吡嗪四唑/羧酸类配体配合物的结构调控与性能研究
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摘要
本论文设计合成了系列吡嗪单四唑、吡嗪双四唑及吡嗪羧酸类配体,并利用这些配体与金属离子配位构筑了45个配合物,解析了其晶体结构。对配体及相应的ZnⅡ、CdⅡ、HgⅡ配合物的荧光性能,部分配合物的磁性、气体吸附等性能以及部分手性配合物的固体圆二色光谱进行了系统研究。结果表明配体的配位模式、取代基团和配位倾向；过渡金属离子的半径、配位能力以及反应条件等在配合物构筑过程中都具有不同程度的影响。研究的具体内容如下：
1.配体2-(5-1H-四唑基)吡嗪与ZnⅡ、CdⅡ、HgⅡ离子反应得到6个配合物,解析了晶体结构。对部分配合物的荧光性能进行了研究。讨论了金属离子、反应条件以及分子间/分子内弱相互作用对配合物结构的影响。该配体及ZnⅡ、CdⅡ配合物具有较好的荧光性能,而HgⅡ配合物则产生荧光猝灭现象。
2.设计合成了6个2,3-二取代-5,6-二(5-1H-四唑基)吡嗪类配体,其中2,3-位取代基团从烷基到芳环基团、毗啶基团再到具有单一手性的桥环取代基团进行了系统地改变。利用该系列配体与金属离子在水热或常规条件下反应合成了23个配合物,解析了晶体结构。对配体及相应d10金属配合物的固态荧光性能进行了研究,并对部分配合物的磁性、气体吸附性能和固体圆二色光谱进行了初步探索。讨论了不同的取代基团对配体的修饰作用以及反应条件等其它因素对配合物的形成和结构所产生的影响。研究结果表明,相对于单四唑配体,此类双四唑配体在构筑配合物过程中呈现出更加复杂新颖的配位模式,不同取代基团的引入也会导致配合物结构的明显变化。
3.采用具有与第二部分介绍的双四唑配体类似的骨架结构,合成表征了具有不同取代基团的4个5,6-二取代-2,3-吡嗪羧酸类配体,这些配体与过渡金属离子反应制得16个配合物,解析了晶体结构。对配体及ZnⅡ、CdⅡ配合物进行了固态荧光性能测试,并对部分配合物的磁性进行了研究。讨论了配体结构特点和不同反应条件等影响配合物构成的因素。结果表明,该系列配体中吡嗪环和羧基的同时存在使其可以采用单齿或多齿等多种模式与金属离子配位,但与上述双四唑配体相比具有较少的配位模式。属性不符
In this dissertation, a series of structurally related pyrazine-based ligands containing tetrazole, bis-tetrazole or carboxylate coordination groups have been designed and synthesized, and forty-five complexes of these ligands with various structures have been prepared and characterized. Luminescent, gas adsorption, magnetic and the solid-state circular dichroism (CD) properties of selected complexes have been studied. The results show that coordination modes, substituting groups and coordination affinity of ligands, the binding nature of metal ions, and reaction conditions have significant influences on the formation and related properties of complexes. The main results have been summarized as follows:
1.2-(1H-tetrazol-5-yl)pyrazine ligand (HL) and its six ZnⅡ, CdⅡ, HgⅡcomplexes have been synthesized and characterized. The luminescent properties of some complexes have been investigated. The influences of the nature of metal ions and reaction conditions, as well as the intramolecular/intermolecular weak interactions in the formation of such complexes have been investigated.
2. A series of structurally related 2,3-substituded-5,6-di(1H-tetrazol-5-yl)-pyrazine ligands bearing different terminal groups, such as alkyl, aryl, pyridine have been designed and prepared, and twenty-three coordination complexes with these ligands have been synthesized and characterized. The luminescent properties of these ligands and some of their complexes in solid state at room temperature, magnetic properties and the solid-state circular dichroism(CD) properties of some complexes have been also studied and discussed. The effects of substituting groups of these ligands and synthesis conditions, as well as other factors on the formation of their coordination complexes have also been discussed. The results show that the variety of substituting groups of the bis(tetrazole)ligands can cause dramatic changes in the formation of their complexes.
3. Four pyrazine-2,3-dicarboxylate ligands with different substituting groups which have similar skeleton to those of pyrazine-based ligands mentioned above and their sixteen metal complexes were synthesized and characterized. The luminescent properties of ZnⅡ, CdⅡcomplexes and the corresponding ligands, magnetic properties of some complexes have also been investigated. The effects of substituting groups of ligands and reaction condinations on the structures and properties of the complexes have been discussed.
1.配体2-(5-1H-四唑基)吡嗪与ZnⅡ、CdⅡ、HgⅡ离子反应得到6个配合物,解析了晶体结构。对部分配合物的荧光性能进行了研究。讨论了金属离子、反应条件以及分子间/分子内弱相互作用对配合物结构的影响。该配体及ZnⅡ、CdⅡ配合物具有较好的荧光性能,而HgⅡ配合物则产生荧光猝灭现象。
2.设计合成了6个2,3-二取代-5,6-二(5-1H-四唑基)吡嗪类配体,其中2,3-位取代基团从烷基到芳环基团、毗啶基团再到具有单一手性的桥环取代基团进行了系统地改变。利用该系列配体与金属离子在水热或常规条件下反应合成了23个配合物,解析了晶体结构。对配体及相应d10金属配合物的固态荧光性能进行了研究,并对部分配合物的磁性、气体吸附性能和固体圆二色光谱进行了初步探索。讨论了不同的取代基团对配体的修饰作用以及反应条件等其它因素对配合物的形成和结构所产生的影响。研究结果表明,相对于单四唑配体,此类双四唑配体在构筑配合物过程中呈现出更加复杂新颖的配位模式,不同取代基团的引入也会导致配合物结构的明显变化。
3.采用具有与第二部分介绍的双四唑配体类似的骨架结构,合成表征了具有不同取代基团的4个5,6-二取代-2,3-吡嗪羧酸类配体,这些配体与过渡金属离子反应制得16个配合物,解析了晶体结构。对配体及ZnⅡ、CdⅡ配合物进行了固态荧光性能测试,并对部分配合物的磁性进行了研究。讨论了配体结构特点和不同反应条件等影响配合物构成的因素。结果表明,该系列配体中吡嗪环和羧基的同时存在使其可以采用单齿或多齿等多种模式与金属离子配位,但与上述双四唑配体相比具有较少的配位模式。属性不符
In this dissertation, a series of structurally related pyrazine-based ligands containing tetrazole, bis-tetrazole or carboxylate coordination groups have been designed and synthesized, and forty-five complexes of these ligands with various structures have been prepared and characterized. Luminescent, gas adsorption, magnetic and the solid-state circular dichroism (CD) properties of selected complexes have been studied. The results show that coordination modes, substituting groups and coordination affinity of ligands, the binding nature of metal ions, and reaction conditions have significant influences on the formation and related properties of complexes. The main results have been summarized as follows:
1.2-(1H-tetrazol-5-yl)pyrazine ligand (HL) and its six ZnⅡ, CdⅡ, HgⅡcomplexes have been synthesized and characterized. The luminescent properties of some complexes have been investigated. The influences of the nature of metal ions and reaction conditions, as well as the intramolecular/intermolecular weak interactions in the formation of such complexes have been investigated.
2. A series of structurally related 2,3-substituded-5,6-di(1H-tetrazol-5-yl)-pyrazine ligands bearing different terminal groups, such as alkyl, aryl, pyridine have been designed and prepared, and twenty-three coordination complexes with these ligands have been synthesized and characterized. The luminescent properties of these ligands and some of their complexes in solid state at room temperature, magnetic properties and the solid-state circular dichroism(CD) properties of some complexes have been also studied and discussed. The effects of substituting groups of these ligands and synthesis conditions, as well as other factors on the formation of their coordination complexes have also been discussed. The results show that the variety of substituting groups of the bis(tetrazole)ligands can cause dramatic changes in the formation of their complexes.
3. Four pyrazine-2,3-dicarboxylate ligands with different substituting groups which have similar skeleton to those of pyrazine-based ligands mentioned above and their sixteen metal complexes were synthesized and characterized. The luminescent properties of ZnⅡ, CdⅡcomplexes and the corresponding ligands, magnetic properties of some complexes have also been investigated. The effects of substituting groups of ligands and reaction condinations on the structures and properties of the complexes have been discussed.
引文
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