改性H-ZSM-34上氯甲烷催化转化制低碳烯烃

doi:10.1016/S1872-2067(12)60681-0

催化学报 ›› 2013, Vol. 34 ›› Issue (11): 2047-2056.DOI: 10.1016/S1872-2067(12)60681-0

改性H-ZSM-34上氯甲烷催化转化制低碳烯烃

徐霆, 宋航, 邓卫平, 张庆红, 王野

厦门大学化学化工学院, 能源材料化学协同创新中心, 固体表面物理化学国家重点实验室, 醇醚酯化工清洁生产国家工程实验室, 福建厦门361005

收稿日期:2013-07-04 修回日期:2013-08-16 出版日期:2013-10-18 发布日期:2013-10-18
通讯作者: Weiping Deng,Ye Wang
基金资助:
国家重点基础研究发展计划(973计划,2010CB732303);国家自然科学基金(21173174,20923004,21033006,21161130522);教育部长江学者与创新团队发展计划(IRT1036).

Catalytic conversion of methyl chloride to lower olefins over modified H-ZSM-34

Ting Xu, Hang Song, Weiping Deng, Qinghong Zhang, Ye Wang

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China

Received:2013-07-04 Revised:2013-08-16 Online:2013-10-18 Published:2013-10-18
Contact: Weiping Deng,Ye Wang
Supported by:
This work was supported by the National Basic Research Program of China (2010CB732303), the National Natural Science Foundation of China (21173174, 20923004, 21033006, and 21161130522), and the Program for Changjiang Scholars and Innovative Research Team in University (IRT1036).

摘要/Abstract

摘要：

比较了几种典型的沸石分子筛在氯甲烷转化制乙烯、丙烯和丁烯等低碳烯烃反应中的催化性能, 发现H-ZSM-34具有较佳的催化活性和选择性. 经乙二胺四乙酸二钠(Na₂H₂EDTA)水溶液处理, 并经离子交换及焙烧后, H-ZSM-34上氯甲烷转化制低碳烯烃的催化性能显著改善. 当Na₂H₂EDTA浓度为0.1 mol/L, 反应温度为673 K, CH₃Cl分压9.2 kPa时, C₂-C₄烯烃选择性和收率分别达82%和61%. 研究还发现, Ce修饰H-ZSM-34催化剂同样可改善氯甲烷制低碳烯烃的选择性和收率. 表征结果表明, Na₂H₂EDTA处理和Ce修饰均降低了H-ZSM-34的酸性. 酸性的降低可抑制低碳烯烃的氢转移反应, 继而避免了其进一步转化为低碳烷烃.

关键词: 氯甲烷, 低碳烯烃, H-ZSM-34, 乙二胺四乙酸二钠处理, 铈修饰, 酸性

Abstract:

Among several typical zeolites, H-ZSM-34 was found to be an efficient catalyst for the conversion of methyl chloride to lower olefins, i.e., ethylene, propylene, and butenes. Treatment of H-ZSM-34 with a Na₂H₂EDTA (EDTA = ethylenediaminetetraacetate) aqueous solution followed by ion exchange and calcination enhanced the catalytic performance significantly. The selectivity to lower olefins increased significantly for certain Na₂H₂EDTA aqueous solution concentrations; when the H-ZSM-34 catalyst was treated with a 0.1 mol/L Na₂H₂EDTA solution, the selectivity and yield of C₂-C₄ olefins reached 82% and 61%, respectively, at 673 K and a CH₃Cl partial pressure of 9.2 kPa. The modification of H-ZSM-34 with Ce ions improved C₂-C₄ olefin selectivity and yield. Catalyst characterization suggests that treatment with Na₂H₂EDTA or modification by Ce decreases the acidity of H-ZSM-34. The weakened acidity of the treated or modified H-ZSM-34 may suppress the hydrogen transfer reaction and prevent lower olefins from further transformation to paraffins.

Key words: Methyl chloride, Lower olefins, H-ZSM-34, Ethylenediaminetetraacetate treatment, Cerium modification, Acidity

徐霆, 宋航, 邓卫平, 张庆红, 王野. 改性H-ZSM-34上氯甲烷催化转化制低碳烯烃[J]. 催化学报, 2013, 34(11): 2047-2056.

Ting Xu, Hang Song, Weiping Deng, Qinghong Zhang, Ye Wang. Catalytic conversion of methyl chloride to lower olefins over modified H-ZSM-34[J]. Chinese Journal of Catalysis, 2013, 34(11): 2047-2056.

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改性H-ZSM-34上氯甲烷催化转化制低碳烯烃

Catalytic conversion of methyl chloride to lower olefins over modified H-ZSM-34

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