Citation: CHEN Hong-Li, ZHU Shu-Yan, HE Jian-Qin, WANG Yi-Meng. Synthesis of Micro-Sized MEL-Type Zeolite Aggregates[J]. Acta Physico-Chimica Sinica, ;2014, 30(9): 1727-1735. doi: 10.3866/PKU.WHXB201407081 shu

Synthesis of Micro-Sized MEL-Type Zeolite Aggregates

1.
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry, East China Normal University, Shanghai 200062, P. R. China

Received Date: 22 April 2014
Available Online: 8 July 2014
Fund Project:

Hierarchical micro-sized zeolite aggregates with the MEL structure were prepared hydrothermally froma tetrabutylammoniumhydroxide (TBAOH)-tetraethyl orthosilicate (TEOS)-H₂O system. The obtained microsized silicalite-2 microspheres had sizes larger than 10 μm, high BET surface area (460 m²·g^-1), and large pore volume (0.74 cm³·g^-1). The formation of micro-sized spheres alleviates preparation and application difficulties. The presence of inter-crystalline mesopores originating from the spontaneous assembly of nano-sized primary particles during hydrothermal synthesis gives the advantages of nanoparticles, reducing diffusion limitations. The introduction of titanium does not strongly affect the morphology and textural properties of the MEL-type zeolite, which are quite similar to those of silicalite-2 aggregates. The micro-sized titanium silicalite-2 (TS-2) microspheres showed comparable catalytic activity in phenol hydroxylation to that of titanium silicalite-1 (TS-1) of size 100-200 nm, and were easily recovered by traditional filtration, simplifying the separation and recovery compared with nano-sized TS-1.
- MEL structure,
- Nano-sized particle,
- Aggregate,
- Hierarchical porosity,
- Hydroxylation of phenol
1. [1]
  
  (1) Corma, A. Chem. Rev. 1995, 95, 559. doi: 10.1021/cr00035a006
2. [2]
  (2) Rabo, J. A.; Schoonover, M.W. Appl. Catal. A: Gen. 2001, 222, 261. doi: 10.1016/S0926-860X(01)00840-7
3. [3]
  (3) Kokotailo, G. T.; Lawton, S. L.; Olson, D. H.; Meier,W. M. Nature 1978, 272, 437. doi: 10.1038/272437a0
4. [4]
  (4) Choi, M.; Na, K.; Kim, J.; Sakamoto, Y.; Terasaki, O.; Ryoo, R. Nature 2009, 461, 246.
5. [5]
  (5) Yue, M. B.; Yang, N.;Wang, Y. M. Acta Phys. -Chim. Sin. 2012, 28, 2115. [岳明波, 杨娜, 王一萌. 物理化学学报, 2012, 28, 2115.] doi: 10.3866/PKU.WHXB201206141
6. [6]
  (6) Kokotailo, G. T.; Chu, P.; Lawton, S. L.; Meier,W. M. Nature 1978, 275, 119. doi: 10.1038/275119a0
7. [7]
  (7) Yu, Q. J.; Cui, C. Y.; Zhang, Q.; Chen, J.; Li, Y.; Sun, J. P.; Li, C. Y.; Cui, Q. K.; Yang, C. H.; Shan, H. H. J. Energy Chem. 2013, 22, 761. doi: 10.1016/S2095-4956(13)60101-1
8. [8]
  (8) Chen, H. L.; Ding, J.;Wang, Y. M. New J. Chem. 2014, 38, 308. doi: 10.1039/c3nj00785e
9. [9]
  (9) Babu, G. P.; Hegde, S. G.; Kulkarni, S. B.; Ratnasamy, P. J. Catal. 1983, 81, 471. doi: 10.1016/0021-9517(83)90185-9
10. [10]
  (10) Kaeding,W.W.; Chu, C.; Young, L. B.; Butter, S. A. J. Catal. 1981, 69, 392.
11. [11]
  (11) Young, L. B.; Butter, S. A.; Kaeding,W.W. J. Catal. 1982, 76, 418. doi: 10.1016/0021-9517(82)90271-8
12. [12]
  (12) Ralph, M, D. J. Catal. 1982, 77, 304. doi: 10.1016/0021-9517(82)90173-7
13. [13]
  (13) Védrine, J. C.; Auroux, A.; Dejaifve, P.; Ducarme, V.; Hoser, H.; Zhou, S. J. Catal. 1982, 73, 147. doi: 10.1016/0021-9517(82)90089-6
14. [14]
  (14) Anderson, J. R.; Foger, K.; Mole, T.; Rajadhyaksha, R. A.; Sanders, J. V. J. Catal. 1979, 58, 114. doi: 10.1016/0021-9517(79)90250-1
15. [15]
  (15) Chang, C. D.; Silvestri, A. J. J. Catal. 1977, 47, 249. doi: 10.1016/0021-9517(77)90172-5
16. [16]
  (16) Meisel, S. L. Chem. Technol. 1976, 6, 86.
17. [17]
  (17) Corma, A. Chem. Rev. 1997, 97, 2373. doi: 10.1021/cr960406n
18. [18]
  (18) Tian, Y.; Li, Y. D. Journal of Chemical Industry and Engineering 2013, 64 (2), 393. [田野, 李永丹. 化工学报, 2013, 64 (2), 393.]
19. [19]
  (19) Song,W.; Justice, R. E.; Jones, C. A.; Grassian, V. H.; Larsen, S. C. Langmuir 2004, 20, 8301. doi: 10.1021/la049516c
20. [20]
  (20) Tosheva, L.; Valtchev, V. P. Chem. Mater. 2005, 17, 2494. doi: 10.1021/cm047908z
21. [21]
  (21) Tokay, B.; Somer, M.; Erdem-Senatalar, A.; Schuth, F.; Thompson, R.W. Microporous Mesoporous Mat. 2009, 118, 143. doi: 10.1016/j.micromeso.2008.08.034
22. [22]
  (22) Cundy, C. S.; Forrest, J. O.; Plaisted, R. J. Microporous Mesoporous Mat. 2003, 66, 143. doi: 10.1016/j.micromeso.2003.08.021
23. [23]
  (23) Cundy, C. S.; Forrest, J. O. Microporous Mesoporous Mat. 2004, 72, 67. doi: 10.1016/j.micromeso.2004.04.006
24. [24]
  (24) Mintova, S.; Gilson, J. P.; Valtchev, V. Nanoscale 2013, 15, 6693.
25. [25]
  (25) Davis, T. M.; Drews, T. O.; Ramanan, H.; He, C.; Dong, J.; Schnablegger, H.; Katsoulakis, M. A.; Kokkoli, E.; McCormick, A. V.; Penn, R. L.; Tsapatsis, M. Nature Mater. 2006, 5, 400. doi: 10.1038/nmat1636
26. [26]
  (26) Fang, Y. M.; Hu, H. Q.; Chen, G. H. Chem. Mater. 2008, 20, 1670. doi: 10.1021/cm703265q
27. [27]
  (27) Liu, S. P.; Yue, M. B.;Wang, Y. M. Acta Phys. -Chim. Sin. 2010, 26, 2224. [刘树萍, 岳明波, 王一萌. 物理化学学报, 2010, 26, 2224.] doi: 10.3866/PKU.WHXB20100806
28. [28]
  (28) Zhang, X. Y.; Liu, D. X.; Xu, D. D.; Asahina, S.; Cychosz, K. A.; Agrawal, K. V.; AlWahedi, Y.; Bhan, A.; Al Hashimi, S.; Terasaki, O.; Thommes, M.; Tsapatsis, M. Science 2012, 336, 1684. doi: 10.1126/science.1221111
29. [29]
  (29) Dong, J. P.; Zou, J.; Long, Y. C. Microporous Mesoporous Mat. 2003, 57, 9. doi: 10.1016/S1387-1811(02)00530-9
30. [30]
  (30) Uzcategui, D.; nzalez, G. Catal. Today 2005, 107-108, 901.
31. [31]
  (31) CiZmek, A.; Subotica, B.; Kralj, D.; Babic-Ivancic, V.; Tonejc, A. Microporous Mater. 1997, 12, 267. doi: 10.1016/S0927-6513(97)00075-8
32. [32]
  (32) Mintova , S.; Petkov, N.; Karaghiosoff, K.; Bein, T. Microporous Mesoporous Mat. 2003, 50, 121.
33. [33]
  (33) Jansen, J. C.; van der Gaag, F. J.; van Bekkum, H. Zeolites 1984, 4, 369. doi: 10.1016/0144-2449(84)90013-7
34. [34]
  (34) Coudurier, G.; Naccache, C.; Vedrine, J. C. J. Chem. Soc. Chem. Commun. 1982, 1413.
35. [35]
  (35) Scarano, D.; Zecchina, A.; Bordiga, S.; Geobaldo, F.; Spoto, G.; Petrini, G.; Leofanti, G.; Padovan, M.; Tozzola, G. J. Chem. Soc. Faraday Trans. 1993, 89, 4123. doi: 10.1039/ft9938904123
36. [36]
  (36) Zecchina, A.; Bordiga, S.; Spoto, G.; Marchese, L.; Petrini, G.; Leofanti, G.; Padovan, M. J. Phys. Chem. 1992, 96, 4985. doi: 10.1021/j100191a047
37. [37]
  (37) Soulard, M.; Bilger, S.; Kessler, H.; Guth, J. L. Zeolites 1987, 7, 463. doi: 10.1016/0144-2449(87)90016-9
38. [38]
  (38) Parker, L. M.; Bibby, D. M.; Patterson, J. E. Zeolites 1984, 4, 168. doi: 10.1016/0144-2449(84)90056-3
39. [39]
  (39) Boxhoorn, G.; Kortbeek, A. G. T. G.; Hays, G. R.; Alma, N. C. M. Zeolites 1984, 4, 15. doi: 10.1016/0144-2449(84)90066-6
40. [40]
  (40) Chezeau, J. M.; Delmotte, L.; Guth, J. L.; Gabelica, Z. Zeolites 1991, 11, 598. doi: 10.1016/S0144-2449(05)80011-9
41. [41]
  (41) Nagy, J. B.; Gabelica, Z.; Derouane, E. G. Chem. Lett. 1982, 11, 1105.
42. [42]
  (42) Nagy, J. B.; Gabelica, Z.; Derouane, E. G. Zeolites 1983, 3, 43. doi: 10.1016/0144-2449(83)90084-2
43. [43]
  (43) Ricchiardi, G.; Damin, A.; Bordiga, S.; Lamberti, C.; Spanò, G.; Rivetti, F.; Zecchina, A. J. Am. Chem. Soc. 2001, 123, 11409. doi: 10.1021/ja010607v
44. [44]
  (44) Wu, P.; Tatsumi, T.; Komatsu, T.; Yashima, T. J. Phys. Chem. B 2001, 105, 2897.
45. [45]
  (45) Thangaraj, A.; Kumar, R.; Mirajkar, S. P.; Ratnasamy, P. J. Catal. 1991, 130, 1. doi: 10.1016/0021-9517(91)90086-J
46. [46]
  (46) Thangaraj, A.; Kumar, R.; Ratnasamy, P. J. Catal. 1991, 131, 294. doi: 10.1016/0021-9517(91)90347-7
47. [47]
  (47) Romano, U.; Esposito, A.; Maspero, F.; Neri, C.; Clerici, M. G. Stud. Surf. Sci. Catal. 1990, 55, 33. doi: 10.1016/S0167-2991(08)60131-7
48. [48]
  (48) Tuel, A.; Taarit, Y. B. Appl. Catal. A: Gen. 1993, 102, 69. doi: 10.1016/0926-860X(93)85155-I
49. [49]
  (49) van der Pol, A. J. H. P.; Verduyn, A. J.; van Hooff, J. H. C. Appl. Catal. A: Gen. 1992, 92, 113. doi: 10.1016/0926-860X(92)80310-9
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