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采用光发射二极管(LED)照明,在近中性 pH 值下,利用天然有机酸和尺寸稳定的阳极-气体扩散电极(DSA-GDE)系统对降压药氯沙坦和缬沙坦进行光电-Fenton 高级氧化。

Advanced oxidation of antihypertensives losartan and valsartan by photo-electro-Fenton at near-neutral pH using natural organic acids and a dimensional stable anode-gas diffusion electrode (DSA-GDE) system under light emission diode (LED) lighting.

机构信息

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

Grupo de Investigación Fundamental y Aplicada en Materiales, Facultad de Ciencias, Universidad Antonio Nariño, Bogotá, D.C., Colombia.

出版信息

Environ Sci Pollut Res Int. 2019 Feb;26(5):4426-4437. doi: 10.1007/s11356-018-2645-3. Epub 2018 Jul 4.

Abstract

In this work photo-electro-Fenton (PEF) processes using a dimensionally stable anode-gas diffusion electrode (DSA-GDE) system under light emission diodes (LED)-type radiation were used in the degradation of the angiotensin-II-receptor antagonists (ARA II), valsartan (VAL), and losartan (LOS), which are used in the treatment of hypertension diseases, and are considered among the emerging contaminants (ECs). Organic acids as citric, tartaric, and oxalic acids were used as complexing agents of iron ions in order to maintain the performance of the Fenton reaction at near-neutral pH value. The results show that at 3.42 mA/cm after 90 min of electro-Fenton (EF) treatment, degradation of 70% of VAL and 100% of LOS were observed. Total degradation of VAL and LOS was reached with a PEF process at the same time with mineralization of 30%. When citric and tartaric acids were used instead of oxalic acid, similar results were obtained, i.e., total degradation of both compounds, LOS and VAL, after 90 min of treatment. The degradation performance can be attributed to the increase of the initial dissolved iron in the system, facilitating the Fe/Fe turnover in the catalytic photo-Fenton reaction and consequently, hydroxyl radical (OH) production. In addition, the increased photo-activity of the complexes can be associated with their high capability to complex Fe and to promote ligand-to-metal charge transfer, which is of key importance to feed Fe to the Fenton process. The results show that the system evaluated was more efficient to eliminate sartan family compounds using LED lighting in comparison with traditional UV-A lamps used in this kind of work. Moreover, three transformation products of VAL degradation and two transformation products of LOS degradation were identified by high-resolution mass spectrometry (HRMS) using hybrid quadrupole-time-of-flight (QTOF) MS and, at the end of the PEF system, the several organic compounds accumulated and no mineralized were effectively treated in a subsequent aerobic biological system.

摘要

在这项工作中,使用发光二极管 (LED) 型辐射下的尺寸稳定阳极-气体扩散电极 (DSA-GDE) 系统的光电-Fenton (PEF) 工艺用于降解血管紧张素-II 受体拮抗剂 (ARA II)、缬沙坦 (VAL) 和氯沙坦 (LOS),这些药物用于治疗高血压疾病,被认为是新兴污染物 (ECs)。柠檬酸、酒石酸和草酸等有机酸被用作铁离子的络合剂,以在近中性 pH 值下维持芬顿反应的性能。结果表明,在 3.42 mA/cm 下进行 90 分钟的电芬顿 (EF) 处理后,观察到 VAL 的降解率为 70%,LOS 的降解率为 100%。在 PEF 过程中,同时达到 VAL 和 LOS 的完全降解和 30%的矿化度。当使用柠檬酸和酒石酸代替草酸时,也得到了类似的结果,即在 90 分钟的处理后,两种化合物(氯沙坦和缬沙坦)完全降解。降解性能可归因于系统中初始溶解铁的增加,促进了催化光芬顿反应中 Fe/Fe 的转化,从而产生羟基自由基 (OH)。此外,配合物的光活性增加可归因于它们络合 Fe 的高能力和促进配体到金属的电荷转移,这对于向芬顿工艺提供 Fe 至关重要。结果表明,与用于此类工作的传统 UV-A 灯相比,使用 LED 照明的评估系统更有效地消除沙坦类化合物。此外,通过使用混合四极杆-飞行时间 (QTOF) MS 的高分辨率质谱 (HRMS) 鉴定了 VAL 降解的三个转化产物和 LOS 降解的两个转化产物,并且在 PEF 系统结束时,有效地处理了随后在有氧生物系统中积累的多种有机化合物而没有矿化。

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