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

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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
Copyright © 2018 American Chemical Society
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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.

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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)

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