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Catalytic degradation of diclofenac from aqueous solutions using peroxymonosulfate activated by magnetic MWCNTs-CoFe3O4 nanoparticles

机译:磁性MWCNTs-CoFe3O4纳米粒子活化过氧化一硫酸盐从水溶液中催化降解双氯芬酸

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CoFe _(3) O _(4) nanoparticles supported on multi-walled carbon nanotubes (MWCNTs-CoFe _(3) O _(4) ) were synthesized by the co-precipitation method as a novel catalyst for degradation of diclofenac (DCF). The comparative experiments indicated that MWCNTs-CoFe _(3) O _(4) has a better catalytic activity in degradation of DCF and activation of peroxymonosulfate (PMS) compared to other catalytic systems. This can be attributed to the interaction of MWCNTs with CoFe _(3) O _(4) in accelerating the absorption process and activating the PMS ( E _(a) = 22.93 kJ mol ~(?1) ). The removal efficiencies of DCF and total organic carbon (TOC) were 99.04% and 50.11%, under optimum conditions, e.g. , pH of 7, PMS dosage of 4 mM, DCF concentration of 30 mg L ~(?1) , catalyst dosage of 500 mg L ~(?1) , and reaction time of 120 min. The oxidation of DCF was fitted by the pseudo-first-order kinetic model and the constant rate was increased by increasing the pH, temperature, dosage of PMS and catalyst. The production of reactive species was studied using scavengers such as TBA and ethanol and the results showed that sulfate radical is the reactive species responsible for the degradation of DCF. The MWCNTs-CoFe _(3) O _(4) catalyst showed high stability and reusability based on five successful repeated reactions, X-ray diffraction and energy dispersive X-ray spectroscopy analysis. Based on the intermediates detected by gas chromatography-mass spectrometry (GC-MS), the possible pathways for DCF catalytic oxidation were proposed. The results explained that the PMS/MWCNTs-CoFe _(3) O _(4) system is a promising method for treating DCF solution due to high efficiency, good reusability of catalyst and greater PMS activation.
机译:通过共沉淀法合成了负载在多壁碳纳米管上的CoFe _(3)O _(4)纳米颗粒(MWCNTs-CoFe _(3)O _(4))作为降解双氯芬酸的新型催化剂(DCF )。对比实验表明,与其他催化体系相比,MWCNTs-CoFe_(3)O_(4)在DCF降解和过氧单硫酸盐(PMS)活化方面具有更好的催化活性。这可以归因于MWCNT与CoFe _(3)O _(4)在加速吸收过程和激活PMS中的相互作用(E _(a)= 22.93 kJ mol〜(?1))。在最佳条件下,例如DCF和DCF的去除效率分别为99.04%和50.11%。 ,pH值为7,PMS剂量为4 mM,DCF浓度为30 mg L〜(?1),催化剂剂量为500 mg L〜(?1),反应时间为120分钟。用拟一级动力学模型拟合DCF的氧化,并通过增加pH值,温度,PMS的用量和催化剂来增加恒定速率。用TBA和乙醇等清除剂研究了反应性物质的产生,结果表明硫酸根是导致DCF降解的反应性物质。基于五个成功的重复反应,X射线衍射和能量色散X射线光谱分析,MWCNTs-CoFe _(3)O _(4)催化剂显示出高稳定性和可重复使用性。基于气相色谱-质谱法(GC-MS)检测到的中间体,提出了DCF催化氧化的可能途径。结果表明,PMS / MWCNTs-CoFe _(3)O _(4)系统具有很高的效率,良好的催化剂可重复使用性和更大的PMS活化能力,是一种处理DCF溶液的有前途的方法。

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