浸渍法制备硅钨酸修饰的炭载钯催化剂电催化甲酸氧化

doi:10.3724/SP.J.1095.2013.30158

摘要/Abstract

摘要： 用浸渍的方法制备了硅钨酸（SiWA）修饰的炭载Pd(Pd/C-SiWA)催化剂。计时电流曲线研究表明，在Pd/C和Pd/C-SiWA催化剂电极上，3000 s时的电流密度分别为0.013和0.082 A/mg，分别为10 s时电流密度的2.5%和14.1%。结果表明，Pd/C-SiWA催化剂对甲酸氧化的电催化稳定性要远远优于Pd/C催化剂。这是因为Pd/C催化剂上SiWA的修饰抑制了甲酸的自分解, 从而减小了CO的毒化作用，改进了Pd/C催化剂对甲酸氧化的电催化和稳定性。

关键词: 直接甲酸燃料电池, 炭载钯催化剂, 硅钨酸修饰, 甲酸氧化, 甲酸分解

Abstract: The silicotungstic acid(SiWA) modified carbon supported Pd(Pd/C-SiWA) catalyst was prepared with immersing method. The chronoamperometric experiment shows that the current density are 0.013 A/mg and 0.082 A/mg at 3000 s for the Pd/C and Pd/C-SiWA catalysts, which are the 2.5% and 14.1% of that at 10 s, respectively. The result suggests that the electrocatalytic activity and stability of the Pd/C-SiWA catalyst for formic acid oxidation are much better than that of the Pd/C catalyst. This is attributed to that the Pd/C-SiWA catalyst inhibits the decomposition of formic acid leading to the decrease in the poisoning effect of CO. Thus, the electrocatalytic stability of the Pd/C catalyst for formic acid oxidation is improved.

Key words: direct formic acid fuel cell, carbon supported Pd catalyst, silicotungstic acid modification, formic acid oxidation, formic acid decomposition

中图分类号:

O646

王秀艳, 赵雪萍, 马树华. 浸渍法制备硅钨酸修饰的炭载钯催化剂电催化甲酸氧化[J]. 应用化学, DOI: 10.3724/SP.J.1095.2013.30158.

WANG Xiuyan1, ZHAO Xueping2, MA Shuhua2*. Preparation of Silicotungstic Acid Modified Carbon Supported Pd Catalyst by Impregnation Method and Its Electrocatalytic Performance for Formic Acid Oxidation[J]. Chinese Journal of Applied Chemistry, DOI: 10.3724/SP.J.1095.2013.30158.

参考文献

[1] Yu X W,Pickup P G. Recent Advances in Direct Formic Acid Fuel cells(DFAFC)[J]. J Power Sources,2008,182(1):124-132.

[2] Larsen R,Ha S,Zakzeski J,et al. Unusually Active Palladium-based Catalysts for the Electrooxidation of Formic Acid[J]. J Power Sources,2006,157(1):78-84.

[3] Ren M J,Kang Y Y,He W,et al. Origin of Performance Degradation of Palladium-based Direct Formic Acid Fuel Cells[J]. Appl Catal B Environ,2011,104(1/2):49-53.

[4] Zhang L L,Lu T H,Bao J C,et al. Preparation Method of an Ultrafine Carbon Supported Pd Catalyst as Anodic Catalyst in a Direct Formic Acid Fuel Cell[J]. Electrochem Commun,2006,8(10):1625-1627.

[5] Lu L,Shen L P,Shi Y,et al. New Insights into Enhanced Electrocatalytic Performances of Carbon Supported Pd-Cu Catalyst for Formic Acid Oxidation[J]. Electrochim Acta,2012,85(1):187-194.

[6] Feng L G,Yao S K,Zhao X,et al. Electrocatalytic Properties of Pd/C Catalyst for Formic Acid Electrooxidation Promoted by Europium Oxide[J]. J Power Sources,2012,197(1):38-43.

[7] Yu X W,Pickup P G. Mechanistic Study of the Deactivation of Carbon Supported Pd during Formic Acid Oxidation[J]. Electrochem Commun,2009,11(10):2012-2014.

[8] Xu C X,Liu Y Q,Wang J P,et al. Nanoporous Pd/Cu Alloy for Formic Acid Electro-oxidation[J]. J Power Sources,2012,199(1):124-131.

[9] Chen Y,Zhou Y M,Tang Y W,et al. Electrocatalytic Properties of Carbon-supported Pt-Ru Catalysts with the High Alloying Degree for Formic Acid Electrooxidation[J]. J Power Sources,2010,195(13):4129-4134.

[10] Yang G X,Chen Y,Zhou Y M,et al. Preparation of Carbon Supported Pd-P Catalyst with High Content of Element Phosphorus and Its Electrocatalytic Performance for Formic Acid Oxidation[J]. Electrochem Commun,2010,12(3):492-495.

[11] YANG Gaixiu,CHEN Tingting,TANG Yawen,et al. Electrocatalytic Performance of Silicotungstic Acid Modified Carbon Supported Pd Catalyst for Oxidation of Fomic Acid[J]. Acta Phys-Chim Sin,2009,25(12):2450-2454(in Chinese).

杨改秀,陈婷婷,唐亚文,等. 硅钨酸修饰炭载Pd催化剂对甲酸氧化的电催化性能[J]. 物理化学学报,2009,25(12):2450-2454.

[12] Lu L,Shen L P,Shi Y,et al. New Insights into Enhanced Electrocatalytic Performance of Carbon Supported Pd-Cu Catalyst for Formic Acid Oxidation[J]. Electrochim Acta,2012,85:187-194.

[13] Shen L P,Li H Z,Lu L,et al. Improvement and Mechanism of Electrocatalytic Performance of Pd-Ni/C Anodic Catalyst in Direct Formic Acid Fuel Cell[J]. Electrochim Acta,2013,89:497-502.

[14] Guo J L,She Y N,Jie M L,et al, Using Scherrer Formular Calculating Size of Crystalline Should Pay Attention to Several Questions[J]. J Inner Mongolia Normal Univ,2009,38(3):357-358.

[15] White J H,Sammells A,Perovskite F. Perovskite Anode Electrocatalysis for Direct Methanol Fuel Cells[J]. J Electrochem Soc,1993,140:2167-2177.