四唑基苯酚配体配合物的合成、结构及性能研究
发布时间：2018-08-11 08:47
【摘要】：近年来,配位聚合物由于新颖多变的拓扑结构及在气体吸附、发光性能、磁性及催化性能等领域的潜在应用成为无机化学及有机化学研究的重要方向之一。含四个氮原子的四唑配体具有多样的配位模式和化学性质,是构筑具有独特结构和性能配合物的一类重要配体。配合物的构建方法多种多样,水热合成法是构筑配合物的重要方法之一,其中水热原位反应为配位化学和有机化学的结合建立了一种新的桥梁,因此越来越多的配位化学工作者致力于水热或溶剂热的原位反应。本论文以4-(1H-四唑-5-基)苯酚(H2L~4)、3-(1H-四唑-5-基)苯酚(H2L~5)和2-(1H-四唑-5-基)苯酚(H2L~6)三个有机化合物为配体或者前驱配体,利用水热法及溶剂挥发等方法设计合成了十五个新的过渡金属配合物,通过红外、X-射线单晶衍射、X-射线粉末衍射测试(PXRD)、热重(TGA)等测试手段对十五个新的配合物进行了结构表征。同时,也深入研究了部分配合物的固态荧光性能、半导体性质和磁性。具体研究内容如下:1、合成了三个不同的四唑基酚衍生物:4-(1H-四唑-5-基)苯酚(H2L~4)、3-(1H-四唑-5-基)苯酚(H2L~5)和2-(1H-四唑-5-基)苯酚(H2L~6)配体,并对其进行了表征。2、利用4-(1H-四唑-5-基)苯酚(H2L~4)、3-(1H-四唑-5-基)苯酚(H2L~5)、2-(1H-四唑-5-基)苯酚(H2L~6)和硝酸盐在水热条件下发生原位反应,得到了基于2,6-二硝基-4-(1H-四唑-5-基)苯酚(H2L1)、2,4,6-三硝基-3-(1H-四唑-5-基)苯酚(H2L2)和2,4-二硝基-6-(1H-四唑-5-基)苯酚(H2L3)配体的十个配合物:{[Zn_3(L~1)_2(OH)_2]·H_2O}_n(1)、[Ag_2(L~1)]_n(2)、[Co(HL~1)_2(H_2O)_4](3)、[Cu_3(L~1)_2(OH)_2(H_2O)]_n(4)、[Cu_7(HL~1)_2(L~1)_6(H_2O)_6]_n(5)、[Cu(L~1)(H_2O)_3]_n(6)、[Cu(HL~1)_2(H_2O)_4·2H_2O](7)、[Ag_2(L~2)]_n(8)、[Ag_8(L~3)_4(H_2O)]_n(9)和[Cu(L~3)(H_2O)_2]_n(10)。对配合物1-10进行了一系列基本表征,结果表明配合物1、4和8为三维结构,2、5和9为二维结构,6和10为一维链结构,3和7为单核结构。讨论配体结构和配位模式对配合物结构的影响。深入研究了配合物1-3和8-9的固态荧光性能、配合物1-6和8-10的半导体性质及配合物3-6和10的磁性。3、利用邻羟基苯腈、NaN3分别与相应的金属盐发生原位反应,得到了两个锌镉配合物[Zn_3(L~6)_3(H_2O)]_n(12)和[Cd(L~6)(H_2O)]_n(13),用4-(1H-四唑-5-基)苯酚(H2L~4)和2-(1H-四唑-5-基)苯酚(H2L~6)配体在不同的条件下合成配合物[Ni_3(L~4)_3(H_2O)_(10)](11)、[Cd_2(HL~6)_4(H_2O)_4](14)和[Co(L6)(H_2O)]_n(15)。对配合物11-15的结构进行了测试表征,结果表明配合物11和14为单核结构,12、13和15为二维结构。讨论了配体的配位模式和金属离子对其结构的影响。并且研究了配体H2L~6和配合物12-14的固态荧光性能,配合物11-14的半导体性质,配合物11的磁性。
[Abstract]:In recent years, coordination polymers have become one of the important research fields in inorganic chemistry and organic chemistry due to their novel topological structure and potential applications in the fields of gas adsorption, luminescence, magnetic properties and catalytic properties. Tetrazolium ligands containing four nitrogen atoms have various coordination modes and chemical properties. They are important ligands with unique structure and properties. Hydrothermal synthesis is one of the most important methods for the construction of coordination compounds, in which hydrothermal in-situ reaction establishes a new bridge for the combination of coordination chemistry and organic chemistry. Therefore, more and more coordination chemists focus on in situ reactions of hydrothermal or solvothermal reactions. In this thesis, three organic compounds, 4- (1H-tetrazol-5-yl) phenol (H2L~4), 3- (1H-tetrazol-5-yl) phenol (H2L~5) and 2- (1H-tetrazol-5-yl) phenol (H2L~6), were used as ligands or precursor ligands. Fifteen new transition metal complexes were designed and synthesized by hydrothermal method and solvent volatilization method. The structures of 15 new complexes were characterized by infrared X-ray single crystal diffraction and X-ray powder diffraction (PXRD), thermogravimetric (TGA). At the same time, the solid state fluorescence properties, semiconductor properties and magnetic properties of some complexes were also studied. Three different tetrazolophenol derivatives: 4- (1H-tetrazol-5-yl) phenol (H2L~4) 3- (1H-tetrazol-5-yl) phenol (H2L~5) and 2- (1H-tetrazol-5-yl) phenol (H2L~6) ligands were synthesized. It was characterized by in situ reaction of 4- (1H-tetrazol-5-yl) phenol (H2L~4) 3- (1H-tetrazol-5-yl) phenol (H2L~5) -2- (1H-tetrazol-5-yl) phenol (H2L~6) with nitrate under hydrothermal conditions. 寰楀埌浜嗗熀浜，
本文编号：2176493
[Abstract]:In recent years, coordination polymers have become one of the important research fields in inorganic chemistry and organic chemistry due to their novel topological structure and potential applications in the fields of gas adsorption, luminescence, magnetic properties and catalytic properties. Tetrazolium ligands containing four nitrogen atoms have various coordination modes and chemical properties. They are important ligands with unique structure and properties. Hydrothermal synthesis is one of the most important methods for the construction of coordination compounds, in which hydrothermal in-situ reaction establishes a new bridge for the combination of coordination chemistry and organic chemistry. Therefore, more and more coordination chemists focus on in situ reactions of hydrothermal or solvothermal reactions. In this thesis, three organic compounds, 4- (1H-tetrazol-5-yl) phenol (H2L~4), 3- (1H-tetrazol-5-yl) phenol (H2L~5) and 2- (1H-tetrazol-5-yl) phenol (H2L~6), were used as ligands or precursor ligands. Fifteen new transition metal complexes were designed and synthesized by hydrothermal method and solvent volatilization method. The structures of 15 new complexes were characterized by infrared X-ray single crystal diffraction and X-ray powder diffraction (PXRD), thermogravimetric (TGA). At the same time, the solid state fluorescence properties, semiconductor properties and magnetic properties of some complexes were also studied. Three different tetrazolophenol derivatives: 4- (1H-tetrazol-5-yl) phenol (H2L~4) 3- (1H-tetrazol-5-yl) phenol (H2L~5) and 2- (1H-tetrazol-5-yl) phenol (H2L~6) ligands were synthesized. It was characterized by in situ reaction of 4- (1H-tetrazol-5-yl) phenol (H2L~4) 3- (1H-tetrazol-5-yl) phenol (H2L~5) -2- (1H-tetrazol-5-yl) phenol (H2L~6) with nitrate under hydrothermal conditions. 寰楀埌浜嗗熀浜，
本文编号：2176493
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