基于羧酸、嘧啶为端基的有机配体的组装化学及其微纳尺度复合材料的合成和性质研究

发布时间：2017-12-27 12:26

  本文关键词：基于羧酸、嘧啶为端基的有机配体的组装化学及其微纳尺度复合材料的合成和性质研究　出处：《山东师范大学》2016年硕士论文　论文类型：学位论文

  更多相关文章： 醚类桥连羧酸配体 咔唑桥连配体 芴桥连配体 纳米复合材料

【摘要】：作为一种多孔材料,金属-有机框架化合物在吸附、分离、传感和催化等领域有着巨大的应用潜力。本文中合成了一系列以羧酸为配位端基的开链冠醚桥连配体、咔唑桥连配体和以嘧啶为端基芴桥连的有机配体。研究了它们与过渡金属、主族金属的组装化学,得到了16例结构新颖的配位化合物,利用X-射线单晶衍射表征了它们的结构,对部分化合物的物理化学性质进行了探究。一、合成了以羧酸为配位端基的开链冠醚桥联柔性配体L1-L4,研究了其与过渡金属的自组装化学,得到5例未见报道的配位化合物,通过X-射线单晶衍射表征了它们的结构。发现一例Cu(II)为金属中心的离散型分子笼。二、合成了以羧酸为配位端基的咔唑桥联的刚性配体L5-L8,研究了它们与主族金属、过渡金属(M=Mg(II),Cd(II),Ni(II))的自组装化学,得到4例新的配位化合物,通过X-射线单晶衍射表征了它们的结构。其中一例三维Cd(II)-MOF可在单晶状态下吸附碘分子。三、通过对合成条件的调控研究得到三种大小形貌比较均匀的微米尺度的Cd(II)-MOF,利用五羰基铁气相氧化沉积的方法得到无定形Fe2O3@Cd-MOF、Fe3O4@Cd-MOF两种铁基纳米复合材料,探究了其对催化罗丹明B降解反应的催化性能。通过一锅法组装合成Cd S量子点@Cd-MOF复合材料,简单研究了其对光解水产氢实验的催化性能。四、合成了一系列以嘧啶为配位端基的芴桥连的有机配体L9-L13,与过渡金属通过自组装得到7例新的配位化合物,通过X-射线单晶衍射表征了它们的结构。通过改变配体取代基、阴离子等条件可实现对化合物结构的调控。
[Abstract]:As a porous material, metal - organic frame compounds have great potential for application in the fields of adsorption, separation, sensing and catalysis. In this paper, a series of ligands of open chain crown ether bridging ligands, carbazole bridging ligands and pyrimidine as the terminal fluorene bridge have been synthesized. The assembly chemistry of them with transition metals and host metals has been studied. 16 novel coordination compounds have been obtained. Their structures have been characterized by X- ray single crystal diffraction, and the physicochemical properties of some compounds have been explored. First, we synthesized the open chain crown ether bridged flexible ligand L1-L4 with carboxylic acid as the coordination end group. We studied its self assembly chemistry with transition metal, and obtained 5 unreported coordination compounds. Their structures were characterized by X- ray single crystal diffraction. A discrete molecular cage with Cu (II) as the metal center was found. Two, we synthesized the rigid ligand L5-L8 with carbazole bridged with carboxylic acid as the coordination end group. We studied their self-assembly chemistry with main group metals, transition metals (M=Mg (II), Cd (II), Ni (II)), and obtained 4 new coordination compounds. Their structures were characterized by X- ray single crystal diffraction. One of the three dimensional Cd (II) -MOF can adsorb iodine molecules in the state of a single crystal. Three, through the research on the regulation of synthesis conditions for uniform micron scale Cd three size morphology (II) -MOF, using the method of gas phase oxidation of iron pentacarbonyl deposited by amorphous Fe2O3@Cd-MOF, Fe3O4@Cd-MOF two kinds of Fe based nano composite material, explores its catalytic performance for the catalytic degradation of Luo Danming B. Cd S quantum dot @Cd-MOF composite was synthesized by one pot method, and its catalytic performance on the photodissociation of aquatic hydrogen was studied. Four, we synthesized a series of organic ligands L9-L13 with pyrimidine as the coordination terminal group, and obtained 7 new coordination compounds by self-assembly with transition metals. Their structures were characterized by X- ray single crystal diffraction. The structure of the compound can be regulated by changing the ligand substituents and anions.
【学位授予单位】：山东师范大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O641.4
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本文编号：1341717