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新型类 Fenton 体系(Mg/Fe-O)降解 4-氯苯酚。

Novel Fenton-like system (Mg/Fe-O) for degradation of 4-chlorophenol.

机构信息

College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610066, China.

College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610066, China; Key Laboratory of Treatment for Special Wastewater of Sichuan Province Higher Education System, Sichuan, Chengdu, 610066, China.

出版信息

Environ Pollut. 2019 Jul;250:906-913. doi: 10.1016/j.envpol.2019.04.096. Epub 2019 Apr 19.

Abstract

A novel heterogeneous Fenton-like system (Mg/Fe-O) which could directly convert oxygen (O) to hydrogen peroxide/hydroxyl radicals (HO/OH) was developed and used to degrade 4-chlorophenol. The Mg/Fe bimetallic particles were prepared by chemical displacement process and characterized by XRD, SEM and TEM. The in situ continuous production of HO/OH and the effect of the mole ratio of Mg to Fe in the Mg/Fe bimetallic particles and the operating parameters on the degradation 4-chlorophenol in Mg/Fe-O system were investigated in detail. It was found that the Mg/Fe bimetallic particles with the mole ratio of Mg to Fe of 32:1 had the best performance for the 4-chlorophenol degradation and the maximum cumulative concentration of HO, the degradation efficiency of 4-chlorophenol and the removal efficiency of TOC in Mg/Fe-O system were 34.5 mg/L, 100% and 91.8%, respectively, at pH 3, O flow rate 400 mL/min, dosage of Mg/Fe bimetallic particles 2 g/L, 4-chlorophenol initial concentration 50 mg/L and reaction time 60 min. It was revealed by radical scavenging experiments that OH, particularly the surface-bound OH, were the predominant reactive oxygen species in Mg/Fe-O system for the degradation of 4-chlorophenol. The main intermediates of 4-chlorophenol degradation were detected by high-resolution liquid chromatography equipped with time-of-flight mass spectrometry (HRLC-ToF-MS) and ion chromatography (IC). Based the results of control experiments and the electrochemical tests, the possible pathway and mechanism of 4-chlorophenol degradation in Mg/Fe-O system were tentatively proposed.

摘要

一种新型的非均相类芬顿体系(Mg/Fe-O),可以直接将氧气(O)转化为过氧化氢/羟基自由基(HO/OH),被开发出来并用于降解 4-氯苯酚。通过化学置换法制备了 Mg/Fe 双金属颗粒,并通过 XRD、SEM 和 TEM 进行了表征。详细研究了 HO/OH 的原位连续生成以及 Mg/Fe 双金属颗粒中 Mg 与 Fe 的摩尔比和操作参数对 Mg/Fe-O 体系中降解 4-氯苯酚的影响。结果表明,Mg 与 Fe 的摩尔比为 32:1 的 Mg/Fe 双金属颗粒在降解 4-氯苯酚方面表现出最佳性能,HO 的最大累积浓度、4-氯苯酚的降解效率和 Mg/Fe-O 体系中 TOC 的去除效率分别为 34.5mg/L、100%和 91.8%,反应条件为 pH 值 3、O 流速 400mL/min、Mg/Fe 双金属颗粒用量 2g/L、4-氯苯酚初始浓度 50mg/L、反应时间 60min。自由基捕获实验表明,OH,特别是表面结合的 OH,是 Mg/Fe-O 体系降解 4-氯苯酚的主要活性氧物质。通过高分辨率液相色谱与飞行时间质谱联用(HRLC-ToF-MS)和离子色谱(IC)检测到了 4-氯苯酚降解的主要中间产物。根据对照实验和电化学测试的结果,初步提出了 4-氯苯酚在 Mg/Fe-O 体系中降解的可能途径和机制。

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