請用此 Handle URI 來引用此文件:
http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/68636
完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 鄭淑芬(Soofin Cheng) | |
dc.contributor.author | Li-Min Tsao | en |
dc.contributor.author | 曹立敏 | zh_TW |
dc.date.accessioned | 2021-06-17T02:28:26Z | - |
dc.date.available | 2022-08-25 | |
dc.date.copyright | 2017-08-25 | |
dc.date.issued | 2017 | |
dc.date.submitted | 2017-08-17 | |
dc.identifier.citation | 1. L. C. Meher, D. V. Sagar and S. N. Naik, Renewable & Sustainable Energy Reviews, 2006, 10, 248-268.
2. B. Katryniok, S. Paul and F. Dumeignil, Acs Catalysis, 2013, 3, 1819-1834. 3. L. C. T. Lacerda, M. D. Pires, S. Correa, L. C. A. Oliveira and T. C. Ramalho, Chemical Physics Letters, 2016, 651, 161-167. 4. M. Besson, P. Gallezot and C. Pinel, Chemical Reviews, 2014, 114, 1827-1870. 5. A. Martin, U. Armbruster and H. Atia, European Journal of Lipid Science and Technology, 2012, 114, 10-23. 6. B. Katryniok, S. Paul, V. Belliere-Baca, P. Rey and F. Dumeignil, Green Chemistry, 2010, 12, 2079-2098. 7. Nojiri, N. Nojiri, Y. Sakai and Y. Watanabe, Catalysis reviews. Science and engineering, 1995, 37, 145-178. 8. A. S. de Oliveira, S. J. S. Vasconcelos, J. R. de Sousa, F. F. de Sousa, J. M. Filho and A. C. Oliveira, Chemical Engineering Journal, 2011, 168, 765-774. 9. A. Ulgen and W. F. Hoelderich, Applied Catalysis A: General, 2011, 400, 34-38. 10. N. R. Shiju, D. R. Brown, K. Wilson and G. Rothenberg, Topics in Catalysis, 2010, 53, 1217-1223. 11. S. Erfle, U. Armbruster, U. Bentrup, A. Martin and A. Brueckner, Applied Catalysis a-General, 2011, 391, 102-109. 12. H. Atia, U. Armbruster and A. Martin, Applied Catalysis a-General, 2011, 393, 331-339. 13. E. Tsukuda, S. Sato, R. Takahashi and T. Sodesawa, Catalysis Communications, 2007, 8, 1349-1353. 14. M. H. Haider, N. F. Dummer, D. Z. Zhang, P. Miedziak, T. E. Davies, S. H. Taylor, D. J. Willock, D. W. Knight, D. Chadwick and G. J. Hutchings, Journal of Catalysis, 2012, 286, 206-213. 15. C. J. Jia, Y. Liu, W. Schmidt, A. H. Lu and F. Schuth, Journal of Catalysis, 2010, 269, 71-79. 16. L. Z. Tao, S. H. Chai, Y. Zuo, W. T. Zheng, Y. Liang and B. Q. Xu, Catalysis Today, 2010, 158, 310-316. 17. L. Z. Tao, B. Yan, Y. Liang and B. Q. Xu, Green Chemistry, 2013, 15, 696-705. 18. S. H. Chai, H. P. Wang, Y. Liang and B. Q. Xu, Journal of Catalysis, 2007, 250, 342-349. 19. F. Cavani, S. Guidetti, C. Trevisanut, E. Ghedini and M. Signoretto, Applied Catalysis a-General, 2011, 409, 267-278. 20. K. Omata, S. Izumi, T. Murayama and W. Ueda, Catalysis Today, 2013, 201, 7-11. 21. A. Drochner, P. Kampe, J. Kunert, J. Ott and H. Vogel, Applied Catalysis a-General, 2005, 289, 74-83. 22. S. Endres, P. Kampe, J. Kunert, A. Drochner and H. Vogel, Applied Catalysis a-General, 2007, 325, 237-243. 23. J. Kunert, A. Drochner, J. Ott, H. Vogel and H. Fuess, Applied Catalysis a-General, 2004, 269, 53-61. 24. T. Jekewitz, N. Blickhan, S. Endres, A. Drochner and H. Vogel, Catalysis Communications, 2012, 20, 25-28. 25. J. Tichý, Applied Catalysis A: General, 1997, 157, 363-385. 26. J. Deleplanque, J. L. Dubois, J. F. Devaux and W. Ueda, Catalysis Today, 2010, 157, 351-358. 27. M. Sadakane, K. Kodato, T. Kuranishi, Y. Nodasaka, K. Sugawara, N. Sakaguchi, T. Nagai, Y. Matsui and W. Ueda, Angewandte Chemie International Edition, 2008, 47, 2493-2496. 28. M. D. Soriano, P. Concepcion, J. M. L. Nieto, F. Cavani, S. Guidetti and C. Trevisanut, Green Chemistry, 2011, 13, 2954-2962. 29. L. Shen, H. Yin, A. Wang, X. Lu and C. Zhang, Chemical Engineering Journal, 2014, 244, 168-177. 30. A. Chieregato, F. Basile, P. Concepcion, S. Guidetti, G. Liosi, M. D. Soriano, C. Trevisanut, F. Cavani and J. M. L. Nietoc, Catalysis Today, 2012, 197, 58-65. 31. A. Chieregato, M. D. Soriano, F. Basile, G. Liosi, S. Zamora, P. Concepcion, F. Cavani and J. M. L. Nieto, Applied Catalysis B-Environmental, 2014, 150, 37-46. 32. T. Ekström, Materials Research Bulletin, 1972, 7, 19-26. 33. A. Glycerine Producers, Physical properties of glycerine and its solutions, Glycerine Producers' Association, New York, 1963. 34. L. G. Possato, W. H. Cassinelli, T. Garetto, S. H. Pulcinelli, C. V. Santilli and L. Martins, Applied Catalysis A: General, 2015, 492, 243-251. 35. L. G. Possato, W. H. Cassinelli, C. I. Meyer, T. Garetto, S. H. Pulcinelli, C. V. Santilli and L. Martins, Applied Catalysis a-General, 2017, 532, 1-11. 36. J. Y. Ying, C. P. Mehnert and M. S. Wong, Angewandte Chemie-International Edition, 1999, 38, 56-77. 37. C. Kresge, M. Leonowicz, W. Roth and J. Vartuli, nature, 1992, 359, 710-712. 38. A. Sayari, Chemistry of Materials, 1996, 8, 1840-1852. 39. J. Beck, J. Vartuli, W. J. Roth, M. Leonowicz, C. Kresge, K. Schmitt, C. Chu, D. H. Olson, E. Sheppard and S. McCullen, Journal of the American Chemical Society, 1992, 114, 10834-10843. 40. C.-Y. Chen, S. L. Burkett, H.-X. Li and M. E. Davis, Microporous Materials, 1993, 2, 27-34. 41. D. Zhao, J. Feng, Q. Huo, N. Melosh, G. H. Fredrickson, B. F. Chmelka and G. D. Stucky, science, 1998, 279, 548-552. 42. S.-Y. Chen, L.-Y. Jang and S. Cheng, Chemistry of materials, 2004, 16, 4174-4180. 43. S.-Y. Chen, C.-Y. Tang, W.-T. Chuang, J.-J. Lee, Y.-L. Tsai, J. C. Chan, C.-Y. Lin, Y.-C. Liu and S. Cheng, Chemistry of Materials, 2008, 20, 3906-3916. 44. X.-R. Ye, Y. Lin, C. Wang, M. H. Engelhard, Y. Wang and C. M. Wai, Journal of Materials Chemistry, 2004, 14, 908-913. 45. Y. Lin, X. Cui, C. H. Yen and C. M. Wai, Langmuir, 2005, 21, 11474-11479. 46. J. Morère, M. Tenorio, M. Torralvo, C. Pando, J. Renuncio and A. Cabanas, The Journal of Supercritical Fluids, 2011, 56, 213-222. 47. J. Morere, M. J. Tenorio, M. J. Torralvo, C. Pando, J. A. R. Renuncio and A. Cabanas, Journal of Supercritical Fluids, 2011, 56, 213-222. 48. J. Pan, J. Liu, S. Guo and Z. Yang, Catalysis letters, 2009, 131, 179-183. 49. S. R. Bathe and P. S. Patil, Solid State Ionics, 2008, 179, 314-323. 50. L. G. Possato, W. H. Cassinelli, C. I. Meyer, T. Garetto, S. H. Pulcinelli, C. V. Santilli and L. Martins, Applied Catalysis A: General, 2017, 532, 1-11. 51. Z. Yin, Y. Xiao, X. Wang, W. Wang, D. Zhao and M. Cao, Nanoscale, 2016, 8, 508-516. 52. Y. S. Yun, K. R. Lee, H. Park, T. Y. Kim, D. Yun, J. W. Han and J. Yi, ACS Catalysis, 2014, 5, 82-94. 53. A. Chieregato, M. D. Soriano, E. Garcia-Gonzalez, G. Puglia, F. Basile, P. Concepcion, C. Bandinelli, J. M. L. Nieto and F. Cavani, Chemsuschem, 2015, 8, 398-406. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/68636 | - |
dc.description.abstract | 甘油脫水氧化形成丙烯酸的反應在工業上具有高度經濟價值,本研究欲探討同時具有酸性及氧化力的觸媒,以一步反應將甘油脫水氧化形成丙烯酸。此催化過程包含兩個連續的反應,先利用觸媒的酸性將甘油脫水形成丙烯醛,丙烯醛緊接著氧化形成丙烯酸。本研究利用不同比例之V/Mo/W金屬氧化物及將其負載於SBA-15上,觀察對催化所造成的影響,同時利用XRD、NH3-TPD、SEM 和 N2 吸脫附技術來探討不同因素所造成的影響。
催化條件測試中發現,當溫度為300oC、N2/O2/glycerol = 71/4.5/1、總體流速為50 mL/min及甘油進樣速率為3 mL/h時,擁有最佳的催化條件,將V/Mo/W金屬氧化物負載於SBA-15上會增加丙烯醛及丙烯酸的選擇率,同時降低氣體CO及CO2的選擇率。已知V對於丙烯醛氧化反應是有幫助的,然而,當V/W比例增加時,會使過度氧化的產物COx增加,而當V/Mo比例增加時,COx選擇率反而下降。在調整金屬比例V/Mo/W = 1/0/4後負載於SBA-15上,觸媒30%W4V1-SBA-15可得到最高的丙烯酸選擇率15%。 | zh_TW |
dc.description.abstract | The catalytic behaviors of bifunctional catalysts with acidic and oxidizing properties were investigated in the one-step oxidehydration of glycerol to acrylic acid. The demonstrated reaction involves two consecutive steps of acid-catalysed glycerol dehydration into acrolein and aldehyde oxidation into acrylic acid. The aim of this study is to optimize the components of V/Mo/W mixed oxides and to examine the effect of supporting V/Mo/W over platelet SBA-15. The catalysts were characterized by XRD, NH3-TPD, SEM and N2 sorption techniques.
The optimal reaction condition was 300oC, N2/O2/glycerol = 71/4.5/1, N2 flow rate of 50 mL/min, glycerol flow rate 3 mL/h. Supporting V/Mo/W mixed oxides on SBA-15 would enhance the yields of acrolein and acrylic acid and decrease the COx yields at the same time. On the other hand, V are active in oxidation reaction. However, the yields of over-oxidized COx products increased when the V/W ratio increased. On the contrary, the COx yield decreased when the V/Mo ratio increased. As a result, the highest yield of acrylic acid was obtained over the SBA-15 supported catalyst with V/Mo/W atomic ratio of 1/0/4. The highest acrylic acid selectivity of 15% was obtained over 30%W4V1-SBA-15 catalyst. | en |
dc.description.provenance | Made available in DSpace on 2021-06-17T02:28:26Z (GMT). No. of bitstreams: 1 ntu-106-R04223156-1.pdf: 3854419 bytes, checksum: 8ed1895f92334177cefd4813396bc144 (MD5) Previous issue date: 2017 | en |
dc.description.tableofcontents | 謝誌...i
中文摘要...ii ABSTRACT...iii 目錄...iv 圖目錄...vi 表目錄...x 第一章 緒論 1-1 研究背景...1 1-2 甘油脫水氧化觸媒、反應機制及其產物分布...3 1-3 介孔材料之簡介...12 1-4 超臨界流體...16 1-5 研究目標...19 第二章 實驗部分...20 2-1 化學藥品...20 2-2 觸媒的製備...21 2-2-1 鎢釩氧化物製備...21 2-2-2 鉬釩氧化物製備...21 2-2-3 扁平狀SBA-15之合成...21 2-2-4 將混和金屬氧化物負載於SBA-15上...21 2-3 觸媒材料的鑑定...22 2-4 催化反應...26 2-5 產物鑑定...27 第三章 觸媒的鑑定...30 3-1 鎢釩氧化物及鉬釩氧化物觸媒...30 3-2 不同釩前驅物合成鎢釩氧化物負載於SBA-15...33 3-3 超臨界乙醇合成不同負載量之鎢釩及鉬釩氧化物負載於SBA- 15...37 3-4 超臨界乙醇合成鎢釩及鉬釩氧化物負載於SBA-15...41 3-5 掃描式電子顯微鏡影像...47 3-6 穿透式電子顯微鏡影像...48 3-7 X-ray光電子能譜...49 第四章 催化反應...50 4-1 氧氣流速對觸媒之催化活性影響...50 4-2 鎢釩及鉬釩氧化物觸媒之催化活性...51 4-3 不同釩前驅物合成觸媒對催化活性之影響...52 4-4 探討接觸時間對催化活性之影響...54 4-5 探討負載量對催化活性之影響...55 4-6 探討負載於SBA-15上金屬氧化物莫耳數對催化活性之影 響...57 第五章 結論 ...59 參考文獻 ... 60 | |
dc.language.iso | zh-TW | |
dc.title | SBA-15負載釩鉬鎢混合金屬氧化物對氣相甘油脫水氧化反應研究 | zh_TW |
dc.title | Gas-phase Oxidehydration of Glycerol over V/Mo/W Mixed Oxides Supported on SBA-15 | en |
dc.type | Thesis | |
dc.date.schoolyear | 105-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 萬本儒(Ben-Zu Wan),陳浩銘(Hao-Ming Chen),鍾博文(Po-Wen Chung) | |
dc.subject.keyword | 甘油,丙烯酸,脫水氧化反應,SBA-15, | zh_TW |
dc.subject.keyword | Glycerol,Acrylic acid,Oxidehydration,SBA-15, | en |
dc.relation.page | 62 | |
dc.identifier.doi | 10.6342/NTU201703844 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2017-08-18 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
顯示於系所單位: | 化學系 |
文件中的檔案:
檔案 | 大小 | 格式 | |
---|---|---|---|
ntu-106-1.pdf 目前未授權公開取用 | 3.76 MB | Adobe PDF |
系統中的文件,除了特別指名其著作權條款之外,均受到著作權保護,並且保留所有的權利。