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Title: Achieving One-Electron Oxidation of a Mononuclear Nonheme Iron(V)-Imido Complex

Abstract

Here, a mononuclear nonheme iron(V)-imido complex bearing a tetraamido macrocyclic ligand (TAML), [FeV(NTs)(TAML)] (1), was oxidized by one-electron oxidants, affording formation of an iron(V)-imido TAML cation radical species, [FeV(NTs)(TAML+•)] (2); 2 is a diamagnetic (S = 0) complex, resulting from the antiferromagnetic coupling of the low-spin iron(V) ion (S = 1/2) with the one-electron oxidized ligand (TAML+•). 2 is a competent oxidant in C–H bond functionalization and nitrene transfer reaction, showing that the reactivity of 2 is greater than that of 1.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [2];  [2];  [3];  [3];  [4];  [4];  [4];  [5]; ORCiD logo [6]
  1. Ewha Womans Univ., Seoul (Korea); Sookmyung Women's Univ., Seoul (Korea)
  2. Ewha Womans Univ., Seoul (Korea)
  3. Univ. of Hyogo, Hyogo (Japan)
  4. Univ. Grenoble Alpes, Grenoble (France)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. Ewha Womans Univ., Seoul (Korea); Chinese Academy of Sciences, Lanzhou (China)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1419655
Grant/Contract Number:  
AC02-76SF00515; ANR-11-LABX-003; NRF-2010-00353; NRF-2012R1A3A2048842; NRF-2017R1C1B2002037; 15H00960; P41GM103393
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 41; 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

Hong, Seungwoo, Lu, Xiaoyan, Lee, Yong -Min, Seo, Mi Sook, Ohta, Takehiro, Ogura, Takashi, Clemancey, Martin, Maldivi, Pascale, Latour, Jean -Marc, Sarangi, Ritimukta, and Nam, Wonwoo. Achieving One-Electron Oxidation of a Mononuclear Nonheme Iron(V)-Imido Complex. United States: N. p., 2017. Web. doi:10.1021/jacs.7b08161.
Hong, Seungwoo, Lu, Xiaoyan, Lee, Yong -Min, Seo, Mi Sook, Ohta, Takehiro, Ogura, Takashi, Clemancey, Martin, Maldivi, Pascale, Latour, Jean -Marc, Sarangi, Ritimukta, & Nam, Wonwoo. Achieving One-Electron Oxidation of a Mononuclear Nonheme Iron(V)-Imido Complex. United States. doi:10.1021/jacs.7b08161.
Hong, Seungwoo, Lu, Xiaoyan, Lee, Yong -Min, Seo, Mi Sook, Ohta, Takehiro, Ogura, Takashi, Clemancey, Martin, Maldivi, Pascale, Latour, Jean -Marc, Sarangi, Ritimukta, and Nam, Wonwoo. Fri . "Achieving One-Electron Oxidation of a Mononuclear Nonheme Iron(V)-Imido Complex". United States. doi:10.1021/jacs.7b08161. https://www.osti.gov/servlets/purl/1419655.
@article{osti_1419655,
title = {Achieving One-Electron Oxidation of a Mononuclear Nonheme Iron(V)-Imido Complex},
author = {Hong, Seungwoo and Lu, Xiaoyan and Lee, Yong -Min and Seo, Mi Sook and Ohta, Takehiro and Ogura, Takashi and Clemancey, Martin and Maldivi, Pascale and Latour, Jean -Marc and Sarangi, Ritimukta and Nam, Wonwoo},
abstractNote = {Here, a mononuclear nonheme iron(V)-imido complex bearing a tetraamido macrocyclic ligand (TAML), [FeV(NTs)(TAML)]– (1), was oxidized by one-electron oxidants, affording formation of an iron(V)-imido TAML cation radical species, [FeV(NTs)(TAML+•)] (2); 2 is a diamagnetic (S = 0) complex, resulting from the antiferromagnetic coupling of the low-spin iron(V) ion (S = 1/2) with the one-electron oxidized ligand (TAML+•). 2 is a competent oxidant in C–H bond functionalization and nitrene transfer reaction, showing that the reactivity of 2 is greater than that of 1.},
doi = {10.1021/jacs.7b08161},
journal = {Journal of the American Chemical Society},
number = 41,
volume = 139,
place = {United States},
year = {2017},
month = {9}
}

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Works referencing / citing this record:

Generation and Reactivity of a One‐Electron‐Oxidized Manganese(V) Imido Complex with a Tetraamido Macrocyclic Ligand
journal, August 2019

  • Shi, Huatian; Xie, Jianhui; Lam, William W. Y.
  • Chemistry – A European Journal, Vol. 25, Issue 56
  • DOI: 10.1002/chem.201902405

C–H activation and nucleophilic substitution in a photochemically generated high valent iron complex
journal, January 2018

  • Lim, Jia Hui; Engelmann, Xenia; Corby, Sacha
  • Chemical Science, Vol. 9, Issue 16
  • DOI: 10.1039/c7sc05378a

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

Generation and Reactivity of a One‐Electron‐Oxidized Manganese(V) Imido Complex with a Tetraamido Macrocyclic Ligand
journal, August 2019

  • Shi, Huatian; Xie, Jianhui; Lam, William W. Y.
  • Chemistry – A European Journal, Vol. 25, Issue 56
  • DOI: 10.1002/chem.201902405

C–H activation and nucleophilic substitution in a photochemically generated high valent iron complex
journal, January 2018

  • Lim, Jia Hui; Engelmann, Xenia; Corby, Sacha
  • Chemical Science, Vol. 9, Issue 16
  • DOI: 10.1039/c7sc05378a

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