Nitrogen fixation and reduction at boron

Currently, the only compounds known to support fixation and functionalization of dinitrogen (N ) under nonmatrix conditions are based on metals. Here we present the observation of N binding and reduction by a nonmetal, specifically a dicoordinate borylene. Depending on the reaction conditions under...

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Bibliographic Details
Published in:Science (American Association for the Advancement of Science) 2018-02, Vol.359 (6378), p.896-900
Main Authors: Légaré, Marc-André, Bélanger-Chabot, Guillaume, Dewhurst, Rian D, Welz, Eileen, Krummenacher, Ivo, Engels, Bernd, Braunschweig, Holger
Format: Article
Language:English
Subjects:
Binding
Boron
Boron compounds
Chemical bonds
Coordination compounds
Crystallography
Distilled water
Electrons
Magnetic resonance spectroscopy
Metal complexes
Nitrogen
Nitrogen fixation
Nitrogen isotopes
NMR
Nonmetals
Nuclear magnetic resonance
Nuclei
Nuclei (nuclear physics)
Observation
Potassium
Protonation
Transition metals
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Summary:Currently, the only compounds known to support fixation and functionalization of dinitrogen (N ) under nonmatrix conditions are based on metals. Here we present the observation of N binding and reduction by a nonmetal, specifically a dicoordinate borylene. Depending on the reaction conditions under which potassium graphite is introduced as a reductant, N binding to two borylene units results in either neutral (B N ) or dianionic ([B N ] ) products that can be interconverted by respective exposure to further reductant or to air. The N isotopologues of the neutral and dianionic molecules were prepared with N-labeled dinitrogen, allowing observation of the nitrogen nuclei by N nuclear magnetic resonance spectroscopy. Protonation of the dianionic compound with distilled water furnishes a diradical product with a central hydrazido B N H unit. All three products were characterized spectroscopically and crystallographically.
ISSN:0036-8075
1095-9203
DOI:10.1126/science.aaq1684