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

被引:45
作者
Liu, Mingyi [1 ,2 ]
Chen, Hanchun [2 ]
Xiao, Pengfei [1 ]
Ji, Haodong [2 ]
机构
[1] Northeast Forestry Univ, Coll Forestry, Harbin 150040, Peoples R China
[2] Peking Univ, Sch Environm & Energy, Ecoenvironm & Resource Efficiency Res Lab, Shenzhen Grad Sch, Shenzhen 518055, Guangdong, Peoples R China
基金
中国国家自然科学基金;
关键词
Hydrolysis-driven oxidation reduction method; Copper-manganese metal oxides; Sulfite activation; Pharmaceuticals and personal care products; DFT calculation; ENHANCED DEGRADATION; RAMAN-SPECTROSCOPY; CATALYZED SULFITE; FACILE SYNTHESIS; OXIDATION; COPPER; KINETICS; PEROXYMONOSULFATE; INACTIVATION; AUTOXIDATION;
D O I
10.1016/j.jhazmat.2023.132658
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
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.
引用
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页数:18
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