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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
Received:15 November 2018,
Revised:2019-02-27,
Online First:15 June 2020,
Published:12 April 2019
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于海斌, 刘强, 周立坤, 陈赞, 罗超, 张贯艳, 乔利娜, 王建杰. MnOx/ZrO2催化剂制备及催化臭氧氧化降解甲基橙[J]. 化工学报, 2019, 70(4): 1436-1445 DOI: 10.11949/j.issn.0438-1157.20181346.
YU Haibin, LIU Qiang, ZHOU Likun, CHEN Zan, LUO Chao, ZHANG Guanyan, QIAO Lina, WANG Jianjie. Preparation of MnOx/ZrO2 catalyst and catalytic ozonation degradation of methylorange[J]. CIESC Journal, 2019, 70(4): 1436-1445 DOI: 10.11949/j.issn.0438-1157.20181346.
于海斌, 刘强, 周立坤, 陈赞, 罗超, 张贯艳, 乔利娜, 王建杰. MnOx/ZrO2催化剂制备及催化臭氧氧化降解甲基橙[J]. 化工学报, 2019, 70(4): 1436-1445 DOI: 10.11949/j.issn.0438-1157.20181346. DOI:
YU Haibin, LIU Qiang, ZHOU Likun, CHEN Zan, LUO Chao, ZHANG Guanyan, QIAO Lina, WANG Jianjie. Preparation of MnOx/ZrO2 catalyst and catalytic ozonation degradation of methylorange[J]. CIESC Journal, 2019, 70(4): 1436-1445 DOI: 10.11949/j.issn.0438-1157.20181346. DOI:
以商品化ZrO
2
为载体,采用等体积浸渍法制备MnO
x
/ZrO
2
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
/ZrO
2
(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
/ZrO
2
(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。
The MnO
x
/ZrO
2
catalyst was prepared by the equal volume impregnation method with commercial ZrO
2
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
/ZrO
2
(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
/ZrO
2
(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
/ZrO
2
(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.
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