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在掺硼金刚石阳极上降解四环素:初始 pH 值、施加电流强度和电解质的影响。

Degradation of tetracycline at a boron-doped diamond anode: influence of initial pH, applied current intensity and electrolyte.

机构信息

UMTP and Department of Chemistry, University of Beira Interior, 6200-001, Covilhã, Portugal.

出版信息

Environ Sci Pollut Res Int. 2014;21(14):8457-65. doi: 10.1007/s11356-014-2778-y. Epub 2014 Mar 26.

Abstract

The anodic oxidation of tetracycline was performed in an up-flow reactor, operating in batch mode with recirculation, using as anode a boron-doped diamond electrode. The influence on the degradation rate of solution initial pH (2 to 12), applied current intensity (25 to 300 A m(-2)) and type of electrolyte (sodium sulphate or sodium chloride) were investigated. For the assays run at equal current density, with sodium sulphate as electrolyte, the solution's initial pH of 2 presented the highest absorbance and chemical oxygen demand removals. Regarding the influence of current density, for equal charge passed, the organic load removal rate decreased with the increase in applied current. When sodium sulphate was used as an electrolyte, high-performance liquid chromatography (HPLC) results have shown an almost complete removal of tetracycline after a 2-h assay. HPLC results have also shown the presence of oxamic acid as one of the intermediates of tetracycline anodic oxidation. The complete removal of tetracycline was much faster in the presence of chloride ions that promoted the complete degradation of this antibiotic in 30 min. However, in the presence of chloride ions, the tetracycline mineralization is slower, as observed by the lower organic carbon removal rate when compared to that of the tetracycline degradation in the presence of sulphate.

摘要

在一个上流式反应器中进行四环素的阳极氧化,采用循环操作方式,以掺硼金刚石电极为阳极。考察了溶液初始 pH 值(2 至 12)、施加电流强度(25 至 300 A m(-2))和电解质类型(硫酸钠或氯化钠)对降解速率的影响。在相同电流密度下、以硫酸钠为电解质的条件下,溶液初始 pH 值为 2 时,吸光度和化学需氧量的去除率最高。就电流密度的影响而言,对于相同的电荷量,随着施加电流的增加,有机负荷去除率降低。当使用硫酸钠作为电解质时,高效液相色谱(HPLC)结果表明,在 2 小时的试验后,四环素几乎完全被去除。HPLC 结果还表明,在四环素阳极氧化的中间产物中存在氨基乙二酸。在氯离子存在的情况下,四环素的去除速度要快得多,氯离子促进了该抗生素在 30 分钟内完全降解。然而,在氯离子存在的情况下,四环素的矿化速度较慢,与硫酸盐存在时的四环素降解相比,有机碳的去除率较低。

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