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Catalytic Silylation of Dinitrogen by a Family of Triiron Complexes

By Ricardo B. Ferreira, Brian J. Cook, Brian J. Knight, Vincent J. Catalano, Ricardo Garcia-Serres and Leslie J. Murray

Abstract

International audienceA series of triiron complexes supported by a tris(beta-diketiminate)cyclophane (L-3) catalyze the reduction of dinitrogen to tris(trimethylsilyl)amine using KC8 and Me3SiCl. Employing Fe3Br3L affords 83 +/- 7 equiv of NH4+/complex after protonolysis, which is a 50% yield, based on reducing equivalents. The series of triiron compounds tested evidence the subtle effects of ancillary donors, including halides, hydrides, sulfides, and carbonyl ligands, and metal oxidation state on N(SiMe3)(3) yield, and highlight Fe-3(mu(3)-N)L as a common species in product mixtures. These results suggest that ancillary ligands can be abstracted with Lewis acids under reducing conditions

Topics: multinucleating ligand, N-2 reduction, N-2 silylation, iron clusters, trinuclear clusters, [CHIM.COOR]Chemical Sciences/Coordination chemistry, [CHIM.CATA]Chemical Sciences/Catalysis
Publisher: 'American Chemical Society (ACS)'
Year: 2018
DOI identifier: 10.1021/acscatal.8b02021
OAI identifier: oai:HAL:hal-01896886v1
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