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使用BDD阳极通过光电芬顿法处理水中的两种沙坦类抗高血压药物:降解动力学、理论分析、初级转化和基质效应。

Treatment of two sartan antihypertensives in water by photo-electro-Fenton using BDD anodes: Degradation kinetics, theoretical analyses, primary transformations and matrix effects.

作者信息

Martínez-Pachón Diana, Serna-Galvis Efraím A, Ibañez María, Hernández Félix, Ávila-Torres Yenny, Torres-Palma Ricardo A, Moncayo-Lasso Alejandro

机构信息

Grupo de Investigación en Ciencias Biológicas y Químicas, Facultad de Ciencias, Universidad Antonio Nariño (UAN), Bogotá D.C., Colombia.

Grupo de Investigación en Remediación Ambiental y Biocatálisis (GIRAB), Instituto de Química, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombia; Grupo de Investigaciones Biomédicas Uniremington, Facultad de Ciencias de La Salud, Corporación Universitaria Remington (Uniremington), Calle 51 No. 51-27, Medellín, Colombia.

出版信息

Chemosphere. 2021 May;270:129491. doi: 10.1016/j.chemosphere.2020.129491. Epub 2020 Dec 30.

Abstract

Degradation of two representative antihypertensives, losartan (LOS) and valsartan (VAL) in water by photo-electro-Fenton (PEF), using a BDD anode in presence of sulfate anion was evaluated. PEF showed a fast elimination of these pollutants (>95% at 30 and 60 min of treatment for LOS and VAL, respectively). The main elimination route was the attacks of radicals produced in the system, having pseudo-first-order rate constants of 0.154 and 0.054 min for LOS and VAL, correspondingly. Theoretical analyses of atomic charges were performed to rationalize the antihypertensives reactivity toward the electrogenerated degrading agents. Afterwards, the primary transformation products were assessed. The transformation products revealed that the degrading species attack the biphenyl-tetrazole, imidazole, and alcohol moieties on LOS. Meanwhile, carboxylic and amide groups, plus the central nucleus, were modified on VAL. These moieties corresponded well with the electron-rich sites indicated by the theoretical calculations. Also, the PEF process removed between 33 and 38% of total organic carbon after 5 h of electrolysis. Finally, it was considered LOS treatment in presence of oxalic acid (a typical organic waste of pharmaceutical industry), in addition to the pollutant degradation in effluents from municipal sewage treatment plants by PEF at pH ∼5. Oxalic acid accelerated LOS degradation. Meanwhile, in the effluent, the process led to 64% of LOS removal after 120 min of treatment, indicating the high potentiality of PEF to degrade antihypertensives in water containing organic and inorganic substances.

摘要

评估了在硫酸根阴离子存在下,使用BDD阳极通过光电芬顿(PEF)法对两种代表性抗高血压药物氯沙坦(LOS)和缬沙坦(VAL)在水中的降解情况。PEF法能快速去除这些污染物(LOS和VAL分别在处理30分钟和60分钟时去除率>95%)。主要的去除途径是系统中产生的自由基的攻击,LOS和VAL的伪一级反应速率常数分别为0.154 min⁻¹和0.054 min⁻¹。进行了原子电荷的理论分析,以解释抗高血压药物对电生成降解剂的反应活性。之后,对主要转化产物进行了评估。转化产物表明,降解物种攻击LOS上的联苯四唑、咪唑和醇部分。同时,VAL上的羧基和酰胺基以及中心核被修饰。这些部分与理论计算表明的富电子位点非常吻合。此外,电解5小时后,PEF过程去除了33%至38%的总有机碳。最后,除了通过PEF在pH约为5的条件下降解城市污水处理厂废水中的污染物外,还考虑了在草酸(制药行业典型的有机废物)存在下对LOS的处理。草酸加速了LOS的降解。同时,在废水中,处理120分钟后该过程导致LOS的去除率达到64%,表明PEF在降解含有有机和无机物质的水中的抗高血压药物方面具有很高的潜力。

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