溶胶溶胶- -凝胶法论文:凝胶法论文:Sol-gelSol-gel 法制备金属掺杂的多孔硅、铝法制备金属掺杂的多孔硅、铝氧化物复合材料氧化物复合材料【中文摘要】介孔 SiO2 材料比表面积较大、孔道大小均匀、孔径可在 2nm 至 50nm 范围内连续调节等特性,使其在分离提纯、生物材料、催化、环境、能源、新型组装材料(或作为纳米反应器制备具有特殊光、电、磁等性能的新型纳米材料等)等领域具有多种潜在的用途,尤其是在生物医学方面如蛋白质固定分离、生物芯片、生物传感器、药物的包埋和控释等具有广阔的应用前景本论文以高分子化合物为模板剂,采用了溶胶凝胶法(Sol-gel)和溶胶凝胶-水热法合成介孔 SiO2 及其金属氧化物掺杂介孔 SiO2 复合材料,详细研究了高分子模板、掺杂金属、煅烧温度等反应条件对产物孔结构的影响规律,初步探讨了其在吸附去除有机染料方面的应用,论文工作包括以下几部分:第一章运用高分子化合物聚乙二醇(PEG)作为模板剂,利用 Sol-gel 法合成出了介孔 SiO2 以及金属氧化物掺杂的复合材料,主要考察了制备过程中 PEG 分子量长度、PEG 质量、金属掺杂量、煅烧温度等条件对材料孔结构的影响。
实验结果表明:可根据 PEG 的分子量、浓度及链的长短进行调节介孔材料的介相结构,一般来讲 PEG 分子量对复合材料的孔结构影响不大,材料的SABETa、Vtot 数值随着 PEG 质量的增加而增加;SiO2 中由于金属氧化物的掺杂使得复合材料的比表面积孔容和孔径减小,可能是氧化物占据了孔道,形成了 Si-O-M 化学键,从而提高了材料的热稳定和水热稳定性;另外考察了煅烧温度的影响,温度过低有机物去除不完全,温度过高可能使得硅骨架坍塌,实验证明 550℃是最佳煅烧温度第二章使用 Sol-gel 法直接合成了 CuO/SiO2 复合材料,采用 X 射线衍射(XRD),N2 等温吸附-脱附法,傅立叶变换红外光谱(FT-IR),高分辨透射电镜(HRTEM)等手段对合成的样品进行表征实验结果表明过渡金属的掺杂引入基本没有改变 SiO2 的骨架,一部分金属离子进入到 Si02 骨架中形成了 M-O-Si 键,形成的 CuO 晶相小颗粒占据了部分孔道,使得材料的比表面积有所下降第三章通过溶胶凝胶-水热法制备了铜的氧化物复合材料,并研究了对有机染料亚甲基蓝的吸附作用实验结果表明 CuO/SiO2 多孔复合材料对亚甲基蓝有良好的吸附效果,在吸附剂(Cs-600-6-15-NaOH-11-12h-140)用量是0.015g,体系 pH=9,搅拌时间为 2h 的条件下,对亚甲基蓝的去除率高达 97.17%。
实验结果表明,以 PEG 为模板,通过溶胶凝胶法可以方便地制备出介孔二氧化硅及其金属掺杂的复合材料,通过 PEG 分子量、添加质量等反应条件可以调节、控制复合材料的孔结构特征,还可以有效地将无机金属氧化物引入到 Si02 骨架中形成 M-O-Si 化学键,赋予介孔二氧化硅新的物理化学特性,制备出多功能的介孔复合材料,广泛的应用于吸附、催化等相关领域英文摘要】Mesoporous SiO2 has some unique structural characteristics such as extremely high surface area、narrow poer size distribution and large adjustable pore sizes (2-50nm), which have made such materials become the researching focus of porus materials. They could have potential application in various fields especially in adsorption and separation, ion exchange, catalysis, molecular host, optoelectronic, photonic devices, sensing, drug delivery and so on.In this paper, mesoporous silica and its metallic oxide doped composite materials were synthesized by sol-gel and hydrothermal methods, using polyethylene glycol (PEG) as template. The influences of reaction condition, such as molecular weight and addation ratio of PEG, doping metal ions, calcination temperature, on porous structure were investigated in details. The application in adsorption of organic dyes in wastewater was studied. The thesis includes the following sections:First, sol-gel method was employed to synthesize mesoporous silica and its metallic oxide doped composites using nonionic surfactants PEG as template. The influence of PEG molecular length and weight, metallic doping amount, calcination temperature on the mesoporous structure of composites was investigated. The results showed that mesoporous structure could be regulated by the molecular weight and concentrations of PEG and length of chains. Generally, molecular weight had few influence on mesoporous structure, however, SABET and Vtot increased with the increment of PEG mass. The pore volume and specific surface of doped composites decreased owing to some metallic oxide occupied pore channel. Chemical bonds of Si-O-M were formed which enhanced the thermal and hydrothermal stability of composites. In addition, influence of calcination temperature was also studied, the organtic could’t be get ride of completely at low temperature and porous framework of silicon collapsed at high temperature. The results showed that the optimum temperature was 550℃.Second, CuO/SiO2 composite was prepared by sol-gel method, the samples were characterized by XRD, N2 isothermal adsorption-desorption method, fourier transform infrared spectroscopy (FTIR), high resolution transmission electron microscopy (HRTEM) and so on. The results showed that: the introduction of CuO didn’t change the framework of SiO2; the bonds of Si-O-M were formed; the specific surface of material declined as a result of small particles of CuO crystal occupying pore channel partially.Third, CuO/SiO2 composites were synthesized by sol-gel-hydrothermal method. The adsorption of methylene blue (MB) was studied. The results showed that CuO/SiO2 mesoporous composite had good absorbability of MB. The maximum removal rate reached 97.17% in the condition that the pH value was 9,0.015g sorbent (Cs-600-6-15-NaOH-11-12h-140) was added.As a whole, the experimental resultes showed that the mesoprous SiO2 and metal ions doped mesoporous SiO2 composite could prepared by sol-gel method and hydrothermal route using PEG as template. The mesoporous structure could be regulated by the molecular weight and concentrations of PEG and length of chains. Inorganic metal oxide could be introduced into the framework of with the formation of Si-O-M bonds which endow mesoporous SiO2 composite with new physical and chemical properties. The multifunctional mesoporous composites could have a wide application at the fileds of adsorption catalysis.【关键词】溶胶-凝胶法 介孔 复合材料 掺杂 水热 吸附【英文关键词】Sol-gel hydrothermal composites mesoporous adulterate/doping adsorption【目录】Sol-gel 法制备金属掺杂的多孔硅、铝氧化物复合材料 摘要 3-5 Abstract 5-6 。