i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 6 ( 2 0 1 1 ) 1 0 3 7 6 e1 0 3 8 3

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The influence of permeability changes for a 7-serpentine

channel pem fuel cell performance

Elena Carcadea a,*, D.B. Ingham b, I. Stefanescu a, R. Ionete a, H. Ene c

a
National R & D Institute for Cryogenics & Isotopic Technologies, 240050 Rm.Valcea, Romania
b
University of Leeds, Centre for Computational Fluid Dynamics, LS2 9JT Leeds, UK
c
Institute of Mathematics of the Romanian Academy, 010702 Bucharest, Romania

article info abstract

Article history: The performance of a fuel cell is determined by several parameters, which describe the
Received 22 February 2010 fundamental, electrochemical and physical properties of the fuel cell layers, operational
Received in revised form conditions, geometry/structure of the flow field. One of these parameters is the perme-
27 July 2010 ability of the porous layers.
Accepted 16 September 2010 The paper presents results obtained for different cases in which we vary the permeability
Available online 9 October 2010 of the gas diffusion/catalyst layers of a 7-serpentine channel fuel cell. Simulations have
been carried out for permeability’s values 10
9 to 10
12 (m2), in order to investigate the
Keywords: influence of this parameter on the water formation and transport. Taking into account
Performance some results related to: water mass fraction distributions at the interface between the
Fuel cell anode/cathode and the membrane, water content, liquid water activity and current
Permeability density, we obtained a range for the optimum permeability (10
12 to 10
10). The main goal
Numerical simulation was to obtain an optimum value of the permeability that will lead to a uniform distribution
of reactant species and current density over the fuel cell active area.
Copyright ª 2010, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
reserved.

1. Introduction evaporation and condensation), or the interaction between

The operation of a PEM fuel cell depends on numerous
transport phenomena (charge-transport and multi-compo-
nent, multi-phase flow in porous media, heat and mass
transfer) and on the different physical properties or operating
parameters (permeability, porosity, relative humidity). To
incorporate all relevant phenomena that take place in the
various fuel cell components, the model must be three-
dimensional, non-isothermal, multi-component and multi-
phase. In addition, the model should take into account charge
transfer, change of phase, electrochemical reactions. This
results in a highly complicated model. The transport
processes then becomes significantly more complicated due
to the coupled flow of liquid water and gaseous reactants in
the porous media. The liquid water transport (capillary action,
the single- and two-phase zones effects on the gas transport/
distribution are topics that remain to be explored. In two-
phase porous systems, it is necessary to account for the effect
of the many different variables (e.g. structure of porous
matrix, fluid properties and pore blockage) can have on the
flow of each phase.
Recent studies indicate that the PEM fuel cell performance
may be strongly influenced by the permeability of the gas
diffusion layer (GDL). The permeability is a material property
that characterizes the resistance to the flow of gas exhibited
by the porous media. It is considered that the permeability of
the GDL components is an important parameter that must be
analyzed for understanding the relationship between the GDL
chemical and structural properties and its function in the PEM
fuel cell.

* Corresponding author. Fax: þ40250732746.

E-mail addresses: lili@icsi.ro, lilicarcadea@yahoo.com (E. Carcadea), D.B.Ingham@leeds.ac.uk (D.B. Ingham), Ene@imar.ro (H. Ene).
0360-3199/$ e see front matter Copyright ª 2010, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.ijhydene.2010.09.050
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 6 ( 2 0 1 1 ) 1 0 3 7 6 e1 0 3 8 3 10377

The relative permeability depends on the parameters, such

as: the structure of the porous media, the saturation of the
media (s), the surface tension of the fluid (s), the contact angle
of the fluid with the solid phase (qc), and the history of flow
through the media. Typically, when a parameter depends on so
many variables it is simplified to a more manageable expres-
sion which captures the most dominant interactions [1]. It has
become common practice in the porous media literature to
assume the relative permeability is a function of the saturation
only, and that is why the model used must describe the two-
phase flow in order to capture the formation, phase change and
transport of water, both in the liquid and gas phases.
In a recent review on gas diffusion layer characterization,
Mathias [2] considered that the permeability is a relevant
parameter in the fuel cell performance. The same parameter
was analyzed analytically by Feser [3] and numerically by
Pharaoh [4], particularly with respect to PEM fuel cells that
employ serpentine flow fields.
Values of the porous media permeability vary greatly in the Fig. 1 e Schematic of the bipolar plate and of fuel channel
modeling literature, spanning a few orders of magnitude, of the simulated PEM fuel cell.
from 10
19 m2 [5] to 10
6 m2 [6]. Experimental determination of
through-plane permeability is reported by Mathias [2] to be of
the order of 5e10  10
12 m2. Prasanna [7] report
1e8  10
11 m2 and show a significant decrease if the Teflon
loading of gas diffusion layer is increased. 2.1. Model equations
It is important to understand the link between the gas
diffusion layer permeability and the transport or reactants and Fuel cell operation is governed by the conservation of mass,
water (vapor and liquid) through this layer. There are many momentum, species and charge. Note that the Navier-Stokes
papers that considered the two phase flow modeling needed equations, the species and charge transport equations, and
for the prediction of the liquid water and for minimization of its the electrochemical equations applied are presented in our
detrimental effect on fuel cell performance. Nam and Kaviany previous work [9] and therefore are not repeated here. The
[8] have modeled the two-phase transport in the multi-layered present paper accounts for the liquid water transport and
cathode GDL using the unsaturated flow theory (UFT), which formation in order to determine the influence of the satura-
assumes a constant gas-phase pressure throughout, and tion for the relative permeability. Therefore, the equations
which therefore neglects the gas flow which is counter to the presented in this section simply describe the aspects related
liquid flow. The UFT theory was also used in this paper to to the two-phase flow in a PEM fuel cell.
account for a 7-serpentine channel PEM fuel cell performance Based on the above assumptions, the liquid water forma-
when we vary the permeability of the porous media. tion and transport is governed by the following conservation

2. Mathematical model e governing

equations Table 1 e Material properties and transport parameters.
Property Value
Using as a basis our one-phase model [9], a two-phase model
Hydrophobic GDL contact angle, c 100
that accounts for both the gas and liquid phases has been
Hydrophilic CL contact angle, c 70
developed. This model takes into consideration the phase Porosity of GCL 0.5
change inside the gas diffusion layer and this allows us to Porosity of CL 0.5
approximate the liquid water transport in the fuel cell.
Mass Flow (Kg/s)
The assumptions made in the two-phase model take into
Anode 1.5ee05
account the assumptions made in the single phase model plus Cathode 1.3ee04
the assumptions needed for implementing the phase change
Mass fraction of H2
of water:
Anode 0.9
Cathode 0
 the fuel cell operates under steady-state conditions
Mass fraction of H2O
 the flow in the channels is considered to be laminar
Anode 0.1
 the membrane is considered impermeable for the gas-phase Cathode 0.22
 the produced water is assumed to be in the liquid phase
Mass fraction of O2
 no other species exist in the liquid phase, i.e. it consists of
Anode 0
liquid water only
Cathode 0.25
 phase change occurs only within the porous electrodes.
10378 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 6 ( 2 0 1 1 ) 1 0 3 7 6 e1 0 3 8 3

Fig. 2 e Water mass fraction distribution at the interface between the anode CL and the membrane.

equation for the volume fraction of liquid water, s, or water It is assumed that the liquid velocity !
u l is equivalent to the
saturation [10]: gas velocity inside the gas channel. Inside the highly resistant
porous zones, the liquid-phase flux is expressed by Darcy’s
V$ðrl !
u l sÞ ¼ Sl (1) law using the relative permeability of the individual phases:
where the subscript l stands for liquid water, rl is the liquid
density, s is the saturation, !
u l is the liquid water velocity and ! Kkrl
ul ¼
Vpl (4)
the source term Sl is the condensation rate that is modeled ml
according to the following formula:
where krl represents the relative permeability of the liquid
   phase.
pwv
psat
Sl ¼ cr max ð1
sÞ Mw;H2 O ; ½
srl  (2) In this paper, the GDL is assumed to be isotropic and the
RT
relative permeability of each individual phase is proportional
This source term in not applied in the PEM fuel cell
to the cube of the phase saturation:
membrane, it is used just in the porous electrodes. The constant
condensation rate cr is given by the expression:cr ¼ 100s
1 .
Equation (2) models various physical processes related to krl ¼ s3 ; krg ¼ ð1
sÞ3 (5)
two-phase flow that can take place inside a fuel cell The unsaturated flow approximation involves a constant
(condensation, vaporization, capillary diffusion, and surface gas-phase pressure across the porous media, and thus the
tension). liquid pressure can be expressed by:
Many fuel cell models that account for two-phase transport
in the gas diffusion layer are based on the unsaturated flow pl ¼
pc þ pg ; Vpl ¼
Vpc ; (6)
theory (UFT). UFT entails an essential assumption, namely: the Thus, using the above equations for replacing the convec-
gas-phase pressure is constant across the porous medium; tive term in Eq. (1), we obtain:
therefore the liquid-phase pressure simply becomes the nega-
tive of capillary pressure between the gas and liquid phases:  
Ks3 dpc
V$ rl Vs ¼ Sl (7)
pc ¼ pg
pl (3) ml ds
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 6 ( 2 0 1 1 ) 1 0 3 7 6 e1 0 3 8 3 10379

Fig. 3 e Water mass fraction distribution at the interface between the cathode CL and the membrane.

The capillary pressure between the gas and liquid phases is where the saturation pressure can be computed as follows:
computed as a function of the saturation, s, by the formula:
log10 psat ¼
2:1794 þ 0:02953$ðT
273:15Þ
9:1837  10
5 ðT
 3 1=2
pc ¼ scosðqÞ JðsÞ (8)
273:15Þ2 þ1:4454  10
7 ðT
273:15Þ3 (12)
K
where the Leverett function, J(s), is given by: nd ¼ 0:0028$l þ 0:05l
3:5  10
19 (13)

JðsÞ ¼ 1:417ð1
sÞ
2:120ð1
sÞ2 þ1:263ð1
sÞ3 if q < 90 (9) nd $jk
1:417s
2:120s2 þ 1:263s3 if q > 90 a¼
Dw VCw (14)
F

In the formula (8), q is the contact angle of the gas diffusion where k is the anode or cathode, Dw and Cw are the water
layer and is dependent upon the hydrophilic ð0 < q < 90 Þ or diffusion coefficient and water concentration across the
hydrophobic ð90 < q < 180 Þ nature of the material used in the membrane, respectively.
GDL fabrication. The surface tensions, for the liquid water air The expressions for the water concentration and water
system is a constant, s ¼ 0:0625 N/m. diffusion coefficient from Eq. (14) are given by [12]:
Properties important in a two-phase flow study and taken rmodry
into consideration in this paper, such as the molar flux of Cwk ¼ lk (15)
Mmodry
water, a, and the osmotic drag coefficient, nd , are evaluated as
functions of the water content, l, and water activity, a. All  
1 1

these parameters are given by the expressions [11]: Dw ¼ Dl exp 2416

303 T
Dl ¼ 10
10 l < 2
(16)
pwv Dl ¼ 10
10 ð1 þ 2ðl
2ÞÞ2  l  3
a¼ þ 2s (10) Dl ¼ 10
10 ð3
1:67ðl
3ÞÞ3  l  4:5
psat
Dl ¼ 1:25  10
10 l  4:5

0:043 þ 17:18$a
39:85a2 þ 36:0a3 0 < a  1 where rm,dry is the dry membrane density, and Mm,dry is the
l¼ (11)
14 þ 1:4$ða
1Þ for 1  a  3 membrane equivalent weight.
10380 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 6 ( 2 0 1 1 ) 1 0 3 7 6 e1 0 3 8 3
Fig. 4 e Liquid water activity in the membrane.
3. Numerical algorithm
The CFD software Fluent was used for all the numerical
calculations performed, using appropriately specified
boundary conditions of the fuel cell under investigation in
order to analyze the fluid flow dynamics and fuel cell perfor-
mance. Thus, the solution to the governing partial differential
equations is uniquely determined.
The numerical simulation model is based on the SIMPLEC
(semi-implicit method for pressure linked equations consis-
tent) algorithm using a segregated solver in Fluent 6.3 [13]. The
source terms generated by the electrochemical reaction are
inserted in to the mass, momentum and species conservation
equations using a User Define Function (UDF) included in the
Fuel Cell Module. The coupled set of equations was solved
iteratively until the relative error in each field reached
a specific convergent standard (usually 10
8).
The geometry analyzed in this work has GDL, CL and MEA
width  length equal to 10 cm  10 cm and on the borders
there is a sponge rubber of size 1.52 cm (width)  1.52 cm
(length). The length of the flow path geometry is 49.17 cm for
each channel. The cross-sectional flow area is 1.5 cm
(height)  1.5 cm (width). The rib between two adjacent
channels is 1.3 cm (in the y-direction). The number of
computational cells used in the model was about 2.2 million
cells. The geometry analyzed in this paper will be also tested
experimentally and a schematic of the bipolar plate and of
fuel channel of the simulated PEM fuel cell is shown in Fig. 1.
Table 1 summarizes few material properties and transport
parameters used in the CFD calculations, which are assumed
based on the data that will be used in experiments. The
feeding gases has a relative humidity of 2.65% for hydrogen
at the anode side (fuel composition in mass fraction terms is
0.9/0.1 for H2/H2O) and 65% for air in the cathode side
(oxidant composition in mass fraction terms is 0.25/0.22/0.53
for O2/H2O/N2) and entered the cell at 80 Celsius. From Table
1, we can see that values for the mass flow rate and mass
fraction were prescribed at the inlet of both the anode and
cathode flow channels in order to solve the problem
described.
Regarding the boundary conditions for the outlets, since
the reactant gas flow channels are separate and generally
have different pressures then pressure boundary conditions
are used. The interfaces between the layers are interior faces,
and therefore no boundary conditions are prescribed. Dirich-
let boundary conditions with constant values are set for the
solid phase potential on the lateral sides of the fuel cell (0V to
the anode and 0.5V to the cathode side) and zero flux condi-
tions are applied at the inlet and outlet.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 6 ( 2 0 1 1 ) 1 0 3 7 6 e1 0 3 8 3
Fig. 5 e Water content at the interface anode/membrane.
4. Results and discussions
To investigate the effects on the cell performance of perme-
ability variations, we conducted numerical analyses based on
a two-phase flow study and four different permeability values
of the porous layers resulting in four cases, namely 10
12 (m2)
(case 1), 10
11 (m2) (case 2), 10
10 (m2) (case 3), and 10
9 (m2)
(case 4). In the cases considered we wanted to see the influ-
ence of this parameter for the water formation and transport,
for the uniformity of reactant species distribution and of
current density over the active area.
Figs. 2 and 3 present the distributions of the water mass
fraction at the interface between the anode catalyst layer and
the membrane, respectively and between cathode catalyst
layer and the membrane for the cases investigated. It can be
noticed that more water appears on the interface between the
anode and the membrane, and also a more uniform profile is
obtained for the case when the permeability of the porous
layers under investigation is smaller (10
12 m2 and 10
11 m2).
Liquid phase transport in a PEM fuel cell is believed to be
the most important process for removing water from fuel cell
cathodes. Liquid water must be prevented from accumulating
on the electrode surfaces, in the pores of the gas diffusion
layers, and in the gas channels. Liquid water in these regions
10381
obstructs the transport of reactants to the active catalyst sites
and thus reducing the performance. At the same time, liquid
water is important for the polymer membrane because it
maintains the hydration level needed for good conductivity
and hence for a better performance.
Fig. 4 presents the liquid water activity at the interface
between the anode and the membrane for the cases investi-
gated. It can be noticed that a large value for this coefficient
and a uniform profile is obtained for the cases with a smaller
permeability of the porous media, especially cases 2 and 3. A
lower permeability in the gas diffusion and catalyst layers
means that there will be more liquid water in the Nafion phase
(membrane) and this can lead to a performance improvement.
To achieve high performance, the amount of water content
in the PEMFC should be in a suitable range that is adequate to
hydrate the membrane but not disturb the transportation of
the reactant gas. The maximum value of the water content
obtained from the Eq. (11) is 16.8, the fully hydrated level,
a value essentially for a liquid equilibrated membrane. From
Fig. 5 we can notice that the maximum value of the water
content obtained for the cases simulated is 5.58, which cannot
be sufficient for a good hydrated membrane. In this case, it is
possible that the inlet gases should be humidified.
The performance characteristics of the fuel cell, based on
a certain parameter can be obtained by varying that
10382 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 6 ( 2 0 1 1 ) 1 0 3 7 6 e1 0 3 8 3
Fig. 6 e Calculated current density at various permeability
values of the porous layers.
parameter while keeping all other parameters constant.
Results obtained for the current density of the fuel cell when
we vary the permeability of the porous layers are presented in
the Fig. 6. The results obtained from these types of para-
metrical studies can allow us to identify the optimum
parameters for the fuel cell performance. From Fig. 6 and the
results presented above we can notice that using low perme-
ability values (10
12, 10
10), there is an increase in the
uniformity of the reactant species distribution and in the
current density over the active area, so the optimum value can
be considered in this range. Usually, low isotropic perme-
ability has a much grater effect on cell performance than
higher isotropic permeability, because the reactants and
water are eventually trapped in the porous media of gas
diffusion and catalyst layers with low permeability.
From Fig. 6 we can notice that the tendency for the average
current density values is to decrease with an increase in the
porous layers permeability, so we can conclude that is very
important to know the effect of different parameters on the
performance of fuel cell.
5. Conclusions
A three-dimensional, two-phase flow and transport model
has been used to simulate the multi-dimensional, multi-
phase flow and transport phenomena at both the anode and
cathode sides in the fuel cell and the cell performance with
different values for the permeability of the porous layers (gas
diffusion and catalyst layers). The simulations are presented
with the emphasis on obtaining physical insight and a better
fundamental understanding afforded by the detailed distri-
butions of the water mass fraction at the interface between
the anode/cathode catalyst layers and the membrane, liquid
water concentration, water content in the PEM, and average
current density as a function of permeability.
Our main goal was to obtain an optimum value of the
permeability of the porous layers in order to increase the
uniformity in the distribution of reactant species and current
density over the active area of the fuel cell. Taking into
account all these aspects, the conclusion that we can draw
from the simulated cases is that a range for an optimum
permeability was established (10
12e10
10).
The numerical simulations and results presented and
analyzed in this paper were obtained using the commercial
code Fluent 6.3 and the Fuel Cell Module 2.2.
This study is part of a parameter sensitivity investigation
of PEMFC models that aims to determine the relative impor-
tance of each parameter analyzed on the modeling results. In
this context, the parameter sensitivity means how the
parameters influence the global performance of a PEM fuel cell
represented by the polarization curve. Some key parameters
used in this type of study are, foe example, the parameters
that characterize the porous layers of the PEM fuel cell, like:
permeability, thermal conductivity, electrical conductivity or
porosity. Also, a comprehensive parameter sensitivity exam-
ination must be carrying out, the reason being the comparison
between the simulation and the future experimental results.
Two-phase flow in low-temperature PEM fuel cells is an
important research subject. Currently, this is still a largely
unexplored area and many issues are needed to be investi-
gated. A fundamental understanding of two-phase transport,
especially in porous gas diffusion layers of PEM fuel cells, is
essential in order to improve the overall performance of this
technology.
Nomenclature
a water vapor activity
S source terms
s volume fraction of liquid water
Greek Letters
4 phase potential, V
l water content of the membrane
a molar flux of water
Subscripts
k anode/cathode
sat saturation value
wv water vapour
c capillary
rl relative to liquid phase
rg relative to gas phase
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