Applied Energy 125 (2014) 189196

Contents lists available at ScienceDirect

Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Design of a photochemical water electrolysis system based on a W-typed

dye-sensitized serial solar module for high hydrogen production
Byeong Sub Kwak a, Jinho Chae b, Misook Kang a,
a
b

Department of Chemistry, College of Science, Yeungnam University, Gyeongsan, Gyeongbuk 712-749, Republic of Korea
Samsung Sumitomo LED Materials, Secheon-ro 2-gil, Dasa-eup, Dalseong-gun, Daegu 711-814, Republic of Korea

h i g h l i g h t s

g r a p h i c a l a b s t r a c t

 A W-typed dye-sensitized serial solar

module was designed for hydrogen

production from water electrolysis.
 The serial module assembled by ve
unit cells showed the overall
conversion efciency of 4.56%.
 When the connected numbers of unit
cells increased, the obtained voltages
were improved.
 When the ve column fabricated Wtyped DSSM was used, 2.1 mL h1 of
hydrogen gas was emitted.
 The actual light-hydrogen conversion
was calculated to be 2.02%.

a r t i c l e

i n f o

Article history:
Received 2 September 2013
Received in revised form 3 March 2014
Accepted 8 March 2014

Keywords:
Hydrogen production
Water electrolysis system
W-typed dye-sensitized serial solar module
Voltage

a b s t r a c t
A W-typed dye-sensitized serial solar module (W-typed DSSM) was designed for hydrogen production
from water electrolysis. The optimal thickness and width of the TiO2 electrode lm were 12 lm and
5 mm, and the optimal thickness of Pt counter electrode lm was 4 nm, respectively. The photocurrent
density, open circuit voltage, and ll factor were 2.13 mA cm2, 3.51 V, and 0.61, respectively, for a serial
module assembled from ve unit cells, which resulted in an overall conversion efciency of 4.56%. The
obtained voltage increased with increasing number of unit cells connected, and was 3.51 V in the ve column fabricated W-typed DSSM. 2.1 mL h1 of hydrogen gas was emitted when a W-typed DSSM assembled from ve columns was connected to carbon electrodes in a water electrolysis system. The rate of
hydrogen evolution in the ve columned W-typed DSSM was 0.00213 L h1. Therefore, the actual
light-hydrogen conversion was calculated to be 2.02%.
2014 Elsevier Ltd. All rights reserved.

1. Introduction
Many techniques have been used to produce hydrogen. Some
of these techniques include water electrolysis [1], natural gas
Corresponding author. Tel.: +82 53 810 2363; fax: +82 53 815 5412.
E-mail address: mskang@ynu.ac.kr (M. Kang).
http://dx.doi.org/10.1016/j.apenergy.2014.03.012
0306-2619/ 2014 Elsevier Ltd. All rights reserved.

reforming [2], coal gasication [3], etc. Although some of these

methods, such as water electrolysis, are efcient in terms of hydrogen recovery, there has been considerable interest in developing a
desirable method for the next generation of energy sources
because of its environmentally friendly manner. However, the
method is cost prohibitive and requires an energy intensive process. In addition, it makes them unsuitable for large scale hydrogen

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B.S. Kwak et al. / Applied Energy 125 (2014) 189196

production. For efcient water cleavage, the conduction band of

the n-type semiconductor needs to be positioned at a more
negative potential than the reduction potential of water, i.e.
Ecurrent < Ereduction (H2/H+), whereas the valence band needs to be
positioned at a more positive potential than the oxidation reaction,
i.e. Evoltage > Eoxidation (OH/O2). Although strong efforts have been
made to develop appropriate semiconductors [4,5], there is no
material that can simultaneously and efciently oxidize and
reduce water without external assistance.

H2 O energy solar ! H2 1=2O2 PEC reactor

A photoelectrochemical cell combines visible light harvesting
by a nanocrystalline semiconductor thin lm with the electrolysis
of water. Photons with energies higher than the band gap of the
semiconductor generates electronhole pairs in the conduction
and valence bands. At the semiconductor surface, holes oxidize
water to oxygen, whereas the photo-excited conduction band electrons are transferred to the counter-electrode of the PEC cell, and
reduce water to form hydrogen gas [68].
These devices, however, have very low conversion efciencies
because most of the semiconductors used for this application have
a large energy band gap. Furthermore, the band edge potentials of
many semiconductors are unsuitable for oxygen and hydrogen
evolution. To split water, a voltage of at least 1.2 eV is required.
On the other hand, the dye-sensitized solar cell in the current
study consisted of a parallel module, and the system did not exceed the maximum voltage of 0.8 eV [913]. Therefore, an efcient
hydrogen production system requires a serially connected unit cell
system to achieve the required voltage, 2.0 eV or more [14,15].
Although this can be achieved easily in the case of a silicon solar
cell, which has achieved more than 18% efciency, the cost of silicon solar cells is too expensive and they are inexible. Therefore,
the race to the development of hydrogen technology has expanded
worldwide [16,17]. By Deng et al. [18], a hybrid amorphous silicon/
photoelectrochemical multi-junction cell for hydrogen production
was designed, and resulted that the triple-junction amorphous silicon (a-Si) solar cells exhibited photovoltaic (PV) efciencies up to
12.7% and open-circuit voltages up to 2.3 V. In a recent development, the race to development hydrogen technology has expanded
beyond the global realm. Mendes et al., reported [19] about dyesensitized solar cells in a tandem arrangement for hydrogen
production by water splitting; they connected two DSCs in serious
operating to cleavage of water, and the effective conversion for

solar and hydrogen were 8.5% and 1.12%, respectively. In addition,

Kim et al. [20] reported the production of 400 mmol hydrogen for
5 h in a light-assisted electrolysis cell operated with a dye-sensitized solar cell. Nevertheless, the system to increase the voltage
of the solar cells was connected in several layers but the hydrogen
production efciency was low. In addition, there was no mention
of the most efcient conditions. Therefore, a more efcient and
simple design is needed for commercialization.
To observe photo-assisted hydrogen production in a photoelectrochemical water splitting system in this study, a photoelectrochemical water electrolysis system that can separate hydrogen
and oxygen gases was designed based on the serial module of
dye-sensitized solar cells. There are typically several serial modules [2123]. In particular, the W-type [24,25] was a well-known
process as the simplest and the position of the electrode structure
with a staggered zigzag, as shown in Scheme 1. A W-typed dyesensitized serial solar module (W-typed DSSM) was also fabricated
in this study. To determine the optimal conditions for high hydrogen evolution, the cell thickness and numbers, and thickness of the
Pt counter electrode were fabricated differently and their impedances were estimated.
2. Experimental
2.1. Design of W-typed dye-sensitized serial solar module (W-typed
DSSM)
To determine the optimal conditions of the module, the unit cell
width, thickness of the TiO2 lm and Pt concentration in the counter electrode were varied. Scheme 2 shows the fabrication process
of the module. First, the FTO glass with a unit surface resistance of
10 X/h was cut to the correct size and dry-etched to prepare the
insulation. The columns were placed on two sides on the center
insulator. Using Ag paste, the two cells were connected and placed
on both sides of the electrodes in the W-type, and a TiO2 paste
(solvothermally synthesized [26] was cross-coated on the FTO
glass substrate and burned for 30 min at 450 C. To prepare TiO2
pastes for the working electrode lms in DSCs, 2.0 g of TiO2 powder
was mixed in a solution consisting of 5.0 g of a-terpineol, 0.5 g of
cellulose, and 20 mL of ethanol. The white colored sol-mixture
was sonicated at a power density of 1200 W cm2 for 24 h. After
the thermal treatment, the TiO2 lm was immersed in the dye
solution formed from 0.3 mM Ruthenium 535 bis-TBA (N719Solaronix SA) for 12 h. The Pt lm for the counter electrode was
coated by ion sputtering (Ion Sputter; Hitachi, E-1030), and the
Pt layer was deposited, carefully avoiding the parts including the
TiO2 lm and isolated part. The Pt lm thickness was controlled
by the sputtering time. A 30 lm thick thermo-hot-melt sealing
sheet was placed between the two electrodes, TiO2 electrode and
a Pt counter electrode, and heated and pressed to 110 C for 10 s.
The electrolyte, iodolyte AN-50 (Solaronix SA), was injected into
the cell through a pin-hole. The pin-hole was then covered using
a glass seal. Finally, a W-typed dye-sensitized serial solar module
was completed.

Glass
TCO
Dye with TiO2
Platinum
Electrolyte
Sealing
Scheme 1. Structure of a W-typed dye-sensitized serial solar module assembled in
this study.

2.2. Photovoltaic efciency of W-typed dye-sensitized serial solar

module
The photocurrentvoltage curve was tested by installing the
voltmeter, ammeter and a variable load between the two electrodes. The electrostatic voltmeter and lock-in amplier were used
and a 150 W Xenon lamp as a light source was adjusted to be similar to the AM-1.5 emission intensity. The light intensity was measured using the power analyzer and thermal smart-sensor. The
voltagecurrent curve were obtained from the open-circuit voltage

B.S. Kwak et al. / Applied Energy 125 (2014) 189196

191

Scheme 2. Fabrication process of the W-typed dye-sensitized serial solar module.

(Voc), short circuit current (Jsc), and ll factor (FF), and the solar energy conversion efciency (g) was evaluated using Eqs. (1) and (2),
respectively [27].

FF J max:power point  V max:power point =J sc  V oc

g% P out =Pin  100

J max:power point  V max:power point =Pin  100
J sc  V oc  FF

The interfacial resistance at the open circuit voltage was measured by recording the impedance behavior at frequencies ranging
from 100 kHz to 0.1 Hz using an impedance spectroscopy analyzer,
and voltage amplication was maintained at 10 mV. In general, to
increase the efciency of the module, the interfacial resistance
should be lowest under all conditions. Therefore, these variables
in the width and thickness of the TiO2 lm and Pt lm thickness
were tested to determine the best conditions for preparing the
module. In the rst step, the width of the TiO2 lms were changed
to 5, 7.5, 10, and 15 mm, and the TiO2 thicknesses in the second
step were adjusted to 4, 8 and 12 lm after nding the optimal
TiO2 width with the lowest interfacial resistance and setting the
width of TiO2. At the same time, the thickness of the Pt lm was
varied (4, 8, 12, and 16 nm), and their impedances were measured.
The impedances of the assembled modules were measured under a range of conditions to determine the optimal conditions with
high photovoltaic efciency. Electrochemical impedance spectra
(EIS) to test the cell resistances were obtained under the same conditions at AC frequencies ranging from 0.1 to 100 kHz and an
amplitude of 10 mV using a CompactStat electrochemical interface
(IVIUM STAT technology). The applied bias voltage and AC amplitude were set to the Voc level of the DSC.
2.3. Hydrogen production using a photochemical water electrolysis
system based on W-typed dye-sensitized serial solar module
A photoelectrochemical system was designed based on the serial module of dye-sensitized solar cells to separate the hydrogen

and oxygen gases from water splitting. As shown in Fig. 1, the

W-typed dye-sensitized serial solar module was connected to
two carbon electrodes (anode and cathode) and water splitting
was performed by electrolysis. The hourly hydrogen emissions
were calculated to the optical-hydrogen conversion efciency. Before calculating the light-hydrogen conversion efciency, there is
normally an assumption that all the current generated from the
W-typed dye-sensitized serial solar module transfers completely
to hydrogen generation by water splitting. Therefore, the actual
efciency of hydrogen generation is likely to be lower than the
theoretical value. In addition, the calculated efciency of a photoelectrochemical cell differs according to the system type. First, the
light-hydrogen conversion efciency was calculated using the following equation [28]:

lSTH 100%  Jsc  V oc =Pin

where Jsc, Voc and Pin mean the photocurrent density of each photoelectrode, optical voltage, and intensity of the light source (input
power, 100 W cm2 in this study), respectively. This equation assumes that 100% of the current generated from the solar electrode
is used for hydrogen production. Thus the efciency maybe is lower
than the calculated efciency because it depends on the actual
light-hydrogen conversion according to Eq. (3). Therefore, the most
obvious method for calculating the actual the hydrogen generation
efciency is to measure how much light energy is converted to
hydrogen. A comparison of the light energy intensity and hydrogen
produced is needed. The hydrogen production efciency can be calculated using the following equation [16]:

lSTH DGH2 O  RH2 =Pin  A;

where DG (H2O) is the standard free enthalpy (237.141 kJ mol1), R

(H2) is the hydrogen generation rate (hydrogen production rate,
L h1), Pin is the intensity of the light source (input power,
100 mW cm2 in this study), and A is the mean irradiated area (irradiated area, 0.0025 m2 in this study).

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B.S. Kwak et al. / Applied Energy 125 (2014) 189196

Fig. 1. Apparatus of a photochemical water electrolysis system based on a W-typed dye-sensitized serial solar module for high hydrogen production designed in this study.

Fig. 2(b) presents TEM images of the TiO2 particles. Spherical

TiO2 particles were observed with a mean particle diameter of
715 nm.

3. Results and discussion

3.1. XRD and TEM analysis of solvothermal synthesized TiO2 particles
used in TiO2 paste

3.2. Impedance measurements on the assembled modules in various

conditions to nd the best conditions with high photovoltaic efciency

X-ray diffraction (XRD, MPD, PANalytical) using nickel-ltered

Cu Ka radiation and transmission electron microscopy (TEM,
H-7600, Hitachi) at 120 kV were used to characterize the solvothermally synthesized TiO2 powders. Fig. 2(a) shows the XRD patterns of the synthesized TiO2 particles. All peaks were assigned to
anatase TiO2 (tetragonal phase JCPDS Card No. 86-1157). The XRD
patterns showed the main peaks at 25.32, 37.86, 48.06, 53.97,
55.09, 62.76, 68.70, 70.33, 74.19, 75.14, and 82.75 2h, which
were assigned to the (1 0 1), (1 0 3), (2 0 0), (1 0 5), (2 2 1), (2 0 4),
(1 1 6), (2 2 0), (1 0 7), (2 1 5), and (2 2 4) planes, respectively.

(b)

10

20

30

40

50

60

A(112)

A(204)

A(211)

A(200)

A(004)

Intensity (a.u.)

A(101)

(a)

The impedances of the W-typed dye-sensitized serial solar

module (W-typed DSSM composed of two cells), which were fabricated by adjusting three parameters, thickness and width of TiO2
lm and thickness of Pt electrode, were measured. Fig. 3(a) shows
the impedance according to the change in the width of the TiO2
lm (5, 7.5, 10, and 15 mm). The lengths of the TiO2 lms were a
constant 40 mm. The impedance spectrum of the W-typed DSSM
showed three semicircles over the frequency range, 0.1100 kHz.

70

2theta/CuKa
Fig. 2. XRD pattern (a) and TEM image (b) of solvothermally synthesized TiO2 powder.

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B.S. Kwak et al. / Applied Energy 125 (2014) 189196

(a)

(b)

14
12
10
8
6
4
2
0

10

20

30

40

50

60

70

Rs ()

R1 ()

R2 ()

R3 ()

5.0 mm

10.1

8.4

17.8

3.1

7.5 mm

11.9

7.2

19.8

5.4

10.0 mm

23.1

9.2

21.4

4.4

15.0 mm

28.7

12.4

20.6

4.2

Fig. 3. Nyquist plots (a) of impedances on the W-typed dye-sensitized serial solar module fabricated according to the width of TiO2 lm and the side view of coated TiO2 lm
(b).

The rst semicircle, R1, is related to charge transfer at the counter

electrode, and was measured in the kHz range. The second semicircle, R2, is related to electron transport at the TiO2/dye/electrolyte
interface in the range, 1100 Hz. The third semicircle, R3, related
to the Nernstian diffusion within the electrolyte in the low-frequency peak (in the mHz range) [29,30]. Here, the ohmic serial
resistance (Rs) is associated with the series resistance of the electrolytes and electric contacts in the W-typed DSSMs. These three
semicircles indicated the Rs, R1, R2, and R3 of an equivalent circuit,
as shown under the table. With the exception of R3, the values increased with increasing TiO2 lm width, particularly the Rs values,
which means that the ohmic serial resistance on FTO glass was signicantly larger, depending on the TiO2 lm width. The surface

(a)

14

resistance, Rs, had a close relationship with FTO glass. In general,

the surface resistance of FTO glass was an approximately 10 X
per unit area. Therefore, proportional increases are natural because
the entire area of FTO increases with increasing the width of TiO2
lms. On the other hand, Fig. 3(b) shows the side of the coated
TiO2 lm. This conrms that the TiO2 lm was attached stably to
FTO glass.
Fig. 4(a) shows Nyquist plots of the impedance measured when
the TiO2 thickness of 4, 8 and 12 lm in the modules was varied.
Here, the widths in all modules were xed to 5 mm, which have
the lowest Rs value (Fig. 3). Although the TiO2 thickness was increased, the circles for Rs, R1 and R3 did not increase. On the other
hand, a smaller R2 was observed when the TiO2 thickness was

22

(b)
5.4

12
20
10

5.3
18

8
6

5.2

16

5.1

4
14

2
0

10

20

30

40

50

60

70

12

5.0

Rs ()

R1 ()

R2 ()

R3 ()

10.1

16.3

20.5

8.9

10.3

16.2

15.4

9.6

12

10.6

17.5

13.2

8.4

10

12

4.9

Fig. 4. Nyquist plots (a) of impedance measured when TiO2 lm thickness of 4, 8 and 12 lm in the modules and the relationships (b) between TiO2 lm thickness,
photovoltaic efciency, and resistance.

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B.S. Kwak et al. / Applied Energy 125 (2014) 189196

greater. The thickness of the TiO2 lms was not considered in this
study when it was more than 12 lm due to lm lift-off from FTO
glass after the calcination process. On the other hand, the resistance decreased remarkably with increasing TiO2 lm thickness
(Fig. 4(b)), but the W-typed DSSM efciency decreased. In general,
the efciency increases with decreasing resistance in solar cells
which are connected in parallel. The efciency of W-typed DSSM
composed of two cells was 5.4% at a 12 lm TiO2 lm thickness
with a 5 mm TiO2 lm width.
Finally, by ion sputtering, the thickness of the Pt electrode was
adjusted by the sputtering time, 4, 8, 12, and 16 nm. Fig. 5(a) presents the impedance measurement in each module. The lowest
resistance was observed when the thickness and width of the
TiO2 lm were xed to 5 mm and 12 lm, respectively, as shown
in Figs. 3 and 4. In the Nyquist plot, the area of the semicircle increased with increasing Pt lm thickness, particularly for R1. This
means that a smaller Pt lm thickness results in a lower resistance
in W-typed DSSM. The optimum thickness was 4 nm. As shown in
Fig. 4(b), the resistance increased proportionally with increasing Pt
lm thickness, but the W-typed DSSM efciency decreased, as
shown in Fig. 5(b).
3.3. Photovoltaic efciency on the W-typed dye-sensitized serial solar
module and hydrogen production ability
Fig. 6(a) shows the IV curves and photoelectric efciencies on
the 2, 3, 4, and 5 columned W-typed DSSM assembled under the
optimum conditions with the lowest resistance, a 5 mm TiO2 lm
width, 12 lm TiO2 lm thickness, and 4 nm Pt electrode thickness.
The open circuit voltage (Voc) increased with increasing column
number, i.e. 1.42 V, 2.11 V, 2.88 V and 3.51 V for a 2, 3, 4, and 5 columned module, respectively. The increase in the number of columns in the serial module occurred in more than approximately
0.7 V increments. On the other hand, the current density was inversely proportional to the open-circuit voltage: 5.36, 4.04, 2.68,
and 2.13 mA cm2 for the 2, 3, 4, and 5-columned serial module,
respectively. On the other hand, the photovoltaic efciency was
not consistent, and was best in the three-columned W-typed DSSM
(photovoltaic efciency 5.11%), and the efciencies in the 4 and 5
column module decreased with increasing serial. These 2, 3, 4,

(a)

14

Fig. 6. IV curves and the photoelectric efciencies on the 2, 3, 4, and 5 columned

W-typed DSSM assembled at the optimum conditions.

and 5 columned W-typed DSSM were connected with a carbon

stick electrode in the photoelectrochemical system for water electrolysis. Consequently, the voltages were improved depending on
the number of unit cells connected in a serial module.
The Fig. 7 shows the hydrogen evolution when a 2, 3, 4, and 5
columned W-typed DSSM was used as the power supply, particularly at voltages more than 1.2 eV. The W-typed DSSM was
connected to each carbon electrode (both the anode and cathode
electrodes were the same as the carbon materials) for water

(b)

30

12

5.5

25

5.0

10
20

4.5

15

4
2
0

4.0

10

10

20

30

40

50

60

70

80

3.5

Rs ()

R1 ()

R2 ()

R3 ()

4 nm

10.2

8.3

18.9

10.3

8 nm

10.4

16.3

20.5

8.9

12 nm

10.8

20.0

22.5

9.3

16 nm

10.1

27.5

22

12.5

12

16

Fig. 5. Nyquist plots (a) of impedances on the W-typed dye-sensitized serial solar module fabricated according to the thickness of the Pt electrode lm and the relationships
and (b) between the thickness of the Pt electrode lm, photovoltaic efciency and resistances.

B.S. Kwak et al. / Applied Energy 125 (2014) 189196

195

The two cells were connected with Ag paste, and arranged in the
shape of a W character. To determine the optimal W-typed DSSM
for high hydrogen evolution, the TiO2 lm thickness and width,
and thickness of the Pt counter electrode lm were varied. The
photovoltaic efciency was not consistent, and was best in the
three-columned W-typed DSSM (photovoltaic efciency of
5.11%); the efciencies in the 4 and 5 columned modules decreased. The voltages increased with increasing number of unit
cells connected in a serial module, but the photocurrent decreased.
When the W-typed DSSM was connected to carbon electrodes
(both the anode and cathode electrodes were the same as the
carbon materials) in the water electrolysis system, hydrogen evolution increased with increasing number of unit cells connected.
Two types of equations for light-hydrogen conversion were
suggested, and a equation, lSTH = DG(H2O)  R(H2)/Pin  A was accepted in this study. As a result, the actual light-hydrogen conversions were calculated to be 0.38%, 0.67%, 1.15%, and 2.02% for the 2,
3, 4, and 5 columned W-typed DSSM, respectively. Overall, this
study shows that the hydrogen evolution can be increased using
a W-typed DSSM.

Acknowledgements

This work was supported by the National Research Foundation

of Korea (NRF) grant funded by the Korea government (MEST) (No.
2012R1A1A3005043), for which the authors are very grateful.

Hydrogen emission for an hour (mlh-1)

(a)

0.3

(b)

0.7

(c)

1.2

(d)

2.1

18
16
14
12
10
8

References
Fig. 7. Hydrogen evolution when the 2, 3, 4, and 5 columned W-typed DSSM were
used as the power supply.

splitting. Hydrogen evolution increased with increasing number of

unit cells connected, resulting in an increase in voltage. For a ve
serial module, hydrogen evolution reached 2.1 mL h1. The lighthydrogen conversions were calculated based on Eqs. (3) and (4)
in the Section 2. When the DSSM efciency in Fig. 6 was applied
to Eq. (3), the light-hydrogen conversions were 7.6%, 8.5%, 7.7%,
and 7.4% for the 2, 3, 4, and 5 columned W-typed DSSM, respectively. As commented in the Section 2, the actual efciency is lower
than the calculated efciency because it depends on the actual
light-hydrogen conversion according to Eq. (3). For example, from
the photocurrent of a solar cell efciency of more than 7%, the actual amount of hydrogen measured was 3.5%, showing a 50% loss of
efciency. Therefore, an attempt was made to obtain the lighthydrogen conversions using Eq. (4) and the slopes (hydrogen evolution rate) in Fig. 7. The R values (the slopes, L h1) for the 2, 3, 4,
and 5 columned W-typed DSSM were 0.00040, 0.00071, 0.00121,
and 0.00213 L h1, respectively. Therefore, the actual light-hydrogen conversions were calculated to be 0.38%, 0.67%, 1.15%, and
2.02%, respectively. This value, however, may contain many errors
because it is difcult to determine them precisely with a small
amount of hydrogen. The unique point where the efciencies obtained by Eq. (3) were similar regardless of the number of W-typed
DSSM connected in series, but the efciencies obtained by Eq. (4)
increased with increasing number of serial modules. In general,
the efciency should increase with increasing voltage. Therefore,
in this study, the light-hydrogen conversion efciency achieved
by the equation of the latter was considered to be more reliable.
4. Conclusion
This study evaluated the enhancement of hydrogen production
from water electrolysis using a W-typed dye-sensitized serial solar
module (W-typed DSSM). FTO glass with unit surface resistance of
10 X/h was cut to the correct size and dry-etched for insulation.
The columns were placed on two sides of the center insulator.

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