臺灣博碩士論文加值系統

本研究是以溶膠凝膠法製備二氧化鈦，希望透過製備方法中改變不同有機酸當催化劑，使其合成所得之二氧化鈦能摻有雜質(如碳或氮)，並利用空氣或氬氣的鍛燒方式，製備出具有可見光催化效果之光觸媒。進行光催化分解氮氧化合物之活性測試結果，顯示以醋酸為催化劑所得之二氧化鈦粉體，在空氣中以200℃鍛燒其可見光催化活性最佳，其在藍光部分NOx去除率達50%，綠光部分去除率達42%，至於紅光部分去除率亦高達35%。UV-vis光譜量測結果顯示，加入不同酸當催化劑有助於可見光吸收效果。FT-IR光譜分析與文獻資料之比對，可說明有機酸在gel生成過程中與鈦原子的鍵結情形。利用XPS檢測結果亦可探討其元素組成中含碳比例比市售光觸媒(UV100)多。本研究將在本文中詳細探討不同有機酸催化劑、鍛燒溫度、鍛燒氣氛與光催化分解氮氧化物其修飾效果而造成結構缺陷，具有可見光催化活性之原因。

In this research, we will discuss structure defect and photocatalytic activity under visible light of photocatalyst prepared by different catalyst of organic acid in the sol-gel process, calcined temperature, calcined atmosphere and the modification effect. We used sol-gel method to prepare titanium dioxide with some impurity like carbon or nitrogen and used different kind of organic acid for catalyst, the photocatalyst was calcined in air or argon to prepared photocatalytic activity under visible light. The titanium dioxide particle used acetic acid for catalyst and calcined in air at 200℃ had the best result of NOx degradation. The NOx remove ratio in blue light is 50%, in green light is 42% and in red light is promoted to 35%. The UV-visible spectrum showed that adding different kind of organic acid would help to improve absorption of visible light. The FT-IR spectrum showed organic acid bonded to the titanium during gel situation. Using the measurement of XPS showed the carbon ratio of element composition was more than common photocatalyst (UV100).

中文摘要••••••i
英文摘要••••••ii
誌謝••••••••iii
目錄••••••••iv
圖目錄••••••vi
表目錄••••••x
第一章、緒論•••••••1
1.1研究緣起•••••••1
1.2研究目的•••••••2
第二章、文獻回顧••••••3
2.1光催化作用•••••••3
2.2光催化原理•••••••4
2.3光觸媒應用•••••••6
2.4二氧化鈦簡介••••••7
2.5二氧化鈦製備方法•••••••12
2.6氮氧化合物(NOx)之光催化動力學•••••••21
2.7二氧化鈦光觸媒之改質•••••••••24
第三章、實驗部分•••••••27
3.1觸媒製備••••••••27
3.2觸媒鑑定分析•••••••33
3.3降解氮氧化合物氣體之活性測試(DeNOx)•••••••36
第四章、結果與討論•••••••40
4.1X光繞射分析•••••••40
4.2紫外光-可見光光吸收分析•••••••46
4.3傅立葉轉換紅外線光譜••••••••53
4.4化學分析電子能譜儀••••••••59
4.5熱重分析••••••••65
4.6場發射掃描式電子顯微鏡•••••••70
4.7降解氮氧化合物氣體之活性測試(DeNOx)••••••••76
第五章、結論••••••••89
參考文獻•••••••91

1. A. Fujishima and K. Honda, 1972, Nature vol.238, pp.37.
2. Sid Devahasdin, Chiun Fan, Jr., Kuyen Li, Daniel H. Chen., 2003, J. Photochem. Photobiol. A: Chem., vol.156, pp.161.
3. Sang Bum Kim, Sung Chang Hong, 2002, Appl. Catal. B: Environ., vol.35, pp.305.
4. Ammar Houas, Hinda Lachheb, Mohamed Ksibi, Elimame Elaloui, Chantal Guillard, Jean-Marie Herrmann, 2001, Appl. Catal. B: Environ., vol.31, pp.145.
5. Kayano Sunada, Toshiya Watanabe, Kazuhito Hashimoto, 2003, J. Photochem. Photobiol. A: Chem., vol.156, pp.227.
6. Linsebigler, A. L., Lu, G. and Yates, J. T. Jr., 1995, Chem. Rev. (Washington, D. C.), vol.95(3), pp.735.
7. 徐玉杜 , ”光觸媒介紹” , 工研院環安中心http://www.e-safety.com.tw/1_main/103_learning/1037_news/ens27/pdf/A2.pdf
8. A. Fujishima, K. Hashimoto, T. Watanabe, 1999, “TiO2 Potocatalysis fundamentals and application”, BKC, Inc.,
p125
9. Levin, E. M. and McMurdie, H. F. ase diagrams for ceramists（figures 4150-4999）, 1975, The Amer. Ceram. Soc., Inc., pp76
10. 高濂，鄭珊，張青紅，陳憲偉，2004，奈米光觸媒，五南出版社。
11. J. Livage, S. Doeuff, M. Henry and C. Sanchez , 1987, J. Non-Cryst. Solids., vol.89, pp.206.
12. K. Nakamoto, 1978, Infrarrd and Raman spcclra of Inorganic and Coordination Compounds., Wiley, 3rd ed., New York.
13. K. H. Von Thiele and M. Panse, 1978, Z. Anorg. Allg. Chem., vol.441, pp.23.
14. S. Doeuff, J. Livage, M. Henry and C. Sanchez , 1990, J. Non-Cryst. Solids., vol. 92, pp.26.
15. J. Livage, in ” Sol-Gel Science and Technology”, eds. by M. A. Aegeter, M. Jr. Jafelicci, D. F. Souza and E. D. Zanotto, 1989,World Sci., Singapore, pp.103.
16. Y. Murakami, T. Matsumoto and Y. Takasu, 1999, J. Phys. Chem. B, vol.103, pp.1836.
17. J.S. Dalton, P.A. Janes, N.G. Jones, J.A. Nicholson, K.R. Hallam, G.C. Allen, 2002, Environ. Pollution, vol.120, pp. 415
19. R. Asahi, T. Morikawa, T. Ohwaki, K. Aoki, Y. Taga, 2001, “Hydrolysis of Titanium Alkoxides: Modification of The Molecular Precursor by Acetic Acid”, Science, vol. 293(13), pp.206.
20. C. Burda, Y. Lou, X. Chen, Anna C. S. Samia, 2003, John Stout, and James L. Gole, Nano Lett., vol. 3, No.8, pp. 1049.
21. Shahed U. M. Khan, Mpfareh Al-Shahry, 2002, William B. Inglter Jr., Sci., vol. 297, pp.2243.
22. T. Ohno, T. Tsubota, M. Toyofuku and Ryoji Inaba, 2004, Catal. Lett., vol. 98, No.4, pp.255
23. K. Baba, R. Hatada, 2001, Surf. Technol., vol. 136, pp.241.
24. Y. Choi, T. Umebayashi, M. Yoshikawa, 2004, J. Mater. Sci., vol. 39, pp.1837.
25. Hiroshi Irie, Yuka Watanabe, and Kazuhito Hashimoto, J. Phys. Chem. B, vol.107, pp.5483.
26. D. Noguchi, Y. Kawamata and T. Nagatomo, 2005, J. Electrochem. Soc., vol. 152, No.9, pp.D124-D129
26. Ming Shen, Zunyi Wu, Hui Huang, Yukou Du, Zhigang Zou, Ping Yang, 2006, Mater. Lett., vol.60, pp.693.
27. M.E. Rincon, M.E. Trujillo-Camacho, A.K. Cuentas-Gallegos, 2005, Catal. Today, vol.107-108, pp.606.
28. Y. Li, Doo-Sun Hwang, Nam Hee Lee, Sun-Jae Kim, 2005, Chem. Phys. Lett., vol.404, pp.25
29. Ming Shen, Zunyi Wu, Hui Huang, Yukou Du, Zhigang Zou, Ping Yang, 2006, Mater. Lett., vol.60, pp.693
30. Shanmugasundaram Sakthivel,Horst Kisch, 2003, Chem. Int.Ed., vol.42, pp.4908.
31. Yao-Hsuan Tseng, Chien-Sheng Kuo, Chia-Hung Huang1,Yuan-Yao Li, Po-Wen Chou, Chia-Liang Cheng and Ming-ShowWong, 2006, Nanotechnol., vol.17, pp.2490.
32. 陳建志，2004，可見光應答型光觸媒製備及催化活性研究，國立清華大學，碩士論文。
33. 土卞田博史(Taoda Hiroshi)，2003，光觸媒圖解，張晶、楊健，商周出版社。
34. 李聖文，2006，以碳氮摻雜法改質光觸媒及其光催化活性研究，國立清華大學，碩士論文。
35. 2001，維基百科全書(http://en.wikipedia.org/wiki.)。