Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 19, Pages 7332-7349Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201906551
Keywords
C-H bond cleavage; high-valent iron-oxo species; nonheme iron enzymes; oxidation catalysis
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Funding
- US Department of Energy
- National Institutes of Health
- National Science Foundation
- University of Minnesota
- National Science Foundation [CHE-1665391]
- National Institutes of Health [R01 GM-38767, R35 GM-131721]
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Nonheme iron enzymes generate powerful and versatile oxidants that perform a wide range of oxidation reactions, including the functionalization of inert C-H bonds, which is a major challenge for chemists. The oxidative abilities of these enzymes have inspired bioinorganic chemists to design synthetic models to mimic their ability to perform some of the most difficult oxidation reactions and study the mechanisms of such transformations. Iron-oxygen intermediates like iron(III)-hydroperoxo and high-valent iron-oxo species have been trapped and identified in investigations of these bio-inspired catalytic systems, with the latter proposed to be the active oxidant for most of these systems. In this Review, we highlight the recent spectroscopic and mechanistic advances that have shed light on the various pathways that can be accessed by bio-inspired nonheme iron systems to form the high-valent iron-oxo intermediates.
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