SnO_2-Sb/碳纳米管复合电极的制备及催化降解低浓度头孢他啶
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摘要
利用溶胶凝胶法制备了SnO_2-Sb掺杂碳纳米管复合材料,采用热压法将其固定在不锈钢网上制成平面二维电极,借助SEM、XRD对其形貌、微观结构及元素结构进行分析,通过循环伏安曲线(CV)、极化曲线(Tafel),线性伏安(LVS)对其电化学性质进行了表征.结果显示,锡锑金属均匀地负载到了碳纳米管上且具有良好的电催化活性和稳定性,金属的掺杂使得碳纳米管电极具有更高的析氧电位和更小的阻抗.使用荧光光谱法测试了羟基自由基的产生能力,通过循环5次降解实验验证了电极的稳定性.降解实验表明,SnO_2-Sb/碳纳米管电极对低浓度头孢他啶具有很高的降解效率,在2 mA·cm~(-2)的电流强度下,60 min内可以达到90%的去除率.最后,针对不同的电解质和电流强度对电催化降解效率的影响,也通过实验数据进行了分析.
SnO_2-Sb/MWCNTs composites were prepared through sol-gel method, and were hot-pressed onto stainless steel mesh to form a 2-D electrode. Scanning electron microscopy(SEM), X-ray diffraction(XRD) and electrochemical measurements were used to investigate the morphology, phase composition and electrochemical performance. It was demonstrated that SnSbO_x was successfully doped onto MWCNTs. Oxygen evolution potential, electrocatalytic activity and stability were substantially improved. Enhanced hydroxyl radical production capability was tested by fluorescence spectrometry method. Service life test was conducted with five cycles of electrochemical degradation of ceftazidime. The results demonstrated that SnO_2-Sb/MWCNTs electrode could reach a 90% removal rate after 60 min under a current density of 2 mA·cm~(-2).
SnO_2-Sb/MWCNTs composites were prepared through sol-gel method, and were hot-pressed onto stainless steel mesh to form a 2-D electrode. Scanning electron microscopy(SEM), X-ray diffraction(XRD) and electrochemical measurements were used to investigate the morphology, phase composition and electrochemical performance. It was demonstrated that SnSbO_x was successfully doped onto MWCNTs. Oxygen evolution potential, electrocatalytic activity and stability were substantially improved. Enhanced hydroxyl radical production capability was tested by fluorescence spectrometry method. Service life test was conducted with five cycles of electrochemical degradation of ceftazidime. The results demonstrated that SnO_2-Sb/MWCNTs electrode could reach a 90% removal rate after 60 min under a current density of 2 mA·cm~(-2).
引文
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[2] SEBASTINE I M,WAKEMAN R J.Consumption and environmental hazards of pharmaceutical substances in the UK [J].Process Safety & Environmental Protection,2003,81(4):229-235.
[3] FENG L,HULLEBUSCH E D V,RODRIGO M A,et al.Removal of residual anti-inflammatory and analgesic pharmaceuticals from aqueous systems by electrochemical advanced oxidation processes.A review [J].Chemical Engineering Journal,2013,228(1):944-964.
[4] WANG J,WANG S.Removal of pharmaceuticals and personal care products (PPCPs) from wastewater:A review.[J].Journal of Environmental Management,2016,182:620-640.
[5] MARTINEZHUITLE C A,RODRIGO M A,SIRES I,et al.Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants:A critical review.[J].Chemical Reviews,2015,115(24):13362-13407.
[6] SARKKA H,BHATNAGAR A,SILLANPAA M.Recent developments of electro-oxidation in water treatment—A review.[J].Journal of Electroanalytical Chemistry,2015,754(2):46-56.
[7] 朱连亮,王玉民,邵长林,等.长寿命Ti/TiO2/SbO2-SnO2/SnO2-Sb-CeO2制备及电催化废水性能[J].环境化学,2014,33(6):992-998.ZHU L L,WANG Y M,SHAO C L,et al.Fabrication of long-life Ti/TiO2/SbO2-SnO2/SnO2-Sb-CeO2 electrodes and application in electrochemical wastewater treatment [J].Environmental Chemistry,2014,33(6):992-998(in Chinese).
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[9] JAME S A,ZHOU Z.Electrochemical carbon nanotube filters for water and wastewater treatment [J].Nanotechnology Reviews,2016,5(1):41-50.
[10] LI F,JIANG X,ZHAO J,et al.Graphene oxide:A promising nanomaterial for energy and environmental applications [J].Nano Energy,2015,16:488-515.
[11] YI F,CHEN S,YUAN C.Effect of activated carbon fiber anode structure and electrolysis conditions on electrochemical degradation of dye wastewater [J].Journal of Hazardous Materials,2008,157(1):79-87.
[12] MOTOC S,MANEA F,POP A,et al.Electrochemical degradation of pharmaceutical effluents on carbon-based electrodes [J].Environmental Engineering & Management Journal,2012,11(11):627-634.
[13] DUAN T,WEN Q,YE C,et al.Enhancing electrocatalytic performance of Sb-doped SnO2,electrode by compositing nitrogen-doped graphene nanosheets [J].Journal of Hazardous Materials,2014,280:304-314.
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[15] LI Y,LI Y,XIE B,et al.Efficient mineralization of ciprofloxacin using a 3D CexZr1-xO2/RGO composite cathode [J].Environmental Science Nano,2016,4(2):425-436.
[16] HU X,YU Y,SUN Z.Preparation and characterization of cerium-doped multiwalled carbon nanotubes electrode for the electrochemical degradation of low-concentration ceftazidime in aqueous solutions [J].Electrochimica Acta,2016,199:80-91.
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[19] LIU Z,ZHU M,ZHAO L,et al.Aqueous tetracycline degradation by coal-based carbon electrocatalytic filtration membrane:Effect of nano antimony-doped tin dioxide coating [J].Chemical Engineering Journal,2016,314:59-68.
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