The benefit of multipore zeolites: Catalytic behaviour of zeolites with intersecting channels of different sizes for alkylation reactions

被引:55
作者
Corma, Avelino [1 ]
Llopis, Francisco J. [2 ]
Martinez, Cristina [1 ]
Sastre, German [1 ]
Valencia, Susana [1 ]
机构
[1] Univ Politecn Valencia, Inst Tecnol Quim, UPV CSIC, Valencia 46022, Spain
[2] Univ Valencia, Dept Ingn Quim, UVEG, Valencia, Spain
关键词
Multipore zeolites; Benzene alkylation with alcohols; Al distribution and proton location in zeolites; Selectivity with multipore zeolites; Ethylbenzene; Cumene; MOLECULAR-DYNAMICS; BETA-ZEOLITE; BENZENE; ISOMERIZATION; ETHYLBENZENE; FLUORIDE; ACIDITY; SITES; DISPROPORTIONATION; CARBONYLATION;
D O I
10.1016/j.jcat.2009.08.012
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
The catalytic behaviour of two multipore zeolites containing channels of different sizes, SSZ-33 (10 windows x 12 MR) and ITQ-22 (8 x 10 x 12 MR pores), for alkylation of benzene with ethanol and benzene with isopropanol or propylene, has been studied and compared to that of zeolites with intersecting channels of the same size, ZSM-5 (10 x 10 MR channels) and Beta (12 x 12 MR channels), which are industrially used for the above-mentioned process. For the alkylation of benzene with ethanol in gas phase, ITQ-22 behaves like the 10 MR ZSM-5 with respect to ethylbenzene selectivity, while the behaviour of SSZ-33 is close to that of a 12 MR zeolite such as Beta. For the alkylation of benzene with isopropanol or propylene in gas and liquid phase, Beta and ITQ-22 give similar selectivity values, which are much better than those obtained with ZSM-5. Meanwhile, SSZ-33 gives intermediate selectivity between that of the 10 MR ZSM-5 and the 12 MR Beta zeolite. ITQ-22, therefore, shows a unique behaviour as a multipurpose alkylation catalyst, with characteristics different from those of previously studied zeolites. The catalytic behaviour of ITQ-22 has been rationalized not only in terms of the topology of the channels but also taking into account the location of the protons. A computational study shows preferential Al location at the 10 MR, near the intersection with the 12 MR channels, and at the intersections between 10 and 12 MR channels. (C) 2009 Elsevier Inc. All rights reserved.
引用
收藏
页码:9 / 17
页数:9
相关论文
共 72 条
[1]  
ALBERTI G, 1996, COMPREHENSIVE SUPRAM, V7, P379
[2]   MECHANISM OF SOME CONVERSIONS OVER ZSM5 CATALYST [J].
ANDERSON, JR ;
MOLE, T ;
CHRISTOV, V .
JOURNAL OF CATALYSIS, 1980, 61 (02) :477-484
[3]  
[Anonymous], 2007, ATLAS ZEOLITE STRUCT
[4]   Influence of the zeolite pore structure on the kinetics of the disproportionation of ethylbenzene [J].
Arsenova-Härtel, N ;
Bludau, H ;
Haag, WO ;
Karge, HG .
MICROPOROUS AND MESOPOROUS MATERIALS, 2000, 35-6 :113-119
[5]   Catalytic and sorption studies related to the para selectivity in the ethylbenzene disproportionation over H-ZSM-5 catalysts [J].
Arsenova-Härtel, N ;
Bludau, H ;
Schumacher, R ;
Haag, WO ;
Karge, HG ;
Brunner, E ;
Wild, U .
JOURNAL OF CATALYSIS, 2000, 191 (02) :326-331
[6]  
BENTHAM MF, 1997, ERDOL ERDGAS KOHLE, V113, P84
[7]   Specificity of sites within eight-membered ring zeolite channels for carbonylation of methyls to acetyls [J].
Bhan, Aditya ;
Allian, Ayman D. ;
Sunley, Glenn J. ;
Law, David J. ;
Iglesia, Enrique .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (16) :4919-4924
[8]   Enzyme-like Specificity in Zeolites: A Unique Site Position in Mordenite for Selective Carbonylation of Methanol and Dimethyl Ether with CO [J].
Boronat, Mercedes ;
Martinez-Sanchez, Cristina ;
Law, David ;
Corma, Avelino .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (48) :16316-16323
[9]   Synthesis in fluoride media and characterisation of aluminosilicate zeolite beta [J].
Camblor, MA ;
Corma, A ;
Valencia, S .
JOURNAL OF MATERIALS CHEMISTRY, 1998, 8 (09) :2137-2145
[10]  
Catlow C.R.A., 1982, LECT NOTES PHYS, V166