咪唑基二羧酸配合物的合成、结构与性质研究
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摘要
本论文以4,5-咪唑二甲酸和N,N’-1,3-咪唑二乙酸为有机配体,在水(溶剂)热条件下,与不同金属离子反应制备出了22个新的金属配合物,探讨了这些配合物的反应条件和网络结构所属的拓扑类型。通过单晶X-射线衍射仪对配合物的晶体结构进行了测定,并对某些配合物的热稳定性及荧光性质进行了研究。结果表明:在4,5-咪唑二甲酸(H_3IDC)配体与过渡金属离子构筑的10个配合物中,金属离子、配体H_3IDC、反应体系的pH值及辅助配体对该类配合物的结构均具有重要的影响,其中配合物7是一个具有一维孔道的金属-有机开放框架结构,并展示出强的蓝色荧光性能和良好的热稳定性,可以作为一种蓝色荧光材料的备选物;在主族金属离子与H_3IDC构筑的7个配合物中,配体展现出两种新的配位模式(μ4-η7和μ5-η7)并建构出三个具有新颖空间拓扑结构(PtS, 4~5.6~5, SrAl2)的三维配位聚合物;在N,N’-1,3-咪唑二乙酸构筑的5个配位聚合物中,配体均以内盐的形式存在,并表现出双单齿、四单齿桥联和双-双齿螯合等多种配位方式。
In this thesis, twenty-two coordination complexes have been synthesized by the hydrothermal (solvothermal) reactions of 4,5-imidazoledicarboxylic acid or N,N’-1,3,- imidazolediacetic acid with many metal salts. The study on synthetic conditions and topological analyses of the coordination polymers are carried out. These complexes structurally characterized by single crystal X-ray diffraction and the thermal stabilities and fluorescent properties of these complexes have been studied. The metal ion, organic ligand, pH value and co-ligands play interesting roles in the topological structures of ten complexes constructed by the transition metals and 4,5-imidazoledicarboxylic acid. Especially, the complex 7 has an Open-Frameworks with 1-D channels and exhibits a strong blue fluorescent emission in the solid state at room temperature, and it may be a good candidate polymer as blue–light emitting materials. In the seven complexes based on the main group metals, 4,5-imidazoledicarboxylic acid exhibit two kind novel coordination modes (μ4-η7 andμ5-η7) and construct three 3-D polymers with novel topology structures (PtS, 45.65,SrAl2); In the five coordination polymers on the basis of the N,N’-1,3,- imidazolediacetate acid, the ligand exists as zwitterionic and exhibits interesting bis-monodentat, tetradentate bridged and bis-bidentate chelate coordination modes.
In this thesis, twenty-two coordination complexes have been synthesized by the hydrothermal (solvothermal) reactions of 4,5-imidazoledicarboxylic acid or N,N’-1,3,- imidazolediacetic acid with many metal salts. The study on synthetic conditions and topological analyses of the coordination polymers are carried out. These complexes structurally characterized by single crystal X-ray diffraction and the thermal stabilities and fluorescent properties of these complexes have been studied. The metal ion, organic ligand, pH value and co-ligands play interesting roles in the topological structures of ten complexes constructed by the transition metals and 4,5-imidazoledicarboxylic acid. Especially, the complex 7 has an Open-Frameworks with 1-D channels and exhibits a strong blue fluorescent emission in the solid state at room temperature, and it may be a good candidate polymer as blue–light emitting materials. In the seven complexes based on the main group metals, 4,5-imidazoledicarboxylic acid exhibit two kind novel coordination modes (μ4-η7 andμ5-η7) and construct three 3-D polymers with novel topology structures (PtS, 45.65,SrAl2); In the five coordination polymers on the basis of the N,N’-1,3,- imidazolediacetate acid, the ligand exists as zwitterionic and exhibits interesting bis-monodentat, tetradentate bridged and bis-bidentate chelate coordination modes.
引文
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