甲醇芳构化中催化剂酸性对脱烷基、烷基化和异构化反应的影响

引用本文: 张金贵, 骞伟中, 汤效平, 沈葵, 王彤, 黄晓凡, 魏飞. 甲醇芳构化中催化剂酸性对脱烷基、烷基化和异构化反应的影响[J]. 物理化学学报, 2013, 29(06): 1281-1288. doi: 10.3866/PKU.WHXB201304101 shu

Citation: ZHANG Jin-Gui, QIAN Wei-Zhong, TANG Xiao-Ping, SHEN Kui, WANG Tong, HUANG Xiao-Fan, WEI Fei. Influence of Catalyst Acidity on Dealkylation, Isomerization and Alkylation in MTA Process[J]. Acta Physico-Chimica Sinica, 2013, 29(06): 1281-1288. doi: 10.3866/PKU.WHXB201304101 shu

甲醇芳构化中催化剂酸性对脱烷基、烷基化和异构化反应的影响

张金贵 ^1, ,
骞伟中 ^1, ,
汤效平 ^1,2, ,
沈葵 ^1, ,
王彤 ^1,2, ,
黄晓凡 ^2, ,
魏飞 ^1,

基金项目:
国家高技术研究发展计划(863)(2012AA051003)资助项目 (863)(2012AA051003)

摘要:

在Zn/P/ZSM-5催化剂上研究了甲醇、二甲苯、甲苯和甲醇等不同进料下芳烃产品分布随反应积碳的变化, 发现催化剂积碳对芳构化反应、脱烷基反应和烷基化反应的影响不同. 在不同硅铝摩尔比(Si/Al 比)和Zn负载量的Zn/P/ZSM-5 催化剂上进行甲醇转化, 考察催化剂酸性位点强度、密度和类型与芳烃收率和产品分布之间的关系, 发现当强酸位点酸密度下降时, 脱烷基反应最先被抑制, 其次是芳构化反应和异构化反应, 而烷基化反应却不受影响. 在Si/Al 比为14, 3% (w) Zn 负载量的Zn/P/ZSM-5 催化剂上可得到75%左右的芳烃收率, 二甲苯收率在35%左右, 具有重要的工业应用前景.

关键词:

English

Influence of Catalyst Acidity on Dealkylation, Isomerization and Alkylation in MTA Process

1.
1 Beijing Key Laboratory of Green Reaction Engineering & Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, P. R. China;
2 Huadian Coal Industry Group Co. Ltd., Beijing, 100031, P. R. China
Received Date: 16 January 2013
Available Online: 17 May 2013
Fund Project:
国家高技术研究发展计划(863)(2012AA051003)资助项目

Abstract:

Relationship between aromatics distribution, in the process of methanol to aromatics (MTA), and the conversion of methanol and the catalyst acidity was investigated over a series of Zn/P/ZSM-5 catalysts with different Si/Al molar ratios and zinc loading. To understand the contribution of aromatization, isomerization, dealkylation and alkylation reactivity of the catalyst to the aromatics distribution, coke deposition degree of Zn/P/ZSM-5 catalyst was tailored as using different feedstocks including methanol, xylene or the mixture of methanol and toluene. With the coke deposition, the amount of different types of acidic sites of catalyst varied significantly, characterized by NH₃-temperature programmed desorption (NH3-TPD) and pyridine-infrared methods. Aromatization, dealkylation, alkylation, and isomerization showed sensitivity to a reduction in the density of strongly acidic sites. Dealkylation reaction was preferentially inhibited just by slightly decreasing the density of strong acid sites. However, aromatization and isomerization reaction were inhibited only when the density of strong acid sites was significantly decreased. In all cases, alkylation was found to be uninfluenced by acidic site density. A Zn/P/ZSM-5 catalyst with Si/Al molar ratio of 14 and 3% (w) Zn loading exhibited aromatics yields of 75% and xylene yields of about 35%, indicating potential for industrial application.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

甲醇芳构化中催化剂酸性对脱烷基、烷基化和异构化反应的影响

English

Influence of Catalyst Acidity on Dealkylation, Isomerization and Alkylation in MTA Process

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

甲醇芳构化中催化剂酸性对脱烷基、烷基化和异构化反应的影响

English

Influence of Catalyst Acidity on Dealkylation, Isomerization and Alkylation in MTA Process

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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