Journal of Materials Engineering and Performance

Performance of Dye-Sensitized Solar Cells (DSSCs) with

Zinc Oxide (ZnO) Nanpowders and Nanorods

Journal: Journal of Materials Engineering and Performance

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Manuscript ID JMEP-17-04-12915.R1

Manuscript Type: Technical Paper

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Date Submitted by the Author: 03-Nov-2017

Complete List of Authors: Chatterjee, Suman ; University of North Bengal, Department of Physics
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Dye-sensitized solar cells, Photovoltaic properties, Zinc Oxide Nanolayer,

Keywords:
Band Structure, Density of States
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Page 1 of 14 Journal of Materials Engineering and Performance

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4 PERFORMANCE OF DYE-SENSITIZED SOLAR CELLS (DSSCs) FABRICATED WITH ZINC
5 OXIDE (ZnO) NANPOWDERS AND NANORODS
6 Suman Chatterjee
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8 Department of Physics, University of North Bengal, Siliguri-734013, India
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11 ABSTRACT
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13 Due to their higher efficiency, along with lower cost of production, many researchers are working on Dye-
14 sensitized solar cells (DSSCs) over last few decades as a substitute technology for nonconventional energy.
15 Nanostructured ZnO has got many interesting useful properties for application as electrode in DSSC. Some
16 of them are wide band gap, large exciton binding energy, good exciton stability and very high breakdown
17 strength. In this work, the device properties of DSSC fabricated is compared through different techniques,
18 ZnO nanorods on a ZnO film and ZnO nano-powders. We used Nanostructured ZnO as photoanode and
Rose Bengal as the Dye to fabricated DSSC cells. Different types of ZnO photoanode and Dye
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20 combinations are subsequently used to study the suitability to fabricate the DSSC cell and investigation are
21 carried out on the photovoltaic properties of the ZnO based DSSC samples. The photovoltaic properties of
22 fabricated cells obtained are discussed in the light of band structure and density of states of different types
of the ZnO nanolayers. The ZnO nanorods fabricated through the sol-gel route have more uniform
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thickness resulting in enhanced photovoltaic properties of the fabricated device.
24
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25 Keywords: Dye-sensitized solar cells, Zinc Oxide nanolayer, Photovoltaic properties, Band Structure,
26 Density of States.
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28 1. Introduction
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The ever-increasing Industrialization and Urbanization has led to the exhaustion of the available fossil
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fuels. This situation has led to find alternative resources of energy in order to meet the energy demands of
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the growing population. In recent years, due to their low fabrication cost and higher efficiency, Dye-
32 sensitized solar cells (DSSCs) have attracted a lot of attention by various researchers [1].
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34 Also, due to some of its fascinating properties ZnO has shown a great deal of research interest for
35 application in DSSCs. ZnO has got many attractive properties such as wide direct band gap (3.27 eV) and
36 large exciton binding energy, which is very useful for obtaining good output characteristics of organic solar
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37 cells [1,2] and so is often utilized as a photoanode material in DSSCs. As an added advantage, greater light
38 penetration is possible, as it is highly transparent. Finally, higher surface-to-volume ratio for greater dye
39 loading is possible with ZnO due to its 1-D single crystal structure formation.
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40 DSSCs are a promising green energy source, [3,4] which can be fabricated at a very low cost. The
41 challenge is to increase its efficiency with low cost components [5]. The dye is one of the most important
42 parameter identified in DSSC research for improvement of efficiency. The absorption spectrum of the dye
43 is important parameters determining the efficiency of the fabricated DSSC [6]. Another important factor for
44 the dye is its anchorage to the surface of ZnO [7]. Generally, due to highly efficient metal-to ligand charge
45 transfer and high charge-transfer absorption in whole visible range, transition metal coordination
46 compounds like ruthenium polypyridyl complexes, are effectively used as sensitizers. However, these
47 complexes contain a heavy metal, ruthenium, which increases the cost of production and undesirable as
48 they are not environment friendly. Also, synthesis of these complexes requires complicated costly process.
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50 Alternatively, natural dyes may be used to fabricate the DSSC’s, which yields much lower but acceptable
51 efficiency of the fabricated cell. However, the natural dyes have some added advantages like easy
52 availability and low cost [8,9]. Way back in 2006, a power conversion efficiency of 11.18% has been
53 achieved [5] with comparatively low cost natural dyes. A class of dye called Anthocyanins can easily
54 transfer electron to the conduction band of ZnO [8]. While extracted from various plants, Anthocyanins
55 gives different sensitizing performances [9]. However, no acceptable explanation behind these results was
56 reported.
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 Journal of Materials Engineering and Performance Page 2 of 14

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3 Based on our previous investigations [10], Rose Bengal dye was identified for further studies in this work.
4 Rose Bengal dye is abundant in tropical countriesError! Bookmark not defined. and widely used as photo
5 sensitizers for preparation of DSSCs [8]. This is one of the best photo sensitizer for ZnO photoanode and is
6 much cheaper than Ru-complex dyes [6]. Rose Bengal belongs to the Xanthene class and also absorbs wide
7 spectrum of solar energy like Anthocyanin. Moreover, for DSSC applications, it matches energetically
8 more with ZnO and usual KI-I2 redox couple. Our hypothesis for selection of dye was also due to the fact
9 that ZnO nanorods have different absorption characteristics with Xanthene, which matches more with ZnO
10 naonrods and produce a greater effect, compared to the ZnO nanopowders reported [11].
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12 Due to some of its fascinating properties, ZnO has shown a substantial interest in DSSC research.
13 Elimination the interface between ITO and the ZnO nanorods is expected to help increase its conversion
14 efficiency. This heterogeneous interface may be eliminated by replacing the ITO layer with a ZnO film. In
15 addition, ZnO functions as a good TCO material, being transparent throughout the whole visible spectrum.
16 This concept of depositing a ZnO film first and subsequently growing ZnO nanorods in the second step,
17 was reported in earlier literature [8]. In this work, we used sol-get technique [8] to grow ZnO nanorods on a
18 ZnO film and compared its photoelectric properties with the DSSC device prepared with ZnO
nanopowders.
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20 Reports of first-principles calculations on pure ZnO and dopants can be found in the literature [12,13].
21 However, very little effort has been made to correlate the experimental data of DSSC with ZnO and band
22 structure of the ZnO nano-layer produced by first principle calculations. The inputs from XRD can be used
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23 to predict material properties by first-principles calculations. XRD data of the crystal structure, such as its
24 lattice parameters, volume and atomic positions, are the main inputs for simulation. Some results of
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25 simulations done by earlier investigations are referred in Figure 1. The simulation results were carried out
26 assuming ZnO Wurtzite cell structure of the ZnO layer [12] and hexagonal crystal structure for nanorods
27 [13]. These simulated results are correct if the values of the crystal structure found out in our samples are
28 same with that assumed in these references. The crystal structure in our samples was confirmed from X-
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29 Ray diffraction analysis.

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31 3. Experimental Details
32 2.1. Fabrication of Electrodes
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34 For preparing ZnO nanoseed from Zinc acetate solution, sol-gel spin-coating technique is followed in our
35 investigation. One side of glass substrates is coated by this method. Zinc acetate dehydrate,
36 (CH3COO)2Zn,2H2O, (98% Merck) (5 mM solution with distilled methanol) was prepared and spin coated
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37 at 1000 rpm for 60s, on ITO-coated glass substrates. Subsequently, the Zinc acetate solution is put through
38 a dropper on a rotating substrate [8,9], for fabricating film of Zinc oxide nano tubes. Layers of ZnO islands
39 were formed with (100) plane of ZnO being parallel to the substrate surface. Subsequently, the substrates
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40 were heated to 3500C for 30 min in an air oven. After evaporation of the solvent, a thin ZnO film was
41 formed. The thickness of the film is controlled by repeating above process for several times. Concentration
42 of the solution and RPM of the substrate, are monitored carefully as they play important roles in adjusting
43 the thickness of the film thus formed. An ITO coated glass is used to form the counter electrode (cathode).
44 For Zinc oxide nanopowders (Zinc oxide nanopowders, <100 nm particle size, 544906 Sigma Aldrich) was
45 mixed with solvent of Toluene methanol azeotropic mixture and screen printed over ITO substrate.
46 2.2. Characterization of ZnO Nanolayer
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48 A Field emission scanning electron microscope (FESEM) with a field emission gun operating at 200 kV
49 was used to study the morphology of the samples. Two representative SEM images of ZnO nano-powders
50 and ZnO nanorods are presented in Figure 2(a) and 2(b) respectively. Upon observation of different images,
51 it was observed that the nanorods are mostly vertically aligned with the substrate. The film of thickness of
52 the ZnO layer is approximately ~2 µm and the nanorods have diameter ranging from 100 to 200nm and an
53 average length of 500 nm. Whereas the nano-powder grains are more or less spherical with an average
54 particle size slightly larger than the nanorods of around 200 nm.
55 2.3. Characterization of Dyes
56 Rose Bengal is one of the commonly used organic dye, used to sensitize the semiconductor layer in DSSC.
57 Rose Bengal having absorption peak at 555 nm, and so individually they absorb a very small portion of the
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Page 3 of 14 Journal of Materials Engineering and Performance

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3 visible spectrum of solar radiations. This gives rise to a low efficiency of DSSCs. The UV–VIZ
4 spectrophotometer (Perkin Elmer model Lamda-35) was used to record the absorption spectra of dyes. For
5 this purpose, both the devices fabricated with ZnO nanorods and ZnO nanopowders, was immersed in a
6 solution of sensitized dye Rose Bengal for 12 hours. Excess dye on the surface is removed by rinsing with
7 ethanol and air-dried at room temperature.
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9 2.4. Fabrication of DSSC Cell
10 Earlier literature [12] describes the fabrication of DSSC cells. Our cells were assembled conventionally
11 following this procedure. The counter electrode was placed on the top of ZnO coated electrode such that its
12 conductive side faces the ZnO film. For preparation of the electrolyte, we used 0.5M potassium iodide
13 mixed with 0.05M iodine in water-free ethylene glycol. Space between the electrodes is filled with the
14 electrolyte while it is drawn by capillary action, when the iodide based liquid electrolyte was touched at the
15 edges of the plates. To hold the electrodes together, we used two binder clips. DSSC fabricated with ZnO
16 nanopowders shows higher current and hence higher power achieved whereas those with ZnO nanorods
17 shows lower current values.
18 2.5. Measurement and Analysis
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20 Keithley model 2400 digital source pico-ammeter was used to measure the Current Voltage characteristics
21 of DSSC in dark and illuminated condition, while an Oriel Xenon-lamp (450 Watt) was used as the light
22 source for the efficiency measurements. By adjusting the distance of the light source from the sample, the
light intensity of 100 mW/cm2 (the equivalent of one sun) was delivered to the surface of the measured
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DSSC solar cell. The value of incident intensity was checked using a Digital Lux Meter Lutron LX-101AS.
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The experiment was carried out at otherwise dark room environment and temperature was checked to be
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around 27°C throughout the experiment to minimize the surrounding effect.
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27 The current-voltage characteristics of DSSCs were obtained under various light intensities.
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The formula used for finding the solar conversion efficiency (η) of a DSSC was
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30 η = Pmax /Pin, (1)
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where Pmax is the maximum output power and Pin denote and the input power. A DSSC usually contains a
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series resistance, Rs and a shunt resistance, Rsh and so the parameter, fill factor (FF) is introduced to
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incorporate their effects
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35 FF = (Imax×Vmax)/(Isc×Voc) (2)
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where the open-circuit voltage is Voc and the short-circuit current is Isc. And for the maximum power
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output, Pmax, Imax is the photocurrent and Vmax, the photo voltage. The solar conversion efficiency of a DSSC
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was calculated by the formula
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40 η = Isc × Voc × FF/Pin (3)

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2.6. The Equivalent Circuit Model of DSSC:
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As shown in Figure 3(a), the equivalent circuit of the single diode model is used to characterize a solar cell.
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The relation between the current I and the voltage V, using this circuit model [14], is given by
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45 ௤ሺ௏ାோೞ ூሻ ௏ାோೞ ூ
46 ‫ܫ = ܫ‬௣௛ − ‫ܫ‬௦ ቂ݁‫ ݌ݔ‬ቄ ቅ − 1ቃ − (4)
஺௞ಳ ் ோೞ೓
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48 where Iph, is the photocurrent, Is, the saturation current of the diode, Rs is the series resistance, Rsh is the
49 shunt resistance. q being the electron charge and A, the ideality factor. Also, kB, and T have the usual
50 meaning, the Boltzmann constant, and absolute temperature respectively.
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52 3. Results and Discussion
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The sensitizing dye must have the following properties in order to achieve high conversion efficiency. The
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dye should be able to absorb light up to the largest wavelength in the sun light spectrum. To present an
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energetic driving force for the electron injection process, the exited state of the adsorbed dye molecule
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should be higher than the conduction band edge of the ZnO. To sustain long time of operation at exposure
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to natural daylight, the adsorbed dye molecule should be stable at the semiconductor-electrolyte interface.
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3 It should also have good adsorption to the semiconductor surface and high solubility to the solvent is
4 required for dye impregnation.
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6 3.1. Selection of the Dye:
7 The HOMO-LUMO energy difference of the semiconducting electrode should be in tune with the peaks of
8 the absorption spectra of the dyes. The performance study of I-V curve of DSSCs with dyes having
9 broadband absorption in the visible spectrum only is focusses in this work, since no single dye can perform
10 efficiently in the entire visible spectrum. Based on our previous studies [13], Rose Bengal dye was
11 identified for further investigation. A comparatively larger fraction of the solar spectrum (460–650 nm) in
12 the visible region is absorbed by the Rose Bengal dye and this dye has been used for further investigations
13 to sensitize different types of ZnO electrodes of the DSSCs.
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15 3.2. Performance of the DSSC:
16 The current vs. voltage characteristics were recorded for DSSCs based on ZnO nanorods and ZnO
17 nanopowders, with varying external resistances under illumination. The ZnO nanorods and ZnO
18 nanopowders has more or less similar value of the open circuit voltage. Which is expected as the ZnO and
the redox couple in the electrolyte determines the open circuit voltage mainly and it can be seen from
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20 Figure 1 that the ZnO nanopowders has got almost same value of the direct band gap as that of the ZnO
21 nanotubes and we are using the same electrolyte for the two systems.
22 The ZnO nanorods shows much higher short circuit current than ZnO nanopowders. This can be attributed
to the band structure and the DOS of two types of ZnO crystal structure as shown in Figure 1. It can be seen
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that the electron density of ZnO nanopowders are very much localized near -4 eV and its density near the
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HOMO-LUMO region is much less. This results in reduction in short circuit current. On the other hand, the
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electron density for Nanorods are much distributed around its Fermi level and it has some other indirect
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band gap energies available for transfer of electrons from the dye indicated by A, B, C, D in Figure 1. This
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makes the electron transfer to ZnO nanorods comparatively much easier resulting in higher short circuit
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current.
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30 3.3. Photovoltaic Properties:
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For measurement of Photovoltaic properties, I-V characteristics of DSSCs based on nanoporous ZnO
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fabricated from Nano Powders and ZnO nanorods fabricated through Sol-gel technique, using Rose Bengal
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dye was recorded. The photocurrent vs. photovoltage characteristics for ZnO-nanorod DSSC is presented in
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Figure 4(b). The energy conversion efficiency of ZnO nanorod DSSCs was found to be lower than that of
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ZnO nanopowder DSSCs in general. It may also be noted that typically 1% -2% efficiency was obtained for
36 ZnO-nanorod-based DSSCs with natural dyes.
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37 All the solar cell characteristics of DSSC cells with ZnO nanorods and nanopowders were calculated from
38 Figure 4(b). These values are Voc, the open-circuit voltage, Isc, short circuit current, the maximum voltage
39 Vmax and the maximum current Imax and presented in Table 1. The current voltage values are fitted with the
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40 Equation 4 for one diode equivalent circuit model [14] in Figure 4(a) by Newton-Raphson’s method.
41 Results of Curve fitting identifies the values of parasitic resistances, series (Rs) and shunt resistance (Rsh),
42 in the equivalent circuit. The parasitic resistances of DSSCs are important parameters that affect its
43 efficiency. ZnO Nanopowder based DSSC has high series resistance, whereas using ZnO Nanorod based
44 DSSC a considerable reduction in series resistance was obtained, resulting in a significant difference in cell
45 performance. It was also noted that the Nanorods have lower shunt resistances. It was also confirmed form
46 the data of Table 1, that for all kinds of cells, for higher the shunt resistance the efficiency is lowered, and
47 efficiency raises with lower series resistances.
48 Also from the I-V characteristics, all cell parameters like Ideality Factor (A), Fill factor (FF), for the cells
49 using two different type of photoanodes are evaluated using Equation (1) and subsequently the energy
50 conversion efficiency (η) is calculated using equation (2). Table 1 summarizes all these results.
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52 The ZnO Nanorods shows lowest fill factor and highest efficiency, whereas Nano-powder shows highest
53 fill factor and lowest efficiency. This improvement in efficiency for the Nanorods is due to improvement in
54 open circuit current achieved through higher density of electron states near the conduction band edge for
55 Nanorods. The efficiency enhancement can also be due to lower thickness of the ZnO nanolayer achieved
56 through the sol-gel fabrication causing lower diffusion length for the electrons. The marginal improvement
57 of fill factor, in Nanopowder based DSSC can be due to higher equivalent shunt resistance though the open
58 circuit voltages are quite high in both cases.
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3 Perfectness of the diode in the equivalent circuit is indicated by the Ideality factor (A) and for a perfect
4 diode, its value is 1.0. In our observation, ideality factor of 4.55 for ZnO Nanorods was observed,
5 compared with 4.57 of ZnO Nano powders. So, as indicated by Ideality factor Nanorods are closer to a
6 perfect diode. Due to same reason, the fill factor of Nanorods is also lower.
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8 4. Conclusion
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10 DSSCs structure was fabricated over an ITO coated glass substrate with two different photoanodes, ZnO
11 nanopowders and nanorods. More uniform thickness was observed for ZnO nanorods grown by the sol-gel
12 method. The efficiency of the DSSC solar cells related to different type of nanostructures of ZnO is
13 discussed. ZnO nanorods were found to be superior when the efficiency of DSSC’s fabricated using
14 different ZnO nanostructures was compared. The DSSC structure with ZnO nanorods results in an open
15 circuit voltage which is much higher than DSSCs with ZnO nanopowders on an ITO glass. Using the
16 equivalent circuit of an one-diode model, parasitic resistances parameters (Rs and Rsh) of DSSCs are
17 calculated from I-V curve and is also presented. In general, a ZnO nanopowder based DSSC has got
inferior qualities than the DSSC’s based on DSSC nanorods fabricated through the sol-gel method.
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21 5. References
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30 4. Y. Amao, T. Komori, Bio-photovoltaic conversion device using chlorine derived from chlorophyll
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41 8. B. Pradhan, S. Kumar, B. Amal, J. Pal, Vertically aligned ZnO nanowire arrays in Rose Bengal-based
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51 12. F.W. Fernandesa, V. Fernando G.de Paivaa, G. P. Thima, Energetic and electronic properties in a
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3 14. E.M.G. Rodrigues, R. Melício, V.M.F. Mendes and J.P.S. Catalão, Simulation of a Solar Cell
4 considering Single-Diode Equivalent Circuit Model, Renewable Energy & Power Quality Journal,
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Figure 1(a): Band structure & DOS of ZnO monolayer [12] from DFT Calculations.
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Figure 4(a): Equivalent circuit of a DSSC cell.
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33 Figure 4(b): Current-voltage curves of DSSC’s based on ZnO Nanotube and Nanopowder.
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 Journal of Materials Engineering and Performance Page 14 of 14

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6 Type of DSSC
Voc (V) Isc (mA) Is (µA) Rs (Ω) Rsh (Ω) A FF η (%)
7 photoanode
8 ZnO Nanorod
9 0.61 2.10 13.26 0.00308 3461 4.55 0.49 1.56
Based DSSC
10 ZnO Nanopowder
11 0.56 1.18 9.88 0.00489 5011 4.57 0.56 1.01
Based DSSC
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