Effects of Ce doping on the Fenton-like reactivity of Cu-based catalyst to the fluconazole

被引:60
作者
Zhang, Nuanqin [1 ,4 ]
Yi, Yunqiang [1 ,4 ]
Lian, Jintao [1 ,4 ]
Fang, Zhanqiang [1 ,2 ,3 ,4 ]
机构
[1] South China Normal Univ, Sch Environm, Guangzhou 510006, Peoples R China
[2] South China Normal Univ, Guangdong Prov Key Lab Chem Pollut & Environm Saf, Guangzhou 510006, Peoples R China
[3] South China Normal Univ, MOE Key Lab Theoret Chem Environm, Guangzhou 510006, Peoples R China
[4] Guangdong Technol Res Ctr Ecol Management & Remed, Guangzhou 510006, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
Fluconazole degradation; Fenton-like; Bimetallic catalyst; Reactivity enhancement; Mechanism; HETEROGENEOUS CATALYSTS; ORGANIC POLLUTANTS; SURFACE-CHEMISTRY; IRON-OXIDES; DEGRADATION; OXIDATION; COMPOSITES; ADSORPTION; NANOPARTICLES; GENERATION;
D O I
10.1016/j.cej.2020.124897
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In order to fully exploit the potential of Cu-based Fenton systems, Ce was utilized to modify the Cu-based catalysts through one-pot synthesis. A typical antifungal drug, fluconazole (FLC), was selected as the target pollutant to evaluate the reactivity of as-synthetic Cu-Ce bimetallic catalysts. Evaluation test results indicated Ce5%CuOy bimetallic materials exhibit the most excellent catalytic activity. Compared to copper monometallic catalyst, its fluconazole degradation efficiency and TOC removal rate are increased by 20% and 15%, respectively. Ce5%CuOy also possess wide pH applicability (3.0-9.0) and maintain high activity after 4 runs. Radical quenching experiments and fluorescent probes tests showed that hydroxyl radicals (center dot OH) played a dominant role in the degradation of FLC. The various characterization illustrated that Ce doping (2.5-5 at%) significantly improved the properties related to catalytic activity, such as morphology Cu(I) ratio, specific surface area, interface electron transfer rate and unpaired electron content. In particular, the increase in the unpaired electron content and Cu(I) ratio endow more electron-rich centers and active sites on the composite surface, which facilitates the H2O2 to receive electrons and decompose into center dot OH. Finally, the degradation intermediates during fluconazole oxidation were identified by LC/MC.
引用
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页数:10
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