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Mathematical modelling and simulation analysis of PEM electrolyzer system

for hydrogen production

Conference Paper · November 2014

DOI: 10.1049/cp.2014.1466

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 Mathematical modelling and simulation analysis of PEM
electrolyzer system for hydrogen production
A.H. Abdol Rahim *, Alhassan Salami Tijani *, Farah Hanun Shukri *, S. Hanapi *, K.I. Sainan*

*Faculty of Mechanical Engineering, Universiti Teknologi MARA, Shah Alam, Selangor, Malaysia
Email: [email protected]

Keywords: Renewable energy, PEM electrolyzer, Hydrogen “green-hydrogen”. These technologies are advanced alkaline
production. electrolyzer, photoelectrochemical and PEM electrolyzer
technologies. Among them PEM electrolyzer offers an
Abstract efficient, flexible and practicality for a high quality of
hydrogen production. In recent times more attention is being
In recent times there is a growing concern about the paid to PEM electrolyzer due to its offers several advantages
environmental impact of conventional energy sources. The compared other method of electrolysis in term of smaller
only solution to the depletion and environmental impact is to mass volume characteristic, higher in current densities, high
rely on sustainable renewable energy sources for various degree of gas purity and better safety level [3].
applications. One of the promising options is PEM
electrolyzer for hydrogen production. In this paper, the 2. Mode of operation of (PEM) electrolyzer
equations related to mathematical models for PEM
system
electrolyzer based on a combination of thermodynamics
fundamental and electrochemical relations are presented. A PEM electrolyzer cell is composed of an anode chamber, a
Simple PEM electrolyzer is analyzed on the basis of well- cathode chamber, two electrode catalyst surfaces and a proton
known Butler-Volmer kinetic for the electrodes and transport exchange membrane [4]. The dissociation of water into
resistance in the polymer-electrolyte. The effect of hydrogen and oxygen is relatively high since water molecules
temperature on operating cell voltage, resistance and ionic have a stable structure at ambient temperature [5]. A
conductivity of the polymer electrolyte are examined. Finally minimum potential of 1.23V (reversible voltage) is applied
different values of exchange current densities at anode and across the electrochemical cell to initiate electrochemical
cathode were tested. The simulation results indicate that as reactions at both anode and cathode electrodes. Water is
temperature increases, there is a significant or sharp decrease introduced at the anode and dissociated into oxygen, protons
in ohmic resistance from 0.198Ω/cm2 at 40oC to 0.125Ω/cm2 and electrons via the following reaction:
at 80oC. However there is a small increase in ionic 1
-
conductivity. From this observation it can be concluded that Anode: H 2O  O 2
2 H
2e (1)
the ionic conductivity of the membrane assembly increases 2
with temperature and this can lead to increase in hydrogen
flow rate. The hydrogen ions are driven through the membrane to the
cathode under an electric field where they combine with the
1. Introduction electrons arriving from the external circuit to form hydrogen
gas:
Energy is an important factor that contributes to the

development of a nation especially in the industrial sector, Cathode: 2 H
2e  H 2 (2)
however due to increasing global energy demand, the fossil
fuel reserves such as coal natural gas and petroleum are The net reaction for entire cell is
depleting at an alarming rate. Fossil fuel such as coal and
methane are known to emit carbon dioxide into the 1
H 2O(liq)  H 2(g)
O 2(g) ΔH 25°=285.84 kJ (3)
atmosphere which are responsible for global warming effects. 2
It is therefore important to look for a more reliable and
sustainable energy source. One of the alternative energy such 2.1 Operating Cell Voltage
as hydrogen has been introduced to replace conventional
energy sources. It contributes towards more sustainable, This single operating cell voltage of PEM electrolyzer is
environmental friendly criteria, energy economy and energy given by the summation of the reversible voltage and the
carrier in the future [1, 2]. It is one of the potential solutions other different overpotentials [6];
to the current energy and environmental pollution crises due
to its carbon free [2]. Nowadays, they have many Vcell  Vrev + ηact + ηΩ (4)
technologies of hydrogen production produce from renewable
energy sources for hydrogen production that offer a promising
2.2 Reversible Voltage   F    F 

ia  io, a exp 1 a   exp  2 a  (10)

Each reaction at the electrodes depends on the reactions of   RT   RT 
water at minimum voltage which corresponds to the
reversible potential. This can be determined by using the The current density at cathode [8];
Gibbs free energy equation [7];
  F    F 

ΔG  ηFVrev (5) ic  io, c exp  2 c   exp 1 c  (11)

  RT   RT 
G
Vrev  (6)
F where R is the universal gas constant, R = 8.314J/mol.K, T is
the variable temperature, T(K), α1 and α2 is the symmetry
where G is the Gibbs free energy of 237.178kJ/K.mole factor which at the anode represents an additional energy
(also known as the lower heating value, (LHV)), Vrev is the fraction of the reduction and cathode represent the oxidation.
reversible voltage, η is the number of the electrons and is η is the number of electrons involved. Moreover, the
activation overpotentials at anode and cathode can be
the Faraday’s Constant. Since all variable in equation (6) is inscribed as [6];
already known, the value of the reversible voltage of the cell
can be calculated as [6];
RT  i 
a  ln a  (12)
kJ  a zF  io,a 

237.178
Vrev  K .mole  1.229V (7)  i 
RT
columbs c   ln c  (13)
2  96485.3  c zF  io,c 
mole 

2.3 Thermoneutral Voltage where z is the stoichiometric coefficient of the number of

electrons involved, αa and αc is the charge transfer coefficients.
In thermodynamic of electrolysis, since the Gibbs free energy The values of αa and αc are 0.5 on the symmetry reactions.
is known as the maximum amount of usable electrical energy The value of the stoichiometric coefficient is 2 since it was
available when the hydrogen recombines with the oxygen, the water electrolysis.
thermoneutral voltage can be identified as the amount of the The value of the exchange current density of anode, io, a , and
energy losses in the electrolysis system. The thermoneutral cathode, io, c can give a very big impact on the activation
voltage can be identified as [6];
overpotential values on both sides. By expressing the
Arrhenius equation, the value of each exchange current
H 0 density at anode and cathode can be identified using these
Vtn  (8)
F equations [8];

where H 0 is the high heating value (HHV) of  EA, a  1 1 

io, a  ioref,a exp      (14)
285.84kJ/K.mole. The value of the thermoneutral voltage can 
 R  T T0 

be clarified as [6];
 EA, c  1 1 
io, c  ioref,c exp      (15)
kJ  R 
285.4   T T0 
Vtn  K.mole  1481Volt (9)
columbs cell
2  96485.3 where T0 is the reference temperature, T0 (K), EA, a and
mole EA, c is the anodic and cathodic active energy (J/mol), also
Since the value of thermoneutral voltage is the amount of ioref, a and ioref,c is the anodic and the cathodic reference
energy losses in the cell, it will not include in Eq. (4) to find exchange current density at reference temperature T0 The
the cell voltage values.
role of activation overpotential can be derived as [6];
2.4 Activation Overvoltage
 act   a
 c (16)
By relating the Butler-Volmer expression, the current density
at the anode and cathode can be expressed interms of charge By referring an example from Choi et al. [8] they suggested
transference phenomena and exchange current density. that the exchange current densities at anode, cathode based on
The current density at anode [8]; platinum electrode catalyst and platinum iridium electrode
catalyst referred on the parameters given in Table 1.
Table 1: Model Parameter for water electrolysis for Pt based The value of activation overpotential at the anode and cathode
anode and cathode electrodes on Nafion® electrolyte [8, 9] can be calculated using Eq. (12) and Eq. (13), using all
Parameters Values Dimension References
parameters related in Table 2.
io , a , Pt 10-12– 10- 2
9 A/cm Platinum electrode catalyst 2.6 Diffusion Overvoltage
io , a , Pt - Ir -7 2 Platinum Iridium electrode
10 A/cm
catalyst The diffusions give a function in overcoming the energy lost
io , c , Pt 10-4– 10-3 A/cm2 Platinum Electrode catalyst presume in the cell due to the mass transport resistance of
electrochemical reaction in the interface of the membrane and
2.5 Ohmic Overvoltage electrode [6]. Considering the value of the diffusions is so
small and may not give major impact on the simulation result,
The ohmic overpotential can be classified into two categories: it can be neglected. Finally, from Eq. (4), the overall
i. Ohmic overpotential due to membrane resistance operating cell voltage can be concluded as;
(ionic resistance).
This is caused by the membrane resistance to the flow of ions.
 i   
It also called voltage drop due to membrane resistance to the Vcell  Vrev

RT
ln a 
 RT ln ic 

flow of ions. This can be expressed as [8];  a zF  io,a 
  c zF  io,c 


  
 ,mem  i (17)   (22)
  t mem 
 Rele
i
  

where Rion 
  0.005139  0.00326exp1268 1  1  

is an ionic resistance as a function of
   303 Tcell  
membrane thickness conductivity,  is the membrane height,
(cm), and  mem is the local ionic conductivity with water 2.7 Molar Flow Rate
content and temperature function. This can be written as [8];
It is known that the current, I can be found using [8];

 1 1 
I  iA (23)
 mem  0.005139  0.00326exp 1268   (18)

  303 Tcell  
where, i is the current density and A is the electrode area. By
governing the Faraday’s law in this electrochemical cell, the
Where  is the degree of membrane humidification.
molar flow rate related can be written as [6];
ii. Interfacial overpotential (electronic resistance).
This is caused by electronic materials such as bipolar plates,
 cell I
electrodes current collectors, etc. The interfacial resistance H2  F (24)
can be expressed as [6]; 2F
 I
O2  cell  F (25)
 ,e  Rele i (19) 4F
 cell I
H 2 O  1.25 F (26)
The ohmic resistance of the electronic materials is; 2F

l The number of electrolytic cells used only one cell.  cell  1 ,

Rele  (20)
A while I is the overall current across the cell. The Faraday
efficiency,  F , I the differential between the experimental
where,  is the material resistivity (Ωm), l is the length of and theoretical hydrogen flow rate. It can be assumed as
the electrons path, and A is the conductor cross-sectional area. 100% since many other literatures agreed that it has the value
The ohmic overpotential due to electronic and ionic over 95% [6]. Since this was explained, the Eq. (24), (25),
resistances is [6]; and (26) can be simplified to be [7];

 ,mem  Rele
Rion i (21) I


H 2  (27)
2F
Table 2: Parameter selection in ohmic I
Parameters Values Unit 
O2  (28)
4F
io,a 10-9 A/cm2
io,c 10-3 A/cm2 I

H 2 O  1.25 (29)
Rele 0.035 mΩ 2F
t,mem 200 μm
λ 17 -
The hydrogen production can be expressed in terms of 2 .2
C e ll V o lta g e (V ) vs C u rre n t D e n s ity (A /c m 2 )

volume flowrate;
2 .1 5

 mol   3600s   0.022414m  m

3 3
Q
H  
H 2  
2 .1
  (30)
 s   1hr   mol  hr


C e ll V o lta g e (V )
2 .0 5

2
The hydrogen volume flowrate can be converted to L/min as
shown below. 1 .9 5

400C
1 .9
600C
m3 1hr 1000 L L 800C
Q
   3
 (31) 1 .8 5
0 0 .2 0 .4 0 .6 0 .8 1 1 .2 1 .4 1 .6 1 .8 2
hr 60 min 1m min C u rre n t D e n s ity (A /c m 2 )

Figure 1: Effect of temperature on operating cell voltage

3. Results and Discussion
3.2. Case 2 – Current Density and Exchange Current Density
The effects of the operating parameters such as current
density, exchange current density, ohmic overvoltage, and Case 2 was focused in finding the current density value by
activation overpotential on the operating cell voltage have manipulating the equation introduced with calculus
been discussed include the effect of temperature on the ohmic relationship. By using Eq. (10) and Eq. (11), the value of
resistance. The hydrogen volume flow rate was analyzed current density at anode and cathode at different temperature
within a range of given current density (0.1 – 2.0A/cm2). All were tested. The equation for activation overvoltage of anode
the results were validated against experimental data from the and cathode below is the same as in Eq. (12) and Eq. (13) but
literature. There were two cases that would affect the result. were represented in different mathematical simplification.
One is the temperature and the current density, and the second The activation overpotential at the anode is given according
one is the relation between the current density and the to Eq. (32) [9]:
exchange current density. This condition has been divided
into two cases and will be discussed in the next sub-chapter.  i 
RT
a  sinh 1  a  (32)
F  2i 
3.1. Case 1 – Temperature and Current Density Relation  o ,a 

Previous experimental manipulation usually focused on a 3.3. Simulation Analysis Result

different range of temperatures such as 40oC, 60oC and 80oC.
The idea of using these parameter relations is to evaluate the The simulation analysis result is focuses on two main
value of voltage drop or voltage losses in an electrochemical variables which are the current density and the exchange
cell whenever the temperature is increased. This phenomenon current density. There are three different values of exchange
can be tested in terms of variation of the resistance current density at anode and cathode – known as condition 1,
conductivity against the temperature and also in the variety of 2 and 3 as shown in Table 3
operating cell voltage against the current density. Since this
modelling uses the PEM, the presence of proton exchange is Table 1: Parameters value use for this analysis.
visible in the water electrolysis which means that the
overpotential of the ohmic cannot be neglected. The process Condition
Parameter
of calculating the operating cell voltage started with the sum 1 2 3
of the reverse voltage with the activation overvoltage. Figure Exchange Current Density -9 -10
1x10 5x10 1x10-12
at Anode (A/cm2)
1 shows the polarization curve of the effect of temperature on Exchange Current Density
the operating cell voltage. It can be observed that at a 1x10-3 5x10-4 1x10-4
at Cathode (A/cm2)
specified temperature, the operating cell voltage increases Current Density (A/cm2) 0.1 : 0.1 : 2.0
sharply at low current density and slowly thereafter with the
current density. At 40oC and 2A/cm2, an operating voltage of 3.3.1. Cell Relation Analysis
2.11 V was achieved. However at higher temperature (80oC), Figure 2 shows relations between current and hydrogen flow
the operating cell voltage drops to 2.01V at 2A/cm2. This rate. It can be observed that as current increases, the hydrogen
constitutes about 4% reduction in operating cell voltage. The flow rate also increases. The simulation result shows a
main parameter responsible for the voltage drop is the maximum of the hydrogen flow rate at 1.1L/min at 160A.
decrease in ohmic resistances as temperature increases. That
is at high temperature the ohmic resistance is decreased and 3.3.2. Effect of Temperature on Resistance and Conductivity
this leads to decrease in operating cell voltage. The effect of of PEM
this result is that the operating cost of the electrolyzer Figure 3 shows the effect of temperature on resistance and the
decreases at higher temperatures due to lower power conductivity. The results indicate that as temperature
consumption. increases, there is a significant or sharp decrease in resistance
from 0.198Ω/cm2 at 40oC to 0.125Ω/cm2 at 80oC. However 3.3.3. Exchange current density effects
there is a small increase in conductivity. From this Figure 5 and 7 are the simulation result of the effect of
observation it can be concluded that the ionic conductivity of exchange current density on operating cell voltage. For
the membrane assembly increases with temperature and this example Figure 5 shows that as the exchange current density
can lead to increase in hydrogen flow rate. The result of the at the anode decreases, the operating cell voltage increases,
simulation in Figure 3 shows similar agreement with and this result obtained at a constant exchange current density
experimental data whose result shown in Figure 4 compares at the cathode. However the result shows that electrolysis
to the result obtain in Figure 3 shows the maximum value of system is able to operate at a lower operating cost when the
the equivalent resistance is 0.45Ω/cm2 at 40oC while the exchange current density is bigger. A similar result was
minimum value is 0.157Ω/cm2 at 80oC. The difference value obtained for a variety of exchange current density at the
is 0.293Ω/cm2. Even though both Figure 3 and 4 shows the cathode and constant exchange current density at anode.
similar pattern, the simulated resistance value has the lowest
amount of resistance compared to the resistance value in the 1 .9 5
C e ll V o lta g e (V ) vs C u rre n t D e n s ity (A /c m 2 ) a t A n o d e , io ,c a t = 1 0 - 3 A /c m 2

experiment.
1 .9

H y d ro g e n V o lu m e (L /m in ) vs C u rre n t(A )
1 .4 1 .8 5

C e ll V o lta g e (V )
1 .2 1 .8
H y d ro g e n M o la r F lo w R a te (L /m in )

1 1 .7 5

0 .8 1 .7
io a = 1 0 - 9 A /c m 2
0 .6 io a = 5 0 - 1 0 A /c m 2
1 .6 5
io a = 1 0 - 1 2 A /c m 2
0 .4
1 .6
0 0 .2 0 .4 0 .6 0 .8 1 1 .2 1 .4 1 .6 1 .8 2

0 .2 C u rre n t D e n s ity (A /c m 2 )

O ve ra ll C e ll H y d ro g e n V o lu m e (L /m in ) Figure 5: Simulated on exchange current density effect

0
0 20 40 60 80
C u rre n t (A )
100 120 140 160 variation at anode
Figure 2: Variation of hydrogen volume against current

R e s is ta n c e (O h m /c m 2 ), C o n d u c tivity (S /c m ) vs Te m p e ra tu re (C )
0 .2

0 .1 8
R e s is ta n c e (O h m /c m 2 ), C o n d u c tiv ity (S /c m )

0 .1 6

0 .1 4

0 .1 2
M A TL A B S im u la te d R e q (O h m /c m 2 )
0 .1
S im u la te d P E M c o n d u c tivity (S /c m )
0 .0 8

0 .0 6

0 .0 4

0 .0 2 Figure 6: Experimental result on exchange current density

0
40 45 50 55 60 65 70 75 80
effect variation at anode [7]
Te m p e ra tu re (C ) C e ll V o lta g e (V ) vs C u rre n t D e n s ity (A /c m 2 ) a t C a th o d e , io ,a n = 1 0 - 9 A /c m 2
1 .9 5
Figure 3: Simulated variation of equivalent resistance
conductivity with temperature 1 .9

1 .8 5
C e ll V o lta g e (V )

1 .8

1 .7 5

1 .7
io c = 1 0 - 3 A /c m 2

1 .6 5 io c = 5 0 - 4 A /c m 2

io c = 1 0 - 4 A /c m 2
1 .6
0 0 .2 0 .4 0 .6 0 .8 1 1 .2 1 .4 1 .6 1 .8 2
C u rre n t D e n s ity (A /c m 2 )

Figure 7: Simulated on exchange current density effect

variation at cathode

Figure 4: Experimental result of equivalent resistance

conductivity with temperature [6]
 This is equivalent to 26.35% reduction in operating cell
voltage.

3.3.5. Electrochemical cell validation

Figure 11 shows the effect of different exchange current
density at both anode and cathode on operating cell voltage. It
can be shown that at a lower exchange current density for
both anode and cathode, there is a corresponding increase in
operating cell voltage. However when the exchange current
density is increased, the operating cell voltage decreases. The
reason is that the water dissociation at the anode side is much
Figure 8: Experimental result on exchange current density slower and therefore it need higher exchange current density
effect variation at cathode [7] to initiate the reaction, when this condition is reached, the
operating cell voltage decreases. On the other hand, when the
The difference between Figure 5 and 7 is that, the operating exchange current density is smaller, the anode oxidation
cell voltage 1.89V that correspond to exchange current reaction requires a higher operating cell voltage.
density of 10-9A/cm2 is much higher compared with Figure 7
whose operating cell voltage that corresponds to exchange 2.8
C e ll V o lt a g e (V ) vs C u rre n t D e n s it y (A / c m 2 )

current density of 10-3A/cm2 is 1.86V is bigger compare to the 2.6

cathode. We can conclude from this result that the amount of
operating cell voltage at anode is much greater than at the
2.4 R e ve rs ib le V o lt a g e (V )
O h m ic D ro p (V )

cathode due to the oxidation effects at the anode. The results 2.2 C a t h o d e O ve rp o t e n t ia l(V )

C e ll V o lta g e (V )
A n o d e o ve rp o t e n t ia l o n P t -IrO 2 (V )

in Figures 6 and 7 follow similar agreement with 2

A n o d e O ve rp o t e n t ia l o n P t (V )

experimental data from [8] as illustrated in Figure 6 and 8. It 1.8

was clear that the anode reaction shows a slower reaction 1.6

compared to the reaction at the cathode. The reasons for this 1.4
phenomena is because of the water dissociation happen at
anode, since the water molecules breaking phenomena 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1
C u rre n t D e n s it y (A / c m 2 )
happens in anode site, which is means it required a lot of
Figure 9: Simulated variation analysis model comparison at
power to break the water molecule into hydrogen charges and
800c
the oxygen molecule. These explain all data value at anode is
much.

3.3.4. Voltage Combination Effect

In Figure 9, the simulation analyses show the effectiveness
for each overpotential with respect to exchange current
density. The line for each overpotential can be calculated
using the Eq. (22). As shown in Figure 9, the reversible
voltage remains constant as current density increases. The
increases in ohmic overvoltage are relatively small as current
density increases. The cathode overpotential increases
steadily by a small amount due to the fast kinetic reaction on
the cathode surface. The reaction at the anode is however
Figure 10: Experimental Result of Variation Analysis Model
slow and sluggish and the overall process is limited by the
Comparison [8]
oxygen evaluation reaction. This phenomenon causes the C e ll V o lta g e (V ) vs C u rre n t D e n s ity (A /c m 2 )
anode overpotential to increase quickly at low current density 2

and slowly increase after some time with current density. 1 .9 5

Comparing the anode and cathode reactions, it can be 1 .9

concluded that, the increase in the operating cell voltage

1 .8 5
(Vcell) of the electrolysis cell is mainly because of the slow
C e ll V o lta g e (V )

kinetics of the dissociation of water at the anode. As shown in 1 .8

Figure 9, an operating cell voltage of 2.58V was obtained at 1 .7 5

1A/cm2 and 80oC for Pt anode. In order to reduce the anode 1 .7 V c e ll1 a t io a = 1 - 9 A /c m 2 , io c = 1 - 3 A /c m 2
polarization effects, iridium-oxide (IrO2) was added to Pt. V c e ll2 a t io a = 5 - 1 0 A /c m 2 , io c = 5 - 4 A /c m 2
1 .6 5
Ioroi et al. [10] reported that addition of IrO2 to Pt at anode, V c e ll3 a t io a = 1 - 1 2 A /c m 2 , io c = 1 - 4 A /c m 2

can increase the efficiency of water electrolysis from 77% to 1 .6

0 0 .2 0 .4 0 .6 0 .8 1 1 .2 1 .4 1 .6 1 .8 2

95% at 300mA/cm2. Thus, with IrO2-Pt electrode at anode, C u rre n t D e n s ity (A /c m 2 )

the operating cell voltages drop to 1.9V at 1A/cm2 and 80oC. Figure 11: Variation of simulated analysis cell voltage
4. Conclusions [8] P. Choi, "A simple model for solid polymer electrolyte
(SPE) water electrolysis," Solid State Ionics, vol. 175, pp.
In this paper, the mathematical model for simple PEM 535-539, 2004.
electrolyzer has been developed based on a combination of [9] F. Marangio, M. Santarelli, and M. Cali, "Theoretical
fundamental thermodynamic and electrochemical relationship. model and experimental analysis of a high pressure PEM
Different operating conditions such as exchange current water electrolyser for hydrogen production,"
density, temperature and current density have been analyzed International Journal of Hydrogen Energy, vol. 34, pp.
for optimized hydrogen production of polymer electrolyte 1143-1158, 2009.
membrane electrolyzer system. It can be concluded from this [10] T. Ioroi, K. Yasuda, Z. Siroma, N. Fujiwara, and Y.
paper that when the operating temperature of the electrolyzer Miyazaki, "Thin film electrocatalyst layer for unitized
system increases, the ohmic resistance decreases. And this regenerative polymer electrolyte fuel cells," Journal of
leads to increase in ionic conductivity in the membrane. Power Sources pp. 583-587, 2002.
Therefore in order to increase the hydrogen flow rate, it is
important to operate the electrolyzer system at the relatively
high temperature.
Acknowledgements
The financial support of the given for this work by the
Universiti Teknologi MARA under the Tabung Amanah HEP
and Tabung Amanah Pembangunan Akademik HEA in the
year of 2012 for this research development and also MOE
FRGS grant (600-RMI/FRGS 5/3 (54/2012)) for supporting
this manuscript is gratefully acknowledge.

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