Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions.
Although stoichiometric transformations using transition metal-N(2) complexes have been well investigated towards the goal of nitrogen fixation under mild reaction conditions, only a few examples of the catalytic transformations of N(2) using transition metal-N(2) complexes as catalysts have been reported. In almost all the catalytic systems, the use of Mo is essential to realize the catalytic transformation of N(2), where Mo-N(2) complexes are considered to work as effective catalysts. Here we show the first successful example of the Fe-catalysed transformation of N(2) into N(SiMe(3))(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)-N(2) complex bearing two Me(3)Si groups as ancillary ligands has an important role as a key reactive intermediate, with the aid of density-functional-theory calculations.