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Effect of KOH Concentration in the Gel Polymer
Electrolyte for Direct Borohydride Fuel Cell
Pao Ling Ng,1 Aliyah Jamaludin,1 Yatimah Alias,2 Wan Jefrey Basirun,2
Zainal Arifin Ahmad,1 Ahmad Azmin Mohamad1
1
Department
2
of Chemistry, Universiti Malaya, 50603 Kuala Lumpur, Malaysia
School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia,
AQ2 14300 Nibong Tebal, Penang, Malaysia
Received 14 January 2011; accepted 8 April 2011
DOI 10.1002/app.34666
Published online 00 Month 2011 in Wiley Online Library (wileyonlinelibrary.com).
ABSTRACT: The performance of a direct borohydride
fuel cell (DBFC) based on a polyacrylamide (PAAm) gel
polymer electrolyte system is investigated at different electrolyte concentrations. The DBFC, constructed using 2M
sodium borohydride (NaBH4) as the fuel and potassium
hydroxide (KOH) solution gelled with PAAm as the electrolytes yield the highest electrical conductivity of 2.73 !
10"1 S cm"1 at 6M KOH. The optimized composition,
PAAm þ 2M NaBH4 þ 6M KOH, and the selected composition, PAAm þ 2M NaBH4 þ 3M KOH are then used in
INTRODUCTION
A fuel cell is an electrochemical energy conversion
device that directly converts hydrogen and oxygen
into water to produce electricity.1,2 High interest in
fuel cell technology development is attributed by its
capability to generate high power density, silently,
and environmental friendly.3,4 There are several
types of fuel cells classified by operating temperature and the type of electrolyte used. For the direct
borohydride fuel cell (DBFC), the liquid electrolyte
used consists of potassium hydroxide (KOH) and a
fuel solution of borohydride-based salt, i.e., potassium borohydride (KBH4)5 or sodium borohydride
(NaBH4).6–8 Meanwhile, the source of oxygen is
obtained freely from the air through the gas diffusion layer. However, the leakage and evaporation of
the liquid electrolyte caused by technical assembly
of the components has been a critical factor for longterm practical operation and causes substantial problems for putting liquid electrolytes into practical use.
To reduce leakage and evaporation problems of this
conventional system, gel polymer electrolytes (GPEs)
Correspondence to: A. A. Mohamad ([email protected]).
Contract grant sponsor: USM-RU Grant; contract grant
number: 811103.
Contract grant sponsor: USM-RU-PRGS; contract grant
number: 8031001.
Journal of Applied Polymer Science, Vol. 000, 000–000 (2011)
C 2011 Wiley Periodicals, Inc.
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preparing the cells. Open-circuit voltages for fuel cells is
about 0.85–0.92 V, and the discharge characteristic produce
discharge capacities of about 257.12–273.12 mAh cm"2 for
cells with PAAm-6M KOH. Current-voltage and current
density-power density plots and internal resistance for
C 2011 Wiley Periodicals, Inc. J
both cells are almost the same. V
Appl Polym Sci 000: 000–000, 2011
Key words: sodium borohydride; gel polymer electrolyte;
potassium hydroxide; alkaline fuel cell
can be introduced into DBFC systems. In fuel cells
or other electrochemical device applications, the
most important properties GPEs need to show are
high ionic conductivity and the ability to sustain
high electrochemical activities.
Polyacrylamide (PAAm) is a polymer formed
from acrylamide subunits that can also be readily
crosslinked. PAAm is a nontoxic polymer. Thus, it is
suitable to be used in wide range of applications such
as in contact lenses industry. PAAm dissolved in
water and produce gel-like characteristic. It is highly
water-absorbent, making it suitable to be employed
as polymer host. The ability of PAAm to entrap water
makes it a good candidate for forming the GPE in
fuel cell applications. Studies on PAAm-based hydrogels with a phosphoric acid (H3PO4) and potassium
carbonate (K2CO3) additives systems have already
demonstrated the ability to be good proton conductors, with conductivities exhibited in the range of
10"3 to 10"1 S cm"1 at ambient temperature.9,10
Since PAAm behaves as a good polymer host for
producing GPEs, optimum compositions of the
PAAm þ NaBH4 þ KOH electrolyte system are prepared in this study to obtain relatively high ionic
conductivity. The effects of different KOH concentrations on fuel cell performance are investigated
incorporating with NaBH4. The electrochemical
properties of the DBFCs are presented through
open circuit voltage (OCV), discharge characteristics, current-voltage (I-V), and current densitypower density (J-P) measurements.
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NG ET AL.
Figure 1 Schematic illustration of a gel polymer electrolytebased alkaline fuel cell. [Color figure can be viewed in the
AQ3 online issue, which is available at wileyonlinelibrary.com.]
Experiment
KOH (Merck) and PAAm (Polysciences, INC., Mw ¼
5,000,000) were used as the starting materials in the
preparation of the gel electrolytes. The GPE solutions were prepared according to the following
steps. PAAm (0.5 g) was first dissolved in 20 mL
distilled water. After the polymer was completely
dissolved, 20 mL of KOH solution at different concentrations (expressed as molarity values) was
added, and the two solutions were mixed by stirring
continuously at room temperature (25% C). When
complete homogenization of the mixture was
obtained, a fixed amount of NaBH4 (2M) was then
added to the resulting solution. The compositions of
the samples were PAAm þ 2M NaBH4 þ x M KOH,
where x ¼ 0, 1, 2, 3, 4, 5, 6, 7, and 8.
For the conductivity measurement, samples of
GPE with different concentrations were connected to
a frequency response analyzer (FRA) module in an
Autolab PGSTAT 30 system (Eco Chemie, B.V.).
Stainless steel (SS) electrodes having a spacer for
holding the GPE were used for conductivity cells.
Ionic conductivity (r) was calculated from the bulk
resistance (Rb) obtained from the impedance spectrum in a frequency range of 0.1 Hz to 1 MHz with
an amplitude of 0.01 V.
The commercial anode C/Ni (ECT, UK) with an
active area of 16.0 cm2 and an air-cathode made of
MnOx/C/Ni (ECT, UK) with an active area of
16.0 cm2 were used for testing the fuel cell performance. The experimental set-up of the GPE-based
DBFC system for this work is shown schematically
F1 in Figure 1. A hollow cylinder with a cathode
attached to one of the open ends was placed inside
a plastic beaker containing an anode at the bottom.
Two wires connected to the anode and cathode
acted as terminals for measuring the current and
voltage of the fuel cell. The mixture of the gelled
electrolyte and fuel solution was then introduced
into the space between the anode and cathode. A
combined volume of 60 mL for the fuel plus electrolyte medium was used in the experiments, and it
was filled up to a certain level such that one side of
the cathode was in contact with the fuel and electrolyte mixture while the other side was exposed to air.
The oxygen present in the air acted as the oxidant.
An optimum concentration and intermediate conductivity values of the electrolytes were used in constructing DBFCs for comparison. The performances of
the cells were evaluated according to their OCV by
storing the cells in an open-circuit condition for 24 h
at 25% C and with discharge profiles at a constant current of 1.0 mA cm"2. The voltage and corresponding
current were measured at different loads to get the IV and J-P characteristic curves. Three cells were evaluated to obtain the average and standard deviation
values for all the cell characteristics.
RESULTS AND DISCUSSION
Analysis of PAAm 1 2M NaBH4 1 KOH
electrolytes
Figure 2 shows the impedance spectrum of the GPE
based on PAAm þ 2M NaBH4 at 0, 3, and 6M of
KOH. The interception of the impedance spectrum
on the real axis gives the bulk resistance (Rb) value.
It can be seen that the GPE without KOH gave a Rb
value of 2.625 X while the GPE with 6M KOH
Figure 2 Impedance spectrum for the PAAm-2M NaBH4
gel polymer electrolyte at different KOH concentrations at
25% C. [Color figure can be viewed in the online issue,
which is available at wileyonlinelibrary.com.]
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AQ1 EFFECT OF KOH CONCENTRATION
3
In DBFC applications, hydrogen (H2) must be supplied to the electrolytes with the addition of fuel solution. H2 is produced when NaBH4 is dissolved in
distilled water according to the reaction:
NaBH4 þ 2H2 O ! NaBO2 þ 4H2
(1)
Or else, eq. (1) also can be explained in detail to eq.
(4) through eq. (2) and (3):
"
BH"
4 þ 2H2 O ! BO2 þ 4H2
(2)
Then, the hydrogen will react to release electrons
Figure 3 Effect of the KOH concentration on the conductivity of gel polymer electrolytes containing 2M NaBH4 at
25% C. [Color figure can be viewed in the online issue,
which is available at wileyonlinelibrary.com.]
yielded lower results than the GPE with 3M KOH,
at 0.713 and 1.168 X, respectively. This decreasing
pattern of Rb is due to the increasing of the charge
carrier, hydroxyl ions (OH") with the addition of
KOH. These mobile ions reduce the ionic resistance
and increase the conductivity of the GPE. Moreover,
the inhomogeneous of electrode–electrolyte surface
contacts is the reason why the Nyquist plot shown
in Figure 2 is nonvertical. The interface between
electrode and electrolyte can be regarded as a
capacitance where the blocking electrode is used to
analyze the impedance spectrum. An ideal capacitance should posses a vertical line with an angel of
90% . However, the angles of y1, y2, and y3 are
slightly lower, at 70, 70, and 80% , respectively, but
they are better than those of solid state KOH-based
electrolytes.11
The variation of the conductivity of PAAm þ 2M
NaBH4 as a function of KOH concentration is given
F3 in Figure 3. It is apparent that the conductivity of
GPE increases with increasing KOH concentration.
The conductivity of PAAm þ 2M NaBH4 without
any addition of KOH is (0.52 6 0.22) ! 10"1 S cm"1.
With 3M KOH added, the conductivity value is (1.73
6 0.02) 10"1 S cm"1. The highest GPE conductivity
value is (2.73 6 0.14) ! 10"1 S cm"1 at 6M KOH
concentration added. This conductivity value is comparable with other PAAm gels giving conductivity
values in the range of 10"3 to 10"2 S cm"1.9 These
results are also in agreement with other polymerKOH-based GPEs.12 However, beyond a 6M KOH
concentration, the conductivity values are slightly
decreased. It is a common understanding that the
formation of ion multiples between high concentration free ions can occur, and this contributes to
decreasing charge carrier. Decreases in ion mobility
affect the conductivity of KOH based electrolytes at
high concentrations.13
H2 ! 2Hþ þ 2e"
(3)
Therefore, eq. (1) also can be written as:
"
þ
"
BH"
4 þ 2H2 O ! BO2 þ 8H þ 8e
(4)
After the addition of KOH into the system, the
reaction take place at the anode is as shown in
eq. (5):
"
"
"
BH"
4 þ 8OH ! BO2 þ 6H2 O þ 8e
(5)
Spontaneously, cathodic reaction also occurs
between oxygen from ambient air with water shown
in eq. (6):
O2 þ 2H2 O þ 4e" ! 4OH"
(6)
From eq. (5), it can be explained that the hydrogen
supplied by the fuel reacts with the OH" supplied
by KOH to produce water and release the electrons.
OH" is the main ionic conductor in the GPE that diffuses continuously between the electrodes. Therefore, even the PAAm þ NaBH4 GPE without the
addition of KOH give a conductivity value [(0.52 6
0.22) ! 10"1 S cm"1]; however, it is critical to supply
OH" to the GPE to complete the chemical reaction.
At higher concentrations of added KOH, there are
more OH" ions available for conduction since most
solutions have conductivity proportional to the ion
concentration. Since GPE was used, the ionic conduction is related with the polymer host. For a polymer to be an optimum ionic conductor, it should
posses the presence of fixed charge sites.14 PAAm as
the polymer host has accommodated the fixed
charge sites with Hþ, where the moving OH" can be
temporarily accepted and released. PAAm exhibits
better properties as a polymer host since it yields
higher conductivity as compared with the chitosan
used in the direct methanol fuel cell by Cui et al.15
However, when a certain concentration is reached,
the conductivity will decrease because of the restricted ion mobility. At concentrations greater than
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NG ET AL.
Figure 4 The open circuit measurement of direct borohydride fuel cells with PAAm-2M NaBH4-KOH gel polymer electrolyte for 24 h of storage. [Color figure can
be viewed in the online issue, which is available at
wileyonlinelibrary.com.]
6M, the conductivity of KOH decreases due to the
solvation of the Kþ ions significantly impacting the
amount of unbound H2O molecules in the GPE.16
Consequently, the GPE resistance will increase and
will reduce the conductivity.
Cell characterization
F4 Figure 4 presents the OCV characteristic of the 2M
NaBH4 DBFC based on PAAm-3M KOH and
PAAm-6M KOH electrolytes. The OCV values of the
cells were at 0.92 and 0.90 V for the PAAm-3M
KOH and PAAm-6M KOH, respectively. The results
for the OCV of both cells with different KOH concentrations remained steady during 24 h of storage
without any significant drops. The range of this
OCV result is comparable with the values of other
reported DBFCs, at about 0.9 V.5
F5
Figure 5 shows the discharge characteristic at a
constant current of 1.0 mA cm"2 as a function of
time for the cells. It is clearly seen that the discharge
time of the cell using the PAAm-3M KOH electrolyte
is 17 h, slightly longer than that of the cell employing PAAm-6M KOH electrolyte at 16 h. The average
nominal voltages at the flat plateau region range
from 0.70 to 0.90 V for both the fabricated cells with
3M and 6M KOH concentrations before hitting cutoff
voltages of 0.80 and 0.70 V, respectively. It was also
observed that the voltages decrease slightly in the
plateau region, which may be due to the concentration polarization caused by reactant depletion or
product accumulation within the cell.14 The voltage
abruptly decreased after the cutoff voltage where the
cell is completely discharged. The calculated discharge capacities obtained were 273.12 and 257.12
mAh cm"2 for 3M and 6M concentration of KOH,
respectively. Such low discharge efficiency is prob-
ably due to the crossover of reactants resulting
because fresh fuel and electrolyte were not continuously fed to the DBFC, as demonstrated by Verma
and Basu.6 Efficient delivery of fuel and electrolyte
can be accomplished by feeding them continuously
to the DBFC. However, in this work, since the
experiment was set up to study the abilities of a
fixed amount of PAAm- NaBH4-KOH, the system
did not include tanks for the fuel and electrolyte.
Figure 6 gives the I-V and J-P curves for the
PAAm-based gel electrolyte DBFCs with 3M and 6M
of KOH. It was observed that the increase in KOH
concentration from 3 to 6M results in slightly higher
I-V and J-P characteristics, and this means that the
performance of the cell with a 6M concentration of
KOH system improves slightly compared with the
cell employing 3M KOH as the electrolyte. From Figure 6 it is expected that the internal resistance (r) of
the cell using the optimum composition of electrolyte (6M KOH) was slightly lower than that of the
cell using 3M KOH, with values of 3.02 and 3.05 X,
respectively. The small difference in the r values of
both cells shows that different KOH concentrations
do not produce significant affects in the ionic resistance of the cells. Once again, this proves that PAAm
is a good polymer host as it provides large free volumes for the OH" to move across and therefore
decreases the intrinsic resistance in the electrolyte.
Furthermore, the highest power densities shown by
the cells with 3 and 6M KOH as electrolytes are
almost the same, namely, 4.27 and 4.92 mW cm"2,
respectively, as shown in Figure 6. However, at
highest current density of 16.25 mA cm"2, cell with
6M KOH performed higher power density of 3.45
mW cm"2. As compared to cell with 3M KOH which
gave 1.96 mW cm"2 at same current density, cell
with 6M KOH is more suitable for application that
needs higher current. The works by Haijun et al.17
and Verma and Basu6 also found that the addition
Figure 5 Discharge characteristic of direct borohydride
fuel cells with PAAm-2M NaBH4-KOH gel polymer electrolyte. [Color figure can be viewed in the online issue,
which is available at wileyonlinelibrary.com.]
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EFFECT OF KOH CONCENTRATION
5
value at 6M of KOH addition. For further comparisons, the intermediate conductivity value of 3M
KOH was also studied. On the basis of cell characterizations, the performances of DBFCs with 3 and
6M KOH were just slightly different. With regards
to power density performance, cell with 6M KOH
has an advantage over cell with 3M KOH since it
produced more than 50% power density at highest
current density. From an economics point of view,
the cost of NaBH4 which matter most, so fixed
amount of NaBH4 was used in this work. At low
and higher currents, the significant differences of
power densities of the DBFCs with different KOH
concentrations recovered had much more economic
interest than the more affordable KOH used.
References
Figure 6 Plot of I-V and J-P for direct borohydride fuel
cells with PAAm-2M NaBH4-KOH gel polymer electrolyte.
[Color figure can be viewed in the online issue, which is
available at wileyonlinelibrary.com.]
of NaOH and KOH have their certain optimum values, but those are not at the highest points of
conductivity.
CONCLUSIONS
PAAm-based gel polymer electrolytes containing 2M
NaBH4 and different concentrations of KOH have
been prepared and gave the highest conductivity
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