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Syntheses, structures, and immobilization of ruthenium(II) complexes with alkoxysilane groups functionalized N,N′-diamine and phosphine ligands
Journal of Coordination Chemistry ( IF 2.2 ) Pub Date : 2020-05-19
Jiao Ji, Li-Miao Shi, Fule Wu, Zhi-Feng Xin, Ai-Quan Jia, Qian-Feng Zhang

Treatment of [RuCl2(PPh3)3] with N-(β-aminoethyl)-γ-aminopropylmethylbimethoxysilane (L1) in tetrahydrofuran at room temperature gave a mononuclear ruthenium(II) complex [Ru(PPh3)2Cl2 (κ2-N,N-L1)] (1). Condensation of γ-aminopropyltriethoxysilane and potassium diphenylphosphine in the molar ratio of 1:1 in tetrahydrofuran afforded phosphine (PPh2)(CH2)3Si(OEt)3 (L2) with ethoxysilane groups. Reaction of [Ru(η6-p-cymene)Cl2]2 with L2 in refluxing tetrahydrofuran afforded a ruthenium(II) phosphine complex [Ru(η6-p-cymene)Cl2(κ-P-L2)] (2). Complexes 1 and 2 were systematically characterized by microanalyses, FT-IR, and NMR spectroscopies. Their structures have been unambiguously established by single-crystal X-ray diffraction. Immobilization of 1 and 2 on SBA-15 and characterization of these hybrid heterogeneous catalysts were studied by transmission electron microscopy (TEM), FT-IR, and low-pressure N2 adsorption/desorption measurements. Transfer hydrogenation of acetophenone was also briefly investigated with the heterogeneous catalysts.



中文翻译:

具有烷氧基硅烷基团的功能化N,N'-二胺和膦配体的钌(II)配合物的合成,结构和固定化

在室温下在四氢呋喃中用N-β-氨基乙基)-γ-氨基丙基甲基联甲氧基硅烷(L1)处理[RuCl 2(PPh 33 ]得到单核钌(II)络合物[Ru(PPh 32 Cl 2κ)2 - NN - L1)](1)。γ-氨基丙基三乙氧基硅烷和二苯基膦钾盐在四氢呋喃中以1:1的比例缩合得到膦(PPh 2)(CH 2具有乙氧基硅烷基团的3 Si(OEt)3L2)。的反应的[Ru(η 6 - p -cymene)氯2 ] 2L2在回流的四氢呋喃中,得到钌(II)膦络合物的[Ru(η 6 - p -cymene)氯2κ - P - L2)](2)。配合物12通过微量分析,傅立叶变换红外光谱(FT-IR)和核磁共振光谱(NMR)进行系统表征。它们的结构已通过单晶X射线衍射明确建立。通过透射电子显微镜(TEM),FT-IR和低压N 2吸附/脱附测量研究了12在SBA-15上的固定以及这些杂化多相催化剂的表征。还用非均相催化剂对苯乙酮的转移氢化进行了简要研究。

更新日期:2020-05-19
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