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用 FeCeO 颗粒在水中对双氯芬酸进行声催化降解。

Sonocatalytic degradation of diclofenac with FeCeO particles in water.

机构信息

School of Environment & Natural Resource, Renmin University of China, Beijing 100872, China.

出版信息

Ultrason Sonochem. 2017 Jan;34:418-425. doi: 10.1016/j.ultsonch.2016.06.023. Epub 2016 Jun 20.

DOI:10.1016/j.ultsonch.2016.06.023
PMID:27773264
Abstract

This paper studies the sonocatalytic degradation of diclofenac in water using FeCeO-catalyzed ultrasound. The effects of pre-adsorption and gas addition were investigated. Nitrogen adsorption/desorption, SEM, XRD, Raman and XPS analyses of FeCeO before and after sonication were characterized. The proposed mechanism was based on the microstructure changes of FeCeO and reactive-species-scavenging performances. The results show that FeCeO has excellent performance in catalyzing an ultrasonic system in water, and 80% of diclofenac was removed in 30min ([Diclofenac]=20mg/L, FeCeO amount=0.5g/L, pH=6, ultrasonic density=3.0W/cm, ultrasonic frequency=20kHz, temperature=298K). The Fe, Ce, and O elements remained highly dispersed in the structure of FeCeO, and the solid solution structure of FeCeO remained stable after the reaction. Ce (III) was gradually oxidized to Ce (IV) and Fe (III) was gradually reduced to Fe (II) after the reaction, which indicates that Fe and Ce ions with different valences coexisted in dynamic equilibrium. The amount of oxygen vacancies in FeCeO significantly decreased after the reaction, which indicates that oxygen vacancy participated in the ultrasonic process. Singlet oxygen O was the primary reactive species in the degradation process, and the hydroxyl radicals OH and superoxide radical anion O also participated in the reaction. FeCeO had excellent chemical stability with negligible leaching ions in the ultrasonic process.

摘要

本文采用 FeCeO 催化超声研究了水中双氯芬酸的声催化降解。考察了预吸附和气体添加的影响。对超声前后的 FeCeO 进行了氮气吸附/解吸、SEM、XRD、拉曼和 XPS 分析。提出的反应机制基于 FeCeO 的微观结构变化和活性物质清除性能。结果表明,FeCeO 在水相超声体系中具有优异的催化性能,在 30min 内可去除 80%的双氯芬酸([Diclofenac]=20mg/L,FeCeO 用量=0.5g/L,pH=6,超声密度=3.0W/cm,超声频率=20kHz,温度=298K)。Fe、Ce 和 O 元素在 FeCeO 的结构中保持高度分散,反应后 FeCeO 的固溶体结构保持稳定。Ce(III) 逐渐被氧化为 Ce(IV),Fe(III) 逐渐被还原为 Fe(II),这表明不同价态的 Fe 和 Ce 离子在动态平衡中共存。反应后 FeCeO 中的氧空位数量明显减少,表明氧空位参与了超声过程。单线态氧 O 是降解过程中的主要活性物质,羟基自由基 OH 和超氧自由基 O 也参与了反应。FeCeO 在超声过程中具有优异的化学稳定性,几乎没有浸出离子。

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