催化学报

催化学报 ›› 2014, Vol. 35 ›› Issue (8): 1260-1266.DOI: 10.1016/S1872-2067(14)60152-2

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HCl存在下CeO2基催化剂上乙烷氧化脱氢制乙烯

郁风驰, 吴雪娇, 张庆红, 王野   

  1. 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:2014-04-17 修回日期:2014-05-19 出版日期:2014-08-01 发布日期:2014-08-05
  • 通讯作者: 王野
  • 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（21033006）；教育部创新团队发展计划（IRT1036）.

Oxidative dehydrogenation of ethane to ethylene in the presence of HCl over CeO2-based catalysts

Fengchi Yu, Xuejiao Wu, Qinghong Zhang, Ye Wang   

  1. 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:2014-04-17 Revised:2014-05-19 Online:2014-08-01 Published:2014-08-05
  • Supported by:

    This work was supported by the National Basic Research Program of China (973 Program, 2010CB732303), the National Natural Science Foundation of China (21033006), and the Program for Changjiang Scholars and Innovative Research Team in University (IRT1036).

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摘要：

报道了一种HCl存在时温和条件下的乙烷氧化脱氢制乙烯催化转化新途径. 研究发现，在多种金属氧化物催化剂中，CeO2呈现最佳乙烯生成的催化性能. 与纳米粒子相比，具有棒状和立方体状形貌的CeO2纳米晶具有较高的乙烷转化率和乙烯选择性. 以MnOx修饰CeO2可进一步提高催化性能. 在8 wt% MnOx-CeO2催化剂上，723K反应2 h时乙烷转化率和乙烯选择性分别为94%和69%. 该催化剂性能稳定，反应100 h乙烯收率可保持在65%-70%. HCl的存在对乙烯的选择性生成起着至关重要的作用，一部分乙烯来自于氯乙烷的脱HCl反应.

关键词: 乙烷, 乙烯, 氧化脱氢, 氯化氢, 二氧化铈

Abstract:

This article reports a new catalytic route for the oxidative dehydrogenation of ethane to ethylene in the presence of HCl at moderate temperatures. CeO2 was found to be the most efficient catalyst for the production of ethylene from the variety of metal oxides examined in this work. CeO2 nanocrystals with rod and cube morphologies showed higher ethane conversions and ethylene selectivities than CeO2 nanoparticles. The modification of CeO2 by MnOx further enhanced the catalytic performance. Ethane conversion of 94% and ethylene selectivity of 69% were obtained after 2 h of reaction at 723 K over an 8 wt% MnOx-CeO2 catalyst. This catalyst was stable and the ethylene yield could be sustained at 65%-70% over 100 h of reaction. The presence of HCl played a key role in the selective production of C2H4, and some of the C2H4 was probably formed from chloroethane by dehydrochlorination.

Key words: Ethane, Ethylene, Oxidative dehydrogenation, Hydrogen chloride, Cerium oxide