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以Co(II)-CeO为新型非均相催化剂介导过一硫酸盐高效活化用于降解难降解有机污染物:降解途径、机理及毒性评估

Efficient activation of peroxymonosulfate mediated by Co(II)-CeO as a novel heterogeneous catalyst for the degradation of refractory organic contaminants: Degradation pathway, mechanism and toxicity assessment.

作者信息

Di Siyuan, Wang Jiahao, Zhai Yixin, Chen Pin, Ning Tao, Shi Chunxiang, Yang Hucheng, Bao Yue, Gao Qiang, Zhu Shukui

机构信息

State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074, China.

Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China.

出版信息

J Hazard Mater. 2022 Aug 5;435:129013. doi: 10.1016/j.jhazmat.2022.129013. Epub 2022 Apr 27.

DOI:10.1016/j.jhazmat.2022.129013
PMID:35523092
Abstract

A series of Co(II)-CeO mixed metal oxides were synthesized by a facile hydrothermal-calcination procedure for activating peroxymonosulfate (PMS) and degrading toxic and difficult biodegradable organics. Co(II)-CeO showed excellent degradation performance toward rhodamine B (RhB), toluidine blue, methylene blue and diclofenac. RhB is a refractory organic contaminant, and ecotoxicological evaluation unraveled its harmfulness to the biosphere. RhB was selected as the model pollutant to investigate catalytic mechanisms. Parameters affecting degradation performance were profoundly investigated, including Co:Ce feed ratio, initial pH, PMS dosage, catalyst dosage, RhB concentration, coexisting ions and reaction temperature. Reaction mechanisms were proposed based on density functional theory calculations and identifications of reactive oxygen species. Improvements have been achieved in seven aspects compared to previous studies, including 100% degradation ratio in both real water samples and each reuse of the catalyst, ultrafast degradation rate, cost-effectiveness of the catalyst, toxicity-attenuation provided by the developed degradation method, high degree of mineralization for the model pollutant, negligible leaching of active sites, and the enhancement of catalytic performance by utilizing trace leached cobalt, endowing the technique with broad applicability and prospect.

摘要

通过简便的水热-煅烧程序合成了一系列Co(II)-CeO混合金属氧化物,用于活化过一硫酸盐(PMS)并降解有毒且难生物降解的有机物。Co(II)-CeO对罗丹明B(RhB)、甲苯胺蓝、亚甲基蓝和双氯芬酸表现出优异的降解性能。RhB是一种难降解的有机污染物,生态毒理学评估揭示了其对生物圈的危害。选择RhB作为模型污染物来研究催化机制。深入研究了影响降解性能的参数,包括Co:Ce进料比、初始pH值、PMS用量、催化剂用量、RhB浓度、共存离子和反应温度。基于密度泛函理论计算和活性氧物种的鉴定提出了反应机制。与先前的研究相比,在七个方面取得了改进,包括在实际水样中以及催化剂的每次重复使用中均实现100%的降解率、超快的降解速率、催化剂的成本效益、所开发的降解方法提供的毒性衰减、模型污染物的高矿化度、活性位点的浸出可忽略不计以及利用微量浸出钴提高催化性能,赋予该技术广泛的适用性和前景。

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