基于含N杂环双羧酸配体构筑的配位聚合物的合成、结构及性质研究
发布时间：2019-05-17 15:48
【摘要】：配位聚合物(coordination polymers,CPs),也称金属有机骨架(Metal organic frameworks,MOFs),作为化学和材料科学中最受关注的研究领域之一,近年来展现出非常迅速的发展趋势,并成为多孔材料家族中一个重要的组成部分。CPs不仅具有丰富的拓扑结构,而且在许多领域具有潜在的应用价值,例如气体吸附和分离、催化、发光、感测和质子传导等。它们的结晶特性、高孔隙率、均匀分布的孔径、大的表面积、可调控的孔表面特性以及潜在的工业规模的可扩展性使得这类材料有着进一步研究的潜能。在诸多配位聚合物的类型中,以稀土离子作为金属中心的一类受到人们广泛的关注。由于稀土离子通常采用八配位或者十二配位的配位模式,并且具有特殊的发光特性,使其构筑的配位聚合物具有多样的结构和优良的光学特性。此外,在有机配体中引入杂原子如N原子,大大提高了新颖结构的配位聚合物生成的可能。本论文选用含N双羧酸配体作为有机配体,金属钪以及铕、铽、钆、铒等镧系金属作为金属中心,在水热及溶剂热的条件下,合成出六个配位聚合物,对这六个配位聚合物的发光、催化以及吸附性能进行了研究。主要工作内容如下:1、分别以2,5-吡啶二羧酸(2,5-pyridinedicarboxylic acid,H_2L~1)、2,3-吡嗪二羧酸(2,3-pyrazinedicarboxylic acid,H_2L~2)为有机配体,金属钪为金属中心,合成了两个配位聚合物[Sc_2L_2~1(HL~1)_2(H_2O)_2]·H_2O(1)和ScL~2(HL~2)(DMF)(2)。化合物1为2D层状结构,化合物2为1D链状结构。化合物1表现出良好的荧光性能和染料吸附性能,此外还有良好的催化性能。化合物2表现出良好的催化性能和荧光性能。(见第二章)2、以镧系元素铕、铽、钆、铒为金属源,分别以2,5-吡嗪二羧酸(2,5-pyrazinedicarboxylic acid,H_2L~3)、2,5-吡啶二羧酸(2,5-pyridinedicarboxylic acid,H_2L~1)为有机配体,合成了四个配位聚合物Na[Eu(C_2O_4)_2(H_2O)]·2H_2O(3)、Na[Tb(C_2O_4)_2(H_2O)]·2H_2O(4)、Na[Gd(C_2O_4)_2(H_2O)]·2H_2O(5)和Er_4L_4~1(DMF)(OH)_4(H_2O)(6)。化合物3-5是同构的,合成过程中有机溶剂发生了原位反应,形成了2D层状结构。化合物6是具有四核簇的3D结构。我们对化合物3-5进行了荧光测试,它们表现出相应镧系金属离子的特征发射光谱,此外还对化合物3进行了染料吸附测试,发现其有一定的染料吸附能力。对于化合物6,我们进行了近红外区的荧光测试,其表现出金属中心铒的特征峰,并且化合物6还有着良好的染料吸附性能。
[Abstract]:Coordination polymer (coordination polymers,CPs), also known as metal organic skeleton (Metal organic frameworks,MOFs), as one of the most concerned research fields in chemistry and material science, has shown a very rapid development trend in recent years. CPs not only has rich topological structure, but also has potential application value in many fields, such as gas adsorption and separation, catalysis, luminous, sensing and proton conduction. Their crystallization characteristics, high porosity, uniform pore size, large surface area, adjustable pore surface characteristics and potential industrial scale scalability make this kind of materials have the potential for further research. Among many types of coordination polymers, rare earth ions as metal centers have attracted extensive attention. Because rare earth ions usually adopt eight or twelve coordination modes and have special luminous properties, the coordination polymers constructed by rare earth ions have various structures and excellent optical properties. In addition, the introduction of hetero atoms such as N atoms into organic ligands greatly improves the possibility of the formation of coordination polymers with novel structures. In this paper, six coordination polymers were synthesized by using N-dicarboxylic acid ligands as organic ligands, Scandium metal and lanthanide metals such as europium, terbium, gadolinium and erbium as metal centers under hydrothermal and solvothermal conditions. The luminous, catalytic and adsorption properties of the six coordination polymers were studied. The main contents are as follows: 1) 2,5-pyridyl dicarboxylic acid (2,5 pyridinedicarboxylic acid,H_2L~1), 2, 3-pyrazide dicarboxylic acid (2, 3 pyrazinedicarboxylic acid,H_2L~2) were used as organic ligands and SC as metal center, respectively. Two coordination polymers [Sc_2L_2~1 (HL~1) _ 2 (H 鈮，
本文编号：2479214
[Abstract]:Coordination polymer (coordination polymers,CPs), also known as metal organic skeleton (Metal organic frameworks,MOFs), as one of the most concerned research fields in chemistry and material science, has shown a very rapid development trend in recent years. CPs not only has rich topological structure, but also has potential application value in many fields, such as gas adsorption and separation, catalysis, luminous, sensing and proton conduction. Their crystallization characteristics, high porosity, uniform pore size, large surface area, adjustable pore surface characteristics and potential industrial scale scalability make this kind of materials have the potential for further research. Among many types of coordination polymers, rare earth ions as metal centers have attracted extensive attention. Because rare earth ions usually adopt eight or twelve coordination modes and have special luminous properties, the coordination polymers constructed by rare earth ions have various structures and excellent optical properties. In addition, the introduction of hetero atoms such as N atoms into organic ligands greatly improves the possibility of the formation of coordination polymers with novel structures. In this paper, six coordination polymers were synthesized by using N-dicarboxylic acid ligands as organic ligands, Scandium metal and lanthanide metals such as europium, terbium, gadolinium and erbium as metal centers under hydrothermal and solvothermal conditions. The luminous, catalytic and adsorption properties of the six coordination polymers were studied. The main contents are as follows: 1) 2,5-pyridyl dicarboxylic acid (2,5 pyridinedicarboxylic acid,H_2L~1), 2, 3-pyrazide dicarboxylic acid (2, 3 pyrazinedicarboxylic acid,H_2L~2) were used as organic ligands and SC as metal center, respectively. Two coordination polymers [Sc_2L_2~1 (HL~1) _ 2 (H 鈮，
本文编号：2479214
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