Ag掺杂Ti/PbO2电极的制备及其在苯酚降解中的应用

doi:10.16085/j.issn.1000-6613.2019-1232

摘要/Abstract

摘要：

使用化学还原和电沉积的方法制备了单质银（Ag）掺杂的Ti/PbO₂电极（Ti/Ag-PbO₂）。在保持镀银液浓度一定的条件下，通过改变镀银的时长制备出三种银含量的钛基体二氧化铅电极（Ti/Ag1-PbO₂、Ti/Ag2-PbO₂、Ti/Ag3-PbO₂）。利用X射线光电子能谱（XPS）和X射线荧光光谱分析（XRF）确定了PbO₂电极中Ag的价态和掺杂量。扫描电子显微镜（SEM）和X射线衍射（XRD）结果表明，Ag掺杂未明显改变电极的表面形态和晶型。根据涂层附着力测试试验发现，掺银PbO₂电极与基底之间有更好的结合力，电极使用寿命提高了约2.5倍。电化学交流阻抗谱（EIS）和循环伏安法（CV）测试结果表明，Ag的掺杂大幅降低了PbO₂电极的电荷转移电阻，提高了电极的电催化活性。利用掺银量2.7%（质量分数）的Ti/PbO₂电极降解100mg/L的苯酚水溶液，相较常规Ti/PbO₂电极，完全降解时间缩短了33.3%，降解能耗下降了34%。

关键词: 电化学, 降解, 氧化, Ti/PbO₂电极

Abstract:

An elemental silver (Ag) doped Ti/PbO₂ electrode (Ti/Ag-PbO₂) was prepared by chemical reduction and electrodeposition. Three titanium-based lead dioxide electrodes with different Ag contents (Ti/Ag1-PbO₂、Ti/Ag2-PbO₂、Ti/Ag3-PbO₂) were prepared by changing the duration of silver plating while maintaining a constant silver plating concentration. The valence state and doping amounts of Ag in the PbO₂ electrode were determined by X-ray photoelectron spectroscopy (XPS) and X-ray fluorescence spectroscopy (XRF). Scanning electron microscopy (SEM) and X-ray diffraction (XRD) results showed that the Ag doping did not significantly change the surface morphology and crystal form of the electrode. According to the coating adhesion test, the silver-doped PbO₂ electrode showed stronger bonding force with the substrate, and the electrode life was improved by about 2.5 times. Electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) tests showed that the doping of Ag significantly reduced the charge transfer resistance of the PbO₂ electrode and improved the electrocatalytic activity of the electrode. The Ti/PbO₂ electrode doped with 2.7% silver was used to degrade 100mg/L phenol aqueous solution. Compared with the conventional Ti/PbO₂ electrode, the complete degradation time was shortened by 33.3%, and the degradation energy consumption decreased by 34%.

Key words: electrochemistry, degradation, oxidation, Ti/PbO₂ electrode

中图分类号:

O646.542

张君泽,王红宁,陈若愚. Ag掺杂Ti/PbO₂电极的制备及其在苯酚降解中的应用[J]. 化工进展, 2020, 39(4): 1414-1421.

Junze ZHANG,Hongning WANG,Ruoyu CHEN. Preparation of silver doped Ti/PbO₂ electrode and its application in phenol degradation[J]. Chemical Industry and Engineering Progress, 2020, 39(4): 1414-1421.

图/表 14

图1 高含量银掺杂钛基体二氧化铅电极与未掺杂钛基体二氧化铅电极的场发射扫描电子显微镜照片

图2 钛基体表面不同涂层的X射线衍射图

图3 银掺杂钛基体二氧化铅电极铅和银的X射线光电子能谱分析图

图4 不同含量银掺杂钛基体二氧化铅电极的电化学阻抗谱和等效电路图

表1 不同电极的电化学阻抗谱模拟参数

电极名称	R_s/Ω·cm^-2	R_ct/Ω·cm^-2
Ti/PbO₂	5.754	2437
Ti/Ag1-PbO₂	5.037	246.6
Ti/Ag2-PbO₂	4.482	79.41
Ti/Ag3-PbO₂	4.465	79.25

图5 不同含量银掺杂钛基体二氧化铅电极的循环伏安曲线

图6 不同含量银掺杂钛基体二氧化铅电极的极化曲线

图7 不同含量银掺杂钛基体二氧化铅电极降解苯酚溶液的效率图

表2 相同电流密度下不同的电极降解能耗[22]

电极名称	降解电压/V	能耗/W·h·L^-1	节约能耗/%
Ti/PbO₂	6.85	12.33
Ti/Ag1-PbO₂	4.80	8.64	29.93
Ti/Ag2-PbO₂	4.60	8.28	32.85
Ti/Ag3-PbO₂	4.51	8.12	34.16

图8 不同含量银掺杂钛基体二氧化铅电极涂层的声发射信号-载荷测量曲线

图9 不同含量银掺杂钛基体二氧化铅电极的稳定性测试图

图10 银掺杂钛基体二氧化铅电极降解苯酚溶液的降解次数-降解时间图

图11 银掺杂钛基体二氧化铅电极使用前后的电化学阻抗谱

图12 银掺杂钛基体二氧化铅电极使用前后的循环伏安曲线

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Ag掺杂Ti/PbO₂电极的制备及其在苯酚降解中的应用

Preparation of silver doped Ti/PbO₂ electrode and its application in phenol degradation

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