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Dalton Trans. 2018 Dec 21;47(47):17004-17010. doi: 10.1039/c8dt04168g. Epub 2018 Nov 21.

Selective hydrosiloxane synthesis via dehydrogenative coupling of silanols with hydrosilanes catalysed by Fe complexes bearing a tetradentate PNNP ligand.

Author information

1
Interdisciplinary Research Centre for Catalytic Chemistry (IRC3), National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan. yumiko-nakajima@aist.go.jp and Faculty of Pure and Applied Sciences, University of Tsukuba, 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, Japan.
2
Interdisciplinary Research Centre for Catalytic Chemistry (IRC3), National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan. yumiko-nakajima@aist.go.jp.

Abstract

A well-defined iron complex system was established using PNNP-R (R = Ph and Cy) as a strong σ-donating ligand with a rigid meridional tetradentate structure. Reactive Fe(0) complexes [{Fe(PNNP-R)}2(μ-N2)] were synthesized by a reaction of the corresponding iron dihalide with NaBEt3H and structurally characterized. The reaction proceeded via the iron dihydride intermediate [Fe(H)2(PNNP-R)], which underwent H2 reductive elimination, supporting the hemilabile behavior of PNNP-R. [{Fe(PNNP-R)}2(μ-N2)] catalyzed the dehydrogenative coupling of silanols with silanes to selectively form various hydrosiloxanes, which are important building blocks for the synthesis of a range of siloxane compounds. This system exhibited higher catalytic efficiency than the previously reported precious-metal-catalyzed systems.

PMID:
30460962
DOI:
10.1039/c8dt04168g

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