Deactivating effect of quinoline during the methylcyclohexane transformation over H-USY zeolite

被引:27
作者
Caeiro, G
Magnoux, P
Lopes, JM
Ribeiro, FR
机构
[1] Inst Super Tecn, Ctr Engn Biol & Quim, P-1049001 Lisbon, Portugal
[2] Univ Poitiers, Catalyse Chim Organ Lab, UMR 6503, F-86022 Poitiers, France
关键词
H-USY zeolite; cracking; methyleyclohexane; quinoline; poisoning; deactivation; coke;
D O I
10.1016/j.apcata.2005.06.016
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 influence of 0.5 wt.% of quinoline (540 pprn of nitrogen) in the feed was tested for the methylcyclohexane transformation at 350 degrees C over an H-USY zeolite (framework SUM ratio of 5.4). The selectivities for the fresh catalyst do not seem to be altered by the presence of quinoline. Oppositely, for the deactivated zeolite, the aromatics yield increases for the tests performed with quinoline. Deactivation with time on stream is very pronounced, even for tests carried Out without the base molecule; this can be attributed to the formation of highly polyaromatic coke molecules that block the acid sites and the microporous Structure. In presence of quinoline, deactivation is enhanced due to its cumulative poisoning effect, especially for smaller contact times. This deactivation is caused by the strong interaction of the nitrogen base with the Bronsted acid sites responsible for the cracking mechanism. Quinoline molecule also participates in coke formation reactions, leading to an increase in the produced amount of coke, particularly of the more polyaromatic compounds insoluble in dichloromethane. (c) 2005 Elsevier B.V. All rights reserved.
引用
收藏
页码:189 / 199
页数:11
相关论文
共 49 条
[1]   Quantum chemical studies of zeolite proton catalyzed reactions [J].
Blaszkowski, SR ;
vanSanten, RA .
TOPICS IN CATALYSIS, 1997, 4 (1-2) :145-156
[2]   Miniaturized method for separation and quantification of nitrogen species in petroleum distillates [J].
Briker, Y ;
Ring, Z ;
Iacchelli, A ;
McLean, N .
FUEL, 2003, 82 (13) :1621-1631
[3]   Methylcyclohexane transformation over HFAU, HBEA, and HMFI zeolites: I. Reaction scheme and mechanisms [J].
Cerqueira, HS ;
Mihindou-Koumba, PC ;
Magnoux, P ;
Guisnet, M .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2001, 40 (04) :1032-1041
[4]   Influence of coke on the acid properties of a USHY zeolite [J].
Cerqueira, HS ;
Ayrault, P ;
Datka, J ;
Guisnet, M .
MICROPOROUS AND MESOPOROUS MATERIALS, 2000, 38 (2-3) :197-205
[5]   CONVERSION OF CYCLOHEXENE OVER Y-ZEOLITES - A MODEL REACTION FOR HYDROGEN TRANSFER [J].
CHENG, WC ;
RAJAGOPALAN, K .
JOURNAL OF CATALYSIS, 1989, 119 (02) :354-358
[6]   THE ROLE OF DIFFERENT TYPES OF ACID SITE IN THE CRACKING OF ALKANES ON ZEOLITE CATALYSTS [J].
CORMA, A ;
PLANELLES, J ;
SANCHEZMARIN, J ;
TOMAS, F .
JOURNAL OF CATALYSIS, 1985, 93 (01) :30-37
[7]   QUINOLINE AS A PROBE MOLECULE FOR DETERMINATION OF EXTERNAL BRONSTED AND LEWIS ACIDITY IN ZEOLITES [J].
CORMA, A ;
FORNES, V ;
REY, F .
ZEOLITES, 1993, 13 (01) :56-59
[8]   NEW SILICA-ALUMINA MAGNESIA FCC ACTIVE MATRIX AND ITS POSSIBILITIES AS A BASIC NITROGEN PASSIVATING COMPOUND [J].
CORMA, A ;
MOCHOLI, FA .
APPLIED CATALYSIS A-GENERAL, 1992, 84 (01) :31-46
[9]  
CORMA A, 1991, APPL CATAL, V67, P307
[10]   ISOMERIZATION, DEHYDROGENATION AND CRACKING OF METHYLCYCLOHEXANE OVER HNAY ZEOLITES [J].
CORMA, A ;
AGUDO, AL .
REACTION KINETICS AND CATALYSIS LETTERS, 1981, 16 (2-3) :253-257