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祝贺庞迪、刘悦等同学合作文章在Chemical Engineering Journal期刊发表

已有 1552 次阅读 2020-9-5 17:04 |个人分类:点滴成果|系统分类:论文交流

Trace Ti3+- and N-codoped TiO2 nanotube array anode for significantly enhanced electrocatalytic degradation of tetracycline and metronidazole

 

Di Pang a, 1, Yue Liu a, 1, Haiou Song b, d *, Duozhe Chen a, Weiqing Zhu a, Rumeng Liu a, Hu Yang c, Aimin Li c, d*, Shupeng Zhang a, d*

A trace Ti3+- and N-codoped TiO2 nanotube array (TiON) anode is fabricated by electrochemical reduction after introducing nitrogen into the TiON. The TiON anode material is characterized by scanning electron microscopy, X-ray diffraction, Raman spectra and X-ray photoelectron spectroscopy. Electrochemical analyses of TiON, including cyclic voltammetry, electrochemical impedance spectroscopy and linear scan voltammetry, are conducted to confirm that the electrochemical performance could be significantly improved by electrochemical reduction and N doping. The achieved TiON anode is applied to the electrocatalytic oxidation of tetracycline (TC) and metronidazole (MNZ). The effect of applied current density, initial solution pH and initial TC/MNZ concentration on the reaction kinetics is systematically evaluated to obtain the optimal conditions. The degradation processes follow an apparent first-order kinetic model in all conditions. After 240 min of reaction time, the TC removal efficiency, chemical oxygen demand (COD) removal rate and total organic carbon (TOC) removal rate are >99%, 92.86% and 74.98%, respectively. The MNZ removal efficiency, COD and TOC removal rate achieved are >99%, 93.03% and 79.30%, respectively, after 240 min of degradation. The excellent removal efficiency of TC and MNZ indicates that this TiON anode is a promising material in the practical application of removing antibiotics from water.

This study has successfully fabricated a TiON anode achieved by electrochemical reduction after introducing trace N and Ti3+ into TiO2 nanotube arrays and applied it to the degradation of antibiotics. The results of CV and EIS confirmed that the conductivity was remarkable improved by electrochemical reduction. LSV revealed that the introduction of trace nitrogen is conducive to the increase of OEP (2.86 V vs. SCE). We chose two kind of antibiotics, TC and MNZ, to study the degradation performance of our TiON anode. The processes of degradation followed an apparent first-order kinetic model. The influences of applied current density, pH value and initial concentration on the degradation processes were evaluated systematically. Applied current density had a positive correlation with degradation efficiency. Acidic conditions are good for antibiotic degradation; this is due to the reduction of oxygen evolution side reactions under acidic conditions. Increased initial concentration in a certain range is conducive to the removal of antibiotics, but when the concentration is too high, more reactive intermediates will participate in the competition of active sites, as a result, the removal efficiency will decrease and energy consumption will increase. For TC, the removal efficiency, COD removal rate and TOC removal rate are 100%, 92.86%, 74.98%, respectively. For MNZ, they are 100%, 93.3% and 79.30%, respectively. The high electrocatalytic activity of TiON make it a promising electrode for effective electrochemical degradation of antibiotics from wastewater in practical applications.

Abstract.bmp




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