稀土掺杂纳米TiO_2的制备、性能及机理研究
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摘要
本项研究以超声波-溶胶-凝胶法制备了Y3+、La3+掺杂TiO2粉体与薄膜,探讨了胶凝过程的主要影响因素与动力学,获得了优化的制备工艺条件。应用XRD、SEM、TEM、EDAX、FT-IR、UV-vis等现代测试手段对样品的组成、结构与性能进行了表征。基于实验、测试并结合理论分析,对稀土掺杂的机理进行了探讨。结果表明：稀土掺杂纳米材料具有锐钛矿相结构,晶粒度在18nm以下,稀土离子主要以稀土氧化物(RE2O3)形式均匀分布在TiO2晶格中,稀土掺杂引起了TiO2光学吸收边的“红移”。以铀酰离子与甲基橙为对象,系统地探讨了稀土掺杂纳米材料的吸附性能与吸附机理,结果表明稀土掺杂纳米材料具有很强的吸附能力,吸附动力学符合Lagergren准二级反应模型,吸附等温式都符合Langmuir方程,为物理吸附与化学吸附共同作用的结果。稀土离子掺杂降低了TiO2晶格中空穴和电子重新复合的几率,稀土掺杂纳米材料对甲基橙的降解在紫外光与可见光下均表现出良好的光催化活性；光催化降解过程符合Langmuir-Hinshelwood拟一级动力学模型与Langmuir方程。稀土掺杂薄膜在紫外光与可见光下也具有良好的光生亲水性,是薄膜表面的污染物光催化降解与薄膜表面结构改变共同作用的结果。
Y3+ and La3+ doped TiO2 powders and films were prepared through ultrasonic-sol-gel method. The primary influence factor of gelling process was investigated and the optimum technological conditions were obtained. The composition, structure and performance of the obtained material were characterized by XRD、SEM、TEM、EDAX、FT-IR and UV-vis. The results showed that the crystalling phase of rare-earth ion doped nanomaterials had the similar structure of anatase, and the particle sizes of these materials were less than 18nm. Rare-earth ions were dispersed uniformly in the crystal lattice of TiO2 in the form of rare-earth oxide (RE2O3). In addition, rare-earth ion doping also resulted in the red shift of the optical absorption edge of TiO2. Based on the experiment and test results and the theoretical analysis, the mechanism of rare-earth ion doping was investigated detailedly. The adsorption performance and mechanism to UO22+ and methyl orange adsorbed by rare-earth ion doped nanomaterials were investigated systematically. The results indicated that Y3+ and La3+ doped TiO2 powders and films exhibited excellent adsorbability, and the adsorption dynamics was in a good accordance with the law of the pseudo-second-order model of Lagergren. The adsorption isotherm fitted the Langmuir equation well. The adsorption mechanism was confirmed to be the combined action of physisorption and chemisorption. Owing to rare-earth ion doping, the compounding probability of electron and cavity was decreased in the crystal lattice of TiO2. Rare-earth ion doped nanomaterials exhibited favorable photocatalysis activity for the degradation of methyl orange under ultraviolet and visible light. The process of photo-catalytic degradation was in line with the law of the pseudo-first-order model of Langmuir-Hinshelwood and Langmuir equation. Y3+ and La3+ doped TiO2 films also possessed favorable photo-induced hydrophilicity under ultraviolet and visible light, which mostly attributed to the coaction of photo-catalytic degradation and the change of film surface structure.
Y3+ and La3+ doped TiO2 powders and films were prepared through ultrasonic-sol-gel method. The primary influence factor of gelling process was investigated and the optimum technological conditions were obtained. The composition, structure and performance of the obtained material were characterized by XRD、SEM、TEM、EDAX、FT-IR and UV-vis. The results showed that the crystalling phase of rare-earth ion doped nanomaterials had the similar structure of anatase, and the particle sizes of these materials were less than 18nm. Rare-earth ions were dispersed uniformly in the crystal lattice of TiO2 in the form of rare-earth oxide (RE2O3). In addition, rare-earth ion doping also resulted in the red shift of the optical absorption edge of TiO2. Based on the experiment and test results and the theoretical analysis, the mechanism of rare-earth ion doping was investigated detailedly. The adsorption performance and mechanism to UO22+ and methyl orange adsorbed by rare-earth ion doped nanomaterials were investigated systematically. The results indicated that Y3+ and La3+ doped TiO2 powders and films exhibited excellent adsorbability, and the adsorption dynamics was in a good accordance with the law of the pseudo-second-order model of Lagergren. The adsorption isotherm fitted the Langmuir equation well. The adsorption mechanism was confirmed to be the combined action of physisorption and chemisorption. Owing to rare-earth ion doping, the compounding probability of electron and cavity was decreased in the crystal lattice of TiO2. Rare-earth ion doped nanomaterials exhibited favorable photocatalysis activity for the degradation of methyl orange under ultraviolet and visible light. The process of photo-catalytic degradation was in line with the law of the pseudo-first-order model of Langmuir-Hinshelwood and Langmuir equation. Y3+ and La3+ doped TiO2 films also possessed favorable photo-induced hydrophilicity under ultraviolet and visible light, which mostly attributed to the coaction of photo-catalytic degradation and the change of film surface structure.
引文
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