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铁线圈阳极施加方波交流电高效电化学生成高铁酸盐(VI)及其处理抗生素。

Efficient electrochemical generation of ferrate(VI) by iron coil anode imposed with square alternating current and treatment of antibiotics.

机构信息

College of Environment, Zhejiang University of Technology, Hangzhou 310014, China.

College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China.

出版信息

J Hazard Mater. 2020 Feb 15;384:121458. doi: 10.1016/j.jhazmat.2019.121458. Epub 2019 Oct 18.

Abstract

Anode passivation is still a main challenge for the electrochemical generation of ferrate(VI, Fe(VI)), leading to the reduction of Fe(VI) production efficiency. In this study, cyclic voltammetry, scanning electronic microscopy, and electrochemical impedance spectroscopy were used to select better anode electrode configurations (iron wire, iron gauze, and iron coil). The results indicate that iron coil had the least degree of passivation. Different imposed current waveforms during the electrochemical generation of Fe(VI) were also investigated, and the iron coil imposed with square alternating current (AC) wave can mitigate the anode passivation, resulting in higher Fe(VI) production efficiency. The optimum conditions for the electrochemical generation of Fe(VI) were evaluated and the optimum temperature (40 ℃), current density (10 mA/cm), AC cycle period (15 s) and electrolyte concentrations (14 M NaOH) were identified. As a result, 0.12 mol/L Fe(VI) concentration and over 50% of current efficiency can be achieved after 3 h electrolysis. The generated Fe(VI) solution was further applied to oxidize doxycycline(DOX) and sulfadiazine(SDZ) as typical antibiotics. Over 80% of DOX can be removed at a Fe(VI) to DOX molar ratio of 5:1 (pH = 4-9), whilst a higher Fe(VI) to SDZ molar ratio of 20:1 (pH = 7) was needed to obtain 75% SDZ removal.

摘要

阳极钝化仍然是电化学生成高铁酸盐(VI,Fe(VI))的主要挑战,导致 Fe(VI)生产效率降低。在这项研究中,使用循环伏安法、扫描电子显微镜和电化学阻抗谱来选择更好的阳极电极结构(铁丝、铁网和铁线圈)。结果表明,铁线圈的钝化程度最低。还研究了电化学生成 Fe(VI)过程中不同的外加电流波形,施加方波交流电(AC)的铁线圈可以减轻阳极钝化,从而提高 Fe(VI)的生产效率。评估了电化学生成 Fe(VI)的最佳条件,确定了最佳温度(40℃)、电流密度(10mA/cm)、AC 循环周期(15s)和电解质浓度(14M NaOH)。结果,经过 3 小时电解后,可以达到 0.12mol/L 的 Fe(VI)浓度和超过 50%的电流效率。生成的 Fe(VI)溶液进一步用于氧化典型抗生素强力霉素(DOX)和磺胺嘧啶(SDZ)。在 Fe(VI)与 DOX 的摩尔比为 5:1(pH=4-9)时,超过 80%的 DOX 可以被去除,而当 Fe(VI)与 SDZ 的摩尔比为 20:1(pH=7)时,需要 75%的 SDZ 去除。

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