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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, 58(49), 17589-17593. doi:10.1002/anie.201908689.

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 Creators:
Chang, Hao-Ching1, Author              
Lin, Yen-Hao2, Author
Werlé, Christophe3, Author
Neese, Frank4, Author              
Lee, Way-Zen2, 5, Author
Bill, Eckhard3, Author
Ye, Shengfa1, Author              
Affiliations:
1Research Group Ye, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541708              
2Department of Chemistry, National Taiwan Normal University, 88, Ting-chou Rd. Sec. 4, 11677 Taipei, Taiwan, ou_persistent22              
3Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr, Germany, ou_persistent22              
4Research Department Neese, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541710              
5Department of Medicinal and Applied Chemistry, Kaohsiung Medical University, 100, Shi-Chuan 1st Rd., 807 Kaohsiung, Taiwan, ou_persistent22              

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Free keywords: EPR spectroscopy; iron; Mössbauer spectroscopy; nitrides; nitrosyl
 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 Mössbauer investigations are presented of unprecedented oxygenation of a paramagnetic iron(V) nitrido intermediate, [FeVN(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: 2019-07-122019-09-182019-12-02
 Publication Status: Published in print
 Pages: 5
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.201908689
 Degree: -

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Title: Angewandte Chemie, International Edition
  Abbreviation : Angew. Chem., Int. Ed.
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: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851