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The azadithiolate complex Fe 2 [(SCH 2 ) 26 NMe](CO) 6 reacts with borane to give an initial 1:1 adduct, which spontaneously decarbonylates to give Fe 2 [(SCH 2 ) 2 NMeBH 3 ](CO) 5 . Featuring a Fe-H-B three-center, two-electron interaction, the pentacarbonyl complex is a structural model for H 2 complexes invoked in the [FeFe]-hydrogenases. The pentacarbonyl compound is a " σ complex", where a B-H σ bond serves as a ligand for iron. The structure of this σ complex was characterized by variable-temperature NMR spectroscopy and X-ray crystallography. Complementary to the 1:1 borane adduct is the quaternary ammonium complex [Fe 2 ](SCH 2 ) 2 NMe 2 ](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.

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