Structure and reactivity of a mononuclear non-haem iron(III)–peroxo complex

Jaeheung Cho, Sujin Jeon, Samuel A. Wilson, Lei V. Liu, Eun A. Kang, Joseph J. Braymer, Mi Hee Lim, Britt Hedman, Keith O. Hodgson, Joan Selverstone Valentine (), Edward I. Solomon () and Wonwoo Nam ()
Additional contact information
Jaeheung Cho: Center for Biomimetic Systems, Ewha Womans University, Seoul 120-750, Korea
Sujin Jeon: Center for Biomimetic Systems, Ewha Womans University, Seoul 120-750, Korea
Samuel A. Wilson: Stanford University, Stanford, California 94305, USA
Lei V. Liu: Stanford University, Stanford, California 94305, USA
Eun A. Kang: Center for Biomimetic Systems, Ewha Womans University, Seoul 120-750, Korea
Joseph J. Braymer: University of Michigan
Mi Hee Lim: University of Michigan
Britt Hedman: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Stanford University
Keith O. Hodgson: Stanford University, Stanford, California 94305, USA
Joan Selverstone Valentine: Center for Biomimetic Systems, Ewha Womans University, Seoul 120-750, Korea
Edward I. Solomon: Stanford University, Stanford, California 94305, USA
Wonwoo Nam: Center for Biomimetic Systems, Ewha Womans University, Seoul 120-750, Korea

Nature, 2011, vol. 478, issue 7370, 502-505

Abstract: Iron–oxygen intermediates identified The iron–oxygen species iron(III)-peroxo, iron(III)-hydroperoxo and iron(IV)-oxo are key intermediates often detected in the catalytic cycles of dioxygen activation by haem and non-haem iron enzymes. The high-resolution crystal structure of a mononuclear non-haem side-on iron(III)-peroxo complex has now been determined, and a series of chemical reactions in which the iron(III)-peroxo complex is cleanly converted to an iron(III)-hydroperoxo complex is described. All three of these iron species have been spectroscopically characterized, and relative reactivity studies demonstrate that iron(III)-hydroperoxo species are viable oxidants in both nucleophilic and electrophilic reactions by iron-containing enzymes. This work shows how a series of biologically important iron–oxygen intermediates make use of a synthetic iron complex bearing a simple but versatile macrocyclic ligand.

Date: 2011
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DOI: 10.1038/nature10535

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