Carbon Supported Pd-Fe Catalyst with Uniform Alloy Structure Prepared with Direct Thermo-decomposition Method for Oxygen Reduction Reaction

doi:10.15541/jim20150213

Abstract

Abstract:

The Pd₃-Fe₁/C catalyst was synthesized with the direct thermo-decomposition method using Pd(CH₃COO)₂ and Fe(CH₃COO)₂ as precursors. The Pd₃-Fe₁/C catalyst was characterized with X-ray diffraction(XRD), transmission electron microscope(TEM) and X-photoelectron spectroscope(XPS). The electrocatalytic performance of the Pd₃-Fe₁/C catalyst was investigated with the cyclic voltammetry and Linear scan voltammograms．The results show that Fe atom has entered into the Pd crystal lattice and formed a single-phase fcc disordered alloyed structure (solid solution). Electrochemical data indicate that the eletrocatalytic activity of the Pd₃-Fe₁/C electrocatalyst for oxygen reduction reaction (ORR) is much higher than that of Pd/C electrocatalyst.

Key words: direct thermo-decomposition, carbon supported Pt-Fe catalyst, uniform alloy, oxygen reduction

CLC Number:

O646

WANG Yan-En, WU Xiao-Jie, HE Cheng-Lei, ZHAO Jia-Ning, TANG Ya-Wen, LU Tian-Hong. Carbon Supported Pd-Fe Catalyst with Uniform Alloy Structure Prepared with Direct Thermo-decomposition Method for Oxygen Reduction Reaction[J]. Journal of Inorganic Materials, 2015, 30(12): 1315-1320.

Figures/Tables 8

Fig. 1 EDS patterns of (a) Pd/C and (b) Pd3-Fe1/C catalysts

Fig. 2 XRD patterns of (a) Pd/C and (b) Pd3-Fe1/C catalysts

Table 1 Structure parameters of Pd/C and Pd3-Fe1/C catalysts

Catalyst	Pd-Pd bond distance/nm	Lattice constant, α/nm	Crystalline size /nm	Atomic fraction of Fe in the Pd₃-Fe₁/C catalyst/%	Atomic fraction of alloying Fe/%	Electrochemical area/ (m²·g^-1)
Pd/C	0.277	0.391	3.51	0	0	44.51
Pd₃-Fe₁/C	0.274	0.387	2.54	25	24.63	52.79

Fig. 3 Pd3d XPS spectra of (a) Pd/C and (b) Pd3-Fe1/C catalysts

Table 2 Binding energy and relative intensities of Pd0 and PdII

Catalyst	Speciation	Binding energy of Pd3d_5/2/eV	Relative intensity/%
Pd/C	Pd⁰	335.26	51.1
Pd/C	Pd^II	336.90	48.9
Pd₃-Fe₁/C	Pd⁰	335.75	73.0
Pd₃-Fe₁/C	Pd^II	337.60	37.0

Fig.4 HRTEM and TEM images of the as-prepared catalysts and the catalysts EDS spectra. (a, b): HRTEM images of (a) Pd/C and (b) Pd3-Fe1/C catalysts; (c): TEM images of the Pd3-Fe1/C catalyst; (d): Overall EDS spectrum of large set of Pd3-Fe1/C particles in (c); (e): EDS spectrum of individual Pd3-Fe1/C particle

Fig. 5 Cyclic voltammograms of (a) Pd/C and (b) Pd3-Fe1/C catalyst electrodes in 0.5 mol/L HClO4 solution

Fig. 6 Linear sweep voltammograms of (a) Pd/C and (b) Pd3- Fe1/C catalyst electrodes in 0.5 mol/L HClO4 solution with saturated oxygen. Scan rate: 5 mV/s, Rotating speed: 2000 r/min

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