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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 吳乃立(Nae-Lih Wu) | |
dc.contributor.author | Yun-Hsiang Shen | en |
dc.contributor.author | 沈運祥 | zh_TW |
dc.date.accessioned | 2021-05-20T21:14:03Z | - |
dc.date.available | 2011-02-20 | |
dc.date.available | 2021-05-20T21:14:03Z | - |
dc.date.copyright | 2011-02-20 | |
dc.date.issued | 2011 | |
dc.date.submitted | 2011-02-10 | |
dc.identifier.citation | 1. M. R. Hoffmann, S. T. Martin, W. Y. Choi, D. W. Bahnemann, 'Environmental applications of semiconductor photocatalysis', Chemical Reviews; 95, 69-96 (1995).
2. A. Wold, 'Photocatalytic properties of TiO2', Chemistry of Materials; 5, 280-283 (1993). 3. X. Chen, H. Y. Zhu, J. C. Zhao, Z. T. Zheng, X. P. Gao, 'Visible-light-driven oxidation of organic contaminants in air with gold nanoparticle catalysts on oxide supports', Angewandte Chemie-International Edition; 47, 5353-5356 (2008). 4. D. Li, W. J. Dong, S. M. Sun, Z. Shi, S. H. Feng, 'Photocatalytic degradation of acid chrome blue k with porphyrin-sensitized TiO2 under visible light', Journal of Physical Chemistry C; 112, 14878-14882 (2008). 5. C. Yogi, K. Kojima, T. Takai, N. Wada, 'Photocatalytic degradation of methylene blue by Au-deposited TiO2 film under UV irradiation', Journal of Materials Science; 44, 821-827 (2009). 6. T. Y. Wei, C. C. Wan, 'Kinetics of photocatalytic oxidation of phenol on TiO2 surface', Journal of Photochemistry and Photobiology a-Chemistry; 69, 241-249 (1992). 7. A. Fujishima, K. Honda, 'Electrochemical photolysis of water at a semiconductor electrode', Nature; 238, 37-38 (1972). 8. O. M. Alfano, D. Bahnemann, A. E. Cassano, R. Dillert, R. Goslich, 'Photocatalysis in water environments using artificial and solar light', Catalysis Today; 58, 199-230 (2000). 9. A. G. Agrios, P. Pichat, 'State of the art and perspectives on materials and applications of photocatalysis over TiO2', Journal of Applied Electrochemistry; 35, 655-663 (2005). 10. J. M. Herrmann, 'Heterogeneous photocatalysis: State of the art and present applications', Topics in Catalysis; 34, 49-65 (2005). 11. A. L. Linsebigler, G. Q. Lu, J. T. Yates, 'Photocatalysis on TiO2 surfaces: Principles, mechanisms, and selected results', Chemical Reviews; 95, 735-758 (1995). 12. A. Fujishima, K. Hashimoto, T. Watanabe, 'TiO2 photocatalysis fundamentals and application', BKC, Inc. (1999). 13. 'Phase diagrams for ceramists figure', The American Ceramic Society, Inc. 4150-4999 (1975). 14. U. Diebold, 'The surface science of titanium dioxide', Surface Science Reports; 48, 53-229 (2003). 15. A. Mills, S. Lehunte, 'An overview of semiconductor photocatalysis', Journal of Photochemistry and Photobiology a-Chemistry; 108, 1-35 (1997). 16. Y. Nosaka, M. A. Fox, 'Kinetics for electron-transfer from laser-pulse-irradiated colloidal semiconductors to adsorbed methylviologen. Dependence of the quantum yield on incident pulse width', Journal of Physical Chemistry; 92, 1893-1897 (1988). 17. J. M. Herrmann, 'Heterogeneous photocatalysis: Fundamentals and applications to the removal of various types of aqueous pollutants', Catalysis Today; 53, 115-129 (1999). 18. A. Hagfeldt, M. Gratzel, 'Light-induced redox reactions in nanocrystalline systems', Chemical Reviews; 95, 49-68 (1995). 19. E. Pelizzetti, C. Minero, V. Maurino, H. Hidaka, N. Serpone, R. Terzian, 'Photocatalytic degradation of dodecane and of some dodecyl derivatives', Annali Di Chimica; 80, 81-87 (1990). 20. L. M. Yang, L. E. Yu, M. B. Ray, 'Photocatalytic oxidation of paracetamol: Dominant reactants, intermediates, and reaction mechanisms', Environmental Science & Technology; 43, 460-465 (2009). 21. X. H. Huang, I. H. El-Sayed, W. Qian, M. A. El-Sayed, 'Cancer cell imaging and photothermal therapy in the near-infrared region by using gold nanorods', Journal of the American Chemical Society; 128, 2115-2120 (2006). 22. D. W. Chen, A. K. Ray, 'Photodegradation kinetics of 4-nitrophenol in TiO2 suspension', Water Research; 32, 3223-3234 (1998). 23. K. Hofstadler, R. Bauer, S. Novalic, G. Heisler, 'New reactor design for photocatalytic wastewater treatment with TiO2 immobilized on fused-silica glass-fibers: Photomineralization of 4-chlorophenol', Environmental Science & Technology; 28, 670-674 (1994). 24. A. Mills, S. Morris, 'Photomineralization of 4-chlorophenol sensitized by titanium dioxide: A study of the initial kinetics of carbon dioxide photogeneration', Journal of Photochemistry and Photobiology a-Chemistry; 71, 75-83 (1993). 25. G. Alsayyed, J. C. Doliveira, P. Pichat, 'Semiconductor-sensitized photodegradation of 4-chlorophenol in water', Journal of Photochemistry and Photobiology a-Chemistry; 58, 99-114 (1991). 26. L. C. Chen, T. C. Chou, 'Kinetics of photodecolorization of methyl orange using titanium dioxide as catalyst', Industrial & Engineering Chemistry Research; 32, 1520-1527 (1993). 27. M. C. Lu, G. D. Roam, J. N. Chen, C. P. Huang, 'Factors affecting the photocatalytic degradation of dichlorvos over titanium dioxide supported on glass', Journal of Photochemistry and Photobiology a-Chemistry; 76, 103-110 (1993). 28. Y. Inel, A. N. Okte, 'Photocatalytic degradation of malonic acid in aqueous suspensions of titanium dioxide: An initial kinetic investigation of CO2 photogeneration', Journal of Photochemistry and Photobiology a-Chemistry; 96, 175-180 (1996). 29. K. Okamoto, Y. Yamamoto, H. Tanaka, A. Itaya, 'Kinetics of heterogeneous photocatalytic decomposition of phenol over anatase TiO2 powder', Bulletin of the Chemical Society of Japan; 58, 2023-2028 (1985). 30. R. W. Matthews, 'Photooxidation of organic impurities in water using thin films of titanium dioxide', Journal of Physical Chemistry; 91, 3328-3333 (1987). 31. R. Terzian, N. Serpone, 'Heterogeneous photocatalyzed oxidation of creosote components: Mineralization of xylenols by illuminated TiO2 in oxygenated aqueous media', Journal of Photochemistry and Photobiology a-Chemistry; 89, 163-175 (1995). 32. E. Hutter, J. H. Fendler, 'Exploitation of localized surface plasmon resonance', Advanced Materials; 16, 1685-1706 (2004). 33. K. Awazu, M. Fujimaki, C. Rockstuhl, J. Tominaga, H. Murakami, Y. Ohki, N. Yoshida, T. Watanabe, 'A plasmonic photocatalyst consisting of sliver nanoparticles embedded in titanium dioxide', Journal of the American Chemical Society; 130, 1676-1680 (2008). 34. M. Haruta, T. Kobayashi, H. Sano, N. Yamada, 'Novel gold catalysts for the oxidation of carbon monoxide at a temperature far below 0℃', Chemistry Letters; 405-408 (1987). 35. M. Valden, X. Lai, D. W. Goodman, 'Onset of catalytic activity of gold clusters on titania with the appearance of nonmetallic properties', Science; 281, 1647-1650 (1998). 36. M. S. Chen, D. W. Goodman, 'The structure of catalytically active gold on titania', Science; 306, 252-255 (2004). 37. D. Vione, C. Minero, V. Maurino, A. E. Carlotti, T. Picatonotto, E. Pelizzetti, 'Degradation of phenol and benzoic acid in the presence of a TiO2-based heterogeneous photocatalyst', Applied Catalysis B-Environmental; 58, 79-88 (2005). 38. B. Balamurugan, T. Maruyama, 'Evidence of an enhanced interband absorption in Au nanoparticles: Size-dependent electronic structure and optical properties', Applied Physics Letters; 87, (2005). 39. V. Augugliaro, L. Palmisano, A. Sclafani, C. Minero, E. Pelizzetti, 'Photocatalytic degradation of phenol in aqueous titanium dioxide dispersions', Toxicological and Environmental Chemistry; 16, 89-109 (1988). 40. C. G. Silva, J. L. Faria, 'Effect of key operational parameters on the photocatalytic oxidation of phenol by nanocrystalline sol-gel TiO2 under UV irradiation', Journal of Molecular Catalysis a-Chemical; 305, 147-154 (2009). | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/10250 | - |
dc.description.abstract | 本研究的目的是想探討利用Au/TiO2對於工業廢水內常見的有機物苯酚進行光催化降解反應,並且觀察中間產物的濃度分佈與選擇性的變化,以及侷域性表面電漿共振 (LSPR) 效應是否可顯著地提升反應速率。
本研究分為三大部分。第一部分是用300 nm的紫外光源對苯酚的兩種不同的初始濃度 (250 ppm or 150 ppm) 分別進行光催化降解反應,結果發現苯酚的反應速率常數幾乎不受初始濃度影響。第二部分則是探討溫度效應對於P25與2.0 wt% Au/P25催化活性的影響,我們發現當溫度由32℃上升到38℃時,苯酚的反應速率常數不升反降。之後將反應溫度提高到55℃時,苯酚的反應速率常數也只有略微提升,推測原因可能與吸附步驟是速率決定步驟有關。第三部分是將300 nm紫外光與575 nm可見光燈管同時打開,觀察Au/TiO2的LSPR效應是否會對反應速率造成顯著的影響。結果發現苯酚的反應速率常數有略為提升,中間產物的部分雖然速率常數提升有限,經過與只照可見光的對照組比較,我們覺得LSPR效應應該有助於提升反應速率。 | zh_TW |
dc.description.abstract | The purpose of this research is to apply Au/TiO2 for the photocatalytic degradation reaction of phenol, a commonly found organic compound in industrial wastewater, and to observe the concentration profiles as well as the selectivity of the intermediates. In addition, we want to investigate whether Localized Surface Plasmon Resonance (LSPR) effect can enhance the reaction rate.
This research is divided into three parts. First, we illuminated the phenol solution with 300 nm UV light only. The initial concentration of phenol solution is 250 ppm and 150 ppm, respectively. We found that the reaction rate constant of phenol was nearly independent of the initial concentration. The second part is to explore the temperature effect on the kinetics when using P25 and 2.0 wt% Au/P25 as the catalyst, individually. We observed that when the reaction temperature increased from 32℃ to 38℃, the reaction rate constant of phenol dropped. Even when we elevated the reaction temperature to 55℃, the reaction rate constant of phenol only slightly increased. We suppose that it is because the adsorption step rather than the surface reaction step is the rate-determining step. The third part is to illuminate the phenol solution with 300 nm UV and 575 nm visible light at the same time. The reaction rate constant of phenol became a little larger when applying dual light sources. As for the mono-hydroxylated intermediates, although the increase in the reaction rate constant was not obvious, when compared with the data obtained by illuminating the solution with UV light only, we believe that LSPR must promote the overall reaction rate of the photocatalytic degradation reaction of phenol. | en |
dc.description.provenance | Made available in DSpace on 2021-05-20T21:14:03Z (GMT). No. of bitstreams: 1 ntu-100-R97524029-1.pdf: 1853972 bytes, checksum: d77aa1075c029e7f93bcccfd5adfa7bc (MD5) Previous issue date: 2011 | en |
dc.description.tableofcontents | 摘要...I
Abstract...II Table of Contents...IV List of Figures...VII List of Tables...XII Chapter 1 Introduction...1 1-1 Background...1 1-2 Motivations and Objectives...1 Chapter 2 Literature Review...3 2-1 An Introduction of Titanium Oxide, TiO2...3 2-1-1 Fundamental Properties...3 2-1-2 Principles of Photocatalysis...9 2-1-3 Mechanisms of Photocatalysis...13 2-1-4 Formation of Hydroxyl Radicals...16 2-1-5 Applications of TiO2 to Photocatalysis...17 2-2 Photocatalytic Oxidation of Phenol...18 2-2-1 Comparison of the Toxicity of the Reactant and Intermediates...19 2-2-2 Effect of Reaction Temperature...19 2-3 Localized Surface Plasmon Resonance (LSPR)...21 2-3-1 Introduction of LSPR...21 2-3-2 Gold Nanoparticles...24 Chapter 3 Experimental...25 3-1 Chemical Reagents and Experimental Instruments...25 3-1-1 Chemical Reagents...25 3-1-2 Experimental Instruments...27 3-2 Photocatalytic Reaction...29 3-2-1 Preparation of Gold Catalysts...29 3-2-2 Schema of Photochemical Reactor...30 3-2-3 Fundamental Experiments...32 3-3 Analyses and Characterization...34 3-3-1 X-ray Diffraction (XRD)...34 3-3-2 High-resolution Transmission Electron Microscopy (HRTEM)...35 3-3-3 UV-Vis Spectrophotometer (UV-Vis)...35 3-3-4 High-performance Liquid Chromatography (HPLC)...36 3-3-5 Kinetic Analyses...36 3-3-6 Solving ODEs with 4th-Order Runge-Kutta Method...40 Chapter 4 Results and Discussion...41 4-1 Characterization of Gold on P25...41 4-1-1 XRD Analyses...41 4-1-2 UV-Vis Analyses...42 4-1-3 TEM Analyses...43 4-1-4 Mieplot Simulation...46 4-2 Photocatalytic Oxidation of Phenol...48 4-2-1 Adsorption of Phenol in Dark Surrounding...48 4-2-2 Effect of P25 (TiO2) Powder Content in Solution...49 4-2-3 Effect of Initial Concentration and the Amount of Gold on P25...52 4-2-4 Effect of Temperature...54 4-2-5 Possible Mechanism...61 4-2-6 Model Fitting-Initial Concentration Effect...62 4-2-7 Model Fitting-Temperature Effect...67 4-2-8 Visible Light Effect...73 Chapter 5 Conclusion...79 Reference ...81 Appendix A...86 | |
dc.language.iso | en | |
dc.title | 利用Au/TiO2在紫外及可見光下降解苯酚水溶液的反應之研究 | zh_TW |
dc.title | Photocatalytic Degradation of Phenol Solution in the Presence of Au/TiO2 Catalyst under the Irradiation of UV and Visible Light | en |
dc.type | Thesis | |
dc.date.schoolyear | 99-1 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 萬本儒(Ben-Zu Wan),吳紀聖(Jeffrey Chi-Sheng Wu) | |
dc.subject.keyword | 二氧化鈦,Au/TiO2,苯酚,光催化降解反應,侷域性表面電漿共振, | zh_TW |
dc.subject.keyword | Titanium dioxide,Au/TiO2,Phenol,Photocatalytic degradation reaction,Localized Surface Plasmon Resonance (LSPR), | en |
dc.relation.page | 90 | |
dc.rights.note | 同意授權(全球公開) | |
dc.date.accepted | 2011-02-10 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
顯示於系所單位: | 化學工程學系 |
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