TiO2-SiO2复合气凝胶的常压干燥制备及光催化降解含油污水活性

Photocatalytic activity of monolithic TiO2-SiO2 composite aerogels obtained by ambient drying for degrading oily wastewater

  • 摘要: 以钛酸四丁酯和正硅酸乙酯为原料,利用溶胶凝胶工艺制备出不同硅含量的TiO2-SiO2复合醇凝胶.结合老化液浸泡和小孔干燥工艺,在常压下干燥得到完整的TiO2-SiO2复合气凝胶块体.采用扫描电子显微镜、BET比表面积测试、X射线粉末衍射等测试手段对复合气凝胶的微观结构和物化性能进行了测试和表征.测试结果表明,复合气凝胶具有良好的性能,Ti和Si元素在气凝胶中分布均匀.随着SiO2含量的增加,复合气凝胶的密度逐渐变小,比表面积增大,孔隙率增加,转变为锐钛矿相的相变温度升高.经高温煅烧晶化处理,复合气凝胶转变为锐钛矿相结构.以乳化后的渤海原油水溶液作为含油污水模拟溶液,测试了复合气凝胶对含油污水的催化降解性能.污水降解结果显示复合气凝胶对渤海原油污水具有较好的催化降解活性.在SiO2摩尔分数低于30%时,随着硅含量的增加,复合气凝胶的光催化降解率升高;但当SiO2摩尔分数高于30%后,继续增加SiO2掺入量,反而造成复合气凝胶催化能力下降.对于SiO2摩尔分数为30%的复合气凝胶,获得了最佳的催化降解效果,90 min催化降解率达95%.

     

    Abstract: TiO2-SiO2 composite aerogels with different contents of SiO2 were synthesized through a sol-gel route with tetrabutyl titanate and tetraethyl orthosilicate as the raw materials. In combination with solution aging and pinhole drying processes, monolithic TiO2-SiO2 composite aerogels were prepared via ambient drying, and their microstructure and the physicochemical properties were studied by scanning electron microscopy, BET method and X-ray diffraction analysis. It is found that the composite aerogels have low density, high specific surface area and show uniform element distribution of Ti and Si. With the increase of SiO2 content, the density of the composite aerogels decreases gradually, the specific surface area and the porosity increase, and the phase transition temperature to anatase rises. By calcination at high temperature, the composite aerogels change into anatase structure. The photocatalytic properties of the calcined samples were investigated by degradation experiments of the aqueous emulsion of crude oil from the Bohai Sea. The experimental results show that the photocatalytic degradation efficiency of the calcined sample increases with the mole fraction of SiO2 increasing till 30%, but it decreases when the mole fraction of SiO2 is above 30%. The best photocatalytic performance is acquired when the calcined sample contains 30% SiO2, with the catalytic degradation efficiency for 90 min being up to 95%.

     

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