Journal of Materials Science

, Volume 44, Issue 14, pp 3777–3783 | Cite as

In situ assembly of ZSM-5 nanocrystals into micro-sized single-crystal-like aggregates via acid-catalyzed hydrolysis of tetraethylorthosilicate

  • Jing Gu
  • Yajing Wu
  • Jun WangEmail author
  • Youdong Lu
  • Xiaoqian Ren


ZSM-5 aggregates were synthesized with the silica source tetraethylorthosilicate (TEOS) being hydrolyzed at acidic conditions to produce siliceous precursors, followed by the addition of aluminum sulfate and tetrapropyl ammonium bromide (TPABr), and with the resulting gel mixture being hydrothermally crystallized at basic conditions. The obtained products were characterized by XRD, SEM, and N2 adsorption. Well crystallized ZSM-5 can be successfully synthesized through the sulfuric acid-catalyzed hydrolysis of TEOS within a short crystallization time 35 h. The thus produced micro-sized single-crystal-like zeolite ZSM-5 aggregates (10 μm) are made of uniformly distributed nanocrystals with sizes of about 200 nm. Moreover, by adjusting the hydrothermal reaction parameters, such as increasing the crystallization temperature, the TPABr/SiO2 ratio and the pH value of reaction solution, the crystallization is accelerated substantially. Also, the moderate H2O/SiO2 molar ratio of 20–60 in the synthesis mixture can lead to pure ZSM-5, and yet the optimal ratio is 40.


Zeolite Crystallization Temperature Crystallization Time Silica Source Silica Precursor 



This study is supported by the Key Natural Science Foundation for Universities of Jiangsu Province (06KJA53012), National Natural Science Foundation of China (No. 20776069) and Program for Changjiang Scholars and Innovative Research Team in University (PCSIRT 0732).

Supplementary material

10853_2009_3508_MOESM1_ESM.doc (1.1 mb)
Supplementary material 1 (DOC 1106 kb)


  1. 1.
    Argauer RJ, Landolt GR (1972) US Patent 3702866Google Scholar
  2. 2.
    Derouane EG, Determmerie S, Gabelica Z, Blom N (1981) Appl Catal 1:201CrossRefGoogle Scholar
  3. 3.
    Hölderich W, Hesse M, Näumann F (1988) Angew Chem Int Ed 27:226CrossRefGoogle Scholar
  4. 4.
    Kumar N, Lindfors LE, Byggningsbacka R (1996) Appl Catal A Gen 139:189CrossRefGoogle Scholar
  5. 5.
    Byggningsbacka R, Kumar N, Lindfors LE (1998) J Catal 178:611CrossRefGoogle Scholar
  6. 6.
    Rajagopalan K, Peters AW, Edwards GC (1986) Appl Catal 23:69CrossRefGoogle Scholar
  7. 7.
    Camblor MA, Corma A, Martínez A, Mocholí FA, Pariente JP (1989) Appl Catal 55:65CrossRefGoogle Scholar
  8. 8.
    Vogel B, Schneider C, Klemm E (2002) Catal Lett 79:107CrossRefGoogle Scholar
  9. 9.
    Davis ME (2002) Nature 417:813CrossRefGoogle Scholar
  10. 10.
    Zheng Z, Hall AS, Guliants VV (2008) J Mater Sci 43:2499. doi: CrossRefGoogle Scholar
  11. 11.
    Tosheva L, Valtchev VP (2005) Chem Mater 17:2494CrossRefGoogle Scholar
  12. 12.
    Mintova S, Voltchev V (2002) Microporous Mesoporous Mater 55:171CrossRefGoogle Scholar
  13. 13.
    Mohamed RM, Aly HM, El-Shahat MF, Ibrahim IA (2005) Microporous Mesoporous Mater 79:7CrossRefGoogle Scholar
  14. 14.
    Reding G, Mäurer T, Kraushaar-Czarnetzki B (2003) Microporous Mesoporous Mater 57:83CrossRefGoogle Scholar
  15. 15.
    Li ZJ, Li S, Luo HM, Yan YS (2004) Adv Funct Mater 14:1019CrossRefGoogle Scholar
  16. 16.
    Cooper CA, Lin YS (2007) J Mater Sci 42:320. doi: CrossRefGoogle Scholar
  17. 17.
    Grieken RV, Sotelo JL, Menéndez JM, Melero JA (2000) Microporous Mesoporous Mater 39:135CrossRefGoogle Scholar
  18. 18.
    Aguado J, Serrano DP, Escola JM, Rodríguez JM (2004) Microporous Mesoporous Mater 75:41CrossRefGoogle Scholar
  19. 19.
    Li Q, Mihailova B, Creaser D, Sterte J (2000) Microporous Mesoporous Mater 40:53CrossRefGoogle Scholar
  20. 20.
    Li Q, Mihailova B, Creaser D, Sterte J (2001) Microporous Mesoporous Mater 43:51CrossRefGoogle Scholar
  21. 21.
    Tuel A, Taârit YB (1994) Zeolites 14:594CrossRefGoogle Scholar
  22. 22.
    Tan B, Rankin SE (2006) J Phys Chem B 110:22353CrossRefGoogle Scholar
  23. 23.
    Wu YJ, Ren XQ, Wang J (2009) Mater Chem Phys 113:773CrossRefGoogle Scholar
  24. 24.
    Wu YJ, Ren XQ, Lu YD, Wang J (2008) Mater Lett 62:317CrossRefGoogle Scholar
  25. 25.
    Brinker CJ, Scherer GW (1985) J Non-Cryst Solids 70:301CrossRefGoogle Scholar
  26. 26.
    Sanchez J, McCormick A (1992) J Phys Chem 96:8973CrossRefGoogle Scholar
  27. 27.
    Šefčík J, McCormick AV (1997) Catal Today 35:205CrossRefGoogle Scholar
  28. 28.
    Serrano DP, Uguina MA, Sanz R, Castillo E, Rodríguez A, Sánchez P (2004) Microporous Mesoporous Mater 69:197CrossRefGoogle Scholar
  29. 29.
    Ding L, Zheng Y, Zhang Z, Ring Z, Chen J (2006) Microporous Mesoporous Mater 94:1CrossRefGoogle Scholar
  30. 30.
    Madhusoodana CD, Das RN, Kameshima Y, Okada K (2005) J Porous Mat 12:273CrossRefGoogle Scholar
  31. 31.
    Thompson RW (1998) Mol Sieves 1:1CrossRefGoogle Scholar
  32. 32.
    Phiriyawirut P, Magaraphan R, Jamieson AM, Wongkasemjit S (2003) Mater Sci Eng A 361:147CrossRefGoogle Scholar
  33. 33.
    Fouad OA, Mohamed RM, Hassan MS, Ibrahim IA (2006) Catal Today 116:82CrossRefGoogle Scholar
  34. 34.
    Mohamed MM, Zidan FI, Fodail MH (2007) J Mater Sci 42:4066. doi: CrossRefGoogle Scholar
  35. 35.
    Lok BM, Cannan TR, Messina CA (1983) Zeolites 3:282CrossRefGoogle Scholar
  36. 36.
    McCormick AV, Bell AT (1989) Catal Rev Sci Eng 31(1–2):97CrossRefGoogle Scholar
  37. 37.
    Persson AE, Schoeman BJ, Sterte J, Otterstedt JE (1995) Zeolites 15:611CrossRefGoogle Scholar
  38. 38.
    Gabelica Z, Derouane EG, Blom N (1983) Appl Catal 5:109CrossRefGoogle Scholar
  39. 39.
    Suzuki K, Kiyozumi Y, Matsuzaki K, Shin S (1987) Appl Catal 35:401CrossRefGoogle Scholar
  40. 40.
    Ko YS, Ahn WS (2004) Powder Technol 145:10CrossRefGoogle Scholar
  41. 41.
    Thoma SG, Nenoff TM (2000) Microporous Mesoporous Mater 41:295CrossRefGoogle Scholar
  42. 42.
    Kim SD, Noh SH, Seong KH, Kim WJ (2004) Microporous Mesoporous Mater 72:185CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC 2009

Authors and Affiliations

  • Jing Gu
    • 1
  • Yajing Wu
    • 1
  • Jun Wang
    • 1
    Email author
  • Youdong Lu
    • 1
  • Xiaoqian Ren
    • 1
  1. 1.State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemistry and Chemical EngineeringNanjing University of TechnologyNanjingChina

Personalised recommendations