博碩士論文 93324012 詳細資訊




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姓名 王麗菁(Li-Jing Wang)  查詢紙本館藏   畢業系所 化學工程與材料工程學系
論文名稱 MFI沸石奈米結晶製備研究
(Synthesis of MFI zeolite nanocrystals)
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摘要(中) 摘要
在本研究中我們預備以先前發展出之快速製作奈米silicalite-1 沸石的方法,進一步合成出含鋁之ZSM-5 沸石。
此一方法乃是將前驅物先濃縮到約30wt% SiO2,將此濃稠前驅物在80℃老化約一天後再以175℃水熱反應進行合成。合成ZSM-5 沸石前,我們必須先更清楚地瞭解製備過程中條件之控制。例如,在濃縮程序的操控步驟、溫度與時間,以及濃縮後的加熱條件。有此部分了解後我們又進行合成ZSM-5 沸石,我們研究在起使配方中之Si/Al比與
TPAOH/Si比例對於合成ZSM-5 沸石大小的影響。發現到當系統中鋁含量增加時,合成出之沸石粒子尺寸也增加。TPAOH之比例在系統中亦有一理想比例,在此比例下合成出之ZSM-5 沸石粒子尺寸最小。在適當之合成條件下我們可在兩天內製備出大小分別為140、110 與50nm之ZSM-5(silicalite)奈米沸石,其Si/Al比分別為50、100 與∞。
摘要(英) Abstract
A procedure was developed in our laboratory to synthesis non-agglomerated silicalite nanocrystals within days, instead of weeks as
required in the literatures. This was achieved by concentrating the precursor sol, aging at 80oC for about a day, followed by a short hydrothermal reaction at 175oC. In this study, the same procedure has been extended to the synthesis of aluminum containing ZSM-5 zeolite nanocrystals.
However, before applying the method to ZSM-5 system, some details of the previous procedures were further investigated to clarify the controlling parameters. For example, the proper way to concentrate the precursor sol, the selection of temperature and duration in the first aging stage, as well as that in the second hydrothermal reaction stage.
After clarifying the controlling parameters, the method was applied to the synthesis of ZSM-5. In addition to the Si/Al ratio, the effect of TPAOH
ratio in the starting recipe was also investigated. It was found that the size
of the resulted nanozeolite increases with the amount of aluminum incorporated. On the other hand, there exists an optimum TPAOH/SiO2 ratio leading to the smallest particles size. Under appropriate conditions,non-agglomerated ZSM-5 (silicalite) nanocrystals of 140, 110 and 50 nm
for Si/Al of 50, 100 and infinite, respectively, were achieved with a total synthesis time shorted than 2 days.
關鍵字(中) ★ Silicalite-1
★ ZSM-5
★ 矽鋁比
★ TPAOH比例
★ MFI 沸石
關鍵字(英) ★ ZSM-5
★ TPAOH ratio
★ Si/Al ratio
★ MFI zeolite
★ Silicalite-1
論文目次 目錄
摘要 ............................................................... I
目錄 ............................................................. III
第一章 背景......................................................... 1
1-1 沸石簡介.........................................................1
1-2 MFI 沸石.........................................................2
1.3 奈米沸石的應用..................................................3
第二章 文獻回顧..................................................... 5
2.1 MFI 前驅物(precursor)的研究.......... ........................5
2.2 MFI 沸石的形成與成長.............................................6
2.2.1 Silicalite-1 沸石的形成與成長........ ........................6
2.2.2 ZSM-5 沸石的形成與成長............ ............................8
2.3 研究方向....... ...........................................10
第三章 Silicalite-1 沸石奈米結晶合成................................ 11
3.1 二段式濃縮法製備奈米silicalite-1 結晶............................ 11
3.1.1 利用二段式濃縮-老化-水熱之程序製備奈米silicalite-1 ................... 11
3.1.2 二段式濃縮合成法之silicalite-1 沸石粒子粒徑分析........................12
3.2 不同水熱溫度對Silicalite-1 沸石之結晶產率影響............................12
3.3 粉末X 射線繞射(PXRD)分析..............................................13
3.4 氮氣恆溫吸附(ASAP)分析................................................14
3.5 TPAOH 比例之影響................................................ 15
3.6 奈米silicalite-1 結晶製備Fiber ....................................15
3.7 結果討論....................................................16
第四章 ZSM-5 沸石奈米結晶合成....................................... 17
4.1 濃縮-老化-水熱之程序製備ZSM-5 沸石.............................17
4.1.1 ZSM-5 沸石沸石粒子粒徑分析.......................................17
4.2 濃縮前加熱對ZSM-5 沸石的影響...................................18
4.3 矽鋁比對ZSM-5 沸石的影響...........................................19
4.3.1 製備矽鋁比為100 之ZSM-5 沸石..............................19
4.3.2 不同鋁含量之ZSM-5 沸石粒子粒徑分析...............................20
4.4 TPAOH 比例對ZSM-5 沸石之影響........................................20
4.4.1 製備不同TPAOH 比例之colloidal ZSM-5 沸石..............................20
4.4.2 以濃縮-老化-水熱之程序製備不同TPAOH 比例之ZSM-5 沸石..........21
4.4.3 TPAOH 比例對不同矽鋁比之ZSM-5 沸石的影響...........................22
4.5 掃瞄式電子顯微鏡(SEM)分析..........................................22
4.6 結果討論................................................23
第五章 結論與建議.................................................. 24
參考文獻........................................................... 26
附錄A 製備Silicalite-1 沸石膜...................................... 29
附錄B ZSM-5 沸石粉末X 射線繞射(PXRD)分析......................... 30
附錄C 實驗藥品..................................................... 31
表目錄............................................................. 32
圖目錄............................................................. 40
參考文獻 參考文獻
Reference List
1. Pu, Shu-Bina; Inui, Tomoyuki Zeolite 1996, 17, 334-39.
2. Colin S.Cundy; James O.Forrest Micropor.Mesopor.Mater. 2004, 72, 67.
3. W.Song; V.H.Grassian; R.E.Justice; S.C.Larsen; C.A.Jones Langmuir 2004, 20,
8301.
4. J.Aguado; D.P.Serrano; J.L.Sotelo; R.Van Grieken; J.M.Escola Ind.Eng.Chem.Res.
2001, 40, 5696-704.
5. D.P.Serrano Applied Catalysis B: Environmental 2004, 49, 257.
6. Valtchev, V. Journal of Materials Chemistry 2002, 12, 1914-18.
7. Alexander, Aerts; Johan, A. Martens Applied Catalysis A: General 2005, 257,
7-17.
8. Shiguang Li; Vu A.Tuan; Richard D.Noble; John L.Falconer Ind.Eng.Chem.Res.
2001, 40, 4577.
9. Yushan Yan Langmuir 2004, 17, 2572.
10. Svetlana Mintova, Shangyi Mo Thomas Bein Chem.Mater 2001, 13, 901-05.
11. Gaynor; Justin F United States Patent 2001, 514966.
12. Sankar Nair; Michael Tsapatsis Micropor.Mesopor.Mater. 2003, 58, 81-89.
13. Zhang, Jian; Luo, Ming; Xiao, Hai; Dong, Junhang Chemistry of Materials 2006,
18, 4-6.
14. Alvaro, Mercedes; Cabeza, Jose F.; Fabuel, David; Garcia, Hermenegildo;
Guijarro, Enrique; De Juan, Jose Luis Martinez Chemistry of Materials 2006, 18,
26-33.
15. Hyun Sung Kim, Seung Mook Lee Kwang Ha Changsoo Jung Yun-Jo Lee Yu
Sung Chun Doseok Kim Bum Ku Rhee Kyung Byung Yoon J.AM.CHEM.SOC.
2004, 126, 673.
16. Feifei, Gao; Guangshan, Zhu; Yue, Chen; Yi, Li; Shilun, Qiu J.Phys.Chem.B 2004,
108, 3426.
17. Feifei, Gao; Guangshan, Zhu; Xiaotian, Li; Binsong, Li; Osamu, Terasaki; Shilun,
Qiu J.Phys.Chem.B 2004, 105, 12704.
18. Xiaotian, Li; Osamu, Terasaki; Pinliang, Ying; Weitao, Zheng; Feng-Shou, Xiao;
Shilun, Qiu Micropor.Mesopor.Mater. 2004, 40, 263.
26
19. Guido Ihlein Adv.Mater 2004, 10, 1117.
20. David P.Serrano; Rafael van Grieken J.Mater.Chem. 2005, 11, 2391-407.
21. Sandra L.Burkett and Mark E.Davis Chem.Mater. 1995, 7, 920-28.
22. Brian J.Schoeman; Oren Regev Zeolite 1996, 17, 447-56.
23. Brian J.Schoeman Micropor.Mesopor.Mater. 1998, 22, 9-22.
24. Brian J.Schoeman Progress inZeolites and Microporous Materials 1997, 105,
674-54.
25. C.S.Tsay; A.S.T.Chiang Micropor.Mesopor.Mater. 1998, 26, 89.
26. Christine, E. A. Kirschhock; Raman, Ravishankar; Frederik, Verspeurt; Piet, J.
Grobet; Pierre, A. Jacobs; Johan, A. Martens J.Phys.Chem.B 1999, 103, 4960-64.
27. Christine, E. A. Kirschhock; Raman, Ravishankar; Frederik Verspeurt; Piet, J.
Grobet; Pierre, A. Jacobs; Johan, A. Martens J.Phys.Chem.B 1999, 103, 4965-71.
28. Christine, E. A. Kirschhock; Raman, Ravishankar; Frederik, Verspeurt; Piet, J.
Grobet; Pierre, A. Jacobs; Johan, A. Martens J.Phys.Chem.B 1999, 103, 4972-78.
29. Christine, E. A. Kirschhock; Raman, Ravishankar; Frederik, Verspeurt; Piet, J.
Grobet; Pierre, A. Jacobs; Johan, A. Martens J.Phys.Chem.B 1999, 103, 11021-27.
30. Christine, E. A. Kirschhock; Veronique, Buschmann; Raman, Ravishankar;
Sebastien, Kremer; Christophe, J. Y. Houssin; Barbara, L. Mojet; Rutger, A. van
Santen; Piet, J. Grobet; Pierre, A. Jacobs; Johan, A. Martens Angew.Chem.Int.Ed.
2001, 40, 2637-40.
31. Peter-Paul, E. A. de Moor; Theo, P. M. Beelen; Rutger, A. vanSanten Microporous
Materials 1997, 9, 117-30.
32. Peter-Paul, E. A. de Moor; Theo, P. M. Beelen; Rutger, A. vanSanten
J.Phys.Chem.B 1999, 103, 1639-50.
33. Dokter, W. H; Gerderen, H. F. van; Beelen, T. P. M; Santen, R. A. van; Bras, W
Angew.Chem.Int.Ed.Engl 1995, 34, 73-75.
34. Qing-Lin, Liu; D, Creaser; J, Sterte Micropor.Mesopor.Mater. 1999, 31, 141-50.
35. Colin S.Cundy Micropor.Mesopor.Mater. 2004, 66, 143-56.
36. S.G.Fegan; B, M Lowe Journal of the Chemical Society, Faraday Transactions
1986, 82, 785-99.
37. S.Mintova; V, Valtchev Micropor.Mesopor.Mater. 2002, 55, 171-79.
38. Cheng, C. H.; Shantz, D. F. Journal of Physical Chemistry B 2005, 109, 19116-25.
27
39. A.E.Persson; J.E.Otterstedt; J.Sterte; B.J.Schoeman Zeolite 1994, 14, 557-67.
40. T.M.Davis, T. O. Drews H. Ramanan C. He J. Dong H. Schnablegger M. A.
Katsoulakis E. Kokkoli A. V. McCormick R. L. Penn and M. Tsapatsis Nature
Materials 2006, 5, 400-09.
41. A.E.Persson; Schoeman, B. J.; Sterte, J.; Otterstedt, J.-E. zeolite 1995, 15, 611-19.
42. Van Grieken, R.; Sotelo, J. L.; Menendez, J. M.; Melero, J. A.
Micropor.Mesopor.Mater. 2000, 39, 135-47.
43. Reding, G.; Maurer, T.; Kraushaar-Czarnetzki, B. Micropor.Mesopor.Mater. 2003,
57, 83-92.
44. Valentin, P. Valtchev; Anne-Cathrine, Faust Micropor.Mesopor.Mater. 2004, 68,
91-95.
45. W.Song; C.A.Jones; R.E.Justice; V.H.Grassian; S.C.Larsen Langmuir 2004, 20,
4696-702.
46. J.Aguado; J.M.Rodriguez; J.M.Escola; D.P.Serrano Micropor.Mesopor.Mater.
2004, 75, 41-49.
47. Li, Qinghua; Wang, Zheng; Hedlund, Jonas; Creaser, Derek; Zhang, Hong; Zou,
Xiaodong; Bons, Anton Jan Microporous and Mesoporous Materials 2005, 78,
1-10.
48. Hsu, C. Y.; Chiang, A. S. T.; Selvin, R.; Thompson, R. W. Journal of Physical
Chemistry B 2005, 109, 18804-14.
49. Serrano, D. P.; Uguina, M. A.; Sanz, R.; Castillo, E.; Rodriguez, A.; Sanchez, P.
Micropor.Mesopor.Mater. 2004, 69, 197-208.
50. Song, W.; Grassian, V. H.; Larsen, S. C. Micropor.Mesopor.Mater. 2006, 88,
77-83.
51. Huang, Limin; Wang, Zhengbao; Sun, Jinyu; Miao, Lei; Li, Quanzhi; Yan, Yushan;
Zhao, Dongyuan Journal of the American Chemical Society 2000, 122, 3530.
指導教授 蔣孝澈(Anthony S.T. Chiang) 審核日期 2006-7-6
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