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过渡金属取代多金属氧酸盐的合成、表征及其光催化性质研究

Research on Synthesis, Charaterization and Photocatalytic Activity of Transition Metal Substitute of Polyoxometalates

【作者】 王立平

【导师】 高丽华;

【作者基本信息】 北京工商大学 , 环境工程, 2010, 硕士

【摘要】 随着工业化的发展,各种危及人类生存的有害物质越来越多地进入环境中,特别是工业染料废水的大量增加使水体污染问题更加突出。一些有毒有机污染物,由于它们的浓度低、结构稳定、并且难生物降解,用常规的污水处理方法很难除去。光催化降解法是近三十年来发展起来的废水处理新方法,具有运行稳定、处理效果好、无二次污染等特点。本论文合成了8种组成为Kn[PW9V2O39Z(H2O)](Z = Zn、Cd、Cr、Mn、Fe、Ni、Co、Cu)的过渡元素取代的磷钨系列杂多配合物,此系列化合物经过与修饰后的树脂负载后又制备了8种杂多配合物复合催化材料(简写为PW9V2Z/Resin)(Z = Zn、Cd、Cr、Mn、Fe、Ni、Co、Cu)。并利用红外光谱、紫外-可见吸收光谱、X射线粉末衍射、扫描电镜和X射线光电子能谱一系列分析手段对制备的16种杂多配合物催化材料剂进行了分析测定和表征。结果表明:所合成的过渡元素取代的系列杂多配合物仍然具有Keggin型结构;复合材料是通过Z-N配位键与修饰后的载体键合。以罗丹明B为模拟有机染料污染物,采用合成的16种过渡元素取代的磷钨系列杂多配合物及其复合材料为光催化剂,通过改变光照时间、催化剂种类、催化剂浓度以及pH值等因素催化条件,进行了紫外光照射下对罗丹明B溶液的光催化降解进行了研究。研究结果表明:过渡元素取代的磷钨系列杂多配合物具有良好的催化活性,最高降解率达到92%;均相体系中,8种催化剂的催化效果均在80%以上;非均相体系中,在60min内,最高降解率达到70%。

【Abstract】 With the fast industrial development, kinds of hazardous pollutants have entered environment. Especially the great increase of industrial wastewater that underlined the pollution in aqueous environment and jeopardized the environment critically. Due to their low concentration, stable structure, and being difficult to degrade biologically, some poisonous organic pollutants can hardly be removed by traditional method. Photocatalytic degradation, a new method of disposing wastewater developed in recent thirty years, features stable reaction, good degradation effect, and non-secondary pollution.This paper synthesized eight phosphotungstic series of heteropoly complexes, which are substituted by the transition elements composing Kn[PW9V2O39Z(H2O)] (Z = Zn, Cd, Cr, Mn, Fe, Ni, Co, Cu). When such series of compounds and the modified sign are loaded, eight heteropoly complexes of compound catalytic materials (abbreviation as PW9V2Z/Resin) (Z = Zn, Cd, Cr, Mn, Fe, Ni, Co, Cu) were produced. In addition, we carried out analytical determination and characterization for the 16 heteropoly compound catalytic material agents by a series of analytical methods such as Infrared spectroscopy, UV - visible absorption spectroscopy, X-ray powder diffraction analysis, scanning electron microscopy and X-ray photoelectron spectroscopy. The results show that the synthesized heteropoly compound series remain as Keggin-type structure; Composite materials are bonded with the modified load through the Z-N coordination bond.This paper studied photocatalytic degradation for Rhodamine B solution under UV irradiation on the condition that Rhodamine B is taken as model organic dye pollutants, which used synthetic 16 kinds phosphotungstic series of heteropoly complexes and composite materials as photocatalyst, by changing the illumination time, catalyst type, catalyst concentration and pH, and other factors catalytic conditions. The results show that phosphotungstic series of heteropoly compounds which are substituted by the transition elements have good catalytic activity, and the maximum degradation rate is up to 92%; the catalytic effects of eight kinds are more than 80% under homogeneous system; the maximum degradation rate is up to 70% in 60min under non-homogeneous system.

【关键词】 杂多酸盐罗丹明B光催化降解负载
【Key words】 polyoxometalatesrhodamine Bphotocatalysisresinload
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