复合式半导体光催化材料的制备及性能的研究
摘要
本论文主要针对宽能隙半导体进行复合或是修饰来提高光催化效率这一目的开展了研究工作。首先,从纳米粒子丰富的表面态能级所带来的子能隙吸收这个侧面进行光催化的研究,通过表面金属阳离子的修饰将这种子能隙吸收扩大,并能够有效的促进电子空穴对分离。其次,制备了二氧化钛包裹银纳米粒子同时负载于蒙脱土表面的复合光催化材料。并与其他材料在光降解细菌方面进行比较,本复合材料效果更佳,使用寿命更长。我们进一步研究了金属银与二氧化钛的复合,制备了由银和二氧化钛纳米粒子共同组成的亚微米空心球。主要探索了此复合体系在紫外光照射下二氧化钛激发的电子扩散到银纳米粒子中并被储存的性能。最后,制备了TiO2/Ag2S的核壳纳米粒子,通过红外光激发光催化氧化乙醛溶液来证明这样一个假设:只要能够完成光激发电子被吸附在半导体表面的氧气分子俘获并形成超氧离子这个过程,就可以实现光催化氧化反应,不论被激发的半导体能级如何分布。
Since the end of 1960s,Fujishima and Honda discovered the photoinduced decomposition of water on TiO2 electrode, semiconductor photocatalysts have attracted much interest. However,to date,there is no one kind of semiconductor can avoid all the drawback in photocatalytic application, even the widely used TiO2. Energy band is too wide to absorb photon in visible light; poor separation of the photoinduced electrons and holes result in the low photocatalytic efficiency; photo-corrosion limits the use of photocatalyst; the conduction band or the valence band of semiconductor does not match the energy level that a specific photocatalytic reaction needs. Therefore, the composite semiconductor photocatalyst are synthesized to solve these problems. That is enhancement of performance by the so-called semiconductor modification, in order to it more suitable for the photocatalytic reaction.
In this paper, the research focuses on the wide-bandgap semiconductor for compositing or modification to improve the photocatalytic efficiency. First, we synthesized metal cations modified cubic zirconia nanoparticles through one-step solvothermal method at low temperature. The photocatalytic studies was processed on the field of rich sub-bandgap absorption which caused by the surface state energy levels of nanoparticles, and the sub-bandgap absorption was expanded through surface modification of metal cations, furthermore, the electron hole pairs were separated more effectively by modification. The surface photovoltage and surface photocurrent measurements were used to test the influence of surface cations modification on sub-bandgap absorption and transitions, and the cationic modification on reducing the grain boundary resistance was investigated too. Moreover, the effect of different metal cations has also been investigated. At the same time came the introduction of theoretical calculations, in order to better explore the mechanisms involved.
Second, the montmorillonite (MMT) supported TiO2 coated Ag nanoparticles composite photocatalytic materials were prepared by solvothermal method. For this composite material, the plasmon effects of Ag nanoparticles can generate electron hole pairs under visible light, smaller nanoparticles of TiO2 can be more effective for the catalytic reaction after excitation, TiO2 coat structure on Ag can reduce the loss of silver, the MMT is conducive to recovery of catalyst. Comparison with other materials, in photo-degradation of bacteria, the effect of this composite material is better and longer.
The Ag and TiO2 composite was further studied, sub-micron hollow spheres composed of Ag and TiO2 nanoparticles were prepared by solvothermal method. In such a composite system, the excited electrons of TiO2 under UV irradiation would diffuse to the silver nanoparticles, and can be stored for a long time. In visible light irradiation, the electron of surface plasmon excitation of silver will be injected into the conduction band of TiO2 to enhance separation of electron hole pair, and increase carrier lifetime, improving photocatalysis. Above all the phenomenon can be observed by surface photovoltage. Degradation of acetaldehyde was carried out in dark to apply the stored energy under UV.
Finally, through research and summarize previous literature, we made a assumption that, as long as the photo excited electrons are trapped by oxygen molecules adsorbed on the semiconductor surface, and forming superoxide ions, the photocatalytic oxidation can be achieved, regardless of the energy level distribution of the photo-excited semiconductor. To prove this hypothesis, we prepared core-shell TiO2/Ag2S nanoparticles, and test its photocatalytic oxidation properties on acetaldehyde solution under infrared light. The core-shell structure is in purpose of preventing photocorrosion of Ag2S and the effective separation of carrier.
Since the end of 1960s,Fujishima and Honda discovered the photoinduced decomposition of water on TiO2 electrode, semiconductor photocatalysts have attracted much interest. However,to date,there is no one kind of semiconductor can avoid all the drawback in photocatalytic application, even the widely used TiO2. Energy band is too wide to absorb photon in visible light; poor separation of the photoinduced electrons and holes result in the low photocatalytic efficiency; photo-corrosion limits the use of photocatalyst; the conduction band or the valence band of semiconductor does not match the energy level that a specific photocatalytic reaction needs. Therefore, the composite semiconductor photocatalyst are synthesized to solve these problems. That is enhancement of performance by the so-called semiconductor modification, in order to it more suitable for the photocatalytic reaction.
In this paper, the research focuses on the wide-bandgap semiconductor for compositing or modification to improve the photocatalytic efficiency. First, we synthesized metal cations modified cubic zirconia nanoparticles through one-step solvothermal method at low temperature. The photocatalytic studies was processed on the field of rich sub-bandgap absorption which caused by the surface state energy levels of nanoparticles, and the sub-bandgap absorption was expanded through surface modification of metal cations, furthermore, the electron hole pairs were separated more effectively by modification. The surface photovoltage and surface photocurrent measurements were used to test the influence of surface cations modification on sub-bandgap absorption and transitions, and the cationic modification on reducing the grain boundary resistance was investigated too. Moreover, the effect of different metal cations has also been investigated. At the same time came the introduction of theoretical calculations, in order to better explore the mechanisms involved.
Second, the montmorillonite (MMT) supported TiO2 coated Ag nanoparticles composite photocatalytic materials were prepared by solvothermal method. For this composite material, the plasmon effects of Ag nanoparticles can generate electron hole pairs under visible light, smaller nanoparticles of TiO2 can be more effective for the catalytic reaction after excitation, TiO2 coat structure on Ag can reduce the loss of silver, the MMT is conducive to recovery of catalyst. Comparison with other materials, in photo-degradation of bacteria, the effect of this composite material is better and longer.
The Ag and TiO2 composite was further studied, sub-micron hollow spheres composed of Ag and TiO2 nanoparticles were prepared by solvothermal method. In such a composite system, the excited electrons of TiO2 under UV irradiation would diffuse to the silver nanoparticles, and can be stored for a long time. In visible light irradiation, the electron of surface plasmon excitation of silver will be injected into the conduction band of TiO2 to enhance separation of electron hole pair, and increase carrier lifetime, improving photocatalysis. Above all the phenomenon can be observed by surface photovoltage. Degradation of acetaldehyde was carried out in dark to apply the stored energy under UV.
Finally, through research and summarize previous literature, we made a assumption that, as long as the photo excited electrons are trapped by oxygen molecules adsorbed on the semiconductor surface, and forming superoxide ions, the photocatalytic oxidation can be achieved, regardless of the energy level distribution of the photo-excited semiconductor. To prove this hypothesis, we prepared core-shell TiO2/Ag2S nanoparticles, and test its photocatalytic oxidation properties on acetaldehyde solution under infrared light. The core-shell structure is in purpose of preventing photocorrosion of Ag2S and the effective separation of carrier.
引文
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