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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

Journal 2022 · IF 8.943 · 发表于 2022 年 1 月 5 日
作者: Dongpo Liu,Muxin Lin,Weirui Chen,Jing Wang,Xingmei Guo,Xukai Li,Laisheng Li
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摘要

Fe-MCM-41 had been widely used as ozonation catalyst, however, the existence of large amount of hydrophilic silanol hindered its interfacial reaction with O 3 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 O 3 decomposition into •OH. F–Fe-MCM-41/O 3 exhibited notably activity with 96.6% IBP removal efficiency within 120 min, while only 78.5% and 80.9% in O 3 alone and Fe-MCM-41/O 3 , respectively. Surface Lewis acid sites and metal hydroxyl groups were considered as important factors for O 3 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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