NHỮNG ĐÓNG GÓP MỚI CỦA LUẬN ÁN
1. Chế tạo được vật liệu siêu acid HPA cố định trên chất mang mao quản trung bình biến tính Al-SBA-15 và chất mang đa mao quản ZSM-5/SBA-15. Đây là các chất mang có diện tích bề mặt lớn, có khả năng gắn kết các phân tử HPA trên bề mặt để tăng sự tiếp xúc của các tâm acid với các chất phản ứng, đồng thời vẫn duy trì được lực acid của HPA (không ảnh hưởng đến tính siêu acid của HPA).
2. HPA được cố định trên các chất mang Al-SBA-15 and ZSM-5/SBA-15 qua tương tác với các nhóm NH4+, Cs+ tạo ra vật liệu có lực và tâm acid mạnh, độ bền gắn kết HPA tốt, độ bền hoạt tính cao. Vật liệu này được sử dụng làm xúc tác acid hiệu quả trong phản ứng tổng hợp fructone có chất phản ứng phân cực.
3. Nghiên cứu so sánh với các xúc tác acid đồng thể như acid sulfuric, acid p-toluenesulfonic, acid HPA không gắn trên chất mang cho thấy, các hệ xúc tác dị thể HPA/Al-SBA-15 và HPA/ZSM-5/SBA-15 tổng hợp được có hoạt tính xúc tác tốt hơn các acid đồng thể và có thể thu hồi tái sử dụng nhiều lần. Do đó, các vật liệu này có khả năng trở thành xúc tác dị thể thay thế cho các xúc tác acid đồng thể ứng dụng trong các phản ứng tổng hợp hữu cơ có chất phản ứng phân cực.
DANH MỤC CÁC CÔNG TRÌNH ĐÃ CÔNG BỐ
1. Thi Hanh Truong, Van Cuong Do, Ngoc Mai Do, Tran Quang Hung, Huan Van Doan, Thi Nhiem Nguyen, Thi Hai Doan, Thi Hoai Nam Le, Tuyen Van Nguyen, Long Giang Bach, Quang Vinh Tran, Study on the HPA immobilisation on Al- SBA-15 support over Brønsted groups, Molecular Catalysis, 2019, 478, 110571. (Q1, IF = 3.687)
2. Quang Vinh Tran, Thi Hanh Truong, Tran Quang Hung, Huan V. Doan, Xuan Nui Pham, Nam Thi Hoai Le, Long Giang Bach & Van Tuyen Nguyen, Preparation and testing of ceasium Brønsted ion-exchanged Al-SBA-15 supported heteropoly acid as heterogeneous catalyst in the fructone fragrancy synthesis, Journal of Porous Materials, 2020, 27(6), 1745-1754. (Q2, IF = 2.183)
3. Truong Thi Hanh, Do Van Cuong, Do Ngoc Mai, Nguyen Thi Nhiem, Doan Thi Hai, Le Thi Hoai Nam and Tran Quang Vinh, Preparation of 12- phosphotungstic acid immobilized on ZSM-5/SBA-15 support for Fructone fragrancy synthesis, Vietnam Journal of Catalysis and Adsorption, 2019, 8 (2), 99-107.
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Hàm Lượng Hpa Trên Chất Mang Của Các Mẫu Khác Nhau. -
Đường Cong Phân Bố Mao Quản Của Vật Liệu Hzsc Và Hpa/hzsc. -
Đánh Giá Hoạt Tính Của Xúc Tác Hpa/hzsc Với Các Xúc Tác Đồng Thể -
Nghiên cứu tổng hợp xúc tác dị thể siêu acid cố định trên các chất mang Al-SBA-15 và ZSM-5/SBA-15 ứng dụng trong phản ứng tổng hợp fructone - 17
Xem toàn bộ 144 trang tài liệu này.
4. Do Van Cuong, Truong Thi Hanh, Do Ngoc Mai, Nguyen Thi Nhiem, Doan Thi Hai, Le Thi Hoai Nam and Tran Quang Vinh, Nghiên cứu ảnh hưởng của dạng ion bù trừ điện tích khung mạng đến khả năng giữ acid 12- phosphotungstic trên vật liệu Al-SBA-15 và ứng dụng làm xúc tác cho phản ứng tổng hợp chất tạo hương Fructon, Vietnam Journal of Catalysis and Adsorption, 2019, 8(3), 08-15.
5. Trương Thị Hạnh, Đỗ Văn Cường, Đỗ Ngọc Mai, Nguyễn Thị Nhiệm, Đoàn Thị Hải, Trần Quang Hưng, Lê Thị Hoài Nam và Trần Quang Vinh, Nghiên cứu chế tạo và so sánh hoạt tính của vật liệu xúc tác dị đa acid được cố định trên các vật liệu vô cơ mao quản Al-SBA-15 và ZSM-5/SBA-15 trong phản ứng tổng hợp chất tạo hương fructon, Tạp chí Hóa học, 2019, 57 (6E1,2), 174- 178.
6. Đỗ Văn Cường, Trương Thị Hạnh, Đỗ Ngọc Mai, Nguyễn Thị Nhiệm, Đoàn Thị Hải, Lê Thị Hoài Nam và Trần Quang Vinh, Nghiên cứu chế tạo xúc tác HPA cố định trên chất mang Al-SBA-15 được trao đổi ion với Cs+ cho phản ứng tổng hợp chất tạo hương Fructon, Tạp chí Hóa học, 2019, 57 (6E1,2), 179- 183.
TÀI LIỆU THAM KHẢO
1. E. Rafiee, S. Eavani, Heterogenization of heteropoly compounds: A review of the structure and synthesis, RSC Adv., 2016, 6 (52), 46433– 46466.
2. https://en.wikipedia.org/wiki/Heteropolymetalate
3. L.D. Chavan, Catalytic and Structural Studies of Some Heteropoly Acids and Polyoxometalates, Doctoral Thesis, Shodhganga, 2017.
4. M.J. Silva, C.M. OliveFT-IRa, Catalysis by Keggin Heteropolyacid Salts, Current Catalysis, 2018, 7, 26–34.
5. L.E. Briand, G.T. Baronetti, H.J. Thomas, The state of the art on Wells–Dawson heteropoly-compounds A review of theFT-IR properties and applications, Applied Catalysis A: General, 2003, 256, 37–50.
6. Bạch Thị Tâm, Nghiên cứu tổng hợp và đặc trưng xúc tác siêu acid dị thể dùng cho phản ứng ester hóa acid 2-keto-l-gulonic trong quá trình tổng hợp vitamin C, Luận án Tiến sĩ, Hà Nội, 2015.
7. F. Cavani, Heteropolycompound-based catalysts: A blend of acid and oxidizing properties, Catalysis Today, 1998, 41, 73–86.
8. Noritaka Mizuno, Makoto Misono, Heteropolyanions in catalysis, Journal of Molecular Catalysis, 1994, 86, 319– 342.
9. N. Mizuno, M. Misono, Heterogeneous Catalysis, Chem Rev, 1998, 98, 199- 218.
10. M.N Timfeeva, Acid catalysis by heteropoly acids, Applied Catalysis A: General, 2003, 256, 19–35.
11. E. Rafiee, S. Eavani, F.K. Nejad, M. Joshaghani, Cs2.5H0.5PW12O40 catalyzed diastereoselective synthesis of b-amino ketones via three component Mannich-type reaction in water, Tetrahedron, 2010, 66, 6858–6863.
12. Y. Iwase, S. Sano, L. Mahardiani, R. Abe, Y. Kamiya, Bimodal cesium hydrogen salts of 12-tungstosilicic acid, CsxH4-xSiW12O40, as highly active solid acid catalysts for transesterification of glycerol tributyrate with methanol, Journal of Catalysis, 2014, 318, 34–42.
13. V.Z. Sasca, O. Verdes, L. Avram, A. Popa, A. Erdőhelyi, A. Oszko, The CsxH3 − xPW12O40 catalysts microstructure model, Applied Catalysis A: General, 2013, 451, 50–57.
14. A. Dolbecq, E. Dumas, C. R. Mayer, P. Mialane, Hybrid Organic- Inorganic
Polyoxometalate Compounds: From Structural Diversity to Applications, Chemical Reviews, 2010, 110, 6009– 6048.
15. Q.Y. Liu, W.L. Wu, J. Wang, X.Q. Ren & Y.R. Wang, Characterization of 12-tungstophosphoric acid impregnated on mesoporous silica SBA-15 and its
catalytic performance in isopropylation of naphtalen with isopropanol, Microporous and Mesoporous Materials, 2004, 76, 51–60.
16. V. Brahmkhatri, A. Patel, 12-Tungstophosphoric acid anchored to SBA-15: An efficient, envFT-IRonmentally benign reusable catalysts for biodiesel production by esterification of free fatty acids, Applied Catalysis A: General, 2011, 403, 161–172.
17. A. Patel, V. Brahmkhatri, Kinetic study of oleic acid esterification over 12-tungstophosphoric acid catalyst anchored to different mesoporous silica supports, Fuel Processing Technology, 2013, 113, 141–149.
18. L. Frattini, M. A. Isaacs, C. M.A. Parlett, K. Wilson, G. Kyriakou, A.F. Lee, Support enhanced -pinene isomerization over HPW/SBA-15, Applied Catalysis B: EnvFT- IRonmental, 2017, 200, 10–18 .
19. B. Sulikowski, R. Rachwalik, Catalytic properties of heteropoly acid/zeolite hybrid materials: Toluenee disproportionation and transalkylation with 1,2,4-trimethylbenzene, Appl. Catal. A Gen., 2003, 256, 173–182.
20. J. Haber, K. Pamin, L. Matachowski, D. Mucha, Catalytic performance of the dodecatungstophosphoric acid on different supports, Appl. Catal. A Gen., 2003, 256, 141–152.
21. A. Patel, N. Narkhede, 12-tungstophosphoric acid anchored to zeolite Hβ: Synthesis, characterization, and biodiesel production by esterification of oleic acid with methanol, Energy Fuels 2012, 26, 6025–6032.
22. N. Narkhede, A. Patel, Biodiesel production by esterification of oleic acid and transesterification of soybean oil using a new solid acid catalyst comprising 12-tungstosilicic acid and zeolite Hβ, Ind. Eng. Chem. Res. 2013, 52, 13637–13644.
23. M. Srinivas, R. Sree, G. Raveendra, C.R. Kumar, P.S.S. Prasad, N. Lingaiah, Selective etherification of glycerol with tert-butanol over 12-tungstophosphoric acid catalysts supported on Y-zeolite, Indian J. Chem., 2014, 53A, 524–529.
24. M. Moosavifar, An appropriate one-pot synthesis of dihydropyrimidinones catalyzed by heteropoly acid supported on zeolite: An efficient and reusable catalyst for the Biginelli reaction, Comptes Rendus Chimie, 2012, 15, 444– 447.
25. C.L. Marchena, R.A. Frenzel, S. Gomez, C. Saux, L.B. Pierella, L.R. Pizzio; Tungstophosphoric acid immobilized on ammonium Y and ZSM-5 zeolites: Synthesis, characterization and catalytic evaluation. Appl. Catal. B EnvFT-IRon. 2013, 130, 187–196.
26. C.L. Marchena, S. Gomez, C. Saux, L.B. Pierella, L.R. Pizzio, Synthesis, characterization and catalytic evaluation of tungstophosphoric acid immobilized on Y zeolite. In Advanced Oxidation Technologies Sustainable Solutions for EnvFT-
112
IRonmental Treatments in Sustainable Energy Developments, CRC Press: Leiden, The Netherlands, 2014, 9, 43–57.
27. C.L. Marchena, S. Gomez, C. Saux, L.B. Pierella, L.R. Pizzio, Tungstophosphoric acid heterogenized onto NH4ZSM-5 as an efficient and recyclable catalyst for the photodegradation of dyes, Quim. Nova, 2015, 38, 518–525.
28. A. Alsalme, A.A. Alsharif, H. Al-Enizi, M. Khan, S.G. Alshammar, Probing the Catalytic Efficiency of Supported Heteropoly Acids for Esterification: Effect of Weak Catalyst Support Interactions, Journal of Chemistry, 2018, 2018, 1– 10.
29. L. Yang, Y. Qia, X. Yuanb, J. Shenb, J. Kimc, DFT-IRect synthesis, characterization and catalytic application of SBA-15 containing heteropolyacid, Journal of Molecular Catalysis A: Chemical, 2005, 229, 199– 205.
30. B.C. Gagea, Y. Lorgouilloux, Y. Altintas, P.A. Jacobs, & J.A. Martens, Bifunctional conversion of n-decane over HPW heteropoly acid incorporated into SBA-15 during synthesis, Journal of Catalysis, 2009, 265(1), 99– 108.
31. Y. Guo, K. Li, X. Yu, J. H. Clark, Mesoporous H3PW12O40-silica composite: Efficient and reusable solid acid catalyst for the synthesis of diphenolic acid from levulinic acid, Applied Catalysis B: EnvFT-IRonmental, 2008, 81, 182– 191.
32. J.E. CastanheFT-IRo, I.M. Fonseca, A.M. Ramos, J. Vital, Tungstophosphoric acid immobilised in SBA-15 as an efficient heterogeneous acid catalyst for the conversion of terpenes and free fatty acids, Microporous and Mesoporous Materials, 2017, 249, 16– 24.
33. X. Sheng, J. Kong, Y. Zhou, Y. Zhang, Z. Zhang, S. Zhou, DFT-IRect synthesis, characterization and catalytic application of SBA-15 mesoporous silica with heteropolyacid incorporated into theFT-IR framework, Microporous and Mesoporous Materials, 2014, 187, 7– 13.
34. T. Pinto, K. Szeto, N. Oueslati, N. Essayem, V. Dufaud and F. Lefebvre, Comparison of the Acidity of Heteropolyacids Encapsulated in or Impregnated on SBA-15, Oil & Gas Science and Technology – Rev. IFP Energies nouvelles, 2016, 71, 25– 38.
35. N.K. Kala Raj, S.S. Deshpande, R.H. Ingle, T. Raja and P. Manikandan, Heterogenized molybdovanadophosphoric acid on amine-functionalized SBA-15 for selective oxidation of alkenes, Catalysis Letters, 2004, 98 (4), 217– 223.
36. L. Zhao, Y. Chi, Q. Yuan, N. Li, W. Yan and X. Li, Phosphotungstic acid anchored to amino–functionalized core–shell magnetic mesoporous silica microspheres: A magnetically recoverable nanocomposite with enhanced photocatalytic activity, Journal of Colloid and Interface Science., 2013, 390(1), 70– 77.
113
37. Ge Li, B. Wang, Q. Sun, W.Q. Xu, Y. Han, Adsorption of lead ion on amino- functionalized fly-ash-based SBA-15 mesoporous molecular sieves prepared via two- step hydrothermal method, Microporous and Mesoporous Materials, 2017, 252, 105–115.
38. A. Popa, V. Sasca, O. Verdes, C. Ianasi, R. Banica, Heteropolyacids anchored on amino-functionalized MCM-41 and SBA-15 and its application to the ethanol conversion reaction, J Therm Anal Calorim, 2017, 127, 319–334.
39. H. Liu, N. Xue, L. Peng, X. Guo, W. Ding, Y. Chen, The hydrophilic/hydrophobic effect of porous solid acid catalysts on mixed liquid phase reaction of esterification, Catalysis Communications, 2009, 10, 1734–1737.
40. X. N. Pham, D. L. Tran, T. D. Pham, Q. M. Nguyen, V. T. Tran Thi, H. Doan Van, One-step synthesis, characterization and oxidative desulfurization of 12-tungstophosphoric heteropolyanions immobilized on amino functionalized SBA- 15, Advanced Powder Technology, 2018, 29(1), 58– 65.
41. X.N. Pham, H.V. Doan, Activity and stability of amino-functionalized SBA-15 immobilized 12-tungstophosphoric acid in the oxidative desulfurization of a diesel fuel model with H2O2 , Chemical Engineering Communications, 2019, 206, 1139–1151.
42. K.M. Parida, S. Rana, S. Mallick, D. Rath, Cesium salts of heteropoly acid immobilized mesoporous silica: An efficient catalyst for acylation of anisole, Journal of Colloid and Interface Science, 2010, 350, 132–139.
43. P.M. Rao, A. Wolfson, M.V. Landau, M. Herskowitza, Efficient immobilization of 12-tungstophosphoric acid catalyst at the surface of silica support grafted with alumina, Catalysis Communication, 2004, 5(6), 327–331.
44. M. Chamack, A.R. Mahjoub, H. Aghayan, Cesium salts of tungsten-substituted molybdophosphoric acid immobilized onto platelet mesoporous silica: Efficient catalysts for oxidative desulfurization of dibenzothiophene, Chemical Engineering Journal, 2014, 255, 686– 694.
45. F. Jing, B. Katryniok, E. Bordes-Richard, S. Paul, Improvement of the catalytic performance of supported (NH4)3HPMo11VO40 catalysts in isobutane selective oxidation, Catalysts Today, 2013, 203, 32– 39.
46. F. Lriefebvre, Synthesis, Characterization and Applications in Catalysis of Polyoxometalate/Zeolite Composites, Inorganics, 2016, 4, 13– 36.
47. S. Anandan, S.Y. Ryu, W.J. Cho, M. Yoon, Heteropolytungstic acid (H3PW12O40) - encapsulated into the titanium-exchanged HY (TiHY) zeolite: A novel photocatalyst
114
for photoreduction of methyl orange, J. Molercular Catalysis A: Chemical, 2003, 195, 201– 208.
48. S. R. Mukai, L. Lin, T. Masuda, K. Hashimoto, Key factors for the encapsulation of Keggin-type heteropoly acids in the supercages of Y-type zeolit, Chemical Engineering Science, 2001, 56, 799– 804.
49. S. R. Mukai, T. Masuda, I. Ogino, K. Hashimoto, Preparation of encaged heteropoly acid catalyst by synthesizing 12-molybdophosphoric acid in the supercages of Y-type zeolite, Applied Catalysis A: General, 1997, 165, 219– 226.
50. H. Wang, R. Wang, Performance evalutaion of “ship-in-the-bottle” type heteropoly acid encaged Y-type zeolite as catalyst for oxidative desulfurization, Collect. Czechoslov. Chem. Commun., 2011, 76, 1595– 1605.
51. R. Wei, M. Guo, J. Wang, Preparation, characterization and catalytic behavior of 12-molybdophosphoric acid encapsulated in the supercage of Cs+ -exchanged Y zeolite, Chin. J. Chem. Eng., 2009, 17, 58– 63.
52. L. Chen, X. Wang, X. Guo, H. Guo, H. Liu, Y. Chen, In situ nanocrystalline HZSM- 5 zeolites encaged heteropoly acid H3PMo12O40 and Ni catalyst for hydroconversion of n-octane, Chem. Eng. Sci., 2007, 62, 4469– 4478.
53. B. Sulikowski, J. Haber, A. Kubacka, K. Pamin, Z. Olejniczak, J. Ptaszynski, Novel “ship-in-the-bottle” type catalyst: Evidence for encapsulation of 12-tungstophosphoric acid in the supercage of synthetic faujasite, Catal. Lett., 1996, 39, 27– 31.
54. Z. Olejniczak, B. Sulikowski, A. Kubacka, M. Gasior, Heterogenization of 12-tungstophosphoric acid on stabilized zeolite Y, Top. Catal., 2000, 11, 391–400.
55. A.D. Newman, A.F. Lee, K. Wilson, N.A. Young, On the Active Site in H3PW12O40/SiO2 Catalysts for Fine Chemical Synthesis, Catalysis Letter, 2005, 102, 45– 50.
56. D. Zhao, J. Feng, Q. Huo, N. Melosh, G.H. Fredrickson, B.F. Chmelka and G.D. Stucky, Tribock Copolymer Syntheses of Mesoporous Silica with Periodic 50 to 300 Angstrom Pores, Science, 1998, 279, 548– 552.
57. K. Cassiers, T. Linssen, M. Mathieu, M. Benjelloun, A Detailed Study of Thermal, Hydrothermal, and Mechanical Stabilities of a Wide Range of Surfactant Assembled Mesoporous Silicas, Chem. Mater. 2002, 14, 2317– 2324.
58. Y. Ahn, S.-Y. Kwak, Functional mesoporous silica with controlled pore size for selective adsorption of free fatty acid and chlorophyll, Microporous and Mesoporous Materials, 2020, 306, 110410.
115
59. V.T. Hoang, Q. Huang, M. Eic, Structure and Diffusion Characterization of SBA-15 materials, Langmur, 2005, 21, 2051– 2057.
60. B. J. Scott, G. WFT-IRnsberger, G.D. Stucky, Mesoporous and Mesostructured Materials for Optical Applications, Chemistry of Materials, 2001, 13, 3140– 3150.
61. P. Yang, G. WFT-IRnsberger, H.C. Huang, S.R. Cordero, M.D. McGehee, B. Scott,
T. Deng, G.M. Whitesides, B.F. Chmelka, S.K. Buratto, G.D. Stucky, MFT-IRrorless Lasing from Mesostructured Waveguides Patterned by Soft Lithography, Science 2000, 287, 465– 467.
62. A.J. Schwanke, R. Balzer and S. Pergher, Microporous and Mesoporous Materials from Natural and Inexpensive Sources, Handbook of Ecomaterials, 2017, 3379–3399.
63. A. Ungureanu, B. Dragoi, V. Hulea, T. Cacciaguerra, D. Meloni, V. Solinas, E. Dumitriu, Effect of aluminium incorporation by the ‘‘pH-adjusting’’ method on the structural, acidic and catalytic properties of mesoporous SBA-15, Microporous and Mesoporous Materials, 2012, 163, 51– 64.
64. A.J.J. Koekkoek , J.A. R. Veen, P.B. Gerrtisen, P. Giltay, P.C.M.M. Magusin, E.J.M. Hensen, Brønsted acidity of Al/SBA-15, Microporous and Mesoporous Materials, 2012, 151, 34– 43.
65. J.S. Yun, S.-E. Bazardorj, S.-K. IHM, Acidity Control of Al-SBA-15 and Its Effect on the Catalytic Performance for Steam Reforming of Dimethyl Ether, Journal of Chemical Engineering of Japan, 2009, 42(1), 180–184.
66. P. Bhange, D.S. Bhange, S. Pradhan, V. Ramaswamy, DFT-IRect synthesis of well- ordered mesoporous Al-SBA-15 and its correlation with the catalytic activity, Applied Catalysis A: General, 2011, 400, 176– 184.
67. J.M.R. Gallo, C. Bisio, G. Gatti, L. Marchese, H.O. Pastore, Physicochemical Characterization and Surface Acid Properties of Mesoporous [Al]-SBA-15 Obtained by DFT-IRect Synthesis, LangmuFT-IR, 2010, 26, 5791– 5800.
68. G. M. Kumaran, S. Garg, K. Soni, M. Kumar, J.K. Gupta, L.D. Sharma, K.S. Rama Rao, G. M. Dhar, Synthesis and characterization of acidic properties of Al-SBA-15 materials with varying Si/Al ratios, Microporous and Mesoporous Materials, 2008, 114, 103–109.
69. S. Zeng, J. Blanchard, M. Breysse, Y. Shi, X. Shu, H. Nie, D. Li, Post-synthesis alumination of SBA-15 in aqueous solution: A versatile tool for the preparation of acidic Al-SBA-15 supports, Micro. Mesoporous Material, 2005, 85, 297– 304.
70. M.G. Cazalilla, J.M. Mérida-Robles, A. Gurbani, E. Rodríguez-Castellon, A. Jiménez-López, Characterization and acidic properties of Al-SBA-15 materials