Parameters influencing the selectivity to propene in the MTO conversion on 10-ring zeolites: directly synthesized zeolites ZSM-5, ZSM-11, and ZSM-22

被引:67
作者
Dyballa, Michael [1 ]
Becker, Peter [1 ]
Trefz, Daniel [1 ]
Klemm, Elias [1 ]
Fischer, Achim [2 ]
Jakob, Harald [2 ]
Hunger, Michael [1 ]
机构
[1] Univ Stuttgart, Inst Chem Technol, D-70550 Stuttgart, Germany
[2] Evon Ind AG, Hanau, Germany
关键词
Methanol-to-olefin conversion; Propene; Dual-cycle concept; 10-Ring zeolites; Bronsted acid site density; TO-OLEFIN CONVERSION; METHANOL CONVERSION; REACTION-MECHANISM; HYDROCARBON FORMATION; METHOXY GROUPS; LIGHT OLEFINS; CO-REACTION; H-ZSM-5; DEACTIVATION; PHOSPHORUS;
D O I
10.1016/j.apcata.2015.11.017
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
Zeolites ZSM-5, ZSM-11, and ZSM-22 (n(si)/n(Al) = 20-1000) were applied as methanol-to-olefin conversion (MTO) catalysts and optimized for high propene selectivities at high methanol conversions, high weight hourly space velocities, and for long catalyst lifetimes. On zeolites ZSM-5 and ZSM-11 with optimized Bronsted acid site densities of 0.13 and 0.15 mmol/g, propene selectivities of 51 and 52%, respectively, at a reaction time of 25 h were reached. In contrast, zeolite ZSM-22 with an optimized acid site density of 0.30 mmol/g showed a maximum propene selectivity of 38% only and a significantly shorter lifetime. Under these conditions, no aromatics could be detected by in situ UV-vis spectroscopy and on-line GC. Thus, an optimized acid site density can suppress the aromatic-based reaction mechanisms by hindering intermolecular hydrogen transfer reactions. Therefore, the acid site optimization could be a promising way for tuning the product selectivity of MTO catalysts on significantly different pore systems. (C) 2015 Elsevier B.V. All rights reserved.
引用
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页码:233 / 243
页数:11
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