Degradation of aqueous carbamazepine in ultrasonic/Fe0/H2O2 systems

Degradation of aqueous carbamazepine in ultrasonic/Fe0/H2O2 systems
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DOI:
10.1016/j.cej.2011.04.002
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发表时间:
2011-08-01
影响因子:
15.1
通讯作者:
Dermesropian, Peter
Dermesropian, Peter
中科院分区:
工程技术1区
文献类型:
--
作者:
Ghauch, Antoine;Baydoun, Habib;Dermesropian, Peter

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研究了改进芬顿法氧化卡马西平(CBZ)的适宜性。用CBZ (42 μ M)作为非卤化药物的探针。实验在室温(21 +/- 2℃)和不同ph值(3、5、7和9)下进行。在低频超声(40 kHz)作用下,H2O2 (12.5 ~ 100 mM)和Fe-0 (0.44 ~ 3.57 mM)添加剂对CBZ产生强大的氧化羟基自由基。结果表明,在中心点OH清除剂(MeOH)的存在下,CBZ没有氧化,证实了芬顿反应的性质。酸洗Fe-0饲喂使CBZ氧化降解率提高了85%。循环实验也证明了Fe-0能够保持其向介质中释放Fe2+的能力,以促进中心点OH的生成,从而降解CBZ(4次循环后>达到80%)。这归因于铁颗粒表面的开裂效应,从而阻止了被动氧化物的形成。该过程在含有不同物种(如Na+、Ca2+、Mg2+、Cl-、SO42-、HCO3-、NO3-等)的天然水中也很有效。中间氧化产物(副产物)采用液相色谱质谱法进行鉴定。然而,随着实验时间的延长,副产物消失。Fe-0/H2O2超声法是一种在温和条件下氧化脱除非卤化药物的有前途的技术。(C) 2011 Elsevier B.V.版权所有
This study investigated the suitability of carbamazepine (CBZ) oxidation by an improved Fenton's process. CBZ (42 mu M) is used as probe for non-halogenated pharmaceuticals. The experiments were performed at room temperature (21 +/- 2 degrees C) and different pHs (3, 5, 7 and 9). Powerful oxidative hydroxyl radicals for CBZ oxidation are produced by H2O2 (12.5-100 mM) and Fe-0 (0.44-3.57 mM) additives under low frequency ultrasonication (40 kHz). Results showed no CBZ oxidation in the presence of an center dot OH scavenger (MeOH), confirming the Fenton's nature of the process. Acid-washed Fe-0 feeding showed increased CBZ oxidative degradation up to 85%. Recycling experiments demonstrated also the ability of Fe-0 to maintain its capability of releasing Fe2+ into the media to promote center dot OH generation for CBZ degradation (>80% after 4 cycles). This was ascribed to the cracking effect on the surface of iron particles preventing thereby the formation of passive oxide. The process was also efficient in natural waters containing different species (e.g. Na+, Ca2+, Mg2+, Cl-, SO42-, HCO3-, NO3-, etc.). Intermediate oxidation products (by-products) were identified by LC/MS. However, by-products disappeared with longer experimental durations. The Fe-0/H2O2 ultrasonic process is a promising technique for oxidative removal of non-halogenated pharmaceuticals under mild conditions. (C) 2011 Elsevier B.V. All rights reserved.