O2 Activation by Non-Heme Iron Enzymes

Solomon, Edward I.; Goudarzi, Serra; Sutherlin, Kyle D.

doi:10.1021/acs.biochem.6b00635

Title: O₂ Activation by Non-Heme Iron Enzymes

Journal Article · Fri Oct 28 00:00:00 EDT 2016 · Biochemistry

DOI:https://doi.org/10.1021/acs.biochem.6b00635· OSTI ID:1360202

Solomon, Edward I. ^[1]; Goudarzi, Serra ^[2]; Sutherlin, Kyle D. ^[2]

Stanford Univ., CA (United States). Dept. of Chemistry; SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., CA (United States). Dept. of Chemistry

The non-heme Fe enzymes are ubiquitous in nature and perform a wide range of functions involving O₂ activation. These had been difficult to study relative to heme enzymes; however, spectroscopic methods have now been developed that provide significant insight into the correlation of structure with function. This Current Topics article summarizes both the molecular mechanism these enzymes use to control O₂ activation in the presence of cosubstrates and the oxygen intermediates these reactions generate. Three types of O₂ activation are observed. First, non-heme reactivity is shown to be different from heme chemistry where a low-spin Fe^III-OOH non-heme intermediate directly reacts with substrate. Also, two subclasses of non-heme Fe enzymes generate high-spin Fe^IV=O intermediates that provide both σ and π frontier molecular orbitals that can control selectivity. Lastly, for several subclasses of non-heme Fe enzymes, substrate binding to the Fe^II site leads to the one electron reductive activation of O₂ to an Fe^III-superoxide capable of H-atom abstraction and electrophilic attack.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; National Institutes of Health (NIH)

Grant/Contract Number:: AC02-76SF00515; GM-40392

OSTI ID:: 1360202

Journal Information:: Biochemistry, Vol. 55, Issue 46; ISSN 0006-2960

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 97 works

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