【摘要】：發(fā)光金屬有機(jī)骨架是一類孔隙率高、比表面積大、孔結(jié)構(gòu)可控、化學(xué)性質(zhì)穩(wěn)定和制備過程簡(jiǎn)單的新型多孔晶態(tài)發(fā)光材料。該類材料在熒光傳感檢測(cè)污染物方面具有檢測(cè)速度快、靈敏度高、選擇性好、穩(wěn)定可靠等優(yōu)點(diǎn),成為新一代的理想發(fā)光材料。此外,擁有不同功能基團(tuán)的發(fā)光金屬有機(jī)骨架可以作為一個(gè)保護(hù)性的支架,避免在主-客體體系中稀土離子的水合淬滅。(1)本論文以4,4'-二苯乙烯基二羧酸(L1)和2,5-二-(3,5-二羧基苯基)噻吩二甲酰胺(L2)作為有機(jī)配體與具有d10結(jié)構(gòu)的過渡金屬鋅和鎘離子構(gòu)筑了三個(gè)發(fā)光金屬有機(jī)骨架材料Zn3 L1）3(DMF)2(MOF1)、Zn3(L1)3(DMA)2(H20)3(MOF2)和[Cd2(H2L)2(H20)5]·5H20·2DMF(MOF3)。通過紅外光譜(FT-IR)、粉末X-射線衍射(PXRD)、熱重(TG)和元素分析(EA)等手段對(duì)發(fā)光金屬有機(jī)骨架材料進(jìn)行了表征和分析,并利用熒光光譜(PL)研究了其光學(xué)性質(zhì)。(2)研究了發(fā)光金屬有機(jī)骨架MOF1和MOF2對(duì)硝基芳香化合物和金屬離子的熒光傳感性能。研究結(jié)果表明,硝基芳香化合物使MOF1和MOF2的熒光強(qiáng)度都發(fā)生了不同程度地淬滅。其中,對(duì)硝基苯胺的熒光淬滅效果最明顯。金屬離子使MOF1和MOF2的熒光強(qiáng)度也發(fā)生了不同程度的淬滅或增強(qiáng)。在所選擇的13種金屬離子中,Fe3+使MOF1和MOF2發(fā)生了明顯的熒光淬滅,而A13+使MOF1的熒光強(qiáng)度發(fā)生了明顯的增強(qiáng)。另外,研究發(fā)現(xiàn)MOF1和MOF2具有良好的循環(huán)穩(wěn)定性和抗干擾性。因此,MOF1和MOF2在選擇性熒光檢測(cè)硝基芳香化合物和金屬離子方面具有潛在的應(yīng)用價(jià)值。(3)研究了發(fā)光金屬有機(jī)骨架MOF3對(duì)硝基芳香化合物和金屬離子的熒光傳感檢測(cè)性能以及敏化稀土離子發(fā)光的作用。研究發(fā)現(xiàn),MOF3對(duì)Fe3+離子和對(duì)硝基苯胺的熒光傳感具有高選擇性、高靈敏性、抗干擾性和循環(huán)穩(wěn)定性。對(duì)于水溶液中稀土離子的敏化研究發(fā)現(xiàn),MOF3對(duì)水溶液中的Eu3+離子具有良好的敏化效果,深入研究發(fā)現(xiàn)隨著敏化濃度和時(shí)間的增加敏化效果越好,并且在紫外燈下呈現(xiàn)出肉眼可見的由藍(lán)到紅的顏色變化實(shí)現(xiàn)了可以調(diào)節(jié)的熒光發(fā)射。
[Abstract]:Luminescent metal organic skeleton is a new kind of porous crystalline luminescent material with high porosity, large specific surface area, controllable pore structure, stable chemical properties and simple preparation process. This kind of material has the advantages of high detection speed, high sensitivity, good selectivity, stability and reliability in the detection of pollutants by fluorescence sensing. It has become a new generation of ideal luminescent materials. In addition, luminescent organometallic skeletons with different functional groups can be used as protective scaffolds. Avoid hydration quenching of rare earth ions in the host-guest system. (1) in this thesis, the organic ligands (L _ 2) and the transition metal zinc (Zn) with d10 structure were used as organic ligands and 2o _ 5- (3o _ 5-dicarboxyphenyl) thiophene dicarboxylic acid (L1) and 2o _ 5- (3o _ 5-dicarboxyphenyl) thiophene dicarboxylic acid (L2) as organic ligands. Three luminescent metal organic skeleton materials Zn3L1) 3 (DMF) 2 (MOF1) Zn3 (L1) 3 (DMA) 2 (H20) 3 (MOF2) and [CD2 (H2L) 2 (H20) 5] 5H202DMF (MOF3) were constructed by cadmium ion. The luminescent metal-organic skeleton materials were characterized by FT-IR, X-ray diffraction (PXRD), thermogravimetry (TG) and elemental analysis (EA). The optical properties were studied by fluorescence spectroscopy (PL). (2) the fluorescence sensing properties of MOF1 and MOF2 p-nitroaromatic compounds and metal ions were studied. The results showed that the fluorescence intensity of MOF1 and MOF2 were quenched to varying degrees by nitroaromatic compounds. The fluorescence quenching effect of p-nitroaniline was the most obvious. The fluorescence intensity of MOF1 and MOF2 was quenched or enhanced in varying degrees by metal ions. Among the 13 metal ions selected, Fe _ 3 can cause the fluorescence quenching of MOF _ 1 and MOF _ 2, while A _ 13 enhances the fluorescence intensity of MOF _ 1. In addition, it is found that MOF 1 and MOF 2 have good cycle stability and anti-interference. Therefore, MOF1 and MOF2 have potential application value in selective fluorescence detection of nitroaromatic compounds and metal ions. (3) the fluorescence sensing properties of luminescent metal organic framework MOF3 for nitroaromatic compounds and metal ions have been studied. Energy and sensitized effect of rare earth ion luminescence. It is found that MOF3 has high selectivity, high sensitivity, anti-interference and cyclic stability for the fluorescence sensing of Fe _ 3 and p-nitroaniline. For the sensitization of rare earth ions in aqueous solution, it is found that MOF3 has a good sensitization effect on EU3 ions in aqueous solution. The further study shows that the better the sensitization effect is with the increase of sensitizing concentration and time. And under the ultraviolet lamp, visible to the naked eye from blue to red color change to achieve adjustable fluorescence emission.
【學(xué)位授予單位】：天津工業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TB383.4;O657.3

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