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题名: Cu0、Cu(2-x)O(x=0,1)/TiO2复合光催化材料的合成及其对2,4-二氯酚降解性能的研究
作者: 王贞
答辩日期: 2014-05-26
导师: 王传义
专业: 材料物理与化学
授予单位: 中国科学院大学
授予地点: 北京
学位: 硕士
关键词: 二氧化钛 ; 零价铜 ; 氧化亚铜 ; 氧化铜 ; 光催化 ; 2,4-二氯酚
摘要: 资源,环境和人类社会的可持续发展将成为二十一世纪的重大课题。随着人口的急剧增长和社会经济的高速发展,人们对水的需求量不断增加,许多国家和地区都面临着水资源短缺的危机,与此同时,水污染日益严重。因此,研究高效环保降解有毒有害污染物,治理水体污染的技术已成为国际上广泛关注的重大课题。光催化技术以其该法以其操作简单、氧化能力强、非选择性地降解有机污染物、无二次污染及可直接利用太阳光等独特性能,成为解决这一问题的最有应用潜力的途径之一,已成为该领域的研究热点。
TiO2作为比较理想的半导体光催化材料,因其无毒、成本低、具有良好的化学稳定性和耐光腐蚀性,成为最具潜力的光催化剂。然而,由于TiO2的禁带宽度为3.2eV,只对紫外光产生响应,而太阳光中紫外光仅占2%,TiO2量子产率低,光谱响应范围窄,这严重阻碍了其实际应用。通过对TiO2进行改性,如和窄带隙半导体复合、贵金属沉积、过渡金属离子掺杂、有机染料敏化等方法,以拓宽二氧化钛的光谱响应范围,提高其对太阳光的利用率,增强光催化效率。
本论文主要通过原位水解的方法,分别将Cu、Cu2O和CuO与TiO2进行复合,得到了Cu/TiO2、 Cu2O/TiO2和 CuO/TiO2复合光催化材料,达到了对TiO2改性、提高其光催化活性和拓宽光谱响应范围的目的。通过SEM、TEM、XPS、XRD等多种表征手段,研究了材料的结构、形貌及其光吸收特性,并且研究了三种材料对2,4-二氯酚的光催化降解行为,探讨了光催化机理。具体内容如下:
1、采用L-抗坏血酸作为还原剂的绿色方法,成功合成了稳定的零价铜Cu纳米颗粒,并且通过改变L-抗坏血酸的浓度合成了具有不同形貌的零价铜Cu纳米颗粒。在此基础上,利用原位水解法,成功将球形零价铜纳米颗粒与二氧化钛进行复合,制备了一系列不同质量比的Cu0@TiO2核壳结构复合光催化材料。通过扫描电子显微镜、透射电子显微镜、紫外–可见漫反射光谱、X−射线光电子能谱和能量色散X射线光谱对该复合物的组成、形貌、光吸收性质进行了表征;通过其在紫外-可见光和可见光下对2,4-二氯酚的降解,研究了其光催化活性及机理。研究结果表明,在紫外-可见光下,零价铜含量为0.5%对2,4-二氯酚的降解效率可以达到99.89%,几乎完全降解;在可见光下,零价铜含量为3%对2,4 -二氯酚的降解效率达到90.31%。
2、成功合成了具有立方结构的Cu2O纳米颗粒,通过原位水解的方法,将其和二氧化钛进行复合,得到了Cu2O/TiO2复合光催化材料。通过扫描电子显微镜、X-射线衍射、紫外-可见漫反射光谱对该复合物的组成、形貌、光吸收性质进行了表征;对比研究了Cu2O纳米颗粒和Cu2O/TiO2复合光催化材料在可见光及紫外-可见光下对2,4-二氯酚的光催化降解性能,探讨了光催化机理。研究结果表明,无论在紫外-可见光还是可见光下,Cu2O/TiO2复合光催化材料的光催化活性都优于Cu2O纳米颗粒,在可见光下光照8小时,Cu2O/TiO2复合物对2,4-二氯酚的降解效率达到92.37%;在紫外-可见光下光照3小时,Cu2O/TiO2复合物对2,4-二氯酚的降解效率为68.6%。
3、利用水热法制备得到CuO纳米颗粒,通过原位水解的方法,将其和二氧化钛进行复合,得到了CuO/TiO2复合光催化材料。通过扫描电子显微镜、透射电子显微镜和X−射线光电子能谱对该复合物的组成、形貌、光吸收性质进行了表征;对比研究了CuO纳米颗粒和CuO/TiO2复合光催化材料在可见光及紫外-可见光下对2,4-二氯酚的光催化降解性能,探讨了光催化机理。研究结果表明,无论在紫外-可见光还是可见光下, CuO/TiO2复合光催化材料的光催化活性都优于CuO纳米颗粒,在可见光下光照8小时, CuO/TiO2复合物对2,4-二氯酚的降解效率达到82.03%;在紫外-可见光下光照3小时, CuO/TiO2复合物对2,4-二氯酚的降解效率为46.52%。
英文摘要:
Resource, environment and sustainable development of human society will be the major task in twenty-first century. With the rapid increase of population and rapid development of social economy, people’s demand for water keeps increasing. Many countries and regions have to face the crisis of water resource shortage, at the same time, water resource pollution to be seriously day by day. Therefore, study of technology for remedying environmental pollution which can degrade the poisonous and harmful pollutants efficiently and environmentally has already become a major subject which has drawn international attention. Photocatalysis technology has characters of simple operation, strong oxidation, non-selective degradation of organic pollutants, no secondary pollution and use the sunlight directly, so it has become one of the most potential applications to solve this problem and become a research focus in this field. TiO2 as the ideal semiconductor photocatalytic materials because of its non-toxic, low cost, good chemical stability and light corrosion resistance has been the most potential photocatalytic material. However, because the band gap of TiO2 is 3.2 eV and only response to the UV light whichaccounts for only a small fraction (2%) of the sun's energy, low quantum yield and narrow spectral response range of TiO2 hinder its practical application seriously. In order to broaden the spectral response rangeof TiO2, improve its utilization rate for sunlight and strengthen the photocatalytic efficiency, there are some ways used to modified the TiO2 for example coupled narrow-band semiconductor, noble metal deposition, transition metal ion doping, organic dye sensitization and so on. This paper mainlycontained following works, Cu/TiO2、 Cu2O/TiO2 and CuO/TiO2photocatalytic materials were obtained by coupled Cu、Cu2O and CuO with TiO2through in-situ hydrolysis, respectively. The material’s structure morphology and properties of optical adsorption were studied by SEM, TEM, XPS, DRS and XRD; morefore, the degradation behavior for three materials has been studied, the. 2,4 -DCP was selected as a model pollutantin this work.photocatalytic mechanismhas also been discussed. Specific content as follows: 1 the stable zero-valence copper nanoparticles were successfully synthesised by green method with L-ascorbic acid as reducing agent, and the zero-valence copper nanoparticles with different morphologies were synthesised by changing the concentration of L-ascorbic acid. On this basis, by coupling copper nanoparticles with titanium, a series of Cu0@TiO2core-shell photocatalytic materials were obtained with different mass ratio. SEM, TEM, UV-Vis, XPS and EDX were employed to characterizethe composition, morphology, property of light absorption of this compound. Photocatalytic activity and mechanism were studied through the degradation of 2,4-dichlorophen under UV-Vis light and visible light. The research result shows that degradation efficiency of 2, 4-dichlorophen can reach 99.89% under UV- Vis ligh was 0.5%t when the content of copper nanoparticles, meanwhile the degradation efficiency can reach 90.31% under visible light when the content of copper nanoparticles was 3%. 2 Cu2O nanoparticles with cubic structure were successfully synthesized.On this basis, by coupling Cu2O nanoparticleswith titanium, Cu2O/TiO2 compound photocatalytic materialswere obtained. SEM, XRD as well as UV-Vis were employedtocharacterizethe composition, morphology, property of light absorption of this compound. Photocatalytic activity and mechanism were studiedthrough the degradation of 2, 4-dichlorophen under UV-Vis light and visible ligh.The research result shows that photocatalytic activity of Cu2O/TiO2 compound is better than Cu2Onanoparticles whether under UV- Vis light or visible light.The degradation efficiency of 2, 4-dichlorophen can reach 68.6% underUV- Vis light in 3 hours, meanwhile the degradation efficiency can reach 92.37%under visible light in 8 hours. 3 CuO nanoparticles were successfully synthesized byhydrothermal method. On this basis, by coupling CuO nanoparticles with titanium, CuO/TiO2 compound photocatalytic materials were obtained. SEM, TEM as well as XPS were employedtocharacterizethe composition, morphology, property of light absorption of this compound.Photocatalytic activity and mechanism were studiedthrough the degradation of 2,4-dichlorophen under UV-Vis light and visible light. The research result shows that photocatalytic activity of CuO/TiO2 compound is better than CuO nanoparticles whether under UV- Vis light or visible light. The degradation efficiency of 2,4-dichlorophen can reach 46.52%under UV- Vis light in 3 hours, meanwhile the degradation efficiency can reach 82.03%under visible light in 8 hours.
内容类型: 学位论文
URI标识: http://ir.xjipc.cas.cn/handle/365002/3415
Appears in Collections:环境科学与技术研究室_学位论文

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作者单位: 中国科学院新疆理化技术研究所

Recommended Citation:
王贞. Cu0、Cu(2-x)O(x=0,1)/TiO2复合光催化材料的合成及其对2,4-二氯酚降解性能的研究[D]. 北京. 中国科学院大学. 2014.
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