摘要
酰胺和喹啉类化合物是两类重要的配体,它们对金属离子有着较强的配位能力和较高的选择性,使其在分析化学、生物化学、功能材料等领域有着广阔的应用前景。本论文报道了一系列柔性酰胺型配体及其稀土超分子配合物的合成、结构表征和荧光性质研究,并研究了不同配体对配合物结构和性质的影响。同时合成了一系列基于喹啉类的有机配体,并深入研究了其对金属离子的荧光选择性。论文共分为六部分：
一、简单综述了稀土发光超分子配合物的离子识别作用及自组装作用；通过阐述不同的荧光机理简单介绍了近年来有机小分子阳离子荧光探针的研究进展。
二、以水杨酰苄胺为末端基,二甘醇和三甘醇为中心骨架,合成了两个结构类似的酰胺类配体,得到了稀土配位聚合物,并探讨了中心骨架的柔性对其结构和荧光性质的调控。
三、设计合成了一系列柔性链酰胺类配体及其稀土硝酸盐配合物,并探讨了中心骨架和末端基对其结构和荧光性质的影响。
四、设计合成了一个基于喹啉类的对锌离子有很好选择性的荧光探针,其对锌离子有好的选择性、强的荧光增强、较大的结合常数,并且可以对锌离子进行比率测定。
五、通过氯乙酰氯将8-羟基喹啉和8-氨基喹啉连接在一起,合成了一个对镉离子有很好选择性的荧光探针。并且它可用不同的荧光增强机理来区分镉离子和锌离子。
六、设计合成了一系列基于喹啉类对铝离子有选择性的探针,并通过结构的改变,来研究其对金属离子荧光选择性的影响。
Salicylamide and Quinoline ligands are two classes of important compounds and they can be widely used in analytical chemistry, biochemistry, and functional material due to their high selectivity and coordination capability to the metal ions. In this dissertation, a series of flexible salicylamide ligands and their rare earth complexes have been synthesized and characterized, and their fluorescent properties have also been investigated in detail. In addition, a few chemical fluorescence sensors based on quinoline platforms have been designed and synthesized, and their selectivity of metal ions have been studied. This dissertation is divided into six parts:
1. A brief review of lanthanide complexes based luminescent switches and sensors where the emission and their self-assemblieis changed by the presence of cations and anions, was concisely given. The design principle and mechanism of chemical sensors and a few examples for cation selectivity were introduced.
2. Two new flexible exo-bidentate ligands incorporating different chain length of the backbone bearing two arms of salicylamide moieties, were designed and synthesized. These two structurally related ligands as building blocks were used for constructing diverse lanthanide polymers with luminescence properties.
3. A series of flexible salicylamide ligands and their lanthanide complexes were prepared and charactered. Their supramolecular structures and solid luminescence properties, which were influenced by the backbone and terminal amide group, were discussed in detail.
4. A fluorescent Zn2+sensor based on the8-aminoquinoline platform has been synthesized. This sensor displays high selectivity, sensitive fluorescence enhancement, strong binding ability and ratiometric response to Zn2+.
5. A fluorescent sensor based on8-aminoquinoline and8-hydroxyquinoline platforms has been synthesized, which displays high selectivity and sensitive fluorescence enhancement to Cd2+in ethanol. Moreover, this sensor can distinguish Cd2+from Zn2+via two different sensing mechanisms.
6. The design and synthesis of a series of fluorescent sensors for Al3+based on Schiff base have been presented. The relationship between the structures of these ligands and their complexes and the selectivity was studied.
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