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

Masahiro Yuki, Hiromasa Tanaka, Kouitsu Sasaki, Yoshihiro Miyake, Kazunari Yoshizawa, Yoshiaki Nishibayashi

Research output: Contribution to journalArticle

76 Citations (Scopus)

Abstract

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 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 Me 3Si groups as ancillary ligands has an important role as a key reactive intermediate, with the aid of density-functional-theory calculations.

Original languageEnglish
Article number1254
JournalNature communications
Volume3
DOIs
Publication statusPublished - Dec 1 2012

Fingerprint

Iron
iron
Nitrogen Fixation
Catalysts
Transition metals
Coordination Complexes
Bearings (structural)
catalysts
Nitrogen fixation
Metals
transition metals
ferrocenes
nitrogenation
Metal complexes
Ligands
Density functional theory
density functional theory
ligands
iron pentacarbonyl

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions. / Yuki, Masahiro; Tanaka, Hiromasa; Sasaki, Kouitsu; Miyake, Yoshihiro; Yoshizawa, Kazunari; Nishibayashi, Yoshiaki.

In: Nature communications, Vol. 3, 1254, 01.12.2012.

Research output: Contribution to journalArticle

Yuki, Masahiro ; Tanaka, Hiromasa ; Sasaki, Kouitsu ; Miyake, Yoshihiro ; Yoshizawa, Kazunari ; Nishibayashi, Yoshiaki. / Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions. In: Nature communications. 2012 ; Vol. 3.
@article{362f692a6c4d4e10b3bd25b2d133d4a3,
title = "Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions",
abstract = "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 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 Me 3Si groups as ancillary ligands has an important role as a key reactive intermediate, with the aid of density-functional-theory calculations.",
author = "Masahiro Yuki and Hiromasa Tanaka and Kouitsu Sasaki and Yoshihiro Miyake and Kazunari Yoshizawa and Yoshiaki Nishibayashi",
year = "2012",
month = "12",
day = "1",
doi = "10.1038/ncomms2264",
language = "English",
volume = "3",
journal = "Nature Communications",
issn = "2041-1723",
publisher = "Nature Publishing Group",

}

TY - JOUR

T1 - Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions

AU - Yuki, Masahiro

AU - Tanaka, Hiromasa

AU - Sasaki, Kouitsu

AU - Miyake, Yoshihiro

AU - Yoshizawa, Kazunari

AU - Nishibayashi, Yoshiaki

PY - 2012/12/1

Y1 - 2012/12/1

N2 - 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 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 Me 3Si groups as ancillary ligands has an important role as a key reactive intermediate, with the aid of density-functional-theory calculations.

AB - 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 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 Me 3Si groups as ancillary ligands has an important role as a key reactive intermediate, with the aid of density-functional-theory calculations.

UR - http://www.scopus.com/inward/record.url?scp=84871723308&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84871723308&partnerID=8YFLogxK

U2 - 10.1038/ncomms2264

DO - 10.1038/ncomms2264

M3 - Article

C2 - 23212383

AN - SCOPUS:84871723308

VL - 3

JO - Nature Communications

JF - Nature Communications

SN - 2041-1723

M1 - 1254

ER -