物理化学学报 >> 2010, Vol. 26 >> Issue (08): 2242-2248.doi: 10.3866/PKU.WHXB20100814

催化和表面结构 上一篇    下一篇

氧化镁改性对纳米HZSM-5分子筛催化甲醇制丙烯的影响

毛东森, 郭强胜, 孟涛   

  1. 上海应用技术学院, 化学与环境工程学院, 应用催化研究所, 上海 200235
  • 收稿日期:2010-03-04 修回日期:2010-04-07 发布日期:2010-07-23
  • 通讯作者: 毛东森 E-mail:dsmao1106@yahoo.com.cm; dsmao@sit.edu.cn
  • 基金资助:

    上海市教委重点科研项目(06ZZ81)和上海市教委重点学科建设项目(J51503)资助

Effect of Magnesium Oxide Modification on the Catalytic Performance of Nanoscale HZSM-5 Zeolite for the Conversion of Methanol to Propylene

MAO Dong-Sen, GUO Qiang-Sheng, MENG Tao   

  1. Research Institute of Applied Catalysis, School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai 200235, P. R. China
  • Received:2010-03-04 Revised:2010-04-07 Published:2010-07-23
  • Contact: MAO Dong-Sen E-mail:dsmao1106@yahoo.com.cm; dsmao@sit.edu.cn
  • Supported by:

    The project was supported by the Key Project of Shanghai Education Committee, China (06ZZ81) and the Leading Academic Discipline Project of Shanghai Education Committee, China (J51503).

摘要:

采用浸渍法制备了一系列不同Mg含量(0-8%, w)的改性纳米HZSM-5分子筛. 利用X射线衍射(XRD)、铝固体魔角旋转核磁共振(27Al MAS NMR)、N2吸附/脱附、氨-程序升温脱附(NH3-TPD)和吡啶吸附傅里叶变换红外(FT-IR)光谱等技术对改性前后样品的结构和酸性进行了详细表征; 并在常压、500 ℃和甲醇空速(WHSV)为1.0 h-1的反应条件下, 在连续流动固定床反应器上考察了其对甲醇制丙烯反应的催化性能. 结果表明, 随着Mg含量的增加, 丙烯和丁烯的选择性逐渐增大, 而甲烷、乙烯和芳烃的选择性逐渐降低. 催化剂的稳定性先随Mg含量的增加而增加, 当Mg含量为2%时达到最大, 之后又随Mg含量的增加而降低. MgO改性对纳米HZSM-5分子筛催化性能的影响主要是由其酸性和织构性能的改变而引起的.

关键词: 甲醇, 丙烯, 纳米HZSM-5分子筛, 氧化镁改性, 选择性, 稳定性

Abstract:

A series of nanoscale HZSM-5 zeolites modified with different amounts (0-8%, w) of magnesium were prepared by an impregnation method and characterized by X-ray diffraction (XRD), Al solid state magic angle spinning nuclear magnetic resonance (27Al MAS NMR), N2-adsorption/desorption, temperature-programmed desorption of NH3 (NH3-TPD), and pyridine adsorption Fourier transform infrared (FT-IR) methods. The conversion of methanol to propylene was tested in a continuous flow fixed-bed microreactor at atmospheric pressure, 500 ℃, and a methanol space velocity (WHSV) of 1.0 h-1. The results indicated that with an increase in the amount of Mg, the selectivity of propylene and butene increased but those of methane, ethylene and aromatics decreased consistently. With an increase in the amount of Mg the stability of the catalyst was found to increase initially, pass through a maximum at 2% and then decrease with higher amounts of Mg. The effect of modification with magnesium oxide on the catalytic performance of the nanoscale HZSM-5 zeolite for the conversion of methanol to propylene can be attributed to the resultant changes in acidity and texture of the modified nanoscale HZSM-5 zeolites.

Key words: Methanol, Propylene, Nanoscale HZSM-5 zeolite, Magnesium oxide modification, Selectivity, Stability

MSC2000: 

  • O643