介孔铁基复合及负载金属氧化物的合成及非均相Fenton催化降解染料废水的研究

发布时间：2018-03-11 00:26

本文选题：非均相Fenton催化剂　切入点：介孔碳　出处：《天津工业大学》2016年硕士论文　论文类型：学位论文

【摘要】：介孔材料作为一种新型的纳米材料,具有较大的比表面积和孔体积,规则整齐且可调的孔道结构。基于这些优点,介孔材料在处理染料废水去除难生物降解有机物方面受到了极大的关注。本文致力于介孔碳和介孔硅材料的制备及改性研究,旨在制备出非均相Fenton催化降解亚甲基蓝染料的高效催化剂。规则介孔碳材料表面亲水性较低,利用过氧化氢处理材料引进含氧官能团,增强碳材料的亲水性和酸性,使其在溶液中分散更加均匀,促进催化剂与溶液中有机物分子的接触,由此增加非均相Fenton催化反应进程。使用双金属负载介孔硅材料,由于双金属的协同作用,使得此类催化剂在非均相Fenton催化降解染料过程中表现出较高的降解速率。本文具体研究内容如下：1.使用F127为模板剂,酚醛树脂为碳源,硝酸铁为铁源,利用螯合剂共组装的方法制备出铁负载介孔碳材料Fe/meso-C,并使用过氧化氢修饰(标记为H-Fe/meso-C),通过XRD、TEM、SEM口N：吸附-脱附等温线表征可以看出,催化剂可以保持整齐有序的三维立体孔道结构,较大的比表面积和孔体积。经过过氧化氢修饰后,材料的表面积,孔体积和孔径均有所增大,表明材料经过过氧化氢对碳基材料的刻蚀,使得孔径扩大,更有利于非均相Fenton催化反应的顺利进行。2.使用低温镁热反应合成介孔硅材料,再经过硬模板法制备出双金属铁铜负载的介孔硅材料Fe-Cu@MPSi,通过XRD、TEM和N2吸附-脱附等温线表征可以看出,催化剂在保持整齐有序的三维立体孔道结构的基础上,又新增一些不规则的孔道结构,使得介孔硅材料表现出比原料SBA-15更大的比表面积和孔体积。而硅作为一种半导体,电子可以在材料上自由传递,使得金属离子更容易变换价态,从而提高非均相Fenton降解效果。同时在材料上负载铁铜双金属不仅可以增加催化活性位点数量,同时双金属的协同作用也使得金属离子可以快速变换价态,从而加速非均相Fenton反应的快速进行。
[Abstract]:As a new type of nano-materials, mesoporous materials have large specific surface area and pore volume, regular and adjustable pore structure. The preparation and modification of mesoporous carbon and mesoporous silicon materials have attracted great attention in the treatment of dyestuff wastewater and the removal of difficult biodegradable organic compounds. A highly efficient catalyst for the degradation of methylene blue dyes catalyzed by heterogeneous Fenton was prepared. The surface hydrophilicity of regular mesoporous carbon materials was low. Oxygen functional groups were introduced into the materials treated with hydrogen peroxide to enhance the hydrophilicity and acidity of carbon materials. The catalyst is more evenly dispersed in the solution, which promotes the contact between the catalyst and the organic molecules in the solution, thus increasing the process of heterogeneous Fenton catalytic reaction. Using bimetallic supported mesoporous silicon material, due to the synergistic effect of bimetallic, The results show that this kind of catalyst has a high degradation rate in heterogeneous Fenton catalytic degradation of dyes. The specific contents of this paper are as follows: 1. Using F127 as template, phenolic resin as carbon source, iron nitrate as Tie Yuan, Iron supported mesoporous carbon materials Fe / meso-C were prepared by chelating agent co-assembly and modified with hydrogen peroxide (labeled H-Fe / meso-Con). The results were obtained by the characterization of XRDX / TM SEM port N: adsorption-desorption isotherm. After hydrogen peroxide modification, the surface area, pore volume and pore size of the catalyst increased. The results show that the pore size of the carbon-based materials is enlarged by hydrogen peroxide etching, which is more favorable to the smooth progress of heterogeneous Fenton catalytic reaction. 2. Mesoporous silicon materials are synthesized by low temperature magnesium thermal reaction. Bimetallic Fe-CuMPSi-supported mesoporous silicon material Fe-CuMPSiwas prepared by hard template method. By means of XRDX TEM and N2 adsorption-desorption isotherms, it can be seen that the catalyst is based on the well-ordered three-dimensional pore structure. In addition, some irregular pore structures are added, which make the mesoporous silicon material exhibit larger specific surface area and pore volume than raw material SBA-15. As a semiconductor, silicon can transfer electrons freely on the material, making metal ions change valence state more easily. Therefore, the degradation efficiency of heterogeneous Fenton can be improved. At the same time, loading iron and copper bimetallic on the material can not only increase the number of catalytic active sites, but also make metal ions change valence state rapidly by the synergistic action of bimetallic ions. Thus accelerating the rapid progress of heterogeneous Fenton reaction.
【学位授予单位】：天津工业大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O643.36

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