溶胶-凝胶法论文：Sol-gel法制备金属掺杂的多孔硅、铝氧化物复合

溶胶-凝胶法论文：Sol-gel法制备金属掺杂的多孔硅、铝氧化物复合材料

【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3-59-23含义9-10

Abstract5-6

第一章 绪论

1.1.1 纳米科学的

1.2 纳米

1.1 纳米结构材料概述9-10

1.1.2 纳米材料的独特性能10

SiO_2特征及制备方法10-1410

1.2.1 纳米SiO_2的结构和特征

1.2.3 负载金属

1.2.3.1 1.2.3.3 微

1.2.2 介孔SiO_2的制备方法10

氧化物的硅基介孔材料制备方法及其意义10-13Sol-gel法11-12

1.2.3.2 水热合成法12

乳液法12-1313

1.2.3.4 机械球磨法131.2.3.5 沉淀法1.3 纳米材料

1.3.2 1.4.1

1.2.4 影响介孔材料性质因素13-14

生成机理以及应用14-16纳米材料的应用15-16非硅基介孔材料研究16-17多孔材料17

1.3.1 生成机理14-151.4 存在的问题16-17

1.4.2 借助计算机功能辅助研究

1.5 国内外

1.4.3 探索材料的新性能17

纳米结构材料前景展望17-1818-19

参考文献19-23

1.6 选题意义及研究思路第二章 Sol-Gel法制备介孔

2.1 引言

SiO_2及其氧化物-介孔二氧化硅复合材料23-4123-24242626-27

2.2 实验部分24-262.2.2 实验过程24-262.3 结果与讨论26-38

2.2.1 主要试剂和原料2.2.3 试样表征2.3.1 介孔二氧化硅

2.3.3

2.3.2 介孔Al_2O_3-SiO_2的制备27-31

2.3.4 介孔2.4 本章小结

介孔MgO-Al_2O_3-SiO_2的制备31-34MnO-MgO-Al_2O_3-SiO_2的制备34-3838-39

参考文献39-41

第三章 Sol-gel法制备铜的氧

3.1 引言

化物与多孔硅、铝氧化物复合材料41-5641-4242

3.2 实验部分42-433.2.2 样品制备42-43

3.2.1 实验原料3.2.3 表征43

3.3 3.3.2 XRD

结果与讨论43-52分析44-4546-49

3.3.1 FT-IR分析43-44

3.3.3 TEM分析45-463.3.4 BET分析

3.4

3.3.5 合成Cu_2O/SiO_2复合材料49-52

结语52-53参考文献53-56第四章 溶胶凝胶-水热法

制备氧化铜掺杂硅铝氧化物复合材料及其对亚甲基蓝的吸附研究56-6957-59

4.1 引言56-57

4.2 实验步骤

4.2.2 CuO/SiO_2纳

4.2.1 主要试剂和原料57

米复合材料的制备过程57亚甲基蓝吸附实验57-59与讨论59-66

4.2.3 CuO/SiO_2纳米复合材料对4.2.4 试样表征59

4.3 结果

4.3.1 溶胶凝胶-水热法制备介孔

4.3.2 CuO/SiO_2复合材料对4.4 本章小结66-67附录70

参考

CuO-MgO-Al_2O_3-SiO_259-64亚甲基蓝的吸附研究64-66文献67-69

致谢69-70

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