配位取向不同的噁二唑类及对称纳米级建筑块的自组装化学及性质研究
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摘要
以自组装战略为基础的有机-无机配位聚合物和超分子配合物化学是目前国际化学界最活跃、最前沿的研究领域之一,亦是合成新型有机-无机复合功能材料的最有效的途径之一。本文合成了一系列1, 3, 4-oxadiazole杂环桥联的弯折型刚性及半刚性配体、4-amino-1, 2, 4-triazole杂环桥联的弯折型刚性配体,并研究了它们的配位反应化学。共合成了四十三个未见文献报道的配位作用及氢键驱动的超分子化合物,通过红外、元素分析、单晶衍射及粉末衍射等方法表征了它们的结构,并对它们的荧光性质、可逆离子交换、热稳定性进行了研究。
I.设计合成了个1, 3, 4-oxadiazole桥联的双臂半刚性的不对称有机配体并研究了它们与Cu(II)、Cu(I)、Co(II)、Ni(II)、Ag(I)、Zn(II)、Cd(II)和Hg(II)等过渡金属的配位化学,合成了三十九个新型配位化合物,表征和分析了所得新化合物的晶体结构。通过对化合物合成条件及反应规律的总结,探讨取代基的位置、配体的配位构型、反应溶剂体系、反应物浓度、反应温度、平衡阴离子对合成的配位化合物结构及化学性质的影响,着重探讨了阴离子可逆交换控制的固态荧光性质的调谐变化。
II.设计合成了部分含异端基的1, 3, 4-噁二唑杂环桥联的刚性、半刚性有机配体,得到了四个新型配位化合物,表征和分析了它们的晶体结构。讨论了在不同取代基及取代基位置下,配体配位能力对构筑新颖化合物影响。并讨论了它们的固态荧光性质。
III.设计合成了六个4-amino-1, 2, 4-triazole杂环桥联的对称双臂纳米级刚性有机配体,部分表征了它们的结构,初步研究了它们的溶剂热反应条件以及固态条件下新化合物的荧光性质。
我们设计合成了一系列1, 3, 4-oxadiazole、4-amino-1, 2, 4-triazole杂环桥联的弯折型配体,,研究结果证明这些配体是构建结构新颖的超分子组装体的良好前体,它们与d-block金属离子之间的自组装反应能够得到结构新颖,物化性质优良的超分子组装体,为设计合成可调谐发光材料及功能材料奠定了实验基础。
The chemistry of organic-inorganic coordination polymers and supramolecular complexes has recently become an active area of increasing interest internationally. Self-assembly of organic ligands and inorganic metal ions is one of the most efficient and widely used approaches for the construction of organic-inorganic composite materials. Recently, remarkable progress has been made in the area of molecular inorganic-organic hybrid compounds. The synthesis and characterization of infinite one-, two-, and three-dimensional networks have been an area of rapid growth. In this thesis, a series of bent ligands bridged by the 1, 3, 4-oxadiazole, 4-amino-1, 2, 4-triazole, respectively, were synthesized. The coordination chemistry based on these new ligands and metal ions was investigated. Totally 44 new coordination compounds were prepared and fully characterized by IR, elemental analysis, X-ray single-crystal diffraction and powdered X-ray diffraction. The luminescent properties, reversible ion-exchange, and thermal stability were investigated.
1. The coordination chemistry based on two-armed unsymmetrical 1, 3, 4-oxadiazole bridging organic semi-rigid ligands and inorganic Cu(II)、Cu(I)、Co(II)、Ni(II)、Ag(I)、Zn(II)、Cd(II) and Hg(II) transition metal salts has been investigated. 44 new supramolecular compounds were synthesized based on them. The results indicate that the bend angle between the two terminal N-donors of the ligands, reactive solvent system,reactants ratio,reactive temperature, the counter-anions and the coordination group have great influence on the final structure and the properties of the product. Their luminescent properties which were influenced by the reversible ion-exchange were investigated in the solid state.
2. Four new coordination polymers based on unsymmetrical 1, 3, 4-oxadiazole bridging organic semi-rigid ligands with different terminal groups were designed and synthesized. Their single crystal structures were characterized and investigated,also the influence of coordinative ability in determining the structure of the compounds was discussed. Their luminescent properties were investigated in the solid state.
3. Six new two-armed symmetrical 4-amino-1, 2, 4-triazole bridging organic nano-scale rigid ligands were designed,synthesized and characterized. Their solvent thermal reactive conditions and luminescent properties were investigated primarily.
We designed and synthesized a series of rigid and semi-rigid bent ligands bridged by 1, 3, 4-oxadiazole, 4-amino-1, 2, 4-triazole, and this study demonstrated that the use of bent ligands bridged by 1, 3, 4-oxadiazole, 4-amino-1, 2, 4-triazole unsymmetrical or symmetrical ligands as precursors to bind transition metals, is in fact an efficient approach for syntheses of novel supramolecular systems with interesting chemical and physical properties.
I.设计合成了个1, 3, 4-oxadiazole桥联的双臂半刚性的不对称有机配体并研究了它们与Cu(II)、Cu(I)、Co(II)、Ni(II)、Ag(I)、Zn(II)、Cd(II)和Hg(II)等过渡金属的配位化学,合成了三十九个新型配位化合物,表征和分析了所得新化合物的晶体结构。通过对化合物合成条件及反应规律的总结,探讨取代基的位置、配体的配位构型、反应溶剂体系、反应物浓度、反应温度、平衡阴离子对合成的配位化合物结构及化学性质的影响,着重探讨了阴离子可逆交换控制的固态荧光性质的调谐变化。
II.设计合成了部分含异端基的1, 3, 4-噁二唑杂环桥联的刚性、半刚性有机配体,得到了四个新型配位化合物,表征和分析了它们的晶体结构。讨论了在不同取代基及取代基位置下,配体配位能力对构筑新颖化合物影响。并讨论了它们的固态荧光性质。
III.设计合成了六个4-amino-1, 2, 4-triazole杂环桥联的对称双臂纳米级刚性有机配体,部分表征了它们的结构,初步研究了它们的溶剂热反应条件以及固态条件下新化合物的荧光性质。
我们设计合成了一系列1, 3, 4-oxadiazole、4-amino-1, 2, 4-triazole杂环桥联的弯折型配体,,研究结果证明这些配体是构建结构新颖的超分子组装体的良好前体,它们与d-block金属离子之间的自组装反应能够得到结构新颖,物化性质优良的超分子组装体,为设计合成可调谐发光材料及功能材料奠定了实验基础。
The chemistry of organic-inorganic coordination polymers and supramolecular complexes has recently become an active area of increasing interest internationally. Self-assembly of organic ligands and inorganic metal ions is one of the most efficient and widely used approaches for the construction of organic-inorganic composite materials. Recently, remarkable progress has been made in the area of molecular inorganic-organic hybrid compounds. The synthesis and characterization of infinite one-, two-, and three-dimensional networks have been an area of rapid growth. In this thesis, a series of bent ligands bridged by the 1, 3, 4-oxadiazole, 4-amino-1, 2, 4-triazole, respectively, were synthesized. The coordination chemistry based on these new ligands and metal ions was investigated. Totally 44 new coordination compounds were prepared and fully characterized by IR, elemental analysis, X-ray single-crystal diffraction and powdered X-ray diffraction. The luminescent properties, reversible ion-exchange, and thermal stability were investigated.
1. The coordination chemistry based on two-armed unsymmetrical 1, 3, 4-oxadiazole bridging organic semi-rigid ligands and inorganic Cu(II)、Cu(I)、Co(II)、Ni(II)、Ag(I)、Zn(II)、Cd(II) and Hg(II) transition metal salts has been investigated. 44 new supramolecular compounds were synthesized based on them. The results indicate that the bend angle between the two terminal N-donors of the ligands, reactive solvent system,reactants ratio,reactive temperature, the counter-anions and the coordination group have great influence on the final structure and the properties of the product. Their luminescent properties which were influenced by the reversible ion-exchange were investigated in the solid state.
2. Four new coordination polymers based on unsymmetrical 1, 3, 4-oxadiazole bridging organic semi-rigid ligands with different terminal groups were designed and synthesized. Their single crystal structures were characterized and investigated,also the influence of coordinative ability in determining the structure of the compounds was discussed. Their luminescent properties were investigated in the solid state.
3. Six new two-armed symmetrical 4-amino-1, 2, 4-triazole bridging organic nano-scale rigid ligands were designed,synthesized and characterized. Their solvent thermal reactive conditions and luminescent properties were investigated primarily.
We designed and synthesized a series of rigid and semi-rigid bent ligands bridged by 1, 3, 4-oxadiazole, 4-amino-1, 2, 4-triazole, and this study demonstrated that the use of bent ligands bridged by 1, 3, 4-oxadiazole, 4-amino-1, 2, 4-triazole unsymmetrical or symmetrical ligands as precursors to bind transition metals, is in fact an efficient approach for syntheses of novel supramolecular systems with interesting chemical and physical properties.
引文
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