Mesoporous aluminosilicates with ordered hexagonal structure, strong acidity, and extraordinary hydrothermal stability at high temperatures

被引:363
作者
Zhang, ZT
Han, Y
Xiao, FS [1 ]
Qiu, SL
Zhu, L
Wang, RW
Yu, Y
Zhang, Z
Zou, BS
Wang, YQ
Sun, HP
Zhao, DY
Wei, Y
机构
[1] Jilin Univ, Dept Chem, Changchun 130023, Peoples R China
[2] Chinese Acad Sci, Ctr Condensed Matter Phys, Beijing Lab Electron Microg, Beijing, Peoples R China
[3] Chinese Acad Sci, Inst Phys, Beijing, Peoples R China
[4] Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
[5] Drexel Univ, Dept Chem, Philadelphia, PA 19104 USA
关键词
D O I
10.1021/ja004138t
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Highly ordered hexagonal mesoporous aluminosilicates (MAS-5) with uniform pore sizes have been successfully synthesized from assembly of preformed aluminosilcate precursors with cetyltrimethylammonium bromide (CTAB) surfactant. The aluminosilicate precursors were obtained by heating, at 100-140 degreesC for 2-10 h. aluminasilica gels at the Al2O3/SiO2/TEAOH/H2O molar ratios of 1.0/7.0-350/10.0-33.0/500-2000. Mesoporous MAS-5 shows extraordinary stability both in boiling water (over 300 h) and in steam (800 degreesC for 2 h). Temperature-programmed desorption of ammonia shows that the acidic strength of MAS-5 is much higher than that of MCM-41 and is comparable to that of microporous Beta zeolite. In catalytic cracking of 1,3,5-triisopropylbenzene and alkylation of isobutane with butene. MAS-5 exhibits greater catalytic activity and selectivity, as compared with MCM-41 and HZSM-5. The MAS-5 samples were characterized with infrared, UV-Raman, and NMR spectroscopy and numerous other techniques. The results suggest that MAS-5 consists of both mesopores and micropores and that the pore walls of MAS-5 contain primary and secondary structural building units, similar to those of microporous zeolites. Such unique structural features might be responsible for the observed strong acidity and high thermal stability of the mesoporous aluminosilicates with well-ordered hexagonal symmetry.
引用
收藏
页码:5014 / 5021
页数:8
相关论文
共 41 条
[1]   RAMAN AND SI-29 MAS NMR-SPECTROSCOPY OF FRAMEWORK MATERIALS CONTAINING 3-MEMBERED RINGS [J].
ANNEN, MJ ;
DAVIS, ME .
MICROPOROUS MATERIALS, 1993, 1 (01) :57-65
[2]   Mesoporous materials [J].
Antonelli, DM ;
Ying, JY .
CURRENT OPINION IN COLLOID & INTERFACE SCIENCE, 1996, 1 (04) :523-529
[3]   A NEW FAMILY OF MESOPOROUS MOLECULAR-SIEVES PREPARED WITH LIQUID-CRYSTAL TEMPLATES [J].
BECK, JS ;
VARTULI, JC ;
ROTH, WJ ;
LEONOWICZ, ME ;
KRESGE, CT ;
SCHMITT, KD ;
CHU, CTW ;
OLSON, DH ;
SHEPPARD, EW ;
MCCULLEN, SB ;
HIGGINS, JB ;
SCHLENKER, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (27) :10834-10843
[4]  
Breck D.W, 1974, ZEOLITE MOL SIEVES
[5]   STUDIES ON MESOPOROUS MATERIALS .1. SYNTHESIS AND CHARACTERIZATION OF MCM-41 [J].
CHEN, CY ;
LI, HX ;
DAVIS, ME .
MICROPOROUS MATERIALS, 1993, 2 (01) :17-26
[6]   From microporous to mesoporous molecular sieve materials and their use in catalysis [J].
Corma, A .
CHEMICAL REVIEWS, 1997, 97 (06) :2373-2419
[7]   Improvement of hydrothermal stability of MCM-41 mesoporous molecular sieve [J].
Das, D ;
Tsai, CM ;
Cheng, SF .
CHEMICAL COMMUNICATIONS, 1999, (05) :473-474
[8]   In situ observation of nucleation and crystal growth in zeolite synthesis. A small-angle X-ray scattering investigation on Si-TPA-MFI [J].
de Moor, PPEA ;
Beelen, TPM ;
van Santen, RA .
JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (10) :1639-1650
[9]   SAXS and USAXS investigation on nanometer-scaled precursors in organic-mediated zeolite crystallization from gelating systems [J].
de Moor, PPEA ;
Beelen, TPM ;
van Santen, RA ;
Tsuji, K ;
Davis, ME .
CHEMISTRY OF MATERIALS, 1999, 11 (01) :36-43
[10]   Alkaline lyotropic silicate-surfactant liquid crystals [J].
Firouzi, A ;
Atef, F ;
Oertli, AG ;
Stucky, GD ;
Chmelka, BF .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (15) :3596-3610