催化学报

催化学报 ›› 2007, Vol. 28 ›› Issue (5): 407-412.

• 研究论文 • 上一篇    下一篇

Cu-HZSM-5上氯苯气相羟化反应及催化剂失活

陈灵晶,林海强,严斌,杨乐夫   

  1. 厦门大学化学系,固体表面物理化学国家重点实验室, 福建厦门 361005
  • 收稿日期:2007-05-25 出版日期:2007-05-25 发布日期:2011-04-28

Gas-Phase Hydroxylation of Chlorobenzene Over Cu-HZSM-5 and Catalyst Deactivation

CHEN Lingjing, LIN Haiqiang*, YAN Bin, YANG Lefu   

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, Xiamen University, Xiamen 361005, Fujian, China
  • Received:2007-05-25 Online:2007-05-25 Published:2011-04-28

PDF

964

被引次数

15

摘要： 研究了Cu-HZSM-5催化剂上的氯苯气相羟化合成苯酚反应及催化剂的失活情况. 发现在773 K和水/氯苯体积比为3的反应条件下, 1.6%Cu-HZSM-5催化剂上氯苯转化率高达82.4%, 苯酚选择性为98.2%, 但催化性能随着反应的进行有逐渐下降的趋势. 采用X射线衍射、氮气静态吸附、X射线能谱和吡啶吸附红外光谱等手段对反应前后的催化剂进行了表征. 结果表明,铜的流失、HZSM-5分子筛骨架脱铝、晶格塌陷和积炭是导致催化剂失活的主要原因.

关键词: 氯苯, 气相羟化, 苯酚, 铜, HZSM-5分子筛, 催化剂失活

Abstract: Catalytic performance and deactivation of the Cu-HZSM-5 catalyst for gas-phase hydroxylation of chlorobenzene to phenol were studied. Under the conditions of 773 K and water/chlorobenzene volume ratio of 3, a chlorobenzene conversion of 82.4% and a phenol selectivity of 98.2% were obtained. Deactivation of the Cu-HZSM-5 catalyst was observed during the reaction. Characterization byX-raydiffraction, N2 static adsorption, energy dispersive X-ray spectroscopy, and infrared spectroscopy of adsorbed pyridine was performed on fresh, used, and regenerated catalysts to study the essence of the catalytic reaction and catalyst deactivation. The leaching of copper from the catalyst, framework dealumination of HZSM-5, and coking were the main causes for the catalyst deactivation.

Key words: chlorobenzene, gas-phase hydroxylation, phenol, copper, HZSM-5 zeolite, catalyst deactivation