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采用硼掺杂金刚石(BDD)电极通过阳极氧化法实现双酚A(BPA)的矿化。

Mineralization of bisphenol A (BPA) by anodic oxidation with boron-doped diamond (BDD) electrode.

作者信息

Murugananthan M, Yoshihara S, Rakuma T, Shirakashi T

机构信息

Satellite Venture Business Laboratory, Utsunomiya University, 7-1-2 Yoto, Utsunomiya, Tochigi 321-8585, Japan.

出版信息

J Hazard Mater. 2008 Jun 15;154(1-3):213-20. doi: 10.1016/j.jhazmat.2007.10.011. Epub 2007 Oct 10.

Abstract

Anodic oxidation of bisphenol A (BPA), a representative endocrine disrupting chemical, was carried out using boron-doped diamond (BDD) electrode at galvanostatic mode. The electro-oxidation behavior of BPA at BDD electrode was investigated by means of cyclic voltammetric technique. The extent of degradation and mineralization of BPA were monitored by HPLC and total organic carbon (TOC) value, respectively. The results obtained, indicate that the BPA removal at BDD depends on the applied current density (Iappl), initial concentration of BPA, pH of electrolyte and supporting medium. Galvanostatic electrolysis at BDD anode cause concomitant generation of hydroxyl radical that leads to the BPA destruction. The kinetics for the BPA degradation follows a pseudo-first order reaction with a higher rate constant 12.8x10(-5) s(-1) for higher Iappl value 35.7 mA cm(-2), indicating that the oxidation reaction is limited by Iappl control. Complete mineralization of BPA was achieved regardless of the variables and accordingly the mineralization current efficiency was calculated from the TOC removal measurements. Considering global oxidation process, the effect of supporting electrolytes has been discussed in terms of the electro generated inorganic oxidants. The better performance of BDD anode was proved on a comparative study with Pt and glassy carbon under similar experimental conditions. A possible reaction mechanism for BPA degradation involving three main aromatic intermediates, identified by GC-MS analysis, was proposed.

摘要

使用掺硼金刚石(BDD)电极在恒电流模式下对典型的内分泌干扰化学物质双酚A(BPA)进行阳极氧化。采用循环伏安技术研究了BPA在BDD电极上的电氧化行为。分别通过高效液相色谱(HPLC)和总有机碳(TOC)值监测BPA的降解程度和矿化程度。所得结果表明,BDD对BPA的去除取决于施加的电流密度(Iappl)、BPA的初始浓度、电解质的pH值和支持介质。BDD阳极的恒电流电解会伴随产生羟基自由基,从而导致BPA被破坏。BPA降解的动力学遵循准一级反应,对于较高的Iappl值35.7 mA cm(-2),速率常数更高,为12.8x10(-5) s(-1),这表明氧化反应受Iappl控制。无论变量如何,BPA都实现了完全矿化,因此根据TOC去除测量值计算了矿化电流效率。考虑到整体氧化过程,从电生成的无机氧化剂方面讨论了支持电解质的影响。在相似实验条件下与铂和玻碳进行的对比研究证明了BDD阳极具有更好的性能。提出了一种涉及通过气相色谱 - 质谱(GC - MS)分析鉴定的三种主要芳香族中间体的BPA降解可能反应机制。

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