钛基PbO2+nano-WO3电极材料的复合共沉积及析氧活性

doi:10.7503/cjcu20140664

高等学校化学学报 ›› 2014, Vol. 35 ›› Issue (12): 2632.doi: 10.7503/cjcu20140664

钛基PbO₂+nano-WO₃电极材料的复合共沉积及析氧活性

丹媛媛^1,², 张丽¹, 陈立庄¹, 岳慧娟², 林海波³(), 陆海彦³

1. 江苏科技大学生物与化学工程学院, 镇江 212003
2. 吉林大学无机合成与制备化学国家重点实验室, 3. 化学学院, 长春 130012

收稿日期:2014-07-16 出版日期:2014-12-10 发布日期:2014-11-29
作者简介:联系人简介: 林海波, 男, 博士, 教授, 博士生导师, 主要从事电化学工程方面的研究. E-mail:lhb910@jlu.edu.cn
基金资助:
国家自然科学基金(批准号: 21201087, 21273097)、江苏省自然科学基金(批准号: BK20130460, BK20131244)、无机合成与制备化学国家重点实验室(吉林大学)开放课题(批准号: 2014-14)和江苏省高等学校自然科学研究项目(批准号: 11KJB150004)资助

Preparation of PbO₂+nano-WO₃ Composite Electrode on Ti Substrate by Composite Electrodeposition and Its Oxygen Evolution Activity^†

DAN Yuanyuan^1,², ZHANG Li¹, CHEN Lizhuang¹, YUE Huijuan², LIN Haibo^3,^*(), LU Haiyan³

1. School of Biology and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China
2. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,3. College of Chemistry, Jilin University, Changchun 130012, China

Received:2014-07-16 Online:2014-12-10 Published:2014-11-29
Contact: LIN Haibo E-mail:lhb910@jlu.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.21201087, 21273097), the Natural Science Foundation of Jiangsu Province of China(Nos.BK20130460, BK20131244), the Open Fund of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry in Jilin University, China(No.2014-14) and the Natural Science Foundation of the Jiangsu Higher Education Institutes, China(No.11KJB150004)

摘要/Abstract

摘要：

利用复合共沉积法, 在涂有中间层SnO₂-Sb₂O₅的Ti基体上制备了PbO₂+nano-WO₃复合电极材料. 采用X射线衍射(XRD)、 X射线光电子能谱(XPS)、扫描电子显微镜(SEM)和双电层电容法等对复合电极表面的组成、结构、形貌及有效电化学面积进行测试. 结果表明, 随着纳米WO₃掺杂量逐渐增大, 复合电极的表面粗糙度和孔隙率逐渐变大, 电化学有效面积也随之增大; 利用线性扫描及Tafel曲线等电化学测试方法研究了nano-WO₃的掺杂对复合电极析氧活性的影响, 结果表明, 掺杂nano-WO₃的复合电极较纯PbO₂电极的析氧活性大幅提高, 其起始析氧电位发生负移, 析氧过电位下降, 最大可降低近300 mV.

关键词: 二氧化铅, 三氧化钨, 复合共沉积, 析氧活性

Abstract:

PbO₂+nano-WO₃ composite electrode materials were prepared by the composite electrodeposition method on Ti substrate with the intermediate SnO₂-Sb₂O₅ layer. The composition, structure and morphology of the composite electrode materials were investigated by X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), scanning electron microscopy(SEM) analyses and double layer capacitance methode. The results indicate that porosity, roughness and electrochemically effective area of the composite electrode surface are increased because of the embedded nano-WO₃. Then, the composite electrodes were used as anodes for oxygen evolution reaction(OER). The activities for the OER of the composites were explained by recording linear scanning voltammograms and Tafel plots. In contrast with the PbO₂ electrode without nano-WO₃, oxygen evolution onset potentials of the composite electrodes become lower, the overpotentials for oxygen evolution of composite electrodes are decreased, and the OER activities are improved significantly. The overpotential for oxygen evolution at the composite electrode could be lowered by approximately 300 mV compared to that of PbO₂ electrode without nano-WO₃.

Key words: PbO₂, WO₃, Composite electrodeposition, Oxygen evolution activity

中图分类号:

O646

TrendMD:

丹媛媛, 张丽, 陈立庄, 岳慧娟, 林海波, 陆海彦. 钛基PbO₂+nano-WO₃电极材料的复合共沉积及析氧活性. 高等学校化学学报, 2014, 35(12): 2632.

DAN Yuanyuan, ZHANG Li, CHEN Lizhuang, YUE Huijuan, LIN Haibo, LU Haiyan. Preparation of PbO₂+nano-WO₃ Composite Electrode on Ti Substrate by Composite Electrodeposition and Its Oxygen Evolution Activity^†. Chem. J. Chinese Universities, 2014, 35(12): 2632.

图/表 9

Fig.1 XRD patterns of PbO2(a), PbO2+nano-WO3 composite(b) and nano-WO3·H2O(c)

Fig.2 TEM image of WO3·H2O nano-sheets

Table 1 Surface composition, double layer capacitance(Cdl) and electrochemically effective area(RF) of PbO2+nano-WO3 composites synthesized with different concentrations of WO3·H2O nano-sheets in the plating suspension

Material	c(WO₃·H₂O)/(mmol·L^-1)	x_W(%)	x_Pb(%)	n(W):n(Pb)	C_dl/(μF·cm^-2)	R_F
PbO₂	0	0	33.33	0:1	69.4	1.15
PbO₂+nano-WO₃	1	1.71	34.26	0.05:1	333.0	5.55
	3	2.74	33.87	0.08:1	859.8	14.33
	5	3.67	33.25	0.11:1	1927.2	32.12
	7	5.26	32.48	0.16:1	3147.0	52.45
	10	5.65	31.69	0.18:1	3406.8	56.78

Fig.3 SEM images of the surfaces of PbO2+nano-WO3 composite electrode materials xW(%): (A) 0; (B) 1.71; (C) 3.67; (D) 5.65.

Fig.4 Linear scanning voltammograms at different composite electrodes in 1 mol/L H2SO4 Scan rate: 1 mV/s. xW(%): a. 0; b. 1.71; c. 2.74; d. 3.67; e. 5.26; f. 5.65.

Fig.5 Linear scanning voltammogram at WO3 electrode in 1 mol/L H2SO4 Scan rate: 1 mV/s.

Fig.6 Tafel plots for oxygen evolution at different composite electrodes in 1 mol/L H2SO4 Scan rate: 1 mV/s. xW(%): a. 0; b. 1.71; c. 2.74; d. 3.67; e. 5.26; f. 5.65.

Table 2 Overpotentials of the oxygen evolution and electrochemical parameters from the Tafel plots

Material	x_W(%)	a	b	$η over *$ /V
PbO₂	0	2.235	0.126	1.848
PbO₂+nano-WO₃	1.71	2.181	0.198	1.587
	2.74	2.167	0.196	1.579
	3.67	2.118	0.186	1.560
	5.26	2.048	0.165	1.553
	5.65	2.018	0.168	1.514

Table 2 Overpotentials of the oxygen evolution and electrochemical parameters from the Tafel plots

Material	x_W(%)	a	b	$η over *$ /V
PbO₂	0	2.235	0.126	1.848
PbO₂+nano-WO₃	1.71	2.181	0.198	1.587
	2.74	2.167	0.196	1.579
	3.67	2.118	0.186	1.560
	5.26	2.048	0.165	1.553
	5.65	2.018	0.168	1.514

Fig.7 SEM image of the PbO2+WO3 composite

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钛基PbO₂+nano-WO₃电极材料的复合共沉积及析氧活性

Preparation of PbO₂+nano-WO₃ Composite Electrode on Ti Substrate by Composite Electrodeposition and Its Oxygen Evolution Activity^†

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