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  Conversion of a Fleeting Open-Shell Iron Nitride into an Iron Nitrosyl

Chang, H.-C., Lin, Y.-H., Werlé, C., Neese, F., Lee, W.-Z., Bill, E., et al. (2019). Conversion of a Fleeting Open-Shell Iron Nitride into an Iron Nitrosyl. Angewandte Chemie, International Edition in English, 58(49), 17589-17593. doi:10.1002/anie.201908689.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0005-A9D7-A Version Permalink: http://hdl.handle.net/21.11116/0000-0005-A9D8-9
Genre: Journal Article

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 Creators:
Chang, Hao-Ching, Author
Lin, Yen-Hao, Author
Werlé, Christophe1, Author              
Neese, Frank, Author
Lee, Way-Zen, Author
Bill, Eckhard2, Author              
Ye, Shengfa, Author
Affiliations:
1Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023874              
2Research Department DeBeer, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023871              

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 Abstract: Terminal metal nitrides have been proposed as key intermediates in a series of pivotal chemical transformations. However, exploring the chemical activity of transient tetragonal iron(V) nitrides is largely impeded by their facile dimerization in fluid solutions. Herein, in situ EPR and Mossbauer investigations are presented of unprecedented oxygenation of a paramagnetic iron(V) nitrido intermediate, [(FeN)-N-V(cyclam-ac)](+) (2, cyclam-ac(-)=1,4,8,11-tetraazacyclotetradecane-1-acetate anion), yielding an iron nitrosyl complex, [Fe(NO)(cyclam-ac)](+) (3). Further theoretical studies suggest that during the reaction a closed-shell singlet O atom is transferred to 2. Consequently, the N-O bond formation does not follow a radical coupling mechanism proposed for the N-N bond formation but is accomplished by three mutual electron-transfer pathways between 2 and the O atom donor, thanks to the ambiphilic nature of 2.

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Language(s): eng - English
 Dates: 2019
 Publication Status: Published in print
 Pages: -
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: ISI: 000491791300001
DOI: 10.1002/anie.201908689
 Degree: -

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Title: Angewandte Chemie, International Edition in English
  Abbreviation : Angew. Chem., Int. Ed. Engl.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 58 (49) Sequence Number: - Start / End Page: 17589 - 17593 Identifier: ISSN: 0570-0833
CoNE: https://pure.mpg.de/cone/journals/resource/0570-0833