Effect of pore size and acidity on the coke formation during ethylbenzene conversion on zeolite catalysts

被引：65

作者：

Huang, Jun ^{[1
]}

Jiang, Yijiao ^{[1
]}

Marthala, V. R. Reddy ^{[1
]}

Bressel, Arne ^{[1
]}

Frey, Joerg ^{[1
]}

Hunger, Michael ^{[1
]}

机构：

[1] Univ Stuttgart, Inst Chem Technol, D-70550 Stuttgart, Germany

来源：

JOURNAL OF CATALYSIS | 2009年 / 263卷 / 02期

关键词：

Ethylbenzene disproportionation; Coke formation; Acidic zeolites; Pore size; Transition state shape selectivity; In situ solid-state NMR spectroscopy; STATE SHAPE SELECTIVITY; IN-SITU IR; UV/VIS SPECTROSCOPY; H/D EXCHANGE; H-Y; DISPROPORTIONATION; NMR; MECHANISM; TRANSALKYLATION; ALKYLBENZENES;

D O I：

10.1016/j.jcat.2009.02.019

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 present work provides solid-state C-13 NMR spectroscopic evidence that the zeolites acidity and the pore size strongly affect the catalytic behavior of ethylbenzene disproportionation and coke formation. The medium-pore zeolite H-ZSM-5 (ca. 0.56 nm) and the large-pore zeolite H-Y (ca. 0.74 nm) used in this study have exclusively Bronsted acid sites, but with different acid strength. Due to the transition state shape selectivity of ethylbenzene disproportionation, ethylbenzene transalkylation on H-Y takes place at low reaction temperature without side-reactions. On H-ZSM-5, dealkylation/realkylation was observed and generation of alkylcarbenium ions resulted in secondary reactions. These alkylcarbenium ions initiate coke formation on zeolite H-ZSM-5 via oligomerization, six-ring closure, and aromatization of alicyclic hydrocarbons. Ethylbenzene disproportionation on large-pore zeolites Y is an attractive reaction due to its low reaction temperature, high selectivity without side-reactions, and low coke formation. Medium-pore zeolite H-ZSM-5 showed higher reactivity for dealkylation of ethylbenzene and protolytic cracking of light alkanes due to its narrow channels and stronger Bronsted acid sites. (C) 2009 Elsevier Inc. All rights reserved.

引用

页码：277 / 283

页数：7

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