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1、沈阳理工大学硕士学位论文 摘 要 本文填装具有光催化作用的粒子电极组成三维电极体系，微弧氧化二氧化钛为三维电极体系的主电极阳极，阳极为微弧氧化5min的钛基（钛网）TiO2/Ti膜，阴极为同等面积的钛网。以Na2SO4溶液为体系支持电解质溶液，20W紫外灯（=253.7nm）为光电催化光源，目标降解物为亚甲基蓝模拟染料废水。三维电极体系中，粒子电极采用溶胶-凝胶制备方法，以钛酸丁酯作钛源、乙醇作溶剂、浓盐酸作催化剂，经过热处理得到，TiO2/GAC和TiO2/-Al2O3。 通过考察三维粒子电极光电催化降解亚甲基蓝模拟染料废水的影响因素，包括粒子电极煅烧温度、负载膜层数、粒子配比、电源电压、亚
2、甲基蓝溶液初始浓度、Na2SO4电解质溶液浓度、电极间距等，探讨得出以下结论： （1）TiO2/GAC 与 GAC 混合粒子三维电极体系 优化条件因素后的三维电极体系，光电催化 3h 能够达到 75.32%，实验结果表明，体系的主电极 TiO2/Ti 网与 TiO2/GAC 在紫外光的照射下均发生光催化作用，TiO2/GAC 与 GAC 的吸附性能能够大大增强其光催化作用， 在外加电压的作用下，体系发生电化学反应，整个光催化与电催化协同作用使得光电催化作用效果明显。 另外， 对 TiO2/GAC 粒子进行了改性， 掺杂了稀土元素并考察其光电催化活性，发现掺杂有利于抑制晶粒生长，能够提高催化剂的
3、光电催化活性，实验表明掺杂铕（Eu）的催化效果最佳。 （2）球状 TiO2/-Al2O3与铁屑混合粒子三维电极体系 优化条件因素后的三维电极体系，光电催化 3h 能够达到 60.39%。实验结果表明，球状 TiO2/-Al2O3与铁屑粒子充当第三电极后，促进了该反应体系对亚甲基蓝的降解率，TiO2/-Al2O3粒子电极，具有光催化活性，与铁屑组成的粒子组合，TiO2/-Al2O3充分发挥了 TiO2的光催化作用，又充当绝缘体增强铁屑的电催化作用，二者有机结合实现光电催化的协同作用，同时，铁屑内电解的作用，使电极内部发生 Fenton 反应，生成 Fenton 试剂，进而加速了有机污染物的吸附及
4、降解速度。 沈阳理工大学硕士学位论文 （3）颗粒 TiO2/-Al2O3粒子与铁屑三维光电体系 优化条件因素后的三维电极体系，光电催化 3h 能够达到 76.17%。与第二个体系相比较，填充物质极其类似，反应也比较类似，实验结果表明，由于负载后的颗粒 TiO2/-Al2O3比球状 TiO2/-Al2O3性质有所改善， 并且其粒径与铁屑粒径相同，使得铁屑与绝缘粒子充分混合，提高了三维电极的复极性光电催化效率，比第二个体系最后降解率有一定的提高。 （4）颗粒 TiO2/-Al2O3粒子与 GAC 三维光电体系 优化条件因素后的三维电极体系，光电催化 3h 能够达到 72.48%。实验结果表明，该体
5、系中 GAC 与颗粒 TiO2/-Al2O3粒子吸附性能使得 TiO2/-Al2O3充分发挥光催化作用，二者充分混合，共同构成复极性三维电极体系，发挥电化学性能，TiO2/-Al2O3粒子的添加，增加了 GAC 的电催化作用，从而形成光电协同反应体系，提高了该体系三维光电催化效率。 四个体系比较最后得出结论，二氧化钛光电催化效率在三维电极体系有显著的提高，微弧氧化钛基（钛网）TiO2/Ti 膜与负载 TiO2的粒子电极，在紫外光的照射下充分发挥光催化作用，而与三维电极的电催化结合，具有协同作用，最终确定三维光电体系的光电催化效率远高于不填装粒子电极同条件下的传统二维电极体系。 关键词：光电催化
6、；微弧氧化；三维电极；TiO2 沈阳理工大学硕士学位论文 Abstract In this paper, filling with catalysis of particle electrode composed of three dimensional electrode system. TiO2 was loaded with the GAC and -Al2O3 by sol-gel method, combining with regulated power supply make up the three-dimensional electrode photoelectrocatal
7、ysis system. Titanium oxide coatings (TiO2/Ti) were formed on the titanium surface by micro-arc oxidation (MAO) in Na3PO4 solution with the concentration of 8g/L. And using the TiO2/Ti as anod electrode( micro-arc oxidation time is 5min), the titanium as counter electrode in the system of three-dime
8、nsional electrode. The photoelectrocatalysis system use Na2SO4 aqueous solution as supporting electrolyte, and UV lamp (20W, =253.7nm) as the illuminant. The photoelectrocatalytic ability of titanium oxide coatings were evaluated by photoelectrocatalytic degradation of methylthionine chloride aqueou
9、s solution. In the sol-gel method, using tetrabutyl titanate as precursor, alcohol as solvent, and HCl as catalyst. After heat treatment, TiO2/GAC and TiO2/-Al2O3 were the loading-particle electrode. In this paper, theres some influence factors had been studied about photoelectrocatalysis degradatio
10、n of methylthionine chloride simulate dye wastewater. Such as particle electrode calcining temperature, load membrane layer, particle ratio, power supply voltage, initial concentration of methylene blue solution, Na2SO4 electrolyte solution concentration, electrode gap and so on. There are the concl
11、usions: (1)Under the best experiment condition, the system have the best efficiency, with the degradation of 75.32% after 3 hours. This three-dimension electrode system filling with GAC and the GAC /TiO2 mixed particles have the high-efficiency degradation. System of main electrode TiO2/Ti nets and
12、GAC/TiO2 electrodes all happened photocatalysis under the uv irradiation. TiO2/GAC and GAC electrodes have the big adsorption property, and that increase the photocatalysis property, under the action of an external voltage, the system occurred electrochemical reactions. Moreover, doping rare-earth e
13、lement to TiO2/GAC can improve the photoelectrocatalysis activity for its restrained the growing of crystalline grain. 沈阳理工大学硕士学位论文 Experiments show that doped Eu catalytic having the best result. (2) Under the best experiment condition, the system have the best efficiency, with the degradation of 6
14、0.39% after 3 hours. This three-dimension electrode system filling with globular TiO2/-Al2O3 and scrap iron mixed particles have the high-efficiency degradation. When the globular TiO2/-Al2O3 and scrap iron particles as the third electrod, the reaction system of methylene blue degradation rates was
15、promoted. The TiO2/-Al2O3 particles have the photocatalytic activity, and then the photocatalytic activity increased obviously after mixed with scrap iron, And it acting as an insulator increase the scrap iron electrocatalysis role. Moreover, scrap iron within the role of electrolysis, and that gene
16、rate Fenton reagents in the Fenton reaction. Further accelerate the speed of adsorption and degradation of organic pollutants. (3) Under the best experiment condition, the system have the best efficiency, with the degradation of 76.17% after 3 hours. This three-dimension electrode system filling with granule TiO2/-Al2O3 and scrap iron mixed particles have the high-efficiency degradation. Comparing with the second system, filling material is extremely similar, reaction
