本文利用电沉积制得ZrO2掺杂铌基二氧化铅电极,通过扫描电镜(SEM)和X射线衍射(XRD)观察表征了Nb/ZrO2+PbO2电极表面形貌特征及组成. 用线性伏安曲线、电化学交流阻抗和循环伏安曲线测试了Nb/ZrO2+PbO2电极电化学性能,及其甲基橙(MO)的降解电催化效果. 结果表明,ZrO2掺杂使Nb/PbO2电极表面更致密、粗糙,结晶尺寸更小,增大了电极比表面积,提高了电极电催化活性. Nb/ZrO2+PbO2电极活性层主要由β-PbO2和少量的α-PbO2以及部分ZrO2共沉积而成. 有较高的析氧电位、吸附电容和较低的电荷转移电阻,其甲基橙(MO)降解电催化活性更佳,降解过程受扩散控制.
The zirconium oxide (ZrO2)-doped niobium based lead oxide (Nb/PbO2) electrode was prepared by electrodeposition. The microstructures and electrochemical properties of Nb/ZrO2+PbO2 electrode were investigated using scanning electron microscopy (SEM), X-ray diffraction (XRD), linear sweep voltammetry, electrochemical impedance spectroscopy and cyclic voltammotry. In addition, the Nb/PbO2 electrode was used as an anode for the electrochemical degradation of methyl orange (MO). Results revealed that the ZrO2 doping made the Nb/PbO2 electrode surface denser and rougher with smaller sized crystal particles, which increased the specific surface area and enhanced the electrocatalytic activity of the electrode. The Nb/ZrO2+PbO2 electrode was mainly composed of β-PbO2 with a small amount of α-PbO2 and ZrO2 formed by codeposition. Accordingly, the Nb/ZrO2+PbO2 electrode possessed higher oxygen-evolution potential, larger adsorption capacity and lower charge-transfer resistance, as well as higher electrocatalytic activity in the degradation of organic materials than the Nb/PbO2 electrode. The MO degradation processes were irreversible and controlled by diffusion.
[1] Kar A, Smith Y R, Subramanian V. Improved photocatalytic degradation of textile dye using titanium dioxide nanotubes formed over titanium wires[J]. Environmental Science and Technology, 2009, 43(9): 3260-3265.
[2] Shakir K, Elkafrawy A F, Ghoneimy H F, et al. Removal of rhodamine B (a basic dye) and thoron (an acidic dye) from dilute aqueous solutions and wastewater simulants by ion flotation[J]. Water Research, 2010, 44(5): 1449-1461.
[3] Ma H Z, Wang B, Luo X Y. Studies on degradation of Methyl Orange wastewater by combined electrochemical process[J]. Journal of Hazardous Materials, 2007, 149(2): 492-498.
[4] Zhou M H, S?rkk? H K, Sillanp?? M K. A comparative experimental study on methyl orange degradation by electrochemical oxidation on BDD and MMO electrodes[J]. Separation and Purification Technology, 2011, 78(3): 290-297.
[5] Zhou J B, Hao S, Gao L P, et al. Study on adsorption performance of coal based activated carbon to radioactive iodine and stable iodine[J]. Annals of Nuclear Energy, 2014, 7: 237-241.
[6] Prigione V, Tigini V, Pezzella C A, et al. Decolourisation and detoxification of textile effluents by fungal biosorption[J]. Water Research, 2008, 42(12): 2911-2920.
[7] Figueroa S, Vázquez L, Alvarez-Gallegos A. Decolorizing textile wastewater with Fenton’s reagent electrogenerated with a solar photovoltaic cell[J]. Water Research, 2009, 43(2): 283-294.
[8] Chu L B, Xing X H, Yu A F, et al. Enhanced ozonation of simulated dyestuff wastewater by microbubbles[J]. Chemosphere, 2007, 68(10): 1854-1860.
[9] Zhan X M, Wang J L, Wen X H, et al. Indirect electrochemical treatment of saline dyestuff wastewater[J]. Environmental Technology, 2001, 22(9): 1105-1111.
[10] Panizza M, Cerisola G. Direct and mediated anodic oxidation of organic pollutants[J]. Chemical Reviews, 2009, 109(12): 6541-6569.
[11] Samet Y, Agengui L, Abdelhédi R. Anodic oxidation of chlorpyrifos in aqueous solution at lead dioxide electrodes[J]. Journal of Electroanalytical Chemistry, 2010, 650(1): 152-158.
[12] Song Y H, Wei G, Xiong R C. Structure and properties of PbO2-CeO2 anodes on stainless steel[J]. Electrochimica Acta, 2007, 52(24): 7022-7027.
[13] Franco D V, Leonardo M, Da S, et al. Influence of the electrolyte composition on the kinetics of the oxygen evolution reaction and ozone production processes[J]. Journal of the Brazilian Chemical Society, 2006, 17(4): 746-751.
[14] Yang W, Yang W, Lin X. Research on PEG modified Bi-doping lead dioxide electrode and mechanism [J]. Applied Surface Science, 2012, 258(15): 5716-5722.
[15] Duan X Y, Tian L F, Liu W, et al. Study on electrochemical oxidation of 4-Chlorophenol on a vitreous carbon electrode using cyclic voltammetry[J]. Electrochimica Acta, 2013, 94: 192-197.