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采用多壁碳纳米管的三维电极反应器电化学降解双氯芬酸。

Electrochemical degradation of diclofenac using three-dimensional electrode reactor with multi-walled carbon nanotubes.

机构信息

Department of Environmental Health Engineering, School of Health, Environment Research Center, Isfahan University of Medical Sciences, Isfahan, Iran.

出版信息

Environ Sci Pollut Res Int. 2018 Sep;25(25):24746-24763. doi: 10.1007/s11356-018-2527-8. Epub 2018 Jun 20.

Abstract

The electro-oxidation treatment of aqueous solution containing diclofenac (DCF) on a Ti/RuO-TiO electrode in the presence of multi-walled carbon nanotubes (MWCNTs) was studied in a three-dimensional electrochemical (3DE) reactor. The response surface methodology (RSM) based on central composite design (CCD) was utilized to determine the influence of different factors. The results revealed that the obtained polynomial experimental model had a high coefficient of determination (R = 0.9762) based on analysis of variance. The optimum condition for the removal of DCF by the 3DE process was obtained with the initial pH of 3.8, the initial DCF concentration of 4 mg/L, the current density of 20 mA/cm, the particle electrode concentration of 70 mg/L, and the electrolysis time of 85 min. The quadratic model developed for DCF removal and subsequently the analysis of the F value illustrated that the initial pH was the most important factor in the removal of DCF. The comparative experiments between electrochemical processes showed the high electrocatalytic activity and removal efficiency of the 3DE reactor with the MWCNT particle electrode. The results also showed that the Ti/RuO-TiO electrode, in addition to its high stability, had a very good electrocatalytic activity in the 3D reactor. The stability and reusability test proved that MWCNTs, as a particle electrode, had a potential to improve the long-term electrocatalytic degradation of DCF in the aqueous solutions. Based on the identified intermediate compounds along with the results of other studies, a possible pathway for the electrochemical oxidation of DCF by the 3DE process catalyzed with MWCNTs was proposed.

摘要

在多壁碳纳米管 (MWCNTs) 的存在下,采用 Ti/RuO-TiO 电极在三维电化学 (3DE) 反应器中处理含有双氯芬酸 (DCF) 的水溶液的电氧化处理。利用基于中心复合设计 (CCD) 的响应面法 (RSM) 来确定不同因素的影响。结果表明,根据方差分析,所得多项式实验模型具有高的确定系数 (R=0.9762)。通过 3DE 工艺去除 DCF 的最佳条件为初始 pH 值为 3.8、初始 DCF 浓度为 4mg/L、电流密度为 20mA/cm、颗粒电极浓度为 70mg/L 和电解时间为 85min。为去除 DCF 而开发的二次模型以及随后的 F 值分析表明,初始 pH 值是去除 DCF 的最重要因素。电化学过程之间的比较实验表明,具有 MWCNT 颗粒电极的 3DE 反应器具有高的电催化活性和去除效率。结果还表明,Ti/RuO-TiO 电极除了具有高稳定性外,在 3D 反应器中还具有非常好的电催化活性。稳定性和可重复使用性测试证明,MWCNTs 作为颗粒电极,具有提高水中 DCF 的长期电催化降解的潜力。根据鉴定的中间化合物以及其他研究的结果,提出了一种可能的通过 3DE 过程催化 MWCNTs 电化学氧化 DCF 的途径。

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