| 研究生: |
朱昱璋 YU-CHANG CHU |
|---|---|
| 論文名稱: |
二氧化鈦奈米管擔載金、鉑觸媒進行紫 |
| 指導教授: |
楊思明
Sze-Ming Yang |
| 口試委員: | |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 化學工程與材料工程學系 Department of Chemical & Materials Engineering |
| 畢業學年度: | 94 |
| 語文別: | 中文 |
| 論文頁數: | 77 |
| 中文關鍵詞: | 金觸媒 、氫 、甲醇 、奈米管 、二氧化鈦 |
| 外文關鍵詞: | TiO2, hydrogen, methanol, gold |
| 相關次數: | 點閱:8 下載:0 |
| 分享至: |
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本研究利用化學法(Chemical Method)將二氧化鈦製備成二氧化
鈦奈米管,比較不同鍛燒溫度對奈米管的成型與表面積的影響,並利
用沉澱固著法(Deposition Precipitation)和初濕含浸法將二氧化鈦擔載
金觸媒;利用光化學沉積法和沉澱固著法製備鉑觸媒,以不同晶相及
不同表面積的二氧化鈦擔載金屬觸媒在紫外光照射下進行甲醇重組
反應產生氫氣。利用XRD、TEM、BET 等不同鑑定方法分析所合成
的二氧化鈦奈米管之結構與表面積,並探討擔載金、鉑觸媒的反應特
性及觸媒活性。
結果顯示,化學法製備的二氧化鈦奈米管管外徑約12 奈米,內
徑8 奈米,長約數百奈米。沉澱固著法製備的二氧化鈦擔載金觸媒,
金顆粒呈半圓球型,顆粒大小約4~7 奈米,沉積於擔體表面或奈米管
中,而初濕含浸法製備的金觸媒其金顆粒大小分佈較為不均。比較光
化學沉積法與沉澱固著法製備的白金觸媒,發現光化學沉積法製備的
鉑觸媒,其擔體上的白金顆粒較沉澱固著法小。活性測試顯示,金觸
媒活性隨鍛燒溫度升高而降低,其中以200℃鍛燒後的金觸媒活性最
佳。而沉澱固著法製備的觸媒反應活性較初濕含浸法製備的觸媒好。
白金觸媒對甲醇重組產氫也有與金觸媒相同的效果,金屬顆粒越小將
會有越好的反應活性。
Titanium nanotubes were prepared from titanium powers by
treating with 10 M NaOH at 110~130℃ for 24 hours(Chemical method).
Excess NaOH was then neutralized with distilled water and HCl(aq). The
TiO2 nanotubes were characterized by X-ray diffraction (XRD), specific
surface area (BET), and transmission election microscope (TEM). Then
we prepare Au/TiO2, Pt/TiO2 by deposition precipitation and incipient
wetness methods. And we prepare Pt/TiO2 by photochemical deposition
method. We can evaluate the activities of these catalysts by hydrogen
production of methanol reforming under ultraviolet light (350nm)
irradiation. We use XRD, BET, and TEM to analyze various catalysts.
The TiO2 nanotubes were prepared by chemical method with inner
diameters of approximately 8 nm and outer diameters 12nm and 100 nm
lengths. The gold on the surface of TiO2 by deposition precipitation
method is hemisphere and the Au particles size is 4~7 nm. And we use
photochemical deposition method to prepare Pt/TiO2, the Pt particles size
is about 1nm. When Au/TiO2 and Pt/TiO2 were calcined at higher
temperature the particles size gets bigger. The catalytic activity is
strongly dependent on the gold and platinum particles size, the smaller
particles produces higher amount of hydrogen.
[1]Masatake Haruta, Yamada N, Kobayashi T, Sano H, Catalysis Letters
405(1987)
[2]Masatake Haruta, Masakazu Date, Applied catalysis A: General 222
427-437(2001)
[3]Salama T, Ohnishi R, Shido T, Ichikawa M, Chem.Commun.105(1997)
[4]E.E Stangland, K.N. Stavens, R.P. Andres, W.N. Delgass, Stud. Surf.
Sci. Catal.130 827(2000)
[5]F. Boccuzzi, A. Chiorino, M. Manzoli, D. Andreeva, T. Tabakova, L.
Ilieva, V. Iadakiev, Cataysis Today 75 169-175(2002)
[6]M. Date, Y. Lchihashi, T. Yamashita, A.Chiorino, F. Boccuzzi, M.
Haruta, Catalysis today 72 89-94(2002)
[7]S. Minico, S. Scire, C. Crisafulli, R. Maggiore, S. Galvagmo,
Applied catalysis B: Environmental 28 245(2000)
[8]Rodolfo Zanella, Catherine Louis, Suzanne Giorgio, Claude R. Henry,
Chae-Ho Shin, Journal of Catalysis 222,357(2004)
[9]M. T. Okumura, M. Haruta, Catalysts Today 74 265(2002)
[10]Misutaka Okumura, Susumu Tsubota, Masataka Haruta, Journal of
Molecular Catalysis A: Chemical 199 73–84 (2003)
[11]Tomoki Akita, Ping Lu, Koji Tanaka, Satoshi Ichikawa, Masatake
Haruta, Surface and Interface Analysis. 31 73-78(2001)
[12]H.Yamashita, H.Nishiguchi, N.Kamada, M.Anpo, Research on
Chemical Intermediates, vol.20 (8) 815-823(1994)
[13]M.R. Hoffmann, S. T. Martin, W. Choi, D.W. Bahnemann, Chem Rev.
Vol.95 69-96 (1995)
[14]J.K Burdett, T. Hughbabds, J.M. Gordon, J.W. Richardson Jr. and J. V.
Smith, J. Am. Chem. Soc. Vol. 109, 3639(1987)
[15]W.Choi, A. Termin, Hoffmann, Journal of Physical Chemistry vol. 98,
13669-13679(1994)
[16]G.Zhao, H.Kozuka, H.Lin, T.Yoko, Thin Solid Films Vol.339
123-128(1999)
[17]R.Asahi, T.Morikawa, T.Ohwaki, K.Aoki, Y.Taga, Science, Vol.293
269-271(2001)
[18]H.Yanashita, Y.Fuji, Y.Ichihshi, S.G.Zhang, K.Ikeue, D.R.Park,
K.Kayano, T.Tatsumi, M.Anpo, Catalysis Today Vol.45
221-227(1998)
[19]Tomoko Kasuga, Masayoshi Hiramatsu, Akihiko Hoson, Toru Sekino,
Koichi Niihara, Adv. Mater.11 No.15(1999)
[20]B.Poudel, W.Z. Wang, C. Dames, J.Y Huang, S. Kunwar, D.Z. Wang,
D. Banerjee, G. Chen, Z.F. Ren, Mater. Res. Soc. Symp. Proc. Vol.826
(2005)
[21]Jianguo Huang, Toyoki Kunitake, Shin-Ya Onoue, ChemComm
1008-1009 (2004)
[22]Xi Liu, Thomas F. Jaramillo, J. Mater. Res. Vol.20 5 (2005)
[23]Gopal K. Mor, Oomman K. Varghese, Maggie Paulose, Craig A.
Grimes, Adv. Func. Mater. 15 1291-1296 (2005)
[24Tomoko Kasuga, Masayoshi Hiramatsu, Akihiko Hoson, Toru Sekino,
Koichi Niihara, Langmuir.14 3160-3163(1998)
[25]Qing Chen, Wuzong Zhou, Gaohui Du, Lian-Mao Peng, Adv.
Mater.14(2002)
[26]Zhong-Yong Yuan, Bao-Lian Su, Colloids and Surfaces A:
Phyicochen. Eng. Aspects 241, 171-183(2004)
[27]B. D. Yao, Y. F. Chan, X. Y. Zhang, W. F. Zhang, Z. T. Yan, N. Wang,
Appl. Phys. Lett. 82 281(2003)
[28]Y.Q.Wang, G.Q.Hu, X.F.Duan, H.L Sun, Q.K. Xue, Chemical Physics
Letters 365 427-431(2002)
[29]Dong-Seok Seo, Jong-Kook Lee, Hwan Kim, Journal od Crystal
Growth 428-432(2001)
[30]M. Lazzeri, A. Vittadina, A. Selloni, Phys. Rev. B 63 155406(2001)
[31]P.M. Oliver, G.W. Watson, E.T. Kelsey, S.C. Parker, Journal Mater.
Chem. 7 563(1997)
[32]Ying Lan, Xueping Gao, Huaiyong Zhu, Zhanfeng Zheng, Tianying,
Yan, Feng Wu, Simon P. Ringer, Deying Song, Adv. Func. Mater.15
1310-1318(2005)
[33]Tomoki Akita, Mitsutaka Okumura, Koji Tanaka, Kayoko Ohkuma,
Masanori Kohyama, Tsuguo Koyanagi, Masakasu Data, Susumu
Tsubota, Masatake Haruta, Surface and Interface analysis 37
265-269(2005)
[34]Y. Zhu, H. Li, Y. Koltypin, R. Y, A. Gedanken, Chem. Commun. 2616
(2001)
[35]A. Nakahira, W. kato, M. Tamai, T. Isshiki, K. Journal of Phys. Chem.
B 39 4239(2004)
[36]J. Yang, Z. Jin, X. Wang, W. Li, J. Zhang, S. Zhang, X. Guo, Z.
Zhang, Journal of Chem. Soc. Dalton Tans 3898(2003)
[37]M. Zhang, Z. Jin, J. Zhang, X. Guo, J. Yang, W. Li, X. Wang, Z.
Zhang, Journal of Mol. Catal. A: Chem 217 203(2004)
[38]Renzhi Ma, Yoshio Bando, Takayoshi Sasaki, Chem. Phys. Lett. 380
577(2003)
[39]Renzhi Ma, Katsutoshi Fukuda, Takayoshi Sasaki, Minoru Osada,
Yoshio Bando, Journal of Phys. Chem. B 109 6210(2005)
[40]G.H. Du, Q. Chen, C. R. Chen, Z. Y. Yuan, L. M. Peng, “The
Structure of Trititanate Nanotubes”, Appl. Phys. Lett. 79 3702(2001)
[41]Q. Chen, G. H. Du, S. Zhang, L. M. Peng, Acta. Crystallor Sect. B 58
587(2002)
[42]Q. Chen, W. Z. Zhou, G. H. Du, L. M. Peng, Adv. Mater. 14 1208
(2002)
[43]Z. R. Tian, J. A. Voigt, J. Liu, B. Mckenzie, H. Xu, Journal of Am.
Chem. Soc. 125 12384(2003)
[44]S. Zhang, L. M. Peng, Q. Chen, G. H. Du, G. Dawson, Z. W. Zhou,
Phys. Rev. Lett. 91 256103(2003)
[45]X. Sun, Y. Li, Chem.-Eur. J. 9 2229(2003)
[46]A. Thorne, A. Kruth, D. Tunstall, J. T. S. Irvine, W. Zhou, Journal of
Phys. Chem. B 109 5439(2005)
[47]S. Zhang, Q. Chen, L. M. Peng, Phys. Rev. B 71 014104(2005)
[48]Q. Zhang, L. Gao, J. Sun, S. Zheng, Chem. Lett. 226(2002)
[49]Chien-Cheng Tsai, Hsisheng Teng, Chem. Mater. 16 4352(2004)
[50]W. Wang, O. K. Varghese, M. Paulose, C. A. Grimes, Journal of
Mater. Res. 19 417(2004)
[51]Chien-Cheng Tsai, Hsisheng Teng, Chem. Mater. 18 367-373 (2006)
[52]V. Idakiev, Z.-Y. Yuan, T. Tabakova, B.-L. Su, Applied Catalysis A:
General 281 149-155(2005)
[53]Tomoko Kasuga, Thin Solid Films 496 141-145 (2006)
[54]D. Andreeva, V. Idakiev, T. Tabakova, A. Andreev, R. Giovanoli,
Journal of Catalysis 158 354(1996)
[55]T. Kawai, T. Sakata, “Photocatalytic Hydrogen Production from
Liquid Methanol and Water”, JCS Chem. Commun. 694-4(1980)
[56]T. Kawai, T. Sakata, Chem. Lett. 81-4(1981)
[57]Sakata T, Kawai Y., Chem Phys Lett 80 341-4(1981)
[58] Sakata T, Kawai T, Hashimoto K, Chem Phys Lett 88 50-4(1982)
[59]G. Bamwenda, S. Tsubota, T. Nakamora, M. Haruta, Journal of
PhotoChem. Photobiol, 89 177(1995)
[60]G. Bamwenda, S. Tsubota, T. Nakamora, M. Haruta, Journal of
PhotoChem. Photobiol, 77 59(1994)
[61]Nae-Lin Wu, Min-Shuei Lee, Zen-Jin Pon, Jin-Zern Hsu, Journal of
Photochemistry and Photobiology A: Chemistry 163, 277-280(2004)
[62]Nae-Lin Wu, Min-Shuei Lee, International Journal of Hydrogen
Energy 29, 1601-1605(2004)
[63]Chen J, Ollis DF, Rulkens WH, Bruning H. ,Water Res 669-76(1999)
[64]Heondo Jeong, Kweon Ill Kim, Tae Hwan Kim, Chang Hyun Ko,
Hwa Choon Park, In Kyu Song, Journal of Power Sources
7636(2006)
[65]M.L Cuberiro, J.L.G. Fierro, Partial, Applied Catalysts A: General
168 307-322(1998)
[66]R. Kumar, S. Ahmed, M. Krumplet, K. Myles, Agron National
Laboratory Report ANL-92/31, Argone IL, USA(1992)
[67]J. L. G. Fierro, M. L. Cuberiro, Applied Catalysis A : General 168
307(1998)
[68]Susann Meyer, Sarah Saborowski, Bernhard Schafer,
ChemPhysChem. 7 572-574(2006)
[69]Amanda Dicknson, David James, Neil Perkins, Tim Cassidy, Michael
Bowker, Journal of Molecular Catalysis A: Chemical 146
211-221(1999)
[70]Michael Bowker, Lucy Millard, Jane Greaves, David James and Jorge
Soares, Gold Buelletin 37/3-4(2004)
[71]Yasuo Ebina, Takayoshi Sasaki, Masaru Harada, Mamoru Watanabe,
Chem. Mater. 14 4390-4395(2002)
[72] C.K. Chang, C.T. Yeh, Y.J. Chen, Applied Catalysts A: General 174
13 (1998)
[73] M. Besson, A. Kallel. P. Gallezot, R. Zanella, Catalysts Comm. 4 471
(2003)
[74]T.Sakata, T. Kawai, Chem. Phys. Lett. 80 341 (1981)
[75]P. Pichat, J.-M. Herrman, J. Didier, HCourbon, M. Mozzanega, Nouv.
J. Chem 5 627 (1981)
[76]A. Kudo, K. Domen, K. Maruya, T. Onishi, Chem. Phys. Lett. 133
517 (1987)
[77]J. Abrahams, R. Davidson, C. Morrison, J. Photochem. 29 353 (1985)