菲（苊）醌亚胺铁、钛、锆、铪配合物的合成、表征及性能研究

发布时间：2018-06-16 20:25

本文选题：菲(苊)醌亚胺配体 + Fe配合物　；参考：《吉林大学》2017年硕士论文

【摘要】：近年来,非纯粹配体的概念被广泛使用,越来越多具有共轭结构和氧化还原性质的新型配体被合成。由于含N类亚胺配体与过渡金属结合后能生成多种结构稳定、催化性质优异的金属有机配合物,所以探究含N类配体在形成配合物时所发生的化学变化尤为重要。本论文设计并合成了以菲醌单亚胺及苊醌双亚胺为配体的Fe、Ti、Zr、Hf为中心金属的配合物。通过X-射线晶体结构测定、穆斯堡尔谱、固体磁性测试、核磁共振等表征手段对这些未被报道过的配合物进行了结构表征与磁性测试,同时也对这些配合物进行了理论计算研究,探索这类配体在反应过程中体现的氧化还原性质。本文第三章中,我们以芳基取代的菲醌单亚胺为配体,与金属Fe、Fe Cl2反应,得到了5种不同的Fe配合物。通过对这些配合物的结构表征,我们发现在配合物形成的过程中,中心金属与配体之间发生氧化还原反应,配体可以容纳来自于中心金属的电子,形成负一价和负二价的稳定状态。同时,我们通过磁性测试与理论计算相结合,研究了这类配合物的磁学性质。本文第四章中,我们以苊醌双亚胺和菲醌单亚胺为配体,通过其金属Mg的配合物与第四副族金属氯化物反应,得到了6种结构稳定的、配体为负二价形式存在的金属配合物。通过核磁共振与晶体结构表征,我们确定了配合物形成过程中,配体的确发生氧化还原变化。对于这类配体的过渡金属配合物的合成方法又有了新的拓展。
[Abstract]:In recent years, the concept of non-pure ligands has been widely used, and more new ligands with conjugated structure and redox properties have been synthesized. Since N-containing imide ligands can form various organometallic complexes with stable structure and excellent catalytic properties, it is particularly important to explore the chemical changes of N-containing ligands in the formation of transition metals. In this paper, the complexes of FetiTiZrHf with phenanthroline monoimide and acenaphthene quinone biimide as central metal have been designed and synthesized. The structures and magnetic properties of these unreported complexes were characterized by X-ray crystal structure determination, Mossbauer spectroscopy, solid state magnetic measurement and nuclear magnetic resonance. At the same time, the redox properties of these ligands in the reaction process were investigated by theoretical calculation. In the third chapter, five different Fe complexes were obtained by the reaction of phenanthroline monoimide with metal Fe (Fe) Cl _ 2 with aryl substituted phenanthroline monoimide as ligand. By characterizing the structures of these complexes, we find that the redox reaction between the central metal and the ligand occurs during the formation of the complexes, and the ligand can hold electrons from the central metal. A stable state of negative monovalent and negative bivalent. At the same time, we have studied the magnetic properties of the complexes by combining the magnetic tests with theoretical calculations. In the fourth chapter, using acenaphthene quinone biimide and phenanthraquinone monoimide as ligands, six metal complexes with negative bivalent form were obtained by the reaction of their metal mg complexes with the fourth sub-group metal chloride. It is confirmed by NMR and crystal structure that the redox changes do occur during the formation of the complexes. The synthesis of transition metal complexes of these ligands has been further expanded.
【学位授予单位】：吉林大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O641.4

【相似文献】