【作者】 杨帆；

【导师】 江学良；

【作者基本信息】 武汉工程大学 ， 材料学， 2010， 硕士

【摘要】 三维有序大孔材料作为一种重要的功能材料被广泛应用于催化、过滤、吸附等领域,其制备方法有许多,如溶胶-凝胶法、电化学沉积法、化学气相沉积法、共沉积法等。而溶胶-凝胶法因其操作简便,工艺较简单,产物纯度较高成为制备三维有序大孔材料最经济实用的方法。TiO₂本身具有高的光催化活性,在环保领域具有广阔的应用前景,为了进一步提高TiO₂的光响应性,对TiO₂的掺杂改性也是目前的研究热点。三氧化二钇（Y₂O₃）也是一种优良的材料,在许多高技术领域也有广泛的应用。本文通过溶胶-凝胶法制备了TiO₂和Y₂O₃微球,并进行掺杂改性制备了硫元素和钇元素掺杂的TiO₂微球及采用异相凝聚法制备聚苯乙烯/TiO₂有机-无机核壳结构的复合微球。主要工作如下:1.采用两阶段种子乳液聚合法制备了单分散P（St-AA）微球并利用自组装技术制备了胶体晶体大球。研究了反应温度、单体用量等对单体转化率和乳胶粒粒径的影响。结果表明:当AA含量占单体总含量的5 wt%时,制备的P（St-AA）聚合物微球单分散性最好,分散系数为3.8%。利用含羧基（5 wt%）的P（St-AA）制备的胶体晶体大球结构优于不含羧基的PSt微球制备的胶晶大球。2.采用溶胶-凝胶法制备了三维有序大孔TiO₂微球和三维有序大孔Y₂O₃微球。结果表明,用这种方法制备三维有序大孔材料是可行的。通过高温煅烧除去有机模板,大球呈现有序孔结构。另外,可以通过调整煅烧温度来控制大孔材料的晶型。当煅烧温度为500℃时,TiO₂为锐钛矿型,当煅烧温度为700℃时,为金红石型。经900℃煅烧的Y₂O₃出现完好衍射峰,表明Y₂O₃为纯相。3.采用微波法对TiO₂微球进行了S元素掺杂实验。采用煅烧法对TiO₂微球进行了Y元素掺杂实验。通过XPS和光催化性能分析测试,证明掺杂后的样品的光催化活性明显优于掺杂前的样品。通过XRD分析测试,表明微波法和煅烧法掺杂并不改变TiO₂晶型,S掺杂样品局部只发生微小畸变,Y掺杂样品衍射峰稍有宽化。4.采用异相凝聚法制备了P（St-AA）微球包覆TiO₂粉体和P（St-AA）微球包覆TiO₂大孔微球有机-无机复合材料。该复合材料的亲油性能有一定的提高。采用含氟的PS微球制备了含氟的有机壳层,期望制备得到为含氟有机多孔PS小球壳层包覆有序大孔TiO₂微球,得到壳-核有机-无机复合材料,广泛用于科研及产业化中。更多还原

【Abstract】 Three-dimensional ordered macroporous materials （3DOM） were applied widely in the fields of catalysis,filtration and adsorption, etc. There many preparation methods for 3DOM, for instance, sol-gel, electrochemical deposition, CVD and co-deposition. The sol-gel method has many advantages such as simple operation and process. In addition, the products which prepared by this method have high purity. So recently, sol-gel method is the way which can be most economical and practical. Furthermore, Titanium dioxide （TiO₂） has been extensively used for its catalytic properties as environmental protection. In order to improve the photocatalytic activity of TiO₂, the doped modification is one of the current research topics in this field. The yttrium oxide （Y₂O₃） is an excellent material which can be used in high-technology industry. The paper reviewed the sol-gel method, doped modification and heterocoagulation used in fabrication of the ordered TiO₂ balls, Y₂O₃ balls, S-doped TiO₂ balls, Y-doped TiO₂ balls and TiO₂/P（St-AA） core/shell composite balls. The main research contents and conclusions are listed as following parts:1. Monodispersed P（St-AA） latex particles were prepared by two-stage seed emulsion polymerization and photonic balls consisting of monodisperse polystyrene （PS） latex particles with carboxyl groups were prepared by using a suspension dispersed system through self-assembly technique. The effects of reaction parameters such as reaction temperature, monomer content on the conversion and size distribution of latex particles were studied. The conclusion indicated: when the concentration of AA based on all of monomers was 5wt.%, the size distribution coefficient reached the minimum value, 3.8%. In addition, the colloidal crystal balls structure was better prepared by P（St-AA） latex particles assembly.2. The three dimensional ordered macroporous TiO₂ balls and Y₂O₃ balls were obtained by sol-gel templating method. The conclusion indicated: this method to prepare three dimensional ordered materials was practicable.Through calcining in order to remove the organic template, the balls have orded pores. In addition, The crystalline type can be fully controllable by adjusting the calcinating temperature. When 500℃and 700℃were selected, anatase and rutile were presented in TiO₂ respectively. When 900℃was selected for Y₂O₃, the whole peak was appeared.3. S-doped TiO₂ can be prepared by microwave irradiation method. Y-doped TiO₂ can be prepared by calcinating method. Through the XPS and catalytic activity analysis, the photocatalysis activity of S-doped and Y-doped TiO₂ is superior to TiO₂ which is undoped. XRD analysis indicated that the two doped method. Only a little local distortion existed in S-doped TiO₂ and the broadening diffraction peak presented on Y-doped TiO₂.4. P（St-AA）/TiO₂ organic/inorganic composite balls can be prepared by heterocoagulation method. The lipophilicity of the composite balls can be improved through this modified method. Then the organic shell with fluorine PS microspheres can be fabricated. The organic porous PS shell with fluorine coated with ordered macroporous TiO₂ balls can be used widely in industrialization.更多还原