Enhancing catalytic ozonation activity of MCM-41 via one-step incorporating fluorine and iron: The interfacial reaction induced by hydrophobic sites and Lewis acid sites
Fe-MCM-41 had been widely used as ozonation catalyst, however, the existence of large amount of hydrophilic silanol hindered its interfacial reaction with O3 and pollutants. To solve this problem, F–Fe-MCM-41 was synthesized by co-doping F and Fe into the framework of MCM-41 to replace silanol with...
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Published in | Chemosphere (Oxford) Vol. 292; p. 133544 |
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Main Authors | , , , , , , |
Format | Journal Article |
Language | English |
Published |
England
Elsevier Ltd
01.04.2022
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Subjects | |
Online Access | Get full text |
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Summary: | Fe-MCM-41 had been widely used as ozonation catalyst, however, the existence of large amount of hydrophilic silanol hindered its interfacial reaction with O3 and pollutants. To solve this problem, F–Fe-MCM-41 was synthesized by co-doping F and Fe into the framework of MCM-41 to replace silanol with Si–F groups through a one-step hydrothermal method. F introduced hydrophobic sites which contributed to more ibuprofen (IBP) chemisorption on the surface of F–Fe-MCM-41. Moreover, doping F also enhanced the acidity, which accelerated O3 decomposition into •OH. F–Fe-MCM-41/O3 exhibited notably activity with 96.6% IBP removal efficiency within 120 min, while only 78.5% and 80.9% in O3 alone and Fe-MCM-41/O3, respectively. Surface Lewis acid sites and metal hydroxyl groups were considered as important factors for O3 activation and •OH generation. F–Fe-MCM-41 exhibited excellent catalytic performance under acidic and alkaline conditions. Comparative experiments revealed that F doping improved the interfacial reaction, especially the interfacial electron transfer, which resulted in the high catalytic activity of F–Fe-MCM-41. F–Fe-MCM-41 possessed good stability and reusability, with only 5.7% decline for IBP removal in five successive cycles. Furthermore, the possible degradation path of IBP was proposed according to DFT calculation and GC-MS analysis.
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•F–Fe-MCM-41 exhibited a good activity in catalytic ozonation for IBP.•Si–F bond successfully replaced silanol in the framework of Fe-MCM-41.•Hydrophobicity of F–Fe-MCM-41 contributed to more IBP chemisorption.•Strong Lewis acidity accelerated ozone decomposition to produce more .•OH;•The interfacial reaction played a dominant role in the catalytic ozonation process. |
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Bibliography: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 0045-6535 1879-1298 |
DOI: | 10.1016/j.chemosphere.2022.133544 |