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Modulation of reaction pathway of Prussian blue analogues derived Zn-Fe double oxides towards organic pollutants oxidation
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-11-08 , DOI: 10.1016/j.cej.2022.140103
Liang Zhang , Bofan Zhang , Yunxia Liu , Zinan Wang , Jafar Hussain Shah , Rile Ge , Wenhui Zhou , Shiro Kubuki , Junhu Wang

The radical-based Fenton-like reaction quenching by various inorganic anions or high concentration of organic matters restrict the practical value in future industrial application. Contrarily, the nonradical-dominated system could efficiently overcome above limitations and achieve excellent catalytic capacity under a wide category of water matrixes. Herein, a series of Zn-Fe double oxides were successfully fabricated via calcination of Zn1-xFex-Fe Prussian blue analogues under ambient atmosphere. Under the coexistence of visible light and peroxymonosulfate (PMS), Zn-Fe double oxides manifested excellent catalytic performance towards various organic pollutants oxidation with trace amount of iron leaching, and even showed superior contaminant decomposition efficiency under high concentration of organic matter and practical aqueous system. Confirmed by radical trapping experiment and electron paramagnetic resonance spectroscopy, the photo-induced electrons and holes can act as triggers to PMS activation and thereby transform reaction routes from radicals to singlet oxygen (1O2)-dominated nonradical pathway over the prepared Zn-Fe double oxides. This work provided new insights and comprehension into modulating radical and nonradical pathways of PMS-based advanced oxidation process for refractory contaminant oxidation via utilizing solar energy.



中文翻译:

普鲁士蓝类似物衍生的 Zn-Fe 双氧化物对有机污染物氧化反应途径的调控

各种无机阴离子或高浓度有机物对自由基类Fenton反应的猝灭限制了未来工业应用的实用价值。相反,非自由基主导的体系可以有效地克服上述限制,并在多种水基质下实现优异的催化能力。本文通过煅烧 Zn 1-x Fe x成功制备了一系列 Zn-Fe 双氧化物。-Fe 普鲁士蓝类似物在环境大气下。在可见光和过一硫酸盐(PMS)共存下,Zn-Fe双氧化物对各种有机污染物氧化表现出优异的催化性能,微量铁浸出,甚至在高浓度有机物和实用水体系下表现出优异的污染物分解效率. 自由基捕获实验和电子顺磁共振谱证实,光诱导电子和空穴可以作为PMS活化的触发器,从而将反应路线从自由基转变为单线态氧( 1 O 2)-在制备的 Zn-Fe 双氧化物上占主导地位的非自由基途径。这项工作为利用太阳能调节基于 PMS 的高级氧化过程的自由基和非自由基途径提供了新的见解和理解,以实现难降解污染物的氧化。

更新日期:2022-11-11
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