Physicochemical characterisation and catalytic activity of primary amine templated aluminosilicate mesoporous catalysts

被引:137
作者
Mokaya, R
Jones, W
机构
[1] Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, Lensfield Road
基金
英国工程与自然科学研究理事会;
关键词
D O I
10.1006/jcat.1997.1851
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Primary amines are used as structure-directing agents in the room temperature assembly of aluminosilicate inorganic species to yield mesoporous materials with physical and textural properties similar to those of MCM-41 but with substantially higher Bronsted acidity, Si and Al are incorporated into the mesoporous framework in proportions dependent on the gel Si/Al ratio. Calcination of the as-synthesised material to remove the occluded amine generates Bronsted acid sites which (depending on Si/Al ratio) are stronger or comparable in strength to those on zeolite-HY (Si/Al = 3.65) but weaker than those on ultrastable-Y zeolite (USY). The materials, designated AI-MMS, exhibit higher Bronsted acidity and catalytic activity for the cracking of cumene compared to equivalent aluminosilicate MCM-41 materials or to amorphous silica-alumina and show considerable stability to catalytic deactivation. AI-MMS samples with Si/Al ratio less than or equal to 20 have catalytic activity higher than the zeolite-HY but exhibit a lower rate of deactivation compared to the zeolite. Ageing of the materials (for 1 year in the calcined form) has no significant effect on their acidity and catalytic activity. Hexagonal ordering and total Bronsted acidity (but not acid strength) of the Al-MMS materials may be improved by using prepolymerised aluminosilicate inorganic precursors. (C) 1997 Academic Press.
引用
收藏
页码:211 / 221
页数:11
相关论文
共 25 条
[1]  
ANTON O, 1988, Patent No. 4720475
[2]   ORGANIC-REACTIONS IN A CLAY MICROENVIRONMENT [J].
BALLANTINE, JA ;
PURNELL, JH ;
THOMAS, JM .
CLAY MINERALS, 1983, 18 (04) :347-356
[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]   PHYSISORPTION OF ARGON, NITROGEN AND OXYGEN BY MCM-41, A MODEL MESOPOROUS ADSORBENT [J].
BRANTON, PJ ;
HALL, PG ;
SING, KSW ;
REICHERT, H ;
SCHUTH, F ;
UNGER, KK .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1994, 90 (19) :2965-2967
[6]   A STUDY OF SURFACE STRUCTURE OF DECATIONIZED Y ZEOLITE BY QUANTITATIVE INFRARED SPECTROSCOPY [J].
HUGHES, TR ;
WHITE, HM .
JOURNAL OF PHYSICAL CHEMISTRY, 1967, 71 (07) :2192-&
[7]   GENERALIZED SYNTHESIS OF PERIODIC SURFACTANT INORGANIC COMPOSITE-MATERIALS [J].
HUO, QS ;
MARGOLESE, DI ;
CIESLA, U ;
FENG, PY ;
GIER, TE ;
SIEGER, P ;
LEON, R ;
PETROFF, PM ;
SCHUTH, F ;
STUCKY, GD .
NATURE, 1994, 368 (6469) :317-321
[8]   ORDERED MESOPOROUS MOLECULAR-SIEVES SYNTHESIZED BY A LIQUID-CRYSTAL TEMPLATE MECHANISM [J].
KRESGE, CT ;
LEONOWICZ, ME ;
ROTH, WJ ;
VARTULI, JC ;
BECK, JS .
NATURE, 1992, 359 (6397) :710-712
[9]   EFFECT OF STRUCTURAL ALUMINUM ON THE MESOPOROUS STRUCTURE OF MCM-41 [J].
LUAN, ZH ;
HE, HY ;
ZHOU, WZ ;
CHENG, CF ;
KLINOWSKI, J .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1995, 91 (17) :2955-2959
[10]   MESOPORE MOLECULAR-SIEVE MCM-41 CONTAINING FRAMEWORK ALUMINUM [J].
LUAN, ZH ;
CHENG, CF ;
ZHOU, WZ ;
KLINOWSKI, J .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (03) :1018-1024