高等学校化学学报

高等学校化学学报 ›› 2012, Vol. 33 ›› Issue (01): 96.doi: 10.3969/j.issn.0251-0790.2012.01.016

• 物理化学 • 上一篇    下一篇

Cr/NaZSM-5催化剂上CO2氧化丙烷脱氢反应

张帆1, 聂颖颖1, 缪长喜2, 乐英红1, 华伟明1, 高滋1   

  1. 1. 复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海 200433;
    2. 中国石油化工股份有限公司上海石油化工研究院, 上海 201208
  • 收稿日期:2011-08-09 出版日期:2012-01-10 发布日期:2011-12-20
  • 通讯作者: 华伟明,男,博士,教授,主要从事多相催化研究.E-mail:wmhua@fudan.edu.cn E-mail:wmhua@fudan.edu.cn
  • 基金资助:

    国家自然科学基金(批准号: 20773027)、 国家"九七三"计划项目(批准号: 2006CB806103)、 上海市科学技术委员会项目(批准号: 08DZ2270500)和上海石油化工研究院项目(批准号: ZC06070002)资助.

Oxidative Dehydrogenation of Propane to Propylene with CO2 over Cr/NaZSM-5 Catalysts

ZHANG Fan1, NIE Ying-Ying1, MIAO Chang-Xi2, YUE Ying-Hong1, HUA Wei-Ming1, GAO Zi1   

  1. 1. Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China;
    2. SINOPEC Shanghai Research Institute of Petrochemical Technology, Shanghai 201208, China
  • Received:2011-08-09 Online:2012-01-10 Published:2011-12-20
  • Contact: Hua Weiming E-mail:wmhua@fudan.edu.cn

PDF (PC)

摘要： 以亚微米级NaZSM-5为载体合成了一系列负载型Cr催化剂, 采用氮气吸附、 XRD、 UV-Vis和H2-TPR对Cr/NaZSM-5催化剂的结构和织构性质进行了表征, 并评价了催化剂在CO2气氛下的丙烷脱氢性能. 硅铝摩尔比为60, Cr质量分数为3%的催化剂具有最高的反应活性, 于550 ℃反应10 min和8 h后的丙烷转化率分别为48.3%和30.1%, 丙烯选择性则分别为86.0%和91.8%. 催化剂中的Cr6+含量和反应初活性具有良好的对应关系, 表明高Cr6+含量对催化剂表现出高的丙烷脱氢活性是至关重要的. CO2气氛下的丙烯产率明显比氮气气氛下的高, 这是由于CO2气氛下催化剂表面有较多量的Cr6+, 并且CO2可通过逆水煤气变换反应除去脱氢反应生成的氢.

关键词: Cr/NaZSM-5, 丙烷, 脱氢, 丙烯, 二氧化碳

Abstract: A series of Cr catalysts supported on submicro NaZSM-5 zeolite was prepared. The obtained samples were characterized by N2 adsorption, XRD, UV-Vis and H2-TPR, and tested as catalysts for dehydroge-nation of propane to propylene in the presence of CO2. The highest activity was achieved on the catalyst with a Cr content of 3% and a Si/Al molar ratio of 60. In this case, the propane conversion and propylene selectivity were 48.3%, 86.0% and 30.1%, 91.8%, respectively after the reaction at 550 ℃ for 10 min and 8 h. There is a good relationship between the initial activity and Cr6+ content of the catalysts, showing that a high content of Cr6+ species in the calcined catalyst is crucial for its high catalytic activity in dehydrogenation of propane to propylene with CO2. A higher propylene yield was obtained during propane dehydrogentaion in the presence of CO2 than N2. This can be attributed to a higher surface concentration of Cr6+ retained on the catalyst in the presence of CO2 as well as the elimination of hydrogen produced by propane dehydrogenation.

Key words: Cr/NaZSM-5, Propane, Dehydrogenation, Propylene, Carbon dioxide

中图分类号: 

TrendMD: