用不同络合剂制备的Pd-Sn/C催化剂在碱性溶液中对乙醇氧化的电催化性能

doi:10.7503/cjcu20130795

高等学校化学学报 ›› 2014, Vol. 35 ›› Issue (3): 602.doi: 10.7503/cjcu20130795

用不同络合剂制备的Pd-Sn/C催化剂在碱性溶液中对乙醇氧化的电催化性能

李巧霞¹, 毛宏敏¹, 朱萍萍¹, 曹晓璐¹, 陆天虹², 徐群杰¹()

1. 上海电力学院环境与化学工程学院, 上海 200090
2. 江苏省新型动力电池重点实验室, 南京师范大学化学与材料科学学院, 南京 210097

收稿日期:2013-08-16 出版日期:2014-03-10 发布日期:2019-08-01
作者简介:联系人简介: 徐群杰, 男, 博士, 教授, 主要从事材料电化学和电催化研究. E-mail: xuqunjie@shiep.edu.cn
基金资助:
国家自然科学基金(批准号: 21103107)资助

Electrocatalytic Performance of Pd-Sn/C Catalyst Prepared with Different Complexants for Ethanol Oxidation in Alkaline Solution^†

LI Qiaoxia¹, MAO Hongmin¹, ZHU Pingping¹, CAO Xiaolu¹, LU Tianhong², XU Qunjie^1,^*()

1. College of Environmental and Chemical Engineering, Shanghai University of Electric Power, Shanghai 200090, China
2. Jiangsu Key Laboratory of New Power Batteries, College of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210097, China

Received:2013-08-16 Online:2014-03-10 Published:2019-08-01
Contact: XU Qunjie E-mail:xuqunjie@shiep.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(No.21103107)

摘要/Abstract

摘要：

采用3种不同的络合剂[柠檬酸三钠、反式-1,2-环己二胺四乙酸·一水(C₁₄H₂₂N₂O₈·H₂O, CyDTA)和氨水]制备了3种Pd-Sn/C催化剂. 用X射线能量色散谱(EDS)、 X射线衍射谱(XRD)和透射电子显微镜(TEM)表征了3种催化剂的平均粒径、形貌和组成. X射线光电子能谱(XPS)的测试结果表明, 3种催化剂表面存在Sn和SnO_x 2种状态. 电化学测试结果表明, 3种催化剂在碱性电解液中对乙醇氧化的电催化性能均优于商业化的Pd/C催化剂, 其中用CyDTA制备的Pd-Sn/C催化剂在碱性溶液中对乙醇氧化的电催化性能最好.

关键词: 乙醇氧化, 钯-锡催化剂, 络合剂, 电催化性能

Abstract:

Three complexants, sodium citrate, trans-1,2-diaminocyclohexane-N,N,N',N' -tetraacetic acid hydrate(C₁₄H₂₂N₂O₈·H₂O, CyDTA) and ammonia, were used to prepare Pd-Sn/C catalysts. It is found that the electrocatalytic performances of these three catalysts for ethanol oxidation in alkaline solution are better than commercialized Pd/C catalyst. The average particle diameter, morphology and composition of the Pd-Sn/C catalysts prepared were characterized by energy dispersive X-ray spectroscopy(EDS), X-ray diffraction(XRD) and transmission electron microscopy(TEM). X-ray photoclectron spectroscopy(XPS) measurement reveales that tin oxide and tin exist on the surface of the catalysts. The results of the electrochemical measurements indicate that the Pd-Sn/C-CyDTA catalyst has the best electrocatalytic performance for ethanol oxidation in alkaline solution.

Key words: Ethanol oxidation, Palladium-tin catalyst, Complexant, Electrocatalytic performance

中图分类号:

O646

TrendMD:

李巧霞, 毛宏敏, 朱萍萍, 曹晓璐, 陆天虹, 徐群杰. 用不同络合剂制备的Pd-Sn/C催化剂在碱性溶液中对乙醇氧化的电催化性能. 高等学校化学学报, 2014, 35(3): 602.

LI Qiaoxia, MAO Hongmin, ZHU Pingping, CAO Xiaolu, LU Tianhong, XU Qunjie. Electrocatalytic Performance of Pd-Sn/C Catalyst Prepared with Different Complexants for Ethanol Oxidation in Alkaline Solution^†. Chem. J. Chinese Universities, 2014, 35(3): 602.

图/表 9

Fig.1 TEM images(A—C) and histogram of particle size distribution(D—F) of Pd-Sn/C-ammonia(A, D), Pd-Sn/C-CyDTA(B, E) and Pd-Sn/C-trisodium citrate(C, F) catalysts

Fig.2 EDS spectra of Pd-Sn/C-ammonia(A), Pd-Sn/C-CyDTA(B), Pd-Sn/C-trisodium citrate(C) catalysts

Fig.3 XRD patterns of the Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-trisodium citrate(c) and Pd/C catalysts(d)

Fig.4 XPS spectra of Pd-Sn/C-CyDTA

Fig.5 Cyclic voltammograms of Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-trisodium citrate(c), Pd/C(d), Pd-Sn/C(e), Sn/C catalysts(f) in 1.0 mol/L KOH(A) or 1.0 mol/L KOH+1.0 mol/L C2H5OH(B) at a scan rate of 50 mV/s

Table 1 Physical and electrochemical patameters of Pd-Sn/C-ammonia, Pd-Sn/C-CyDTA, Pd-Sn/C-trisodium citrate and Pd/C, Pd-Sn/C*

Catalyst	Crystallite size/nm		EASA/(m²·g^-1)	E_op/V	E_p/V	i_p/(mA·cm^-2)
Catalyst	XRD		EASA/(m²·g^-1)	E_op/V	E_p/V	TEM
Pd-Sn/C-CyDTA	4.5	5.09	297.62	-0.632	-0.046	122.06
Pd-Sn/C-trisodium citrate	6.0	4.76	212.24	-0.702	-0.089	111.51
Pd-Sn/C-ammonia	5.4	5.18	178.59	-0.655	-0.125	97.83
Pd-Sn/C			131.09	-0.587	-0.081	60.16
Pd/C	10.1		88.53	-0.615	-0.177	49.16

Fig.6 Cycle stabilities of Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-trisodium citrate(c), Pd/C(d), Pd-Sn/C(e) catalysts in 1.0 mol/L KOH+1.0 mol/L C2H5OH at a scan rate of 50 mV/s

Fig.7 Chronoamperpmetric curves of Pd-Sn/C-ammonia(a), Pd-Sn/C-CyDTA(b), Pd-Sn/C-triso-dium citrate(c), Pd/C(d), Pd-Sn/C(e), Sn/C catalysts(f) in 1.0 mol/L KOH+1.0 mol/L C2H5OH solution for 3600 s at -0.25 V

Fig.8 Polarization curves for the Pd-Sn/C-CyDTA electrocalyst in 1.0 mol/L KOH and different concentrations of ethanolc(C2H5OH)/(mol·L-1): a. 1.0; b. 2.0; c. 3.0; d. 4.0; e. 5.0.

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用不同络合剂制备的Pd-Sn/C催化剂在碱性溶液中对乙醇氧化的电催化性能

Electrocatalytic Performance of Pd-Sn/C Catalyst Prepared with Different Complexants for Ethanol Oxidation in Alkaline Solution^†

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用不同络合剂制备的Pd-Sn/C催化剂在碱性溶液中对乙醇氧化的电催化性能

Electrocatalytic Performance of Pd-Sn/C Catalyst Prepared with Different Complexants for Ethanol Oxidation in Alkaline Solution†

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Electrocatalytic Performance of Pd-Sn/C Catalyst Prepared with Different Complexants for Ethanol Oxidation in Alkaline Solution^†