Transactions on Electrical and Electronic Materials Online ISSN 2092-7592

https://doi.org/10.1007/s42341-019-00158-y Print ISSN 1229-7607

REGULAR PAPER

Performance of Natural Dyes in Dye‑Sensitized Solar Cell

as Photosensitizer
Sujan Kumar Das1   · Sumon Ganguli2 · Humayun Kabir1 · Jahirul Islam Khandaker1 · Farid Ahmed1

Received: 28 May 2019 / Revised: 14 October 2019 / Accepted: 1 November 2019

© The Korean Institute of Electrical and Electronic Material Engineers 2019

Abstract
In this research work five types of titanium dioxide (­ TiO2) nanocrystalline sol–gel paste with three different types of dye
have been prepared and layered on Indium Tin-Oxide coated glass to fabricate dye-sensitized solar cells. The dyes extracted
from Malabar spinach seeds (MSS), Red spinach and Pomegranate burgs were used as photosensitizer. All the electrical
properties investigated by LCR meter were found to be improved with MSS dye but sample with 0.3 M ­HNO3 (sample-3)
exhibited the best electrical properties. The current–voltage characteristics for all the samples showed ideal behavior. The
highest maximum power of 176.3 μW and efficiency of 9.23% was found for sample-3 with MSS dye. The smallest crystal-
lite size was found to be 28.82 nm for sample-3 by XRD data which was also supported by the SEM results. Thus, this study
reveals that MSS dye has the great potential to be used as photosensitizer.

* Sujan Kumar Das

skdas@juniv.edu
1
Department of Physics, Jahangirnagar University,
Savar, Dhaka 1342, Bangladesh
2
Department of Applied Chemistry and Chemical
Engineering, University of Chittagong, Chittagong 4331,
Bangladesh

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Graphic Abstract
Keywords  Dye-sensitized · Solar cell · TiO2 · Electrical properties · Photosensitizer
1 Introduction
The world’s current energy consumption rate is ten thou-
sand times less than the sun provides [1]. Photovoltaic
cells are the device to utilize this huge resource and will
play a vital role in future sustainable energy system. Sili-
con based solid-state junction devices are dominating
photovoltaic solar energy converter due to their stability
and durability. Fabrication and design of crystalline or
amorphous silicon based solar cells are very expensive.
Hence the photovoltaic electricity production cost is still
high to compete with fossil or nuclear energy. The thin
film solar cells prepared by inorganic or organic semi-
conductors offer a very low cost fabrication and may be
attractive alternatives [2–5]. Instead of the flat morphology
used by conventional thin-film cells, inorganic or organic
semiconductor nanomaterials are used to form junctions
of very high contact area. The prototype of this family
of devices is the dye-sensitized solar cell (DSSC), which
accomplishes optical absorption and charge separation by
combining a light-absorbing material (the photosensitizer)
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Transactions on Electrical and Electronic Materials
with a wide band gap semiconductor of nanocrystalline
morphology [6, 7].
The DSSC is used in conjunction with ionic liquids
[8], electrolytes [9], polymer electrolytes [10] or organic
[11] as well as inorganic hole conductors [12–16]. Some
other DSSCs employ blends of organic materials, such as
polymeric [17], or molecular semiconductors [18] as well
as hybrid cells using a p-type semiconducting polymer, in
conjunction with a fullerene [19] or CdSe ‘nanorods’ [20].
Without expensive and energy-intensive high temperature
and high vacuum processes these DSSCs can be fabricated.
The DSSCs have large flexibility in its shape, color and
transparency which makes them the most potential technolo-
gies for photovoltaic applications [9, 21–27]. Currently, in
the laboratory, DSSCs have reached 13% efficiency under
standard reporting conditions [28, 29]. Excellent stability
under long-term illumination and high temperatures has
been reached fostering industrial applications.
The efficiency of solar cells is one of the most key factors
for solar cells. In order to become an efficient solar cell, the
photosensitizer must have the ability to absorb the available
Transactions on Electrical and Electronic Materials

light spectrum. Different photosensitizers have different
absorption of available light, thus a variation in efficiency
and cost [30]. The highly toxic ruthenium-based inorganic
dyes, which are expensive, are commonly used as photo-
sensitizer in solar cell due to their high absorption prop-
erty of solar spectra. Dyes extracted from natural sources
have attracted immense attention to use as photosensitizer
[31–38] for high light-harvesting efficiency, large absorp-
tion coefficients, low cost [23, 39, 40], easy preparation and
environment friendliness [41–50]. Natural dyes are extracted
from flowers and plants such as petals of male flowers Luffa
cylindrica L. [51], spinach [52], Aloe Vera and Cladode of
Cactus [53], R. luteola, B. integerrima, P. granatum Pleni-
flora, C. orientalis, R. gredensis, C. orientalis, A. flammea,
S. sclarea, and C. ajacis, etc. [54], red amaranth leaves [55],
red cabbage [56], turmeric plants root [57] and they have
been used as sensitizer in ­TiO2-based DSSCs.
In this work an attempt has been taken to investigate the
light absorbing power of some natural dyes extracted from
different plant leaves and fruits. The purpose of this study is
also to fabricate dye sensitized solar cells by a simple press-
ing technique and to examine the performance of natural
dyes extracted from Pomegranate burgs, Malabar spinach
seeds and Red spinach as sensitizer.
2 Experiments
2.1 Dye Extraction
Three types of natural dyes were extracted from Pome-
granate (botanical name Punica granatum), Malabar spin-
ach (botanical name Basella alba) seeds, and Red spin-
ach (botanical name Basella rubra L.). Pomegranate skin
was grinded down by mortar then 20 gm of them soaked
in 200 ml water and stirred 2 h by magnetic stirrer. Then
the dye was filtered. Malabar spinach dye was achieved by
blending the sample with a warming commercial blender to
obtain a slurry mixture. The slurry mixture was then filtered
subsequently. Red spinach dye was extracted by heating the
sample with water and then filtered. The dye extraction
involves the removal of water from the desired sample.
2.2 Preparation of ­TiO2 Paste
TiO2 sol–gel paste was produced in the laboratory using
nanocrystalline grade ­TiO2 powder. Following types of sam-
ple paste were produced as shown in Table 1 and then coated
on the conductive layer side of ITO coated glass.
2.3 Preparation of Electrode
At first the conducting side of Indium Tin Oxide (ITO)
coated glass was identified and keeping the conducting side
up, the glass on three sides was taped. Any fingerprints or
oils were wiped off using a tissue wetted with ethanol. The
titanium dioxide paste was then spread on the glass slide
using a glass rod by simple pressing technique. The tape
served as a 50–60 µm spacer to control the thickness of the
paste layer.
Carefully the tape was removed without scratching the
­TiO2 coating. This electrode was put on top of a hot plate
and heated it at approximately 350 °C for 3 h. Then the elec-
trode was soaked into the dye solution for overnight. After
taking out the ­TiO2/dye electrode from the dye solution it
was washed with fresh ethanol and dried at room tempera-
ture for a day.
A plastic film was cut having dimensions of 1.5 cm by
2 cm to get the counter electrode spacer. A hole on the film
was created. A spacer was then produced on conducting side
of mercury (Hg) coated counter electrode.
2.4 Preparation of Electrolyte
The iodine ( I − ) and triiodide ( I3− ) as a redox couple was used
as electrolyte. To get the iodide electrolyte solution, 0.05 M
0.064 g Iodine (I2) was dissolved in 10 mL of ethylene gly-
col and then added 0.5 M 0.83 g Potassium Iodide (KI).
The solution was stirred at room temperature and stored in
a dark container.

Table 1  Composition of different composite formulations

Chemicals sample TiO2 (gm) EtOH HNO3 PEG (ml) TiCl4 and 2-propanol Titan X-100 Ultra-
(1:4) mixture (ml) (ml) sonication
(min)

Sample-1 2 15 ml … … 0.5 … 40

Sample-2 2 … 2 ml 0.4 M 1.4 0.5 0.5 40
Sample-3 2 … 2 ml 0.3 M 1.4 3 0.5 40
Sample-4 2 … 2 ml 0.2 M 1.4 4 0.5 40
Sample-5 2 … 2 ml 0.1 M 1.4 5 0.5 40

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2.5 DSSC Assembling
Mercury (Hg) coated slide was placed face down on top
of the dry organic dye soaked ­TiO2 coated side of the sec-
ond slide. Two binder clips were used to hold the two sides
together (Fig. 1).
Then with an eyedropper one to two drops of liquid I −
/I3 electrolyte solution was added to the crease between the
−
two slides.
2.6 Characterization
2.6.1 Electrical Properties
The electrical properties (dielectric constant, capacitance
and impedance) of the samples were measured by Agilent
4263B LCR meter with the frequency ranges from 1 to
500 kHz at room temperature.
2.6.2 DC Current–Voltage (I–V) Measurements
The I–V characteristics of the dye sensitized solar cell can be
drawn using the circuit diagram by measuring both current
and voltage. Figure 2 illustrates a solar cell connected to the
circuit for I–V measurements.
Figure 3 shows a typical forward bias I–V curve of an
illuminated PV cell. The maximum power point ­(Pmax) is the
product of the maximum cell current ­(Imax) and the voltage
­(Vmax) where the power output of the cell is greatest. This
point is located at the “knee” of the curve. When the voltage
source is zero, the current is equal to the short-circuit current
­(ISC) and when the voltage source is an open circuit ­(VOC),
then the current is equal to zero.
The fill factor (FF) is a measure of how far the I–V char-
acteristics of an actual PV cell differ from those of an ideal
cell. The ideal solar cell has a fill factor equal to one but
losses from series and shunt resistances. The fill factor is
defined as [58]:
Fig. 1  Assembling of sensitize and counter electrode
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I V
FF = max max (1)
ISC VOC
The efficiency (η) of the solar cell can be defined as the
ratio of electrical power to the optical power incident on the
cell. It can be expressed as follows:
FF ⋅ ISC ⋅ VOC
η= (2)
Incident optical power
Incident optical power at the solar cell sample is
Incident optical power
P (3)
= × Illuminated surface area of the solar cell
4𝜋R2
where P is the power of the illuminating light source and R is
the distance of the light source from the surface of the solar
cell. In our experiment P is 60 W and R is 50 cm.
2.6.3 Scanning Electron Microscopy (SEM)
­ iO2 film
To investigate the morphology of the dye modified T
on glass plate, SEM (scanning electron microscopy) images
were obtained on a SEM instrument (FEI Inspect S 50)
equipped with a computer with relevant software. Surface
micrographs of the sample were obtained from computer.
Rh
V
A
Fig. 2  Experimental circuit diagram for I–V characteristics measure-
ment
Fig. 3  Typical forward bias I–V characteristics of a PV cell
Transactions on Electrical and Electronic Materials
2.6.4 X‑Ray Diffraction (XRD)
The structural properties of the samples were characterized
by a Bruker’s X-ray Diffractometer with Cu-Kα radiation
using the wavelength of 1.54178 Å. The powder diffrac-
tion technique was used with a primary beam of 40 kV and
30 mV for a 2θ scan recorded from 10° to 70° with the
sampling pitch of 0.02°. A nickel filter was placed in front
of the sample to reduce radiation. The crystallite sizes for
(101) plane of the films were calculated by using the Scher-
rer formula [59],
K𝜆
B= , (4)
𝛽 cos 𝜃
where B is the crystallite size, K is the constant known as
shape factor (K = 0.94), β is the full width at half maximum
(FWHM) in radian, λ is the X-ray wavelength, and θ is the
Bragg’s angle of diffracted rays.
The spacing between the crystal phases “d” was calcu-
lated using Bragg’s equation [60]
2d sin 𝜃 = n𝜆 (5)
The integrated intensity of the samples was investigated
by using the following equation:
Integrated intensity (I) = Peak height (h) × FWHM. (6)
3 Results and Discussion
Most of the data presented for electrical properties were
average values of at least five samples. Sometimes for the
confirmation of the result the same work had done more
than once.
3.1 Structural Analysis
The crystalline phase of synthesized nano-TiO2 films was
analyzed by XRD and their XRD patterns are shown in
Fig. 4a, b. The polycrystalline anatase phase was confirmed
by (101), (004), (200), (211), and (204) diffraction peaks
[61–63]. An XRD study of the layer detected only a crystal-
line phase of anatase.
Based on the peak widths shown in Table 2, the average
dimension of the crystallites was found to be about 32 nm.
XRD patterns of annealed films of ­TiO2 featuring diffraction
by the crystal planes of anatase [64, 65]. The higher intensity
peak was produced by the T ­ iO2 paste for (101) plane for all
the sample.
Sample-4 showed the highest crystallite size and sam-
ple-3 showed the lowest crystallite size. These results can
be gazed from the SEM data and fully support the d-spacing
value calculated from XRD data. From the figure it was clear
that sample-4 exhibited the lowest value and sample-3 had
highest value of inter-planar distance. These data agreed
very well with the data obtained from the morphological
study.
The integrated intensity of the films was investigated by
using the Eq. (4). From Fig. 5 it was seen that the integrated
intensity had the maximum magnitude for sample-4. Sam-
ple-2 exhibited the lowest integrated intensity.
3.2 Morphological Study
The morphological properties of the sample were studied
by taking the scanning electron microscopy (SEM) image.
The Fig. 6a–c are the images of the surface of the samples.
From these figures it was observed that the composites
were more uniformly distributed in sample-2. Sample-3
had more crack but had the lowest grain size. These results
agreed with the crystallite size obtained from XRD data.
3.3 Electrical Properties Study
3.3.1 Capacitance
The capacitance of five different DSSCs electrode with
respect to frequency from 1 to 500  kHz was measured.
Capacitance started decreasing with the increasing fre-
quency for all the samples. The large value of capacitance
at low frequency could be attributed to the interfacial polari-
zation caused by space charge and intermediate field distor-
tion. Figure 7a, b showed the variation of capacitance with
frequency in semi-log scale for sample-3 with different dyes
and for different samples with Malabar spinach seeds dye
respectively.
From Fig. 7b it was obvious that sample-5 had poor level
of capacitance in comparison with the other samples and
sample-3 had the maximum. Again sample-3 exhibited max-
imum capacitance for Malabar spinach seeds dye as shown
in Fig. 7a. The decrease in capacitance with the increase
in frequency could be explained as it loses the dielectric
behavior and shows semiconducting property.
3.3.2 Dielectric Constant
The dielectric constant showed a decreasing trend with
increasing frequency [shown in Fig. 8] which agreed with
the capacitance data. This is due to the dielectric dispersion
as a result of the lag of the molecules behind the alternation
of the electric field which was observed when frequency is
less than 10 kHz. Generally, the polarizability (α) increased
with the increase of dipolar moment, orientation and reori-
entation motion which is the cause to the decrease of dielec-
tric constant at higher frequency.
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Fig. 4  XRD pattern for a sample-2 and sample-3, and b sample-4 and sample-5

Sample-2 showed the maximum dielectric constant at 3.3.3 Impedance

lower frequency and sample-3 showed maximum at higher
frequency region for Malabar spinach seeds dye. From Generally, impedance decrease with increasing frequency
Fig. 8b it was clear that sample-3 had the highest dielectric due to the tendency of electric dipole to align along the
constant for Red spinach dye. electric field at higher frequency region. Figure 9a showed

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Table 2  XRD data for the Sample no. Peak height (h) 2 𝜃 (°) cos 𝜽 FWHM β (radian) Crystallite size (nm) d-spacing (Å)
different samples
2 1097.50 25.2352 0.9759 0.00446 33.2656 3.52923
3 1044.19 25.0876 0.9761 0.00515 28.8174 3.54966
4 1575.65 25.4278 0.9755 0.00446 33.2782 3.50294
5 1441.51 25.0221 0.9763 0.00466 31.8809 3.51339

Fig. 5  Variation of integrated
intensity for different samples

Fig. 6  SEM image for a sample-2, b sample-3, and c sample-4

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the variation of impedance with frequency for sample-3 reasonable because the low frequency AC field is not suf-
with three types of dye. From this figure it was clear that ficient to activate the charge carriers but with the increase
impedance was high at low frequency region and started to in frequency their mobility increases yielding the decrease
decrease with the increase of frequency. This behavior is in impedance. Sample-3 showed the smallest impedance

Fig. 7  Variation of capacitance with frequency for a sample-3 with three types of dye, and b different samples with Malabar spinach seeds dye

Fig. 8  Variation of dielectric constant with frequency for a sample-3 with three types of dye, and b different samples with Malabar spinach seeds
dye

Fig. 9  Variation of impedance with frequency for a sample-3 with three types of dye, and b different samples with Malabar spinach seeds dye

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for Malabar spinach seeds dye. This result was expected for
solar cell application.
From Fig. 9b it was obvious that sample-3 had the low-
est impedance and sample-2 had the maximum for Malabar
spinach seeds dye. Impedance results revealed that sample-3
with Malabar spinach seeds dye was the best for dye-sensi-
tized solar cell application.
3.4 DC Current–Voltage (I–V) Characteristics
The current–voltage (I–V) characteristic of the fabricated
dye-sensitized solar cell was measured using the circuit dia-
gram as shown in Fig. 2. The I–V curve showed the ideal
behavior. Figure 10a, b illustrated the I–V characteristics of
sample-3 with three types dye and of different samples with
Malabar spinach dye, respectively. Sample-3 with Malabar
spinach seeds dye exhibited maximum current as shown in
Fig. 10a and the maximum current was 505.3 μA for 0.1 V
which was lower than silicon type solar cell [66–68]. Com-
paring the results obtaining for different dyes it could be
concluded that Malabar spinach seeds dye was more efficient
than others.
Figure 10b revealed that sample-3 had the maximum cur-
rent where the sample-5 had the lowest. This result agreed
with the results obtained from impedance analysis.
According to Fig. 3 several solar cell parameters such
as short-circuit current ­(ISC), open-circuit voltage ­(VOC),
maximum current (­ Imax), maximum voltage (­ Vmax), maxi-
mum power ­(Pmax), and fill factor (FF) were determined
from the I–V curves of the fabricated dye-sensitized solar
cell. Table 3 showed the characterized parameters of the
different solar cells with Malabar spinach seeds dye as
sensitizer. Here the maximum power is the product of
maximum current ­(Imax) and the maximum voltage ­(Vmax).
From Table 3 it was clear that short-circuit, open-cir-
cuit voltage, maximum current, maximum power and effi-
ciency all these parameters were maximum for sample-3
with Malabar spinach seeds dye. It is quite inherence that
efficiency has strong dependency on the maximum power.
As maximum power is maximum for sample-3 with MSS
dye, it also has highest efficiency than other synthesized
samples. RS dye containing sample has better efficiency
than the reported [69]. Maximum power of 176.3 × 10−6 W
was the highest for sample-3 whose fill factor was the low-
est. Sample-3 with MSS dye showed maximum efficiency.
Different solar cell parameters were determined also
for sample-3 with different dyes according to the previ-
ously discussed technique. These parameters were listed
in Table 4. From these results it was obvious that sample-3
showed better result for Malabar spinach seeds dye for all
the parameters.

Fig. 10  I–V characteristics for a sample-3 with different dyes, and b different samples with Malabar spinach seeds dye

Table 3  Solar cell parameters of the different dye-sensitized solar cells with MSS dye electrolyte
Sample ISC (μA) VOC (V) ISCVOC ­(10−6 W) Imax (μA) Vmax (V) Pmax ­(10−6 W) FF Efficiency η (%)

Sample-2 380 0.505 191.9 315 0.32 100.8 0.525 5.28%

Sample-3 510 0.710 362.1 410 0.43 176.3 0.487 9.23%
Sample-4 480 0.610 292.8 380 0.39 148.2 0.506 7.76%
Sample-5 340 0.500 170.0 300 0.30 90.0 0.529 4.71

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Table 4  Solar cell parameters of Sensitizer ISC (μA) VOC (V)
the sample-3 with types of dye
as electrolyte MSS dye 510 0.71
RS dye 345 0.505
PB dye 300 0.41
4 Conclusions
Sol–gel simple pressing method was followed to prepare
titanium dioxide nanocrystalline paste of five different
compositions and produce light sensitize electrode on ITO
coated glass. Three types of dye were extracted to use as sen-
sitizer from Malabar spinach seeds, Red spinach leaves and
Pomegranate burgs leaves. The electrical, crystalline and
morphological properties of the electrode were improved.
From the I–V characteristics it is clearly evident that the
contact behavior is ideal. Sample-3 electrode with Malabar
spinach seeds dye gave maximum voltage and current. XRD
showed the smallest crystallite size and maximum inter pla-
nar distance for sample-3. The same results were also found
by SEM.
So it can be said that electrical property by Inductance
Analyzer, Scanning Electron Microscopy, X-ray diffraction
showed that Sample-3 electrode of T ­ iO2 with Malabar Spin-
ach Seeds dye as sensitizer is more efficient for solar energy
converter.
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