β-PbO2/Sb-SnO2/Ti电极的苯酚电催化性能研究

doi:10.13208/j.electrochem.131021

电化学（中英文） ›› 2014, Vol. 20 ›› Issue (5): 493-498. doi: 10.13208/j.electrochem.131021

β-PbO₂/Sb-SnO₂/Ti电极的苯酚电催化性能研究

李鹏¹，赵跃民²，王立章^1*，张延乐³，芦兆青¹

1. 中国矿业大学环境与测绘学院环境工程专业，江苏徐州 221116；2. 中国矿业大学化学化工学院矿物加工专业，江苏徐州 221116；3. 徐州市工程咨询中心，江苏徐州 221116

收稿日期:2013-10-21 修回日期:2013-12-05 出版日期:2014-10-28 发布日期:2013-12-10
通讯作者: 王立章 E-mail:wlzh0731@126.com
基金资助:
国家自然科学基金项目（No. 50908226）、国家自然科学基金创新研究群体项目(No. 51221462)、江苏省自然科学基金基础研究计划资助项目（No. BK201124）和江苏省研究生培养创新工程（No. CXLX13-956）资助

Electro-Catalytic Properties of β-PbO₂/Sb-SnO₂/Ti Electrode on Phenol Oxidation

LI Peng¹; ZHAO Yue-min², WANG Li-zhang^1*, ZHANG Yan-le³, LU Zhao-qing¹

1. School of Environment and Spatial Informatics, China University of Mining and Technology, Xuzhou 22116, Jiangsu, China; 2. School of Chemical Engineering and Technology, China University of Mining and Technology, Xuzhou 22116, Jiangsu, China; 3. Xuzhou engineering consulting center, Xuzhou 22116, Jiangsu, China

Received:2013-10-21 Revised:2013-12-05 Published:2014-10-28 Online:2013-12-10
Contact: WANG Li-zhang E-mail:wlzh0731@126.com

摘要/Abstract

摘要： 采用刷涂热解和电镀制得了β-PbO₂/Sb-SnO₂/Ti电极. 采用X射线衍射（X-ray Diffraction，XRD）和扫描电镜（Scanning Electron Microscope，SEM）进行分析与观察，Sb-SnO₂中间层抑制PbF₂的生成，NaF促进二氧化铅晶粒的成型与分散，消除了β-PbO₂聚团. 据谢乐公式（Scherrer）计算晶粒尺寸为25.2 nm，电极表面结晶度高达100%. 极化测试显示，β-PbO₂/Sb-SnO₂/Ti电极扩散段电位区、析氧电位和Tafel斜率分别为1.85 ~ 2.15 V、2.08 V和0.84，优于β-PbO₂/Ti电极的1.40 ~ 1.80 V、1.75 V和0.36. 使用β-PbO₂/Sb-SnO₂/Ti、β-PbO₂/Ti电极在9 mA·cm^-2电流密度对苯酚模拟废水处理240 min，前者COD（Chemical Oxygen Demand）去除率、电流效率（Instant Current Efficiency）高达90.1%和63.28%，优于后者66.9%和44.96%. 寿命测试表明，β-PbO₂/Sb-SnO₂/Ti电极与β-PbO₂/Ti电极相比延长10倍，工业寿命可达8.6a，有较高的工程应用价值.

关键词: Sb-SnO₂中间层；&beta, -PbO₂/Ti；极化特性；电流效率；加速寿命测试

Abstract: The combination technology of brush pyrolysis and electroplating was employed in the preparation of β-PbO₂/Sb-SnO₂/Ti electrode. X-ray Diffraction (XRD) and Scanning Electron Microscope (SEM) results showed that the Sb-SnO₂ as an interlayer would restrain the formation of lead fluoride and the crystallization degree on the electrode surface could be as high as 100%. The grain size was calculated by Scherrer formula to be 25.2 nm and the agglomeration of lead dioxide was effectively eliminated. The potential span of diffusion control phase, oxygen evolution potential, Tafel slope for the β-PbO₂/Sb-SnO₂/Ti electrode during the polarization were 1.85 ~ 2.15 V, 2.08 V and 0.84, respectively, which exhibited much better electrochemical properties as compared with those of the β-PbO₂/Ti electrode with the values of 1.40 ~ 1.80 V, 1.75 V and 0.36, respectively. Furthermore, the β-PbO₂/Sb-SnO₂/Ti and β-PbO₂/Ti electrodes were taken as anodes participating in the electrocatalysis degradation of phenol simulated wastewater under current density 9 mA·cm^-2 within 240 min. Experimental results revealed that the efficiencies of chemical oxygen demand (COD) removal and instant current efficiency (ICE) during phenol degradation were 90.1% and 63.28% for the β-PbO₂/Sb-SnO₂/Ti electrode, while 66.9% and 44.96% for the β-PbO₂/Ti electrode. Ultimately, the accelerated life test was performed to evaluate the service time of β-PbO₂/Sb-SnO₂/Ti. The results presented that the industrial life of β-PbO₂/Sb-SnO₂/Ti was 8.6a, which is 10 times longer than that of β-PbO₂/Ti,suggesting that β-PbO₂/Sb-SnO₂/Ti would have a relatively high engineering application value.

Key words: stannic and antimony oxides interlayer, β-PbO₂/Ti, polarization curve, instant current efficiency, accelerated life test

中图分类号:

TQ050.4
X703

李鹏，赵跃民，王立章*，张延乐，芦兆青. β-PbO₂/Sb-SnO₂/Ti电极的苯酚电催化性能研究[J]. 电化学（中英文）, 2014, 20(5): 493-498.

LI Peng; ZHAO Yue-min, WANG Li-zhang*, ZHANG Yan-le, LU Zhao-qing. Electro-Catalytic Properties of β-PbO₂/Sb-SnO₂/Ti Electrode on Phenol Oxidation[J]. Journal of Electrochemistry, 2014, 20(5): 493-498.

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https://electrochem.xmu.edu.cn/CN/Y2014/V20/I5/493

参考文献

[1] Lin H, Niu J F, Ding S Y, et al. Electrochemical degradation of perfluorooctanoic acid (PFOA) by Ti/SnO2-Sb, Ti/SnO2-Sb/PbO2 and Ti/SnO2-Sb/MnO2[J]. Water Research, 2012, 46(7): 2281-2289.
[2] Devillers D, Mahé E. Modified titanium electrodes: Application to Ti/TiO2/PbO2 dimensionally stable anodes[J]. Electrochimica Acta, 2010, 55(27): 8207-8214.
[3] Lopez M. C, Vong Y. M, Rojas M A M, et al. Formation and growth of PbO2 inside TiO2 nanotubes for environmental applications[J]. Applied Catalysis B: Environmental, 2014, 144: 174-181.
[4] Li G T, Qu J H, Zhang X W, et al. Electrochemically assisted photocatalytic degradation of Acid Orange 7 with β-PbO2 electrodes modified by TiO2[J]. Water research, 2006, 40(2): 213-220.
[5] García J. G, Iniesta J, Expósito E, et al. Early stages of lead dioxide electrodeposition on rough titanium[J]. Thin Solid Films, 1999, 352(1/2): 49-56.
[6] Ueda M, Watanabe A, Kameyama T. Performance characteristics of a new type of lead dioxide-coated titanium anode[J]. Journal of Applied Electrochemistry, 1995, 25(9): 817-822.
[7] Meissner E. How to understand the reversible capacity decay of the lead dioxide electrode[J]. Journal of Power Sources, 1999, 78(1/2): 99-114.
[8] Wang Y Q(王雅琼), Tong H Y(童宏扬), Xu W L(许文林). Structure change and failure behavior of Ti/SnO2+Sb2O3/PbO2 anodes during electrolysis process in H2SO4 solution[J]. Journal of Chemical Industry and Engineering(化工学报), 2004, 55(9): 1560-1563.
[9] Devilliers D, Baudin T, Dinh M T, et al. Selective electrodeposition of PbO2 on anodised-polycrystalline titanium[J]. Electrochimica Acta, 2004, 49(14): 2369-2377.
[10] Yeo I H, Kim S, Jacobson R, et al. Electrocatalysis of anodic oxygen transfer reaction: comparison of structural date with electrocatalytic phenomena for bismuth-doped lead dioxide[J]. Journal of Electrochemical Society, 1989, 136(5): 1395-1401.
[11] Li H Y, Chen Y, Zhang Y H, et al. Preparation of Ti/PbO2-Sn anodes for electrochemical degradation of phenol[J]. Journal of Electroanalytical Chemistry, 2013, 689: 193-200.
[12] Yang X P, Zou R Y, Huo F, et al. Preparation and characterization of Ti/SnO2-Sb2O3-Nb2O5/PbO2 thin film as electrode material for the degradation of phenol[J]. Journal of Hazardous Materials, 2009, 164(1): 367-373.
[13] Yang W H(杨卫华), Wang H H(王鸿辉), Fu F(付芳). Preparation and performance of Ti/Sb-SnO2/β-PbO2 electrode modified with rare earth[J]. Rare Metal Materials and Engineering(稀有金属材料与工程), 2010, 39(7): 1215-1218.
[14] Liang Z H(梁镇海), Bian S T(边书田), Ren S C(任所才), et al. Properties of Ti/PbO2 anode in sulfuric acid[J]. Rare Metal Materials and Engineering(稀有金属材料与工程), 2001, 30(3): 232-234.
[15] Duan X Y, Ma F, Yuan Z X, et al. Electrochemical degradation of phenol in aqueous solution using PbO2 anode[J]. Journal of the Taiwan Institute of Chemical Engineers, 2013, 44(1): 95-102.
[16] Vicent F, Morallón E, Quijada C, et al. Characterization and stability of doped SnO2 anodes[J]. Journal of Applied Electrochemistry, 1988, 28(6): 607-612.
[17] An H, Li Q, Tao D J, et al. The synthesis and characterization of Ti/SnO2-Sb2O3/PbO2 electrodes: The influence of morphology caused by different electrochemical deposition time[J]. Applied Surface Science, 2011, 258(1): 218-224.
[18] Feng Y J(冯玉杰), Shen H(沈宏), Cui Y H(崔玉虹), et al. Preparation and evaluation on the electro-catalytic character risitics of Ti-base lead dioxide electrode[J]. Journal of Molecular Catalysis, 2002, 16(3): 181-186.
[19] Uvarow V, Popov I. Metrological characterization of X-ray diffraction methods at different acquisition geometries for determination of crystallite size in nano-scale materials[J]. Materials Characterization, 2013, 85: 111-123.
[20] Comninellis C, Pulgarin C. Anodic oxidation of phenol for waste water treatment[J]. Journal of Applied Electrochemistry, 1991, 21(8): 703-708.
[21] Cao J L(曹江林), Wu Z C(吴祖成), Li H X(李红霞), et al. Inactivation of PbO2 anodes during oxygen evolution in sulfuric acid solution[J]. Acta Physico-Chimica Sinica, 2007, 23(10):1515-1519.
[22] Ren X B(任秀斌), Lu H Y(陆海彦), Liu Y N(刘亚男), et al. 3-Dimensional growth mechanism of lead dioxide electrode on the Ti substrate in the process of electrochemical deposition[J]. Acta Chemica Sinica(化学学报), 2009, 67(9): 888-892.
[23] Velichenko A B, Girenko D V, Danilov F I. Mechanism of lead dioxide electrodeposition[J]. Journal of Electroanalytical Chemistry, 1996, 405(1/2): 127-132.
[24] Neboj?a D N, Djendji D V. Influence of the complex formation on the morphology of lead powder particles produced by the electrodeposition processes[J]. Advanced Powder Technology, 2013, 24(3): 674-682.
[25] Johnson D C, Feng J, Houk L L. Direct electrochemical degradation of organic wastes in aqueous media[J]. Electrochimica Acta, 2000, 46(2/3): 323-330.
[26] Ding H Y(丁海洋), Feng Y J(冯玉杰), Liu J F(刘峻峰). Comparison of electrocatalytic performance of different anodes with cyclic voltammetry and Tafel curves[J]. Chinese Journal of catalysis, 2007, 28(7): 646-650.
[27] Wang Y Q(王雅琼), Gu S(顾衫), Xu W L(许文林), et al. Electrochemical oxidation of phenol on Ti-based PbO2 electrodes[J]. Rare Metal Materials and Engineering(稀有金属材料与工程), 2007, 36(5): 874-878.

β-PbO₂/Sb-SnO₂/Ti电极的苯酚电催化性能研究

Electro-Catalytic Properties of β-PbO₂/Sb-SnO₂/Ti Electrode on Phenol Oxidation

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