Triggering N(2) uptake via redox-induced expulsion of coordinated NH(3) and N(2) silylation at trigonal bipyramidal iron

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The biological reduction of N-2 to give NH3 may occur by one of two predominant pathways in which nitrogenous NxHy intermediates, including hydrazine (N2H4), diazene (N2H2), nitride (N-3(-)) and imide (NH2-), may be involved. To test the validity of hypotheses on iron's direct role in the stepwise reduction of N-2, model systems for iron are needed. Such systems can test the chemical compatibility of iron with various proposed NxHy intermediates and the reactivity patterns of such species. Here we describe a trigonal bipyramidal Si(o-C6H4PR2)(3)Fe-L scaffold (R = Ph or i-Pr) in which the apical site is occupied by nitrogenous ligands such as N-2, N-2 H-4, NH3 and N2R. The system accommodates terminally bound N-2 in the three formal oxidation states (iron(0), +1 and +2). N-2 uptake is demonstrated by the displacement of its reduction partners NH3 and N2H4, and N-2 functionalizaton is illustrated by electrophilic silylation.
Publisher
NATURE PUBLISHING GROUP
Issue Date
2010-07
Language
English
Article Type
Article
Keywords

RAY CRYSTAL-STRUCTURES; TRIS(PHOSPHINO)SILYL LIGANDS; FEMO COFACTOR; COMPLEXES; DINITROGEN; REDUCTION; NITROGENASE; REACTIVITY; DIAZENE; METAL

Citation

NATURE CHEMISTRY, v.2, no.7, pp.558 - 565

ISSN
1755-4330
DOI
10.1038/NCHEM.660
URI
http://hdl.handle.net/10203/97759
Appears in Collection
CH-Journal Papers(저널논문)
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