化工学报 ›› 2008, Vol. 59 ›› Issue (8): 2007-2013.

• 催化、动力学与反应器 • 上一篇    下一篇

Raney Ni催化剂上苯酚液相原位加氢表观动力学

项益智;卢春山;张群峰;马磊;巫晓琼;李小年   

  1. 浙江工业大学工业催化研究所,绿色化学合成技术国家重点实验室培养基地,浙江 杭州 310032
  • 出版日期:2008-08-05 发布日期:2008-08-05

Apparent kinetics of in-situ hydrogenation of phenol in liquid phase over Raney Ni catalyst

XIANG Yizhi;LU Chunshan;ZHANG Qunfeng;MA Lei;WU Xiaoqiong;LI Xiaonian   

  • Online:2008-08-05 Published:2008-08-05

摘要:

考察了Raney Ni催化剂作用下,反应条件(温度、压力、空速、苯酚浓度和甲醇与水的配比)对苯酚液相原位加氢反应性能的影响规律。结果表明,较高的反应温度和压力以及较低的液体空速和甲醇含量有利于提高苯酚的转化率和环己醇的选择性,但是苯酚的浓度对反应性能的影响不大。针对该反应体系的动力学研究表明,苯酚原位加氢生成环己醇和环己酮的表观浓度级数α1α2分别为0.93和1.09,β1β2分别为3.82和3.47,表观活化能Ea1Ea2分别为67.8 kJ•mol-1和80.2 kJ•mol-1。将动力学研究结果与各个反应条件对反应性能的影响规律相关联,解释了不同反应条件引起苯酚加氢反应速率以及生成环己醇和环己酮选择性差异的原因。

关键词:

苯酚, 原位加氢, Raney Ni, 表观动力学

Abstract:

The effect of reaction conditions on the performance of in-situ hydrogenation of phenol in liquid phase over Raney Ni catalyst was studied.The results indicated that higher phenol conversion and cyclohexanol selectivity could be obtained under the condition of higher temperature and pressure, and lower space velocity and methanol content, while phenol concentration had almost no effect on the reaction performance.The study of apparent kinetics indicated that the reaction orders with respect to phenol and adsorbed hydrogen for cyclohexanol formation (α1 and β1) were 0.93 and 3.82, respectively, and those for cyclohexanone formation (α2 and β2) were 1.09 and 3.47, respectively.The apparent activation energy to cyclohexanol (Ea1) and cyclohexanone (Ea2) were 67.8 kJ•mol-1 and 80.2 kJ•mol-1, respectively.The role of reaction conditions on the in-situ hydrogenation performance of phenol (hydrogenation rate, selectivity of products) could be clarified on the basis of the apparent kinetics results.

Key words:

苯酚, 原位加氢, Raney Ni, 表观动力学