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Catalytic Reduction of N2 to NH3 by an Fe–N2 Complex Featuring a C-Atom Anchor
Open accessAbstract
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).
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Cites
Phenol-hypochlorite reaction for determination of ammonia
Weatherburn, M. W. (1967) · Analytical Chemistry · doi:10.1021/ac60252a045 · Cited by 4,099
Structure–function relationships of alternative nitrogenases
Eady, R. R. (1996) · Chemical Reviews · doi:10.1021/cr950057h · Cited by 877
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Metadata
- Authors
- Creutz, S. E., & Peters, J. C.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-01-09
- Volume
- 136
- Issue
- 3
- Pages
- 1105-1115
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2158012127
- Cited by
- 335
- References
- 2
- FWCI
- 10.70
- Type
- journal article
- Language
- en
- Open access
- green
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