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磁性碳负载普鲁士蓝纳米复合材料活化过一硫酸盐用于单线态氧和超氧自由基降解有机污染物。

Activation of peroxymonosulfate by magnetic carbon supported Prussian blue nanocomposite for the degradation of organic contaminants with singlet oxygen and superoxide radicals.

机构信息

School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200, China.

Engineering Research Centre for Cleaner Production of Textile Printing and Dyeing, Ministry of Education, Wuhan, 430200, China.

出版信息

Chemosphere. 2019 Mar;218:1071-1081. doi: 10.1016/j.chemosphere.2018.11.197. Epub 2018 Nov 29.

Abstract

In order to develop efficient and green catalyst for organic pollutants removal, magnetic carbon supported Prussian blue nanocomposite FeO@C/PB was prepared for the first time. The performance of FeO@C/PB in activating peroxymonosulfate (PMS) for the degradation of 2,4-dichlorophenol (2,4-DCP) was investigated. 2,4-DCP could be effectively degraded under the "FeO@C/PB + PMS" system within a broad pH range of 2-9. Without pH adjustment (pH 3), 2,4-DCP (20 mg/L) was completely degraded in 50 min along with a 70% removal of TOC; while the required time for complete degradation of 2,4-DCP was shortened to 40 min under initial solution pH at 7. FeO@C/PB could also activate PMS for the degradation of phenol, Acid Orange II, Reactive brilliant red X-3B, Rhodamine B and Methylene blue. The degradation rates higher than 95% could be achieved for all these contaminants within the time scale of 15-60 min. The studies of radical-quenching and electron paramagnetic resonance demonstrated that singlet oxygen (O) and superoxide radicals (O), rather than sulfate (SO) and hydroxyl (OH) radicals, were the dominant species responsible for the oxidation of organic pollutants. The plausible mechanism of the catalytic degradation was proposed and the enhanced activity of FeO@C/PB was assumed to be related to the increased electron transfer owing to the synergic effect between the magnetic carbon and the mixed-valence units in PB. FeO@C/PB is promising in wastewater treatment owing to its high efficiency, excellent stability and reusability, environmental friendliness and magnetic separability.

摘要

为了开发高效、绿色的有机污染物去除催化剂,首次制备了磁性碳负载普鲁士蓝纳米复合材料 FeO@C/PB。研究了 FeO@C/PB 在活化过一硫酸盐(PMS)降解 2,4-二氯苯酚(2,4-DCP)中的性能。在较宽的 pH 值范围(2-9)内,无需 pH 调节(pH 3),FeO@C/PB+PMS 体系中 2,4-DCP(20mg/L)可在 50min 内有效降解,TOC 去除率达 70%;而在初始溶液 pH 值为 7 时,2,4-DCP 的完全降解时间缩短至 40min。FeO@C/PB 还可以活化 PMS 降解苯酚、酸性橙 II、活性艳红 X-3B、罗丹明 B 和亚甲蓝。在 15-60min 的时间内,所有这些污染物的降解率均高于 95%。自由基猝灭和电子顺磁共振研究表明,单线态氧(O)和超氧自由基(O),而不是硫酸盐(SO)和羟基(OH)自由基,是氧化有机污染物的主要物种。提出了催化降解的可能机制,并假设 FeO@C/PB 的增强活性与磁性碳和 PB 中混合价单元之间的协同效应导致的电子转移增加有关。由于其高效、稳定性和可重复使用性、环境友好性和磁性分离性,FeO@C/PB 在废水处理中具有广阔的应用前景。

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