Literature DB >> 16201783

Photochemical generation of a highly reactive iron-oxo intermediate. A true iron(V)-oxo species?

Dilusha N Harischandra1, Rui Zhang, Martin Newcomb.   

Abstract

Laser flash photolysis of 5,10,15-tris(pentafluorophenyl)corrole-iron(IV) chlorate or nitrate, prepared from the corresponding chloride, gave a highly reactive iron-oxo transient identified as an iron(V)-oxo species on the basis of its UV-visible spectrum and high reactivity as well as by analogy to photochemical ligand cleavage reactions of related manganese species. The transient was shown to be an oxo transfer agent in a preparative reaction with cis-cyclooctene. Representative rate constants for oxidation reactions by the new transient at ambient temperature were k = 5900 M-1 s-1 for cyclooctene and k = 570 M-1 s-1 for ethylbenzene. The new transient is more than 6 orders of magnitude more reactive with typical organic reductants than expected for an iron(IV)-oxo corrole radical cation and 100 times more reactive than an analogous positively charged iron(IV)-oxo porphyrin radical cation. Slow electron transfer isomerization of ligand iron(V)-oxo species to iron(IV)-oxo ligand radical cations might be important in reactions of porphyrin-iron catalysts in the laboratory and in nature.

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Year:  2005        PMID: 16201783     DOI: 10.1021/ja0542439

Source DB:  PubMed          Journal:  J Am Chem Soc        ISSN: 0002-7863            Impact factor:   15.419


  19 in total

1.  Cytochrome p450 compound I.

Authors:  Martin Newcomb; Rui Zhang; R Esala P Chandrasena; James A Halgrimson; John H Horner; Thomas M Makris; Stephen G Sligar
Journal:  J Am Chem Soc       Date:  2006-04-12       Impact factor: 15.419

2.  Transition metal spin state energetics and noninnocent systems: challenges for DFT in the bioinorganic arena.

Authors:  Abhik Ghosh
Journal:  J Biol Inorg Chem       Date:  2006-07-14       Impact factor: 3.358

3.  A Synthetic Oxygen Atom Transfer Photocycle from a Diruthenium Oxyanion Complex.

Authors:  Amanda R Corcos; József S Pap; Tzuhsiung Yang; John F Berry
Journal:  J Am Chem Soc       Date:  2016-07-28       Impact factor: 15.419

4.  Photochemical generation and kinetic studies of a putative porphyrin-ruthenium(V)-oxo species.

Authors:  Rui Zhang; Eric Vanover; Weilong Luo; Martin Newcomb
Journal:  Dalton Trans       Date:  2014-06-21       Impact factor: 4.390

5.  Photocatalytic Oxygenation of Substrates by Dioxygen with Protonated Manganese(III) Corrolazine.

Authors:  Jieun Jung; Heather M Neu; Pannee Leeladee; Maxime A Siegler; Kei Ohkubo; David P Goldberg; Shunichi Fukuzumi
Journal:  Inorg Chem       Date:  2016-03-14       Impact factor: 5.165

6.  Spectra and kinetic studies of the compound I derivative of cytochrome P450 119.

Authors:  Xin Sheng; John H Horner; Martin Newcomb
Journal:  J Am Chem Soc       Date:  2008-09-13       Impact factor: 15.419

7.  Photochemical production of a highly reactive porphyrin-iron-oxo species.

Authors:  Zhengzheng Pan; Rui Zhang; Leslie W-M Fung; Martin Newcomb
Journal:  Inorg Chem       Date:  2007-02-07       Impact factor: 5.165

Review 8.  Hydrocarbon hydroxylation by cytochrome P450 enzymes.

Authors:  Paul R Ortiz de Montellano
Journal:  Chem Rev       Date:  2010-02-10       Impact factor: 60.622

Review 9.  Laser flash photolysis generation of high-valent transition metal-oxo species: insights from kinetic studies in real time.

Authors:  Rui Zhang; Martin Newcomb
Journal:  Acc Chem Res       Date:  2008-02-16       Impact factor: 22.384

10.  Quantitative production of compound I from a cytochrome P450 enzyme at low temperatures. Kinetics, activation parameters, and kinetic isotope effects for oxidation of benzyl alcohol.

Authors:  Qin Wang; Xin Sheng; John H Horner; Martin Newcomb
Journal:  J Am Chem Soc       Date:  2009-08-05       Impact factor: 15.419

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