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Electrochemical oxidation of ceftazidime with graphite/CNT-Ce/PbO2-Ce anode: Parameter optimization, toxicity analysis and degradation pathway.
Environmental Pollution ( IF 8.9 ) Pub Date : 2020-03-30 , DOI: 10.1016/j.envpol.2020.114436
Pingzhou Duan 1 , Shiheng Gao 1 , Jiawei Lei 1 , Xiang Li 1 , Xiang Hu 1
Affiliation  

In this work, the electrochemical degradation of antibiotic ceftazidime has been studied using a novel rare earth metal Ce and carbon nanotubes codoped PbO2 electrode. A competitively high oxygen evolution potential (2.4 V) and enhanced catalytic surface area were obtained, evidence by LSV and CV electrochemical characterization. The G/CNT-Ce/PbO2-Ce electrode possessed a more compact structure and a smaller grain size than the other PbO2 and Ce-PbO2 electrodes, exhibiting a prolonged service lifetime, evidence by accelerated lifespan test and recycling degradation experiment. As electrolysis time reached 120 min, the removal efficiency of ceftazidime and TOC arrived at 100.0% and 54.2% respectively in 0.05 M Na2SO4 solution containing 50 mg⋅L-1 ceftazidime. The effect of applied current density, pH value, initial ceftazidime concentration and chloride contents on the degradation performance were systematically evaluated. The results demonstrated that electrochemical oxidation of ceftazidime over the G/CNT-Ce/PbO2-Ce electrode was highly effective, and the mineralization rate was greatly improved, compared with pristine PbO2 electrode. Considering the toxicity was increased after 30 min electrolysis, the intermediates were quantitatively investigated through HPLC-MS, GC-MS and IC technology. According to the identified products, a reaction mechanism has been proposed and pyridine and aminothiazole were detected with concentration from approximately 1 to 3 mg⋅L-1, which were regarded as toxic byproducts during electrooxidation. Further electrocatalyzing by ring cleavage reaction and complete mineralization to CO2, NO3- and NH4+ was proposed, which demonstrated the G/CNT-Ce/PbO2-Ce electrode exhibited high efficiency for ceftazidime removal in mild conditions.

中文翻译:

头孢他啶用石墨/ CNT-Ce / PbO2-Ce阳极的电化学氧化:参数优化,毒性分析和降解途径。

在这项工作中,已经使用新型稀土金属Ce和碳纳米管共掺杂的PbO2电极研究了抗生素头孢他啶的电化学降解。LSV和CV电化学表征证明,该产品具有极高的析氧潜力(2.4 V)和较高的催化表面积。与其他PbO2和Ce-PbO2电极相比,G / CNT-Ce / PbO2-Ce电极具有更紧凑的结构和更小的晶粒尺寸,具有更长的使用寿命,这是通过加速寿命试验和循环降解实验证明的。当电解时间达到120分钟时,在含有50 mg·L-1头孢他啶的0.05 M Na2SO4溶液中,头孢他啶和TOC的去除率分别达到100.0%和54.2%。施加的电流密度,pH值,系统评价了头孢他啶的初始浓度和氯化物含量对降解性能的影响。结果表明,与原始的PbO2电极相比,头孢他啶在G / CNT-Ce / PbO2-Ce电极上的电化学氧化非常有效,成矿速率大大提高。考虑到电解30分钟后毒性增加,通过HPLC-MS,GC-MS和IC技术对中间体进行了定量研究。根据鉴定出的产物,提出了一种反应机理,并检测到吡啶和氨基噻唑的浓度约为1至3 mg·L-1,它们被认为是电氧化过程中的有毒副产物。提出了通过环裂解反应进一步电催化并完全矿化为CO2,NO3-和NH4 +的方法,
更新日期:2020-04-20
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