非晶态Pd-P/聚吡咯/泡沫Ni电极对五氯苯酚的催化还原

doi:10.15541/jim20190582

摘要/Abstract

摘要：

电催化还原氯代有机物具有效率高和环境友好等优点。研究采用电化学沉积法在泡沫Ni上制备了非晶态Pd-P/聚吡咯/泡沫Ni(Pd-P/PPy/foam Ni)复合电极, 用于电催化还原法去除水中的五氯苯酚(PCP)。扫描电镜(SEM)、透射电镜(TEM)、X射线衍射分析(XRD)和X射线光电子能谱分析(XPS)等表征结果表明, 掺杂P使Pd催化剂分散均匀, 粒径变小, 且由晶态结构转变为非晶态。由电催化还原PCP发现, 掺杂P明显提高了电极的催化活性。在n(Pd)/n(P)为1 : 3, Pd负载量为0.15 mg/cm ², H₂SO₄浓度为0.2 mol/L, 阴极电位为-1.2 V条件下, 处理180 min后, PCP的降解率达到90.8%。另外, Pd-P/PPy/foam Ni电极重复使用8次, 仍保持良好的稳定性。

关键词: Pd-P/PPy/foam Ni, 非晶态, 电催化还原

Abstract:

Electrocatalytic hydrodechlorination technology possesses great potential in the field of chlorinated organic compound treatment due to the high efficiency, environmental friendliness, etc. The amorphous Pd-P/polypyrrole(PPy)/foam Ni electrode was prepared by electrochemical deposition for electrochemical hydrodechlorination of the pentachlorophenol (PCP). Morphology and chemical structure of Pd-P on the PPy/foam Ni electrode was investigated by the Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), X-ray diffraction analysis (XRD), and X-ray photoelectron spectroscope (XPS). The result indicated that the Pd-P catalyst was evenly dispersed on the PPy/foam Ni electrode with small particles and changed from crystalline state to amorphous state. The electrocatalytic reduction of PCP certificated that the doping of P significantly increased the catalytic activity of the electrode. The degradation efficiency of PCP reached 90.8% after electrocatalytic reduction for 180 min under the condition of n(Pd)/n(P)=1 : 3, Pd loading=0.15 mg/cm ², C_H2SO4=0.20 mol/L and V_cathode=-1.2 V. In addition, the Pd-P/PPy/foam Ni electrode exhibited high electrocatalytic stability after reused for 8 times without any notable deactivation.

Key words: Pd-P/PPy/foam Ni electrode, amorphous, electrocatalytic reduction

中图分类号:

TQ174

王婧, 崔春月, 田侠, 张雪, 王颖, 辛言君. 非晶态Pd-P/聚吡咯/泡沫Ni电极对五氯苯酚的催化还原[J]. 无机材料学报, 2020, 35(10): 1157-1162.

WANG Jing, CUI Chunyue, TIAN Xia, ZHANG Xue, WANG Ying, XIN Yanjun. Amorphous Pd-P/Polypyrrole/Foam Ni Electrode: Electrocatalytic Hydrodechlorination of Pentachlorophenol[J]. Journal of Inorganic Materials, 2020, 35(10): 1157-1162.

图/表 9

图1 Pd/PPy/foam Ni(a)和Pd-P/PPy/foam Ni(b)的SEM和TEM(插图)照片

Fig. 1 SEM and TEM (insets) images of Pd/PPy/foam Ni (a) and Pd-P/PPy/foam Ni (b) Pd loading: 0.15 mg/cm2, n(Pd) : n(P) = 1 : 3

图2 Pd/PPy/foam Ni和Pd-P/PPy/foam Ni的XRD图谱

Fig. 2 XRD patterns of Pd/PPy/foam Ni and Pd-P/PPy/foam Ni

图3 Pd/PPy/foam Ni(a)和Pd-P/PPy/foam Ni(b)的HR-TEM照片及其SAED斑点

Fig. 3 HR-TEM images and correponding SAED patterns of Pd/PPy/foam Ni (a) and Pd-P/PPy/foam Ni (b)

图4 Pd-P/PPy/foam Ni 的XPS全谱图(a); Pd/PPy/foam Ni和Pd-P/PPy/foam Ni的Pd 3d XPS图谱(b)

Fig. 4 XPS spectra of Pd-P/PPy/foam Ni (a); Pd3d survey scan spectra of Pd/PPy/foam Ni and Pd-P/PPy/foam Ni (b)

图5 PPy/foam Ni、Pd/PPy/foam Ni 和 Pd-P/PPy/foam Ni电极的线性伏安曲线

Fig. 5 Linear voltammetry curves of PPy/foam Ni, Pd/PPy/ foam Ni and Pd-P/PPy/foam Ni

图6 Pd和P的摩尔比对水中PCP电催化还原效果的影响

Fig. 6 Effect of molar ratio between Pd and P on the dechlorination of PCP in water

图7 阴极电位对PCP降解效果的影响

Fig. 7 Effects of cathode potential on degradation of PCP (n(Pd) : n(P)=1 : 3, anolyte: 0.2 mol/L H2SO4, Na2SO4 concentration: 0.10 mol/L)

图8 Na2SO4浓度对PCP降解效果影响

Fig. 8 Effect of Na2SO4 concentration on degradation of PCP (n(Pd) : n(P)=1 : 3, cathode potential -1.2 V, H2SO4 concentration: 0.20 mol/L)

图9 PCP降解率与电极使用次数的关系

Fig. 9 Relationship between the degradation efficiency of PCP and cycling number (n(Pd) : n(P)=1 : 3, H2SO4 concentration: 0.20 mol/L, Cathode potential: -1.2 V)

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