Compositional and kinetic study on the rapid crystallization of ZSM-5 in the absence of organic template under stirring

被引:124
作者
Kim, SD
Noh, SH
Seong, KH
Kim, WJ
机构
[1] Konkuk Univ, Dept Chem & Mat Engn, Seoul 143701, South Korea
[2] SK Corp, Fine Chem Res Team, Taejon 305712, South Korea
关键词
organic-free ZSM-5; stirring; SiO2/Al2O3 molar ratio; Na2O content; structure directing role;
D O I
10.1016/j.micromeso.2004.04.024
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The MFI type high silica zeolite, ZSM-5 with well-defined crystal morphology was successively synthesized in the absence of organic template within a short reaction time under stirring at 200 rpm and 463 K. The results clearly show that Na+ cation plays a structure directing role as well as a charge balancing role. In addition, it is interesting to notice that when the SiO2/Al2O3 molar ratio is as high as 80.0, higher Na2O content seems to be required to obtain pure ZSM-5. Otherwise, the crystallization path is more likely to direct toward the formation of a dense phase, keatite rather than ZSM-5, indicating the structure directing role of Na+ cation. On the other hand, as the SiO2/Al2O3 molar ratio decreases to lower than 30, the crystallization tends to direct toward the formation of mordenite, which is more aluminous than ZSM-5. In this case, the Na2O content should be as low as possible to direct the crystallization toward the formation of pure ZSM-5. The NMR study suggests that organic-free ZSM-5 with tetrahedrally coordinated Al only can be easily crystallized within 8 h of reaction. The kinetic study based on 14Na(2)O-100SiO(2)-xAl(2)O(3)-2500H(2)O (x = 1.5, 2 and 3) was conducted at 423, 443 and 463 K, respectively, and the results suggest that the higher the Al2O3 content is, the higher the temperature is preferred, enhancing the rate of crystallization with the increase in temperature. (C) 2004 Elsevier Inc. All rights reserved.
引用
收藏
页码:185 / 192
页数:8
相关论文
共 25 条
[1]   Synthesis, characterization and catalytic activity of ZSM-5 zeolites having variable silicon-to-aluminum ratios [J].
Ali, MA ;
Brisdon, B ;
Thomas, WJ .
APPLIED CATALYSIS A-GENERAL, 2003, 252 (01) :149-162
[2]  
Argauer R.J., 1972, US Pat., Patent No. [3702886, US3702886A]
[3]   INVESTIGATION OF NA,TPA-ZSM-5 ZEOLITE SYNTHESIS BY CHEMICAL METHODS [J].
CUNDY, CS ;
HENTY, MS ;
PLAISTED, RJ .
ZEOLITES, 1995, 15 (04) :342-352
[4]  
DAI FY, 1986, STUD SURF SCI CATAL, V28, P223
[5]  
DAI FY, 1989, ACS SYM SER, V398, P244
[6]   ANALYSIS OF THE FORMATION OF MONODISPERSE POPULATIONS BY HOMOGENEOUS NUCLEATION [J].
DENOUDEN, CJJ ;
THOMPSON, RW .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1991, 143 (01) :77-84
[7]  
ENGELHARDT G, 1987, HIGH RESOLUTION SOLI, P212
[8]  
Grose R.W., 1981, US Patent, Patent No. 4257885
[9]  
Kalipcilar H, 2001, CRYST RES TECHNOL, V36, P1197, DOI 10.1002/1521-4079(200111)36:11<1197::AID-CRAT1197>3.0.CO
[10]  
2-D