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催化剂Ru/ZrO2-CeO2催化湿式氧化苯酚
引用本文:王建兵,祝万鹏,王伟,杨少霞.催化剂Ru/ZrO2-CeO2催化湿式氧化苯酚[J].环境科学,2007,28(7):1460-1465.
作者姓名:王建兵  祝万鹏  王伟  杨少霞
作者单位:清华大学环境科学与工程系,北京100084;清华大学环境科学与工程系,北京100084;中国矿业大学北京校区化学与环境工程学院,北京 100083;清华大学环境科学与工程系,北京100084
基金项目:国家高技术研究发展计划(863)项目(2002AA601260);国家自然科学基金项目(50508017)
摘    要:催化剂Ru/ZrO2-CeO2催化湿式氧化苯酚的过程表明,Ru/ZrO2-CeO2可以显著提高COD和苯酚去除效果,当反应温度为170℃,压力为3 MPa,反应120 min后,COD和苯酚的去除率分别达到了99%和100%.试验还考察了不同反应条件对苯酚溶液COD去除的影响,并获得了最优的反应条件:温度为170℃,压力为3 MPa,催化剂的投加量为5 g/L,搅拌速度为500 r/min.通过对中间产物的分析,本研究提出了催化湿式氧化苯酚的简单路径图,认为苯酚首先被氧化成小分子有机酸,接着小分子有机酸被氧化成二氧化碳和水.前一个过程是快速反应,后一个过程中的乙酸氧化是慢速过程,需要在高温下才能完成.乙酸的氧化主要是自由基攻击α碳上的C—H键,先生成甲酸,并最终生成二氧化碳和水.

关 键 词:催化湿式氧化  苯酚  Ru/ZrO2-CeO2  催化剂
文章编号:0250-3301(2007)07-1460-06
收稿时间:8/8/2006 12:00:00 AM
修稿时间:2006-08-082006-09-22

Catalytic Wet Air Oxidation of Phenol with Ru/ZrO2-CeO2 Catalyst
WANG Jian-bing,ZHU Wan-peng,WANG Wei and YANG Shao-xia.Catalytic Wet Air Oxidation of Phenol with Ru/ZrO2-CeO2 Catalyst[J].Chinese Journal of Environmental Science,2007,28(7):1460-1465.
Authors:WANG Jian-bing  ZHU Wan-peng  WANG Wei and YANG Shao-xia
Institution:1.Department of Environmental Science and Engineering, Tsinghua University, Beijing 100084, China; 2. School of Chemical and Environmental Engineering, Beijing Campus, China University of Mining and Technology, Beijing 100083, China; 3. Department of Power Engineering, Beijing Campus, North China Electric Power University, Beijing 102206, China
Abstract:Wet air oxidation of phenol with Ru/ZrO2-CeO2 was systematically investigated and results showed that Ru/ZrO2-CeO2 could significantly increase the removal of COD and phenol. At the reaction temperature of 170 degrees C and pressure of 3MPa, about 99% COD and 100% phenol was removed respectively after 120 min. The optimal conditions were: reaction temperature, 170 degrees C; reaction pressure, 3 MPa; catalyst dosage, 5 g/L; agitator speed, 500 r/min. By analyzing intermediates, a simplified scheme of phenol oxidation was brought out. It includes two main steps. The first step is the production of organic acids, which is fast. The second step is the oxidation of organic acid, in which the oxidation of acetic acid is slow. Complete oxidation of acetic acid needs high temperature at which the radicals assault the C-H bond of a carbon and acetic acid is oxidized into carbon dioxide and water through formic acid.
Keywords:catalytic wet air oxidation  phenol  Ru/ZrO2-CeO2  catalyst
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