基于HA和MOF功能材料的构建及其在离子吸附、载药和荧光传感方面的应用研究

发布时间：2019-06-08 08:13

【摘要】：21世纪以来,功能性材料以其特有的性质吸引了广泛的关注。本论文主要研究制备了羟基磷灰石(HA)、磁性羟基磷灰石复合材料(Fe2O3@HA)和金属有机骨架复合磁性材料(Au-Fe3O4@Tb-BTC),以及其在离子吸附,载药和荧光传感等方面的应用研究,主要研究内容如下：采用水热法成功制备了羟基磷灰石纳米棒、花状和球形羟基磷灰石聚集体。同时,考察了其作为离子吸附载体材料,对几种重金属离子(Pb2+, Cu2+, Mn2+,Zn2+)的吸附性能。首先,考察了羟基磷灰石的浓度,吸附时间,重金属离子的类型和羟基磷灰石的结构与形貌等因素对重金属离子吸附量的影响情况。在这些多因素研究基础上,确定了最佳的离子吸附条件。进一步,以对Pb2+离子的吸附实验为载体,借助XRD、SEM、ICP-AES、FT-IR和Raman光谱等系列分析检测手段对,深入考察了羟基磷灰石的吸附机理。分析结果揭示,羟基磷灰石对重金属离子的吸附主要受其比表面积和离子交换产生的共沉淀的影响较为显著,为进一步探求具有更强吸附能力的环保型吸附载体材料提供了些许参考。利用微波水热法合成了纳米级别的、排列比较规则的金属有机框架材料MIL-53(Fe),对制备的MIL-53(Fe)材料通过水热法进行羟基磷灰石包裹。然后,把这种HA@MIL-53(Fe)复合材料进行煅烧,使其形成磁性的多孔核壳材料。通过X-射线衍射,扫描电镜和透射电镜对复合材料的结构和形貌进行检测。最后,将该材料对布洛芬进行载药和缓释实验,并对实验数据进行分析,来研究该材料对布洛芬的载药性能和缓释性能。结果显示,此载体材料不仅具有一定的磁性良好的载药和缓释性能,载药量达到25.6%。120小时后,药物布洛芬的释放量达到89.8%。结果表明所合成的样品有望应用在药物载体领域。通过层层自组装的方法制备了一种以Tb-BTC为壳的多功能磁性微球Au@Fe3O4@Tb-BTC。采用X-射线衍射,扫描电镜和透射电镜对这种多功能磁性核壳微球进行结构和形貌表征,发现Au@Fe3O4确实包裹在以Tb-BTC为壳的里面。通过这种方法使得这种材料同时具备了磁性和良好的荧光性质,那我们就利用这种材料的磁性核荧光性质对硝基苯(NB),邻硝基甲苯(2-NT),对硝基甲苯(4-NT),2,4-二硝基甲苯(2,4-DNT),2,6-二硝基甲苯(2,6-DNT),2,4,6-三硝基酚(PA)和2,4,6-三硝基甲苯这7中硝基化合物的荧光传感进行研究,发现这种材料对NB,4-NT,2-NT,2,6-DNT, PA,2,4-DNT, TNT的Ksv分别是9490M-1,10439M-1,13372M-1,39177M-1,50866M-1,60244M-1,148431 M-1.样品对硝基芳烃化合物的荧光猝灭效率为TNT2,4-DNTPA2,6-DNT2-NT4-NTNB,可能是由于这种材料对硝基芳烃化合物的荧光猝灭效率与硝基芳烃化合物的硝基数目有关,并且利用循环实验验证了该种材料能够循环使用来降低不必要的污染。
[Abstract]:Since the 21 st century, functional materials have attracted extensive attention because of their unique properties. In this paper, hydroxyapatite (HA), magnetic hydroxyapatite composites (Fe2O3@HA) and organometallic skeleton composite magnetic materials (Au-Fe3O4@Tb-BTC) were prepared and their ion adsorption was studied. The main research contents are as follows: hydroxyapatite nanorods, floral and spherical hydroxyapatite aggregates were successfully prepared by hydrothermal method. At the same time, the adsorption properties of several heavy metal ions (Pb2, Cu2, Mn2, Zn2) as ion adsorption carrier materials were investigated. Firstly, the effects of hydroxyapatite concentration, adsorption time, the type of heavy metal ions and the structure and morphology of hydroxyapatite on the adsorption capacity of heavy metal ions were investigated. On the basis of these multi-factor studies, the optimum ion adsorption conditions were determined. Furthermore, the adsorption mechanism of hydroxyapatite was investigated by a series of analysis and detection methods, such as XRD,SEM,ICP-AES,FT-IR and Raman spectra, on the basis of the adsorption experiment of Pb2 ions. The results show that the adsorption of heavy metal ions by hydroxyapatite is mainly affected by the specific surface area and coprecipitation produced by ion exchange. It provides some reference for further exploration of environmentally friendly adsorption carrier materials with stronger adsorption capacity. Nanometer and regular organometallic frame material MIL-53 (Fe), was synthesized by microwave hydrothermal method. The prepared MIL-53 (Fe) material was coated with hydroxyapatite by hydrothermal method. Then, the HA@MIL-53 (Fe) composites were calcined to form magnetic porous core-shell materials. The structure and morphology of the composites were detected by X-ray diffraction, scanning electron microscope and transmission electron microscope. Finally, the drug loading and sustained release experiments of ibuprofen were carried out, and the experimental data were analyzed to study the drug loading and sustained release properties of ibuprofen. The results showed that the carrier material not only had good magnetic drug loading and sustained release performance, but also reached 25.6%. After 120 hours, the drug release rate of ibuprofen reached 88.8%. The results show that the synthesized samples are expected to be used in the field of drug carriers. A multifunctional magnetic microspheres Au@Fe3O4@Tb-BTC. with Tb-BTC as shell was prepared by layer self-assembly. The structure and morphology of the multifunctional magnetic core-shell microspheres were characterized by X-ray diffraction, scanning electron microscope and transmission electron microscope. It was found that Au@Fe3O4 was indeed wrapped in the shell of Tb-BTC. By this method, the material has both magnetic and good fluorescence properties, so we use the magnetic nuclear fluorescence properties of this material, p-nitrobenzene (NB), o-nitrotoluene (2-NT), p-nitrotoluene (4-NT). The fluorescence sensing of nitro compounds in 2,4 dinitrotoluene (2,4 DNT), 2,6 dinitrotoluene (2,6 DNT), 2,4,6 trinitrophenol (PA) and 2,4,6 trinitrotoluene was studied. It was found that this material could be used for NB,. The Ksv of 4 NT, 2, 6 DNT and PA,2,4-DNT, TNT are 9490M, 10439m, 13372M, 39177M, 50866M, 60244M, 14843M, respectively, which are 9490m, 10439m, 13372m, 39177m, 50866m, 60244m, 148431, respectively. The fluorescence quenching efficiency of the sample to nitroaromatic compounds is TNT2,4-DNTPA2,6-DNT2-NT4-NTNB, which may be due to the fact that the fluorescence quenching efficiency of nitroaromatic compounds is related to the number of nitro groups of nitroaromatic compounds. The recycling experiments show that the material can be recycled to reduce unnecessary pollution.
【学位授予单位】：安徽大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：TB34

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