Comparison of kinetic behavior of non-catalytic/catalytic liquid-phase oxidation of cyclohexane

LIU Changjun; TANG Shengwei; TAN Pinghua; LIU Yingying; LIANG Bin; MIN Enze

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Comparison of kinetic behavior of non-catalytic/catalytic liquid-phase oxidation of cyclohexane

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- Comparison of kinetic behavior of non-catalytic/catalytic liquid-phase oxidation of cyclohexane
- CIESC Journal Issue 8, Pages: 1992-1999(2008)
- 作者机构：
  
  1. 四川大学化工学院，四川省多相流传质与反应工程重点实验室,四川,成都,610065
  2. 中国石油化工股份有限公司石油化工科学研究院,北京,100083
- 作者简介：
- 基金信息：
- DOI：
  CLC：
- Online First：05 August 2008，
  
  Published：05 August 2008
- 稿件说明：
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LIU Changjun, TANG Shengwei, TAN Pinghua, et al. Comparison of kinetic behavior of non-catalytic/catalytic liquid-phase oxidation of cyclohexane[J]. CIESC Journal, 2008, (8): 1992-1999.
DOI：

LIU Changjun, TANG Shengwei, TAN Pinghua, et al. Comparison of kinetic behavior of non-catalytic/catalytic liquid-phase oxidation of cyclohexane[J]. CIESC Journal, 2008, (8): 1992-1999. DOI：

摘要

分别以不同氧浓度气体及纯氧作为氧源

利用鼓泡塔反应器在1.1 MPa、不同温度、不同气体流量条件下比较了环己烷液相非催化氧化和催化氧化反应特性。通过比较分析，讨论了环己烷液相氧化的链式反应机理。理论分析和实验数据表明，环己烷液相催化氧化反应诱导期短，其表观速率与环己烷浓度和氧气浓度都为一级;而非催化氧化反应诱导期长，是由烃直接氧化引发过程控制，只有当过氧化氢积累到一定浓度以后，过氧化物分解产生自由基速率变得显著，反应才表现出自催化反应特征。而在催化剂存在的情况下，环己基过氧化氢分解非常迅速，环己基过氧化氢浓度在整个反应过程中稳定在一个很低的水平，反应由氧化生成酮的链传递反应过程控制。

Abstract

The kinetic behavior of the liquid-phase oxidation of cyclohexane was investigated in a bubble column under 1.1 MPa at various temperatures

in which gases with O2 concentrations ranging from 5% to 99% were used as oxidants.By comparing the non-catalytic and catalytic oxidation of cyclohexane

the free radical mechanism of the oxidation was discussed in detail.Both the mechanism analysis and experimental data showed that the catalyzed liquid-phase oxidation of cyclohexane was a reaction of first-order with respect to both cyclohexane and oxygen.For the non-catalytic oxidation

an induction period was obvious.During the non-catalytic oxidation of cyclohexane by oxygen

the chain initiating reaction was the rate determining step.Beyond the induction period

the reaction was accelerated and exhibited auto-catalytic behavior due to the release of radicals through the decomposition of cyclohexyl hydroperoxide when its concentration accumulated to a certain degree.On the other hand

in catalytic oxidation the cyclohexyl hydroperoxide decomposed rather quickly

and then accelerated the reaction.And during the reaction

the concentration of cyclohexyl hydroperoxide kept very low and the chain propagation became the rate limiting step.

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Related Institution

四川大学化工学院, 四川省多相流传质与反应工程重点实验室

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