化工学报 ›› 2019, Vol. 70 ›› Issue (4): 1436-1445.DOI: 10.11949/j.issn.0438-1157.20181346

• 催化、动力学与反应器 • 上一篇    下一篇

MnO x /ZrO2 催化剂制备及催化臭氧氧化降解甲基橙

于海斌1,2(),刘强1,周立坤2,陈赞2,罗超2,张贯艳1,乔利娜3,王建杰3   

  1. 1. 河北工业大学化工学院,天津 300132
    2. 中海油天津化工研究设计院有限公司,天津 300131
    3. 天津大学化工学院,天津 300072
  • 收稿日期:2018-11-15 修回日期:2019-02-27 出版日期:2019-04-05 发布日期:2019-04-05
  • 通讯作者: 于海斌
  • 作者简介:于海斌(1970—),男,教授级高级工程师,<email>yuhaibin9227@163.com</email>
  • 基金资助:
    天津市科技计划项目(18YFZCSF01440)

Preparation of MnO x /ZrO2 catalyst and catalytic ozonation degradation of methylorange

Haibin YU1,2(),Qiang LIU1,Likun ZHOU2,Zan CHEN2,Chao LUO2,Guanyan ZHANG1,Jianjie QIAO Lina WANG3   

  1. 1. School of Chemical Engineering, Hebei University of Technology, Tianjin 300132, China
    2. CenerTech Tianjin Chemical Research and Design Institute Limited Liability Company, Tianjin 300131, China, 3School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
  • Received:2018-11-15 Revised:2019-02-27 Online:2019-04-05 Published:2019-04-05
  • Contact: Haibin YU

摘要:

以商品化ZrO2为载体,采用等体积浸渍法制备MnO x /ZrO2催化剂,对目标污染物甲基橙溶液进行催化臭氧降解效果研究。比较不同焙烧温度(350、400、500和550℃)、不同MnO x 负载量(5%、10%、15%和18%)等制备条件对催化剂活性的影响,结果表明:在400℃,MnO x 负载量为15%时,催化剂对催化臭氧降解甲基橙溶液表现出最好的活性。反应进行60 min后,甲基橙溶液的脱色率达92.8%,较单独臭氧氧化提高了36.1%。催化剂15%MnO x /ZrO2(400℃)的酸碱使用范围(pH为2.7、6.5、8.7、10.8)实验表明:甲基橙溶液不同初始pH条件同样会影响催化剂的活性,且pH=2.7时表现出最好的催化效果,甲基橙脱色率可达95%。循环实验表明,15%MnO x /ZrO2(400℃)具有较好的稳定性,催化剂循环使用三次后,甲基橙溶液脱色率仍保持在85%以上,且活性组分的流失是降低催化剂活性的一个重要原因。

关键词: 等体积浸渍法, 催化剂, 甲基橙, 催化臭氧氧化, 脱色反应

Abstract:

The MnO x /ZrO2 catalyst was prepared by the equal volume impregnation method with commercial ZrO2 as carrier, and the catalytic ozone degradation effect of the target pollutant methyl orange solution was studied. The factors of calcination temperature and MnO x loading content were studied to determine the optimal catalyst preparation condition. It turned out that, the catalyst would get the best catalytic activity with 15% MnO x loading and being calcined at 400℃, and the decolorization efficiency of methyl orange was 92.8% over the catalyst of 15%MnO x /ZrO2 (400℃), which increased by 36.1% compared with that in the ozonation without catalyst after 60 min of reaction. Also, the initial pH of methyl orange solution (pH =2.7,6.5,8.7,10.8) was investigated during the catalytic ozonation process. The 15%MnO x /ZrO2 (400℃) catalyst performed a higher catalytic efficiency of 95% at pH=2.7 than that value of 6.5 without adjustment by acid or alkali. The catalyst cycle test showed a better stability for 15%MnO x /ZrO2 (400℃), and the decolorization rate of methyl orange slightly drop down to about 85% after three times reuse. Moreover,the loss of MnO x was an important reason for the descent of catalyst activity by characterization experiments.

Key words: incipient wetness impregnation method, catalyst, methyl orange, catalytic ozonation, decolorization reaction

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