Optik - International Journal for Light and Electron Optics 179 (2019) 252–258

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Optik
journal homepage: www.elsevier.com/locate/ijleo

Improvement of efficiency of Dye Sensitized Solar Cells by

T
optimizing the combination ratio of Natural Red and Yellow dyes
⁎
F. Kabira,d, M.M.H. Bhuiyanb, , M.R. Hossaina,d, H. Bashara, M.S. Rahamanb,
M.S. Manira, S.M. Ullahc, S.S. Uddind, M.Z.I. Mollaha, R.A. Khana, S. Huqued,
M.A. Khana
a
Institute of Radiation and Polymer Technology, Atomic Energy Research Establishment, Bangladesh Atomic Energy Commission, P.O. Box 3787,
Dhaka, 1000, Bangladesh
b
Institute of Nuclear Science & Technology, Atomic Energy Research Establishment, Bangladesh Atomic Energy Commission, P.O. Box 3787, Dhaka,
1000, Bangladesh
c
Department of Electrical and Electronic Engineering, University of Dhaka, Dhaka, Bangladesh
d
Institute of Energy, University of Dhaka, Dhaka, Bangladesh

A R T IC LE I N F O ABS TRA CT

Keywords: To improve the efficiency of dye-sensitized solar cells (DSSCs),light absorption properties of
DSSC organic dye must be tuned to have a maximum response throughout visible and near infra-red
combination of dyes spectrum. This work is focused on the study of DSSC based on the combination of red (Red
natural yellow dye spinach) and yellow (Turmeric) natural dyes used as sensitizers for semiconductor TiO2 as
natural red dye
electron conductor in order to improve the efficiency.Combination of natural dye with optimized
curcumin
choice of the agents indicated improved photovoltaic impacts contrasted with single individual
betacyanin
dye sensitization and increased the absorption of solar light and allowed utilization of the photon
energy more efficiently.Power conversion efficiency (η %) of natural yellow dye extracted from
turmeric (Curcuma longa) was obtained 0.378% and for natural red dye extracted from red spi-
nach (Amaranthusdubius) was 0.134%.The maximum open circuit voltage (VOC = 499.3 mV) and
the short circuit current-density (JSC = 4.264 mA cm−2) were obtained from DSSC sensitized by
the optimum combination of 60% yellow (Turmeric) and 40% red (Red Spinach) and corre-
sponding maximum efficiency (η %) was reached 1.078%. Thus efficiency with combined dyes is
about 2.85 and 8.04 times higher than that of the efficiency of individual single yellow and red
dyes, respectively.

1. Introduction

Mankind needs sustainable sources of energy. With increasing demand for energy one of the main reasons for recent research is to
discover clean and sustainable energy. Today, the enormous amount of the energy is generated by consuming non-renewable energy
sources (coal, oil, gaseous petrol et cetera). Exhaustion of the traditional non-renewable energy resources is only a question of time.
Also, consuming non-renewable and traditional sources releases ozone depleting substances into the atmosphere, while nuclear
energy stance natural issues identified with uranium and the storage or disposal of nuclear waste. The intercession of the human race
with nature has reached a level that demands an earnest re-assessment of possible energy supply techniques with a focus on

⁎
Corresponding author.
E-mail address: mosharraf22003@yahoo.com (M.M.H. Bhuiyan).

https://doi.org/10.1016/j.ijleo.2018.10.150
Received 6 July 2018; Received in revised form 20 September 2018; Accepted 23 October 2018
0030-4026/ © 2018 Elsevier GmbH. All rights reserved.
F. Kabir et al. Optik - International Journal for Light and Electron Optics 179 (2019) 252–258

sustainability, unless undesirable changes in atmosphere and environment are accepted. Employment of solar energy, biofuels,
biomass, wind, geothermal, hydro et cetera can be viewed as the best alternative to traditional energy [1]. Rapid development of
sustainable energy and effectiveness, and technological miscellaneousness of energy sources, would bring energy security. Although
there are other inexhaustible and renewable energy resources, solar energy is the most effectively exploitable. There are many kinds
of photovoltaics system present in the market. First generation or traditional silicon solar cells, second generation or thin film solar
cell technology and finally third generation or emerging solar cell technology. Emerging photovoltaics include: organic solar cells,
copper zinc tin sulfide solar cell (CZTS), quantum dot solar cells, perovskite solar cells, dye-sensitized solar cells (DDSCs) et cetera
[2–5]. Some of them are still in the research stage.
Since their appearance in 1991 [6,7], DSSCs have drawn an extensive consideration from the scientific society because of their
low fabrication cost and easy assembling process. DSSC has the ability to absorb more sunlight per surface area than traditional
silicon-based solar cells. DSSCs can likewise work in low-light conditions, for instance, indirect sunlight and cloudy skies. They are
efficient, easy to manufacture and built from inexhaustible and stable asset materials. Most of the materials used for DSSC’s are low-
cost, just a couple of exorbitant materials are necessary, for example, Ru (Ruthenium) and Pt (Platinum).
A regular DSSC is assembled by placing a mesoporousthin layer of titanium dioxide nanoparticles [8–14], covered with organic
molecular dye, electrolyte, platinum-based catalyst and counter electrode.Natural molecular dye (chlorophyll, betacyanin, betalia-
n,anthrocyanin, xanthophyllus, beta-Carotene) has the ability to absorbs sunlight and transform solar energy into electrical energy
[15–16]. The thickness of TiO2, thin film is ordinarily around 10-15 micrometers, which plays a vital role in both the excitation of
electron from dye molecule, separation of electron and the electron exchange process from electrolyte to dye molecules in the DSSC
[17–20].
To improve the efficiency of dye-sensitized solar cells (DSSCs) the light absorption properties of organic dye must be tuned to have
a maximum response throughout visible and near infra-red spectrum.The absorption spectrum of most efficient dye sensitized solar
cell today is between 300– 800 nm, but from visible to infrared region their efficiencies are quite low. An option to obtain anextended
range of light absorption throughout the visible near infra-redspectrum is to use a combination of organic dye which have different
spectral property.
So, this study essentially indicates that combination of natural dyes with an optimized choice of the agents indicated improved
photovoltaic impacts contrasted with single individual dye sensitization and increased the absorption of solar light and allowed
utilization of the photon energy more efficiently.

2. Experimental procedure

2.1. Materials

TiO2 (Degussa P25), Triton X-100 (C8H17C6H4(OCH2CH2)), Citric acid (C6H8O7),Titanium IV Isopropoxide (Ti [OCH (CH3)2]4),
Polyethylene glycol (HO(C2H4O)n H), Iodine (I2), Potassium iodide (KI) and Fluorine doped tin oxide (FTO) glass. All chemicals and
reagents were purchased from Dyesol, Australia and Merck, Germany and used as received without any further purification.

2.2. Methods

2.2.1. TiO2 film fabrication

To prepare the slurry of Degussa P25 (1.0 g) was grind in agate mortar with 3 ml 0.1 M citric acid, 0.01 ml PEG, 0.005 ml Triton X-
100and 0.01 ml Titanium IV Isopropoxidewere mixed homogeneously. Prepared TiO2 paste was scraped on a transparent FTO glass
with resistivity of 8 Ω/sq by “Doctor Blade” coating technique. The coated film is allowed to dry in the ambient air for 10 minutes and
then annealed at 450◦C in a muffle furnace for 1 hour.The subsequent film thickness is around 10-20 μm.

2.2.2. Dye extraction

For natural yellow dye turmeric(Curcuma longa)was washed cautiously andpeel off the skins and thickly sliced. From that point
onward, it was kept in air for 12 hours without daylight for drying.Peeled turmeric was squashed utilizing mortar pestle and im-
mersed into ethanol. The proportion between turmeric to ethanol was 1g: 10 ml. After 24 h, the extract was filtered and used as
sensitizer supply for DSSC.
For natural red dye,at first red spinach (Amaranthusdubius) was washed and cut carefully. Then red spinach was heated at 60°C for
one hour. The ratio between red spinach to distill water was 1g: 10 ml. After that, the liquid solution was taken into another beaker
and was cooled down. Then with the help of separatory funnel and chloroform, betacyanin pigment (the pigment that was responsible
for red color) was collected other pigments were separated.

2.2.3. Preparation of electrolyte

The electrolyte used in the DSSCs consists of iodine (I-) and triiodide (I3-) as a redox couple. For the preparation of Iodide
electrolyte solution, 0.064 g (0.05 M) Iodine was dissolved in 10 mL of ethylene glycol followed by 0.83 g (0.5M) Potassium Iodide.
The solution was then stirred and stored in a dark container away from light.

2.2.4. Cell preparation

The FTO substrate coated with TiO2 thin film (about 10 cm2) was immersed in the natural dye solution for 1 hour to fabricate

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Fig. 1. Chemical structure of (a) curcumin [21] and (b) betacyanin [22].

working anode. At this point color particles were adsorbed by TiO2 film then the anode was rinsed in deionized water for a few
seconds to wash out unbound dyes. After that dye absorbed TiO2 film was dried in an oven at 30°C for 20 minutes. For counter
electrode or cathode another FTO glass was coated with carbon of candle nip technique. The working electrode (anode) then bonded
together to a counter electrode (cathode) by paper binder clips and redox electrolyte solution was injected into the cell (Fig. 1).

2.2.5. Measurement of the photoelectric parameters of DSSC

A UV–vis spectrophotometer (Jasco, V650) was employed to assess the absorption spectra of natural yellow dye (curcumin),
natural red dye (betacyanin) and combination of natural yellow and red dye. In addition, current–voltage (I–V) curve was observed
under the simulated white light source (100 mW/cm2 and AM 1.5),the energy conversion efficiency can be defined as follows:
Isc × Voc × FF
η=
Pin (1)
Vmax × Imax
Where, Fill factor FF = ,Vmax=Maximum output value of voltage, Imax= Maximum output value of current, Voc =Open-
Voc × Isc
circuit voltage, Isc =Short-circuit current and Pin = Energy of the incident photon.
Energy gap of dye can be determined by using the formula of equation 2 [16]. Here, E is the photon energy or optical energy gap.

hc
E = hv =
λ (2)
−34 8
Where, h = Planck’s constant (6.63 × 10 Js), v =Frequency, λ =Wavelengthand c = Speed of light (3.0 × 10 m/s)
The absorption coefficient characterizes how far into a material, the light of a particular wavelength can penetrate before it is
absorbed [16]. The absorption coefficient is obtained by using equation 3

4πk
Absorption coefficient =
λ (3)
−5
Where, K = Boltzmann constant K (8.316 × 10 eV)

3. Results and discussion

3.1. FT-IR characterization

Fig. 2 shows the IR spectra of the spectral range within the wave band of 4000∼450 cm−1. For yellow dye 684.90 cm−1 were
attributed to Ti-O-Ti bridging stretch modes [23]. C = C stretching appeared at 878.57 cm−1 for apatitic structure [24]. CO-O-CO
stretching appeared at 1044.30 cm-1 for anhydride [24–25]. C- O stretching appeared at 1044.36 cm−1 [23,25] and C-N stretching
appeared at 1352 cm−1 forporphyrins [26]. Titanium carboxylate stretching appeared at 1650.66 cm−1[27]. 2829.59 cm−1 and
2976.34 cm−1 C-H stretching for Alkane [28] and 3341.14 cm−1 for vibration of phenol (Ar-OH) and alcohol (R-OH) of free hydroxyl
group [24,31].
For red spinach CO-O-CO stretching appeared at 1060 cm-1 for anhydride [24–25]. C- O stretching appeared at 1320.69 cm−1and
1342.77 cm−1 [23,25]. C- N stretching appeared at 1382.38 cm−1 for aromatic amine [26,29]. Titanium carboxylate stretching
appeared at 1642.22 cm−1[27]. 3271.31 cm−1 for vibration of phenol (Ar-OH) and alcohol (R-OH) of free hydroxyl group [24,31].
For combination of 60% turmeric and 40% red spinach 635.07 cm−1 were attributed to Ti-O-Ti bridging stretch modes [23].
Stretching of C- O appeared at 1104.10 cm−1 [23,25] and stretching of C-N appeared at 1352 cm − 1 for porphyrins [26]. Stretching
of C- N appeared at 1514.18 cm−1 for aromatic amine [30]. Titanium carboxylate stretchingappeared at 1627.23 cm-1 [27].
3283.00 cm−1 for vibration of phenol (Ar-OH) and alcohol (R-OH) of free hydroxyl group [24,31].
As we can see from the FTIR spectra of the combination of natural yellow and red dyes that no new bond is formed. We can
assume that in case of the combination of these two natural pigments they don’t react with each other but, they simply coexist side by
side without any reaction.

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Fig. 2. FTIR spectra of (I) Red dye adsorbed by TiO2 (II) Yellow dye adsorbed by TiO2, (III) 60% Yellow and 40% Red dye combination adsorbed by
TiO2.

3.2. UV–vis spectroscopy

3.2.1. Absorption spectra

Fig. 3 shows the UV-Vis absorption spectra of natural red dye extracted from red spinach, natural yellow dye extracted from
turmeric and the combination of 40% red dye and 60% yellow dye in the visible light spectrum (350 nm −800 nm) respectively.
From Fig. 3, the absorption peak of natural red dye can be seen at 514 nm, and for turmeric absorption peak located at 421 nm.
Combination of 40% red spinach and 60% turmeric the absorption peak can be seen at 420 nm [16].
The absorption peak for natural red dye (extracted from red spinach) and yellow dye (extracted from turmeric) attributed to the
existing of betacyanin and curcumin pigment respectively. Though red spinach is identified to be rich in betacyanin but there are also
some chlorophyll present because all plants contained chlorophyll even if theamount is little. Like chlorophyll, both betacyanin and
curcumin are capable in photosynthesis under the presence of visible light [16,30].
For natural red dye with an absorption range of 400-600 nm and peak absorbance at 514 nm as shown in Fig. 3. For natural yellow
dye with an absorption range of 350-600 nm and peak absorbance at 421 nm as shown in Fig. 3. Band gap and absorbing wavelength
of the dyes are inversely proportional, energy band gap decreases with increasing absorption wavelength [16,32–34].

3.2.2. Band gap estimation and absorption coefficient of the dyes

Energy band gap is the difference between conduction band and valence band. This optical energy band gap is used for analyzing
what portion of solar spectrum as absorbed by the DSSC. Table 1 demonstrates the energy band gap of DI water as an extract solvent
for red spinach to extract the betacyanin pigment for natural red dye, ethanol extract solvent for turmeric to extract the curcumin
pigment for natural yellow dye and the bandgap of 60% yellow and 40% red dye combination. Natural red dye has the lowest band
gap 2.42 eV compared to yellow dye’s band gap 2.95 eV. Similarly, natural red dye has the lowest absorption coefficient 2.11 Km-
1
compared to yellow dye’s absorption coefficient 2.58 Km-1.
Table 1: Photon energy and absorption coefficient (α) of the dyes

Fig. 3. UV–vis absorption spectra of natural red, yellow and combination of dye.

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Table 1
Photon energy and absorption coefficient (α) of the dyes.
Dye Peak Absorption Range Energy Band Gap Absorption
Absorbance (nm) (eV) coefficient(α)
(nm) Km-1

100% Yellow Dye 421 350-600 2.95 2.58

60% Yellow + 40% Red 430 350-600 2.88 2.52
100% Red Dye 514 400-600 2.42 2.11

3.3. Photoelectrical properties of DSSCs sensitized with curcumin and betacyanin pigment

Current-voltage (I-V) performance of DSSCs sensitized by red dye (betacyanin), yellow dye (curcumin) and combinations of
natural yellow and red dyes was performed under AM 1.5 simulated sunlightsource (100 mW/cm2). The performance of DSSC is
assess by the open circuit voltage (Voc), short circuit current (Isc) and fill factor (FF). As shown in Table 2, the highest fill factor was
the combination of 60% yellow and 40% red dye was 50.7% which is higher compared to red spinach’s 48.1% and turmeric’s 44.9%.
Fig. 4 represents the current vs different dye composition. As we can see from the Fig. 4, the combination of both natural red and
yellow dye gives higher current compared to single individual dye sensitized DSSC.
Fig. 5 represents how the different combinations of dye improved photovoltaic impacts contrasted with single individual dye
sensitization, and increased the absorption of solar light, and allowed utilization of the photon energy more efficiently.
100% red dye’s efficiency is the lowest 0.134% compared to other dye’s efficiency. As we combined yellow dye with red dye, the
efficiency increased significantly. As the percentage of yellow dye increase in the combination, DSSC’s efficiency increase gradually.
Every combination of yellow and red dye has higher efficiency than 100% red dye. For 60% yellow and 40% red dye combination has
the maximum efficiency 1.079%.
On the other hand, 100% yellow dye’s efficiency is 0.378%. As we added red dye with yellow dye, the combination’s efficiency
also increased.The efficiency (1.079%.) of DSSC with combined dye (60% yellow and 40% red) is about 2.85 and 8 times higher than
that of the efficiency of individual single yellow (100%) and red dyes (100%), respectively.
In summary, all the combination of dye has higher efficiency than individual dye. So the combination of dyes has a positive
impact to increase the efficiency of DSSC.

4. Conclusions

In this study, curcumin and betacyanin pigments was used as dye sensitizer. Both of these pigments have the ability to absorb
sunlight and convert solar energy into electrochemical energy. According to this study, it is clear that the combination of curcumin
and betacyanin has a positive impact on the efficiency. In this study 5 different combinations with ratios (20% to 80 %) red (Red
Spinach) and yellow (Turmeric) natural dyes were used as sensitizers for semiconductor TiO2 as electron conductor. From the UV-vis
study, the combination of dyes obtained a wide range of absorption spectra and absorbance of light than the both individual dyes. As
a result, combination of natural dye shows better cell performance than the single individual dyes. From the FTIR spectra, for the
combination of natural yellow and red dyes, that no new bond is formed. We can assume that in case of the combination of these two
natural pigments they don’t react with each other, rather they simply coexist side by side without any reaction. The power conversion
efficiency (η) of natural yellow dye (100%) was 0.378% and for natural red dye(100%) was 0.134%. But the optimum combination of
60% yellow (Turmeric) and 40% red (Red Spinach), the maximum efficiency was reached to 1.079%. So, the optimum combination
of dyes is an effective method to improve the efficiency of DSSCs.

Acknowledgement

This research work is financed by the Ministry of Science & Technology, Government of the Peoples Republic of Bangladesh under
special Allocation Research project for Science & Technology (Ref. No. : 39.009.006.01.00.057.2015-2016/PHY’S-370/1299 Date:
08/12/2015).

Table 2
IV performance of DSSCs measured under AM 1.5 sunlight illuminations (100 mWcm−2).
Combination of Dye Voc(mV) Isc(mA) FF η%

100% Yellow 499.5 1.575 0.481 0.378

80% Yellow + 20% Red 479.3 2.258 0.457 0.495
60% Yellow + 40% Red 499.3 4.264 0.507 1.079
50% Yellow + 50% Red 458.5 3.728 0.465 0.795
40% Yellow + 60% Red 389.6 2.594 0.431 0.436
20% Yellow + 80% Red 366.1 1.409 0.404 0.208
100% Red 338.4 0.882 0.449 0.134

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Fig. 4. Current vs. Different Dye Composition.

Fig. 5. Efficiency vs. Different Dye Composition.

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