme iron sites in proteins.

Authors:  Ivan V Korendovych; Sergey V Kryatov; William M Reiff; Elena V Rybak-Akimova
Journal:  Inorg Chem       Date:  2005-11-28       Impact factor: 5.165

6.  Dioxygen Activation and Methane Hydroxylation by Soluble Methane Monooxygenase: A Tale of Two Irons and Three Proteins A list of abbreviations can be found in Section 7.

Authors:  Maarten Merkx; Daniel A. Kopp; Matthew H. Sazinsky; Jessica L. Blazyk; Jens Müller; Stephen J. Lippard
Journal:  Angew Chem Int Ed Engl       Date:  2001-08-03       Impact factor: 15.336

7.  Carboxylate as the protonation site in (Peroxo)diiron(III) model complexes of soluble methane monooxygenase and related diiron proteins.

Authors:  Loi H Do; Takahiro Hayashi; Pierre Moënne-Loccoz; Stephen J Lippard
Journal:  J Am Chem Soc       Date:  2010-02-03       Impact factor: 15.419

8.  Use of a chemical trigger for electron transfer to characterize a precursor to cluster X in assembly of the iron-radical cofactor of Escherichia coli ribonucleotide reductase.

Authors:  Lana Saleh; Carsten Krebs; Brenda A Ley; Sunail Naik; Boi Hanh Huynh; J Martin Bollinger
Journal:  Biochemistry       Date:  2004-05-25       Impact factor: 3.162

9.  Revisiting the mechanism of dioxygen activation in soluble methane monooxygenase from M. capsulatus (Bath): evidence for a multi-step, proton-dependent reaction pathway.

Authors:  Christine E Tinberg; Stephen J Lippard
Journal:  Biochemistry       Date:  2009-12-29       Impact factor: 3.162

10.  Role of carboxylate bridges in modulating nonheme diiron(II)/O(2) reactivity.

Authors:  Miquel Costas; Clyde W Cady; Sergey V Kryatov; Manabendra Ray; Meghan J Ryan; Elena V Rybak-Akimova; Lawrence Que
Journal:  Inorg Chem       Date:  2003-11-17       Impact factor: 5.165

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  3 in total

1.  Versatile reactivity of a solvent-coordinated diiron(II) compound: synthesis and dioxygen reactivity of a mixed-valent Fe(II)Fe(III) species.

Authors:  Amit Majumdar; Ulf-Peter Apfel; Yunbo Jiang; Pierre Moënne-Loccoz; Stephen J Lippard
Journal:  Inorg Chem       Date:  2013-12-20       Impact factor: 5.165

2.  Pulsed Multifrequency Electron Paramagnetic Resonance Spectroscopy Reveals Key Branch Points for One- vs Two-Electron Reactivity in Mn/Fe Proteins.

Authors:  Effie C Kisgeropoulos; Yunqiao J Gan; Samuel M Greer; Joseph M Hazel; Hannah S Shafaat
Journal:  J Am Chem Soc       Date:  2022-07-05       Impact factor: 16.383

3.  (19)F NMR study of ligand dynamics in carboxylate-bridged diiron(II) complexes supported by a macrocyclic ligand.

Authors:  Mikael A Minier; Stephen J Lippard
Journal:  Dalton Trans       Date:  2015-09-29       Impact factor: 4.390

  3 in total

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