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

J Hazard Mater

Eco-environment and Resource Efficiency Research Laboratory, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen, Guangdong 518055, China. Electronic address:

Published: January 2024

Copper-manganese composite metal oxides (CuMnO) 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 Mn and Cu exist in CuMnO, 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 SO and •O played a nonnegligible role in the process of degrading CTC. Density functional theory (DFT) calculations show that higher Fukui indices (f and f) of CTC sites are more vulnerable to free radical attack. CuMnO 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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http://dx.doi.org/10.1016/j.jhazmat.2023.132658DOI Listing

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