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Acc Chem Res. 2007 Jul;40(7):532-42. Epub 2007 May 9.

Reactivity of high-valent iron-oxo species in enzymes and synthetic reagents: a tale of many states.

Author information

  • 1Department of Organic Chemistry and The Lise Meitner-Minerva Center for Computational Quantum Chemistry, The Hebrew University of Jerusalem, Givat Ram Campus, 91904 Jerusalem, Israel. sason@yfaat.ch.huji.ac.il

Abstract

The Account discusses the phenomenon of two-state reactivity (TSR) or multistate reactivity (MSR) in high-valent metal-oxo reagents, projecting its wide-ranging applicability starting from the bare species, through the reagents made by Que, Nam, and collaborators, to the Mn(V)-oxo substituted polyoxometalate, all the way to Compound I species of heme enzymes. The Account shows how the behaviors of all these variegated species derive from a simple set of electronic structure principles. Experimental trends that demonstrate TSR and MSR are discussed. Diagnostic mechanistic probes are proposed for the TSR/MSR scenario, based on kinetic isotope effect, stereochemical studies, and magnetic- and electric-field effects.

PMID:
17488054
DOI:
10.1021/ar600042c
[PubMed - indexed for MEDLINE]
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