含銅鎳金屬—有機多孔材料的制備及其吸附性能研究
發(fā)布時間:2018-05-08 22:02
本文選題:金屬-有機多孔材料 + 亞甲基藍; 參考:《浙江師范大學》2015年碩士論文
【摘要】:新材料的開發(fā)及應用對現代經濟的發(fā)展至關重要。金屬-有機多孔材料作為包含多交叉學科知識特征的材料倍受重視,被廣泛應用于吸附分離、催化、光學、磁學等領域。迄今為止,含銅鎳金屬-有機多孔材料應用于液相吸附的研究報道較少。因此,對于環(huán)境保護的要求,可以利用其所具有的大比表面積、孔隙率高、協同效應、結構多樣化等特點處理染料廢水。本文采用水熱合成法,合成了Cu-BTC和Ni/Cu-BTC兩種金屬-有機多孔材料。運用N2吸脫附等溫線、TG/DTA、XRD、SEM等技術對其進行了表征。Cu-BTC和Ni/Cu-BTC樣品結構與文獻中報道的一致。Cu-BTC和Ni/Cu-BTC的BET比表面積分別為1379m2/g和1156m2/g,熱穩(wěn)定溫度可達623K。研究了不同的吸附平衡時間、溫度、初始濃度、pH條件下,Cu-BTC和Ni/Cu-BTC靜態(tài)法吸附分離模型廢水中的亞甲基藍和剛果紅染料分子性能。結果表明,兩種多孔材料在240min時可達到吸附平衡狀態(tài)。隨著溶液初始濃度的增加,亞甲基藍和剛果紅染料分子的飽和吸附量隨之增加,并且吸附容量隨溫度的升高而增加。運用Langmuir、Freundlich、Tekmin三種吸附模型,以及準一級動力學、準二級動力學、顆粒內擴散三種動力學模型,對吸附過程進行描述。Cu-BTC和Ni/Cu-BTC的吸附等溫線擬合結果較為符合Langmuir模型。動力學擬合結果顯示,兩種材料對亞甲基藍和剛果紅的吸附過程符合準二級動力學模型。熱力學參數表明,兩種染料分子在兩種金屬-有機多孔材料上的吸附過程是自發(fā)的吸熱過程。含雙金屬不飽和配位的Ni/Cu-BTC對剛果紅的飽和吸附量(1078mg/g)明顯高于單金屬Cu-BTC的吸附量(877mg/g)。表明摻雜了Cu和Ni兩種金屬元素的Ni/Cu-BTC材料具有更優(yōu)良的染料吸附性能。另外,本文研究了以金屬-有機多孔材料Cu-BTC為模板,糠醇為碳源,采用硬模板法合成了新型介孔炭材料FAPC-1。運用N2吸脫附等溫線、TG/DTA、 XRD、TEM、FT-IR等手段對樣品進行了表征。結果表明,樣品的BET比表面積為664m2/g,孔容為0.64cm3/g,孔徑集中在4nm左右。實驗結果表明所合成的炭材料具有介孔結構。研究了常溫低壓范圍,介孔炭材料FAPC-1對二氧化碳的靜態(tài)吸附效果,結果表明其飽和吸附量可以達到2.14mmol/g,高于相關文獻報道值。本論文的工作表明含有單金屬尤其雙金屬不飽和配位的有機多孔材料在印染廢水凈化領域具有重要應用前景。同時,采用Cu-BTC為模板得到的介孔炭材料在C02氣體吸附存儲領域具有應用潛力。
[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.
【學位授予單位】:浙江師范大學
【學位級別】:碩士
【學位授予年份】:2015
【分類號】:TB383.4
【參考文獻】
相關期刊論文 前1條
1 劉玉臣;胡鑫;鞏睿;于會賢;唐曉丹;朱偉東;代偉;;微孔-介孔高比表面積佛手渣基活性炭的制備[J];化工新型材料;2012年09期
,本文編號:1863249
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