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负载在多壁碳纳米管上的磁性 CuNiFeO 纳米粒子作为一种新型催化剂用于过一硫酸盐活化和降解活性黑 5。

Magnetic CuNiFeO nanoparticles loaded on multi-walled carbon nanotubes as a novel catalyst for peroxymonosulfate activation and degradation of reactive black 5.

机构信息

Department of Environment, College of Environmental Engineering, Branch Bushehr, Islamic Azad University, Bushehr, Iran.

Department of Environmental Health Engineering, Behbahan Faculty of Medical Sciences, Behbahan, Iran.

出版信息

Environ Sci Pollut Res Int. 2021 Oct;28(40):57099-57114. doi: 10.1007/s11356-021-14590-2. Epub 2021 Jun 3.

Abstract

Novel copper-nickel ferrite nanocatalyst loaded on multi-walled carbon nanotube (MWCNTs-CuNiFeO) was synthesized and applied to activate peroxymonosulfate (PMS) in the degradation of the reactive black 5 (RB5). The structure of the catalyst was well characterized by scanning electron microscope (SEM), Fourier-transform infrared spectroscopy (FTIR), and X-ray powder diffraction (XRD). The MWCNTs-CuNiFeO/PMS system showed a high performance in the degradation of RB5 with a kinetic rate of 1.5-2.5 times higher than homogeneous and heterogeneous systems. Maximum degradation efficiency (99.60%) was obtained at an initial pH of 7, catalyst dosage of 250 mg/L, PMS dosage of 4 mM, the temperature of 25 °C, and reaction time of 15 min. Anion experiments emphasized that the presence of nitrate, carbonate, and phosphate in the solution reduced the degradation efficiency by producing reactive species with low oxidation potential. The RB5 degradation rate evolved with temperature, and the activation energy was obtained to be 44.48 kJ/mol. The mechanism of PMS activation and production of free radicals was proposed based on tert-butyl alcohol (TBA), ethanol (EtOH), and potassium iodide (KI) scavengers. Trapping experiments showed that both sulfate (SO) and hydroxyl (OH) radicals are involved in the catalytic degradation of RB5. The effective treatment of real wastewater and tap water by the MWCNTs-CuNiFeO/PMS system requires a long reaction time. Gas chromatography-mass spectrometry (GC-MS) analysis indicated that RB5 can be degraded via methylation, decarboxylation, hydroxylation, and ring/chain cleavage pathways. The stable catalytic activity after three consecutive cycles suggested that MWCNTs-CuFeO is a novel reusability catalyst in PMS activation.

摘要

新型负载于多壁碳纳米管上的铜镍铁氧体纳米催化剂(MWCNTs-CuNiFeO)被合成并应用于激活过一硫酸盐(PMS)以降解活性黑 5(RB5)。通过扫描电子显微镜(SEM)、傅里叶变换红外光谱(FTIR)和 X 射线粉末衍射(XRD)对催化剂的结构进行了很好的表征。MWCNTs-CuNiFeO/PMS 体系在 RB5 的降解中表现出较高的性能,其动力学速率比均相和非均相体系高 1.5-2.5 倍。在初始 pH 值为 7、催化剂用量为 250mg/L、PMS 用量为 4mM、温度为 25°C、反应时间为 15min 的条件下,最大降解效率(99.60%)。阴离子实验强调,溶液中硝酸盐、碳酸盐和磷酸盐的存在会通过产生氧化电位较低的活性物质而降低降解效率。RB5 的降解速率随温度变化而变化,得到的活化能为 44.48kJ/mol。基于叔丁醇(TBA)、乙醇(EtOH)和碘化钾(KI)清除剂,提出了 PMS 活化和自由基生成的机制。捕获实验表明,硫酸盐(SO)和羟基(OH)自由基都参与了 RB5 的催化降解。MWCNTs-CuNiFeO/PMS 体系对实际废水和自来水的有效处理需要较长的反应时间。气相色谱-质谱联用(GC-MS)分析表明,RB5 可以通过甲基化、脱羧、羟化和环/链断裂途径降解。三次连续循环后的稳定催化活性表明 MWCNTs-CuFeO 是一种新型的 PMS 激活可重复使用催化剂。

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