Insights into Mechanism of Catalytic Ozonation over Practicable Mesoporous Mn-CeOx/γ-Al2O3 Catalysts

View Author Information
Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, Dalian University of Technology, Linggong Road 2#, Dalian 116024, China
Cite this: Ind. Eng. Chem. Res. 2018, 57, 6, 1943–1953
Publication Date (Web):January 25, 2018
https://doi.org/10.1021/acs.iecr.7b04516
Copyright © 2018 American Chemical Society
Article Views
1131
Altmetric
-
Citations
LEARN ABOUT THESE METRICS
Read OnlinePDF (7 MB)
Supporting Info (1)»

Abstract

The practicable mesoporous γ-Al2O3-supported manganese–cerium mixed oxides (Mn-CeOx/γ-Al2O3) catalysts were prepared in large quantities by a facile impregnation–calcination method. Characterization results demonstrated that the Mn-CeOx/γ-Al2O3 catalyst retained the mesoporous structure of γ-Al2O3 and existed in multivalence redox couples of Mn4+/3+ and Ce4+/3+. The surface property, catalytic performance, reaction kinetics, and mechanism of γ-Al2O3 and Mn-CeOx/γ-Al2O3 in catalytic ozonation of bromaminic acid (BAA) were investigated in-detail. The protonated surface hydroxyl groups S–OH2+ on Mn-CeOx/γ-Al2O3 were the active sites for ozone decomposition, and HO and O2•– were main reactive oxygen species. The multivalence redox couples of Mn3+/4+ and Ce3+/4+, along with electron transfer between these redox couples and lattice oxygen, resulted in the synergistically catalytic effect between Mn and Ce in Mn-CeOx. A catalytic ozonation mechanism over Mn-CeOx/γ-Al2O3 was tentatively proposed. The pilot-scale tests showed that the proposed catalytic ozonation has huge potential for the practical application in wastewater treatment.

Supporting Information

ARTICLE SECTIONS
Jump To

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.iecr.7b04516.

  • Description of the preparation process of Mn-CeOx/γ-Al2O3; the characterization techniques, including SEM-EDS, XRD, BET, XPS, FTIR, and the point of zero charges (pHPZC); catalytic ozonation procedure; analytical methods; BAA decolorization; intermediate product analysis; and pilot results (PDF)

Terms & Conditions

Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

Cited By


This article is cited by 26 publications.

  1. Qiang Cao, Fengyan Lou, Na Liu, Jisong Zhang, Lidong Wu. Continuous Catalytic Ozonation of Antibiotics Using Mn and Cu Oxides on γ-Al2O3 Pellets in a Micropacked Bed Reactor. ACS ES&T Water 2021, 1 (8) , 1911-1920. https://doi.org/10.1021/acsestwater.1c00141
  2. Shengjuan Shao, Du Lei, Yao Song, Lina Liang, Youzhi Liu, Weizhou Jiao. Cu–MnOX/γ-Al2O3 Catalyzed Ozonation of Nitrobenzene in a High-Gravity Rotating Packed Bed. Industrial & Engineering Chemistry Research 2021, 60 (5) , 2123-2135. https://doi.org/10.1021/acs.iecr.0c05751
  3. Jiayao Li, Weifeng Song, Xingchen Mao, Qiuhua Li, Zefeng Yu. Catalytic Ozonation of Dairy Farming Wastewater Using a Mn–Fe–Ce/γ-Al2O3 Ternary Catalyst: Performance, Generation, and Quenching of Hydroxyl Radicals. The Journal of Physical Chemistry C 2020, 124 (24) , 13215-13224. https://doi.org/10.1021/acs.jpcc.0c02925
  4. Da Wang, Haodan Xu, Jun Ma, Xiaohui Lu, Jingyao Qi, Shuang Song. Morphology Control Studies of MnTiO3 Nanostructures with Exposed {0001} Facets as a High-Performance Catalyst for Water Purification. ACS Applied Materials & Interfaces 2018, 10 (37) , 31631-31640. https://doi.org/10.1021/acsami.8b11132
  5. Haibao Liu, Yue Gao, Jie Wang, Jingwen Pan, Baoyu Gao, Qinyan Yue. Catalytic ozonation performance and mechanism of [email protected]γ-Al2O3/O3 in the treatment of sulfate-containing hypersaline antibiotic wastewater. Science of The Total Environment 2022, 807 , 150867. https://doi.org/10.1016/j.scitotenv.2021.150867
  6. Hariraj Singh, Brijesh Kumar Mishra. Recent applications, reaction mechanism, and future perspective of hybrid ozonation process for water and wastewater treatment. 2022,,, 459-484. https://doi.org/10.1016/B978-0-323-85583-9.00009-0
  7. Shengjuan Shao, Zhixing Li, Kechang Gao, Jingwen Zhang, Youzhi Liu, Weizhou Jiao. Preparation of Cu-MnOX/γ-Al2O3 by high gravity-assisted impregnation method for heterogeneous catalytic ozonation of nitrobenzene. Separation and Purification Technology 2022, 280 , 119896. https://doi.org/10.1016/j.seppur.2021.119896
  8. Zhixing Li, Jiaxin Jing, Kechang Gao, Gaomiao Ren, Jingwen Zhang, Weizhou Jiao, Youzhi Liu. Degradation of nitrobenzene by high-gravity intensified heterogeneous catalytic ozonation with Mn-Fe/ZSM-5 catalysts. Chemical Engineering and Processing - Process Intensification 2021, 169 , 108642. https://doi.org/10.1016/j.cep.2021.108642
  9. Jing Liu, Lingjie Ke, Lei Sun, Fei Pan, Xiangjuan Yuan, Dongsheng Xia. Unraveling the multiple roles of Ag species incorporation into OMS-2 for efficient catalytic ozonation: Structural properties and mechanism investigation. Journal of Environmental Chemical Engineering 2021, 9 (5) , 106199. https://doi.org/10.1016/j.jece.2021.106199
  10. Soumya Ranjan Mishra, Md. Ahmaruzzaman. Cerium oxide and its nanocomposites: Structure, synthesis, and wastewater treatment applications. Materials Today Communications 2021, 28 , 102562. https://doi.org/10.1016/j.mtcomm.2021.102562
  11. Yuanmei Chen, Yutang Xiao, Guanping Wang, Wei Shi, Linquan Sun, Yanfang Chen, Aichun Miao. A pilot-scale test on the treatment of biological pretreated leachate by the synergy of ozonation-biological treatment-catalytic ozonation. Environmental Engineering Research 2021, 26 (4) , 200349-0. https://doi.org/10.4491/eer.2020.349
  12. Shengkai Xu, Jiaxin Yang, Rafaat Hussein, Guangqing Liu, Bensheng Su. Heterogeneous ozonation of ofloxacin using MnO x ‐CeO x /γ‐Al 2 O 3 as a catalyst: Performances, degradation kinetics and possible degradation pathways. Water Environment Research 2021, 93 (8) , 1361-1369. https://doi.org/10.1002/wer.1524
  13. Hongbin Jiang, Rao Zhang, Jialiang Hao, Xiaochen Xu, Jie Chen, Yun Zhang, Fenglin Yang. Design, preparation, characterization, and application of MnxCu1-xOy/γ-Al2O3 catalysts in ozonation to achieve simultaneous organic carbon and nitrogen removal in pyridine wastewater. Science of The Total Environment 2021, 774 , 145189. https://doi.org/10.1016/j.scitotenv.2021.145189
  14. Pengwei Yan, Zhonglin Chen, Shuyu Wang, Yanchi Zhou, Li Li, Lei Yuan, Jimin Shen, Qianqian Jin, Xiaoxiao Zhang, Jing Kang. Catalytic ozonation of iohexol with α-Fe0.9Mn0.1OOH in water: Efficiency, degradation mechanism and toxicity evaluation. Journal of Hazardous Materials 2021, 402 , 123574. https://doi.org/10.1016/j.jhazmat.2020.123574
  15. Hua Chen, Cunxia Fang, Xingmin Gao, Guanyun Jiang, Xiaoning Wang, Sheng-Peng Sun, Winston Duo Wu, Zhangxiong Wu. Sintering- and oxidation-resistant ultrasmall Cu(I)/(II) oxides supported on defect-rich mesoporous alumina microspheres boosting catalytic ozonation. Journal of Colloid and Interface Science 2021, 581 , 964-978. https://doi.org/10.1016/j.jcis.2020.09.002
  16. Tongdong Shen, Wentao Su, Qiangqiang Yang, Jun Ni, Shaoping Tong. Synergetic mechanism for basic and acid sites of MgMxOy (M = Fe, Mn) double oxides in catalytic ozonation of p-hydroxybenzoic acid and acetic acid. Applied Catalysis B: Environmental 2020, 279 , 119346. https://doi.org/10.1016/j.apcatb.2020.119346
  17. Hongbin Jiang, Xiaochen Xu, Rao Zhang, Jie Chen, Yexin Wang, Yun Zhang, Fenglin Yang. A novel combined treatment for pyridine waste gas using liquid absorption, catalytic ozonation, and sulfur autotrophic denitrification (LA-CO-SAD). Chemical Engineering Journal 2020, 400 , 125997. https://doi.org/10.1016/j.cej.2020.125997
  18. Manju Kurian. Cerium oxide based materials for water treatment – A review. Journal of Environmental Chemical Engineering 2020, 8 (5) , 104439. https://doi.org/10.1016/j.jece.2020.104439
  19. Bing Liu, Peng An, Jie Chen, Xiaochen Xu, Lifen Liu, Fenglin Yang. A novel method for preparation of polyaluminum phosphoric sulfate (PAPS) coagulant using SAPO-34 mother liquor: Characterization and coagulation performance. Process Safety and Environmental Protection 2020, 140 , 380-391. https://doi.org/10.1016/j.psep.2020.04.036
  20. Xingyue Wei, Shengjuan Shao, Xin Ding, Weizhou Jiao, Youzhi Liu. Degradation of phenol with heterogeneous catalytic ozonation enhanced by high gravity technology. Journal of Cleaner Production 2020, 248 , 119179. https://doi.org/10.1016/j.jclepro.2019.119179
  21. Lei Xu, Shaoyu Tang, Kaixuan Wang, Xiao Ma, Junfeng Niu. Insights into the degradation and detoxication mechanisms of aqueous capecitabine in electrochemical oxidation process. Chemosphere 2020, 241 , 125058. https://doi.org/10.1016/j.chemosphere.2019.125058
  22. Jianrui Niu, Haobin Liu, Hengli Qian, Jie Liu, Mengyuan Ma, Erhong Duan, Lei Yu. Preparation of metal-doped Cu–Mn/HTS-1 catalysts and their mechanisms in efficient degradation of toluene. Journal of Environmental Sciences 2020, 88 , 260-272. https://doi.org/10.1016/j.jes.2019.08.019
  23. Tongdong Shen, Xiaofang Zhang, Kun-Yi Andrew Lin, Shaoping Tong. Solid base Mg-doped ZnO for heterogeneous catalytic ozonation of isoniazid: Performance and mechanism. Science of The Total Environment 2020, 703 , 134983. https://doi.org/10.1016/j.scitotenv.2019.134983
  24. Jianlong Wang, Hai Chen. Catalytic ozonation for water and wastewater treatment: Recent advances and perspective. Science of The Total Environment 2020, 704 , 135249. https://doi.org/10.1016/j.scitotenv.2019.135249
  25. Omid Nemati Sani, Ali Asghar Navaei fezabady, Mohsen Yazdani, Mahmoud Taghavi. Catalytic ozonation of ciprofloxacin using γ-Al2O3 nanoparticles in synthetic and real wastewaters. Journal of Water Process Engineering 2019, 32 , 100894. https://doi.org/10.1016/j.jwpe.2019.100894
  26. Cunxia Fang, Xingmin Gao, Xiangcheng Zhang, Jiahui Zhu, Sheng-Peng Sun, Xiaoning Wang, Winston Duo Wu, Zhangxiong Wu. Facile synthesis of alkaline-earth metal manganites for the efficient degradation of phenolic compounds via catalytic ozonation and evaluation of the reaction mechanism. Journal of Colloid and Interface Science 2019, 551 , 164-176. https://doi.org/10.1016/j.jcis.2019.05.010