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Characterization of a Borane ? Complex of a Diiron Dithiolate: Model for an Elusive Dihydrogen Adduct.


ABSTRACT: The azadithiolate complex Fe2[(SCH2)26NMe](CO)6 reacts with borane to give an initial 1:1 adduct, which spontaneously decarbonylates to give Fe2[(SCH2)2NMeBH3](CO)5. Featuring a Fe-H-B three-center, two-electron interaction, the pentacarbonyl complex is a structural model for H2 complexes invoked in the [FeFe]-hydrogenases. The pentacarbonyl compound is a "? complex", where a B-H ? bond serves as a ligand for iron. The structure of this ? complex was characterized by variable-temperature NMR spectroscopy and X-ray crystallography. Complementary to the 1:1 borane adduct is the quaternary ammonium complex [Fe2](SCH2)2NMe2](CO)6]+, which was also characterized. It represents a kinetically robust analogue of the N-protonated amine cofactor, as indicated by its mild reduction potential.

SUBMITTER: Lalaoui N 

PROVIDER: S-EPMC5538135 | biostudies-literature | 2017 Jun

REPOSITORIES: biostudies-literature

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Characterization of a Borane <i>σ</i> Complex of a Diiron Dithiolate: Model for an Elusive Dihydrogen Adduct.

Lalaoui Noémie N   Woods Toby T   Rauchfuss Thomas B TB   Zampella Giuseppe G  

Organometallics 20170516 11


The azadithiolate complex Fe<sub>2</sub>[(SCH<sub>2</sub>)<sub>26</sub>NMe](CO)<sub>6</sub> reacts with borane to give an initial 1:1 adduct, which spontaneously decarbonylates to give Fe<sub>2</sub>[(SCH<sub>2</sub>)<sub>2</sub>NMeBH<sub>3</sub>](CO)<sub>5</sub>. Featuring a Fe-H-B three-center, two-electron interaction, the pentacarbonyl complex is a structural model for H<sub>2</sub> complexes invoked in the [FeFe]-hydrogenases. The pentacarbonyl compound is a "<i>σ</i> complex", where a B-H  ...[more]

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