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含噻吩羧酸配體的金屬有機骨架材料的合成及性能研究

發(fā)布時間:2018-11-08 20:01
【摘要】:金屬有機骨架材料(MOFs)作為一種多孔材料在眾多領域中得到了廣泛應用,它的結(jié)構(gòu)具有多樣性,高度可調(diào)性和可裁剪性,使其無論是在學術界還是工業(yè)領域都引起了極大的關注。這不僅僅是因為他們的美學結(jié)構(gòu)特性,而且它們在很多領域展現(xiàn)出卓越的應用性能,尤其對催化領域的研究引起了人們注意。MOFs中存在均勻分布的活性位點,以及含有大的孔道,保證了每個活性位點的可接觸性,因此,MOFs是很好的異相催化劑。設計合成含有功能化的金屬有機骨架材料引起了人們的興趣,有機配體設計合成對修筑功能性金屬有機骨架材料扮演著至關重要的角色。設計含有功能位點的有機配體,為金屬有機骨架材料提供了杰出的應用價值。本文中,我們在金屬有機骨架材料中引入S或噻吩,利用噻吩線性配體合成的金屬有機骨架中裸露的S位點,用來選擇識別金屬離子,并且能夠與金屬離子形成配位鍵,進而能夠選擇吸附金屬離子。因此本文設計合成兩個含有噻吩的有機配體與稀土鹽合成了一系列的金屬有機骨架材料。對其合成方法、結(jié)構(gòu)、表征以及并應用該材料對金屬離子檢驗與吸附以及其它性質(zhì)進行了詳細的研究。第一章,闡述了近幾年來金屬有機骨架材料的在催化、熒光、吸附領域中的具體應用以及所取得的進展情況,并且介紹本文的選題意義。第二章,我們設計合成了含有噻吩官能團的有機配體,[2,3-b]并二噻吩基-2,6-二酸,用其分別于與稀土金屬離子通過溶劑法合成出四個配位聚合物{[Ln2L6DMF4]?1.5H2O}n(1)(Ln=Eu(Ⅲ)(1),Y(Ⅲ)(2),Dy(Ⅲ)(3),Yb(Ⅲ)(4)),該配位聚合物含有三角形的孔道,并對這四個配合物的結(jié)構(gòu)做了的研究,研究結(jié)果表明四個配合物為同構(gòu)型的,還詳細的研究和討論配合物1的對爆炸物硝基苯以及對Al3+的熒光識別性質(zhì)。第三章,我們同樣選用含有噻吩官能團的有機配體,[2,3-b]苯并二噻吩基-2,6-酸,利用該配體與稀土Er(Ⅲ)合成了金屬有機骨架材料,該配合物含有菱形的孔道及不飽和位點,用該配合物來催化硅腈化反應,因為該配合物孔道中含有裸露的S位點,應用該位點對金屬離子進行選擇吸附性質(zhì)研究。第四章,最后對文中所提到的五種金屬有機骨架材料的結(jié)構(gòu)特征,功能性質(zhì)進行歸納,為以后金屬有機骨架材料的發(fā)展應用提供了新的方向。最后,對MOFs的應用前景做了展望。
[Abstract]:As a porous material, (MOFs) has been widely used in many fields. It has aroused great concern in both academic and industrial fields. This is not only because of their aesthetic structural properties, but also because of their excellent application performance in many fields, especially in the field of catalysis. The existence of uniformly distributed active sites in MOFs. MOFs is a good heterogeneous catalyst because it contains large pore channels to ensure the accessibility of each active site. The design and synthesis of organometallic skeleton materials with functionalization has attracted much attention. The design and synthesis of organic ligands plays an important role in the construction of functional organometallic skeleton materials. The design of organic ligands with functional sites provides an excellent application value for organometallic skeleton materials. In this paper, we introduce S or thiophene into the organometallic skeleton, and use the exposed S site in the organometallic skeleton synthesized by the thiophene linear ligand to select and recognize metal ions and form coordination bonds with metal ions. In turn, it is possible to choose to adsorb metal ions. Therefore, two organic ligands containing thiophene and rare earth salts were designed to synthesize a series of metal organic skeleton materials. The synthesis method, structure, characterization and application of this material to metal ions were studied in detail. In the first chapter, the applications of organometallic skeleton materials in catalysis, fluorescence and adsorption fields and their progress in recent years are described, and the significance of this paper is introduced. In chapter 2, we have designed and synthesized organic ligands containing thiophene functional groups, [2o _ 3-b] and dithiophene -2o _ 6-dicarboxylic acid, Four coordination polymers {[Ln2L6DMF4]? 1.5H2O} n (1) (Ln=Eu (鈪,

本文編號:2319508

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