Catalytic Ozonation of Ethyl Acetate with Assistance of MMn2O4 (M = Cu, Co, Ni and Mg) Catalysts through In Situ DRIFTS Experiments and Density Functional Theory Calculations
{"title":"Catalytic Ozonation of Ethyl Acetate with Assistance of MMn2O4 (M = Cu, Co, Ni and Mg) Catalysts through In Situ DRIFTS Experiments and Density Functional Theory Calculations","authors":"Yulin Sun, Peixi Liu, Yiwei Zhang, Yong He, Yanqun Zhu, Zhihua Wang","doi":"10.3390/catal13121491","DOIUrl":null,"url":null,"abstract":"Catalytic ozonation, with enhanced efficiency and reduced byproduct formation at lower temperatures, proved to be efficient in ethyl acetate (EA) degradation. In this work, MMn2O4 (M = Cu, Co, Ni, Mg) catalysts were prepared via a redox-precipitation method to explore the catalytic ozonation mechanism of EA. Among all the catalysts, CuMn exhibited superior catalytic activity at 120 °C, achieving nearly 100% EA conversion and above 90% CO2 selectivity with an O3/EA molar ratio of 10. Many characterizations were conducted, such as SEM, BET and XPS, for revealing the properties of the catalysts. Plentiful active sites, abundant oxygen vacancies, more acid sites and higher reduction ability contributed to the excellent performance of CuMn. Moreover, the addition of NO induced a degree of inhibition to EA conversion due to its competition for ozone. H2O had little effect on the catalytic ozonation of CuMn, as the conversion of EA could reach a stable platform at ~89% even with 5.0 vol.% of H2O. The presence of SO2 usually caused catalyst deactivation. However, the conversion could gradually recover once SO2 was discontinued due to the reactivation of ozone. A detailed reaction mechanism for catalytic ozonation was proposed via in situ DRIFTS measurements and DFT calculations.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"80 12","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2023-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysts","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.3390/catal13121491","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
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Abstract
Catalytic ozonation, with enhanced efficiency and reduced byproduct formation at lower temperatures, proved to be efficient in ethyl acetate (EA) degradation. In this work, MMn2O4 (M = Cu, Co, Ni, Mg) catalysts were prepared via a redox-precipitation method to explore the catalytic ozonation mechanism of EA. Among all the catalysts, CuMn exhibited superior catalytic activity at 120 °C, achieving nearly 100% EA conversion and above 90% CO2 selectivity with an O3/EA molar ratio of 10. Many characterizations were conducted, such as SEM, BET and XPS, for revealing the properties of the catalysts. Plentiful active sites, abundant oxygen vacancies, more acid sites and higher reduction ability contributed to the excellent performance of CuMn. Moreover, the addition of NO induced a degree of inhibition to EA conversion due to its competition for ozone. H2O had little effect on the catalytic ozonation of CuMn, as the conversion of EA could reach a stable platform at ~89% even with 5.0 vol.% of H2O. The presence of SO2 usually caused catalyst deactivation. However, the conversion could gradually recover once SO2 was discontinued due to the reactivation of ozone. A detailed reaction mechanism for catalytic ozonation was proposed via in situ DRIFTS measurements and DFT calculations.
期刊介绍:
Catalysts (ISSN 2073-4344) is an international open access journal of catalysts and catalyzed reactions. Catalysts publishes reviews, regular research papers (articles) and short communications. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced.