12-钨磷酸基金属有机骨架复合材料的合成、表征及染料吸附性质研究

发布时间：2018-06-06 03:04

本文选题：多金属氧酸盐 + 金属有机骨架　；参考：《东北师范大学》2017年硕士论文

【摘要】：近些年来,随着社会、经济和工业的不断发展,有机染料在工业生产和日常生活中扮演着极其重要的角色,它使我们的生活色彩斑斓。然而,大量未经过合理处理的染料废水被直接地排放,由于大部分染料分子是毒性的甚至是致癌的,这对于水体环境和人类健康产生了巨大的威胁。因此,在染料废水排放到环境中之前,我们迫切地需要找到一种有效的方法来处理废水中的有机染料分子。目前,在现存的多种处理方法中,吸附是一种简单和方便的染料污水治理方式。本论文首次将Keggin型的多酸H_3PW_(12)O_(40)(PW_(12))引入到无毒多孔的金属有机骨架MIL-101(Fe)中获得了一个POM@MOF复合材料(记为PW_(12)@MIL-101(Fe)),并且对此材料进行了表征和染料吸附性质的研究。1.复合材料的合成和表征通过H_3PW_(12)O_(40),FeCl3·6H2O和对苯二甲酸(H2bdc)的一锅溶剂热反应获得了PW_(12)@MIL-101(Fe)复合物。我们采用傅里叶变换红外光谱(FTIR),X-射线粉末衍射(XRD),热重分析(TGA),电感耦合等离子光谱发生仪(ICP),扫描电子显微镜(SEM),能谱分析(EDS),EDS元素分布,~(31)P核磁波谱(~(31)P NMR)和N_2吸附-脱附等温线等测试对该复合材料进行了详细的表征。这些测试结果共同证明H_3PW_(12)O_(40)成功地嵌入到MIL-101(Fe)的孔道中。2.复合材料的染料吸附性质研究此部分主要探究了以下五个方面内容:(1)染料浓度的影响;(2)吸附量和去除率的计算;(3)MIL-101(Fe)和PW_(12)@MIL-101(Fe)对不同类型有机染料的吸附能力对比;(4)复合材料对于混合染料的选择性吸附;(5)复合材料的可重复使用性和稳定性。实验结果表明,对于40 mg/L的MB溶液,MB的吸附率在30min内达到96.2%。此外,复合物也能够迅速去除97.3%的MB从1 ppm(1 mg/L)的MB染料溶液中。值得一提的是,在100ml 100mg/L MB溶液中加入20mg PW_(12)-5g@MIL-101(Fe)时,复合材料对MB的吸附量为473.7 mg/g。在染料吸附测验中,单独的MIL-101(Fe)在30min内对阳离子型的亚甲基蓝(MB)和罗丹明B(RhB)染料的去除率分别为30.7%和28.3%,对于阴离子型的甲基橙(MO)染料的去除率能够达到82%。然而,在引入高电负性的多酸阴离子到MIL-101(Fe)的骨架中之后,其吸附能力发生了极大的改变。PW_(12)@MIL-101(Fe)复合材料在最初的5min内对阳离子染料MB和RhB的吸附率能够达到99%和96%,对于阴离子染料MO的吸附率能达到16%。这种材料还可以选择性地捕获阳离子染料在MB,RhB和MO组成的三元混合染料体系中。此外,该材料能够很容易地脱附再利用,并且复合材料的结构在吸附实验中是完整的。因此,它是去除染料废水中阳离子有机污染物的一种有前景且环保的吸附剂。
[Abstract]:In recent years, with the continuous development of society, economy and industry, organic dyes play an extremely important role in industrial production and daily life. It makes our life colorful. However, a large number of dye wastewater, which has not been properly treated, is discharged directly, because most dye molecules are toxic or even carcinogenic. There is a great threat to the water environment and human health. So, before the dye wastewater is discharged to the environment, we urgently need to find an effective method to deal with the organic dye molecules in the wastewater. At present, in the existing treatment methods, adsorption is a simple and convenient method for treatment of dye wastewater. The Keggin polyacid H_3PW_ (12) O_ (40) (40) (PW_ (12)) was first introduced into the non-toxic porous metal organic framework MIL-101 (Fe) to obtain a POM@MOF composite (recorded as PW_ (12) @MIL-101 (Fe)), and the material was characterized and the dye adsorbability was studied. The synthesis and characterization of the.1. composite materials were carried out by H_3PW_ (12) (40). PW_ (12) @MIL-101 (Fe) complex was obtained by one pot solvothermal reaction of O and terephthalic acid (H2bdc). We used Fourier transform infrared spectroscopy (FTIR), X- ray powder diffraction (XRD), thermogravimetric analysis (TGA), inductively coupled plasma spectrograph (ICP), scanning electron microscope (SEM), energy spectrum analysis (EDS), element distribution, and ~ (31) magnetic nuclear magnetic spectroscopy (~ (31) P NMR) and N_2 adsorption - desorption isotherms and other tests to characterize the composites in detail. These results show that H_3PW_ (12) O_ (40) is successfully embedded in the MIL-101 (Fe) channel of the dye adsorption properties of.2. composites. This part is mainly to explore the following five aspects: (1) the influence of dye concentration; (2) Calculation of adsorption and removal rate; (3) the adsorption capacity of MIL-101 (Fe) and PW_ (12) @MIL-101 (Fe) on different types of organic dyes; (4) selective adsorption of composite dyes for mixed dyes; (5) reproducibility and stability of the composite. The experimental results show that the adsorption rate of MB is reached to 96.2%. in the MB solution of 40 mg/L. In addition, the complex can also quickly remove 97.3% MB from 1 ppm (1 mg/L) of MB dye solution. It is worth mentioning that when 20mg PW_ (12) -5g@MIL-101 (Fe) is added to the 100ml 100mg/L MB solution, the adsorption capacity of the composite material to MB is 473.7. The removal rates of B and Luo Danming B (RhB) dyes are 30.7% and 28.3% respectively. The removal rate of anionic methyl orange (MO) dyes can reach 82%., however, after the introduction of high electronegativity polyanic anions to the skeleton of MIL-101 (Fe), the adsorption capacity of the dyestuffs has undergone a great change in.PW_ (12) @MIL-101 (Fe) composite in the initial 5min. The adsorption rate of cationic dyes MB and RhB can reach 99% and 96%, and the adsorption rate of the anion dye MO can reach 16%.. The material can also selectively capture the three element mixed dye system composed of MB, RhB and MO. In addition, the material can be easily reused and reused, and the structure of the composite material is adsorbed. The experiment is complete. Therefore, it is a promising and environmentally friendly adsorbent for removing cationic organic pollutants from dye wastewater.
【学位授予单位】：东北师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TB33;O647.3

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