Nature of the peroxo intermediate of the W48F/D84E ribonucleotide reductase variant: implications for O2 activation by binuclear non-heme iron enzymes

Journal of the American Chemical Society
A J SkulanE I Solomon

Abstract

Analysis of the spectroscopic signatures of the R2-W48F/D84E biferric peroxo intermediate identifies a cis mu-1,2 peroxo coordination geometry. DFT geometry optimizations on both R2-W48F/D84E and R2-wild-type peroxo intermediate models including constraints imposed by the protein also identify the cis mu-1,2 peroxo geometry as the most stable peroxo intermediate structure. This study provides significant insight into the electronic structure and reactivity of the R2-W48F/D84E peroxo intermediate, structurally related cis mu-1,2 peroxo model complexes, and other enzymatic biferric peroxo intermediates.

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Citations

Mar 12, 2011·Accounts of Chemical Research·Christine E Tinberg, Stephen J Lippard
Mar 1, 2007·Journal of the American Chemical Society·David RinaldoRichard A Friesner
Jun 26, 2008·Journal of the American Chemical Society·Jennifer K SchwartzEdward I Solomon
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Aug 27, 2009·Proceedings of the National Academy of Sciences of the United States of America·Van V VuLawrence Que
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