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Electrochemistry Communications 10 (2008) 4751


www.elsevier.com/locate/elecom

Contact resistance between gas diusion layer and catalyst


layer of PEM fuel cell
Iwao Nitta
a

a,*

, Olli Himanen b, Mikko Mikkola

Helsinki University of Technology, Laboratory of Advanced Energy Systems, P.O. Box 2200, 02015 TKK, Finland
b
VTT Technical Research Center of Finland, Fuel Cells, P.O. Box 1000, 02044 VTT, Finland
Received 10 September 2007; received in revised form 25 October 2007; accepted 27 October 2007
Available online 4 November 2007

Abstract
In this study, the electrical contact resistance between gas diusion layer (GDL) and catalyst layer (CL) on an electrolyte membrane
was experimentally evaluated as a function of compression. The contact resistances between the GDL and CL decreased nonlinearly as
the GDL thickness decreased due to the compression pressure. The values of the contact resistance between the GDL and CL were found
to be more than one order of magnitude larger than the contact resistance between the GDL and graphite, and even comparable to the
ionic resistance of the membrane. Because of the large value and variation in contact resistance between the GDL and CL, severe current
distribution may be created inside the cell. The results reported here should be highly useful in providing a more accurate picture of the
transport phenomena in a fuel cell.
2007 Elsevier B.V. All rights reserved.
Keywords: Inhomogeneous compression; Contact resistance; Gas diusion layer; Catalyst layer; PEM Fuel cell

1. Introduction
Polymer electrolyte membrane (PEM) fuel cell has
gained attention as a highly promising power source for
a wide range of applications because of its high eciency,
high energy density, quick start capability and environmentally friendly operation [14]. One of the most important
technological hurdles to overcome is the relatively poor life
time of the fuel cell stack. Of all the factors limiting the lifetime of PEM fuel cells, damage in membrane is of particular importance. This is especially the case when membranes
are becoming thinner, which is necessary for performance
improvement and cost reasons. Even minute damages in
such membranes, caused e.g. by local pressure or current
distributions and consequent local heat spots, could
become potential failure sites after a long operation period.
Therefore, detailed experimental assessments of the physi-

Corresponding author. Tel.: +358 9 451 3209; fax: +358 9 451 3195.
E-mail address: iwao.nitta@tkk. (I. Nitta).

1388-2481/$ - see front matter 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.elecom.2007.10.029

cal properties of fuel cell components, such as contact resistance, must be conducted and subsequently, modeling
mass, charge and heat transport in a fuel cell is necessary
to investigate the local phenomena and to predict overall
consequences.
Because of computational limitations and a lack of
experimental data, the geometric and modeling parameters
and operating conditions in the models are typically simplied or based on rough assumptions. These simplications
or assumptions may lead into underestimation of actual
phenomena occurring in the fuel cell, and as a consequence,
the modeled results may not reect real fuel cell conditions.
To the authors knowledge, only few experimental studies
on contact resistance between the gas diusion layer
(GDL) and catalyst layer (CL) have been carried out [5]
and it has been typically estimated roughly or simply overlooked in modeling studies [6,7]. This parameter, however,
may be a key factor to determine the current and temperature distribution inside the cell and needs to be investigated
in sucient detail. This is rstly because the value itself can
be substantially larger than the contact resistance at other

48

I. Nitta et al. / Electrochemistry Communications 10 (2008) 4751

interfaces since the CL contains electrically non-conductive


material and the roughness of GDL and CL are very dierent. And secondarily, signicant variation in the contact
resistance values over the cell area can exist because of
the rib/channel structure of the neighboring bipolar plate
as discussed in authors previous paper [8]. The purpose
of this paper, therefore, is to present a method for determining the contact resistance between the GDL and CL
as a function of compressed GDL thickness and to provide
reliable data for modelers.
2. Experimental
Experiments were based on AC impedance spectroscopy
in a symmetrical H2/H2 cell. The H2/H2 cell can be used to
study phenomena occurring in a PEM fuel cell, see e.g. [9
14]. In H2/H2 cell hydrogen is fed into both the anode and
cathode compartments. The anode and cathode reactions
of a H2/H2 cell are:
H2 ! 2H 2e anode
2H 2e ! H2 cathode

1
2

Since the electrochemical kinetics of the reaction in Eq.


(2) is substantially faster than that of the oxygen reduction reaction, the activation overpotential is small, which
makes the AC impedance measurement easier and helps
in obtaining accurate results. Furthermore, since the heat
production by the reaction in this system is smaller than
in PEM fuel cell systems, the H2/H2 cell can be assumed
isothermal. This is important because membrane properties such as water uptake and proton conductivity depend
on temperature [15,16]. Other advantage in the H2/H2 cell
is that because there is no water production in this system
the water content of the cell can be accurately controlled
by reactant humidication conditions. When membrane
parameters can be assumed constant the contact resistance between the GDL and CL can be calculated by
subtracting the membrane resistance and other bulk and
contact resistances from the measured total cell
resistance.

The schematic of the measurement system and the H2/


H2 cell employed in this study are illustrated in Fig. 1a
and b, respectively. The system was basically similar to
the one developed by Himanen et al. [14] with slight
modications.
The ow rates of hydrogen were kept at constant
20 ml min1 by mass ow controllers (Brooks 5850S).
Hydrogen was humidied in a commercial humidication
unit (Fuel Cell Technologies Inc.) before introduction into
the cell. The H2/H2 cell consisted of the cell body and two
cylindrical graphite current collectors (ISEM-3 grade,
Tanso Ab), between which the MEA (Gore Primea Series 5510) and circular GDLs (SGL SIGRACET GDL 10BA) with a diameter of 8.5 mm were placed. The current
collectors could move in the cell frame, allowing separation
of sealing pressure onto the gaskets and compression onto
the active cell area. The compression pressure was controlled using a pneumatic cylinder and pressure controller.
The same concept of cell structure is presented in more
detail by Ihonen et al. [17].
To achieve uniform compression on the GDLs and
MEA, the current collectors were not grooved, i.e. there
were no gas channels. Hydrogen entered the cell from the
inlet hole located in the center of the current collector,
spread radially from the center and exited through the outlet located at its outer edge. The cell temperature was set to
40 C and controlled using a West 6100 controller, four
heating elements (Watlow EB) inside the cell frame and
K-type thermocouples in the current collectors. The dew
point temperature of hydrogen was varied from 45 to
55 C to ensure that the membrane was fully hydrated.
The temperature of the gas pipes between the humidier
and the H2/H2 cell was always set to 5 C higher than the
dew point temperature to avoid water accumulation inside
the pipe. Potential probes were attached to the current
collectors.
Prior to the AC impedance measurement, the cell was
run in fuel cell mode to ensure gas tightness, and subsequently ushed with humidied nitrogen for 3 h to remove
oxygen and to achieve water equilibrium condition. The

b
H2 tank

compression pressure

out-flow
in-flow

cell body

GDL

PC

mass flow controller


gasket

PC

humidification unit

impedance
analyzer

MEA
H2/H2 cell

potentiostat

in-flow

current collector

out-flow

exhaust

compression pressure

Fig. 1. Schematic of measurement system: (a) whole system, and (b) enlarged H2/H2 cell.

I. Nitta et al. / Electrochemistry Communications 10 (2008) 4751

AC impedance spectra were recorded with an impedance


spectrum analyzer (Zahner IM6 Electrochemical Workstation) and potentiostat (Zahner PP240 Power Potentiostat)
by sweeping the frequency from 500 mHz to 20 kHz. The
measurements were conducted in galvanostatic mode with
20 mA amplitude and 0 mA DC-level. After the AC impedance spectra were obtained, the compression pressure onto
the active area was increased stepwise from 0.66 to
4.71 MPa and the same procedure was repeated. Recording
the impedance spectrum was repeated ve times for each
compression pressure.
3. Results and discussion
Fig. 2 shows typical examples of the spectra obtained
from the AC impedance measurement with various compression pressures onto the active area. The high frequency
arc is associated with the charge transfer across the catalyst
interface and the low frequency arc is attributed to both
adsorption and desorption of hydrogen on the electrode
surface and water transport in the membrane [911]. The
real axis intercept of the impedance spectrum at high frequency indicates the total cell resistance, Rcell. Only the
Rcell, which includes the bulk resistances of MEA, GDL
and graphite current collectors, and the contact resistances
between the components, is needed here. The detailed analysis of impedance behavior of the cell is beyond the scope
of this study and left for future work.
The measured impedance spectrum, as expected, shifted
to the left as higher compression pressure was applied, indicating a decrease of the Rcell. The measurements with dierent inlet hydrogen humidities showed that the membrane
was fully humidied and the measurements were repeatable
(see Fig. 2).
The compression pressure applied to the active area was
converted to the compressed GDL thickness, based on a

study of mechanical properties of the GDL [18]. The


obtained Rcell as a function of compressed GDL thickness
and compression pressure on the active area is illustrated in
Fig. 3. Fig. 3 also includes the negligibly small contact
resistance between the GDL and graphite current collector,
Rc(GDL/GR), and the bulk GDL resistance, Rb(GDL), which
were evaluated in a previous study [8], and the membrane
resistances Rm calculated as described below.
The Rcell decreased nonlinearly as the GDL was compressed. This was mainly due to the reduction of contact
resistances between the GDL and CL, Rc(GDL/CL). The
error estimate of Rcell was obtained by repeating the measurement and represents the 90% condence limit when
the applied compression pressure to the active area
exceeded 1 MPa. This error was small enough to warrant
a detailed analysis of the results. However, the error limits
were larger at the lowest compression pressure of
0.66 MPa, because Rcell was found to be fairly susceptible
to the assembling process when low compression pressures
were applied.
For the calculation of the Rm, the values of conductivity
for membrane humidied with water vapor, such as
reported by Cleghorn et al. [19], could not be used in this
study. This is because the water uptake of the membrane
from saturated water vapor and liquid water are signicantly dierent, see e.g. [20,21]. Severe ooding was
thought to occur in the cell since there was no ow eld
channel and humid hydrogen was used, and thus, the
MEA was at least partially in contact with liquid water.
Therefore, the membrane conductivity was calculated from
the assumed water content of the membrane, k. k is dened
as the number of water molecules per sulfonic acid group

(k = mol H2O/mol SO


3 H ) and can be calculated from
k

WU  EW
Mw

compression pressure on the active area (MPa)


4.71 3.93 3.32 2.82 2.27 1.72 1.11 0.66

-3

x10
4

0.16

* dew point temperature: 55 C


o
** dew ponint temperature: 45 C

Pressure (MPa)

0.14

resistance ( cm2)

1.72*
2.27*
2.82*
3.32*
3.93*
3.93**

Im(Z) ( cm2)

49

0.12

total cell resistance


contact resistance (GDL/GR) [8]
bulk resistance of GDL [8]
membrane resistance (WU: 20%)
membrane resistance (WU: 30%)

0.10
0.08
0.06
0.04

0.02
0

0
0.05

0.06

0.07

0.08

Re(Z) ( cm2)
Fig. 2. Impedance curves measured with compression pressure of 1.72
3.93 MPa on the active area.

150

200
250
300
compressed GDL thickness (m)

Fig. 3. Resistance as a function of compressed GDL thickness and


compression pressure on the active area.

I. Nitta et al. / Electrochemistry Communications 10 (2008) 4751

compression pressure on the active area (MPa)


4.71 3.93 3.32 2.82 2.27 1.72 1.11 0.66
0.06

70

0.05

60

0.04
50

0.03
0.02

40

0.01

30

ratio of 2*Rc(GDL/CL) to Rcell (%)

where WU is the water uptake of the membrane dened as


the mass of water in the membrane divided by the mass of
dry membrane (WU = Kg H2O/Kg dry membrane), EW is
the equivalent weight of the membrane dened as the
weight of membrane per mole of sulfonic acid groups

(EW = Kg membrane/mol SO


3 H ) and Mw is the molar
mass of water.
The published values of WU have considerable variation. The WU of 32% measured by Kolde et al. [22] may
be too high compared to the case in this measurement,
because their membrane was equilibrated with boiling
water, which lead to higher WU values than those when
the membrane was soaked in water at lower temperature
as reported by Springer et al. [23]. Another possible reason
for the high WU value measured in [22] is that they used
the plain membrane and not the MEA as in this study.
As observed by Matic et al. [12], water content in the membrane with CLs is highly uneven, which may yield substantially dierent WU values compared to the plain
membrane. This is because the CL is usually hydrophobized to enhance the water removal, and therefore, the measurement may give a lower value of WU for a membrane
with CL. On the other hand, the WU of 10% for the
MEA measured by Himanen et al. [14] was so small that
the calculated membrane resistance exceeded the total cell
resistance in Fig. 3. This was most probably due to the
inaccuracies in the measurement. Based on above review
of literature, the value of WU was assumed to be between
20 and 30%. Using these values of WU and the value of
EW given by the manufacturer, 1.1 kg mol1 [22], the k
was calculated to be between 12.2 and 18.3.
The membrane conductivity, rmem, which is a function
of the water content k and the temperature T can be calculated with the empirical equation for a Naon membrane
[23] with a correlation for the Gore membrane [24],


1
1

rmem 100 0:005139k  0:00326 exp 2222
303 T

contact resistance, Rc(GDL/CL) ( cm2)

50

0
150

200
250
compressed GDL thickness (m)

300

Fig. 4. Contact resistance between the GDL and CL, and ratio of two of
the contact resistance to total cell resistance.

1460 times larger than the Rc(GDL/GR) depending on the


compression. This is most probably due to the presence
of non-conductive material in the CL. Compared to a value
of Rc(GDL/CL) reported by Makharia et al. [5], the values
obtained here are more than 10 times larger. This is most
probably because they used a GDL coated with an MPL,
which reduces the Rc(GDL/CL), see e.g. [25].
Fig. 4 also includes the ratio of two of Rc(GDL/CL) to
Rcell. The Rc(GDL/CL) is the dominant part of the Rcell and
quite comparable to the Rm, especially when the small compression pressure was applied. Even with the very high
compression pressure which compressed the GDL to 40%
of the initial thickness, the Rc(GDL/CL) accounts for 35%
of the Rcell. These results indicate that the Rc(GDL/CL) cannot be neglected.
4. Summary and conclusion

4
Eq. (4) yields the rmem to be 7.5 and 11.5 S m1 with the
WU value of 20 and 30%, respectively. The area specic
resistance of membrane was then calculated with xed
thickness of membrane, 25 lm. The membrane swelling
due to water uptake was not considered here. Furthermore,
the Rm was assumed to independent of the compression
pressure. The area specic resistance of bulk CL and
graphite current collector was ascertained small enough
[8] and neglected.
The results for Rc(GDL/CL) which were obtained by subtraction of the Rc(GDL/GR), Rb(GDL) and Rm from the Rcell
are shown in Fig. 4. The error bars of the Rc(GDL/CL) were
calculated based on the error estimates of the measured
total cell resistances and the variation in the membrane
resistance calculated with two dierent WU values. The
Rc(GDL/CL) nonlinearly decreased as the GDL was compressed. The values of the Rc(GDL/CL) were found to be

The aim of this study was to provide an accurate modeling parameter for the contact resistance between the
GDL and CL, which has typically been ignored in previous
modeling studies. Using the H2/H2 cell and applying the
AC impedance method, the contact resistance between
the GDL and CL was evaluated as a function of compressed GDL thickness.
The evaluated values of contact resistance between the
GDL and CL changed nonlinearly from 0.044 to
0.0078 X cm2 when the GDL was compressed from 300
to 140 lm thickness, respectively. The important nding
of this study was that the contact resistance between the
GDL and CL was relatively large, an order of magnitude
larger than the contact resistance between the GDL and
graphite current collector and even comparable to the
membrane resistance. The contact resistance between the
GDL and CL, and membrane resistance form the dominant part of the cell resistance.

I. Nitta et al. / Electrochemistry Communications 10 (2008) 4751

The high value of the contact resistance between the


GDL and CL and its signicant variation with compression suggest that uneven compression pressure on the
active area of a fuel cell due to the rib/channel structure
of the ow eld plate may give rise to a notable current
density distribution. A modeling study which takes into
account the uneven compression pressure and pressuredependent material parameters may provide insight into
how local variation of compression aects the local transport phenomena and cell operation. Furthermore, measurements with an MPL coated GDL will be carried out
in the future.
Acknowledgement
The author gratefully acknowledges the nancial support from the Fortum foundation.
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