Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 27, Pages 8586-8598Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b04828
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Funding
- National Institutes of Health [GM065313, GM116463, GM114787]
- Max Planck Society
- NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES [F31GM116463, R15GM114787, R01GM065313] Funding Source: NIH RePORTER
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Distinguishing the reactivity differences between N-2 complexes having different binding modes is crucial for the design of effective N-2-functionalizing reactions. Here, we compare the reactions of a K-bridged, dinuclear FeNNFe complex with a monomeric Fe(N-2) complex where the bimetallic core is broken up by the addition of chelating agents. The new anionic iron(0) dinitrogen complex has enhanced electron density at the distal N atoms of coordinated N-2, and though the N-2 is not as weakened in this monomeric compound, it is much more reactive toward silylation by (CH3)(3)SiI (TMSI). Double silylation of N-2 gives a three-coordinate iron(III) hydrazido(2-) complex, which is finely balanced between coexisting S = 1/2 and S = 3/2 states that are characterized by crystallography, spectroscopy, and computations. These results give insight into the interdependence between binding modes, alkali dependence, reactivity, and magnetic properties within an iron system that functionalizes N-2.
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