换向脉冲电沉积法制备Ti/TNTs/Sb–SnO_2阳极及其性能研究
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摘要
以Ti阳极氧化所得TiO_2纳米管(TNTs)为基体,采用换向脉冲电沉积制备Sb掺杂SnO_2电极(Ti/TNTs/Sb–SnO_2)。采用X射线衍射、扫描电镜、能谱等手段对其微观结构、表面形貌及元素组成进行分析,研究了它作为阳极对对硝基苯酚(p-NP)的电催化氧化降解能力。结果表明,当负向脉冲电流为60 m A时,换向脉冲电沉积法制备的Ti/TNTs/Sb–SnO_2电极的表面覆盖层均匀,致密,无裂缝。阳极极化曲线的分析结果表明,该电极的析氧电位为2.28 V,用其降解对硝基苯酚2.5 h后,去除效率达81%。
TiO_2nanotubes(TNTs) were obtained by anodization of Ti, and then used as a substrate for preparing a Sb-doped SnO_2 electrode(Ti/TNTs/Sb–SnO_2) by reverse pulse electrodeposition. The microstructure, surface morphology and elemental composition of the electrode were analyzed by X-ray diffraction, scanning electron microscopy and energy-dispersive spectroscopy, respectively. The electrocatalytic oxidation property of the Ti/TNTs/Sb–SnO_2 electrode as anode for the degradation of p-nitrophenol(p-NP) was studied. The results showed that the Ti/TNTs/Sb–SnO_2 electrode prepared at a negative current of 60 mA features a uniform and compact surface without any cracks and has an oxygen evolution potential of ca.2.28 V. The degradation rate of p-NP at the Ti/TNTs/Sb–SnO_2 anode reached 81% after electrolysis for 2.5 h.
TiO_2nanotubes(TNTs) were obtained by anodization of Ti, and then used as a substrate for preparing a Sb-doped SnO_2 electrode(Ti/TNTs/Sb–SnO_2) by reverse pulse electrodeposition. The microstructure, surface morphology and elemental composition of the electrode were analyzed by X-ray diffraction, scanning electron microscopy and energy-dispersive spectroscopy, respectively. The electrocatalytic oxidation property of the Ti/TNTs/Sb–SnO_2 electrode as anode for the degradation of p-nitrophenol(p-NP) was studied. The results showed that the Ti/TNTs/Sb–SnO_2 electrode prepared at a negative current of 60 mA features a uniform and compact surface without any cracks and has an oxygen evolution potential of ca.2.28 V. The degradation rate of p-NP at the Ti/TNTs/Sb–SnO_2 anode reached 81% after electrolysis for 2.5 h.
引文
[1]WANG H,HUANG Y M.Prussian-blue-modified iron oxide magnetic nanoparticles as effective peroxidase-like catalysts to degrade methylene blue with H2O2[J].Journal of Hazardous Materials,2011,191(1/2/3):163-169.
[2]JI F,LI C L,ZHANG J H,et al.Heterogeneous photo-Fenton decolorization of methylene blue over Li Fe(WO4)2 catalyst[J].Journal of Hazardous Materials,2011,186(2/3):1979-1984.
[3]HUANG X F,ZHAO G H,LIU M C,et al.Highly sensitive electrochemical determination of 1-naphthol based on high-index facet Sn O2 modified electrode[J].Electrochimica Acta,2012,83:478-484.
[4]ANDREOZZI R,CAPRIO V,INSOLA A,et al.Advanced oxidation processes(AOP)for water purification and recovery[J].Catalysis Today,1999,53(1):51-59.
[5]PIMENTEL M,OTURAN N,DEZOTTI M,et al.Phenol degradation by advanced electrochemical oxidation process electro-Fenton using a carbon felt cathode[J].Applied Catalysis B:Environmental,2008,83(1/2):140-149.
[6]ZHANG L C,XU L,HE J,et al.Preparation of Ti/Sn O2–Sb electrodes modified by carbon nanotube for anodic oxidation of dye wastewater and combination with nanofiltration[J].Electrochimica Acta,2014,117:192-201.
[7]LI X Y,WU Y,ZHU W,et al.Enhanced electrochemical oxidation of synthetic dyeing wastewater using Sn O2–Sb-doped Ti O2-coated granular activated carbon electrodes with high hydroxyl radical yields[J].Electrochimica Acta,2016,220:276-284.
[8]WANG Q,JIN T,HU Z X,et al.Ti O2-NTs/Sn O2–Sb anode for efficient electrocatalytic degradation of organic pollutants:effect of Ti O2-NTs architecture[J].Separation and Purification Technology,2013,102:180-186.
[9]GUO Y,DUAN T G,CHEN Y,et al.Solvothermal fabrication of three-dimensionally sphere-stacking Sb–Sn O2 electrode based on Ti O2 nanotube arrays[J].Ceramics International,2015,41(7):8723-8729.
[10]WU T,ZHAO G H,LEI Y Z,et al.Distinctive tin dioxide anode fabricated by pulse electrodeposition:high oxygen evolution potential and efficient electrochemical degradation of fluorobenzene[J].The Journal of Physical Chemistry C,2011,115(10):3888-3898.
[11]ALIF A,BOULE P.Photochemistry and environment Part XIV.Phototransformation of nitrophenols induced by excitation of nitrite and nitrate ions[J].Journal of Photochemistry and Photobiology A:Chemistry,1991,59(3):357-367.
[12]TAKAHASHI N,NAKAI T,SATOH Y,et al.Variation of biodegradability of nitrogenous organic compounds by ozonation[J].Water Research,1994,28(7):1563-1570.
[13]WU Z C,CONG Y Q,ZHOU M H,et al.p-Nitrophenol abatement by the combination of electrocatalysis and activated carbon[J].Chemical Engineering Journal,2005,106(1):83-90.
[14]张茜,温玉娟,杨悦锁,等.土壤含水层处理系统去除对硝基酚[J].化工学报,2015,66(4):1440-1448.
[15]HAN W Q,ZHONG C Q,LIANG L Y,et al.Electrochemical degradation of triazole fungicides in aqueous solution using Ti O2-NTs/Sn O2–Sb/Pb O2 anode:experimental and DFT studies[J].Electrochimica Acta,2014,130:179-186.
[16]LIU S M,DING W Y,CHAI W P.Influence of Sb doping on crystal structure and electrical property of Sn O2 nanoparticles prepared by chemical coprecipitation[J].Physica B:Condensed Matter,2011,406(11):2303-2307.
[17]CHEN Y,NI Q,HAN W Q,et al.Electroless deposition of Sn Ox–Sb nanocoating in ordered titania pores for enhancing electrical conductivity[J].Scripta Materialia,2011,65(11):986-989.
[18]MONTILLA F,MORALLóN E,DE BATTISTI A,et al.Preparation and characterization of antimony-doped tin dioxide electrodes.Part 1.Electrochemical characterization[J].The Journal of Physical Chemistry B,2004,108(16):5036-5043.
[2]JI F,LI C L,ZHANG J H,et al.Heterogeneous photo-Fenton decolorization of methylene blue over Li Fe(WO4)2 catalyst[J].Journal of Hazardous Materials,2011,186(2/3):1979-1984.
[3]HUANG X F,ZHAO G H,LIU M C,et al.Highly sensitive electrochemical determination of 1-naphthol based on high-index facet Sn O2 modified electrode[J].Electrochimica Acta,2012,83:478-484.
[4]ANDREOZZI R,CAPRIO V,INSOLA A,et al.Advanced oxidation processes(AOP)for water purification and recovery[J].Catalysis Today,1999,53(1):51-59.
[5]PIMENTEL M,OTURAN N,DEZOTTI M,et al.Phenol degradation by advanced electrochemical oxidation process electro-Fenton using a carbon felt cathode[J].Applied Catalysis B:Environmental,2008,83(1/2):140-149.
[6]ZHANG L C,XU L,HE J,et al.Preparation of Ti/Sn O2–Sb electrodes modified by carbon nanotube for anodic oxidation of dye wastewater and combination with nanofiltration[J].Electrochimica Acta,2014,117:192-201.
[7]LI X Y,WU Y,ZHU W,et al.Enhanced electrochemical oxidation of synthetic dyeing wastewater using Sn O2–Sb-doped Ti O2-coated granular activated carbon electrodes with high hydroxyl radical yields[J].Electrochimica Acta,2016,220:276-284.
[8]WANG Q,JIN T,HU Z X,et al.Ti O2-NTs/Sn O2–Sb anode for efficient electrocatalytic degradation of organic pollutants:effect of Ti O2-NTs architecture[J].Separation and Purification Technology,2013,102:180-186.
[9]GUO Y,DUAN T G,CHEN Y,et al.Solvothermal fabrication of three-dimensionally sphere-stacking Sb–Sn O2 electrode based on Ti O2 nanotube arrays[J].Ceramics International,2015,41(7):8723-8729.
[10]WU T,ZHAO G H,LEI Y Z,et al.Distinctive tin dioxide anode fabricated by pulse electrodeposition:high oxygen evolution potential and efficient electrochemical degradation of fluorobenzene[J].The Journal of Physical Chemistry C,2011,115(10):3888-3898.
[11]ALIF A,BOULE P.Photochemistry and environment Part XIV.Phototransformation of nitrophenols induced by excitation of nitrite and nitrate ions[J].Journal of Photochemistry and Photobiology A:Chemistry,1991,59(3):357-367.
[12]TAKAHASHI N,NAKAI T,SATOH Y,et al.Variation of biodegradability of nitrogenous organic compounds by ozonation[J].Water Research,1994,28(7):1563-1570.
[13]WU Z C,CONG Y Q,ZHOU M H,et al.p-Nitrophenol abatement by the combination of electrocatalysis and activated carbon[J].Chemical Engineering Journal,2005,106(1):83-90.
[14]张茜,温玉娟,杨悦锁,等.土壤含水层处理系统去除对硝基酚[J].化工学报,2015,66(4):1440-1448.
[15]HAN W Q,ZHONG C Q,LIANG L Y,et al.Electrochemical degradation of triazole fungicides in aqueous solution using Ti O2-NTs/Sn O2–Sb/Pb O2 anode:experimental and DFT studies[J].Electrochimica Acta,2014,130:179-186.
[16]LIU S M,DING W Y,CHAI W P.Influence of Sb doping on crystal structure and electrical property of Sn O2 nanoparticles prepared by chemical coprecipitation[J].Physica B:Condensed Matter,2011,406(11):2303-2307.
[17]CHEN Y,NI Q,HAN W Q,et al.Electroless deposition of Sn Ox–Sb nanocoating in ordered titania pores for enhancing electrical conductivity[J].Scripta Materialia,2011,65(11):986-989.
[18]MONTILLA F,MORALLóN E,DE BATTISTI A,et al.Preparation and characterization of antimony-doped tin dioxide electrodes.Part 1.Electrochemical characterization[J].The Journal of Physical Chemistry B,2004,108(16):5036-5043.