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Corresponding Author

Hui Yang(yangh@sari.ac.cn)

Abstract

A Pd/Ni bimetallic nanostructured electrocatalyst was fabricated via a two-step reduction route. Owing to an epitaxial growth of Pd atoms on the surface of Ni nanoparticles, heterostructured Pd/Ni nanocomposites were formed and verified by high resolution transmission electron microscopy combined with energy-dispersion X-ray spectroscopy. X-ray diffraction confirmed that the as-prepared Pd/Ni nanocomposites possessed a single face-centered-cubic (fcc) Pd structure, probably due to a weaker diffraction intensity of metallic Ni and/or overlapping by that of Pd. The intrinsic catalytic activity on the Pd/Ni is higher than that on the Pd. Moreover, the durability of formic acid oxidation on the Pd/Ni was much enhanced over the Pd nanoparticles. The change in electronic structure of the surface coordination unsaturated Pd atoms and the possible dissolution of Ni species from the Pd/Ni heterostructure may account for such an improved durability for formic acid oxidation.

Graphical Abstract

Keywords

formic acid oxidation, electrocatalysis, Pd/Ni heterostructure, durability

Publication Date

2012-12-28

Online Available Date

2012-09-07

Revised Date

2012-09-05

Received Date

2012-06-08

References

[1] Wang J Y, Zhang H X, Jiang K, et al. From HCOOH to CO at Pd electrodes: A surface-enhanced infrared spectroscopy study[J]. Journal of the American Chemical Society, 2011, 133(38): 14876-14879.

[2] Zhang H X, Wang S H, Jiang K, et al. In situ spectroscopic investigation of CO accumulation and poisoning on Pd black surfaces in concentrated HCOOH[J]. Journal of Power Sources, 2012, 199(1): 165-169.

[3] Yu X W, Pickup P G. Mechanistic study of the deactivation of carbon supported Pd during formic acid oxidation[J]. Electrochmistry Communications, 2009, 11(10): 2012-2014.

[4] Ren M J, Kang Y Y, He W, et al. Origin of performance degradation of palladium-based direct formic acid fuel cells[J]. Applied Catalysis B: Environmental, 2011, 104(1/2): 49-53.

[5] Wang X M, Xia Y Y. Electrocatalytic performance of PdCo-C catalyst for formic acid oxidation[J]. Electrochemistry Communications, 2008, 10(10): 1644-1646.

[6] Hann J L, Stafford K M, Morgan R D, et al. Performance of the direct formic acid fuel cell with electrochemically modified palladium-antimony anode catalyst[J]. Electrochimica Acta, 2010, 55(7): 2477-2481.

[7] Hammer B, N?rskov J K. Theoretical surface science and catalysis-calculations and concepts[J]. Advances in Catalysis, 2000, 45: 71-129.

[8] Ruban A, Hammer B, Stoltze P, et al. Surface electronic structure and reactivity of transition and noble metals[J]. Journal of Molecular Catalysis A: Chemical, 1997, 115(3): 421-429.

[9] Bligaard T, N?rskov J K. Ligand effects in heterogeneous catalysis and electrochemistry[J]. Electrochimica Acta, 2007, 52(18): 5512-5516.

[10] Strasser P, Koh S, Anniyev T, et al. Lattice-strain control of the activity in dealloyed core-shell fuel cell catalysts[J]. Nature Chemistry, 2010, 2(6): 454-460.

[11] Wang D S, Li Y D. Bimetallic nanocrystals: Liquid-phase synthesis and catalytic applications[J] Advanced Materials, 2011, 23(9): 1044-1060.

[12] Zhang S, Shao Y Y, Yin G P, et al. Electrostatic self-assembly of a Pt-around-Au nanocomposite with high activity towards formic acid oxidation[J]. Angewandte Chemie International Edition, 2010, 49(12): 2211-2214.

[13] Li R S, Wei Z, Huang T, et al. Ultrasonic-assisted synthesis of Pd-nialloycatalysts supported on multi-walled carbon nanotubes for formic acid electrooxidation[J]. Electrochimica Acta, 2011, 56(19): 6860-6865.

[14] Kibler L A, El-Aziz A M, Hoyer R, et al. Tuning reaction rates by lateral strain in a palladium monolayer[J]. Angewandte Chemie International Edition, 2005, 44(14): 2080-2084.

[15] Oezaslan M, Heggen M, Strasser P. Size-dependent morphology of dealloyed bimetallic catalysts: Linking the nano to the macro scal[J]. Journal of the American Chemical Society, 2012, 134(1): 514-524.

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