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Catalytic reduction of N2 to NH3 by an Fe-N2 complex featuring a C-atom anchor


, : Catalytic reduction of N2 to NH3 by an Fe-N2 complex featuring a C-atom anchor. Journal of the American Chemical Society 136(3): 1105-1115

While recent spectroscopic studies have established the presence of an interstitial carbon atom at the center of the iron-molybdenum cofactor (FeMoco) of MoFe-nitrogenase, its role is unknown. We have pursued Fe-N2 model chemistry to explore a hypothesis whereby this C-atom (previously denoted as a light X-atom) may provide a flexible trans interaction with an Fe center to expose an Fe-N2 binding site. In this context, we now report on Fe complexes of a new tris(phosphino)alkyl (CP(iPr)3) ligand featuring an axial carbon donor. It is established that the iron center in this scaffold binds dinitrogen trans to the C(alkyl)-atom anchor in three distinct and structurally characterized oxidation states. Fe-C(alkyl) lengthening is observed upon reduction, reflective of significant ionic character in the Fe-C(alkyl) interaction. The anionic (CP(iPr)3)FeN2(-) species can be functionalized by a silyl electrophile to generate (CP(iPr)3)Fe-N2SiR3. (CP(iPr)3)FeN2(-) also functions as a modest catalyst for the reduction of N2 to NH3 when supplied with electrons and protons at -78 °C under 1 atm N2 (4.6 equiv NH3/Fe).

US$19.90

PMID: 24350667

DOI: 10.1021/ja4114962


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