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Improving Water Management and Performance of an Air-Cooled Fuel

Cell System Using Pressurized Air for Aviation Applications
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 Journal of The Electrochemical Society, 2021 168 084503

Improving Water Management and Performance of an Air-Cooled

Fuel Cell System Using Pressurized Air for Aviation Applications
Nammin Lee,1 Masoomeh Ghasemi,1 Bonghyun Kim,1 Seungbeen Choe,1 Kisung Lim,1 Seung
Woo Lee,2 Seung Soon Jang,3 and Hyunchul Ju1,z
1
Department of Mechanical Engineering, Inha University 100 Inha-ro Michuhol-Gu, Incheon 22212, Republic of Korea
2
Geroge W. Woodruff school of Mechanical Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0405,
United States of America
3
School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0245, United States
of America

Air-cooled fuel cell systems feature a light-weight and simple design and are thus recognized as a suitable technology for drone and
aviation applications. As compared to liquid-cooled fuel cell systems, however, they suffer from low specific power per unit
volume and unstable performance due to severe electrolyte dehydration and nonuniform profiles of current density and temperature
inside a fuel cell stack. Here, we present a high-pressure air-cooled fuel cell system in which atmospheric air is pre-compressed by
a compressor and then fed into the fuel cell stack. To minimize the compressor power consumption, the system is designed to
recirculate the exhaust air from the fuel cell stack. A three-dimensional two-phase fuel cell model is implemented with a high-
pressure air-cooled fuel cell system mainly consisting of an air-cooled fuel cell stack, compressor, air chamber and duct, and heat
exchanger and is used to predict superior fuel cell performances under various high-pressure conditions. Simulation results show
that the fuel cell operation at 2 atm allows an increase of up to two times the stack power and 1.5 times the net system power
compared to a 1-atm fuel cell operation.
© 2021 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited. This is an open access
article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/
by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. [DOI: 10.1149/
1945-7111/ac1704]

Manuscript submitted May 6, 2021; revised manuscript received June 30, 2021. Published August 4, 2021.

List of symbols z Transport resistance coefficient

Greek symbols
a Ratio of electrochemically active surface area of α Transfer coefficient
CL to CL volume, [m−1] γ Reaction order
aECSA Electrochemically active surface area of Pt, δ Component thickness, [m ]
[m2g−Pt1] ε Volume fraction
aPt Active volumetric surface area of Pt, [m−1] η Surface overpotential, [V ]
ac Volumetric surface area of ionomer, [m−1] κ Proton conductivity, [Sm−1]
A Area, [m2 ] ϕ Phase potential, [V ]
Ci Molar concentration of species, [mol m−3] ρ Density, [kgm−3]
D Species diffusivity, [m2 s−1] σ Electronic conductivity, [Sm−1]
E Activation energy, [kJ mol−1] τ Viscous shear stress, [Nm−2]
EW Equivalent weight of a dry membrane, [kg mol−1] ξ Stoichiometric flow ratio
F Faraday’s constant, 96,487 [C mol−1] Superscripts
i0 Exchange current density, [kJ mol−1] c Catalyst coverage coefficient
h fg Latent heat of vapor-water phase change, eff Effective
[kJ mol−1] g Gas
I Applied current density, [kJ mol−1] l Liquid
I/C Ionomer-to-carbon weight ratio Pt Platinum
j Transfer current density, [Am−3] ref Reference value
k Thermal conductivity, [Wm−1 K−1] Subscripts
K Hydraulic permeability, [m2 ] a Anode
LPt Pt loading, [mg cm−2 ] c Cathode, carbon
n Number of electrons transferred in the electrode CL Catalyst layer
reaction e Electrolyte
nPt Number of Pt particles on a carbon surface GC Gas channel
MW Molecular weight, [kg mol−1] GDL Gas diffusion layer
P Pressure, [Pa] H2 Hydrogen
r Particle radius, [m] i Species
R Universal gas constant, [8.314 J mol−1 K−1] in Channel inlet
s Liquid saturation mem Membrane
T Temperature, [K] O2 Oxygen
u⃗ Fluid velocity and superficial velocity in a porous s Solid, surface
medium, [ms−1] sp Set-point
T Temperature
u Momentum equation
w Water
0 Initial or standard conditions: T = 298.15 K; P =
z
E-mail: [email protected] 101.3 kPa (1 atm)
 Journal of The Electrochemical Society, 2021 168 084503

concentration overpotentials.11,12 The main concern with air-cooled

With the urgent need for efficient and clean power sources for PEMFCs is that their performance varies widely with operating
aviation applications such as drones and unmanned aerial vehicles conditions. Increasing the cathode air supply with the use of cooling
(UAVs), various technologies and strategies to develop convenient fans can mitigate the mass transport issue but can cause dry out of
power sources have been studied.1 During the past few decades, the membrane due to the high flow rate of ambient dry air.13
proton exchange membrane fuel cells (PEMFCs) have attracted New techniques are being sought to optimize performance by
much attention as efficient and clean alternatives to existing power understanding the internal workings of these devices.14 Recently, an
supplies. PEMFCs boast zero pollution, low operating temperatures, air-cooled PEMFC stack with an active area of 100 cm2 and 24 cells
fast response to load change, no limitation by the Carnot cycle, and was designed by Devrim et al.15 for a portable power generator. In
outstanding energy conversion efficiency.2–4 this system, PEMFC stack temperature was monitored and auto-
In terms of cooling methods of PEMFC stacks, PEMFCs can be matically adjusted during the operation using a blower equipped
categorized into circulating liquid-cooled and air-cooled PEMFC with an electronic on-off control setup. It was found that the PEMFC
stacks. In addition, phase change cooling is applied to special performance was significantly improved by reaching cell tempera-
PEMFC stacks, which is still under study and not widely used.5 ture up to 65 °C, which can be contributed to the increase in the gas
Currently, liquid cooling is employed in the majority of PEMFC diffusivity and membrane conductivity. However, the cell perfor-
stacks. Among all liquid-based cooling systems for PEMFCs, water mance was diminished by increasing operation temperature from
cooling is prevalently employed because water exhibits relatively 65 °C to 80 °C, due to reduction in the relative humidity of the
high thermal conductivity and high specific heat capacity than other reactant gases that decreases the water content in the membrane and
commonly available liquids at room temperature and atmospheric the membrane proton conductivity. In another study, three different
pressure.6 Therefore, better thermal conditions should be expected cooling plate designs for an air-cooled PEMFC stack were numeri-
with the use of water cooling for PEMFCs. However, a great amount cally and experimentally investigated. The cooling plate design,
of parasitic power could be consumed to ensure the circulation of which has larger cooling channels, was found to show a more
water coolant.7 uniform distribution of temperatures.16
Compared with water-cooled PEMFCs, air-cooled, and open- Recently, for a passive air-cooled fuel cell, it was numerically
cathode PEMFCs have been widely preferred for aviation applica- determined that using a thinner membrane and higher ionomer
tion, particularly in the range of up to a few kW, because they are fraction in the cathode catalyst layer (CL) can result in a lower ionic
characterized by simple system design, reduced weight, easy resistance, lower temperature rise along the cathode flow path, and
operation, low cost, increased gross efficiency, and less parasitic higher cell performance.17 Jang et al.18 investigated the impacts of
power failure.8,9 The fundamental aspect of open-cathode or air- the opening ratio of cathode flow fields on mass transfer and water
breathing is based on the utilization of ambient air and natural management capability of air-breathing PEMFCs. It was shown that
convection in the surrounding environment instead of a compressed the performance of a PEMFC was greatly enhanced through a higher
flow of oxidants or air past the cathodes. Nevertheless, the major opening ratio of the air flow field, a conclusion of which is in line
disadvantages of open-cathode or air-breathing PEMFCs are low with experimentally reported results.19 They concluded that a
maximum current densities, problems in extreme climate conditions, circular opening design yields the best performance and highest
and unstable performance.10 The cathode is usually the major source limiting current density. Adzakpa et al.20 employed a three-dimen-
of voltage loss as a result of the relatively weak mass transport sional fuel cell model to assess the dynamic thermal behaviors of an
mechanism of natural convection of air; this leads to significant air-cooled PEMFC stack that was designed to be cooled by air

Figure 1. Schematic illustration of a passive air-cooled PEMFC system using pressurized air.
 Journal of The Electrochemical Society, 2021 168 084503

flowing from the bottom to the top. The temperature difference of velocity and a diffusive flux representing the difference between
approximately 5 °C was estimated at 0.25 A cm−2 with an air flow an individual phase velocity and the mixture velocity.
rate of 3.4452 l min−1. 6) The power consumptions of blowers for fuel supply and air
Despite the several advantages of air-cooled fuel cell systems for recirculation are insignificant compared to that of the air
aviation applications over water-cooled fuel cell systems such as compressor and thus neglected.
their simple design and low weight, air-cooled fuel cell systems
exhibit low and unstable performance due mainly to severe electro-
lyte dehydration caused by the high flow rate of ambient dry air. To Governing equations and source terms.—According to the
solve these critical issues, we investigate the effects of injecting above-mentioned assumptions, the transient PEMFC model is
high-pressure hydrogen and air into a passive air-cooled fuel cell developed based on five principles of conservation: mass, species,
system. As outside air is drawn, pressurized, and supplied to the fuel momentum, thermal energy, and charge.
cell stack, the air flow rate required for waste heat removal is
expected to decrease significantly due to the increase in air density. Mass conservation
According to Eq. 1, a five-fold increase in the density of incoming
air (ρair ) would result in approximately a five-fold decrease in the ∂(ερ)
+ ∇ · (ρu ⃗) = 0 [ 2]
volumetric air flow rate (Vair
̇ ), which could significantly mitigate the ∂t
level of electrolyte dehydration.

̇ =
Vair
(U0 −T
∂U0
∂T )
− Vcell × I × A active
[1]
Momentum conservation
ρair cp, air (Tout − Tin )
1 ⎡ ∂(ρu ⃗) ⎛1⎞ ⎤
⎢ + ⎜ ⎟ ∇ · (ρuu⃗ ⃗) ⎥ = −∇P + ∇ · τ + Su [3]
This advanced air-cooled fuel cell system using pressurized inlet ε ⎣ ∂t ⎝ε⎠ ⎦
gases is illustrated in Fig. 1. It is worth mentioning that maintaining
the hydrogen pressure on the anode side and the air pressure on the
cathode side equal is also critical to ensure the durability of the PEM
and minimize the degree of gas crossover through the membrane. Energy conservation
Regarding the parasitic power consumed to pressurize the inlet
gases, as illustrated in Fig. 1, hydrogen fuel is usually stored in the ∂(ερCp T )cell
⃗ p T ) = ∇ · (k eff ∇T ) + ST
+ ∇·(ρuC [4]
on-board hydrogen tank at high pressures and thus no additional ∂t
power is required to blow the high-pressure hydrogen gas through
the fuel cell stack. However, the air in the atmosphere should be
pressurized by a compressor, for which additional power consump-
tion is required. To save the power consumed in air compression and Species conservation
achieve high hydrogen utilization, most of the exhaust air may be
recirculated into the system. To realize the new air-cooled fuel cell ∂ερm g
system technology, the improvement of fuel cell stack performance + ∇ · (γi ρm i u ⃗) = ∇ · [ρ g Dig, eff ∇(m gi )]
∂t
by pressurization should dominate the parasitic power consumption l
by the pressurization and recirculation. In this study, a three +∇ · [(m ig − m il ) j ⃗ ] + Si [5]
dimensional (3D) transient two-phase fuel cell model is applied to
the air-cooled fuel cell geometry and simulated under various inlet .—(flow channels and porous media)
pressures. In addition to demonstrating the trade-off between fuel
cell stack power improvement and parasitic power consumption by Mw ρmem ∂λ ⎡⎛ ρ mem ⎞ mem ⎤
+ ∇ · ⎢⎜ ⎟D ∇λ⎥ Mw
gas pressurization and recirculation, particular emphasis is placed on EW ∂t ⎣⎝ EW ⎠ w ⎦
investigating the effects of oxygen depletion during fuel cell
operations and water management capability as a function of air ⎡ ⎛ I ⎞⎤ ⎡⎛ κ mem ⎞ ⎤
−∇ · ⎢n d ⎜ ⎟ ⎥ Mw + ∇ · ⎢⎜ l ⎟ ∇P l ⎥ = 0 [6]
discharge and recirculation. ⎣ ⎝ F ⎠⎦ ⎣⎝ ν ⎠ ⎦

Numerical Model (water transport in the membrane)

The multi-scale 3D transient two-phase PEMFCs model pre-
sented in our previous study21,22 is employed to investigate the Charge conservation
transient response of the high-pressure air-cooled system. The model
∇ · (κ eff ∇ϕe) + Sϕ = 0 (proton transport) [7]
was experimentally validated against the polarization curves mea-
sured for the various cell designs and operating conditions.22 The
model takes into account the major components of a PEMFC, ∇ · (σ eff ∇ϕs ) − Sϕ = 0 (electron transport) [8]
including BPs, CLs, gas diffusion layers (GDLs), microporous
layers (MPLs), gas channels (GCs), coolant channels (CCs), and a .—The above governing equations are fully coupled through the
PEM. The following are the main assumptions for the development source/sink terms presented in Table I. The Butler-Volmer equations
of the above-mentioned system model: that describe the hydrogen oxidation reaction (HOR) at the anode CL
and the oxygen reduction response (ORR) at the cathode CL are also
1) Gas mixtures follow the ideal gas law. given in Table I. Based on Darcy’s law for porous media, the
2) The gravitational effect is negligible. momentum source/sink terms are derived and marked by Su in Eq.
3) Gaseous flow is laminar and incompressible. (9). The additional oxygen depletion through the ionomer/water
4) Porous components (e.g., GDL, MPL, and CL) were character- films covering the Pt and carbon particles was considered by using a
ized by their effective porosity and permeability. microscale CL model, which is coupled with the 3D PEMFC model.
5) Multi-phase mixture approach is used for the modeling of gas Tables II and III present the microscopic CL properties and key
and liquid flow in the porous components wherein the multi- correlations of the microscale CL model. Please refer to Chinannai
phase flow is described in terms of a mass-averaged mixture et al.21 for additional information on “microscale modeling.”
 Journal of The Electrochemical Society, 2021 168 084503

Table I. Source/sink terms of the PEMFC model.

μ
Momentum For porous media Su = − K u ⃗ [9]

Si = ⎡⎣ −∇ ·
Species For water in CLs si j ⎤ [10]
( )+nd ⃗
F
I nF ⎦ i
M
For other species in CLs Si = ⎡⎣ nFi ⎤⎦ Mi [11]
sj

Energy In CLs I2 [12]

ST,c = j η − T( dU0
dT )+ k eff
In the membrane Ie2 [13]
ST =
k eff
In two-phase region ST = h fg ∇ · ( K l g
v
λ λ ∇Pc + λl ρu ⃗ ) [14]

Charge In CLs Sϕ = j [15]

⎧ Mi = chemical formula of species i [16]
⎪
Electrochemical reactions ∑ si Miz = ne−, where ⎨ si = stoichiometric coefficient
k ⎪
⎩ n = number of electrons transferred
HOR: H2 − 2H+ = 2e−
ORR: 2H2O − O2 − 4H+ = 4e−
Transfer current density, [A / m3] 1 [17]
⎡ E
HOR in anode CL: j = (1 − s )1.5ai 0,refa ( )
CH2
CH2, ref
2
exp ⎣ − Ra ( 1
T
−
1
353.15 ) ⎤⎦ (exp ( αa + αc
RT
Fη))
⎛ COPt ⎞3 / 4 [18]
ORR in cathode CL: j = −ai 0,refc ⎜ C 2 ⎟ exp − Rc
⎝ O2, ref ⎠
E
( ( 1
T
−
1
353.15 ) ) exp (− αc
Ru T
Fη )
Overpotential HOR in the anode CL η = ϕs − ϕe [19]
ORR in the cathode CL η = ϕs − ϕe − E0 [20]
[21]
E0 = 1.229 − 0.9 × 10−3(T − 298.15) +
RT
2F (ln p H2 +
1
2
ln PO2 )

Table II. Properties of microscale CL.

Description Values References

−3
Density of carbon particle, ρc 1.95 g cm 23
Density of Pt particle, ρPt 21.45 g cm−3 23
Density of water, ρw 1.0 g cm−3 23
Density of ionomer, ρe 1.9 g cm−3 23
Pt/C ratio 70 wt % 21
Radius of carbon particle, rc 25 mm 23
Transport resistance coefficient of ionomer film, z e 4 21
Transport resistance coefficient of Pt particle, zPt 5.4 21
Transport resistance coefficient of water film, zw 6.5 21

To predict the two-phase transport and flooding in various determined by the waste heat generation and the set-point tempera-
PEMFC components, the present PEMFC model adopted the ture of the air outlet (Tsp ). From Table VIII, it can be observed that
multi-phase mixture approach provided by Wang and Cheng.24 the cathode stoichiometry range is much higher than that for water-
The key correlations of the multi-phase mixture model are listed in cooled PEMFC operations. A PEMFC can be operated in galvano-
Table IV. The thermophysical and transport properties of individual static mode or potentiostatic mode, and thus either a constant current
fuel cell components as well as the expressions for the transport density I or constant voltage Vcell are applied to the outer surface of
properties are summarized in Tables V and VI. the cathode BP as shown in Eq. (67). The source/sink terms and
various constitutive expressions of the present air-cooled PEMFC
Operating/boundary conditions and numerical implementa- model were numerically implemented by using the user-defined
tion.—The present 3D PEMFC model is implemented with the functions of a commercial CFD package, ANSYS Fluent (ver. 19;
single-cell geometry shown in Fig. 2. To reduce the expensive and ANSYS, Inc., USA). A grid-independent study was performed to
time-consuming computational turnaround time, the performances of determine the optimum number of grid points to ensure accurate
the air-cooled PEMFC stack and system in Fig. 1 were estimated simulation results. The minimum number of grid points identified is
based on the simulation results from the single PEMFC in Fig. 2. approximately 150,000 grid points for the computational region
Table VII lists the operating conditions and cell dimensions for the highlighted with a yellow box in Fig. 2. To perform numerical
single-cell simulations. The boundary conditions applied to the simulations of described geometry and operational conditions, the
single PEMFC are summarized in Table VII. To approximate a model requires 32 GB of computational memory and 3 h for 1000
typical air-cooled PEMFC stack environment in which waste heat iterations (totally 20 h), using an AMD Ryzen 5 3600 6-core
generated in the stack is mainly removed by the air flow, no-flux and processor CPU at 3.59 GHz. Moreover, to ensure efficient and
adiabatic boundary conditions are applied to all external surfaces converging solutions, the convergence criteria for the simulations
except for the hydrogen and air inlet and outlet regions (see Fig. 2). were set to maximum residuals under 10−6 and a mass and energy
Therefore, as expressed in Eq. (64), the air inlet velocity is imbalance less than 1%.
 Journal of The Electrochemical Society, 2021 168 084503

Table III. Key correlations for the microscale CL model.

Description Expressions Eq. No.

Carbon volume fraction (εc )

εc =
LPt
δCL ( ) 1
ρc wt %
[22]

Pt particle volume fraction (εPt ) εPt =

1 LPt [23]
ρPt δCL
Ionomer volume fraction (εe ) εe = () I
C
ρc
ε
ρe c
[24]

Volumetric surface area of carbon (ac) ac =

3εc
(rc + δe )2 [25]
rc3
Electrochemically active surface area of Pt (aECSA ) aECSA =
3 [26]
rPt·ρPt
Volumetric surface area of Pt (aPt) aPt =
aECSA LPt [27]
δCL
Number of Pt particles on a single carbon particle (nPt) rc 3 [28]
nPt =
ρc
ρPt ( )(
rPt
wt %
1 − wt % )
CL thickness (δCL ) ⎡ I ρC ⎛⎜ 1 ⎞⎟ + ⎛⎜ 1 + 1 ⎞⎟ ⎤ [29]
δCL = ⎢
()
⎢ C ρe ⎝ ρC × wt % ⎠ ⎝ ρPt ρC × wt % ⎠ ⎥
1 − εCL ⎥ LPt
⎢⎣ ⎥⎦
Thickness of the ionomer film (δe ) ⎡ 1 ⎤ [30]
( ε
δe = ⎢ 1 + εe 3 − 1⎥ rc
⎣ c ⎦
)
Thickness of water film (δ w ) ⎡ 1 ⎤ [31]
( ε s
δ w = ⎢ 1 + εe + ε 3 − 1⎥ rc − δe
⎣ c c ⎦
)
Effective ionomer film thickness (δeeff ) δeeff =
(rc + δe + δ w )2
δe
[32]
2
npt . r pt
Effective water film thicknesses (rc + δe + δ w )2 [33]
δweff = 2 δw
npt . r pt
Oxygen balance in a single Pt/C particle domain COg2 − COPt2 = (Rw + Re + Rpt ) 4F
I [34]
Transfer current density for the ORR (jc) ⎛ O C Pt ⎞ c
γ [35]
jc = −apt i 0,refc ⎜ C 2 ⎟ exp − Rc
⎝ O2, ref ⎠
E
( ( 1
T
−
1
353.15 ) ) exp (− αc
RT
Fηc )
Oxygen transport resistance across the water film (Rw) 1 ⎡ δ δ eff ⎤ [36]
Rw = δ . a ⎢zw D w + D w ⎥
CL c ⎣ O 2, w O 2, w ⎦

Oxygen transport resistances across the ionomer film (Re) 1 ⎡ δ δeeff ⎤ [37]
Re = δCL . ac ⎢
z e + DO 2, e ⎥
⎣ e DO2, e ⎦
Interfacial resistance between the electrolyte film and Pt particle (RPt) 1 ⎡ rPt 3 1 − wt % δe ⎤ [38]
RPt = δCL . ac ⎣
(rc + δe )2 ρPt
⎢zPt r 2
Pt ρc ( )(
rc wt % ) ⎥
DO 2, e ⎦

Results and Discussion respectively. The degree of hydrogen and oxygen depletion near
the downstream region of the cell is substantially reduced as the
In this study, we assess the effects of using pressurized air for air-
operating pressure increases. To analyze the detailed polarization
cooled fuel cell stacks that are expected to mitigate the degree of
behaviors under the different operating pressure conditions, the
electrolyte dehydration, favorably enhancing cell performance. Four
activation and ohmic overpotentials at various fuel cell components
different inlet air pressures (Pair) of 1.0, 2.0, 3.0, and 5.0 atm were
are compared in Fig. 7. By raising the operating pressure, the
chosen in this study and simulated under 30% humidification of both
activation overpotential in the cathode CL is reduced by approxi-
hydrogen and air inlet flows. Table VII summarizes the operating
mately 3.75–14.1 mV, which is a combined result of a weakening of
conditions and key simulation results in which it can be observed
reactant depletion (Figs. 5 and 6) and a more uniform current density
that the inlet air velocity (uin, c ) to maintain the same set-point
distribution (Fig. 8) under higher operating pressures. The effects of
temperature of 50 °C (Tsp ) at the air outlet decreases with increasing high-pressure operation are more evident in the reduction of ohmic
air inlet pressure. Owing to the lower air velocity under the higher overpotential. As a result of the superior hydration of electrolytes
air pressure condition, the cell voltage at the operating current under the higher operating pressure shown in Figs. 3 and 4, the
density of 0.45 A cm−2 is significantly improved from 0.68 V at ohmic overpotentials in the anode and cathode CLs and membrane
Pair = 1 atm to 0.88 V at Pair = 5 atm, clearly indicating the are considerably lowered by raising the operating pressure. Figure 8
beneficial influence of blowing the high-pressure air through an air- shows the current density distributions in the membrane where the
cooled fuel cell stack. The water content (λ) contours in the anode higher local current density is observed near the air inlet region and
and cathode CLs are plotted in Figs. 3 and 4, respectively. It is continues to decrease toward the cathode outlet. This trend is mainly
evident that the level of electrolyte hydration in the CLs is greatly due to the increase in temperature along the air flow path, and lower
improved from λavg = 3 ∼ 4 at Pair = 1 atm to λavg = 9 ∼ 13 at water content and oxygen concentration in the downstream region of
Pair = 5 atm. In addition, the local water content is higher near the the cell. Along the in-plane direction, the local current density
region where the hydrogen outlet and air inlet are adjacent, which is becomes higher under the cooling channels than in the reactant air
mainly due to the lower local temperature at the air inlet. The channel region, which clearly indicates that the performance is
hydration regions in the anode and cathode CLs tend to expand mainly determined by the extent of electrolyte hydration (Fig. 4)
towards the hydrogen inlet region as the operating pressure increases rather than oxygen transport limitation (Fig. 6). At Pair = 5 atm, the
and the required air flow rate decreases. current density distribution characteristic that decreases toward the
Figures 5 and 6 display the contours of hydrogen concentration in air outlet is somewhat weaken, which is due to improvements in
the anode CL and oxygen concentration in the cathode CL, electrolyte hydration and oxygen transport (see Figs. 3, 4, and 6).
 Journal of The Electrochemical Society, 2021 168 084503

Table IV. Two-phase correlations for the multiphase mixture model.

Description Expressions Eq. No

Mixture density [kg m −3] ρ = ρl s + ρ g (1 − s ) [39]

[40]
Gas mixture density [kg m −3] ρg = ( )∑ P
Ru T
1
mi
g

i Mi

Mixture velocity [kg m −2 s−1] ρu ⃗ = ρl u ⃗ l + ρ g u ⃗ g [41]

Mixture mass fraction ρl smil + ρ g (1 − s) mig [42]
mi = ρ
Relative permeability krl = s 4 [43]
krg = (1 − s )4 [44]
Mixture kinematic viscosity −1 [45]
v= ( krl
vl
+
krg
vg )n
Gas composition μg 1 xi μi [46]
vg = ρg
= ρg
∑ n
∑ j = 1 xj ϕij
i=1
−1 / 2 ⎡ ⎛ μ ⎞1 / 2 Mj 1 / 4 ⎤
2 [47]
where ϕij =
1
8 (1+
Mi
Mj ) ⎢1 + ⎜ μi ⎟
⎣ ⎝ j⎠ ( )
Mi
⎥
⎦
and
⎧ μ = 0.21 × 10−6T 0.66 [48]
⎪ H2
⎪ μ w = 0.00584 × 10−6T1.29
μi [Nsm−2] = ⎨ , T in kelvin
⎪ μ N2 = 0.237 × 10−6T 0.76
⎪ −6 0.78
⎩ μO2 = 0.246 × 10 T
Relative mobility krl [49]
λl = v
vl
λ g = 1 − λl [50]
Diffusive mass flux [kg m −2 s−1] →
⎯ K l g [51]
j l = ρl u ⃗ l − λl ρu ⃗ = v
λ λ ∇Pc
Capillary pressure [Pa] ε 1/2 [52]
Pc = Pg − P l = σ cos θ ()K
J (s )
Leverett function ⎧1.417 (1 − s ) − 2.120 (1 − s )2 + 1.263 (1 − s )3 if θc < 90∘ [53]
J (s ) = ⎨
⎩ 1.417s − 2.120s 2 + 1.263s3 if θc > 90∘

More importantly, the uniformity in the current distribution is key to maximizing the net electrical power delivered by the air-
greatly improved with increasing operating pressure due mainly to cooled fuel cell system, changes in the oxygen and nitrogen
the increase in the reactant air concentration. The above results concentrations during fuel cell operation are investigated for various
clearly indicate the beneficial effect of pressurizing inlet air flow for values of rcharge. Figure 9 shows the evolution of the oxygen and
air-cooled fuel cell operations. nitrogen concentrations under different operating pressure condi-
According to the system configuration in Fig. 1, the air flowing tions wherein the volume occupied by air (including the air pipeline
out of the fuel cell stack must be recirculated to reduce the and the chamber) was assumed to be twice the cathode volume in the
compressor power consumed for pressurizing the atmospheric air. fuel cell stack (see Fig. 1). When rcharge = 1 is applied (only air in
Oxygen is consumed by an ORR inside the fuel cell stack while moles equal to the number of moles of oxygen consumed by the
outside air is newly drawn into the system to maintain the same ORR is supplied from the outside), oxygen in the air-cooled system
operating pressure. Therefore, the fraction of oxygen in the air in the is shortly depleted at t = 7.29s for Pair = 2 atm, t = 10.95s for
system continuously decreases with operating time, requiring that Pair = 3 atm, and t = 18.28s for Pair = 5 atm. As rcharge increases, the
some of the recirculated air should be discharged and more air than rates of oxygen concentration drop and nitrogen concentration rise
the amount of oxygen consumed by the ORR should be supplied into become slower and almost reach constant values above certain
the air-cooled system. Here, we define an air charge ratio rcharge, i.e.,
values of rcharge (CO*2 and C N*2 ). Higher values of CO*2 are achieved
the molar flow rate of air newly drawn from the outside into the air-
cooled stack normalized by the molar flow rate of oxygen consumed with higher rcharge and/or higher Pair. Based on the calculated results
by the ORR. in Fig. 9, an rcharge of 6, 7, and 8 were chosen and simulated for this
study.
̇
Nair Figure 10 compares the evolutions of the stack power output
rcharge = . [69] ̇ ), and net
(i 4F ) ncell ̇ ), power consumption of air compressor (Wcomp
(Wstack
̇
power delivered by the air-cooled system (Wnet ) under three different
i
As shown in Fig. 1, once the molar air flow rate of rcharge 4F ncell is air charge ratio conditions (rcharge = 6, 7, and 8). Wstack
̇ initially drops
introduced from the outside and compressed through the air and then stabilizes at a constant value, which indicates that Wstack ̇ is
compressor, the molar oxygen consumption rate during fuel cell mainly influenced by the evolution profile of the oxygen concentra-
i
operation is 4F ncell and the amount of air discharged from the air- tion shown in Fig. 9. Even though a higher Wstack ̇ was produced with
i a higher rcharge, the net power delivered by the system, Wnet ̇ , is a
cooled stack is (rcharge − 1) 4F ncell. It should be noted that oxygen in
̇
combined result of Wstack ̇ , rendering the optimum value of
and Wcomp
the circulating air is finally depleted with rcharge < 4, 78, since
outside air is drawn into the system while oxygen is consumed in the rcharge highly dependent on fuel cell operating conditions (mainly
PEMFC stack. Because the determination of the optimum rcharge is operating pressure and current density). Because Wcomp ̇ substantially
 Journal of The Electrochemical Society, 2021 168 084503

Table V. Thermophysical and transport properties of individual fuel cell components.

Description Value References

−1 −1
Thermal conductivity of CL/MPL/GDL/membrane/BP, (kCL eff eff
kMPL eff
kGDL eff
k mem eff
kBP ) 1.5/1.5/1.2/0.95/16.2 Wm K 25
−1 −1
Thermal conductivities of H2/H2O/N2/O2, (k H2 / k H2 O / k N2 / k O2 ) 0.2040/0.0237/0.0293/0.029Wm K 26
Porosity of GDL/MPL/CL, (εGDL / εMPL / εCL ) 0.6/0.4/0.4 17
Tortuosity of GDL, CL, MPL, and membrane 2.0 22
Contact angles of GDL/CL (θ) 92°/92° 22
−3
Exchange current density of HOR × ratio of the reaction area to electrode volume, (aI0,a
ref
1.2 × 10 Am 22
10
)
ref
Exchange current density for ORR, (I0,c ) 3.0 × 10−5 Acm−2 23
−1
Activation energy of anode, (Ea ) 10.0 kJmol 22
Activation energy of cathode, (Ec) 70.0 kJmol−1 22
Transfer coefficient of HOR, (αa = αc ) 1 27
Transfer coefficient of OOR, (αc ) 1 27
Reaction order for anode/cathode, (γa γc ) 0.5/0.75 21
Reference H2/O2 molar concentration, (C ref ) 40.88 mol m−3 22
Permeability of GDL/MPL/CL/mem, (KGDL /KMPL / KCL / Kmem ) 1.0 × 10−12/1.0 × 10−13 28
/1.0 × 10−13/1.0 × 10−30 m2
Dry membrane density, (ρdry, mem ) 2000 kg mol−1 27
Equivalent weight of electrolyte in membrane, (EW ) 1.1 kg mol−1 26
Faraday’s constant, (F) 96,485 C mol−1
Universal gas constant, (Ru) 8.314 J mol−1K−1
H2 diffusivity in anode gas channel, (D0,g H2, a ) 1.1028 × 10−4 m2 s−1 26
H2O diffusivity in anode gas channel, (D0gH2 O, a ) 7.35 × 10−5 m2 s−1 26
O2 diffusivity in cathode gas channel, (D0,g O2, c )) 3.2348 × 10−4 m2 s−1 26
H2O diffusivity in cathode gas channel, (D0,g H2 O, c ) 7.35 × 10−5 m2s−1 26
O2 diffusivities through ionomer film and water film, (DO2, e and DO2, w , respectively) 0.58 × 10−10 m2 s−1 26
−1
Effective electronic conductivity in CLs, (σCL ) 1,000 Sm 27
Effective electronic conductivity in GDLs, (σGDL ) 10,000 Sm−1 27
Effective electronic conductivity in BP, (σBP ) 20,000 S m−1 27

Figure 2. Computational domain, mesh configurations, and cell dimensions of passive air-cooled single-cell with key boundary conditions. The size of the
computational domain is reduced to the area of the yellow dashed box (150,000 grid points) utilizing the geometric symmetry condition.

increases by raising the operating pressure and/or air flow rate, a Pair = 2 atm, 7 for Pair = 3 atm, and 6 for Pair = 5 atm. According
higher operating pressure results in a lower optimum value of rcharge. to the simulation results in Fig. 10, a fuel cell operation under 2 atm
The optimum values of rcharge were predicted to be 8 for conditions is superior to that under 3 atm and 5 atm conditions in
 Journal of The Electrochemical Society, 2021 168 084503

Table VI. Transport properties in the electrolyte.

Description Expressions

Binary gas diffusivity (Dig ) T 3 / 2 P0 [54]

For nonporous regions Dig = Dog () ( )
T0 P
ε [55]
effective diffusivity (Dig, eff ) For porous regions Dig, eff = Dg
τk i
Membrane water content [λ) ⎧ λ = 0.043 + 17.81a − 39.85a 2 + 36.0a3 for 0 < a ⩽ 1 [56]
λ=⎨ g
⎩ λl = 22
Cwg Ru T [57]
where a denotes the water activity, a = Psat
Electro-osmotic drag (EOD) coefficient of water (nd ) nd =
2.5λ [58]
22
Proton conductivity (κ ) ⎡ ⎤ [59]
κ = (0.5139λ − 0.326) exp ⎣1268 ( 1
303
−
1
T ) ⎥⎦
Water diffusion coefficient (Dwmem ) ⎧ 2.692661843 ·10−10 for λ ⩽ 2 [60]
⎪ −10 (7.9728 − 2416 / T ) for 2 < λ ⩽ 3}
⎪{0.87 (3 − λ ) + 2.95 (λ − 2) · 10 ·e
⎪ 2.95 4
⎪ { ( − λ ) + 1.642454 (λ − 3)} · 10−10 ·e(7.9728 − 2416 / T ) for 3
⎪ <λ⩽
⎪
Dwmem =⎨ 4
⎪
⎪ (2.563 − 0.33λ + 0.0264λ2 − 0.000671λ3)
⎪ · 10−10 · e(79728 − 2416 / T ) for 4
⎪
⎪ <λ⩽
⎪
⎩ λag= 1

Table VII. Cell dimensions and operating conditions.

Description Value

GC Width, WcGC 1 mm
Depth, dcGC 1 mm
CC Width, WcCC 1.5 mm
Depth, dcGC 1 mm
Thickness BPs, δaBP / δcBP 0.05 mm
GDLs, δaGDL / δcGDL 0.5/0.25 mm
MPLs, δaMPL / δcMPL 0.03 mm
CLs, δaCL / δcCL 0.03 mm
Membrane, δmem 0.025 mm
Cell length, L 300 mm
Active area, Aactive 7.8 cm2 (0.26 cm × 30 cm)
Cathode inlet area, Ain, c 0.273 cm2 (10.25 cm × 0.26 cm)
Operating current density, I 0.45 A cm−2
Inlet temperature, Tin 25 °C
Set-point outlet temperature, Tsp 50 °C or 80 °C
RH (anode/cathode) 30%/30%
Anode stoichiometry, ξa 1.1
Cathode stoichiometry, ξc (1atm/2atm/3atm/5atm) 89.34/78.18/75.00/72.65
Cathode inlet velocity, uin, c (1atm/2atm/3atm/5atm) 2.3334/1.0162/0.6489/0.3766

Table VIII. Boundary conditions.

Description Expression

Anode inlet velocity ξa

I
Aactive [63]
2F
uin, a = CH2 Ain, a
Cathode inlet velocity ⎛ dU0 ⎞ [64]
⎜U0 − T − Vcell ⎟·I ·Aactive
⎝ dT ⎠
uin, c = ρCP Ain, c (Tout − Tin )
Stoichiometry in cathode ξc = uin, c ·
4F ·CO 2
·
Ain, c [65]
I Aactive
Electric potential on the anode’s outer BP surface ϕs = 0 [66]
Electric potential on the cathode’s outer BP surface ϕs = Vcell or σ ∇ϕs = I [67]
Thermal boundary except at the inlet and outlet regions ∂T
=0 [68]
∂n
 Journal of The Electrochemical Society, 2021 168 084503

Figure 3. Water content profiles for the middle plane of the anode CL under different operating pressures.

Figure 4. Water content profiles for the middle plane of the cathode CL under different operating pressures.

Figure 5. Hydrogen concentration distributions for the middle plane of the anode CL under different operating pressures.

terms of the net power delivered (Wneṫ ), and hence further simula- Pair = 2 atm, which is almost double compared to that at 1 atm
tions were carried out at Pair = 2 atm. Based on the single cell (20.20 kW). Although a higher compressor power (Wcomp ̇ =
performance at Pair = 1 atm (Vcell = 0.68 V at i = 0.45 A cm−2 as 7.83 kW) is required at 2 atm due to the larger air pressure, the
shown in Fig. 7), the reference fuel cell stack (ncell = 220, AMEA = net power is improved from Wnet ̇ = 19.39 kW at 1 atm to
300 cm2) was designed to operate at Pair = 2 atm in potentiostatic ̇ = 32.52 kW at 2 atm. Wcomp
Wnet ̇ can be reduced by increasing the
mode corresponding to the single-cell voltage of 0.68 V. For the
set-point temperature (Tsp ) that lowers the air flow rate required for stack
purposes of comparison, two different set-point temperatures of
50 °C and 80 °C were considered and the key simulation results are cooling. By raising Tsp from 50 °C to 80 °C, Wcomṗ is reduced from 7.83
shown in Fig. 11 along with the simulation results at Pair = 1 atm kW to 4.14 kW. As seen in Fig. 11a, however, the degree of electrolyte
and i = 0.45 A cm−2. At the same set-point temperature (Tsp = dehydration becomes more severe at Tsp = 80 °C, resulting in a much
̇ ) around 40.35 kW was produced with
50 °C), the stack power (Wstack lower stack and net power (Wstack̇ = 21.31 kW and Wnet ̇ = 17.17 kW )
 Journal of The Electrochemical Society, 2021 168 084503

Figure 6. Oxygen concentration distributions for the middle plane of the cathode CL under different operating pressures.

Figure 7. Comparison of cell voltages and individual voltage losses under different operating pressures.

Figure 8. Current density distributions in the membrane under different operating pressures.

̇
compared to Wstack = 40.35 kW and Wnet ̇ = 32.52kW at Tsp = 50 °C, Conclusions
respectively. The above results clearly indicate that the power con- To improve the low volumetric power density of passive air-
̇ ) to blow high-pressure air through a fuel cell stack is
sumption (Wcomp cooled fuel cell systems at ambient pressure, this paper numerically
̇ , the high-pressure air-cooled fuel cell
substantial and to minimize Wcomp analyzes the merits of operating the air-cooled fuel cell systems at
system requires a high degree of optimization in terms of system elevated pressures. In the high-pressure air-cooled fuel cell system,
configuration, design, and operating strategy. the power consumption of the air compressor was substantial and
 Journal of The Electrochemical Society, 2021 168 084503

Figure 9. Evolution curves of nitrogen and oxygen concentrations during a 2-hour operation at an air charge ratio (rcharge ) from 1 to 10 under different operating
pressures: (a) 2 atm; (b) 3 atm; (c) 5 atm.

hence the exhaust air out of the fuel cell stack was recirculated in the resulting mitigation of electrolyte dehydration. There is, however, a
system. In addition, some of the recirculated air had to be discharged trade-off between fuel cell stack power improvement and parasitic
and, instead, outside air was newly drawn into the system to retard power consumption by air pressurization and recirculation.
the rate of oxygen depletion and nitrogen accumulation in the air Comparing the three pressurization conditions of 2 atm, 3 atm,
stream. The simulation results clearly show that the fuel cell stack and 5 atm, the stack power was highest at 5 atm but the highest net
power was greatly improved by pressurizing the air owing to the power (Wneṫ ) was achieved at 2 atm. As atmospheric air was
lower air velocity under the higher air pressure condition and the pressurized to 2 atm, the stack power and net system power was
Journal of The Electrochemical Society, 2021 168 084503

Figure 10. Evolution of the stack power output

̇
Wstack (ncell = 220, Aactive = 300 cm2 ), the air com-
pressor power consumption Wcomp ̇ , and the net
system power Wnet ̇ during a 2-hour operation. The
air charge ratio rcharge varies from 6 to 8 under
different operating pressures: (a) 2 atm; (b) 3 atm;
(c) 5 atm.
 Journal of The Electrochemical Society, 2021 168 084503

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