Effect of organic dye variation from teak leaves (Tectona grandis),

tamarind leaves (Tamarindus indica) and daun ungu leaves

(Graphtophyllum pictum) on dye-sensitized solar cell (DSSC)
performance
Satria Arief WBa , Nadila Yasuria, Setia Budi Sasongkoa
Hendri Widiyandarib*,
a

Department of Chemical Engineering Faculty of Engineering, Diponegoro University, Semarang Indonesia

E-mail: satriaawb@yahoo.co.id

b*)

Department of Physics Faculty of Science and Mathematics, Diponegoro University, Semarang Indonesia
E-mail:h.widiyandari@undip.ac.id

ABSTRACT
We have succesful to produce the natural dyes that extracted from teak leaves (Tectonia grandis), tamarind leaves
(Tamarindus indica) and daun ungu leaves (Graphtophyllum pictum) using simple extraction technique.The dyes
have shown absorption in broad range of the visible region (400-700 nm) and appreciable adsorption onto the
semiconductor (TiO2) surface. The produced natural dyes were then used as sensitizers in dye-sensitized solar
cells (DSSCs) and their characteristics were studied. The range of FF (Fill Factor) value from 0,28 to 0,479 and
0,001% to 0,05% efficiency. Among the three dyes studied, the extract of tamarind leaves has shown the best
photosensitization effects in term of the cell output.

1. INTRODUCTION
One of the humans biggest challenges is to replace fossil-based fuel with renewable energy while keeping its
availability in the center energy thirst booming, caused by exponential growth of humans population. In Indonesia,
total energy consumption reaches 300,417 GWh in 1980, and then it grows to 625,500 GWh in 1990. In the middle
[1]
of 2009 it reaches 1,490,892 GWh . This is quite daunting because the fossil-based fuel predicted to be depleted
in 12 years.
This challenge has been answered with some low-cost solutions with variety of raw materials. Sun light is a cheap
and clean source of energy, and has been used by the nature to maintain many kind of life in the earth. This
reliable source of energy could be one of the best solutions towards this energy challenge, in a more mass-scale
solution. One of the technologies to utilize sun light energy is photovoltaic.
Up until now, most of commercially used photovoltaic technologies are based on inorganic materials, and of course,
a high cost and high energy production is needed. Moreover, some of the materials, like CdTe, are a toxic and not
quite abundant in the nature. Organic-based photovoltaic could solve the problem, but the efficiency of organicbased photovoltaic is far from inorganic ones.
Organic-based photovoltaic uses donor-acceptor type organic materials, forming hetero-junction that leads to
exciton separation to be two carriers. Both carriers transported to the electrode, including the organic material,
which is used to form prior excitons. A good photovoltaic material is the material that could collect light and
transport carrier seamlessly. Dye-sensitized solar cell (DSSC) divides those characteristics by forming interface
between semiconductor and dye to generate exciton and using electrolyte-semiconductor to transport carrier.
Generally, DSSC used ruthenium-complex as dye to absorb sun light. Ruthenium-complex have some molecul
[2]
structures, such as CYC-B3, CVC-B1 and SJW-E1. The efficiency of the cell ranged from 7-12% . This ruthenium
based DSSC is too expensive to be commercially produced. Beside of that, ruthenium-complex is one of
[3] [4]
frontrunner in cancer-cure molecule research, as it could induce apoptosis on cancer cells
.
To solve the problem, some alternatives to replace ruthenium-complex is by using organic dye that are extracted
from variety of plants. Chang & Lo studies the use of mulberry and pomegranate mixture as dye in DSSC. The
[5]
study reveals that the efficiency of DSSC is 0.722% . Calogero & Di Marco studies the mixture of red Sicilian
[6]
orange (Citrus sinensis) and purple eggplant (Solanum melongena, L.) and it reveals 0.66% efficiency .

The uses of those plants are fine and the efficiency shows that they have potential to be the material to
manufacture dye. But the use of food source as the energy source could lead to new problem as it could disturb the
stability and diversity of food source. More than that, most of the plant based materials are not available in
Indonesia, and it will be another problem that arises.
This research will study the possibility of using teak leaves (Tectonia grandis), tamarind leaves (Tamarindus indica)
and daun ungu leaves (Graphtophyllum pictum), as the material of dye. The three leaves of these plants are not
used as food sources, in fact, the leaves of these plants havent been used widely while they are abundant in
Indonesia. The dye extracted from these leaves are characterized using UV-Vis Spectrophotometer to understand
their light absorbance and the DSSC prototypes using this three kind of dyes are characterized using Solar
Simulator to understand their photoelectric performances.

2. EXPERIMENTAL METHOD
2.1 Materials
Ethanol (A.R. grade, 99,98%, Merck, Canada) was used for extracting natural dyes from leaves of plants. Fresh
leaves of teak (Tectona grandis), tamarind (Tamarindus indica) and daun ungu (Graphtophyllum pictum). Titanium
paste (20 nm) as a semiconductor agent, H2PtCl6 as a counter electrode and Tri-Iodide EL-HPE as a elecrolyte
were obtained from Dyesol, Australia. And also FTO-coated (Flourine-doped Tin Oxide) was used as substrates for
preparing TiO2 thin film electrode and Platinum counter electrode was obtained from Dyesol, Australia. And ethanol
(70%, Merck, Canada) used to clean the FTO-coated from impurities before sintering. Thermoplastic as spacer
used to close outside of active area to prevent leak of electrolyte was injection in this side.
2.2 Preparation of Natural Dye Solutions (Extracts)
The natural dyes were extracted with ethanol employing the following procedure : Each of fresh leaves were
washed with water and dried. Fresh leaves of tamarind (Tamarindus indica), teak (Tectona grandis) and daun ungu
(Graphtophyllum pictum), respectively, were crushed using mortar, these were kept in glass bottles and filled with
ethanol (A.R. grade, 99,98%, Merck, Canada), ratio wight ethanol and leave is 1 : 3. These solutions were kept for
one day in the dark at room temperature. The solid residues were filtrated out and the resulting filtrates were used
as dye solutions.
2.3 Preparations of Photo Anode and Counter Electrode
FTO was bitbraced as open side to injection the electrolyte, and then washed in Utrasonic Bath with ethanol (70%,
o
Merck, Canada) during 5 minutes at 15 C. TiO2 thin film electrodes (photoanodes) were prepared by spreading
highly transparent paste of TiO2 (20 nm, Dyesol, Australia) with doctor blade methode on active side FTO-coated
conductive glass 1 x 1 cm, with once spread. After spreading paste, the adhesive tapes were removed and films
o
o
o
were annealed in tubular furnace (Branstead Thermolyne) at 325 C, 375 C, 450 C during 5 minutes, 5 minutes and
o
15 minutes respectively, and was cooled until 30 C. The dyes were anchored onto the surface of TiO thin film
electrode by immersing it for overnight. The dye-coated films were air dried and used as photoelectrode inthe cell.
The platinum counter electrode was prepared on another FTO-coated glass, FTO was washed in Ultrasonic Bath
o
with ethanol (70%, Merck, Canada) during 5 minutes at 15 C. Spread H2PtCl6 (Dyesol, Australia) by using doctor
o
o
blade method on FTO and anneling in turbular furnace at 400 C during 15 minutes, and was cooled until 30 C.
2.4 Assembly of Sandwich Type DSSC
Thermoplastic as a spacer was put on the outside of active area of photoelectrode. The photoelectrode was put
over platinum counter electode in such a way that the conductive side of both the electrodes faced each other and
clip it. And the electrolyte was injected through open side. This assembly DSSC can be characterized by Solar
Simulator A.M (1,5 G) to get characteristics of current and voltage.

3. RESULT AND DISCUSSION

3.1 Dye Absorbtion Characteristics
Extracted solutions that gathered from teak leaves, tamarind elaves and daun ungu leaves is used as sensitizer on
DSSC need to be characterized to understand their absorption spectra. The charaterization of dye is done by using
UV-Vis Spectrophotometre

(a)

(b)

(c)

Figure 1. Extract from tamarind leaves (a), teak leaves (b) and daun ungu leaves (c)
Figure 2 shows that three dyes have visible light (400-700 nm) absorption. Tamarind leaves extract and teak
leaves extract on 666 nm and daun ungu extract on 655 nm. These profiles of absorption shows that three of the
dye can be used as the sensitizer on DSSC. This phenomenon happens due to the use of semiconductor. On this
experiment we used VLA (Visible Light Activated) nanoparticle semiconductor, TiO2. The spectrum of VLA TiO2 is
[7]
shown on Figure 3.

(b)

(a)

666

666

(c)

655

Figure 2. Absorption Spectra of tamarind leaves extract (a), teak leaves extract (b) and daun ungu extract (c)

Figure 3. TiO2 Absorption Spectrum

[7]

3.2 Electric Current and Voltage Characteristics

Photovoltaic performance can be represented into FF (Fill Factor) and (efficiency). Those values can be obtained
by knowing the characteristics of its electrical current and voltage. Working electrode layered by 20 nm TiO 2. The
working electrodes then dipped in dye sensitizers from tamarind leaves extract, teak leaves extract and daun ungu
extract for 24 hours and then assembled to be DSSC prototypes, shown in Figure 4.

Figure 4. DSSC Prototypes using extraxct of tamarind leaves (a), teak leaves (b) and daun ungu leaves (c)
These DSSC prototypes then charaterized by using Solar Simulator AM (Air Mass) and Source Meter Ketiley 2400.
By doing this charaterization we get to know the electric current (I) and voltage (V). The Solar Simulator AM 1,5 G
and Source Meter Ketiley 2004 is shown on Figure 5.

Figure 5. Solar Simultaror AM (Air Mass) and Source Meter Ketiley 2004

Figure 6. I-V Graphics of DSSC Prototype from tamarind leaves (a), teak leaves (b) and daun ungu leaves (c)
The data gained from the instrument is shown in Figure 6. These data is shown in I-V graphics. These data can be
used to understand its IsC (Short Circuit Current), JSC (Short Circuit Current Density), VOC (Open Circuit Voltage),
Imax (Maximum Current), Vmax (Maximum Voltage), PMax (Maximum Power), FF (Fill Factor) and (Efficiency). FF
[8]
and efficiency can be obtained by using these formulas:

By some mathematical calculation, it is obtained:

Table 1. Photovoltaic parameters of three DSSC prototypes

Dye

ISC
(mA)

JSC
2

(mA/cm )

VOC

Imax

Vmax

Pmax

(V)

(mA)

(V)

(mW)

FF

Efisiensi
(%)

Teak

0.022

0.022

0.29

0.01

0.18

0.0018

0.28

0.0018

Tamarind

0.185

0.185

0.557

0.13

0.38

0.05

0.479

0.05

Daun Ungu

0.011

0.011

0.23

0.007

0.15

0.001

0.415

0.001

Table 1 show that DSSC that use tamarind leaves extract shows the best photovoltaic performance above all. The
tamarind leaves based prototype have FF values at 0.479 and 0.05 % efficiency, the teak leaves based prototype
have FF values 0,28 and 0,0018% efficiency, and prototype with daun ungu extract have 0.415 FF value and
[9]
0,001% efficiency. A typical grade B solar cell has FF ranged from 0,4 to 0,7 .
Tamarind leaves extract and teak leaves extract has same group pigment, that is flavonoid, but it shows different
DSSC photovoltaic performance. This phenomenon is happened because the difference in sensitization action
dyes that differs in semiconductors surface adsorption. This is due to difference of electron transfer from dye
[8]
molecules to conduction band of semiconductors . Impure dye causing dye aggregation in semiconductor film
[6]
that disturbs light absorption

4. CONCLUSIONS
Three natural dyes extracted from the leaves of teak (Tectona grandis), tamarind (Tamarindus indica) and
daun ungu (Graphtophyllum pictum) were used as sensitizer and their photovoltaic characteristics were studied.
Three of dyes have visible light (400-700 nm) absorption, leaves of teak and tamarind on 666 nm and daun ungu
on 655 nm. The DSSCs made using the extracted leaves of tamarind dyes shows the FF (Fill Factor) value is
0,479 and 0,05% efficiency is the best photovoltaic performance. Tamarind leaves extract and teak leaves extract
has same group pigment, that is flavonoid, but it shows different DSSC photovoltaic performance. This
phenomenon is happened because the difference in sensitization action dyes that differs in semiconductors surface
adsorption. This is due to difference of electron transfer from dye molecules to conduction band of semiconductors.

REFERENCES
[1] Silitonga AS. A review on prospect of Jatropha curcas for biodiesel in Indonesia. Journal of Renewable
and Sustainable Energy Reviews, vol. 15, pp.3733-3756. 2010
[2] Vougioukalakis, GC. Contributions to the development of ruthenium-based sensitizers for dye-sensitized
solar cells. Coordination Chemistry Reciews vol.255 pp.2602-2621. 2011
[3] Hufziger, KT. Ruthenium dihydroxybipyridine complexes are tumor activated prodrugs due to low pH and
blue light induced ligand release. Journal of Inorganic Biochemistry, vol 130, pp.10311. 2013
[4] Yang, Ki Liu. Photovoltaic properties of dye-sensitized solar cells associated with amphipilic structure of
ruthenium conplex dyes. Journal of colloid and interface science, vol 372, pp.73-79. 2013
[5] Chang, H and Lo, YJ. Pomegranate leves and mulberry fruits as natural sensitizers for dye-sensitizers
solar cells. Solar Energy, vol 84, pp.1833-1837. 2010
[6] Calogero, G. and Di Marco, G. Red Sicilian Orange and purple eggplants fruits as natural sensitizers for
dye-sensitized solar cells Solar Energy Materials and Solar Cells ,v ol.92, pp.1341-1346. 2008

[7] Simya, OK., Selvam M., Karthik A., and Rajendran V., Dye-sensitized solar cell based on visible light
active TiO2 heterojunction nanoparticles. Journal of Synthetic Materials, vol 188, pp.124-129. 2013
[8] Kushwaha, R., Srivastava P., and Bahadur L., Natural Pigments from Plants Used as Sensitizersfor TiO 2
Based Dye-Sensintized Solar Cells. 2013
[9] Vos, AD. Detailed balance limit of the efficiency of tandem solarcell. Journal of Physics: Applied Physics,
vol 14, pp. 839. 2009