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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7

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Numerical optimization of bipolar plates and gas

diffusion electrodes for PBI-based PEM fuel cells

S.A. Grigoriev a,b,*, A.A. Kalinnikov b, N.V. Kuleshov a, P. Millet c

a
National Research University, Moscow Power Engineering Institute, Krasnokazarmennaya 14,
111250 Moscow, Russia
b
National Research Center, Kurchatov Institute, Kurchatov sq. 1, 123182 Moscow, Russia
c
Institut de Chimie Moléculaire et des Matériaux, UMR CNRS n
8182, Université Paris Sud 11, bât 410,
91405 Orsay Cedex, France

article info abstract

Article history: This paper is devoted to the numerical optimization of the geometry of some key cell
Received 14 June 2012 components (flow-field channels, current transfer ribs of bipolar plates, gas diffusion elec-
Received in revised form trodes) of high-temperature PEM fuel cells using H3PO4-doped Poly Benzimidazole (PBI) as
11 October 2012 solid polymer electrolyte. Some design specifications as well as optimum values of key
Accepted 4 December 2012 operating parameters are proposed to increase the efficiency of such fuel cells. For this
Available online 10 January 2013 purpose physicochemical model and corresponding novel effective technique for solving of
2D transport equation have been developed. Results of the numerical analysis of dependence
Keywords: of fuel cell performances upon the geometry of cathodic and anodic flow-field channels,
Fuel cell operating temperature and gas diffusion electrode parameters are provided. In particular, it
Proton-exchange membrane was demonstrated that optimum relative width of current-transfer rib (i.e. the ratio between
Poly benzimidazole width of rib divided to sum of widths of rib and channel) is determined mainly by compe-
Bipolar plate tition between diffusion and current conductivity in a gas diffusion electrode and is
Gas diffusion electrode approximately equal to 0.30e0.35 for the parameters of cell components used in this study.
Mathematical modeling Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
reserved.

1. Introduction - negligibly low electro-osmotic water transport by protons;

The modeling of a fuel cell that uses Poly BenzImidazole
(PBI) doped with orthophosphoric acid (PBI$xH3PO4) as solid
polymer electrolyte requires to take into account a number
of specific characteristics of these materials. The main
differences between PBI$xH3PO4 and more conventional
fluoropolymer (such as Nafion) solid polymer electrolyte
are:
- lower proton conductivity;
- significantly lower exchange current density of electro-
chemical reactions on electrolyteecatalyst interfaces;
- higher gas permeability.
Therefore, at first sight, the modeling of H2/O2 fuel cells
with high-temperature polymer electrolyte PBI$xH3PO4 is
easier because:
- there is no liquid water and no need to consider two-phase
(liquidegas) flows;
- there is no electro-osmotic water transfer across the
membrane during operation.
According to the literature, several research groups have
already developed mathematical models for such fuel cells. For

* Corresponding author. National Research University, Moscow Power Engineering Institute, Krasnokazarmennaya 14, 111250 Moscow,
Russia. Tel./fax: þ7 495 362 76 94.
E-mail address: S.Grigoriev@hepti.kiae.ru (S.A. Grigoriev).
0360-3199/$ e see front matter Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijhydene.2012.12.021
8558 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7
Nomenclature
1
F Faraday constant, 96,487 C mol
R universal gas constant, 8.314 J mol1 K1
P pressure, Pa
T temperature, K
t temperature,
C
C gas component concentration, mol m3
N flow vector, mol m2 s
K gas permeability, mol m1 Pa s1
D diffusion factor, m2 s1
h overpotential, V
4 potential, V
r resistivity, U m
I current density, A cm2
j flow potential, mol m1 s
G(x, y, x) Green’s function
3 porosity
Indexes
H hydrogen
w water
O oxygen
N nitrogen
example, a dynamic one-dimensional isothermal model has
been developed by Cheddie and Munroe [1] in order to account
for both stationary and transient modes of fuel cell operation. A
more sophisticated three-dimension model of a PBI PEM fuel
cell has been described in Ref. [2]. This model takes into
account all transfer and polarization phenomena, and model
results have been compared with published experimental data
obtained under similar conditions of operation. This model can
predict the oxygen depletion effect which is known to occur in
the catalyst area under the bipolar plate ribs. Another model
that predicts polarization characteristic of PBI PEM fuel cell has
been reported in Ref. [3]. This model allows to take into account
the effects of porous medium cell components and their effect
during fuel cell operation. Another one-dimension model
describing polarization characteristic of a PBI fuel cell has been
described in Ref. [4]. Ref. [5] is devoted to the development of
two-phase model of PBI-based PEM fuel cell. It takes into
account all transfer and polarization phenomena that occur
during the operation of the fuel cell and numerically examined
convective and diffusive fuel transports. In Ref. [6], a one-
dimension mathematical model is used to optimize the gas
diffusion electrode parameters (permeability, porosity, hydro-
phobicity). Ref. [7] describes a mathematical model that can be
used to predict the behavior of polarization curves. This model
is suitable for fuel cells where reactants and water product are
in gas or steam phases. The influence of electrode kinetics is
taken into account by using ButlereVolmer charge transfer
equations, ohmic losses and also mass transfer influence on
kinetics and thermodynamics with catalytic layers covered by
electrolyte film. In Ref. [8], it is shown how a pseudo-two-
dimension model can be used to model high-temperature
PEM fuel cell. In particular, the transfer of gaseous reactants
through the membrane is described. In Ref. [9], a two-
dimension model of mass transfer in high-temperature fuel
g gas diffusion electrode
c cathode
a anode
m membrane
bp bipolar plate
cc cathode catalytic layer
Main parameters of anodic and cathodic gas channels
Relative humidity 0%
Main parameters of cathodic and anode gas diffusion electrode [23]
Thickness, hcg 100 or 200 mm
Porosity, 3 cg 0.7
Specific electric resistance longitudinal, rgx ¼ 0.25 mU m2;
transversal, rgy ¼ 5 mU m2
Main parameters of cathodic catalytic layer
Specific content of platinum mc ¼ 1 mg cm2
Porosity 3 0 ¼ 0.5
Equilibrium cathodic potential 3 eq ¼ 1.11 V
Mass fraction of platinum in catalyst Xcm ¼ 0.4
Active specific surface of catalyst Ssp ¼ 30 m2 g1
Main membrane parameters
Thickness hm ¼ 30 mm
cell with linear flow channels is described. Results show that
convection can have a strong influence on reactant transport to
the anode even when such linear flow channels are used. In
Ref. [10], a dynamic two-dimension nonisothermal model is
described. It is used to calculate average temperature in the
PEM fuel cell and this in turn allows the definition of charac-
teristics of double electrode layers. In Ref. [11], a two-dimension
model that takes into consideration membrane consisting of
gas-intake channels and electrocatalytic layers is described.
Main transfer phenomena are taken into account except
crossing particles through the membrane. Results of this model
have been supported by experimental data and have been used
to analyze the influence of catalytic layer’s properties on fuel
cell operation. In Ref. [12], an advanced two-dimension model
is described. It has been developed for studying the dependence
of fuel cells characteristics on membrane structure and oper-
ating temperature. The purpose of the present work is to report
on the optimization of the geometry of some key cell compo-
nents (widths of flow channels and current transfer ribs of
bipolar plates, thickness of gas diffusion electrode) of these
high-temperature PEM fuel cells using H3PO4-doped Poly
Benzimidazole (PBI) as solid polymer electrolyte, and evaluate
their impact on mass and charge transfers.
2. Mathematical model
A schematic diagram of the model fuel cell showing the
different cell components is provided in Fig. 1. Individual
contributions of the different cell components to the overall
fuel cell behavior are calculated separately. The different cell
components with common boundaries are inter-connected
using appropriate boundary (continuity) conditions. The
following assumptions have been made in the calculations:
 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7 8559

 2
y m
a 2b 8 D ¼ KRT ; (3)
z
s
1 where R ¼ 8.315 m3 Pa mol1 K1 is the constant of perfect gas.
x
3 The temperature dependence of proton conductivity in PBI
Cwc0 CNc0 COc0 membranes usually takes the form:
hbp 6


B
sðTÞT ¼ A exp  : (4)
hcg Cwcg, CNcg, COcg NOсg 5 T
Nwcg

hm Nwm
7
Cwm In Eq. (4), the pre-exponential factor (A) and the activation
hag Cwac,CHac NHag 4 energy (B) both depend on humidity level and phosphoric acid
Nwag
g content (doping x in %). When x ¼ 6 (a usual value), the pre-
Cwa, CHa 2
hbp exponential factor A and activation energy B can be approxi-
mated by:
8

a 2b J S
B ¼ 33; 200  16; 000$RH ; A ¼ expð11:4  1:5$RHÞ : (5)
mol cm K

Fig. 1 e Schematic diagram of the PBI-based fuel cell. 1 e The measurement of electro-osmotic drag of water across
cathodic gas channel; 2 e anodic gas channel; 3 e cathodic PBI$xH3PO4 membranes has been thoroughly investigated in
gas diffusion electrode; 4 e anodic gas diffusion electrode; Ref. [22]. The electro-osmotic transfer coefficient and the
5 e membrane; 6 e cathodic catalytic layer; 7 e anodic associated hydrogen crossover current were found to be
catalytic layer; 8 e bipolar plates. almost equal to zero and were therefore neglected in our
work.
1. main processes (mass transfer, momentum transfer, and The ButlereVolmer equations used to describe the charge
flows of gas mixtures) take place at constant and homo- transfer kinetics in anodic and cathodic layers are:
geneous temperature;     
aRda F aOxa F
2. limitations due to mass and charge transfer in the anodic ia ¼ i0a exp  ðha Þ  exp ðha Þ ; (6)
RT RT
catalytic layer (H2 oxidation) are neglected due to high
kinetics (the oxygen reduction reaction at the cathode is     
aRdc F aOxc F
considered to be rate-determining); ic ¼ i0c exp  ðhc Þ  exp ðhc Þ ; (7)
RT RT
3. the electronic resistivity of both cathodic and anodic elec-
trocatalytic layers is negligible; where indexes a and c are making reference to anode and
4. cathodic and anodic catalytic layers are usually very thin cathode respectively; a is the charge transfer coefficient; i0 is
and transfer processes in these layers are considered as the exchange current density per unit of active platinum
one-dimension processes only. area.
It is shown in Ref. [17] that a value a ¼ 0.73 is appropriate to
The model takes into account the main membrane account for experimental results but following Ref. [18],
parameters. Values of hydrogen and oxygen permeability with a value a ¼ 0.5 has been used in this work.
operating temperature have been approximated from the data Following to Ref. [18], it is assumed that aRd ¼ aOx for anode
provided in Ref. [13]: and cathode.

8


> 12 3172 mol cm 10 3172 mol m
>
< KH ¼ 4:18$10 exp  ¼ 4:18$10 exp  ;
T cm2 Pa s T m2 Pa s


 (1)
>
>
: KO ¼ 1:07$1012 exp 3213 mol cm ¼ 1:07$1010 exp 3213 mol m ;
T cm2 Pa s T m2 Pa s

where KH and KO are the hydrogen and oxygen permeabilities The exchange current density has been calculated using [19]:
across PBI$6H3PO4 membrane respectively.
g 

The permeability of water vapor KW depending on Ci EC T
i0 ¼ i0ref aPteff exp  1 ; (8)
Ciref RT Tref
temperature T and doping degree s has been estimated from
the data of Refs. [14,15]: where i0ref is the exchange current density measured at the

 reference temperature Tref and for the reference concentra-
3172 mol m
KW ¼ 3:2$109 exp   4:7$ð6  sÞ : (2) tion of reactant Ciref; Ci is the concentration of reactant at the
T m2 Pa s
catalytic layer surface.
Diffusion factors D related with permeability K is deter- For PBI$6H3PO4 membrane when the operating temperature
mined by relation: is 150
C and the relative humidity 10%, the oxygen solubility
8560 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7

coefficient (Henri coefficient) H ¼ 6.8  106 mol m3 Pa1 and electrode conductivity in various directions is taken into
slightly depends on temperature. The Henri coefficient is twice account:
larger for hydrogen. Thus, the Ci concentration is obtained from
1 v 4g 1 v 4g
2 2
the partial pressure Pi: þ ¼ 0; 0  x  a þ b; 0  y  hg : (10)
rgx vx2 rgy vy2
Ci ¼ H$Pi ;
aPteff is the specific platinum surface per unit volume of Boundary conditions at x ¼ 0, a þ b are determined from task
catalytic layer; its value is obtained from aPteff ¼ (mPt/hc)SPt, symmetry:
where mPt is the weight of platinum per unit of catalytic layer v4g
surface, hc is the thickness of the catalytic layer, SPt is the x ¼ 0; a þ b; ¼ 0: (11)
vx
value of active surface per unit of mass. On the boundary with gas channel at y ¼ hg there is no
In this work, a cathodic exchange current density normal component of the vector current. On the boundary
i0ref ¼ 2.63$108 A cm2 (CrefO ¼ 0.107 mol m3, Tref ¼ 150
C) with gas diffusion electrode rib potential defined by the output
has been used in the calculation [16]. voltage of the fuel cell with account of the ohmic losses on the
The reaction order g is supposed to be close to unity for the collector current rib:
cathodic reaction [20]. An activation energy EC ¼ 72.4 kJ mol1 8
>
> a þ b

and g ¼ 1 have been used [21]. >

< a < x  a þ b; 4g ¼ 4out þ rbp hbp þ hcr IS ;
a (12)
> v4g
>
2.1. Potential distribution in catalytic layers : 0  x  a;
>
vy
¼ 0:

Here rbp((a þ b)/a)(hbp þ hcr)IS is the potential loss due to

Models of agglomerate catalytic layers are commonly used
resistance of bipolar plate rib and the contact resistance
to model PBI fuel cells. They rely on the assumption that
between the rib and gas diffusion electrode, presented as
catalyst particles (platinum on carbon carrier) are clustered
rbp((a þ b)/a)hcrIS.
into small spherical agglomerates which are limited in size
At the interface between the catalytic layer ( y ¼ 0) is
and filled with polymeric electrolyte. The gas reactant
necessary condition for the preservation of the normal
(hydrogen or oxygen) arriving through the pores of catalytic
components of the current vector:
layers then dissolves in the electrolyte phase and diffuses to
the reaction centers. Agglomerate models provide the best 1 v4g
¼ IðxÞ: (13)
way to account for experimental data as far as catalytic rgy vy
layers with polymeric electrolyte of Nafion type are con-
Similarly, for the boundary conditions for the anode gas
cerned. However, this “agglomerate approach” is useless for
diffusion electrode at y ¼ hg:
catalytic layers based on PBI$xH3PO4 for the following 8
>
reasons: > a < x  a þ b; v4g ¼ 0;
>
<
vy (14)
1. gas permeability of PBI$xH3PO4 at usual operating temper- >
> a þ b

>
: 0  x  a; 4g ¼ rbp hbp þ hcr IS ;
atures is almost twice higher than gas permeability of a
Nafion type polymer electrolyte; at y ¼ 0:
2. the exchange current density at the platinum/PBI$xH3PO4
1 v4gc
interface is almost three orders of magnitude lower than at ¼ IðxÞ: (15)
rgy vy
the platinum/Nafion interface (although this effect is
partially compensated by a larger solubility of hydrogen Equation of potential distribution in the cathode catalytic
and oxygen in PBI$xH3PO4). layer is solvable with known current density I(x). At the
interface between the catalytic layer ( y ¼ 0) it is needed to add
For these reasons, the concentration distribution of active the condition of sewing potentials:
gases inside agglomerates is almost homogeneous and this is
4gc ðx; 0Þ  4ga ðx; 0Þ ¼ 3 eq  hðx; 0Þ  IðxÞRm ðxÞ: (16)
why application of homogeneous models for catalytic layers
of high-temperature fuel cell is more appropriate. The use of condition (16) allows determining the current
Overpotentials distribution in cathodic catalytic layer is density in the iterative process.
described taking into account the accepted assumptions as
follows:
2.3. Membrane
8
>
> 2
d h
>
>
< 2 ¼ rp iC ðhÞ; Only diffusion of water is considered in the membrane according
dy  (9)
>
> dh dh
to our assumptions. Stationary distribution of water concen-
>
> ¼ 0; ¼ rp I x ; 0  y  hcc :
: dyy¼0 
dy y¼hcc tration inside the membrane is described by diffusion equation
and it could be expressed by the following first order equation:

2.2. Gas diffusion electrodes dCw IðxÞ

Dwm ¼ const ¼ Nwm ¼ qwm ;
dy F
(17)
Potentials distribution of in cathodic gas diffusion electrode is y ¼ 0; Cw ¼ Cwgc ;
described by the Laplace equation where heterogeneity of y ¼ hm ; Cw ¼ Cwga ;
 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7 8561

where Cw is the concentration of water vapor for equilibrium And system (21) must be supplemented by equation of flow
content of water inside the membrane; Dwm is the effective conservation:
value of diffusion coefficient of water inside the membrane;
VNH ¼ 0: (24)
qwm is the value of water vapor flow through membrane
expressed in A m2 s1; Cwgc and Cwga are the concentrations Value of fluxes N in (23) and (24) can be expressed in terms
of water vapor at the interface of the membrane and the of the corresponding scalar potentials j. The expression for
cathodic and anodic catalytic layers. the flow through the potentials:
The solution to Eq. (16) is:
Nigj ¼ Vjigj ; i ¼ fH; w; Og; j ¼ fa; cg: (25)
y

Cw ¼ Cwgc þ Cwga  Cwgc ;

hm And for components of vector N:
(18)

FDwm
qwm ¼ Cwgc  Cwga : 8
IðxÞhm >
> vjigj
>
< Nigjx ¼ vx
Ohmic resistance Rm can be obtained directly from the ; i ¼ fH; w; Og; j ¼ fa; cg: (26)
spatial distribution of water concentration (18): > N ¼ vjigj
>
>
: igjy
vy
Z
Cwgc

Cw Substituting (26) into equation (25) we can get Laplace equa-
Rm ¼ hm rm dCw ; (19)
Cwsat tion for flow potentials:
Cwgc

where rm(Cw/Cwsat) is the resistivity of high-temperature v2 jigj v2 jigj

Djigj ¼ þ ¼ 0; i ¼ fH; w; Og; j ¼ fa; cg: (27)
polymer electrolyte depending on relative humidity. vx2 vy2

Solutions of equation (27) determine the distribution of the

2.4. Conservation equations for momentum, components flows for given boundary conditions. Flow
concentration and flow components distribution is determined only by the boundary conditions
and the geometry of the boundary and does not depend on the
Transport of the gas-phase components is described by Ste- parameters of the gas diffusion electrode.
faneMaxwell equations. It is taken into account in steady- Boundary conditions for all potentials j and the flow vector
state transport equations that the nitrogen flow in the elec- N in the cross section of membrane-electrode assembly have
trodes is absent. StefaneMaxwell equations for cathode gas a standard form:
diffusion electrode are as follows: 8
>
> vj
8
 >
> y ¼ 0; 0  x  a þ b; Ny ¼ FðxÞ; ¼ FðxÞ;
>
Cw NO  CO Nw Cg  Cw  CO >
> vy
>
> >
>
< 3 g Cg VCw ¼ s 3 g  Nw ; >
>


DwO DwN
 >
> vj
>
CO Nw  Cw NO Cg  Cw  CO
(20) < 0  y  hg ; x ¼ 0; a þ b; Nx ¼ 0; ¼ 0;
>
> 3 g Cg VCO ¼ s 3 g  NO ; vx
: t (28)
DwO DwN >
> vj
>
> y ¼ hg ; 0  x  a; Ny ¼ 0; ¼ 0;
>
> vy
And for anode gas diffusion electrode: >
>
>
> vj
8 >
>
>

 : y ¼ hg ; a  x  a þ b; Nx ¼ 0; vx ¼ 0:
<
Cw NH  CH Nw
3 g Cg VCw 3g¼s ;
DwH (21)
>
: Cg ¼ CH þ Cw ; Thus, the boundary conditions for all flows differ only by
the function F(x), which is the flow of the component at y ¼ 0
where Dij are coefficients of mutual diffusion for components (catalytic layer). This fact allows the use of a universal Green
‘i’ and ‘j’; s(3 g) is diagonal tortuosity tensor, which expresses function G(x, y, x), which is defined as follows:
the dependence of the effective diffusion coefficient of gas 8
>
> v2 Gðx; y; xÞ v2 Gðx; y; xÞ
from the parameters of the porous medium, in accordance >
> þ ¼ 0;
>
> vx2 vy2
with the Bruggeman correction Deff ¼ D3 s1: >
>
>
>
>
> vGðx; y; xÞ
0 1 >
> y ¼ 0; 0  x  a þ b; ¼ dðx  xÞ;
>
> vy
1 0 >
>
sð3 Þ ¼ @ 0 1 pffiffiffi A: (22) <
= 3 vGðx; y; xÞ (29)
> 0  y  hg ; x ¼ 0; a þ b; ¼ 0;
>
> vx
>
>
>
> vGðx; y; xÞ
Tortuosity tensor takes into account that permeability of >
> y ¼ hg ; 0  x  a; ¼ 0;
>
> vy
gas diffusion electrodes (Sigracet carbon paper) in the direc- >
>
>
>
>
> vGðx; y; xÞ
tion parallel to the surface is higher than in perpendicular >
: y ¼ hg ; a  x  a þ b; ¼ 0:
direction, it is assumed that the gas flow is parallel to the vx
surface in straight channels. If the function G(x, y, x) is known, the potential j(x, y) can be
The system of equation (20) must be supplemented by the calculated by simple integration:
conservation equations of flows:
Zaþb

VNw ¼ 0; jðx; yÞ ¼ FðxÞ$Gðx; y; xÞdx: (30)
(23)
VNO ¼ 0: 0
8562 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7

Use of function G(x, y, x) can significantly simplify the task For concentrations of gaseous components, which are
solution as a whole due to the following factors: determined by the equations of the first order (31), only one
boundary condition at y ¼ hg, a < x < (a þ b):
1. At each iteration step at task solving as a whole is not neces-

sary to determine the flows solved a new two-dimensional Cw ¼ Cw0 ;
y ¼ hg ; a < x < a þ b; (34)
problem. Everything reduces to the calculation of the CO ¼ CO0 :
integral (30). Functions F0(x) and FH(x) defined as the value of flows on the
2. If the values of potential flows are known, then the two- boundary with the anode catalyst layer can be expressed as
dimensional problem of determining the gas component follows:
concentrations is reduced to ordinary differential equations.
In this case, the diffusion equation, expressed in terms of 8

>
>
IðxÞ 1
the potentials of the total mass flow j0 ðN0 ¼ Nw þ NO ¼ Vj0 Þ < F0 x ¼  þ qwm ;
F 2 (35)
and oxygen flow jO, in the cathode gas diffusion electrode > F x
¼ IðxÞ :
>
: H
are as follows: 2F

8


> vCw Cw Cg  Cw  CO vjO Cg  Cw  CO CO vj0
>
> 3 g Cg ¼ þ þ  ;
>
> vx DwO DwN vx DwN DwO vx
>
> 
 
>
>
>
> vCO Cw Cg  Cw  CO vjO CO vj0
>
< 3 g Cg vx ¼  DwO þ
>
DON vx
þ
DwO vx
;


  (31)
>
> vC 1 Cw Cg  Cw  CO vjO Cg  Cw  CO CO vj0
> 3 g Cg w ¼ pffiffiffiffiffi
> þ þ  ;
>
> vy 3g DwO DwN vy DwN DwO vy
>
>
>
>

>
> vC 1 Cw Cg  Cw  CO vjO CO vj0
>
: 3 g Cg O ¼ pffiffiffiffiffi þ þ :
vy 3 g DwO DON vy DwO vy

3. Green’s function is calculated in a similar way can be used For concentrations of gaseous components, which are
to calculate the diffusion processes in the anode gas determined by the equations of the first order (32), only one
diffusion electrode. In this case, the diffusion equation, boundary condition at y ¼ hg, a < x < a þ b:
expressed in terms of the potentials of the total mass flux j0 
Cw ¼ Cw0 ;
ðN0 ¼ Nw þ NH ¼ Vj0 Þ and hydrogen flow jH, in the anode y ¼ hg ; a < x < a þ b; (36)
CH ¼ CH0 :
gas diffusion electrode are as follows:
8
>
> vC C vjH CH vj0 3. Numerical procedures and algorithms
>
> 3 g Cg w ¼ w  ;
>
>
< vx DwH
vx DwH vx 
vCw 1 Cw vjH CH vj0 (32) System of transport equations was solved by the grid tech-
>
> 3 g Cg ¼ p ffiffiffiffi
ffi  ;
>
> vy 3 g DwH vy DwH vy nique. Approximation of the temporal and spatial derivatives is
>
>
: CH ¼ Cg  Cw :
carried out by quasi implicit method. Partition of the domain of
the physical parameters was carried out uniformly as follows:
4. Green’s function can be efficiently used for the calculation 8
>
> hx
of the transport processes in channels with the same >
< xi ¼ i; 0  i  Nx ;
geometry in different conditions. At such a calculation is nx
hy (37)
>
>
necessary to calculate the multiple two-dimensional > j
: y ¼ j; 0  j  Ny ;
ny
transport processes in different conditions. Using the
Green’s function eliminates the need to repeatedly calcu- where (nx þ 1), (ny þ 1) are the number of nodes in the x and y,
late the two-dimensional problems, and significantly respectively; xi, yj are the coordinates of the points; hx, hy are
increases the efficiency of such calculations. dimensions of the layers, hx for all areas is the same and equal
to (a þ b).
Function F0(x) and FO(x), defined as the value of flows on the The values of the physical parameters are defined directly
boundary with the cathode catalyst layer, expressed as follows: in the grid points xi, yj. The exceptions are the values of the
8
 components flow vectors N, which are defined in the points:
>
IðxÞ 1
>
< F0 x ¼
F 4
þ qwm ; 

>
IðxÞ
(33) Nxi;j ; xiþ1=2 ¼ ðxi þxiþ1 Þ=2; y .
i ;
>
: FO x ¼  ; (38)
4F Nyi;j ; / xi ; yjþ1=2 ¼ yj þ yjþ1 2 :

where I(x) is current density generated by the cathode catalyst Such a definition of the nodal points of components of the
layer at the point x; qwm is relative value of the water flow flow vector can achieve second-order accuracy in determining
through the membrane (Nwm ¼ qwm(I(x)/F )). the values of the physical parameters.
 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7 8563

3.1. Method of calculating the Green’s function Explicitly, the resulting system of linear equations as follows:

Green’s function defined by (29) was solved by the by relaxa-  !

k
tion method. For this we consider the system of equations i1 þ hiþ1
hkþ1 kþ1
2 1 dic hj
 hkþ1
þ þ
similar to (29): Dy2 i
Dy2 Dt dh

8  dic hkj
> hk
>
> vG0 ðx; y; x; tÞ v2 G0 ðx; y; x; tÞ v2 G0 ðx; y; x; tÞ ¼  i þ ic hkj  hkj : (45)
>
> ¼ þ ; Dt dh
>
> vt vx2 vy2
>
>
>
> 0
vG ðx; y; x; tÞ
>
> y ¼ 0; 0  x  a þ b; ¼ dðx  xÞ; On boundary ( j ¼ 0; y ¼ 0) and ( j ¼ Ny; y ¼ hc) the following
>
>
>
> vy
>
> 0 relations take place:
< 0  y  hgc ; x ¼ 0; a þ b vG ðx; y; x; tÞ ¼ 0;
>
vx (39) 
>
> vG0 ðx; y; x; tÞ i1 ¼ hiþ1 þ 2rp IS Dy;
i ¼ 0; hkþ1 kþ1
>
> y ¼ h ; 0  x  a; ¼ 0; (46)
>
>
gc
vy i ¼ ny ; hkþ1 ¼ hi1 :
kþ1
>
>
iþ1
>
> vGðx; y; x; tÞ
>
> y ¼ h ; a  x  a þ b; ¼ 0;
>
> gc
vx Stated grid problem is solved by the sweep method.
>
>
>
> t ¼ 0; G0
ðx; y; x; tÞ ¼ G ðx; y; xÞ; As a whole iteration converges, the diagonal elements of
>
>
0
: 0  i; k  nx ; 0  j  ny : the system (45) are larger than the sum of modules of its
diagonal elements.
This system differs from (29) by a dependency from fictitious
time t. It is assumed that:
3.3. Solution of potential distribution equation in gas
t/N; G0 ðx; y; x; tÞ/Gðx; y; xÞ: (40)
diffusion electrodes
Statement of the task (39) on set the grid implicitly as follows:

 Tasks of potential distribution in the cathode and anode gas
2 2 1  1
Glijk þ þ þ Gli1jk þ Gliþ1jk diffusion electrode (10)e(15) are solved by the relaxation
Dx2 Dy2 Dt Dx2
 1 (41) method. The corresponding grid problem is formulated as
l1 1
þ Gij1k þ Gijþ1k
l l
¼ Gijk : follows:
Dy2 Dt
!
2 2 1  1
On the boundaries the derivatives of the Green function are 4lij þ þ þ 4li1j þ 4liþ1j
approximated as follows: rgx Dx2 rgy Dy2 Dt rgx Dx2
(47)
8  1 4l1
ij
>
> Glijþ1k  Glij1k þ 4lij1 þ 4lijþ1 ¼ :
>
> j ¼ 0; 0  i  nx ; ¼ dik ; rgy Dy2 Dt
>
>
< 2Dy
0  j  ny ; i ¼ 0; nx ; Gi1jk ¼ Giþ1jk ;
l l
(42) On the boundaries derivatives of the potentials 4 for the
>
>
> j ¼ ny ; 0  i  nxa ; Glijþ1k ¼ Glij1k ;
>
>
> cathode gas diffusion electrode are approximated as
: j ¼ n ; n þ 1 < i  n ; Gl ¼ 0:
y xa x ijk follows:

Grid problem (41) and (42) was solved by the standard 8

> 1 4gcijþ1  4gcij1
l l
>
>
method of alternating directions. Problem must be solved nx >
> j ¼ 0; 0  i  nx ; ¼ Ili ;
>
> rgc 2Dy
times for different positions of the source on the x axis. >
>
>
< 0  j  n ; i ¼ 0; n ; 4kþ1 ¼ 4kþ1 ;
y x gci1j gciþ1j
(48)
>
> a þ b

3.2. Solution of potential distribution equation in >

>
>
> j ¼ ny ; 0  i  nxa ; 4lgcij ¼ Uout  rbp hbp þ hcr IlS ;
>
> a
cathode catalytic layer >
>
: j ¼ n ; n þ 1 < i  n ; 4kþ1 ¼ 4kþ1 :
y xa x gcijþ1 gcij1

Potential distribution equation (9) with the boundary condi-

tions was solved by the relaxation method on a uniform grid. Similarly, for the anode gas diffusion electrode:
For this we consider the system of equations similar to (9): 8
> 1 4gaijþ1  4gaij1
l l
>
>
8 >
> j ¼ 0; 0  i  nx ; ¼ Ili ;
> vh v2 h >
> rga 2Dy
>
> >
>
< ¼ 2  rp iC ðhÞ; >
< 0  j  n ; i ¼ 0; n ; 4l
vt  vx  (43) y x gai1j ¼ 4gaiþ1j ;
l
  (49)
> dh ¼ 0; dh
>
> ¼ rp I; hð0; xÞ ¼ h0 ; 0  x  hc ; t > 0: >
>
: dx dxx¼hc >
> a þ b
l
x¼0 >
> j ¼ ny ; 0  i  nxa ; 4gaij ¼ rbp a hbp þ hcr IS ;
l
>
>
>
>
Approximation of the temporal and spatial derivatives is : j ¼ n ; n þ 1 < i  n ; 4l ¼ 4l :
y xa x gaijþ1 gaij1
carried out by quasi implicit method. We used the Taylor
expansion of the nonlinear function ic(h) up to the first order of Grid problem (47)e(49) was solved by the method of alter-
accuracy. Thus, setting the grid problem is as follows: nating directions.

8 
>
> 1  kþ1  dic hkj 
< hj  hj
kþ1 k
¼ hjþ1  2hj þ hj1  ic hj 
kþ1 kþ1 k
hkþ1  hkj ;
> Dt r p Dy2 dh j (44)
>
:
0  j  ny :
8564 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7

3.4. Numerical determination of the volumetric dYi

¼ Fi ðY1 ; Y2 ; .; Yn Þ; i ¼ 1; 2; .; n; 0  x  hg : (54)
concentration of gas components in gas diffusion electrodes dx
In the cathode gas diffusion electrode Yi ¼ {Cw, CO}, in the
The system of equation (31) and a cathode (32) for the anode anode gas diffusion electrode Yi ¼ {CH}.
gas diffusion electrode is solved as described below. Equations The system of equations of the first order as (54) with the
are integrated as a system of ordinary differential equations. known boundary conditions can be integrated by a method of
For task solutions one boundary condition is needed. RungeeKutta.
Region, on which defines the transport equation is divided General diagram of the numerical solution of the set task is
into two parts, as shown in Fig. 2. Solution of the equations is shown in Fig. 3 and consists of the following stages:
carried out in two stages.
On a first stage the equations for cathode gas diffusion 1. Calculation of the Green’s function for the transport prob-
electrode are integrated: lems in the cathode and anode gas diffusion electrode.
8 

>
> vCw Cw Cg Cw CO vjO Green’s function does not change during the subsequent
>
>
1:5
3 g Cg ¼ þ
>
> vy DwO DwN vy iterations.
>
>
 
< Cg Cw CO CO vj0 2. Initial approximation of the current distribution I(x) and
þ  ; (50)
>
> DwN DwO vy concentrations.
>
> 
 
>
> vCO Cw Cg Cw CO vjO CO vj0 3. Carried out the integration of equation (9). Overvoltage
>
>
:3 1:5
g Cg ¼  þ þ ; distribution on the boundaries of the cathode catalyst layer
vy DwO DON vy DwO vy
is defined.
and equation for anode gas diffusion electrode is integrated:
4. Calculations of flows at the gas diffusion electrodes
vCH Cw vjH CH vj0 boundaries.
3 g Cg ¼  : (51) 5. Based on the known Green’s function potentials of flow in
vy DwH vy DwH vy
the volume of gas diffusion electrodes are calculated.
Direction of integration is along Y-axis to the direction from
6. System of equations for cathode (31) and anode (32) gas
the flow channel ( y ¼ hg) to the catalytic layer ( y ¼ 0). Initial
diffusion electrode is solved.
conditions for equations (50) and (51) are conditions on the
7. Calculations of the following approximation for the current
boundary of gas diffusion electrodes with flow channels.
distribution I(x) in the cathode catalyst layer according to
On the second stage equation for cathode gas diffusion
the iteration, based on the condition of sewing of potentials
electrode is integrated:
8

in the anodic and cathode regions (16):
>
> vCw Cw Cg Cw CO vjO h

i
>
<
3 g Cg
vx
¼
DwO
þ
DwN vx

I x ¼I x þa
3 eq  hðx; 0Þ þ 4gc x; 0  4ga x; 0
; (55)

 (52)
Rm ðxÞ
Cg Cw CO CO vj0
þ  ;
>
>
DwN DwO vx
>
: vCO


Cw Cg Cw CO vjO CO vj0
where a is iteration parameter (a < 1).
3 g Cg ¼ þ þ ; 8. Calculations of value of the numerical process error.
vx DwO DON vx DwO vx
Depending on the results computational process can be
and equation for anode gas diffusion electrode is integrated:

vCw Cw vjH CH vj0

3 g Cg ¼  : (53)
vx DwH vx DwH vx Calculation G(x,y,ξ)
Direction of integration is along the X direction from the edge
of the flow channel (x ¼ a) to the outer boundary of the domain
Initial approximation of
(x ¼ 0). The initial conditions for (52) and (53) are the solution of Exit
current distribution I(x) and
a similar equation (50) and (51) obtained in the first phase at concentrations
x ¼ a. Equations (50)e(53) have the general form:
Calculation of overvoltage
GAS CHANNEL distribution in cathode Calculation of errors
hg
catalytic layer
I
….

II
Calculation of flows Calculation of next
…. on gas diffusion approximation of I(x)
….
electrode boundaries
….

Y
0 Calculation of flow Calculation of concentration
0 a a+b potentials in gas distributions in gas diffusion
X diffusion electrode electrode

Fig. 2 e Direction of integration of transfer equation in gas Fig. 3 e General diagram of the numerical solution of the
diffusion electrodes. set task.
 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7 8565

completed, or the iteration progresses, there the value of

iteration a may be modified.

4. Results and discussion

A series of calculations aimed at optimizing main geometry

parameters of gas channels and current-carrying ribs by
averaging current densities at fixed exit voltage and different
values of operating temperature, pressure, thickness of gas
diffusion electrodes, have been carried out. Main results
(the relationship between current density and the relative
width of current-carrying rib of bipolar plate and full width of
channel þ current-carrying rib) are plotted in Figs. 4e8.
The calculation results of the spatial distribution of the
Fig. 5 e The dependence of average current density (A/cm2)
current density at the surface of the cathode catalytic layer
upon width of cathodic channel and relative width of
and the oxygen concentration in the cathode gas diffusion
current-carrying rib of the bipolar plate. Temperature
electrode (for temperature 160
C, 1 bar pressure, gas diffusion
T [ 140
C, pressure 1 bar, thickness of gas diffusion
electrode thickness 200 mm, a þ b ¼ 2 mm, a/(a þ b) ¼ 0.35) are
electrode 200 mm. 4out [ 0.5 V.
shown in Fig. 9. In order to demonstrate the influence of mass
transfer effects, the calculations were carried out at the
output voltage 4out ¼ 0.
Oxygen concentrations and current density are character- 2. for each aggregate width of channel and rib (a þ b), there
ized by a sharp kink at the current-carrying edge of bipolar exist a specific value of the relative width of current-
plate rib. Oxygen concentration varies significantly only under carrying rib a/(a þ b) for which the average current
the rib. The value of the longitudinal gas diffusion electrode density is maximum. The optimal value of a/(a þ b) at fixed
conductivity causes decreasing of the current density under aggregate width of channel and rib does not depend on
the flow channel. external operating condition and is approximately equal to
From these results, it can be concluded that: 0.3. An increase of the thickness of the gas diffusion elec-
trode will slightly decrease the optimal rib width. The
1. an increase of the rib width at fixed thickness of gas aggregate width of channel and rib has also an effect on the
diffusion electrode leads to slowing-down mass transfer value of the optimal relative width of current-carrying rib.
processes and decreasing average current densities. A The optimum relative width of the rib increases with an
decrease of the width of the current-carrying rib of the increase of channel width and reaches a value of 0.35 when
bipolar plates leads to increasing ohmic losses on the rib (a þ b) ¼ 5 mm.
itself and on the gas diffusion electrodes but improves the
transport of gases between catalytic layer and flow Such relationship could be explained by considering the
channels. ratio between longitudinal conductivity of gas diffusion

Fig. 4 e The dependence of average current density (A/cm2)
upon width of cathodic channel and relative width of
current-carrying rib of the bipolar plate. Temperature
T [ 160
C, pressure 1 bar, thickness of gas diffusion
electrode 200 mm. 4out [ 0.5 V.
Fig. 6 e The dependence of average current density (A/cm2)
upon width of cathodic channel and relative width of
current-carrying rib of the bipolar plate. Temperature
T [ 180
C, pressure 1 bar, thickness of gas diffusion
electrode 200 mm. 4out [ 0.5 V.
8566 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7
Fig. 7 e The dependence of average current density (A/cm2)
upon width of cathodic channel and relative width of
current-carrying rib of the bipolar plate. Temperature
T [ 160
C, pressure 3 bar, thickness of gas diffusion
electrode 200 mm. 4out [ 0.5 V.
electrode and rate of diffusion of oxygen and water vapor
under the bipolar plate’s rib. Thus, optimum width of current-
transfer rib is entirely determined by longitudinal conduc-
tivity of gas diffusion electrode and its gas porosity. It should
be noted that the properties of Sigracet gas diffusion elec-
trodes have been used in these calculations and that results
could be slightly different if different materials were used.
The optimum value of the current density increases with
increase of pressure, temperature and with decreases of gas
diffusion electrode thickness of overall channel width.
However, higher operating temperatures tend to reduce
significantly the lifetime of the membranes and higher oper-
ating pressures are expensive because of the energy required
for the compression of gases. The gas resistance of the cell can
significantly increase when the width of the channel is
Fig. 8 e The dependence of average current density (A/cm2)
upon width of cathodic channel and r elative width of
current-carrying rib of the bipolar plate. Temperature
T [ 160
C, pressure 1 bar, thickness of gas diffusion
electrode 100 mm. 4out [ 0.5 V.
Fig. 9 e Spatial distribution of relative volumetric
concentration of oxygen in cathode gas diffusion electrode
and current density distribution in cathode catalytic layer.
Temperature T [ 160
C, pressure 1 bar, gas diffusion
electrode thickness 200 mm. 4out [ 0 V.
reduced or when larger membrane-electrode assemblies are
used. Therefore, it is necessary to adjust channel width to the
electric power requirements.
In the current density range up to 1 A cm2, it is necessary
to increase operating temperature and pressure and to reduce
thickness of gas diffusion electrode in order to increase the
fuel cell output power. At high current densities (above
1 A cm2) and at maximum operating pressure, mass transfer
limitations begin to appear, and an increase in operating
temperature has a larger impact than an increase in operating
pressure.
From a more general viewpoint, the current density is
homogeneously distributed over the surface of the catalytic
layers. It can be concluded that the value of current density is
controlled by the two following major factors:
1. oxygen concentration changes have a limited effect and
only under current transfer ribs. In addition, when the
maximum pressure is applied, the current density still
increases when the oxygen concentration decreases; this is
due to a better humidity under current transfer rib and the
associated decrease of the specific resistance of the poly-
mer electrolyte.
2. longitudinal conductivity of the gas diffusion electrode.
This factor causes a decrease of current density below the
flow-field channel. The effect is more significant for the
minimum thickness of the gas diffusion electrode.
 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 8 ( 2 0 1 3 ) 8 5 5 7 e8 5 6 7
The distribution of concentration of gaseous components
has the following features:
1. oxygen concentration value changes sharply at the edge of
the current transfer rib of the bipolar plate.
2. in case of the complicated mass transfer conditions (thin
gas diffusion electrode and a wide rib) even at the 20%
humidity of air the partial pressure of water vapor will
exceed full pressure (because of at temperature 160e200
C
the pressure of saturated water vapor is 6e16 bar). Strong
limitations on an oxygen supply can be observed at
approaching to this critical point.
5. Conclusions
A physicochemical model of a PEM fuel cell cells using H3PO4-
doped Poly Benzimidazole (PBI) as solid polymer electrolyte
has been developed. Model calculations show that a special
correlation is required between cell component parameters to
obtain a maximum current density. In particular, the flow-
field design must be adapted to gas diffusion electrode
parameters. The model is used to propose optimum values for
operating parameters and some design requirements to opti-
mize fuel cell efficiency.
Acknowledgment
This work has been financially supported by the Ministry for
Education and Science of the Russian Federation within the
framework of the Federal Principal Scientific-Technical Program
“Scientific and Pedagogical Staff for Innovative Russia” for
2009e2013 (government contract no. 14.740.12.1359).
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