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采用电化学氧化-过硫酸钠法在掺硼金刚石阳极上降解抗生素氨苄西林。

Degradation of antibiotic ampicillin on boron-doped diamond anode using the combined electrochemical oxidation - Sodium persulfate process.

机构信息

Department of Environmental Engineering, University of Western Macedonia, GR-50100, Kozani, Greece.

Department of Chemical Engineering, University of Patras, Caratheodory 1, University Campus, GR-26504, Patras, Greece.

出版信息

J Environ Manage. 2018 Oct 1;223:878-887. doi: 10.1016/j.jenvman.2018.06.099. Epub 2018 Jul 7.

DOI:10.1016/j.jenvman.2018.06.099
PMID:29990877
Abstract

In this work, the electrochemical oxidation of antibiotic ampicillin (AMP) on a boron-doped diamond anode in the presence of sodium persulfate (SPS) was investigated (EO/SPS process). Experiments were conducted at AMP concentrations between 0.8 and 3 mg/L, SPS concentrations between 100 and 500 mg/L, current densities between 5 and 110 mA/cm, in three water matrices (ultrapure water, bottled water and secondary treated wastewater), using 0.1 M NaSO as the supporting electrolyte. AMP degradation follows a pseudo-first order kinetic expression with the apparent rate constant increasing with (i) increasing SPS concentration (from 0.08 min to 0.36 min at 0 and 500 mg/L SPS, respectively, 1.1 mg/L AMP, 25 mA/cm), (ii) increasing current (from 0.08 min to 0.6 min at 5 and 110 mA/cm, respectively, 1.1 mg/L AMP, 250 mg/L SPS), and (iii) decreasing AMP concentration (from 0.16 min to 0.31 min at 3 and 0.8 mg/L, respectively, 250 mg/L SPS, 25 mA/cm). The presence of various anions (mainly bicarbonates) in bottled water did not impact AMP degradation. The observed kinetic constant decreased by 40% in the presence of 10 mg/L humic acid. On the other hand, process efficiency was enhanced almost 3.5 times in secondary effluent due to the electrogeneration of active chlorine species that promote indirect oxidation reactions in the bulk solution. The efficacy of the EO/SPS process was compared to and found to be considerably greater than a process where SPS was activated by simulated solar irradiation at an intensity of 7.3 × 10 E/(L.s) (SLR/SPS process). Coupling the two processes (EO/SLR/SPS) resulted in a cumulative, in terms of AMP degradation, effect. The combined process was tested for AMP degradation, mineralization and inhibition to Vibrio fischeri in wastewater; fast AMP removal was accompanied by low mineralization and incomplete toxicity removal.

摘要

在这项工作中,研究了在过硫酸钠(SPS)存在下,抗生素氨苄西林(AMP)在掺硼金刚石阳极上的电化学氧化(EO/SPS 工艺)。实验在 AMP 浓度为 0.8 至 3mg/L、SPS 浓度为 100 至 500mg/L、电流密度为 5 至 110mA/cm 的条件下进行,在三种水基质(超纯水、瓶装水和二级处理废水)中,使用 0.1M NaSO 作为支持电解质。AMP 的降解符合准一级动力学表达式,表观速率常数随(i)SPS 浓度的增加而增加(在 0 和 500mg/L SPS 时分别为 0.08 分钟至 0.36 分钟,1.1mg/L AMP,25mA/cm),(ii)电流的增加(在 5 和 110mA/cm 时分别为 0.08 分钟至 0.6 分钟,1.1mg/L AMP,250mg/L SPS),和(iii)AMP 浓度的降低(在 3 和 0.8mg/L 时分别为 0.16 分钟至 0.31 分钟,250mg/L SPS,25mA/cm)。瓶装水中存在各种阴离子(主要是碳酸氢盐)并不影响 AMP 的降解。在 10mg/L 腐殖酸存在下,观察到的动力学常数降低了 40%。另一方面,由于在 bulk 溶液中电生成活性氯物种,间接氧化反应得到增强,二级出水的处理效率提高了近 3.5 倍。EO/SPS 工艺的效果与通过模拟太阳辐射在 7.3×10E/(L.s)(SLR/SPS 工艺)强度下激活 SPS 的工艺进行了比较,发现前者的效果明显优于后者。将这两个过程(EO/SLR/SPS)结合起来,在 AMP 降解方面产生了累积效应。该组合工艺在废水处理中用于 AMP 降解、矿化和对发光弧菌的抑制测试;快速去除 AMP 的同时伴随着低矿化度和不完全的毒性去除。

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