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多壁碳纳米管修饰玻碳电极阳极氧化法对水中萘普生的电化学降解

Electrochemical degradation of naproxen from water by anodic oxidation with multiwall carbon nanotubes glassy carbon electrode.

作者信息

Díaz Eva, Stożek Sonia, Patiño Yolanda, Ordóñez Salvador

机构信息

Department of Chemical and Environmental Engineering, University of Oviedo, Faculty of Chemistry, Julián Clavería s/n, 33006 Oviedo, Spain E-mail:

出版信息

Water Sci Technol. 2019 Feb;79(3):480-488. doi: 10.2166/wst.2019.070.

Abstract

Naproxen (NPX) degradation was investigated by anodic oxidation both at constant potential and by cyclic voltammetry, using this last technique for optimizing reaction conditions and catalyst properties. Three multiwall carbon nanotubes (MWCNTs)-promoted electrodes were used (MWCNT, MWCNT-COOH and MWCNT-NH) and a two steps oxidation process was observed in all the cases. At the optimized conditions (volume of MWCNT = 15 μL), the influence of the scan rate indicates the diffusion-adsorption control of the process. Likewise, the kinetic study of NPX degradation at fix potential, considering two different stirring speeds (250 and 500 rpm), indicates that degradation rate increases with the stirring speed. After 20 h, NPX is degraded even an 82.5%, whereas the mineralization reaches almost 70%, as it was obtained from total organic carbon analysis. The pH effect was also analysed, in the range 5-11, observing a positive effect at low pH. Concerning the surface chemistry of the electrode, MWCNT-NH, with the highest isoelectric point (4.70), is the most promising material due to the improved interactions with the reactant. From these observations, a pathway is proposed, which includes two steps of electrochemical oxidation followed by subsequent oxidation steps, until mineralization of the NPX, attributed mainly to active chlorine species and ·OH.

摘要

通过恒电位阳极氧化和循环伏安法研究了萘普生(NPX)的降解情况,采用后一种技术来优化反应条件和催化剂性能。使用了三种多壁碳纳米管(MWCNT)促进的电极(MWCNT、MWCNT-COOH和MWCNT-NH),并且在所有情况下均观察到两步氧化过程。在优化条件下(MWCNT体积 = 15 μL),扫描速率的影响表明该过程受扩散吸附控制。同样,在固定电位下对NPX降解的动力学研究,考虑两种不同的搅拌速度(250和500 rpm),表明降解速率随搅拌速度增加。20小时后,NPX降解率甚至达到82.5%,而矿化率几乎达到70%,这是通过总有机碳分析得到的结果。还分析了pH值在5 - 11范围内的影响,发现在低pH值时有积极作用。关于电极的表面化学性质,等电点最高(4.70)的MWCNT-NH是最有前景的材料,因为它与反应物的相互作用得到了改善。基于这些观察结果,提出了一条途径,包括两步电化学氧化,随后是后续的氧化步骤,直至NPX矿化,主要归因于活性氯物种和·OH。

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