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a,b
a,*
, Cun Li
a,*
a
Department of Chemistry, Nanjing Normal University, Nanjing 210097, PR China
Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, PR China
Received 3 July 2006; received in revised form 18 July 2006; accepted 24 July 2006
Available online 30 August 2006
Abstract
It was reported for the rst time that the carbon supported Pd (Pd/C) catalyst was prepared in the aqueous solution with NH4F and
H3BO3. The average size and the relative crystallinity of the Pd particles in the Pd/C catalyst prepared with this method are much lower
than that of the Pd/C catalyst prepared with general reduction method because PdCl2 can form the complex with NH4F. Therefore, the
electrocatalytic activity and stability of the Pd/C catalyst prepared with this method for the formic acid oxidation in the direct formic
acid fuel cell (DFAFC) are better than that of the Pd/C catalyst prepared with the general reduction method. This preparation method is
very simple. Therefore, it is hopeful to have a practical application in the catalyst preparation.
2006 Elsevier B.V. All rights reserved.
Keywords: Carbon supported Pd catalyst; Formic acid; Direct formic acid fuel cell
Recently, the advantages of DFAFC has being progressively recognized comparing with direct methanol fuel cell
(DMFC) [1]. For example, as a strong electrolyte, formic
acid can facilitate the proton transport within the anode
compartment [2]. It has two orders of magnitude smaller
crossover ux through a Naon membrane than methanol
and then as high as 20 M concentrated formic acid can be
used in the operation of DFAFC [3]. Thus, the power density of DFAFC can be higher than that of DMFC although
the energy density of methanol is higher than that of formic
acid.
In recent years, Ha et al. [13] investigated the Pd/C catalyst as the anodic catalyst for DFAFC and found that the
electrocatalytic activity of Pd for the formic acid oxidation
is better than that of Pt [4,5]. It was reported that when the
average size of the Pd particles is small, the electrocatalytic
activity of Pd catalyst for the formic acid oxidation is high
[6]. However, the average size of the Pd particles in the Pd/
*
1388-2481/$ - see front matter 2006 Elsevier B.V. All rights reserved.
doi:10.1016/j.elecom.2006.07.033
Intensity (a.u.)
1626
a
0
20
40
60
80
2/( )
Fig. 2. The XRD patterns of: (a) the Pd/C-1 and (b) Pd/C-2 catalysts.
2.5
absorbance
2.0
1.5
1.0
0.5
0.0
200
300
400
500
wavelength/nm
Fig. 1. The UVvis absorption spectra of 1.8 104 M PdCl2 solution: (a)
before and (b) after adding NH4F + H3BO3.
a
6
b
I/mA.cm-2
10
I/mA.cm-2
1627
b
0
0
200
400
600
800
1000
t/s
Fig. 5. The chronoamperometric curves of 0.5 M HCOOH in 0.5 M
H2SO4 solution at: (a) the Pd/C-1 and (b) Pd/C-2 catalyst electrodes.
Fixed potential: 0.10 V.
2
0
-2
-0.2
0.0
0.2
0.4
0.6
0.8
E/V(vs.SCE)
Fig. 4. The cyclic voltammograms of 0.5 M HCOOH in 0.5 M H2SO4
solution at: (a) the Pd/C-1 and (b) Pd/C-2 catalyst electrodes.
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