华南理工大学学报(自然科学版) ›› 2017, Vol. 45 ›› Issue (6): 117-123,130.doi: 10.3969/j.issn.1000-565X.2017.06.018

• 化学化工 • 上一篇    下一篇

苯酚在 CeO2 -ZSM-5固定床反应器上的湿式催化降解

杨逸 张会平 鄢瑛   

  1. 华南理工大学 化学与化工学院,广东 广州 510640
  • 收稿日期:2016-07-07 修回日期:2016-12-30 出版日期:2017-06-25 发布日期:2017-05-02
  • 通信作者: 鄢瑛(1982-),女,博士,副研究员,主要从事吸附与催化反应工程研究. E-mail:yingyan@scut.edu.cn
  • 作者简介:杨逸(1994-),男,博士生,主要从事废水处理研究. E-mail:y.y05@mail.scut.edu.cn
  • 基金资助:

    国家自然科学基金资助项目(21376101);华南理工大学中央高校基本科研基金资助项目(2015Z2116);珠江科 技新星专项(201610010171)

Catalytic Wet Peroxide Oxidation of Phenol on CeO2 -ZSM-5 Fixed Bed Reactor

YANG Yi ZHANG Hui-ping YAN Ying   

  1. School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510640,Guangdong,China
  • Received:2016-07-07 Revised:2016-12-30 Online:2017-06-25 Published:2017-05-02
  • Contact: 鄢瑛(1982-),女,博士,副研究员,主要从事吸附与催化反应工程研究. E-mail:yingyan@scut.edu.cn
  • About author:杨逸(1994-),男,博士生,主要从事废水处理研究. E-mail:y.y05@mail.scut.edu.cn
  • Supported by:

     Supported by the National Natural Science Foundation of China(21376101)

摘要: 采用浸渍法制备 CeO2 -ZSM-5 分子筛催化剂,并将其用于固定床反应器来湿式催 化氧化苯酚废水. 采用 X 射线衍射、N2 吸附和脱附对分子筛的物相结构、比表面积和孔结 构进行表征,然后对比不同温度、床层高度、进料流速对苯酚转化率、H2 O2 转化率、TOC (总有机碳)转化率、活性组分浸出率和 CO2 选择性的影响. 表征结果表明,CeO2 -ZSM-5 分子筛催化剂为微孔材料,负载活性组分前后其晶型没有明显变化,但比表面积减小. 活性评价实验结果表明:随着温度的升高和进料流速的减小,H2 O2  转化率、苯酚转化率、 TOC 转化率和 CO2 选择性逐渐增大;随着床层高度的增加,H2 O2  转化率、苯酚转化率、 TOC 转化率逐渐增大,CO2 选择性则逐渐降低;各条件下,催化剂活性组分浸出率较小,稳定性较好,且降解过程不产生副产物.

关键词: 苯酚, 固定床反应器, 湿式催化氧化, 浸渍法, 催化剂活性

Abstract:

In this paper,first,CeO2 -ZSM-5 zeolite catalysts were prepared by means of impregnation method and were applied to the catalytic wet peroxide oxidation of phenol in a fixed bed reactor.Then,the phase structure,specific surface area and pore structure of CeO2 -ZSM-5 were characterized via XRD and N2adsorption-desorption.Finally,the effects of temperature,bed height and feed flow rate on the conversion rates of phenol,H2O2 and total organic carbon (TOC),as well as on the cerium leaching concentration and the selectivity of CO2 ,were investiga- ted.Characterization results show that CeO2 -ZSM-5 catalysts are micro-pore materials; and that,after the loading of active components,the crystal form of CeO2 -ZSM-5 almost keeps unchanged but the specific surface area decrea- ses.Moreover,from the activity evaluation results,it is found that (1) the conversion rates of phenol,H2O2 and TOC,as well as the selectivity of CO2 all increase with the increase of temperature and with the decrease of feed flow rate; (2) with the increase of bed height,the conversion rates of phenol,H2O2 and TOC all increase,while the selectivity of CO2 decreases; (3) the cerium leaching concentration is small under all conditions,which means that the catalysts possess good stability; and (4) no by-products are observed in the process of CWPO.

Key words: phenol, fixed bed reactor, catalytic wet peroxide oxidation, impregnation method, catalyst activity

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