Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions

Masahiro Yuki, Hiromasa Tanaka, Kouitsu Sasaki, Yoshihiro Miyake, Kazunari Yoshizawa () and Yoshiaki Nishibayashi ()
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Masahiro Yuki: Institute of Engineering Innovation, School of Engineering, University of Tokyo, Yayoi, Bunkyo-ku, Tokyo 113-8656, Japan.
Hiromasa Tanaka: Institute for Materials Chemistry and Engineering, International Research Center for Molecular Systems, Kyushu University, Nishi-ku, Fukuoka 819-0395, Japan.
Kouitsu Sasaki: Institute of Engineering Innovation, School of Engineering, University of Tokyo, Yayoi, Bunkyo-ku, Tokyo 113-8656, Japan.
Yoshihiro Miyake: Institute of Engineering Innovation, School of Engineering, University of Tokyo, Yayoi, Bunkyo-ku, Tokyo 113-8656, Japan.
Kazunari Yoshizawa: Institute for Materials Chemistry and Engineering, International Research Center for Molecular Systems, Kyushu University, Nishi-ku, Fukuoka 819-0395, Japan.
Yoshiaki Nishibayashi: Institute of Engineering Innovation, School of Engineering, University of Tokyo, Yayoi, Bunkyo-ku, Tokyo 113-8656, Japan.

Nature Communications, 2012, vol. 3, issue 1, 1-6

Abstract: 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.

Date: 2012
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DOI: 10.1038/ncomms2264

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