H-gallosilicate (MFI) propane aromatization catalyst - Influence of calcination temperature on acidity, activity and deactivation due to coking

被引:40
作者
Choudhary, VR [1 ]
Sivadinarayana, C [1 ]
Kinage, AK [1 ]
Devadas, P [1 ]
Guisnet, M [1 ]
机构
[1] UNIV POITIERS,UFR SCI,URA CNRS 350,F-86022 POITIERS,FRANCE
关键词
propane aromatization; H-gallosilicate (MFI) zeolite; deactivation due to coking; degalliation of zeolite;
D O I
10.1016/0926-860X(95)00277-4
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
H-Gallosilicate (MFI) (bulk Si/Ga = 33) calcined at different temperatures (600-1100 degrees C) has been characterized for its acidity/acid strength distribution (by step wise thermal desorption and chemisorption of pyridine at 100-400 degrees C), acid function by acid catalyzed model reactions (viz. isooctane cracking (at 400 degrees C) for external acid sites and o-xylene isomerization (at 400 degrees C) and toluene disproportionation (at 500 degrees C) for overall acid sites), crystallinity by XRD, incorporation of Ga in the zeolite framework by Ga-71 MAS NMR and FTIR, and framework and non-framework Ga by Si-29 MAS NMR and bulk chemical analysis. influence of the calcination temperature on the catalytic activity/selectivity and catalyst deactivation due to coking in the propane aromatization process (at 550 degrees C) has also been thoroughly investigated. The acidity, framework Ga, crystallinity and catalytic activity and catalyst deactivation in the propane aromatization are found to be strongly influenced by the calcination temperature, mostly because of the extensive degalliation of the zeolite, depending upon the calcination temperature. The product selectivity, shape selectivity and dehydrogenation activity relative to cracking activity, of the zeolite in the propane aromatization are influenced strongly by the calcination temperature and also by the catalyst deactivation due to coking.
引用
收藏
页码:125 / 142
页数:18
相关论文
共 17 条
[1]   ON THE ENHANCED DEHYDROGENATION VERSUS CRACKING ABILITY OF AN ACIDIC GALLIUM MFI - A TENTATIVE ACID-BASE INTERACTION-MODEL [J].
BANDIERA, J ;
TAARIT, YB .
APPLIED CATALYSIS, 1991, 76 (02) :199-208
[2]   AROMATIZATION OF PROPANE OVER MFI-GALLOSILICATES [J].
BAYENSE, CR ;
VANDERPOL, AJHP ;
VANHOOFF, JHC .
APPLIED CATALYSIS, 1991, 72 (01) :81-98
[3]   AROMATIZATION OF PROPANE OVER GALLIUM-CONTAINING H-ZSM-5 ZEOLITES - INFLUENCE OF THE PREPARATION METHOD ON THE PRODUCT SELECTIVITY AND THE CATALYTIC STABILITY [J].
BAYENSE, CR ;
VANHOOFF, JHC .
APPLIED CATALYSIS, 1991, 79 (01) :127-140
[4]   GAS-CHROMATOGRAPHIC ADSORPTION DESORPTION TECHNIQUES FOR MEASURING ACID STRENGTH DISTRIBUTION ON SOLID CATALYSTS [J].
CHOUDHARY, VR .
JOURNAL OF CHROMATOGRAPHY, 1983, 268 (02) :207-218
[5]   TITRATION OF ACTIVE ACID SITES ON ZEOLITES BY SELECTIVE POISONING OF STRONGER ACID SITES [J].
CHOUDHARY, VR .
ZEOLITES, 1987, 7 (03) :272-276
[6]   A GC PULSE METHOD BASED ON TEMPERATURE PROGRAMMED DESORPTION UNDER CHROMATOGRAPHIC CONDITIONS FOR MEASURING IRREVERSIBLE ADSORPTION ON SOLID CATALYSTS [J].
CHOUDHARY, VR ;
NAYAK, VS .
APPLIED CATALYSIS, 1982, 4 (01) :31-36
[7]   COMPARISON BETWEEN CATALYTICALLY IMPORTANT ZEOLITES FOR THEIR CATALYTIC PROPERTIES AND DEACTIVATION [J].
CHOUDHARY, VR ;
AKOLEKAR, DB .
JOURNAL OF CATALYSIS, 1990, 125 (01) :143-156
[8]  
CHOUDHARY VR, IN PRESS JCATAL
[9]  
GIANNETTO G, 1993, J CATAL, V145, P86
[10]   THE ACTIVE-SITE OF ACIDIC ALUMINOSILICATE CATALYSTS [J].
HAAG, WO ;
LAGO, RM ;
WEISZ, PB .
NATURE, 1984, 309 (5969) :589-591