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纳米TiO2的合成及其对酞酸酯类污染物的降解

Synthesis of Nanocrystalline Titania and Photocatalytic Degradation of Phthalate Esters

【作者】 初人合

【导师】 闫吉昌;

【作者基本信息】 东北师范大学 , 分析化学, 2005, 硕士

【摘要】 纳米 TiO2具有纳米粒子特有的表面效应、小体积效应、量子尺寸效应和宏观量子隧道效应等,并具有光催化活性较高、紫外线屏蔽性强、热导性好、分散性好等独特的性能,在化工、医药、航空航天及环境工程等众多领域具有重要的应用价值。而且,与其他 n 型半导体相比,TiO2毒性低,效果好。本文综述了国内外光催化氧化技术降解环境污染物的研究概况,在此基础上,采用多种方法如液相水解法、溶剂热法、模板法等合成了纳米级的 TiO2,并用 X 射线粉末衍射(XRD)、透射电子显微镜(TEM)、扫描电子显微镜(SEM)等进行了表征,筛选出成本低、操作简单的合成方法,即强迫水解法。对所合成的 TiO2进行了金属铁离子的掺杂研究。酞酸酯又称邻苯二甲酸酯,是一大类工业上广泛用作增塑剂的化合物,难以降解,因此是全球最普遍存在的环境污染物。它可通过饮水、进食、皮肤接触和呼吸等途径进入人体,有很大的危害性。本文对国内外目前为止设计和应用的光催化反应器进行了概述,首次选出自制简单易操作的装置研究了三种酞酸酯类化合物邻苯二甲酸二丁酯(DBP)、邻苯二甲酸二乙酯(DEP)、邻苯二甲酸二甲酯(DMP)的光催化降解性,考察了光照时间、催化剂用量、外加氧化剂、溶液 pH 值等因素对降解效率的影响。确定了最佳的条件为:H2O2的浓度为 0.05 mol/L,最佳降解 pH 值在 5.5 到 6.5 之间,最佳催化剂浓度为 0.8‰。结果表明水解法制备的 TiO2对此类化合物具有较好的降解效果,紫外灯照射一小时后降解率达到 90%以上,比目前通用的生物降解法降解时间和成本大大降低。最后通过 GC-MS法检测出的中间产物首次讨论了酞酸酯类化合物可能的降解途径。

【Abstract】 The photocatalytic degradation organic pollutant in the world was reviewed. The methods to degrade organic pollutants in wastewater and the application in wastewater treatment are also discussed. And nanometer titania was synthesisd by hydrolysis of TiCl4,sol-gel method, template method and solvent hydrothermal method and the best method: hydrolysis method, was selected. As a result, interesting shapes (shuttle-like, sphere with needles, uniform particles, belts and tubes) titania were prepared. This process simplification will lower production cost and make continuous process possible. The products were analyzed using X-ray diffractometer(XRD) , transmission electron microscopy(TEM) and scanning electron microscopy(SEM). The photocatalytic reactors designed and used were reviewed too. Phthalate esters(PAEs) are a group of compound. They are widely used as plasticiser and are enviroment contamination around the world. The photocatalyzed degradation of phthalate esters in aqueous suspensions of titanium dioxide has been investigated under a variety of conditions. The favorite conditions: c(H2O2)= 0.05mol/L, pH=5.56.5, c(catalyst)= 0.8‰. The degradation products were analyzed by GC–MS technique and probable pathways for the formation of these products are proposed.

  • 【分类号】O643.36
  • 【被引频次】1
  • 【下载频次】345
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