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  1. NTU Theses and Dissertations Repository
  2. 理學院
  3. 化學系
請用此 Handle URI 來引用此文件: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/15727
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dc.contributor.advisor鄭淑芬(Soo-fin Cheng)
dc.contributor.authorYi-Chieh Chenen
dc.contributor.author陳奕价zh_TW
dc.date.accessioned2021-06-07T17:50:51Z-
dc.date.copyright2012-11-22
dc.date.issued2012
dc.date.submitted2012-11-08
dc.identifier.citation1. Kresge, C. T.; Leonowicz,M.E. ; Roth, W.J. ; Vartuli J.C.; and Beck, J. S.; Nature, 1992, 359, 710.
2. Beck, J. S. ; Vartuli, J.C. ; Roth,W.J. ; Leonowicz, M.E. ; Kresge, C. T. ; Schmitt K. D.,; Chu, C. T-W.; Olson, D. H.; Sheppard, E. W. ; Higgins, S. B.; and Schlenker, J. L.; J. Am. Chem. Soc., 1992, 114, 10834.
3. Sayari, A. ;Chem. Mater., 1996, 8, 1840.
4. Neumann,R. ; Khenkin, K. ;Chem. Commun., 1996, 23, 2643.
5. Hartmann, M. ; popll, A.; Kenvan, L.; J. Phys. Chem., 1996, 100, 9906.
6. Hayward, R. C. ; Henning, P. A.; Chemlka,B. F.; Stucky, G.D.; Micropor. Mesopor. Mater. , 2001, 44, 619.
7. Ying,J. Y.; Mehnert, C. P. ; Wong, M. S. ; Angew. Chem. Int. Ed., 1999, 38, 56.
8. Goyal, P. S.; Aswal, V. K.; Current Sci., 2001, 80, 972.
9. Chen,C. Y.; Burkett,S. L. ; Li, H. X. ; Davis, M. E.;Microporous Mater., 1993,2,27.
10. Huo, Q.; Margolese, D. I.; Ciesla, U.; Feng, P.; Gier, T. E.; Sieger, P. ; Leon, R. ; Petroff, P. M.; Schuth,F.; Stucky,G. D. ; Nature, 1994, 368, 317
11. Sakamoto, Y. ; Kaneda, M.; Terasaki, O.; Zhao, D. Yuan,; Kim, J. M.; Stucky, G. H. ; Shin, J.; Ryoo, R.; Nature, 2000, 408, 449.
12. Kim,M.J.; Ryoo, R. Chem. Master. 1999 , 11,487
13. Che, S.; Sakamoto, Y.; Terasaki, O.; Tatsumi, T. Chem. Master. 2001, 13, 2237
14. Che, S.; Sakamoto, Y.; Terasaki, O.; Tatsumi, T. Chem. Lett. 2002, 2, 214.
15. Chao, M. C.; Lin, H. P.; Wang, D.S.; Mou, C.Y. Chem. Lett. 2004,33,374
16. Dai, L. X.; Teng, Y.H.; Tabata, K.; Suzuki, E.; Tatsumi, T. Micro. Meso. Master.2001,44-45,573.
17. Che, S.; Sakamoto, Y.; Yoshitake, H.; Terasaki, O.; Tatsumi, T.J. Phys. Chem.B 2001, 105, 10565
18. Dai, L. X.; Teng, Y.H.; Tabata, K.; Suzuki, E.; Tatsumi, T.Chem. Master. 2001, 13, 208.
19. Israelachvili,J. N.; Mitchell, D. J.; Niham, B. W.; J. Chem. Soc., Faraday Trans., 2, 1976, 72, 1525.
20. Israelachvili, J. N.; Mitchell, D. J.; Niham,B. W.; Biochim. Biophys. Acta, 1977, 470, 185
21. Hyde,S. T.; Pure Appl. Chem., 1992, 64, 1617.
22. Fogden, A. ; Hyde, S. T. ; Lundberg,G. J.; J. Chem. Soc., Faraday Trans., 1991, 87, 949.
23. Bijma, K.; Rank,E. ; Engberts, J.B.F.N.; J. Colloid Interface Sci., 1998, 205, 245.
24. Ray, A.; Nemethy, G. J. Am. Chem. Soc., 1971, 93, 6787.
25. Gaillon, L.; Lelievere, J.; Gaboriaud, R. ; J. Colloid Interface Sci., 1999, 213, 287.
26. Cacace, M. G.; Landau, F.M.; Ramden,J. J. Q.; ReV. Biophys., 1997,30, 241.
27. Leontidis,E. C. O.; Colloid Interface Sci., 2002,7,81.
28. Koop, T.; LUO, B.; Tsias, A.; Peter, T.; Nature., 2000, 406, 611.
29. Baldwin, R. L.; Biophys. J., 1996, 71, 2056.
30. Collins, K. D.; Washabaogh,M.W. ;Q. ReV. Biophys., 1985, 18,323.
31. Liu, M. C.; Sheu,H. S.; Cheng,S.F.; Chem.Common., 2002, 2854.
32. Liu,M. C.; Dissertation,Ph.D.; National Taiwan University, Taipei, Taiwan, ROC, 2005.
33. Ogura,M.; Miyishi,H.; Naik, S. P.; Okubo, T.; J. Am. Chem. Soc., 2004, 126, 10937.
34. Liu,M. C.; Sheu, H. S. Cheng, S. F.; J. Am. Chem. Soc., 2009, 131, 3998.
35. Kao, H. M.; Shen, T. Y.; Wu, J. D.; Lee,L. P.; Microporous and Mesoporous Materials., 2008, 110, 461.
36. Nigam,P. S.; Singh,A.; Progress in Energy and Combustion Sience., 2011, 37, 52.
37. Turkevich, J.; Catal. Rev.-Sci. Eng. 1983, 1, 1.
38. Ward, W. J. Molecular sieve catalysts, in applied industrial catalysis, Academic press, New York, 1984, 3.
39. Lmelik, B.; Naccache, Y.; Bentaaiit, J.; Vedrine, J.; Coudurier, C. G. ; Praliaud, H. Catalysis by zeolite, Elesevier, Amstordam, 1980.
40. Bhatia, S. Zeolite catalysis principles and application, CRC press, FLORIDA, 1990.
41. Atlas of Zeolite Structure Types, Zeolites 1999, 12, 5.
42. Meier, W. M.; Olson, D. H.; Zeolites, 1992, 12, 5, 16.
43. Ryoo, R.; Kim, J. M.; Ko, C. H.; Shin, C. H.; J. Phys. Chem. 1996, 100, 17718.
44. Ryoo, R.; Jun, S.; Kim, J. M.; Kim, M. J. Chem. Commun. 1997, 2225.
45. Kim, J. M.; Jun, S.; Ryoo, R. J. Phys. Chem. B 1999, 103, 6200.
46. Mokaya, R.; Jones, W.; Chem. Commun. 1997, 2185.
47. Mokaya, R.; Jones, W.; Chem. Commun. 1998, 1839.
48. Mokaya, R.; Jones, W.; Angew. Chem. Int. Ed. 1999, 38, 2930.
49. Zhao, D.; Feng, J.; Huo, Q.; Melosh, N.; Fredrickson, G. H.; Chmelka, B.F.; Stucky, G. D. Science 1998, 279,548.
50. Tanev, P. T.; Pinnavaia, T.J. Science 1995, 267, 865.
51. Karlsson, A.; Stocker, M.; Schmidt, R. Microporous Mesoporuos Mater. 1999, 27, 181.
52. Huang, L.; Guo, W.; Deng, P.; Xue, Z. Li, Q. J. Phys. Chem. B. 2000, 104, 2817
53. Kloetstra, K. R.; van Bekkum, H.; Jansen, R. J. Chem. Commum. 1997,2281.
54. Xia, Q. H.; Hidajat, K.; Kawi, S. Chem. Commun.2000, 2229.
55. Charvolin, J.; Sadoc, J. F. J. Phys. Paris 1998, 49, 521.
56. Yuan, X. D.; Shen, J.; Li, G. H.; Kim, J. M.; Park, S. E. Chin. J. Catal. 2002, 23, 435.
57. Mokaya, R. Chem. Commun. 2000, 1451
58. Mokaya, R. J. Am. Chem. Soc. 2002, 124, 10636.
59. Karlsson, A.; Stocker, M.; Schafer, K. Stud. Surf. Sci. Catal. 2000, 129, 106.
60. Corma, A. Chem. Rev. 1997, 97, 2373.
61. Kresge, C. T.; Leonowicz, M. E.; Roth, W. J.; Vartuli, J. C.; Beck, J. S. Nature 1992, 359, 710.
62. Van Bekkum, H.; Flanigen, E. M.; Jacobs, P. A.; Jansen, J.C. Stud. Surf. Sci. Catal. 2001, 137, 69.
63. Robson, H.; ACS. Symp. Ser. 1989, 398,436.
64. Liu, Y.; Zhang, W.; Pinnanaia, T. J. J. Am. Chem. Soc. 2000, 122, 8791.
65. Kresge, C. T.; Leonwicz, M. E.; Roth, W. J.; Vartuli, J. C.; Beck, J.s. Nature 1992, 359, 710.
66. Yang, Q.; Li, Yi.; Zhang, L.; Yang, J.; Liu, J.; Li, C. J. Phys. Chem. B2004, 108, 7934.
dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/15727-
dc.description.abstract本研究在鹼性條件(pH8-10)下利用共沉澱法合成,以陽離子型界面活性劑CTEABr(Cetyltriethylammonium bromide)作為模板,矽源為sodium silicate (Na2SiO3),加入NaAlO2作為鋁源來合成不同孔洞結構之含鋁介孔二氧化矽。利用不同陰離子來調控孔洞結構,其中(Cl-與NO3-)可以分別得到具有三維立方堆積孔洞結構(3D-cubic,Pm3n)之介孔材料SBA-1-alk與二維六方堆積孔洞結構(2D-hexagonal,p6mm)之介孔材料HMM-alk,加入的鋁金屬含量達到Al/Si=5%。接著將矽源換成ZSM-5沸石晶種合成具有結晶性孔壁的ZSBA-1-alk結構,並以CTMABr作為模板合成二維六方堆積孔洞結構MCM-41分別與非晶相孔壁的Al-SBA-1-alk和Al-HMM-alk做比較。所合成的材料經由XRD、N2 adsorption-desorption isotherm、FT-IR、Al-NMR 和TPD等技術鑑定,可得知所合成出來的材料有很好的二維或三維介孔結構、表面積達到900 m2/g、加入晶種的ZSBA-1-alk酸含量比SBA-1-alk高,孔壁具有ZSM-5的結晶性、大部分的鋁離子是在骨架的四面體中心。最後利用所製備含鋁介孔材料作為酸觸媒,催法2,4-di-tert-butylphenol及cinnamyl alcohol的烷基化反應,結果三維立方堆積的Al-SBA-1-alk催化活性高於二維六方堆積的Al-MCM-41及Al-HMM-alk,而含沸石晶種的5Al-ZSBA-1-alk的催化效果最好,flavan的產率在95 °c反應4小時可以達到56%(mol/g catal)。zh_TW
dc.description.abstractAl-incorporated 3D-cubic(Pm3n) SBA-1-alk and 2D-hexagonal(p6mm) HMM-alk were synthesized by one-pot method in alkaline condition (pH=8-10) by using CTEABr (Cetyltriethylammonium bromide) as the template NaAlO2 as Al source, and Na-silicate as the silica source in the presence of NO3- and Cl- anions, respectively. Furthermore, Al-incorporated ZSM-5 seeds were used as the Al and Si sources to synthesize cubic Al-ZSBA-1-alk. Meanwhile, Al-MCM-41 was compared using CTMABr as the template in order to compared the properties with Al-SBA-1-alk and Al-HMM-alk. The resultant materials were characterized by X-ray diffraction (XRD), N2 adsorption-desorption isotherm, FT-IR, Al-NMR and TPD. The small-angle XRD patterns of Al-SBA-1-alk and Al-HMM-alk confirmed the 3-D cubic Pm3n phase and 2-D hexagonal p6mm phases. ZSBA-1-alk exhibited an absorption band at 550 cm-1 in the FT-IR spectrum, which is assigned to the stretching of five-membered T-O-T (T = Si or Al) rings in ZSM-5. In Al-NMR most Al is assigned to the tetrahedrally-coordinated Al species The materials were tested as catalysts in alkylation of 2,4-di-tert-butylphenol with cinnamyl alcohol.3D-cubic Al-SBA-1-alk showed better activity than 2D-hexagonal Al-HMM-alk and Al-MCM-41, while 5Al-ZSBA-1-alk gave the best catalyst activity and yield reached 56%(mol/g catal) at 95 °C in 4 hours.en
dc.description.provenanceMade available in DSpace on 2021-06-07T17:50:51Z (GMT). No. of bitstreams: 1
ntu-101-R99223169-1.pdf: 2677291 bytes, checksum: 50a5c6c9c3140a93405614d55cd664cf (MD5)
Previous issue date: 2012
en
dc.description.tableofcontents摘要 I
Abstract II
目錄 III
圖目錄 V
表目錄 Ⅶ
第一章 緒論 1
1-1 界面活性劑微胞性質及介孔材料SBA-1的簡介 1
1-2堆積參數(g)對微胞結構的影響 8
1-3鹼式法與酸式法生成SBA-1之性質比較 10
1-4 沸石的簡介 11
1-5沸石奈米粒子自組裝之介孔分子篩材料簡介 13
1-6研究目的 15
第二章 實驗部分 16
2-1 化學藥品 16
2-2 合成步驟 17
2-2-1合成界面活性劑CTEABr(Hexadecyltriethylammonium bromide) 17
2-2-2鹼式法合成Al-SBA-1-alk 17
2-2-3鹼式法合成Al-HMM-alk 17
2-2-4合成Al-MCM-41 18
2-2-5以Al-ZSM-5為晶種的SBA-1-alk(簡稱Al-ZSBA-1-alk)之合成 18
2-3鑑定介孔材料之儀器與方法 19
2-4催化反應 24
2-5產物及反應物鑑定 26
第三章 結果與討論 28
3-1界面活性劑的鑑定 28
3-2 純矽SBA-1-alk的結構鑑定 29
3-3 含鋁的SBA-1-alk(簡稱Al-SBA-1-alk)與含鋁及ZSM-5晶種的ZSBA-1-alk(簡稱Al-ZSBA-1-alk)介孔分子篩之合成與鑑定 30
3-4 Al-HMM-alk與Al-MCM-41材料結構鑑定 36
3-5催化反應 44
第四章 結論 51
第五章 參考文獻 52
dc.language.isozh-TW
dc.title不同結構之含鋁介孔材料之合成與催化反應比較zh_TW
dc.titlePreparation and catalytic activities of Al-incorporated mesoporous material with different structuresen
dc.typeThesis
dc.date.schoolyear101-1
dc.description.degree碩士
dc.contributor.oralexamcommittee蔡 蘊 明(Yeun-Min Tsai),簡 淑 華(Shu-Hua Chien)
dc.subject.keyword含鋁中孔洞材料,界面活性劑,催化反應,zh_TW
dc.subject.keywordmesoporous material,SBA-1,CTEABr,catalytic reaction,en
dc.relation.page55
dc.rights.note未授權
dc.date.accepted2012-11-08
dc.contributor.author-college理學院zh_TW
dc.contributor.author-dept化學研究所zh_TW
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