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Synthesis of a Nitrogenase PN -Cluster Model with [Fe8 S7 (µ-Sthiolate )2 ] Core from the All-Ferric [Fe4 S4 (Sthiolate )4 ] Cubane Synthon.
Moula, Golam; Nagasaki, Ayaka; Matsumoto, Tsuyoshi; Miehlich, Matthias E; Meyer, Karsten; Cramer, Roger E; Tatsumi, Kazuyuki.
Afiliação
  • Moula G; Research Center for Materials Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, 464-8602, Japan.
  • Nagasaki A; Research Center for Materials Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, 464-8602, Japan.
  • Matsumoto T; Institute of Transformative Bio-Molecules (WPI-ITbM), Nagoya University, Furo-cho, Chikusa-ku, Nagoya, 464-8601, Japan.
  • Miehlich ME; Department of Chemistry and Pharmacy, Inorganic Chemistry, Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Egerlandstrasse 1, 91058, Erlangen, Germany.
  • Meyer K; Department of Chemistry and Pharmacy, Inorganic Chemistry, Friedrich-Alexander-University Erlangen-Nürnberg (FAU), Egerlandstrasse 1, 91058, Erlangen, Germany.
  • Cramer RE; Department of Chemistry, University of Hawaii, Honolulu, HI, 96822, USA.
  • Tatsumi K; Research Center for Materials Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, 464-8602, Japan.
Angew Chem Int Ed Engl ; 60(29): 15792-15797, 2021 07 12.
Article em En | MEDLINE | ID: mdl-33928749
ABSTRACT
Constructing synthetic models of the nitrogenase PN -cluster has been a long-standing synthetic challenge. Here, we report an optimal nitrogenase PN -cluster model [{(TbtS)(OEt2 )Fe4 S3 }2 (µ-STbt)2 (µ6 -S)] (2) [Tbt=2,4,6-tris{bis(trimethylsilyl)methyl}phenyl] that is the closest synthetic mimic constructed to date. Of note is that two thiolate ligands and one hexacoordinated sulfide are connecting the two Fe4 S3 incomplete cubanes similar to the native PN -cluster, which has never been achieved. Cluster 2 has been characterized by X-ray crystallography and relevant physico-chemical methods. The variable temperature magnetic moments of 2 indicate a singlet ground state (S=0). The Mössbauer spectrum of 2 exhibits two doublets with an intensity ratio of 31, which suggests the presence of two types of iron sites. The synthetic pathway of the cluster 2 could indicate the native PN -cluster maturation process as it has been achieved from the Fe4 S4 cubane Fe4 S4 (STbt)4 (1).
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Texto completo: 1 Base de dados: MEDLINE Assunto principal: Enxofre / Compostos Férricos / Ferro / Nitrogenase Tipo de estudo: Prognostic_studies País como assunto: Cuba Idioma: En Ano de publicação: 2021 Tipo de documento: Article

Texto completo: 1 Base de dados: MEDLINE Assunto principal: Enxofre / Compostos Férricos / Ferro / Nitrogenase Tipo de estudo: Prognostic_studies País como assunto: Cuba Idioma: En Ano de publicação: 2021 Tipo de documento: Article