含铜镍金属—有机多孔材料的制备及其吸附性能研究

发布时间：2018-05-08 22:02

本文选题：金属-有机多孔材料 + 亚甲基蓝　；参考：《浙江师范大学》2015年硕士论文

【摘要】：新材料的开发及应用对现代经济的发展至关重要。金属-有机多孔材料作为包含多交叉学科知识特征的材料倍受重视,被广泛应用于吸附分离、催化、光学、磁学等领域。迄今为止,含铜镍金属-有机多孔材料应用于液相吸附的研究报道较少。因此,对于环境保护的要求,可以利用其所具有的大比表面积、孔隙率高、协同效应、结构多样化等特点处理染料废水。本文采用水热合成法,合成了Cu-BTC和Ni/Cu-BTC两种金属-有机多孔材料。运用N2吸脱附等温线、TG/DTA、XRD、SEM等技术对其进行了表征。Cu-BTC和Ni/Cu-BTC样品结构与文献中报道的一致。Cu-BTC和Ni/Cu-BTC的BET比表面积分别为1379m2/g和1156m2/g,热稳定温度可达623K。研究了不同的吸附平衡时间、温度、初始浓度、pH条件下,Cu-BTC和Ni/Cu-BTC静态法吸附分离模型废水中的亚甲基蓝和刚果红染料分子性能。结果表明,两种多孔材料在240min时可达到吸附平衡状态。随着溶液初始浓度的增加,亚甲基蓝和刚果红染料分子的饱和吸附量随之增加,并且吸附容量随温度的升高而增加。运用Langmuir、Freundlich、Tekmin三种吸附模型,以及准一级动力学、准二级动力学、颗粒内扩散三种动力学模型,对吸附过程进行描述。Cu-BTC和Ni/Cu-BTC的吸附等温线拟合结果较为符合Langmuir模型。动力学拟合结果显示,两种材料对亚甲基蓝和刚果红的吸附过程符合准二级动力学模型。热力学参数表明,两种染料分子在两种金属-有机多孔材料上的吸附过程是自发的吸热过程。含双金属不饱和配位的Ni/Cu-BTC对刚果红的饱和吸附量(1078mg/g)明显高于单金属Cu-BTC的吸附量(877mg/g)。表明掺杂了Cu和Ni两种金属元素的Ni/Cu-BTC材料具有更优良的染料吸附性能。另外,本文研究了以金属-有机多孔材料Cu-BTC为模板,糠醇为碳源,采用硬模板法合成了新型介孔炭材料FAPC-1。运用N2吸脱附等温线、TG/DTA、 XRD、TEM、FT-IR等手段对样品进行了表征。结果表明,样品的BET比表面积为664m2/g,孔容为0.64cm3/g,孔径集中在4nm左右。实验结果表明所合成的炭材料具有介孔结构。研究了常温低压范围,介孔炭材料FAPC-1对二氧化碳的静态吸附效果,结果表明其饱和吸附量可以达到2.14mmol/g,高于相关文献报道值。本论文的工作表明含有单金属尤其双金属不饱和配位的有机多孔材料在印染废水净化领域具有重要应用前景。同时,采用Cu-BTC为模板得到的介孔炭材料在C02气体吸附存储领域具有应用潜力。
[Abstract]:The development and application of new materials is very important to the development of modern economy. Metal-organic porous materials have been widely used in adsorption separation, catalysis, optics, magnetism and so on. So far, there are few reports on the application of copper-nickel-organic porous materials in liquid phase adsorption. Therefore, for environmental protection, dye wastewater can be treated by its characteristics of large specific surface area, high porosity, synergistic effect and diversified structure. In this paper, two kinds of metal-organic porous materials, Cu-BTC and Ni/Cu-BTC, were synthesized by hydrothermal synthesis. The structure of Cu-BTC and Ni/Cu-BTC samples were characterized by N _ 2 absorption-desorption isotherm TG- / DTA-XRDX SEM. The BET specific surface areas of .Cu-BTC and Ni/Cu-BTC were 1379m2/g and 1156m ~ 2 / g, respectively, and the thermal stability temperature was 623K. The molecular properties of methylene blue and Congo red dyes in model wastewater were studied by static adsorption of Cu-BTC and Ni/Cu-BTC at different adsorption equilibrium time, temperature and initial concentration. The results show that the adsorption equilibrium of the two porous materials can be reached at 240min. The saturated adsorption capacity of methylene blue and Congo red dye increases with the increase of initial solution concentration, and the adsorption capacity increases with the increase of temperature. Using three adsorption models of Langmuir-Freundlichl Tekmin, as well as three kinetic models of quasi-first-order kinetics, quasi-second-order kinetics and intra-particle diffusion, the adsorption isotherm fitting results of Cu-BTC and Ni/Cu-BTC are in good agreement with Langmuir model. The kinetic fitting results show that the adsorption process of methylene blue and Congo red is in accordance with the quasi-second-order kinetic model. The thermodynamic parameters show that the adsorption of two dye molecules on two metal-organic porous materials is a spontaneous endothermic process. The saturated adsorption of Congo red by Ni/Cu-BTC with bimetallic unsaturated coordination is significantly higher than that of monometallic Cu-BTC by 1078mg / g. The results show that the Ni/Cu-BTC materials doped with Cu and Ni have better dye adsorption properties. In addition, a new mesoporous carbon material FAPC-1 was synthesized by hard template method using metal-organic porous material Cu-BTC as template and furfuryl alcohol as carbon source. The samples were characterized by N _ 2 adsorption and desorption isotherm TG / DTA, XRDX Tem FT-IR and so on. The results show that the BET surface area of the sample is 664m2 / g, the pore volume is 0.64cm3 / g, and the pore size is about 4nm. The experimental results show that the synthesized carbon materials have mesoporous structure. The static adsorption effect of mesoporous carbon material FAPC-1 on carbon dioxide at room temperature and low pressure was studied. The results show that the saturated adsorption capacity can reach 2.14 mmol / g, which is higher than that reported in related literatures. The work of this paper shows that organic porous materials containing monometallic, especially bimetallic unsaturated coordination materials have important application prospects in the field of printing and dyeing wastewater purification. At the same time, the mesoporous carbon materials prepared by using Cu-BTC as template have potential application in CO2 gas adsorption storage.
【学位授予单位】：浙江师范大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TB383.4

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