4.7 Article

Sulfite activation by Jahn-Teller-driven oxygen vacancies Cu-Mn composite oxide for chlortetracycline degradation

Journal

JOURNAL OF HAZARDOUS MATERIALS
Volume 461, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.jhazmat.2023.132658

Keywords

Hydrolysis-driven oxidation reduction method; Copper-manganese metal oxides; Sulfite activation; Pharmaceuticals and personal care products; DFT calculation

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Copper-manganese composite metal oxides were used for the first time to activate sulfite and degrade chlortetracycline hydrochloride. The study identified the optimal degradation conditions and confirmed the important role of reactive oxygen species in the degradation process. The copper-manganese composite metal oxides showed excellent catalytic performance and stability, with potential applications in water treatment.
Copper-manganese composite metal oxides (CuMnOy) were prepared by hydrolysis-driven oxidation-reduction method and used to activate sulfite to degrade chlortetracycline hydrochloride (CTC) for the first time. The Jahn -Teller ions Mn3+ and Cu2+ exist in CuMnOy, which form a solid electric charge transport redox system and ensure the continuous generation of reactive oxygen species (ROS). Through the systematic study of the experimental parameters such as sulfite concentration, catalyst metal molar ratio, catalyst amounts and initial pH, the optimal degradation rate of CTC could reach 91.74% within 10 min and 94.46% after 30 min. The major reactive radicals were determined by radical quenching experiments and electron paramagnetic resonance (EPR) trapping techniques, and it was confirmed that SO4 center dot-and center dot O2- played a nonnegligible role in the process of degrading CTC. Density functional theory (DFT) calculations show that higher Fukui indices (f -and f 0) of CTC sites are more vulnerable to free radical attack. CuMnOy has low CTC degradation intermediate toxicity, high catalytic performance, good anti-interference ability, reusability and stability, and possesses decent application potential in the actual water treatment field.

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