4.7 Article

Efficient catalytic ozonation of ethyl acetate over Cu-Mn catalysts: Further insights into the reaction mechanism

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 477, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2023.147282

Keywords

Redox-precipitation method; Ethyl acetate; Catalytic ozonation; Cu-Mn oxides; Reaction mechanism

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A series of Cu-Mn oxides catalysts were synthesized using different precipitants for the catalytic ozonation of ethyl acetate (EA). CuMn-II with H2C2O4 as precipitant exhibited the best catalytic activity due to its abundant surface defects, oxygen vacancies, larger specific surface area, higher content of Mn3+, and more acid sites.
A series of Cu-Mn oxides were synthesized by the redox-precipitation method with different precipitants to evaluate the catalytic ozonation of ethyl acetate (EA). It was found that CuMn-II (with H2C2O4 as precipitant) exhibited the best catalytic activity, which achieved an EA conversion of 99 % at 120 degrees C with an O3/EA molar ratio of 10. The reaction temperature, O3/EA molar ratio, ozone utilization rate, and COx selectivity were also discussed. Meanwhile, many characterizations were conducted to reveal the properties of catalysts, such as SEM, XRD, BET, XPS, H2-TPR and NH3-TPD. Abundant surface defects, plentiful oxygen vacancies, larger specific surface area, higher content of Mn3+ and more acid sites contributed to the superior performance of CuMn-II. Catalyst poisoning occurred when SO2 was added, however, the conversion of EA could gradually recover to 88 % once SO2 was stopped. In-situ DRIFTS measurement was carried out to reveal the formation of intermediate species during the reaction. Combined with DFT calculations, a reaction mechanism for the catalytic ozonation of EA over CuMn2O4 catalysts was proposed.

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