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Effects of Ce doping on the Fenton-like reactivity of Cu-based catalyst to the fluconazole
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-04-04 , DOI: 10.1016/j.cej.2020.124897
Nuanqin Zhang , Yunqiang Yi , Jintao Lian , Zhanqiang Fang

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 (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 OH. Finally, the degradation intermediates during fluconazole oxidation were identified by LC/MC.



中文翻译:

Ce掺杂对Cu基催化剂对氟康唑类芬顿反应性的影响

为了充分利用铜基Fenton体系的潜力,利用Ce通过一锅法合成法对铜基催化剂进行了改性。选择一种典型的抗真菌药物氟康唑(FLC)作为目标污染物,以评估合成的Cu-Ce双金属催化剂的反应性。评估测试结果表明,Ce 5% CuO y双金属材料表现出最优异的催化活性。与铜单金属催化剂相比,氟康唑的降解效率和TOC去除率分别提高了20%和15%。Ce 5% CuO y还具有广泛的pH适用性(3.0–9.0),并且在运行4次后仍保持高活性。自由基淬灭实验和荧光探针测试表明,羟基自由基(OH)在FLC的降解中起主要作用。各种表征表明,Ce掺杂(2.5-5 at%)显着改善了与催化活性有关的特性,例如形态Cu(I)比,比表面积,界面电子传输速率和不成对电子含量。特别地,未成对电子含量和Cu(I)比的增加在复合材料表面上赋予了更多的富电子中心和活性位,这有利于H 2 O 2接收电子并分解成OH。最后,通过LC / MC鉴定了氟康唑氧化过程中的降解中间体。

更新日期:2020-04-20
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