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Efficient catalytic ozonation for ibuprofen through electron-deficient/rich centers over cerium-manganese doped carbon

SEPARATION AND PURIFICATION TECHNOLOGY [2024]
Hengxi He, Weirui Chen, Jiaxin Zhou, Xukai Li, Jing Wang, Laisheng Li
ABSTRACT

The sluggish Me (n+m)+ / Me n+ redox cycle greatly restrained the catalytic ozonation performance of metal-based catalysts. To break this bottleneck, we adopted an interfacial oxidation reaction to create electron-deficient/rich centers within carbon skeleton derived from MOF (C-MOF) by utilizing the electronegativity difference between cerium (Ce) and manganese (Mn), and evaluated its catalytic ozonation activity with ibuprofen (IBP) as model pollutant. XPS, H 2 -TPR, LSV and EPR characterizations as well as DFT calculation demonstrated that there existed electron-deficient Ce sites and electron-rich Mn sites on CeO x /MnO x /C-MOF. Under the co-function of Ce and Mn sites, CeO x /MnO x /C-MOF/O 3 process achieved 100% IBP removal in 90 min, which was 3.1 times of sole ozonation process. IBP could be absorbed at the electron-deficient Ce center and directionally donate its electron to the O 3 around electron-rich Mn center. Singlet oxygen ( 1 O 2 ) played the major role in IBP degradation. Cl − , HCO 3 − , NO 3 − and SO 4 2− demonstrated limited inhibitions on IBP degradation. This work provided a sustainable strategy for breaking the rate-limiting step in the traditional catalytic ozonation.

MATERIALS

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