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连续体系中电间接氧化和电氯化过程中多种含胺药物降解的比较。

Comparison of the degradation of multiple amine-containing pharmaceuticals during electroindirect oxidation and electrochlorination processes in continuous system.

机构信息

Graduate Institute of Environmental Engineering, National Taiwan University, 71, Chou-Shan Rd., Taipei 10673, Taiwan.

School of Public Health, Taipei Medical University, 250, Wu-Xing Street, Taipei 11031, Taiwan.

出版信息

Water Res. 2021 Sep 15;203:117517. doi: 10.1016/j.watres.2021.117517. Epub 2021 Aug 6.

Abstract

The degradation of pharmaceuticals by electrochemical oxidation (EO) in simulated wastewater containing multiple pharmaceuticals was compared between batch and continuous reactors. Despite the excellent efficiencies achieved in batch experiments, the practical/large-scale applications of EO-degrading amine-containing pharmaceuticals has not yet been accomplished. This paper presents the results of continuous experiments with one of the most promising electrochemical configurations of Pt/Ti electrodes before proceeding to application. In the continuous electrooxidation system (without chloride), direct oxidation on the electrode surface and oxidation by hydroxyl radicals were the main pathways. Due to their short lifespans, the radicals could not be transferred to the bulk solution, and the removal of pharmaceuticals followed the order of sulfamethoxazole (SMX) > paracetamol (PAR) > diclofenac (DIC). In the electrochlorination system (with chloride), oxidation by residual chlorine was the main pathway. The removal of pharmaceuticals followed the order of sulfamethoxazole (SMX) > diclofenac (DIC) > paracetamol (PAR). High SMX removal was realized because of the high reaction rate of SMX with free chlorine. Among the pharmaceuticals, PAR had the lowest removal because it is a neutral species with a low mass transfer rate without the attraction of electrostatic force. These results are consistent with the predictions from our previous batch-scale study, which showed that the reaction rate of dissociated compounds could be increased by the addition of electrostatic force. Furthermore, multiple coexisting pharmaceuticals, such as SMX and PAR or DIC, may form dimers that can be transferred to complex structures and cause higher toxicity.

摘要

在含有多种药物的模拟废水中,电化学氧化(EO)对药物的降解在批式和连续式反应器中进行了比较。尽管在批式实验中取得了优异的效率,但含胺的药物的 EO 降解的实际/大规模应用尚未实现。本文介绍了在进行应用之前,使用最有前途的 Pt/Ti 电极电化学配置之一进行连续实验的结果。在连续电氧化系统(无氯)中,电极表面的直接氧化和羟基自由基氧化是主要途径。由于自由基的寿命短,无法转移到主体溶液中,药物的去除顺序为磺胺甲噁唑(SMX)>对乙酰氨基酚(PAR)>双氯芬酸(DIC)。在电氯化系统(有氯)中,残留氯的氧化是主要途径。药物的去除顺序为磺胺甲噁唑(SMX)>双氯芬酸(DIC)>对乙酰氨基酚(PAR)。由于 SMX 与游离氯的高反应速率,实现了高 SMX 去除率。在这些药物中,PAR 的去除率最低,因为它是一种中性物质,传质速率低,没有静电力的吸引。这些结果与我们之前的批处理研究的预测一致,该研究表明,加入静电力可以提高离解化合物的反应速率。此外,多种共存药物(如 SMX 和 PAR 或 DIC)可能形成二聚体,可转移到复杂结构并导致更高的毒性。

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