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Title: A Mononuclear Nonheme Iron(IV)–Amido Complex Relevant for the Compound II Chemistry of Cytochrome P450

Abstract

A mononuclear nonheme iron(IV)–amido complex bearing a tetraamido macrocyclic ligand, [(TAML)Fe IV(NHTs)] - (1), was synthesized via a hydrogen atom (H atom) abstraction reaction of an iron(V)–imido complex, [(TAML)FeV(NTs)]- (2), and fully characterized using various spectroscopies. We then investigated (1) the pK a of 1, (2) the reaction of 1 with a carbon-centered radical, and (3) the H atom abstraction reaction of 1. To the best of our knowledge, the present study reports for the first time the synthesis and chemical properties/reactions of a high-valent iron(IV)–amido complex.

Authors:
 [1];  [1];  [1]; ORCiD logo [1];  [2];  [2];  [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Ewha Womans Univ., Seoul (Korea). Dept. of Chemistry and Nano Science
  2. Univ. Grenoble Alpes, Genoble (France)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Institutes of Health (NIH)
OSTI Identifier:
1493335
Grant/Contract Number:  
AC02-76SF00515; P41GM103393; A0040807648
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 1; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lu, Xiaoyan, Li, Xiao-Xi, Seo, Mi Sook, Lee, Yong-Min, Clémancey, Martin, Maldivi, Pascale, Latour, Jean-Marc, Sarangi, Ritimukta, Fukuzumi, Shunichi, and Nam, Wonwoo. A Mononuclear Nonheme Iron(IV)–Amido Complex Relevant for the Compound II Chemistry of Cytochrome P450. United States: N. p., 2018. Web. doi:10.1021/jacs.8b11045.
Lu, Xiaoyan, Li, Xiao-Xi, Seo, Mi Sook, Lee, Yong-Min, Clémancey, Martin, Maldivi, Pascale, Latour, Jean-Marc, Sarangi, Ritimukta, Fukuzumi, Shunichi, & Nam, Wonwoo. A Mononuclear Nonheme Iron(IV)–Amido Complex Relevant for the Compound II Chemistry of Cytochrome P450. United States. doi:10.1021/jacs.8b11045.
Lu, Xiaoyan, Li, Xiao-Xi, Seo, Mi Sook, Lee, Yong-Min, Clémancey, Martin, Maldivi, Pascale, Latour, Jean-Marc, Sarangi, Ritimukta, Fukuzumi, Shunichi, and Nam, Wonwoo. Sat . "A Mononuclear Nonheme Iron(IV)–Amido Complex Relevant for the Compound II Chemistry of Cytochrome P450". United States. doi:10.1021/jacs.8b11045. https://www.osti.gov/servlets/purl/1493335.
@article{osti_1493335,
title = {A Mononuclear Nonheme Iron(IV)–Amido Complex Relevant for the Compound II Chemistry of Cytochrome P450},
author = {Lu, Xiaoyan and Li, Xiao-Xi and Seo, Mi Sook and Lee, Yong-Min and Clémancey, Martin and Maldivi, Pascale and Latour, Jean-Marc and Sarangi, Ritimukta and Fukuzumi, Shunichi and Nam, Wonwoo},
abstractNote = {A mononuclear nonheme iron(IV)–amido complex bearing a tetraamido macrocyclic ligand, [(TAML)FeIV(NHTs)]- (1), was synthesized via a hydrogen atom (H atom) abstraction reaction of an iron(V)–imido complex, [(TAML)FeV(NTs)]- (2), and fully characterized using various spectroscopies. We then investigated (1) the pKa of 1, (2) the reaction of 1 with a carbon-centered radical, and (3) the H atom abstraction reaction of 1. To the best of our knowledge, the present study reports for the first time the synthesis and chemical properties/reactions of a high-valent iron(IV)–amido complex.},
doi = {10.1021/jacs.8b11045},
journal = {Journal of the American Chemical Society},
number = 1,
volume = 141,
place = {United States},
year = {2018},
month = {11}
}

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Works referencing / citing this record:

Octahedral iron( iv )–tosylimido complexes exhibiting single electron-oxidation reactivity
journal, January 2019

  • Sabenya, Gerard; Gamba, Ilaria; Gómez, Laura
  • Chemical Science, Vol. 10, Issue 41
  • DOI: 10.1039/c9sc02526j