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Updated: Oct 13, 2025
Imine Metathesis by Silica-Supported Catalysts Using the Methodology of Surface Organometallic Chemistry
Published on: October 18, 2019
Synthesis of silyl iron dinitrogen complexes for activation of dihydrogen and catalytic silylation of dinitrogen
Guoliang Chang1, Peng Zhang1, Wenjing Yang1
1School of Chemistry and Chemical Engineering, Key Laboratory of Special Functional Aggregated Materials, Ministry of Education, Shandong University, Shanda Nanlu 27, 250100 Jinan, People's Republic of China. xli63@sdu.edu.cn.
Abstract:
Three novel iron dinitrogen hydrides, [FeH(iPr-PSiMeP)(N2)(PMe3)] (1), [FeH(iPr-PSiPhP)(N2)(PMe3)] (2), and [FeH(iPr-PSiPh)(N2)(PMe3)] (3), supported by a silyl ligand are synthesized for the first time by changing the electronic effect and steric hindrance of the ligands through the reaction of ligands L1-L3 with Fe(PMe3)4 in a nitrogen atmosphere. The ligands containing an electron-donating group with large steric hindrance on the phosphorus atom are beneficial for the formation of dinitrogen complexes. A penta-coordinate iron hydride [FeH(iPr-PSiPh)(PMe3)2] (4) was formed through the reaction of ligand L3 with Fe(PMe3)4 in an argon atmosphere under the same conditions. The reactions between complexes 1-3 with an atmospheric pressure of dihydrogen gas resulted in Fe(II) dihydrides, [(iPr-PSiMe(μ-H)P)Fe(H)2(PMe3)] (5), [(iPr-PSiPh(μ-H)P)Fe(H)2(PMe3)] (6) and [(iPr-PSiPh(μ-H))Fe(H)2(PMe3)2] (7), with an η2-(Si-H) coordination. The isolation of dihydrides 5-7 demonstrates the ability of the dinitrogen complexes 1-3 to realize the activation of dihydrogen under ambient temperature and pressure. The molecular structures of complexes 1-7 were elucidated by single crystal X-ray diffraction analysis. The iron dinitrogen hydrides 1-3 are effective catalysts for the silylation of dinitrogen under ambient conditions and among them 3 is the best catalyst.
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