期刊
JOURNAL OF CATALYSIS
卷 303, 期 -, 页码 135-140出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2013.03.021
关键词
Methanol-to-hydrocarbons; Methanol-to-olefins; Zeolite; Hydrocarbon pool; Olefin and aromatic methylation; HZSM-5; Selectivity
资金
- Dow Chemical Company
- National Science Foundation [CBET 1055846]
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1055846] Funding Source: National Science Foundation
The observed product distribution in methanol-to-hydrocarbons (MTH) catalysis can be rationalized based on the relative rates of propagation of the aromatic- and olefin-based cycles that operate on the zeolite catalyst. We report that the ratio of ethene to 2-methylbutane + 2-methyl-2-butene (ethene/2MB) yield can be used to describe the propagation of aromatic and olefin methylation/cracking cycles. The co-reaction of C-12-ethene with C-13-dimethyl ether (DME) shows that the rate of DME conversion (1.62 mol C (mol Al s)(-1)) is similar to 20 times faster than ethene conversion (0.08 mol C (mol Al s)(-1)), suggesting that ethene can be considered as terminal product for MTH at 623 K. At iso-conversion conditions at 548 K, propene is co-fed with DME to increase propagation of the olefin-based cycle and correspondingly a 1.7-fold decrease in the ethene/2MB yield is observed. Similarly, the co-reaction of toluene with DME increases propagation of the aromatic-based cycle and a 2.1-fold increase in the ethene/2MB yield is observed. The ethene/2MB yield also increased by a factor of 2 as DME conversion increased from 5% to 62%, which is consistent with the observed concurrent increase in selectivity to ethene and methylbenzenes. For the reaction of DME alone, increasing the temperature from 548 K to 723 K increases the propagation of the olefin-based cycle and a corresponding decrease in the ethene/2MB yield from 4.7 to 1.3 is also observed. The ethene/2MB yield varies systematically with feed composition, conversion, and temperature, showing that this ratio describes the relative propagation of the aromatic to olefin methylation/cracking cycles in MTH conversion on H-ZSM-5. (c) 2013 Elsevier Inc. All rights reserved.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据