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不同电化学高级氧化工艺对阿米替林抗抑郁药降解的研究。

Study of degradation of amitriptyline antidepressant by different electrochemical advanced oxidation processes.

机构信息

Laboratorio de Química Verde, Departamento de Química Analítica e Inorgánica, Facultad de Ciencias Químicas, Universidad de Concepción, Edmundo Larenas 129, Concepción, Chile.

Laboratorio de Procesos Químicos Aplicados, Departamento de Ingeniería Civil, Facultad de Ingeniería, Universidad Católica de La Santísima Concepción, Alonso de Ribera 2850, Concepción, Chile.

出版信息

Chemosphere. 2021 Jul;274:129683. doi: 10.1016/j.chemosphere.2021.129683. Epub 2021 Jan 19.

DOI:10.1016/j.chemosphere.2021.129683
PMID:33540303
Abstract

Amitriptyline (AMT) is the most widely used tricyclic antidepressant and is classified as a recalcitrant emergent contaminant because it has been detected in different sources of water. Its accumulation in water and soil represents a risk for different living creatures. To remove amitriptyline from wastewater, the Advanced Oxidation Processes (AOPs) stands up as an interesting option since generate highly oxidized species as hydroxyl radicals (OH) by environmentally friendly mechanism. In this work, the oxidation and mineralization of AMT solution have been comparatively studied by 3 Electrochemical AOPs (EAOPs) where the OH is produced by anodic oxidation of HO (AO-HO), or by electro-Fenton (EF) or photoelectro-Fenton (PEF). PEF process with a BDD anode showed the best performance for degradation and mineralization of this drug due to the synergistic action of highly reactive physiosorbed BDD (OH), homogeneous OH and UVA radiation. This process achieved total degradation of AMT at 50 min of electrolysis and 95% of mineralization after 360 min of treatment with 0.5 mmol L Fe at 100 mA cm. Six aromatic intermediates for the drug mineralization were identified in short time of electrolysis by GC-MS, including a chloroaromatic by-product formed from the attack of active chlorine. Short-chain carboxylic acids like succinic, malic, oxalic and formic acid were quantified by ion-exclusion HPLC. Furthermore, the formation of NO ions was monitored. Finally, the organic intermediates identified by chromatographic techniques were used to propose the reaction sequence for the total mineralization of AMT.

摘要

阿米替林(AMT)是最广泛使用的三环类抗抑郁药,被归类为难治性新兴污染物,因为它已在不同水源中被检测到。它在水和土壤中的积累对不同的生物都构成了风险。为了从废水中去除阿米替林,高级氧化工艺(AOPs)是一种很有前途的选择,因为它通过环保机制产生高氧化性物质如羟基自由基(OH)。在这项工作中,通过 3 种电化学 AOP(EAOPs)比较研究了 AMT 溶液的氧化和矿化,其中 OH 通过 HO 的阳极氧化(AO-HO)、电芬顿(EF)或光电芬顿(PEF)产生。PEF 工艺使用 BDD 阳极由于高反应性物理吸附 BDD(OH)、均相 OH 和 UVA 辐射的协同作用,对该药物的降解和矿化表现出最佳性能。该过程在 50 分钟的电解和 360 分钟的处理后实现了 AMT 的完全降解,在 100 mA·cm 时用 0.5 mmol·L Fe 处理后达到 95%的矿化率。通过 GC-MS 在短时间的电解中鉴定了 6 种用于药物矿化的芳香族中间体,包括由活性氯攻击形成的氯代芳烃副产物。通过离子排斥 HPLC 定量了短链羧酸,如琥珀酸、苹果酸、草酸和甲酸。此外,还监测了 NO 离子的形成。最后,通过色谱技术鉴定的有机中间体被用于提出 AMT 完全矿化的反应序列。

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