欢迎访问《电化学(中英文)》期刊官方网站,今天是
研究论文

PdCu合金纳米晶体的制备和电催化活性研究

  • 武海滨 ,
  • 张瑞中 ,
  • 陈卫
展开
  • 电分析化学国家重点实验室,中国科学院长春应用化学研究所,吉林 长春 130022

收稿日期: 2011-12-15

  修回日期: 2012-01-13

  网络出版日期: 2012-01-23

基金资助

国家自然科学基金(No. 21043013)和中国科学院长春应用化学研究所人才引进启动基金资助

Synthesis and Electrocatalysis of PdCu Alloy Nanocrystals

  • WU Hai-Bin ,
  • ZHANG Rui-Zhong ,
  • CHEN Wei
Expand
  • State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China

Received date: 2011-12-15

  Revised date: 2012-01-13

  Online published: 2012-01-23

摘要

改变表面活性剂1-十八烯(ODE)和油胺(OLA)或油酸(OA)的配比,以1,2-二羟基十六烷二醇作还原剂同时还原乙酰丙酮铜Cu(acac)2和乙酰丙酮钯Pd(acac)2一步法制备了单分散的球形和米花形的PdCu纳米粒子.透射电子显微镜和XRD等结构表征表明,两种形状的PdCu纳米粒子均为(111)面占优的合金纳米晶体,其平均粒径分别为12.7 ± 0.18 和 20.4 ± 0.31 nm.电化学循环伏安法(CV)测定了两种PdCu合金纳米粒子对甲酸氧化的电催化活性.结果表明,在球形PdCu纳米粒子上得到的甲酸氧化峰电流密度约为米花状纳米粒子(PdCu-B)上的5.6倍.同时,前者显示出了更好的抗CO毒化能力.计时电流测量也表明,球状PdCu纳米粒子比米花状纳米粒子有更好的电催化稳定性能.

本文引用格式

武海滨 , 张瑞中 , 陈卫 . PdCu合金纳米晶体的制备和电催化活性研究[J]. 电化学, 2013 , 19(2) : 115 -119 . DOI: 10.61558/2993-074X.2943

Abstract

Monodispersed PdCu alloy nanoparticles were synthesized by co-reduction of Cu(acac)2 and Pd(acac)2 with 1, 2-hexadecanediol. The spherical and popcorn-like shapes of PdCu alloy nanoparticles were obtained by changing the ratios of mixed surface protecting ligands of 1-octadecene, and oleylamine or oleic acid. TEM and XRD measurements showed that both PdCu nanoparticles are alloy nanocrystals dominated with (111) planes and the average sizes are 12.7 ± 0.18 and 20.4 ± 0.31 nm for he spherical and popcorn-like PdCu nanoparticles, respectively. The electrocatalytic activities of the PdCu nanocrystals for formic acid oxidation were evaluated by electrochemical cyclic voltammetry (CV). The result showed that the peak current density of formic acid oxidation on the spherical PdCu nanocrystals is 6.5 times higher than that on the popcorn-like PdCu nanoparticles. Moreover, by comparing the ratio of the current density of the first anodic peak to the cathodic peak, the spherical PdCu nanocrystals exhibit better tolerance to CO poisoning than that of the popcorn-like counterparts. Chronoamperometric measurement indicated that the spherical PdCu nanocrystals have better activity and stability for formic acid oxidation compared to the popcorn-like PdCu nanoparticles.

参考文献

[1] Rice C, Ha R I, Masel R I, et al. Direct formic acid fuel cells [J]. Journal of Power Sources, 2002, 111(1): 83-89.
[2] Dillon R, Srinivasan S, Arico A S, et al. International activities in DMFC R&D: status of technologies and potential applications [J]. Journal of Power Sources 2004, 127(1/2): 112-126.
[3] Zhu Y M, Ha S Y, Masel R I. High power density direct formic acid fuel cells [J]. Journal of Power Sources 2004, 130(1/2): 8-14.
[4] Tian N, Zhou Z Y, Ding Y, et al. Synthesis of tetrahexahedral platinum nanocrystals with high-index facets and high electro-oxidation activity [J]. Science, 2007, 316(5825): 732-735.
[5] Chen W, Kim J M, Sun S H, et al. Composition effects of FePt alloy nanoparticles on the electro-oxidation of formic acid [J]. Langmuir, 2007, 23(22): 11303-11310.
[6] Chen W, Chen S W. Iridium-platinum alloy nanoparticles: Composition-dependent electrocatalytic activity for formic acid oxidation [J]. Journal of Material Chemistry, 2011, 21(25): 9169-9178.
[7] Tian N, Zhou Z Y, Yu N F, et al. Direct electrodeposition of tetrahexahedral Pd nanocrystals with high-index facets and high catalytic activity for ethanol electrooxidation [J]. Journal of the American Chemical Society, 2010, 132(22): 7580-7581.
[8] Chen W, Chen S W. Oxygen electroreduction catalyzed by gold nanoclusters: strong core size effects [J]. Angewandte Chemie International Edition, 2009, 48(24): 4386-4389.
[9] Zhou Z Y, Huang Z Z, Chen D J, et al. High-index faceted platinum nanocrystals supported on carbon black as highly efficient catalysts for ethanol electrooxidation [J]. Angewandte Chemie International Edition, 2010, 49(2): 411-414.
[10] Lu Y Z, Chen W, One- pot synthesis of heterostructured Pt-Ru nanocrystals for catalytic formic acid oxidation [J]. Chemical Communications, 2011, 47(9): 2541-2543.
[11] Chen W, Xu L P, Chen S W, Enhanced electrocatalytic oxidation of formic acid by platinum deposition on ruthenium nanoparticle surfaces [J]. Journal of Electroanalytical Chemistry, 2009, 631(1/2): 36-42.
[12] Chen W, Kim J, Sun S H, et al. Electrocatalytic reduction of oxygen by FePt alloy nanoparticles [J]. Journal of Physical Chemistry C, 2008, 112(10): 3891-3898.
[13] Lu Y Z, Chen W. Nanoneedle-covered Pd-Ag nanotubes: high electrocatalytic activity for formic acid oxidation [J]. Journal of Physical Chemistry C, 2010, 114(49): 21190-21200.
[14] Shao M H, Shoemaker K, Peles A, et al. Pt monolayer on porous Pd-Cu alloys as oxygen reduction electrocatalysts [J]. Journal of the American Chemical Society, 2010, 132 (27): 9253-9255.
[15] Kariuki N N, Wang X, Mawdsley J R, et al. Colloidal synthesis and characterization of carbon-supported Pd-Cu nanoparticle oxygen reduction electrocatalysts [J]. Chemistry of Materials, 2010, 22 (14): 4144-4152.
[16] Wang X P, Kariuki N, Vaughey J T, et al. Bimetallic Pd-Cu oxygen reduction electrocatalysts [J]. Journal of The Electrochemical Society, 2008, 155(6): B602-B609.
[17] Park K H, Lee Y W, Kang S W, et al. A facile one-pot synthesis and enhanced formic acid oxidation of monodisperse Pd-Cu nanocatalysts [J]. Chemistry - An Asian Journal, 2011, 6(6): 1515-1519.
[18] Clavilier J, Armand D, Sun S G, et al. Electrochemical adsorption behaviour of platinum stepped surfaces in sulphuric acid solutions [J]. Journal of Electroanalytical Chemistry, 1986, 205(1/2): 267-277.
[19] Lebedeva N P, Koper M T M, Feliu J M, et al. Mechanism and kinetics of the electrochemical CO adlayer oxidation on Pt(111) [J]. Journal of Electroanalytical Chemistry, 2002, 524-525: 242-251.
[20] Chen W, Kim J, Sun S H, et al. Electro-oxidation of formic acid catalyzed by FePt nanoparticles [J]. Physical Chemistry Chemical Physics, 2006, 8(23): 2779-2786.
文章导航

/