物理化学学报 >> 2010, Vol. 26 >> Issue (12): 3305-3309.doi: 10.3866/PKU.WHXB20101228

催化和表面结构 上一篇    下一篇

甲醇芳构化反应中Ag/ZSM-5催化剂的失活特性

田涛1,2, 骞伟中1, 汤效平1, 恽松1, 魏飞1   

  1. 1. 北京市绿色反应工程与工艺重点实验室, 清华大学化工系, 北京100084;

    2. 中石化经济技术研究院, 北京100029
  • 收稿日期:2010-08-06 修回日期:2010-10-15 发布日期:2010-12-01
  • 通讯作者: 骞伟中 E-mail:qianwz@mail.tsinghua.edu.cn
  • 基金资助:

    国家自然科学重点基金(20736004, 20736007)和教育部新世纪优秀人才计划(NECT-07-0489)资助项目

Deactivation of Ag/ZSM-5 Catalyst in the Aromatization of Methanol

TIAN Tao1,2, QIAN Wei-Zhong1, TANG Xiao-Ping1, YUN Song1, WEI Fei1   

  1. 1. Beijing Key Laboratory of Green Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, P. R. China;

    2. Economics & Development Research Institute, SINOPEC, Beijing 100029, P. R. China
  • Received:2010-08-06 Revised:2010-10-15 Published:2010-12-01
  • Contact: QIAN Wei-Zhong E-mail:qianwz@mail.tsinghua.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20736004, 20736007) and Program for New Century Excellent Talents in Universities of the Ministry of Education of China (NECT-07-0489).

摘要:

通过四次连续反应-再生循环实验对甲醇芳构化催化剂Ag/ZSM-5进行了失活再生研究, 结果表明催化剂通过烧碳可以得到部分再生. 对反应-再生后的催化剂进行了X射线衍射(XRD)、透射电子显微镜(TEM)表征, 证实芳构化过程中催化剂的ZSM-5骨架结构保持完好, 金属烧结也不严重. 傅里叶红外光谱(FTIR)和氨-程序升温脱附(NH3-TPD)实验证实了反应生成的水使催化剂在475 °C发生水热脱铝, 进而导致Brønsted 酸流失及催化剂的芳构化反应能力不可逆下降.

关键词: 甲醇, 芳构化, Ag/ZSM-5, 失活, 再生

Abstract:

The deactivation and regeneration properties of the methanol aromatization catalyst, Ag/ ZSM-5, were investigated by a continuous reaction-catalyst regeneration experiment over four cycles. The activity of the catalyst decreased gradually over the long reaction and was only partly recovered after coke burning. Characterization of the regenerated catalyst by X-ray diffraction (XRD) and transmission electron microscope (TEM) revealed that the ZSM-5 framework remained unchanged and that the sintering of the Ag nanoparticles was not serious. Analyses by Fourier transform Infrared spectroscopy (FTIR) and ammonia-temperature programmed desorption (NH3-TPD) experiment confirmed that the hydrothermal de-alumination of the catalyst by water in large amounts at 475 °C during aromatization resulted in a significant loss of Brønsted acidity. Consequently, an irreversible decrease in the aromatization ability of the catalyst was apparent.

Key words: Methanol, Aromatization, Ag/ZSM-5, Deactivation, Regeneration

MSC2000: 

  • O643