Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions
Abstract
Although stoichiometric transformations using transition metal-N2 complexes have been well investigated towards the goal of nitrogen fixation under mild reaction conditions, only a few examples of the catalytic transformations of N2 using transition metal-N2 complexes as catalysts have been reported. In almost all the catalytic systems, the use of Mo is essential to realize the catalytic transformation of N2, where Mo-N2 complexes are considered to work as effective catalysts. Here we show the first successful example of the Fe-catalysed transformation of N2 into N(SiMe3)3 under ambient conditions, in which iron complexes such as iron pentacarbonyl [Fe(CO)5] and ferrocenes have been found to work as effective catalysts. A plausible reaction pathway is proposed, where Fe(II)-N2 complex bearing two Me3Si groups as ancillary ligands has an important role as a key reactive intermediate, with the aid of density-functional-theory calculations.
- Publication:
-
Nature Communications
- Pub Date:
- December 2012
- DOI:
- 10.1038/ncomms2264
- Bibcode:
- 2012NatCo...3.1254Y