•  
  •  
 

Corresponding Author

Fang-zu YANG(fzyang@xmu.edu.cn)

Abstract

The Pd-Ni alloy nanoparticles with nickel atomic contents of 12.0%, 16.4% and 22.6% were successfully electrodeposited from a Pd-Ni alloy electrolyte by square wave pulse plating. The alloy nanoparticles were in the spherical shape with a diameter of 50 ~ 80 nm. As the growth potential of the alloy was negatively shifted, the nickel content of the alloy was increased, and the size of the nanoparticles was almost the same, whereas the number, the degree of crosslinking and the real active area of the nanoparticles were increased. As the nickel content of the alloy nanoparticles increased, the peak current for weakly adsorbing hydrogen was increased. The alloy nanoparticles electrodes were shown in a good electrocatalytic oxidation activity to formic acid. The electrocatalytic oxidation stability of the alloy nanoparticles was increased by the increases of the number and the degree of crosslinking.

Graphical Abstract

Keywords

Pd-Ni alloy, nanoparticles, formic acid, oxidation, electrocatalysis

Publication Date

2014-02-25

Online Available Date

2014-02-24

Revised Date

2013-01-11

Received Date

2012-12-05

References

[1] Rhee Y. Crossover of formic acid through Nafion? membranes[J]. Journal of Power Sources, 2003, 117(1/2): 35-38.
[2] Demirci U. Direct liquid-feed fuel cells: Thermodynamic and environmental concerns[J]. Journal of Power Sources, 2007, 169(2): 239-246.
[3] 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.
[4] Rice C. Catalysts for direct formic acid fuel cells[J]. Journal of Power Sources, 2003, 115(2): 229-235.
[5] 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.
[6] Capon A, Parson R. The oxidation of formic acid at noble metal electrodes: I. Review of previous work[J]. Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, 1973, 44: 1-7.
[7] Capon A, Parsons R. The oxidation of formic acid at noble metal electrodes: Part III. Intermediates and mechanism on platinum electrodes[J]. Journal of Electroanalytical Chemistry, 1973, 45: 205-231.
[8] Chen W, Kim J, Sun S, et al. Composition effects of FePt alloy nanoparticles on the electro-oxidation of formic acid[J]. Langmuir, 2007, 23(22): 11303-11310.
[9] Tripkovic A V, Popovic K D, Stevanovic R M, et al. Activity of a PtBi alloy in the electrochemical oxidation of formic acid[J]. Electrochemistry Communications, 2006, 8(9): 1492-1498.
[10] Huang J, Hou H, You T. Highly efficient electrocatalytic oxidation of formic acid by electrospun carbon nanofiber-supported PtxAu100-x bimetallic electrocatalyst[J]. Electrochemistry Communications, 2009, 11(6): 1281-1284.
[11] Liu W, Huang J. Electro-oxidation of formic acid on carbon supported Pt-Os catalyst[J]. Journal of Power Sources, 2009, 189(2): 1012-1015.
[12] Huang Y, Zhou X, Liao J, et al. Synthesis of Pd/C catalysts with designed lattice constants for the electro-oxidation of formic acid[J]. Electrochemistry Communications, 2008, 10(8): 1155-1157.
[13] Zhu Y, Kang Y, Zou Z, et al. A facile preparation of carbon-supported Pd nanoparticles for electrocatalytic oxidation of formic acid[J]. Electrochemistry Communications, 2008, 10(5): 802-805.
[14] Wang R, Liao S, Ji S. High performance Pd-based catalysts for oxidation of formic acid[J]. Journal of Power Sources, 2008, 180(1): 205-208.
[15] Yang G X (杨改秀),Chen T T (陈婷婷),Tang Y W (唐亚文),et al. Electrocatalytic performance of silicotungstic acid modified carbon supported Pd catalyst for oxidation of fomic acid[J]. Acta Physico-Chimica Sinica (物理化学学报),2009, 25(12): 2450-2454.
[16] Hong Y J (洪玉洁), Shen J Z (沈娟章), Li H Z (李焕芝), et al. Effect of electrolyte on electrocatalytic performance of carbon supported Pd catalyst for formic acid oxidation[J]. Chinese Journal of Inorganic Chemistry (无机化学学报), 2011, 27(7): 1383-1387.
[17] Arenz M, Stamenkovic V, Schmidt T J, et al. The electro-oxidation of formic acid on Pt-Pd single crystal bimetallic surfaces[J]. Physical Chemistry Chemical Physics, 2003, 5(19): 4242-4251.
[18] Zhang H X, Wang C, Wang J Y, et al. Carbon-supported Pd-Pt nanoalloy with low Pt content and superior catalysis for formic acid electro-oxidation[J]. Journal of Physical Chemistry C, 2010, 114(14): 6446-6451.
[19] Yang L J (杨莉君), Su H N (苏华能), Shu T (舒婷), et al. Enhanced electro-oxidation of formic acid by PdPt bimetallic catalyst with CeO2-modified carbon support[J]. Scientia Sinica Chimica (中国科学:化学), 2011, 41(12): 1817-1825.
[20] Zhang S, Qing M, Zhang H, et al. Electrocatalytic oxidation of formic acid on functional MWCNTs supported nanostructured Pd-Au catalyst[J]. Electrochemistry Communications, 2009, 11(11): 2249-2252.
[21] Du C, Chen M, Wang W, et al. Electrodeposited PdNi2 alloy with novelly enhanced catalytic activity for electrooxidation of formic acid[J]. Electrochemistry Communications, 2010, 12(6): 843-846.
[22] Xi C M (奚彩明), Shi Y (施毅), Zhao J Y (赵佳越), et al. Electrocatalytic oxidation of formic acid on the carbon supported Pd-Ni alloy nanoparticles[J]. Chemical Journal of Chinese Universities (高等学校化学学报), 2011, 32(6): 1349-1353.
[23] Demirci U B. Theoretical means for searching bimetallic alloys as anode electrocatalysts for direct liquid-feed fuel cells[J]. Journal of Power Sources, 2007, 173(1): 11-18.
[24] Hammer B, N?rskov J K. Theoretical surface science and catalysis—calculations and concepts[J]. Advances in Catalysis, 2000, 45, 71-129.
[25] Lim B, Jiang M, Tao J, et al. Shape-controlled synthesis of Pd nanocrystals in aqueous solutions[J]. Advanced Functional Materials, 2009, 19(2): 189-200.
[26] Chen J, Lim B, Lee E, et al. Shape-controlled synthesis of platinum nanocrystals for catalytic and electrocatalytic applications[J]. Nano Today, 2009, 4(1): 81-95.
[27] Tian N, Zhou Z Y, Sun S G, et al. Synthesis of tetrahexahedral platinum nanocrystals with high-index facets and high electro-oxidation activity[J]. Science, 2007, 316(5825): 732-735.
[28] Yue J P (岳俊培), Yang F Z (杨防祖), Tian Z Q (田中群), et al. Electrocrystallization of Pd-Ni alloys on glassy carbon electrode[J]. Acta Physico-Chimica Sinica (物理化学学报), 2011, 27(6): 1446-1450.
[29] 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.
[30] Li H Z (李焕芝), Shen J Z (沈娟章), Yang G X (杨改秀), et al. Anodic Pd catalyst in direct formic acid fuel cell and its electrocatalytic stability[J]. Chemical Journal of Chinese Universities (高等学校化学学报), 2011, 32(7): 1445-1450.
[31] Yue J P, Yang F Z, Tian Z Q, et al. Effects of nickel ion contents on electrodeposition, composition, structure and properties of palladium-nickel alloys[J]. Transactions of the Institute of Metal Finishing, 2011, 89 (5): 249-254.
[32] Tominaka S, Momma T, Osaka T. Electrodeposited Pd-Co catalyst for direct methanol fuel cell electrodes: Preparation and characterization[J]. Electrochimica Acta, 2008, 53(14): 4679-4686.
[33] Meng H, Sun S, Masse J P, et al. Electrosynthesis of Pd single-crystal nanothorns and their application in the oxidation of formic acid[J]. Chemistry of Materials, 2008, 20(22): 6998-7002.
[34] Liu H, Song C, Zhang L, et al. A review of anode catalysis in the direct methanol fuel cell[J]. Journal of Power Sources, 2006, 155(2), 95-110.

Share

COinS
 
 

To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.