电化学先进方法减轻氟化抗抑郁药氟西汀（Prozac）及其反应副产物,Applied Catalysis B: Environment and Energy

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电化学先进方法减轻氟化抗抑郁药氟西汀（Prozac）及其反应副产物
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2016-10-20 06:53:46
Claudio Salazar, Carlota Ridruejo, Enric Brillas, Jorge Yáñez, Héctor D. Mansilla, Ignasi Sirés

在硫酸盐介质中，通过电生H ₂ O ₂（AO-H ₂ O ₂），电Fenton（EF）和光电Fenton（PEF）的阳极氧化，在pH 3.0的硫酸盐介质中，对氟化抗抑郁药氟西汀的降解进行了比较研究。）。实验在配备具有Pt，的RuO未分割的罐式反应器用100ml溶液中进行₂为基础的或硼掺杂的金刚石（BDD）阳极和用于连续H成空气扩散阴极₂ ö ₂生产。由于大量吸附的BDD（OH）产生，BDD阳极显示出更高的矿化速率，而BDD（OH）具有很大的氧化药物和中间体的反应性。由于Fenton反应大量增加了OH的生成，使用0.50mM Fe ²⁺的EF可以提高降解速率。由于UVA辐射具有额外的光解作用，使用PEF的降解速度甚至更快。最有效的方法是PEF和BDD阳极，在300分钟时达到94％的矿化度。氟西汀的衰变遵循伪一级动力学，其顺序更快：AO-H ₂ O ₂＆lt; EF＆lt; PEF。阐明了电流密度和药物浓度对矿化速率和氟西汀衰变的影响。GC-MS发现，羟基自由基可将氟西汀氧化成四种芳族副产物。另外，由于活性氯反应而鉴定出氯代芳族化合物，该活性氯是由BDD阳极处氯离子的氧化原位形成的。鉴定了四种短链线性羧酸，它们是草酸和甲酸，较丰富。在PEF中，氟西汀的氟原子以氟离子的形式完全释放，而所有情况下初始氮都转化为硝酸根离子。最后提出了通过电化学先进方法进行氟西汀矿化的反应途径。

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Abatement of the fluorinated antidepressant fluoxetine (Prozac) and its reaction by-products by electrochemical advanced methods

The degradation of the fluorinated antidepressant fluoxetine, as hydrochloride, was comparatively studied in sulfate medium at pH 3.0 by anodic oxidation with electrogenerated H₂O₂ (AO-H₂O₂), electro-Fenton (EF) and photoelectro-Fenton (PEF). Experiments were performed with 100mL solutions in an undivided tank reactor equipped with a Pt, RuO₂-based or boron-doped diamond (BDD) anode and an air-diffusion cathode for continuous H₂O₂ production. The BDD anode showed higher mineralization rate due to the great production of physisorbed BDD(OH), which has large reactivity to oxidize the drug and intermediates. The degradation rate was enhanced by EF with 0.50mM Fe²⁺ due to the additional production of OH in the bulk from Fenton’s reaction. The degradation was even faster using PEF owing to the additional photolytic action of UVA radiation. The most effective process was PEF with a BDD anode achieving 94% mineralization at 300min. The fluoxetine decay followed a pseudo-first-order kinetics, being quicker in the order:AO-H₂O₂ <EF<PEF. The effect of the current density and drug concentration on the mineralization rate and fluoxetine decay was clarified. Oxidation of fluoxetine by hydroxyl radicals yielded four aromatic by-products, as found by GC–MS. Additionally, a chloroaromatic compound was identified as a result of the reaction of active chlorine, which was formed in situ from the oxidation of chloride ion at the BDD anode. Four short-chain linear carboxylic acids, being oxalic and formic acid more abundant, were identified. In PEF, fluorine atoms of fluoxetine were completely released as fluoride ion, whereas the initial nitrogen was converted into nitrate ion in all cases. A reaction pathway for fluoxetine mineralization by the electrochemical advanced methods is finally proposed.

更新日期：2016-10-20

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