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氨基酸衍生物席夫碱稀土配合物合成及催化性能研究

Study on the Synthesis and Their Catalytic Properties of Rare Earth Schiff-base Complexes with Amino Acid Derivatives

【作者】 张志攀

【导师】 景欢旺;

【作者基本信息】 兰州大学 , 物理化学, 2008, 硕士

【摘要】 稀土金属离子由于d和f轨道的存在而具有4到12的各种配位数,容易与多种配体形成结构各异的配合物。其中稀土元素与氨基酸席夫碱配体形成的配合物具有多样的稳定结构和良好的生物活性、光学特性,并在催化及功能材料等领域都有广泛的应用前景。氨基酸是人体蛋白质等与生命有关的基本物质,氨基酸及其衍生物具有较低的毒性和耐药性;同时,它又是天然的廉价手性源,可应用于多种有机反应的不对称催化。环状碳酸酯是由二氧化碳化学固定得到的,作为中间体和极性有机溶剂具有广泛应用价值,可应用于有机合成、气体分离、电池介电质及金属萃取等领域。本研究小组近年来致力于研究环状碳酸酯的手性和非手性合成,并建立了多种手性和非手性催化体系。本文由母配体二-(3,5-二特丁基水杨醛缩胺乙基)氨(H2L)}和不同手性氨基酸衍生物反应合成了未见文献报道的六种手性席夫碱配体(H2L1~H2L5,H3L6),再与LaCl3·7H2O配位合成相应的稀土镧配合物;用核磁共振光谱、红外光谱、质谱和元素分析对配体及其配合物进行了表征。最后考察了稀土催化剂对环氧化合物和二氧化碳的偶联反应的催化性能,其结果为下一步工作指出明确的方向,从而进一步了解物质性质与其结构的密切联系。

【Abstract】 Rare earth metal ions have 4 to 12 coordination number for the existence of d and f orbits,the complexes are easily synthesized from coordination of rare earth metal and multiplicate ligands.Among them,the lanthanide complexes with amino acid Schiff bases,which have various stable structures and the vital bioactivity and excellent luminescence,were widely used in the fields of catalysis and material etc.Amino acids are the basic unit of composition of the materials of life,amino acids and their derivatives with low toxicity and resistance are widely applied to chiral catalysis of various oganic reactions as natural and cheap chiral resource.Cyclic carbonates attained by chemical fixation of CO2 are applied to the fields of oganic synthesis,gas separation,battery electromedium,metal extraction etc as chemical intermediate and polar organic solvent.In recent years,our group has been studying on symmetric and asymmetric synthesis of cyclic carbonates and the establishment of a variety of chiral and achiral catalytic systems.In my paper,eight new chiral schiff base ligands(H2L1~H2L5,H3L6)were synthesized by the reaction of the mother ligand[(2-OH-3,5-di-t-Bu-C6H2)CH=NCH2CH2]2NH(H2L)with the chiral amino acid derivatives,their lanthanide complexes prepared from the coordination of the ligands and Lanthanum compound(LaCl3·7H2O);The ligands and their lanthanide complexes were characterized by nuclear magnetic resonance, mass spectrometry、infrared spectroscopy and elemental analysis.Finally the catalytic properties of the complexes were studied on the coupling reaction of the epoxides and CO2,and the results clearly pointed out what the next step of our work is.It made us further understanding affinity of material properties and structure.

  • 【网络出版投稿人】 兰州大学
  • 【网络出版年期】2009年 01期
  • 【分类号】O627.3
  • 【被引频次】1
  • 【下载频次】541
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