Physica E 121 (2020) 114127

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Physica E: Low-dimensional Systems and Nanostructures

journal homepage: http://www.elsevier.com/locate/physe

Li doped ZnO based DSSC: Characterization and preparation of

nanopowders and electrical performance of its DSSC
Seval Aksoy a, Ozgur Polat b, c, Kamuran Gorgun d, Yasemin Caglar e, Mujdat Caglar e, *
a
Department of Physics, Faculty of Science, Sinop University, Sinop, Turkey
b
CEITEC BUT, Brno University of Technology, Purky� nova 123, 612 00, Brno, Czech Republic
c
Institute of Physical Engineering, Brno University of Technology, Technick�
a 2, 616 69, Brno, Czech Republic
d
Department of Chemistry, Faculty of Arts and Science, Eskisehir Osmangazi University, Eskisehir, 26480, Turkey
e
Department of Physics, Faculty of Science, Eskisehir Technical University, Yunusemre Campus, Eskisehir, 26470, Turkey

A R T I C L E I N F O A B S T R A C T

Keywords: In this study, microwave-assisted hydrothermal method (MW-HT) has been used to synthesize the nanopowders
Li doped ZnO nanopowders of Li doped ZnO, which are used in fabrication of dye-sensitized solar cell (DSSC). XRD examinations have shown
Microwave assisted hydrothermal that Li doped ZnO nanopowders synthesized in different concentration have highly crystallized hexagonal
DSSC
structure. To investigate the morphology of nanopowders, scanning electron microscopy (SEM) has been used
and the results have revealed the nanoflower morphology of Li doped ZnO powders. Kubelka-Munk function has
been utilized to determine the band gap of bare and dye loaded Li doped ZnO samples and an increase from 3.21
eV to 3.24 eV has been observed in the band gap as increasing Li content. The results of solar cell performance of
the fabricated Li doped ZnO based DSSC samples have been exhibited that the efficiency of cells increases as the
Li doping ratio is boosted and it has been observed the highest efficiency value of 1.23% for LZ10-DSSC.

1. Introduction
The increase in traditional energy consumption as a result of the
growth in the world population has triggered the interest in the search
for new renewable energy sources. Solar energy is known to be one of
the most promising renewable energy sources in the future. Therefore,
using solar energy in the future will have a positive effect on national
economies. Dye-sensitized solar cell (DSSC), proposed by O’Regan and
Gra€tzel in 1991 [1], was classified as a third-generation photovoltaic
device for the conversion of visible light to electrical energy. DSSC has
many advantages such as being cheap, no need for clean room tech­
nology, and being able to operate in low light conditions and in full
sunlight. In a DSSC, photoelectrons are generally excited from a
light-sensitized dye and injected from the photo-anode semiconductor
into the external circuit. To achieve higher power conversion efficiency,
various wide band oxides such as TiO2 [2], ZnO [3] and SnO2 [4] are
used as photoelectrode materials in DSSCs.
Since the ZnO, which can be obtained in different morphologies
(nanorod [5], nanoflower [6], nanotube [7], nanowire [8]) has a higher
of electron mobility than TiO2, it has been studied in recent years on
DSSC fabrication. Because the undoped ZnO films naturally contain
oxygen vacancies and zinc interstitials, it can be easily doped with
different elements to be improved its many physical properties. So, the
properties of ZnO can be changed by dopants. The main purpose of
doping with anions or cations is not only to optimize the band gap, but
also to modify the electrical properties. The incorporation of Li element
significantly varies the morphological and electrical properties of ZnO
nanostructure. In recent years, DSSCs that are fabricated with doped
ZnO have been studied very much since the doping elements alter the
morphology of nanopowders. The studies on the performance of DSSCs
fabricated with ZnOs doped with different elements such as Ru [9], Eu
[10], La [11], Sn [12] and Al [13] are available in the literature. But so
far, there are a few studies with Li doped ZnO on DSSC. In one of these
studies, Bhattacharjee et al. [14], obtained Li doped ZnO nanofibers by
hydrothermal method and investigated their structural and morpho­
logical properties. They observed that the diameter of the nanofibers
decreased with the Li contribution. They made DSSC fabrication with Li
doped ZnO nanofibers and examined cell performance. The authors
found the highest conversion efficiency of 0.59% for the LZ01-DSSC.
In this study, Li doped ZnO nanopowders (ZnO:Li-Npd) were ob­
tained by microwave-assisted hydrothermal method (MW-HT) in
different concentration and the structural and morphological properties

* Corresponding author.
E-mail address: mcaglar@eskisehir.edu.tr (M. Caglar).

https://doi.org/10.1016/j.physe.2020.114127
Received 31 December 2019; Received in revised form 24 March 2020; Accepted 26 March 2020
Available online 2 April 2020
1386-9477/© 2020 Elsevier B.V. All rights reserved.
S. Aksoy et al. Physica E: Low-dimensional Systems and Nanostructures 121 (2020) 114127

Table 1
The structural parameters of ZnO: Li-Npds.
Npds Code (hkl) 2θ d (Å) D a (Å) c (Å)
(degree) (nm)

LZ01 (100) 31.412 2.848 34 3.2885 5.2627

(002) 34.072 2.631
(101) 35.901 2.501
(102) 47.198 1.926
(110) 56.252 1.635
LZ1 (100) 31.342 2.854 35 3.2955 5.2718
(002) 34.012 2.636
(101) 35.832 2.506
(102) 47.127 1.928
(110) 56.173 1.638
LZ5 (100) 31.354 2.853 37 3.2944 5.2706
(002) 34.019 2.635
(101) 35.837 2.506
(102) 47.140 1.928
(110) 56.190 1.637
LZ10 (100) 31.137 2.872 40 3.3167 5.3025
(002) 33.809 2.651
(101) 35.626 2.520
(102) 46.931 1.936
(110) 55.937 1.642
Zincite (JCPDS No. (100) 31.770 2.814 – 3.2498 5.2066
Fig. 1. Schematic representation of a ZnO: Li-DSSCs. 36-1451) (002) 34.422 2.603
(101) 36.253 2.476
(102) 47.539 1.911
(110) 56.603 1.625

of these nanopowders were investigated because these properties have
significant effect on the photovoltaic performance of DSSCs. In addition,
the absorption measurements of the films coated on FTO substrate by
doctor blade method using Li doped ZnO nanopowders were made to
investigate the effect of N719 dye. And also, the reflectance measure­
ments were used to determine the band gap of the nanopowders. In the
available literature, there is no Li doped ZnO based DSSC (ZnO:Li-DSSC)
study fabricated by MW-HT. Furthermore, it should be emphasized that
the obtained efficiency value (1.23%) is higher than the mentioned
study and other ZnO based DSSC solar cells produced via only hydro­
thermal method.
2. Experimental details
2.1. Synthesis of ZnO:Li-Npds
The chemicals used in solution preparation were zinc acetate dihy­
drate (Zn(CH3CO2)⋅2H2O), Sigma-Aldrich), sodium hydroxide (NaOH,
Sigma-Aldrich) and lithium (II) acetate dihydrate (Li(CH3CO2). 2H2O),
Sigma-Aldrich). The method used for fabricating ZnO:Li-Npd via a MW-
HT is similar to that described elsewhere [15]. Differently, Lithium ac­
etate dihydrate solutions was prepared for Li doping. LiAc was added as
0.1; 1; 5 and 10 wt% into the Zinc acetate dihydrate solution. The
samples are named LZ01, LZ1, LZ5 and LZ10, respectively.
2.2. DSSC fabrication
The ZnO:Li paste was prepared by the following procedure. 0.1 g of
synthesized powder was taken up in mortar. 100 ml of water was added
and stirred. Triton X and acetyl acetone were then added and the paste
was prepared. The obtained paste was applied on to the FTO substrate by
doctor blading method and then it was annealed for 1 h at 400 � C in air
and then cooled. Thus, Li doped ZnO films were created. The thickness of
these films is about 20 μm. For DSSC fabrication, these photoelectrodes
(Li doped ZnO films) were immersed into a 0.5 mM cis-bis (2.20-bipyr­
idyl-4.40-dicarbox-ylato)-ruthenium (II) bis-tetrabutylammonium
(known as N719 dye, Solaronix) for 2 h. After the hole on the Pt
counter electrode was covered with meltonix, the ZnO:Li photoelectrode
and the Pt counter electrode were sandwiched. Finally, iodide/tri-iodide
redox couple electrolyte (Iodolyte Z, Solaronix) was injected in a space
between ZnO:Li/N719 and Pt counter electrode. The active area of the
DSSC was about 0.25 cm2. The schematic diagram of ZnO:Li-DSSC is
given in Fig. 1.
2.3. Characterization of ZnO: Li-Npds and DSSCs
The morphology of ZnO: Li-Npds were inspected using ZEISS Ultra­
plus SEM. The crystallinity of the ZnO: Li-Npds was monitored with the
help of BRUKER D2 PHASER CuKα X-ray powder diffractometer. The
absorption spectra and diffuse reflectance spectra (DRS) were recorded
on SCHIMADZU UV spectrophotometer. Photocurrent-voltage charac­
teristics of the ZnO: Li-DSSCs were measured by FYTRONIX OPTOSENSE
on solar simulator under illumination with power density of AM1.5 (100
mW/cm2).
3. Results and discussion
Fig. 2 (a) demonstrates the X-ray powder diffraction spectra of the
ZnO: Li-Npds. The characteristics peaks of zincite phase (JCPDS No. 36-
1451, zincite phase) that have hexagonal wurtzite structure are shown
in this figure. It is seen that obtained powders have polycrystalline na­
ture. All structural parameters of zincite and ZnO: Li-Npds including d-
spacing and diffraction angle are tabulated in Table 1. It should be
mentioned that whenever a foreign atom with different ionic radius is
introduced to a lattice structure, the lattice of this structure can expand
or contract depending upon the ionic radii difference between host and

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S. Aksoy et al.
Fig. 2. XRD spectra a) between 30 and 60� b) between 35 and 36� of the Li: ZnO-NPd.
dopant atom. Fig. 2 displays that the peaks move towards lower 2θ
values as the Li doping level is boosted. In order to show the peak
shifting, the most intense peak (101) of all compounds is exhibited in
Fig. 2 (b) and it can be also seen in Table 1. Such shift in the XRD spectra
can be explained by the ionic radius difference between Li (0.076 nm for
1þ) and Zn (0.074 nm for 2þ). When Li bigger ionic radius is substituted
into Zn sites with smaller ionic radius, the unit cell of Zn1-xLixO will
increase and 2θ diffraction angles shift to lower angles because of the
Bragg’s law. The crystallite size of the obtained powders has been
calculated via employing Scherrer Equation [16] and substracted lattice
parameters and crystallite sizes are provided in Table 1. It can be noticed
from Table that the lattice parameters increase as the Li dopant level is
advanced, which confirms the peak shifting in the XRD images. More­
over, the crystallite size of the samples raises with Li doping.
SEM images of the ZnO: Li-Npds are presented in Fig. 3 at various
magnifications. Low magnification SEM images reveal the full flower
structures, which are formed by the bundles of many well-aligned
nanorods. The details of nanorods are seen at higher magnification in
the same figure. It is noticed that the length of nanorods is around couple
micron with width around 300 nm. Furthermore, the hexagonal struc­
ture shape of nanorods can be seen at higher magnification, which is
confirmed by XRD investigation. One can see that the morphology of
rods varies via Li doping level. The rods start to become sharper with
advancing the Li doping level. Therefore, it can be said that the increase
in density, as well as the change in morphology, cause an increase in the
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Physica E: Low-dimensional Systems and Nanostructures 121 (2020) 114127
surface area, which plays an important role in enhancing dye loading
and light harvesting.
The absorption spectra, taken between 300 nm and 900 nm wave­
length, of the synthesized Li doped ZnO films can be seen in Fig. 4 (a)
without dye loading and in Fig. 4 (b) with 2 h dye loading. When the
powders are not loaded by dye, the absorbance peak around 360 nm can
be noticeable and it corresponds to the optical absorption edge of ZnO.
Yet, when the powders are loaded by dyes for 2 h, the two peaks become
visible one around 360 nm and other one about 530 nm. The second
peak is associated to the π - π* orbital transition. Therefore, Fig. 4 (b)
exhibits that 2 h loading time was enough for the absorbtion of dye onto
ZnO rods. The sharp absorption starting at approximately 340 nm in
both figures belongs to FTO used as the substrate.
The reflectance of bare and dye loaded Li doped ZnO films was taken
with the diffuse reflectance spectrum and data are presented in Fig. 5.
The reflectance of bare Li doped ZnO represents that the reflectivity
increases as the Li doping level goes up, Fig. 5 (a), which underlines that
Li substituted ZnO powder is well crystallized. It is also noted that
reflectivity rises with the wavelength. Furthermore, it can be noticed
that the dye loaded Li doped ZnO powders illustrate lower reflectance
than the bare sample, Fig. 5 (b).
The optical band gaps of the bare and dye loaded Li doped ZnO films
have been determined via utilizing the Kubelka Munk function F(R)
[17]. Fig. 6 (a) represents the Kubelka-Munk graph of the bare Li doped
ZnO films. The band gap values of all ZnO films were determined from
S. Aksoy et al. Physica E: Low-dimensional Systems and Nanostructures 121 (2020) 114127

Fig. 3. SEM images of the ZnO: Li-Npds.

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S. Aksoy et al. Physica E: Low-dimensional Systems and Nanostructures 121 (2020) 114127

Fig. 4. Absorbance spectra of the bare (a) and dye loaded ZnO: Li films (b).

Fig. 5. Reflectance spectra of the bare and dye loaded ZnO:Li films.

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S. Aksoy et al. Physica E: Low-dimensional Systems and Nanostructures 121 (2020) 114127

the point that cuts the energy axis of the linear part of the graph given in
inset in Fig. 6(a). It is seen that the band gap of ZnO slightly increases as
the Li doping ratio is elevated from 0.1% (3.21 eV) to 10% (3.24 eV).
The band gap of the samples was substracted as extrapolating the linear
portion of the plot that cuts the energy axis. When the band gap of dye
loaded samples are considered, Fig. 6 (b), the presence of two band gaps,
one around 3.3 eV and other one about 2.3 eV (see inset figure), becomes
visible. The gap at higher photon energy is connected to the band gap
ZnO, yet, the band gap at lower energy is ascribed to the high energy π -
π* orbital transition, which belongs to the ruthenium. Therefore, it can
be said that the ruthenium complex is excited and resulted to the metal
to ligand charge transfer (MLCT) excited state from which an electron is
injected directly to the ZnO conduction band [18].
Fig. 7(a–d) exhibits characteristic current density vs voltage curves
of the studied DSSCs under different illumination power density of light.
The short current density (Jsc), the open circuit voltage (Voc), the fill
factor (FF) and power conversion efficiency (n %) values are presented
in Table 2. It is seen that n values increase as the applied light density
rises. Furthermore, it is noted that as the Li doping level escalates, n
values advance. Fig. 7 (e) compares the current density and voltage
values of Li doped ZnO powders at 100 mW/cm2 power density of light.
It is shown that the current density and voltage values 10% Li doped
sample are higher than that of other examined samples. In our previous
study, we investigated the solar performance of undoped ZnO 2 h dye
loaded sample [19]. It has been documented that 2 h dye loaded ZnO
material has the n value of 0.23% at 100 mW/cm2 simulated sunlight. It
is seen that Li doped ZnO samples hold larger n value than the undoped
ZnO. For example, the n value of LZ01-DSSC is 0.50%, on the other hand,
the power conversion efficiency of LZ10-DSSC is 1.23% at 100 mW/cm2
simulated sunlight. It is seen that the improvement is more than fivefold
compared to the undoped ZnO sample. Such increment in power con­
version efficiency may be related to the changing in morphology and
improvement in crystallinity leading to higher dye absorption and less
resistance to the electron transfer [20,21]. In the literature, similar to Li
alkali metal used in this study, there are some DSSC studies fabricated
with other alkali metal doped ZnO such as sodium and potassium.
Miavaghi et al. [22] have grown K doped ZnO nanotapers on an ITO
substrate by using electrochemical method and performed DSSC fabri­ Fig. 6. Kubelka-Munk function of bare and dye loaded ZnO:Li films.
cation. They found the conversion efficiency around 2.84% in undoped
ZnO nanotaper based DSSCs. They reported that the conversion effi­
ciency increased up to 4.32% in K doped ZnO nanotaper based DSSCs.
Polat [23] has fabricated the undoped and Na doped ZnO nanorods on
ZnO seeded FTO substrates by utilizing chemical bath deposition. In this been investigated. It has been exhibited that the efficiency of cells in­
work, the effect of Na doping on the effectiveness of ZnO nanorod DSSCs creases as the Li doping ratio is boosted and it reaches the highest effi­
was investigated and the maximum conversion efficiency of DSSCs was ciency value of 1.23% for LZ10-DSSC. The reason might be the change in
found to be 0.22% for 2 at.% Na atoms. This value is so close to the morphology and improvement in crystallinity leading to enhance dye
efficiency value of undoped ZnO DSSC reported in our previous study absorption light harvesting.
[19].
Declaration of competing interest
4. Conclusions
None.
XRD examinations have shown that Li doped ZnO powders, synthe­
sized by MW-HT technique, have highly crystallized hexagonal struc­ CRediT authorship contribution statement
ture. Moreover, SEM investigation has revealed the nanoflower
morphology of Li doped ZnO powders. Kubelka-Munk function has been Seval Aksoy: Writing - original draft. Ozgur Polat: Writing - review
utilized to determine the band gap of bare and dye loaded Li doped ZnO & editing. Kamuran Gorgun: Investigation, Methodology. Yasemin
samples. It has been shown that the dye samples have two band gaps at Caglar: Supervision. Mujdat Caglar: Conceptualization.
around 3.2 eV and 2.2 eV, which are connected to ZnO and ruthenium,
respectively. Furthermore, solar cell performance of the samples has

6
S. Aksoy et al. Physica E: Low-dimensional Systems and Nanostructures 121 (2020) 114127

Fig. 7. J-V graph of (a) LZ01-DSSC (b) LZ1-DSSC (c) LZ5-DSSC (d) LZ10-DSSC and (e) ZnO:Li-DSSCs at 100 mW/cm2.

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S. Aksoy et al. Physica E: Low-dimensional Systems and Nanostructures 121 (2020) 114127

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