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Solar Energy
journal homepage: www.elsevier.com

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Nanostructured photoanode and counter electrode materials for efficient
Dye-Sensitized Solar Cells (DSSCs)
Nayab Abdul Karim , Umer Mehmood ⁎⁠ , Hafiza Fizza Zahid , Tahira Asif

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Department of Polymer and Process Engineering, University of Engineering and Technology Lahore, Pakistan

ARTICLE INFO ABSTRACT

Keywords: The access of dye-sensitized solar cells (DSSCs) in the photovoltaic market is still a challenge owing to low
Nanostructured power-conversion-efficiency (PCE) and stability. The foremost aim of this review is to emphasize the technical

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Photoanode issues in DSSCs that reduce their efficiency. A DSSC consists of glass substrates, photoanode, photosensitizer,
Counter-electrode electrolyte and catalytic counter-electrode. Electrode materials play a critical role in the photovoltaic (PV) perfor-
DSSCs
mance of DSSCs. The PV performance of DSSCs depends on many factors e.g. electron collection at photoanode,
Photovoltaics
light harvesting efficiency of photoanode, a scattering of electrons inside the photoanode, and the fast reduction
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Efficiency
of an electrolyte at the counter electrode. In this review, physical, electronic, and morphological properties of
electrodes materials will be examined for efficient DSSCs. This review paper comprises of four parts. First part
highlights the importance, structure and charge transport mechanism of DSSCs. The second section describes the
types, electronic and morphological properties of photoanode materials. The third part covers the nature and
catalytic properties of materials used for counter-electrodes. Finally, challenges, market and future directions of
DSSCs will be described in the last part of this review.
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1. Introduction purposes (Hassanien et al., 2018). At present, many new technologies

have been introduced in the market to convert the renewable incident
The demand of energy is increasing day by day. Extracting energy solar radiation into electricity. These technologies have proven them-
from fossil fuel is the major cause of environmental pollution (Louwen selves to be the best alternative of wind, thermal and geothermal tech-
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et al., 2016; van Ooteghem, 2010). The rapid increase of population
has a direct impact on energy demand. The emission of greenhouse
gasses in the environment is increasing owing to the burning of fossil
fuels. Greenhouse gasses are increasing the earth temperature, which
can cause a serious natural disaster. Moreover, the environmental pol-
lution has affected human health. However, energy is required to run
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nologies. However, solar energy conversion via photovoltaic cells could
be the best alternate. It can be beneficial predominantly in remote ar-
eas where an extension of the grid or installation of grid system is eco-
nomically or technically not feasible (Hammond, 1972; Hosenuzzaman
et al., 2015; Lewis, 2007; Schiermeier et al., 2008). Moreover, PV can
also reduce the demand of fossil fuels. Thus, emissions of COx, NOx

the wheel of industry. Stopping the wheel of the industry will increase
the poverty in the world. Therefore, an alternative source of energy is
crucial to replace the oil, gas, and coal (Owusu and Asumadu-Sarkodie,
2016). Solar energy, the source of renewable energy could be consid-
ered as an alternative source of energy. It is abundantly available on the
earth. Also, there is no combustion reaction involved during the genera-
tion of energy (Hosenuzzaman et al., 2015; Kabir et al., 2018; Roslan et
al., 2018).
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and SOx can be minimized by applying PV source of renewable energy
(Shahsavari and Akbari, 2018).
PV technologies are conventionally categorized into three genera-
tions (Jean et al., 2015), as shown in Fig. 1. The photovoltaic mar-
ket is still dominated with silicon (Si) based solar cells. They are sta-
ble and show the efficiency of about 15–20%. However, high produc-
tion cost (owing to high energy demand in their production) and their

rigidity are major disadvantages of Si solar cells (Płaczek-Popko, 2017).

The ultimate source of solar energy is the sun. It provides an ap- The second generation solar cells (SGSCs) are made of amorphous sil-
proximately 1.4 χ105⁠ TW of energy on the surface of the earth. How- icon, Copper Indium Gallium Selenide (CIGS), and Cadmium telluride
ever, only 3.6 χ 104⁠ TW of energy is available for utilization in useful (CdTe). Generally, they show the power-conversion efficiency (PCE) of

⁎ Corresponding author.
Email address: umermehmood@uet.edu.pk (U. Mehmood)

https://doi.org/10.1016/j.solener.2019.04.057
Received 2 January 2019; Received in revised form 18 March 2019; Accepted 16 April 2019
Available online xxx
0038-092/ © 2019.
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

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Fig. 1. Generations of photovoltaic solar cells (Jean et al., 2015).

10–15% (Green, 2002). Like first-generation solar cells, high temper- 2.1. Structure of DSSC
ature/energy treatments augment their production cost. Furthermore,
SGSCs also consist of scare elements (shown in Fig. 1), which is another The conventional structure and arrangement of each component in

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disadvantage of these types of cells (Lee and Ebong, 2017). With in-
tense R&D efforts in materials science, several organic thin film PV cells
have emerged that have high potential, including DSSCs, perovskite so-
lar cells, and quantum dot solar cells (Yan and Saunders, 2014).
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Perovskite solar cells are the newest and the most efficient tech-
nology, with the best-achieved efficiency significantly exceeding that
of amorphous Si cells and approaching that of CdTe and CIGS cells
(Djurišić et al., 2016). Since this is new technology, the stability and
lifetime issues have not been as comprehensively studied as for some
other types of solar cells. Concerning polymer solar cells, they are less
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DSSCs are shown in Fig. 2. Its structure consist of conductive glass sub-
strates, a dye-sensitized metal oxide semiconductor electrode, a catalyst
counter electrode, and an electrolyte solution inserted between the two
electrodes.
The role of each component is described as:
• Substrate must be transparent in nature. It provides a gateway to so-
lar radiation to absorb into active solar material. It also provides the
surface for the deposition of the anode (semiconductor metal oxide)
and cathode (catalyst) materials. Furthermore, it acts as a current col-

efficient as compared to DSSCs (Liu et al., 2013; Zhang et al., 2015).
Therefore, DSSCs owing to their ease of fabrication process and low cost
have got attention in the photovoltaic market. The PCE of DSSCs has
increased from ∼7% to ∼14% (Lee et al., 2017). DSSCs are the only
type of organic material based solar cells with significant commercial
deployment such as facility capable of generating ∼2000 kWh per year
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lector, thus should also possess good electrical conductivity. The over-
all performance of DSSCs also depends on the substrate conductivity
and transmittance. It is reported that transmittance must be greater
than 80% (J. Gong et al., 2012).
• Mesoporous photoanode consists of semiconductor metal oxide. It
provides surface area for the dye adsorption. Normally, it is used in

in Switzerland (Fakharuddin et al., 2014). Moreover, DSSCs have ten-
dency to even work in the cloudy environment and diffuse sunlight,
where other thin-film solar cells fail to work (Iwata et al., 2018).
Dye-sensitized solar cells market is expected to exceed 130 million
US $ by 2023 (Sharifi et al., 2014). However, the low power-conver-
sion-efficiency (PCE) is still a barrier in further penetration of DSSCs
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the paste form. The PCE of DSSCs strongly depend on morphology,
surface area, porosity, crystallinity, and the conduction band of the
semiconductor materials. Higher the surface area of material greater
will be the dye absorption (Taehan Chŏn’gi Hakhoe. et al., 2009).
• Dye sensitizer is attached to metal oxide semiconductor through a
covalent bond. It is the heart of DSSCs. It absorbs sunlight and be

technology into the photovoltaic market. The Improvement in elec-

tronic, morphological and optical properties of DSSCs materials is still
needed to enhance the PCE of DSSCs. The electrodes (photoanode
and counter-electrode) of DSSC play a vital role during photovoltaic
processes of DSSCs. The low light harvesting efficiency, electron-hole
recombination, dark current, slow electron transfer rate, and high inter-
face resistance at counter electrodes reduce the PCE of DSSCs. All these
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defects can be reduced or minimized by selecting proper electrode ma-

terials. In this review: the physical, electronic, and morphological prop-
erties of electrode materials and their effect on PCE of DSSCs will be
examined.

2. Structure and working principle

DSSCs possess different structure and working mechanism compared

to silicon solar cells. In the following section, the structure and working
principle of DSSC will be explained in detail.
Fig. 2. Components and conventional structure of DSSCs (X. Yang et al., 2013).

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N.A. Karim et al.
comes excited. There are two types of photosensitizers: a) Ruthe-
nium-based metal sensitizers and b) metal-free organic sensitizer.
• An electrolyte having redox couple in the salt solution is inserted be-
tween the electrodes. Technically, it is used to regenerate the oxidized
dye.
• Counter electrode (CE) consists of thin film of catalyst deposited on
transparent conductive glass substrate.
2.2. Mechanism and Kinetics of charge transport in DSSCs
The mechanism of DSSCs with energy level diagram is shown in Fig.
3.
Dye molecules are attached to metal oxide semiconductor through
covalent bond. The adsorbed dye absorbs solar radiation and, electrons
in the dye are become excited. Electrons tend to move from lower en-
ergy level to higher energy level. The highest occupied molecular orbital
(HOMO) is considered as low energy orbital while the lowest unoccu-
pied molecular orbital (LUMO) is considered as the high energy orbital.
The electrons are then infused into the conduction band (CB) of the
metal oxide semiconductor. They pass through a mesoporous thin film
of semiconductor and finally collect at conductive substrate. Electrons
from photoanode then reach at CE through an external circuit. Mean-
while, electrolyte regenerates the oxidized dye and then diffuses toward
the counter electrode. At counter electrode, a reduction reaction takes
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place and the electrolyte is regenerated here. In this way, the working
cycle of DSSC is completed.
For efficient charge transport in DSSCs, energy level of each com-
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ponent must be properly aligned. For example, the LUMO of dye must
be at high energy level than the CB of semiconductor. In the same way,
redox potential of electrolyte must lie above the HOMO level of dye.
Moreover, CB of semiconductor metal oxide must lie above the redox
potential of electrolyte (Dhafina et al., 2018; M.-W. Lee et al., 2015;
Pastore, 2017). All these processes occur in a narrow time scale (Zhao
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et al., 2016). Kinetics of different processes (excitation, injection and re-
generation) in DSSCs is illustrated in Fig. 4. The arrows show the exci-
tation of electron from HOMO to LUMO in dye. It normally takes 60 ns.
The injection of electron from LUMO of the dye to the CB of semicon-
ductor takes 50 fs −1.7 picoseconds. Similarly, the process of recombi-
nation of injected electron with the oxidized dye completes in a frac-
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tion of nanoseconds. While the recombination of injected electrons in
semiconductor with electrolyte take 10 microseconds. However, the re-
generation of sensitizer by electrolyte takes only 10 ns (Michael Grätzel,
2000). Thus, the fast regeneration of sensitizer and electrolyte is critical
to attain the high PCE and stability of devices. However, the kinetic re-
tardation occurs due to charge recombination (Grätzel, 2005).
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Fig. 3. Energy level diagram and working principle of DSSCs (Holmberg et al., 2014).
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Both recombination reactions take place at the photoanode electrode
PE/dye and PE/electrolyte interfaces (Thomas et al., 2014). The reduc-
tion in recombination can reduce the dark current. Open circuit volt-
age (Vo⁠ c) of the DSSCs can be enhanced by minimizing the dark current
(Id⁠ ark), according to this equation (Ebrahim, 2011):
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where Boltzmann constant is represented by kB⁠ , T shows the absolute
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temperature of the cell, q denotes the number of the electrons, and Ii⁠ nj
represents injection current.
3. Photoanode electrode (PE) material for DSSCs
The photoanode acts as an electron collector and overall perfor-
mance of device depend on shape, size, morphology and band-gap of
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PE material. Therefore, it must possess the following key characteristics
(Shakeel Ahmad et al., 2017):
• High surface area for high dye adsorption
• Conduction band of PE should promote the high electron injection
from dye to the semiconductor.
• Optimum pore size for efficient diffusion of dye
• PE should possess high photo-corrosion resistance
• PE should have light scattering ability, surface roughness and electron
acceptor ability
• It must have good adhesion with conductive substrates
The collective improvements in these rudiments (Lee et al., 2007;
Sawatsuk et al., 2009; Jang et al., 2004) conduce to higher charge-col-
lection efficiency.
3.1. Metal oxide semiconductors
Prominent metal oxides having band-gaps greater than 3 eV
(Eg⁠ > 3 eV) for example TiO2⁠ , ZnO, SnO2⁠ , SrTiO3⁠ , Zn2⁠ SnO4⁠ , WO3⁠ , and
Nb2⁠ O5⁠ have been generally used as PE material owing to their good
photo-corrosion resistance and superior electronic properties (Shakeel
Ahmad et al., 2017). Their band positions are shown in Fig. 5
(Highfield, 2015).
Akhtar and his co-workers (Akhtar, 2015) synthesized ZnO nanopar-
ticles for DSSCs. They employed them as photoanode and achieved
the PCE of 4.1%. They reasonably obtained good dye absorption of
∼2.75 × 10−⁠ 7 mol/cm2⁠ through the surface of ZnO Nano Particle (NPs)
thin film. Guo and Aegerter (1999) spin coated Nb2⁠ O5⁠ thin film (hav-
ing thickness of 6 μm) on FTO glass substrate and then heated
N.A. Karim et al.
Fig. 4. Electron transport Kinetics in the DSSCs (Michael Grätzel, 2000).
in air at 520 °C. They used it as a photoanode of DSSCs and found
the PCE of 5%. Alexander Birkel et al. (Birkel et al., 2012) employed
solvothermal reaction to prepare SnO2⁠ nanocrystals (NCs). They used
SnO2⁠ nanocrystals as a photoanode (PE) of DSSCs and found PCE of
3.2%. Haidong Zheng et al. first time used WO3⁠ nanoparticles film
as a PE and got an efficiency of up to 0.75%. (Zheng et al., 2010).
Multi-cation oxides have also been used to enhance the PCE of DSSCs.
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Bing Tan et al. (Bing Tan et al., 2007) prepared Zn2⁠ SnO4⁠ nanoparti-
cles for the photoanode of DSSCs. An overall PCE as high as 3.8% has
been achieved under 1 sun AM 1.5 illumination. Sousan Gholamrezaei
et al. (Gholamrezaei et al., 2016) used sol–gel method to prepare SrTiO3⁠
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nanostructures. They investigated the effect of morphology and paste
formation on cell’s efficiency. They found the PCE of 0.58% with FF of
59%.
Table 1 show the PCE of DSSCs fabricated with a variety of PE mate-
rials. Currently, TiO2⁠ semiconductor is considered as the best PE mater-
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ial for DSSC and cell based on TiO2⁠ has shown the record PCE of 14.5%
(Kakiage et al., 2015). Besides, TiO2⁠ is a low cost, non-toxic, and widely
available metal oxide.
Alternatively, Zinc Oxide (ZnO) possesses similar electronic prop-
erties as that of TiO2⁠ . Even, it slightly shows higher electron mobility
than TiO2⁠ . But its instability against the acidic environment reduces the
lifetime of DSSCs. Furthermore, the aggregation of dye occurs on the
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thin film of ZnO, which reduces the performance of device (Minoura
and Yoshida, 2008). Similarly, many other oxides like SrTiO3⁠ , Zn2⁠ SnO4⁠ ,
SnO2⁠ , and WO3⁠ have been used as PE of DSSCs. However, the PCE of
DSSCs based on these materials is far lower than TiO2⁠ .
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Fig. 5. Band positions of different semiconductor metal oxides (Akhtar, 2015).
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Normally, TiO2⁠ is found in three crystalline forms. These include ru-
tile (Eg⁠ = 3.05 eV), anatase (Eg⁠ = 3.20 eV) and brookite (3.28 eV) (Lau et
al., 2014; Valencia et al., 2010). Anatase form of TiO2⁠ has a higher sur-
face area, an optimum band gap and higher coefficient of electron dif-
fusion as compared to rutile. On the other hand, brookite form of TiO2⁠
is difficult to synthesize and, is therefore not recommended for DSSCs
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photoanode (N.-G. Park et al., 2000). Consequently, the anatase TiO2⁠ is
extensively utilized as the major constituent of the PE in DSSCs. All fur-
ther discussion will be based on anatase TiO2⁠ .
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3.2. Factors affecting the performance of photoanode electrode (PE)
The performance of PE depends on the surface area, morphology,
and purity of metal oxides. Conventional TiO2⁠ film possesses high trans-
parency. But it has low light-harvesting efficiency (LHE) owing to poor
light scattering inside the film. Low light scattering could be attributed
to nanometer size of TiO2⁠ particles. In addition, low mobility of TiO2⁠
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nanoparticles also promote the charge recombination reactions of in-
jected electrons and photosensitizer and electrolyte. The aim of this part
is to emphasize the main factors affecting the performance of photoan-
ode. This section also explains the key factors to improve the perfor-
mance of PE for efficient DSSCs.
3.2.1. Effect of Size/surface area of TiO2⁠
The size of TiO2⁠ particles in the PE film can influence the solar cell
performance in many ways (Dhungel and Park, 2013). Porous TiO2⁠ films
with larger particle size show lower surface area and vice versa (Chou
et al., 2007). Films with large particle size provide small surface area
for dye adsorption, which ultimately reduces the light absorbed by sen-
sitized PE resulting in low photocurrent from the cell. On the other
hand, films comprising of smaller particles show larger number of grain
boundaries to be overcome by the electrons injected by excited dye mol-
ecules, which enhance the probability of trapping of electron (Gracia et
al., 2004; Gregg, 2004).
Properties of mesoporous TiO2⁠ strongly depend on the synthesis
method (Bagheri et al., 2015). TiO2⁠ can be synthesized by several
methods. These include hydrothermal processing, sol-gel method, mi-
crowave process, and template methods. Tammy et al. (Chou et al.,
2007) prepared TiO2⁠ by way of sol-gel processing. They found that the
dye adsorption on TiO2⁠ film depends on the particle size and surface
area of TiO2⁠ . Fig. 6a shows the relation between the particle size and
amount of dye adsorbed. It illustrates that the adsorption of dye in-
creases with increasing particle size. However, surface area decreases
with an increase of particle size. Thus, there must be a trade-off among
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

Table 1
PCE of DSSCs based on different metal oxide photoanode.

Sr. No PE PCE % Ref

1 ZnO NPs 4.10 Akhtar (2015)

2 ZnO NS 5.31 Y.-C. Chen et al. (2018)
3 ZnO 5.60 Minoura and Yoshida (2008)

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4 ZnO Platelets 5.63 De Marco et al. (2017)
5 ZnO Nanotubes 1.60 Abd-Ellah et al. (2013)
7 Nb2⁠ O5⁠ (6 μm) 5.00 Guo and Aegerter (1999)

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8 Nb2⁠ O5⁠ (4 μm) 4.10 Ou et al. (2012)
9 Nb2⁠ O5⁠ NPs 3.15 Liu et al. (2016)
10 SnO2⁠ NCs 3.20 Birkel et al. (2012)
11 SnO2⁠ 2.85 Basu et al. (2016)
12 SnO2⁠ NPs 2.88 Wanninayake et al. (2016)
13 WO3⁠ NPs 0.75 Zheng et al. (2010)
14 WO3⁠ NPs 0.29 Hara et al. (2011)
15 WO3⁠ Nanotubes 0.76 Hara et al. (2011)
16 WO3⁠ 3.32 Elbohy et al. (2018)

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17 WO3⁠ Nanorods 1.51 Yong et al. (2013)
18 Zn2⁠ SnO4⁠ NPs 3.80 Bing Tan et al. (2007)
19 Zn2⁠ SnO4⁠ Nanofibers 3.70 Choi et al. (2013)
20 Zn2⁠ SnO4⁠ beads 6.30 Hwang et al. (2015)
21 SrTiO3⁠ NPs 0.58 Gholamrezaei et al. (2016)
22 SrTiO3⁠ Nanocrystalline 1.80 Burnside et al. (1999)
23 TiO2⁠ 14.5 Kakiage et al. (2015)
24 TiO2⁠ 11.9 Ozawa et al. (2016)
25 TiO2⁠ 10.2 C.-C. Chou et al. (2014)

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the particle size, surface area, and the dye adsorption amount. They
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also found out that the PCE of DSSCs increase with the increase of
dye adsorption owing to increase of current density (shown in Fig.
6b). E.C.Muniz et al. prepared anatase TiO2⁠ colloidal dispersions by hy-
drothermal method and the particle size of synthesized TiO2⁠ was found
in the range of between 15 and 20 nm. They used mesoporous films
as PE of DSSCs and found PCE of 5.2%. TiO2⁠ aerogels are 3-dimen-
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sional interconnected network structures offer high surface area, large

pores and low density. S. Alwin et al. (Alwin et al., 2017) synthesized
TiO2⁠ aerogels by a microwave assisted sol-gel method with an average
particle size of 14.5 nm. They employed it as a photo-anode material
in quasi-solid DSSCs and achieved PCE of 5.2% with current density
Fig. 6. (a) Dye adsorption as a function of particle size and (b) efficiency of DSSC as a
of 15.18 mA/cm2⁠ and an open circuit voltage of 0.62 V. Tapan Kumar function of dye adsorption (Chou et al., 2007).
Das et al. (Das et al., 2018) used template method to fabricate TiO2⁠
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photoanode. A sol-gel method was employed to synthesize nano-porous
TiO2⁠ . In this method, dextran (TNPO-D) and glucose (TNPO-G) were
used as templates. The calcination caused the decomposition of templat-
ing agents and created nano-pores of 10 nm in TiO2⁠ . Then employed in
DSSCs and got PCE of 4.1% and 3.7% with TNPO-D and TNPO-G, re-
spectively.
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DSSCs based on different nanostructures of anatase TiO2⁠ photoanodes
are summarized in Table 2.
3.2.2.1. Nanofibers (NFs) Nanofibers show intense light absorption in
the visible region. This is partly derived optical path length extending
from the wavelength of incident light caused by scattering of light in a
layer of TiO2⁠ nanofibers (Chuangchote et al., 2008; Ilahi et al., 2017).

Fig. 7. shows the TEM images of TiO2⁠ particles produced by (a)
sol-gel method (Muniz et al., 2011), (b) hydrothermal method (Muniz et
al., 2011), (c) Microwave assisted method (Alwin et al., 2017), and (d)
Template method.
3.2.2. Morphology
The recombination of injected electrons with an electrolyte is the
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Surawut et al. (Chuangchote et al., 2008) fabricated TiO2⁠ nanofibers
using electrospinning and sol-gel techniques. After calcination, anatase
TiO2⁠ nanofibers exhibited the one-dimensional structure of high crys-
tallinity and an average diameter of ∼250 nm. They obtained the quan-
tum efficiency (QE) of 85% at the wavelength of 540 nm with the con-
version efficiency of 10.3%. Prakash Joshi and his coworkers (Joshi et
al., 2010) used the composite of electrospun TiO2⁠ NFs and TiO2⁠ NPs for

main lose path in DSSCs. It enhances the dark current and ultimately
reduces the performance of device (Longo and De Paoli, 2003). Al-
though, mesoporous structure TiO2⁠ possesses an excellent dye adsorp-
tion capability. But it experiences low electrical conductivity owing
to more interfaces between particles. Moreover, penetration of elec-
trolyte into pores also promotes the recombination reaction. These bar-
riers encourage the development of new morphologies or nanostruc-
tures of TiO2⁠ with good electrical conductivity and dye adsorption abil-
ity (Shakeel Ahmad et al., 2017). Several nanostructures of TiO2⁠ like
nanowires, nanotubes, nanorods, and hollowspheres have been fabri-
cated for efficient DSSCs. In this subsection, we will briefly discuss the
effect of each structure/ morphology on the PCE of DSSCs. The PCE of
photoanode in DSSCs. They found that the PE made by 15% TiO2⁠
nanofibers exhibited the best efficiency of 8.8%. Cao et al. (2016) syn-
thesized novel hierarchical nanorod-branched TiO2⁠ nanofiber non-wo-
ven fabric film for DSSCs. They achieved PCE of 6.26% with greatly
improved short-circuit current density (Js⁠ c).
3.2.2.2. Nanowires (NWs) The insertion of NWs can improve an energy
barrier at the interface of semiconductor/electrolyte, reduce the elec-
tron transfer to the electrolyte and decrease the density of surface
traps, which are considered to be the recombination centers. Motonari
Adachi and his coworkers (Adachi et al., 2004) fabricated TiO2⁠

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N.A. Karim et al.
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Fig. 7. HRTEM images of TiO2⁠ particles produced by (a) Sol-gel Method (Phonkhokkong, n.d.), (b) hydrothermal method (Muniz et al., 2011), (c) Microwave assisted method (Alwin et
al., 2017) and (d) Template method (Das et al., 2018).
nanowires by using low temperature surfactant-assisted self-assembling
processes. By using this photoanode in DSSCs, they achieved the PCE
of 9.3%. Liu et al. (2018) synthesized nanowires directly on the con-
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ductive glass substrate via two-step solvothermal reaction. They used
them as photoanode and found PCE of 5.30%. Similarly, ultra-long hi-
erarchical bud-like branched TiO2⁠ nanowire arrays on FTO glass sub-
strate have been prepared via a two-step solution route (Liu et al.,
2017). DSSCs based on this photoanode showed the PCE of 6%. Liu et
al. (2015) used the hydrothermal method to synthesize TiO2⁠ nanowire
arrays on titanium mesh substrate. The average diameter of synthesized
nanowire was 80 nm. By using these TiO2⁠ nanowire arrays as photoan-
ode in DSSCs, they found the PCE of 3.43%.
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3.2.2.3. Hollow spheres Hollow spheres of TiO2⁠ possess good light scat-
tering ability as well as high charge generation capacity. These promis-
ing features enhance the overall performance of DSSCs. Koo et al.
(2008) fabricated bifunctional hollow spheres of TiO2⁠ for PE of DSSCs
and got the record efficiency of 10.34% under one sun illumination.
Sun et al. (2017) fabricated TiO2⁠ double layer films composed of hol-
low spheres as overlayer and nanoparticles as an underlayer. Then,
they co-sensitized the thin film with Bi2⁠ S3⁠ quantum-dots (QDs) and
N719 dye for DSSCs and achieved PCE of 7.50%. Yolk-shell hollow
spheres were synthesized by Li et al. (2015). They used one-pot tem-
plate-free solvothermal method to synthesize this nanostructure. This
distinctive configuration showed higher light scattering capability en-
suing in PCE as high as 11%.
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

Table 2 3.2.3. Nanocomposites of anatase TiO2⁠ with carbon allotropes

Photovoltaic performance of DSSCs based on different Morphologies.
Even though bare TiO2⁠ possesses many extraordinary properties for
Sr. PCE the perfect PE, but the performance of the pristine TiO2⁠ based DSSCs is
No Structure of TiO2⁠ based Photoanode (%) Ref. still low for high-performance applications. Instead of this, the synthesis
of different morphologies of TiO2⁠ requires a complex and complicated
1 Nanofibers 10.3 Chuangchote et al. process. For example, to control the length, diameter and thickness
(2008)

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of nanotubes and nanorods needed precise reaction conditions (Low
Nanofibers/Nanoparticles 8.80 Joshi et al. (2010)
Nanofibers 6.26 Cao et al. (2016) and Lai, 2018). Therefore, in order to avoid complex synthesis process,
Nanofibers 7.00 Yang and Leung nanocomposites of carbonaceous materials with TiO2⁠ have been pro-

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(2011) posed to get high-performance DSSCs. Carbon allotropes have good elec-
Nanofibers 8.50 Hwang et al. (2012)
trical conductivity, high electron mobility, and good stability against
Nanofibers 7.53 Krysova et al. (2013)
2 Nanowires 9.30 Adachi et al. (2004) electrolytes (Batmunkh et al., 2015). Particularly, carbon nanotubes and
Nanowires 5.30 Y.-Y. Liu et al. graphene have proved themselves as efficient fillers for PE of DSSCs. It
(2018) is owing to their high electron mobility and light harvesting properties
Nanowires 6.00 Y.-Y. Liu et al. (Batmunkh et al., 2015; Low and Lai, 2018). This section will compre-
(2017)
hensively review the applications of nanocomposites of carbonaceous
Nanowires 3.43 Liu et al. (2015)
materials with TiO2⁠ for efficient DSSCs.

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Nanowires/Nanoparticles 7.34 Lee et al. (2016)
Nanowires 8.51 Wang and Bai 3.2.3.1. Carbon nanoparticles/TiO2⁠ based composites Carbon black is sel-
(2014) dom used in PE of DSSCs. The addition of carbon black as an impurity
3 Hollowspheres 10.34 Koo et al. (2008)
in TiO2⁠ nanoporous film could be considered as an extrinsic semicon-
Hollowspheres/ Nanoparticles 7.50 Sun et al. (2017)
yolk-shell microspheres 11.0 Li et al. (2015)
ductor layer. The conduction band of carbon black is higher as com-
Hollowspheres/ nanorod 4.57 Dai et al. (2012) pared to TiO2⁠ . The higher conduction band of carbon black could en-
Hollowspheres doped with N 8.08 Cui et al. (2017) hance the conduction band energy level of carbon black/TiO2⁠ film.
Hollowspheres 5.13 P. Zhang et al. Therefore, a higher output voltage is obtained by using carbon black/
(2016)

D
TiO2⁠ as a PE (Ting and Chao, 2010). This mechanism is also shown in
4 Nanotubes (L = 3.6 μm, T = 17 nm, 4.70 Paulose et al.
D = 46 nm) (2006a) Fig. 9.
Nanotubes (L = 5 μm, T = 20 nm, 4.80 Bwana (2009) Ting and Chao (Ting and Chao, 2010) improved the PCE of DSSCs
D = 100 nm) by applying the triangular arrangement between TiO2⁠ /carbon black
TE
Nanotubes (L = 20 μm, T = 24 nm, 6.89 Shankar et al. nanocomposite and dye, as shown in Fig. 10. They found an increase in
D = 132 nm) (2007)
open circuit voltage (Vo⁠ c) from 0.5 V to 0.6 V. Also, the short-circuit cur-
Nanotubes (L = 6 μm, T = 20 nm, 4.24 Paulose et al.
(2006b)
rent density and PCE were improved.
D = 110 nm)
Nanotubes (L = 5.7 μm, T = 8 nm, 3.00 Kai Zhu et al. (2007) Kang et al. (Kang et al., 2007) used thermally treated carbon black
D = 30 nm) for carbon/TiO2⁠ nanocomposites. They used nanocomposite thin film
as a photoanode and found 31% improvement in the efficiency of
EC

3.2.2.4. Nanotubes One-dimensional nanotubes considerably improve
the electron transport properties of TiO2⁠ . Nanotubes provide the
smooth electronic path for injected electrons and hence the electrical
conductivity is improved. Moreover, there are far less inter-crystalline
RR
DSSCs. D.Y. Kim et al. (2012) also used hydrothermal method to prepare
nanoporous carbon/TiO2⁠ films and employed them as PE in DSSCs. They
achieved the PCE of 3.4% by applying carbon/ TiO2⁠ PE and this PCE was
higher than that of standard Pt based DSSCs (2.54%). Three different
sizes of spherical carbon particles (700 nm, 500 nm and 250 nm) were
synthesized by Yang et al. (G. Yang et al., 2011) using hydrothermal

contacts in nanotubes as compared to TiO2⁠ NPs, which accelerate elec-
tron transport. The fast electron transport significantly minimizes the
recombination reaction, as illustrated in Fig. 8. Length, diameter, and
thickness of tubes also affect the performance of DSSCs (Kai Zhu et al.,
2006; D. Kim et al., 2008; Roy et al., 2010; L. Sun et al., 2010).
Effect of thickness: There must be an optimum wall thickness for
CO
method and then incorporated into TiO2⁠ nanoparticles. They attained
the PCE of 7.2% by using 500 nm carbon particles, higher than that of
standard cell (5.6%). Guo et al. (Guo et al., 2012) synthesized rectangu-
lar bunched TiO2⁠ nanorod and aligned this structure on carbon fibers to
make photoanode. By using this structure, they found the efficiency of
1.28%, which was 68% higher than that of that of the NRs-only. Jang et
al. (Jang et al., 2013) employed glucose-based carbon integrated TiO2⁠

the formation of a space charge layer, which can accelerate the fast elec-
tron transport to minimize the recombination. If the tube wall is too
thin, it will not bear the space charge layer and the transportation of
electrons will be obstructed and condensed to that alike in a usual NPs
PE. This will uphold the recombination reactions and hence the effi-
ciency will be reduced.
Length of tube: Length of the tube affects the overall PCE of DSSCs.
UN
PE film for DSSCs. The DSSCs based on glucose/TiO2⁠ PE showed 11.6%
higher PCE as compared to conventional device.
3.2.3.2. Carbon nanotubes/TiO2⁠ based composites Recombination occur
at interfaces of TiO2⁠ /dye and TiO2⁠ /electrolyte in DSSCs (Jarl Nissfolk
et al., 2006). Photoanode based on 1-D nanostructure have been widely
used to minimize the recombination reactions in DSSCs. The promising
member of this class is carbon nanotubes (CNTs, MWCNTs, and SWC-

The longer length will absorb more dye and thus higher will be the cur-
rent density. However, in order to enhance the charge collection effi-
ciency, the length of the tube must be less than the electron diffusion
length. It is because the current density depends on the charge collec-
tion efficiency of PE.
Tube diameter: Adsorption of dye depends on the inner diameter
or pore size of the tube. Larger the pore size lower will be the surface
area for dye adsorption and vice versa. In addition, the spacing between
tubes is also a critical parameter for the dye adsorption. More spacing
will allow the high rate of dye adsorption.
Effect of length, diameter and thickness of nanotubes on the perfor-
mance of DSSCs has been summarized in Table 2.
NTs) possess high electron mobility and provide an effective transport
path for injected electrons (Cai et al., 2015). Instead of providing an ef-
fective transport path (Y. Liu et al., 2018), high conductivity of CNTs
also play a crucial role in the high performance of DSSCs (Peng et al.,
2017). A statistical concept of percolation can be used to describe the
configuration of an inestimable cluster of connected trails (He and
Tjong, 2014). Letting down the percolation threshold is a critical con-
cern to attain light economical conductive composite material. Parti

7
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

F
OO
PR
D
TE
EC

Fig. 8. (a) DSSCs based on TiO2⁠ nanotubes based PE, nanotubes were grown on Ti substrate and (b) comparison of electron transport paths in NPs and nanotubes (Jennings et al., 2008).
RR
CO

Fig. 10. Triangular arrangement between TiO2⁠ /carbon black nanocomposite and dye
(Ting and Chao, 2010).
UN

Fig. 9. Vo⁠ c enhancement mechanism by using extrinsic semiconductor layer of carbon
black/TiO2⁠ (Batmunkh et al., 2015).
cles with large aspect ratio were reported to have a low threshold than
spheres due to a larger excluded volume at the same weight. Therefore,
the use of CNTs in place of carbon black leads to a lower percolation
threshold and higher maximum conductivity in CNTs/TiO2⁠ composites
(Sandler et al., 2003).
Alignment and dispersion of CNTs are also important for high per-
formance. The alignment of CNTs made composites to exhibit a great
anisotropic behavior in the two directions. It has been observed that
the conductivity in the parallel direction is higher than that in the per

8
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

pendicular direction (Guan et al., 2013; Q. Wang et al., 2012). In the

same way, the PCE of DSSCs is strongly affected by the dispersion of
CNTs in the base fluid (Sun et al., 2011). However, it has been found
out that the dispersion of CNTs in base fluids (water, ethanol etc.) is
very difficult owing to a lack of hydrophilic groups (Munkhbayar et
al., 2013). Therefore, the functionalization of CNTs is carried out to en-

F
hance the dispersibility of CNTs in the solvent.
The mechanism of charge recombination reduction can be explained
as the conduction band (EC⁠ B) of CNTs (∼0 eV vs. NHE: for MWCNTs) is

OO
lower than TiO2⁠ (−0.5 eV vs. NHE), this difference would shift the Fermi
level (FL) towards more positive or downward (Anusorn Kongkanand
et al., 2007). The mechanism of the downward shift of Fermi level ow-
ing to MWCNTs has also been explained in Fig. 11a (Du et al., 2013).
The shifting towards more positive potential depends on CNTs contents.
The charge injection efficiency increases with the increase of CNTs con-
tents owing to shifting of FL towards more positive potential (Anusorn

PR
Kongkanand et al., 2007). Similarly, the charge collection efficiency is
another critical factor, which is associated with the transport of elec-
trons in the PE of DSSCs (Sommeling et al., 2006). The addition of CNTs
increases the conductivity of PE by providing an effective transport path
for the movement of electrons inside the PE (Brown et al., 2008). Addi-
tionally, the fast transport of electrons reduces the recombination of in-
jected electrons with electrolyte, as shown in Fig. 11b. This reduction in
recombination enhances the overall fill factor (FF) of DSSCs and hence

D
improves PCE.
However, Guai et al. (2012) observed that the semiconducting SW-
CNTs provide better photovoltaic performance as compared to metal-
lic SWCNTs. It could be attributed to non-continuous band structure of
TE
s-SWCNTs, whilst metallic based SWCNTs possess zero band-gap (Dang
et al., 2011). 3D-network of s-SWCNTs/TiO2⁠ provides better charge
Fig. 12. Energy level illustration of DSSCs with (a) semiconducting SWCNTs and (b)
transport path for the injected electrons within the structure of PE. This metallic SWCNTs incorporated in TiO2⁠ films (Guai et al., 2012).
structure also minimizes the charge recombination of injected electrons
with an electrolyte owing to high energy barrier compared to m-SWC-
NTs. Fig. 12 shows that the higher energy barrier restricts the backflow
EC

bon particles (Chen et al., 2012; Tang et al., 2010; H. Wang et al.,
of electrons and improves the overall performance of devices.
2012; Yang et al., 2010). The reason is that the weak interaction of
3.2.3.3. Graphene/TiO2⁠ based composites Graphene possesses tunable
CNTs with the spherical TiO2⁠ nanoparticles limits the overall efficiency
bandgap, high surface area, and high electron mobility. Owing to these
of DSSCs owing to higher charge recombination with electrolyte com-
characteristics, graphene is considered as an ideal additive material for
pared to graphene. On the contrary, single sheet of graphene provides
the PE of DSSCs. Moreover, 2D-graphene sheet provides an effective
better contact with TiO2⁠ nanocrystallites on the nanoscale. In addition,
charge transport path for the injected electrons (Roy-Mayhew and
RR

Aksay, 2014). Many experimental investigations show that the
graphene-based PEs provide better PCE as compared to CNTs and car
CO
graphene has a work function (–4.42 eV) (Tang et al., 2010), which pre-
cisely lies between the EC⁠ B of TiO2⁠ (–4.4 eV) (Hagfeldt et al., 2010) and
FTO conductive glass substrate (–4.7 eV) (Hagfeldt et al., 2010). This
suitable energy level provides the stepwise transfer of photo-generated
electrons from TiO2⁠ conduction band to FTO substrate (shown in Fig.
13a). Fig. 13b shows that graphene bridges the TiO2⁠ and FTO (Dembele
et al., 2015; Yang et al., 2010). These advantages make graphene as a

perfect material for the photoanode of an efficient DSSC.

Nanocomposites of anatase TiO2⁠ with carbon allotropes and their ef-
fect on the PCE of DSSCs have been summarized in Table 3.

3.2.4. Doping of different elements

TiO2⁠ NPs have a tendency to absorb UV-light, which can cause
UV-degradation of materials. In addition, it also shows low electron mo-
UN

bility. Doping of different metals can be used to modify the electronic

Fig. 11. Effect CNTs inclusion: (a) Energy level shift and (b) Improvement in the electrical
conductivity (Du et al., 2013).
properties of TiO2⁠ (Hoye et al., 2013). It is basically the insertion of a
small amount of impurity into TiO2⁠ - lattice. The doping of different el-
ements increases the conductivity by increasing the free charges in the
materials. N-type dopants have higher valency compared to host ma-
terials and donate electrons to host materials. Similarly, holes are do-
nated by p-type materials having lower valency compared to native ma-
terial. In general, trap states as well as the electronic structure of TiO2⁠
are directly affected by doping of impurities (Duan et al., 2012). Doping
can replace either cation (Ti4⁠ +) or anion (O2⁠ −) in TiO2⁠ , depending on
the type of dopants. Dopants could be metallic (cationic) or non-metal-
lic (anionic). Electronic structure of TiO2⁠ shows that the conduc

9
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

Table 3
PCEs of DSSCs based on naocomposites of carbon allotropes with anatase TiO2⁠ .

Sr. Photoanode (Carbon Allotropes with PCE

No TiO2⁠ ) (%) Ref.

1 Carbon Black (CB) 0.17 Ting and Chao (2010)

2 Thermally treated CB 5.60 Kang et al. (2007)

F
3 Nanoporous carbon 3.40 D. Y. Kim et al.
(2012)
4 spherical carbon particles 7.20 G. Yang et al. (2011)

OO
5 Carbon fibers 1.28 Guo et al. (2012)
6 (COOH)-functionalized MWCNTs 7.95 Benetti et al. (2016)
7 0.2% and 0.4% CNTs (Layered 10.5 Barberio et al. (2016)
TiO2⁠ /CNT/TiO2⁠ )
8 0.010 wt% MWCNTs 9.00 Dembele et al. (2013)
9 0.1 wt% MWCNTs 6.21 Delekar et al. (2018)
10 Plasma-Treated Carbon Nanotubes 6.34 S. Zhang et al. (2011)
11 MWCNTs 7.37 Muduli et al. (2009)
12 CNTs 5.15 Sawatsuk et al.

PR
(2009)
13. 0.1% MWCNTs 1.96 Chang et al. (2012)
14 Multilayer MWCNTs nanocomposites 7.53 Anjidani et al. (2017)
15 0.3% MWCNTs 9.05 Chan et al. (2013)
16 Modified MWCNTs 5.94 Choi et al. (2010)
17 0.1 wt% of MWCNT 5.02 Lee et al. (2008)
18 (TiO2⁠ /MWCNTs) hybrid nanofibers 5.63 Du et al. (2013)
19 0.025 wt% MWCNTs 10.3 Sawatsuk et al.
(2009)
20 TiO2⁠ /MWCNTs with electric field 5.15 Jin et al. (2011)

D
21 0.32 wt% MWCNTs 3.85 Golobostanfard and
Abdizadeh, (2014a)
22 Acid treated SWCNT 2.16 Golobostanfard and
Abdizadeh (2014b)
Fig. 13. (a) Energy level diagram of Graphene/TiO2⁠ based DSSCs (Low and Lai, 2018) and
TE
23 0.1% MWCNTs (14.64 μm thickness) 10.24 Yang and Leung
(b) Charge transfer mechanism in composite anode (Dembele et al., 2015).
(2013)
24 0.025 w % CNTs into a Cr-doped TiO2⁠ 7.47 Massihi et al. (2013)
tion band (CB) edge is constituted by Ti4⁠ + 3d bands and valence band 25 MWCNT 7.27 Kilic et al. (2016)
edge is constituted by O2⁠ − 2p bands. Thus replacing the Ti4⁠ + by us- 26 Three layers of TiO2-GR 5.11 Wang and Cho (2017)
ing different cations affects the CB and replacing O2⁠ − by different an- nanocomposites
27 0.005 wt% Graphene nanoribbon 7.18 Akilimali et al. (2018)
ions affects the VB energy. (Duan et al., 2012). The higher atomic ra-
EC

28 0.16% graphene 4.03 Mehmood et al.

dius of dopant than the replacing material could impede the overall per- (2015)
formance of devices. Therefore, the atomic radius of dopant should be 29 Graphene 4.28 Zhu et al. (2014)
equivalent to target materials (cation or anion) (Duan et al., 2012). Two 30 TiO2⁠ (13 μm)-graphene (15 μl) 8.07 Tsai et al. (2015)
or more than two dopants can also be incorporated in semiconductor 31 Graphene oxide nanosheets 4.65 Wang et al. (2015)
32 Graphene with 8 printing layers of 6.49 Zhang et al. (2014)
materials. Each dopant will discretely affect the performance of devices
TiO2⁠
(Ko et al., 2005). Multi-dopants can strengthen the effect of each other 33 Graphene 6.46 Pishdar and
RR

(J.C. Zhang et al., 2011) and may also minimize the detrimental effects Samadpour (2016)
caused by the other dopant (Berglund et al., 2013). 34 Functionalized Graphene 8.13 Chen et al. (2012)
35 1% Graphene/titanate nanotubes 8.67 Tang and Hu (2012)
There are number of ways of introducing the dopant into the lattice
(GTNTs)
of TiO2⁠ : 36 Nafion-coated graphene prepared by 2.70 S. Sun et al. (2010)
Heterogeneous coagulation
• Simple mixing method: Dopant material is physically mixed with 37 Nitrogen-doped graphene@nickel 9.75 Ranganathan et al.
TiO2⁠ . In this case, TiO2⁠ may be present in suspension or paste form. oxide (2017)
CO

The prepared materials can be deposited on glass substrate through

sol–gel, hydrothermal, electrochemical deposition, atomic layer depo-
sition, or electrospinning methods (Nah et al., 2010). material and its catalytic activity. The theoretical open circuit voltage
• Anodization and thermal oxidation can be used to deposit a Ti-dopant (Vo⁠ c) of DSSCs is defined as the difference of redox potential of elec-
alloy (M. Yang et al., 2011). trolyte and the Fermi level of semiconductor. The open circuit voltage
is always obtained at zero current. However, the obtained photovoltage
The PCEs of DSSCs based on doped-TiO2⁠ with different dopants are
UN

listed in Table.4.
4. Catalytic materials for counter electrode (CE)
There are three functions of CE in DSSCs (Thomas et al., 2014; Yun
et al., 2014): (a) The deposited material on substrate acts as a cata-
lyst and accelerates the reduction reaction, (b) It provides electrons for
the regeneration of charge transport mediator (electrolyte), and (c) elec-
trons from the external circuit meet at the CE and then inject into the
cell. The photovoltaic parameters of DSSCs strongly depends on the CE
is always less than the open circuit voltage of cell. This lose in volt-
age could be due to the over-potential of CE, which comes from the
transfer of electron via charge transport mediator and through the in-
terface of electrolyte and CE (Guan et al., 2013). The ionic conductiv-
ity of electrolyte strongly influences the transportation of electrons (for-
mer). On the other hands the catalytic activity of catalyst materials de-
termines the interface resistance of CE and electrolyte. The magnitude
of interface resistance determines the rate of transfer of electrons (lat-
ter) (Papageorgiou, 2004).
For efficient DSSCs, CE must fulfill the following requirements: op-
timum thickness of catalyst material on conductive substrates, high
catalytic activity, good conductivity, high surface area, porous struc-
ture, corrosion resistance against electrolytes, good adhesion with sub-
strates, and energy level alignment with electrolyte (Kim et al., 2006;
Papageorgiou et al., 1997). Platinum (Pt) is considered as an ideal ma-
terial for an efficient DSSC. It possesses high catalytic activity, electri
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

Table.4 the particle size, good distribution and better adhesion of Pt nanopar-
PCEs of DSSCs based on doped TiO2⁠ photoanodes.
ticles on FTO substrate, urea-assisted homogeneous deposition ethylene
Sr. PCE glycol (HD-EG) method was explored by Song et al. (Song et al., 2012).
No Dopants (%) Ref. The CE prepared by HD-EG method was utilized in DSSC. The device as-
sembled with this type of CE electrode showed a PCE of 9.34%. So far,
1 Niobium (Nb): 2.5 mol% Nb-doped 8.00 Nikolay et al. (2011) Pt based DSSC with cobalt (III/II) Co2⁠ +/Co3⁠ + complex as an electrolyte
TiO2.

2 2.5 mol% Nb-doped TiO2⁠ 7.41 Kim et al. (2013)
3 5% Nb doped-TiO2⁠ 5.34 Saurdi et al. (2016)
4 5% Cerium (Ce) doped-TiO2⁠ 6.30 J.W. Lee et al. (2015)
F
has achieved the PCE of 13.8% (Kakiage et al., 2015).
Thus, it can be demonstrated that Pt nanoparticles based CE shows
much better performance than the bulk Pt. The reason is that Pt

OO
5 0.1% Ce doped-TiO2⁠ 7.65 Zhang et al. (2012b) nanoparticles have high electrical conductivity, low charge transport re-
6 0.2% Scandium (Sc) doped-TiO2⁠ 9.60 Latini et al. (2013)
sistance, high surface area, high corrosion resistance, and high transmit-
7 0.2% Tungsten (W) doped-TiO2⁠ 9.10 X. Zhang et al. (2011)
8 50 ppm Tungsten (W) doped-TiO2⁠ 7.42 Tong et al. (2014) tance (Wu et al., 2017). The characteristics features make Pt nanopar-
9 Chromium (Cr)/TiO2⁠ 2.97 Asemi et al. (2017) ticles as an ideal material for DSSCs (Thomas et al., 2014). Other mor-
10 10% Cr–TiO2⁠ 8.40 C. Kim et al. (2008) phologies of Pt like nanotubes, nanorods, multipods, and nanowires
11 50 ppm Cr doped-TiO2⁠ 6.35 Xie et al. (2013) have also been synthesized and utilized in DSSCs. These structures also
12 0.5 mol % Sn-doped TiO2 8.31 Duan et al. (2012)
give promising results. Some of these structures are shown in Fig. 14
13 3.7% Sn-Doped TiO2 6.24 Ako et al. (2015)
(Wu et al., 2017).

PR
14 Ho3+ ⁠ -Yb3 ⁠ +-F−⁠ tri-doped TiO
2⁠ 6.99 Wei et al. (2017)
15 Er3⁠ +-Yb3⁠ +/ TiO2⁠ 8.10 W. Liu et al. (2017) By using Pt as a catalyst material for the CE of DSSCs, PCE has been
16 Sm /Y / TiO2⁠
3
⁠ + 3
⁠ + 4.09 Qin et al. (2017) achieved more than 12%. Thus, Pt is considered as a preferred cata-
17 Ho3+ ⁠ -Yb3 ⁠ +-F−⁠ tri-doped TiO
2 ⁠ 7.18 Song et al. (2017) lyst for efficient DSSCs due to its high catalytic activity and electrical
18 Er3⁠ +-Yb3⁠ +/TiO2⁠ 7.08 Yu et al. (2013)
19 NaYF4:Yb3⁠ +, Er3⁠ +/ TiO2⁠ 6.71 Zhu et al. (2015)
conductivity (Kakiage et al., 2014; Yella et al., 2011). In addition to
20 NaYF4:Yb3⁠ +, Er3⁠ +/ TiO2⁠ 4.32 Zhang et al. (2013) merits, Pt also has some disadvantages e.g. high cost (more expansive
21 1 mol% Sb-doped TiO2⁠ 8.13 M. Wang et al. (2012) than gold), low abundance, and poor corrosion resistance against iodine
22 3% Ni doped TiO2⁠ 4.00 Sakthivel et al. (2018) based charge transport mediator. It reacts with iodine and forms unsta-

D
23 Ni-doped TiO2⁠ 6.84 C.-S. Chou et al.
ble products like PtI4⁠ or H2⁠ PtI6⁠ . These product degrade the catalytic ac-
(2014)
24 N-doped TiO2⁠ 6.50 Cahyorini et al. (2011) tivity of Pt (Calogero et al., 2011; Olsen et al., 2000).
25 N,S-TiO2⁠ @Ag 8.22 Lim et al. (2015a) These demerits encourage the researchers to develop new CE ma-
26 N, La Co-Doped TiO2⁠ 5.33 Jiang et al. (2016) terials for DSSCs. Many alternative materials for the CE like Pt alloys,
TE
27 N-doped TiO2⁠ multilayer 8.00 Dissanayake et al. carbon materials, conducting polymers, and transition metals have been
photoelectrode (2017)
utilized as catalysts for CE. Here, we will briefly discuss the characteris-
28 Nanocrystalline nitrogen-doped TiO2⁠ 8.00 Ma et al. (2005)
29 S-Doped TiO2⁠ nanoparticles 6.91 Mahmoud et al. tics of each material.
(2018)
30 0.5 mol.% Mg and La co-doped TiO2⁠ 8.04 Wang et al. (2015) 4.2. Platinum alloys
31 F-doped TiO2⁠ 8.07 S. Yang et al. (2013)
EC

There are two objectives to make Pt alloys for CE of DSSCs. One is

cal conductivity and stability as compared to other materials (Thomas et
al., 2014). But it is an expensive material and also shows weak corrosion
resistance against iodine based electrolyte. Therefore, other alternative
materials like carbon allotropes (activated carbon, CNTs and graphene),
conducting polymers (CP), and transition metals have also been inves-
RR
to reduce the amount of Pt, which ultimately reduces the overall cost
of DSSCs. The other objective of making Pt alloys is to enhance the
catalytic activity and corrosion resistance of CE materials. Many Pt al-
loys have been synthesized and utilized as counter-electrode materials
in DSSCs. These alloys gave the promising photovoltaic performance.

tigated and introduced to substitute Pt. In this section, we will briefly Different Pt alloys and PCE of DSSCs have been summarized in Table 5.
discuss different CEs materials.
4.3. Carbon
4.1. Platinum
The development of low-cost catalyst material is an extremely im-
Platinum (Pt) is frequently used catalyst material for the CE of portant for the commercialization of DSSCs. Along with low cost, cat-
alyst material should exhibit good catalytic properties and high corro-
CO

DSSCs. It is normally sputtered on conductive glass substrate. Its thick-

ness is normally in the range of about 0.2–2 μm (Wu et al., 2017a). The sion chemical resistance. Carbon could be the first choice to replace
Pt. It is abundantly available on the Earth's crust. Moreover, it pos-
effect of thickness of Pt film on substrates was investigated by Fang and
sesses all features that are mandatory for the catalyst material. For ex-
his co-workers (Fang et al., 2004). They found that the thickness of film
ample, it exhibits good catalytic activity, high conductivity, high surface
significantly influences the conductivity of CE. Within limit, the conduc-
area, porosity, and chemical resistance against electrolyte and dye solu-
tivity increases with thickness. However, the thickness of Pt film does
tion. Carbon allotropes like activated carbon, Carbon black, CNTs, and
not affect the interface resistance between CE and electrolyte. Instead
graphene have been used as catalyst materials in DSSCs (Murakami and
UN

of sputtering technique, electrochemical deposition, cyclic voltammetric

Grätzel, 2008). DSSCs based on carbon CE and their PCEs are listed in
deposition, thermal decomposition, and thermal vapor deposition can
Table 6.
also be used to deposit Pt on conductive substrate (P. Li et al., 2008;
Olsen et al., 2000; Zhou et al., 2008).
4.3.1. Carbon black (CB)
Dao et al. (Dao and Choi, 2013) used thermal decomposition method
Spherical carbon black nanoparticles (as shown in Fig. 15a) show an
to deposit Pt on FTO substrates. The platinum precursor material was
amorphous quasi-graphitic molecular structure. CB is a suitable material
decomposed on FTO substrate by controlling the thermal decomposi-
for a CE, owing to its high surface area, excellent electrical conductivity
tion rate. It was observed that the morphology, thickness, and catalytic
and the catalytic activity towards the reduction of
activity of Pt nanoparticles depend on the heating rate. They found
(redox species) (Wroblowa and Saunders, 1973). The catalytic
that the CE fabricated with the heating rate of 1.2 °C min−⁠ 1 showed
activity of carbon black materials depends on particle morphology,
the charge transfer resistance of 0.86 Ω cm−⁠ 1. The PCE of DSSC based
on this catalytic film showed the PCE of 9.30%. To better control

11
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

F
OO
PR
D
TE
Fig. 14. SEM micrographs of (a) nanocups of Pt, (b) Pt nanoflowers, (c) Pt Nanowires and (d) Pt nanofiber networks (Wu et al., 2017).

Table 5 als of PVDF in the CE film. However, when they heated the CB paste
PCE of DSSCs based on Pt alloys CEs.
at 450 °C, they got the efficiency of 8.35%, which was nearly equal to
Sr. No CEs PCE (%) Ref. Pt-based electrode (8.29%).
EC

The particle size of CB also plays a crucial role in the photovoltaic

1 Pt0⁠ .02Co
2 Pt3⁠ Ni
4 Pt0⁠ .06Ni0⁠ .94
5 PtFe
6 PtMo
7 PtMo0⁠ .05
RR
10.23 He et al. (2014) performance of DSSCs. This effect was investigated by Kim et al. (Kim
8.78 J. Wan et al. (2014) and Rhee, 2012). They varied the particle size of CB from 20 nm to
8.21 Peng et al. (2009)
90 nm. They observed that the catalytic activity of CE increases with the
7.30 Yang et al. (2016)
6.75 Tang et al. (2015) decrease of particle size. It is because the decrease in particle size in-
7.05 Cai et al. (2014) creases the surface area of the catalyst material. They achieved the PCE

8 PtCr0⁠ .05 6.88 Dao et al. (2015a) of 7.2% with FF of 0.656 by employing 20 nm CB nanoparticles and a
9 PtPd1⁠ .25 7.22 Vojislav R. Stamenkovic et al. (2007)
9 μm thick film of CB. This performance was similar to Pt-based CE (PCE
10 PtRu3 6.80 V. R. Stamenkovic et al. (2007)
11 PtAu 3.40 C. Wang et al. (2012) of 7.6% and FF of 0.658).
12 PtCoNi 8.71 Yang et al. (2016)
13 PtPdNi 8.28 Yang et al. (2016) 4.3.2. Carbon nanotubes (CNTs)
15 PtCuNi 9.66 Yang and Tang (2016)
The cylindrical structure of carbon nanotubes (CNTs) are shown in
Fig. 15b (MWCNTs). CNTs also belong to one-dimensional carbon fam-
CO

thickness of CE, preparation conditions, and particle size (Wu and Ma,
2014).
Moreover, Murakami and his coworkers (Murakami and Grätzel,
2008) found out that the thickness of carbon black plays a crucial role
in the photovoltaic performance of DSSCs. They found an increase in FF
from 46% to 72% with thickness (up to 10 μm) of carbon layer on con-
UN
ily. CNTs are classified into SWCNTs and MWCNTs having diameters of
0.8–2 nm and 5–20 nm, respectively. Similarly, the length of CNTs can
be varied from 100 nm to a few centimeters. The aspect ratio of CNTs
is approximately 132 000 000:1, which is appreciably higher than other
materials. Therefore, CNTs show outstanding strength and stiffness (X.
Wang et al., 2009). Furthermore, CNTs also show extraordinary ther-
mal, electrical and mechanical properties (J. Gong et al., 2012; Popov,

ductive glass substrates. They achieved the highest efficiency of 9.1%
for a 14.5 μm thick layer of carbon. They also observed that higher the
surface area of carbon black, lower will be the charge transfer resistance
(RC⁠ T).
The influence of the preparation conditions of CB on the photo-
voltaic performance of DSSC was investigated by Wu et al. (Wu et al.,
2016). The paste of CB was prepared by using poly(vinylidene fluoride)
(PVDF) as a binder material. They used doctor blade method to deposit
carbon black paste on conductive glass substrates. They heated the elec-
trode at 350 °C and then employed in DSSCs. The performance of fab-
ricated DSSCs was found to be poor owing to the presence of residu
2004). These characteristics make CNTs as an ideal material for nan-
otechnology, optics, and photovoltaic applications. However, the cat-
alytic activity and ultimate efficiency of DSSCs depends on the length,
diameter and structure of CNTs (MWCNTs or SWCNTs).
SWCNTs as a CE material were used by Suzuki et al. (Suzuki et al.,
2003). They attained overall efficiency of 4.6% comparable to that of
Pt based DSSCs prepared under the same environment. In this study,
they deposited Pt on conductive substrate by sputtering technique. CNT
fibers of different diameters were prepared by Peng et al. (Pan et al.,
2013). They applied them as catalyst materials for the CE of DSSCs.

12
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

Table 6 Table 6 (Continued)

Power conversion efficiency of DSSCs based on carbon allotropes CEs.
Counter Electrode Electrolyte PCE/% Ref
Counter Electrode Electrolyte PCE/% Ref
Reduced graphene oxide Co3⁠ +/2+ 8.94 Ju et al.
Carbon nanofiber 7.00 Veerappan (rGO) (2014)
et al. Graphene nanosheet 6.93 S.-Y. Jang
(2011) (400 °C, 4 h) et al.

F
Carbon black + graphite 6.67 Kay and (2012)
Grätzel Reduced graphene oxide/ 3.43 Li et al.
(1996) TaON (2013)

OO
Carbon black + PEDOT 7.60 Zhang et Graphene oxide (GO) 4.48 Dao et al.
al. (2014)
(2012a) RuO2⁠ /(rGO) 8.32 Dao et al.
Hollow active carbon 7.21 Park et al. (2015b)
nanofiber (2013)
Carbon black 9.10 Murakami
et al. They found that the CNT fiber of 60 μm exhibited the outstanding
(2006)
catalytic activity. The DSSCs fabricated with CNT fiber of 60 μm and
Carbon black 8.35 Wu et al.
Thiolate/ Disulfide (T−⁠ /T2⁠ ) electrolyte gave the PCE of 7.33%, much

PR
(2016)
Carbon black 7.20 Kim and higher than that of Pt-based solar cell (2.06%). They also fabricated the
Rhee DSSC using I−⁠ /I3⁠ −⁠ charge transport mediator with 60 μm CNT fibers and
(2012)
achieved PCE of 5.97%. The core-shell of CNT–PEDOT was synthesized
Carbon black Co3⁠ +/2+ 8.81 I.-P. Liu et
al. (2017) by Shin et al.(Shin et al., 2011). They used emulsion polymerization
MWCNTs encapsulating 7.43 Zheng et technique to synthesize core-shell structure of CNT–PEDOT. This ma-
nickel compounds on Ni al. (2018) terial showed high conductivity as well as good catalytic activity. The
foils
ZnO/ MWCNTs 1-Hexyl-3-methyl- 7.07 Chew et
DSSC based on this novel material showed the PCE of 4.62%. Verti-

D
imidazolium iodide ionic al. (2018) cally aligned SWCNTs were prepared by Lin et al. (Hao et al., 2012).
liquid They directly synthesized SWCNTs on FTO substrate by contact transfer
Spray Coated CNTs 1.98 Widodo et methods. This substrate was then employed as a CE of DSSCs and gave
al. (2015)
the PCE of 5.25%. Nam et al. (2010) screen-printed randomly dispersed
TE
Cu2⁠ ZnSnS4⁠ /CNT composites – 6.30 Nemala et
al. (2016) MWCNT on FTO glass substrate. They employed it as a CE of DSSCs
CNTs/Pt – 8.21 Dao and and found PCE of 8.03%. In another method, CNTs have been vertically
Choi grown on the conductive glass substrate. The fabricated CE was utilized
(2018) in DSSC with PCE of 10.04% (Nam et al., 2010).
MWCNTs 7.67 Lee et al.
(2009)
4.3.3. Graphene (GR) sheets
EC

SWCNTs 7.81 Mei et al.

(2010) Fig. 15c shows the 2D-structure of the graphene sheet. It consists of
MWCNTs – 4.69 Luo et al. a monolayer of carbon atoms. The closely packed carbon atoms consti-
(2017)
tute a honeycomb-like structure. Each atom in this structure is sp2⁠ hy-
3D-SWCNTs 8.31 Ma et al.
(2014) bridized and bond length between two adjacent carbon atoms (C C) is
Graphene nanoplatelets 5.73 Kavan et 1.42 Å (Banks et al., 2005). Owing to these structural features, graphene
(NPs) al. possesses some unique characteristics such as high carrier mobility (∼10
RR

(2011a)
000 cm2⁠ V−⁠ 1 s−⁠ 1) (Chen et al., 2008; Du et al., 2008), high specific sur-
Graphene NPs Co3⁠ +/2+ 9.40 Kavan et
al. face area (2630 m2⁠ g−⁠ 1) (McAllister et al., 2007; Peigney et al., 2001),
(2011c) good thermal conductivity (∼3000 W m−⁠ 1 K−⁠ 1) (Stankovich et al., 2006),
Graphene NPs Co3⁠ +/2+ 9.30 Kavan et and high optical transparency (97.7%) (Bunch et al., 2007). Besides, it
al.
also shows outstanding catalytic activity and can be further enhanced
(2011b)
Nitrogen-doped NPs Co3⁠ +/2+ 9.04 Ju et al.
by oxidation. Similarly, the structural defects in the graphene also influ-
CO

(2013) ence the catalytic activity (Low and Lai, 2018; Lu et al., 2015).
Honeycomb-structured 7.80 Hui Wang Roy-Mayhew et al. (2010) observed that the C/O ratio in graphene
graphene et al. oxide significantly affects the catalytic activity of the material. At the
(2013)
ratio of 13, they found the highest catalytic activity. The graphene ox-
Graphene nano-foam (CVD 5.20 J.-S. Lee
grown) et al. ide with C/O ratio of 13 was then utilized as a CE material of DSSCs.
(2012) They obtained the PCE of 5.0%, which was very close to Pt-based
Reduced graphene oxide 3.60 H.-S. Jang DSSC. Kavan et al. (2011c) fabricated an optically transparent cath-
UN

(rGO) et al.
ode for DSSCs using graphene nanoplatelets and found PCE of 5% and
(2012)
Graphene quantum dots 2.15 Wei et al.
FF of 0.52 compared to a PCE of 6.89% and FF of 0.74 for the refer-
(2014) ence Pt electrode. The film of graphene nanoplatelets (GNPs) showed
Nitrogen-doped graphene 4.20 Xue et al. 85% transparency. Kavan et al. (2011b) used GNP film on FTO as
film (2012) a cathode with Co2⁠ +⁠/3⁠ +(L)2⁠ redox couple (where L is 6-(1H-pyra-
Sulfur-doped rGO Co3⁠ +/2+ 4.23 Luo et al.
zol-1-yl)-2,2−⁠ -bipyridine) and Y1⁠ 23-sensitized TiO2⁠ photoanode. They
(2014)
CVD-3D graphene network 8.45 Ahn et al. found the overall efficiency of 8%. G. Wang et al. (2012) employed
(2014) in-situ polymerization technique to synthesize nanocomposites of PANi
Hydrogen-graphene Co3⁠ +/2+ 5.96 Jeon et al. and 2D-graphene. The DSSCs fabricated by employing graphene–PANI
nanoplatelets (2015)
nanocomposite as a CE showed the PCE of 6.09%, which was closed to
Fluorinated graphene 2.56 Das et al.
(2011)

13
N.A. Karim et al. Solar Energy xxx (xxxx) xxx-xxx

F
OO
PR
D
TE
Fig. 15. SEM images of (a) spherical carbon black nano-particles (Murakami and Grätzel, 2008), (b) MWCNTs (Shokrieh et al., 2013), and Graphene mono layer (Graphene Supermarket
:: 2. Research Materials :: 5. Chemical Vapor Deposition (CVD) Graphene :: CVD Graphene on Metals :: CVD Graphene on Copper Foil :: 4" Monolayer Graphene on Circular Cu foil,
EC

n.d.).

Pt based device (6.88%). Lee et al. (K.S. Lee et al., 2012) prepared PE-
DOT–graphene composite material for photoanode of DSSCs and found
the PCE of 6.26%. Dou et al. (Dou et al., 2012) used hydrothermal
method to synthesize Ni1⁠ 2P5⁠ –graphene composite for the CE of DSSCs.
Ni1⁠ 2P5⁠ –graphene composite shows an outstanding catalytic activity to-
RR
4.4. Conductive polymers
Various kinds of conducting polymers can work as CEs in DSSCs.
With the development of nanomaterial, the nanostructure has been
introduced into previously mentioned polymers. These polymers are

wards the reduction of redox species and gives the PCE of 5.7%. The
metal-graphene composites not only increase the catalytic activity and
conductivity but also minimize the charge transport resistance at the
CE/electrolyte interface. The insertion of metals on graphene sheets pro-
duces active sites, which ultimately enhance the catalytic activity of
graphene. Moreover, the inclusion of metal also acts as a spacer be-
CO
readily deposited by either chemical or electrochemical polymerization
process. And they are readily modified into aligned nanostructure that
might enhance charge transport and surface area simultaneously. Fur-
thermore, by the inclusion of a second component, high-performance
polymer composite can be easily obtained, such as, carbon nanotube ad-
ditive. polyaniline (PANI), Poly(3,4- ethylenedioxythiophene) (PEDOT),

tween thin layers of graphene. The spacer promotes the fast diffusion
of electrolyte by creating an electrode–electrolyte contact (Wang and
Hu, 2012). Owing to the outstanding catalytic activity of carbon/car-
bon nanocomposites, Choi et al. (H. Kim et al., 2012) synthesized MW-
CNTs–graphene for a CE of DSSCs. They used chemical vapour deposi-
tion (CVD) technique to deposit MWCNTs on the top of graphene layer.
The device based on MWCNTs–graphene CE showed the PCE of 3%
UN
and polypyrrole (PPy) are the most investigated polymer materials (H.
Sun et al., 2015).
4.4.1. Polythiophene
A soft-template method was used to synthesize nanofibers of PEDOT
with diameters of 10–50 nm. A high electrical conductivity up to 83 S
cm−⁠ 1 was obtained. Using nanofibers as a CE in DSSCs gave the PCE

of 9.2% (T.H. Lee et al., 2012). It was much higher than its bulk PE-
with open circuit voltage of 0.76 V and short circuit current density of
DOT counterpart (6.8%) and Pt-based DSSCs (8.6%) (T.H. Lee et al.,
5.6 mA cm−⁠ 2. This performance was superior to that of MWCNTs CE.
2012). Ahmad et al. (Ahmad et al., 2010) used electro-oxidative poly-
Mehmood et al. (Mehmood et al., 2016) used carbon/carbon composite
merization technique to prepare PEDOT porous layer on conductive
of activated carbon, MWCNTs and graphene as CEs and found the over-
FTO substrate. The polymerization was carried out in the hydropho-
all efficiency of 10.73%. TEM image of carbon/carbon composite of ac-
bic ionic liquid medium. PEDOT prepared using this method showed
tivated carbon, MWCNTs and graphene composites and corresponding
the conductivity of 195 S cm−⁠ 1. The DSSCs fabricated using this con-
current–voltage characteristics of DSSCs are shown in Fig. 16a and 16b,
ductive film showed the PCE of 7.93% comparable to that of Pt-based
respectively.
DSSCs (8.71%). The electrodeposition technique was used by Pringle et
al. (Pringle et al., 2010) to prepare PEDOT films on ITO based flexible

14
N.A. Karim et al.
Fig. 16. (a) TEM image of carbon/carbon composite of activated carbon, MWCNTs and graphene composites and (b) corresponding current-voltage characteristics of DSSCs (Mehmood et
al., 2016).
substrate of Polyethylene naphthalate terephthalate. Highly transpar-
D
ent film of PEDOT was obtained by just dipping a substrate for five
minutes. The higher PCE of 8.0% was obtained by using this transpar-
ent film as a CE in DSSCs. Zhang et al. (Yan and Zhang, 2013) mod-
ified the poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PE-
TE
DOT:PSS) film using PEG and acetylene black (AB). PEG acts as a binder
and improves the overall conductivity of the system. It also enhances
the catalytic activity of PEDOT:PSS film towards the reduction of tri-
iodide ions. The addition of acetylene black (AB) further improves the
catalytic activity. DSSCs fabricated using modified PEDOT:PSS film as a
CE showed the PCE of 4.39% comparable to Pt-based DSSCs (4.50%).
EC
Trevisan et al. (Trevisan et al., 2011) carried out electropolymerization
of EDOT to form PEDOT-nanotubes (NTs) using ZnO nanowires as a
template. The catalytic activity of PEDOT-NT CEs was found to be bet-
ter than that of flat structure. The DSSCs fabricated with PEDOT-NT
CE showed the higher efficiency of 8.3%, slightly lower than Pt based
cell (8.5%). Similarly; T.H. Lee et al. (2012) spin-coated PEDOT-NFs as
RR
a methanol-based colloidal dispersion. Thin film of PEDOT-NF as a CE
showed low surface resistance and high porosity. Thus, the fabricated
DSSCs based on PEDOT-NF as a CE exhibited the PCE of 9.2%. This
performance was superior to that of bulk PEDOT based DSSCs (6.8%).
Poly(3,4-propylenedioxythiophene) (PProDOT) can also replace Pt. It
possesses high surface area and avoids the formation of any passive
CO
layer at the interface of electrolyte and CE. DSSCs fabricated with this
material by using I2⁠ based and Cobalt based electrolyte give the PCE
of 9.25% and 10.08%, respectively (Wu et al., 2017). Besides, the flex-
ible DSSCs can be facilitated by depositing a thin film of PProDOT on
flexible substrates. Moreover, pristine Polythiophene has also been em-
ployed as CE of DSSCs; but DSSC with Pth as a CE showed very low
PCE. However, Pth/Graphene composite as a CE showed promising re-
UN
sults (Bora et al., 2015).
4.4.2. Polyaniline (PANI)
PANi can be prepared by the addition polymerization of aniline
monomer. It possesses high electrical conductivity, good chemical sta-
bility, and redox properties. Therefore, it is one of the most widely
used CE materials (Kang et al., 1998). Nanoparticles (NPs) of PANi
with diameter of 100 nm were prepared by Wu and his co-workers (Q.
Li et al., 2008) through an aqueous oxidative polymerization reaction.
They found that the PANi based DSSCs exhibited PCE of 7.15%, which
was slightly higher than the Pt-based DSSCs. They used redox
15
Solar Energy xxx (xxxx) xxx-xxx
F
OO
PR
couple in their work. The electrocatalytic performance of PANi was fur-
ther improved by synthesizing an oriented PANI nanowire array via
in-situ polymerization (Hong Wang et al., 2013b). By applying oriented
PANI nanowire arrays as a CE material, DSSCs achieved a higher effi-
ciency of 8.24%. This PCE was much higher than the bulk PANi-based
DSSC (5.97%) and Pt based DSSC (6.78%). PANI nanoribbons were syn-
thesized by Hou et al. (Hou et al., 2016) for the CE of DSSCs. They
achieved a comparable efficiency of 7.23% with Pt based DSSC (7.42%).
Transparent thin film of PANi as a CE has been prepared by Tai et al.
(Tai et al., 2011) for the application of DSSCs. A bifacial DSSCs was pre-
pared by employing this transparent PANi film. Upon sunlight irradia-
tion from front and rear sides, the DSSCs showed the PCE of 6.54 and
4.26%, from the front and the rear side, respectively. Similarly, bifa-
cial DSSCs has been fabricated by Wu and his co-workers using trans-
parent PANI CE (Wu et al., 2014). It has been observed that more dye
molecules can be excited by simultaneous sunlight irradiation from both
sides. Higher the excitations more will be the current density. The bifa-
cial DSSCs with transparent PANi CE attained the overall efficiency of
8.35%, which was about 24.6% higher than the DSSC irradiated from
the front only.
Adding the second phase to PANi matrix is another way to improve
the catalytic properties of PANi. Nanocomposite of PANi/graphene were
prepared by L. Wan et al. (2014) via in situ polymerization. They
achieved the PCE of 4.46% by using nanocomposites (NCs) as CE ma-
terials, which was comparable to 5.71% for the Pt-based DSSCs. Wang
and his co-workers (G. Wang et al., 2012) also used PANi/ graphene
NCs as CE of DSSCs and got the PCE of 6.09%, which was comparable
to 6.88% of the cell with Pt CE. X. Chen et al. (2018) prepared ternary
NCs consisting of nickel NPs, PANI, and graphene (Ni–PANI–GR com-
posites) and used as a catalyst for the CE to replace the Pt in DSSCs. The
DSSCs fabricated using Ni–PANI–GR NCs as a catalyst exhibits an over-
all PCE of 5.80% higher than the Pt-based DSSCs (5.30%). Gao et al. (Q.
Li et al., 2008) synthesized Poly (vinyl pyrrolidone) (PVP)/polyaniline
(PANI) nanocomposites and applied them as transparent CE for bifacial
quasi-solid-state DSSCs. The bifacial DSSCs with PVP/PANI CE showed
an overall PCE of 5.81% under illumination from the front side, which
was superior to Pt based DSSC (5.70%).
4.4.3. Polypyrrole (PPy)
Polypyrrole (PPy) is prepared by the addition polymerization of
pyrrole (Py). High polymerization yield, good catalytic activity, and
N.A. Karim et al.
high conductivity make it a strong candidate for the CE of DSSCs
(Hwang et al., 2014; Wu et al., 2008). Electro-polymerization and
vapor-phase polymerization methods have been used by Xia et al.
(Murakami and Grätzel, 2008) to deposit PPy thin film on conductive
glass substrates. The DSSCs fabricated using these CEs showed the PCE
of 3.2% and 3.4%, respectively. Both were lower than the Pt-based
DSSCs (4.4%). Spherical NPs of PPy with the diameter of 85 nm have
been prepared by Im et al. (Jeon et al., 2011) for the application of CE
of DSSCs. They further improved the conductivity of PPy NPs by treat-
ing with HCl. They employed the treated PPy as a CE of DSSCs and at-
tained the efficiency of 7.73% slightly lower than the Pt -based DSSCs
(8.20%). Similarly, the discrete spherical NPs of PPy with particle size
of ∼85 nm and electrical conductivity of ∼10 S cm−⁠ 1 were prepared by
Jeon et al. (Jeon et al., 2011) through chemical oxidative polymeriza-
tion technique. They also treated the synthesized NPs with HCl. The
treated PPy NPs CE showed the higher efficiency of 6.83% as compared
to non-treated PPy NPs CE (5.28%). Bu and his co-workers (Bu et al.,
2013) developed a novel transparent and stable PPy counter electrode
for DSSCs. Upon illumination from front and rear-side, DSSCs based on
this type of CE showed the PCEs of 5.74% and 3.06%, respectively. Lim
et al. (Lim et al., 2015b) fabricated nanocomposites of polypyrrole/re-
duced graphene oxide for CE of DSSCs. The PCE of DSSCs based on this
type of CE was 2.21%, slightly higher than the Pt based DSSCs (2.19%).
Conductive polymers have many advantages such as light weight,
D
easy processing, flexible for mass production, good conductivity and cat-
alytic activity. Moreover, their electronic properties can be tuned eas-
ily through doping or varying synthesis conditions. However, polymer
degradation and low chemical stability against charge transport media-
TE
tor are still major challenges. Thus, there is a need of further research
and development in this area.
4.5. Transition metal compounds
Transition metals possess excellent catalytic activity. It can be at-
EC
tributed to their ability of electron donating or electron withdrawing
from other substances, depending on the reaction nature. They form
complexes with other reagent and then act as catalysts. Transition met-
als in complexes supply electrons and become oxidized or become re-
duced when loan electrons from other reagents. The catalytic proper-
ties of transition metal complexes also depend on their adsorption or
RR
absorption characteristics. Transition metals and their complexes have
been used as catalyst materials in DSSCs to replace expensive Pt mate-
rial (Jiang et al., 2009; M. Wang et al., 2009). In this section, we will
briefly review the catalytic performance of transition metal compounds
and their applications for the CEs of DSSCs. Major transition metal com-
pounds include sulfides, nitrides, oxides, carbides, and nitrides.
Carbide compounds, for example, Cr3⁠ C2⁠ , MoC, TiC, Ta4⁠ C3⁠ , VC and
CO
WC are considered as attractive CE materials because of their good cat-
alytic activity, high selectivity, good conductivity and, superior stabil-
ity against electrolytes. DSSCs based on Mo2⁠ C, ZrC, NbC, Cr3⁠ C2⁠ , TiC,
and VC CEs showed PCEs of 5.83%, 3.85%, 2.46%, 5.79%, 6.52% and
6.38%, respectively. Similarly, WC and W2⁠ C were also used in DSSCs
and showed the overall PCE of 6.68% and 6.23% respectively (Gao et
al., 2018; Wu et al., 2013). Moreover, Lee et al. (Jang et al., 2010)
UN
achieved an overall PCE of 7.01% by employing WC as a CE in DSSC.
However, they found that the catalytic activity of WC is still lower than
Pt (8.23%). Commercially available WC and Mo2⁠ C have also been used
by Lee et al as CE of DSSCs. They achieved the power-conversion-effi-
ciency of 5.35% and 5.70%, much lower than Pt-based DSSC (7.89%)
(Wu et al., 2011a).
Thus, carbides have a greater tendency to replace the expensive plat-
inum material. However, the propensity of carbides to form particle
agglomeration during synthesis process and high energy consumption
16
Solar Energy xxx (xxxx) xxx-xxx
limit their applications for the counter electrode of DSSCs (Wu et al.,
2011a).
Similar to carbides, the nitrides were also employed as catalysts to
the CE of DSSCs. Ti sheet decorated with TiN nanotube arrays were
prepared by Gao group by using anodization and nitridation processes
(Jiang et al., 2009). The DSSCs fabricated using such a CE material
F
gave the PCE of 7.37%, which was slightly lower than the Pt-based de-
vices (7.45%). A surface-nitride Ni foil for the CE material of DSSCs
was prepared by Gao et al. (Jiang et al., 2010). The cell based on this
OO
material showed the PCE of 5.68%, lower than that of conventional
DSSC (8.41%). The main reason for the low PCE could be accredited to
the lower surface area of compact nitride CE film (Jiang et al., 2010).
Nanoparticles of metal nitrides like ZrN, NbN, VN, TiN and CrN were
prepared by Wu et al. (Wu et al., 2012) using urea-metal path. They
utilized them as catalyst materials for the CE of DSSCs and found the
PCE of 3.68% (ZrN), 1.20% (NbN), 5.92% (VN), 6.23% (TiN) and 5.44%
(CrN), respectively. Flexible Mo2⁠ N and W2⁠ N thin films on a Ti sheet
PR
were prepared by the same group and found the PCE values of 6.38%
(W2⁠ N) and 5.81% (Mo2⁠ N). They used the sputtering method to deposit
these materials on Ti sheet. However, their efficiency was still lower
than the conventional Pt-based DSSCs (7.01%) (Wu and Ma, 2014).
Instead of carbides and nitrides based catalysts, oxide materials also
have a tendency to replace Pt catalyst in DSSCs. Nanorods of WO2⁠ and
blocks of WO3⁠ were prepared by Ma and his team (Wu et al., 2011b)
for CEs of DSSCs. The devices based on these catalysts show the PCE of
7.25% and 4.67%, respectively. In addition, the same group prepared
WO2⁠ .72 catalyst for the CE and attained the PCE of 8.03%, slightly lower
than the conventional DSSC (8.08%) (Zhou et al., 2013). Similarly, the
other oxides like TaOx⁠ , V2⁠ O3⁠ , Nb2⁠ O5⁠ , also showed the good PCE values
of 6.79%, 5.40, and 4.84%, respectively (Wu et al., 2012; Yun et al.,
2013). Three allotropic forms of Nb2⁠ O5⁠ e.g. monoclinic (M Nb2⁠ O5⁠ ),
orthorhombic (O Nb2⁠ O5⁠ ), and hexagonal (H Nb2⁠ O5⁠ ) were synthe-
sized to examine the effect of size of crystal on the catalytic activity of
CEs (Lin et al., 2011). DSSCs based on these allotropic forms of Nb2⁠ O5⁠
showed the PCE of 5.82%, 4.55%, and 5.68%, respectively (Lin et al.,
2011). V2⁠ O5⁠ as a thin film CE of DSSCs was employed by Xia et al.
(Xia et al., 2010). They obtained the PCE of 2.0%, which was closed to
the Ag based CE DSSCs. Similarly the nanocrystals of RuO2⁠ were pre-
pared by Wang et al. (Hou et al., 2014) via hydrothermal process. These
nanocrystals showed the promising behavior as a CE and showed the
PCE of 7.22%, which was greater than the conventional Pt based DSSCs
(7.17%). Lin et al. attained the overall efficiency 7.88% by applying
NbO2⁠ catalyst for triiodide reduction. This performance was comparable
with Pt based device (7.65%) (Lin et al., 2011). Hierarchical structures
of Fe3⁠ O4⁠ was synthesized by Wang group (L. Wang et al., 2014). They
employed them as CEs of DSSCs and found the PCE of 7.65%. This pho-
tovoltaic performance was superior to that of pyrolytic Pt based DSSCs
(6.88%).
Semitransparent thin film of CoS was prepared by Grätzel et al. (M.
Wang et al., 2009) on ITO/PEN substrate. DSSCs based on this type of
CE showed the PCE of 6.5%, which was equal to device with Pt as a CE
material. Cost effective nanocrystals of Co9⁠ S8⁠ were prepared by Tuan et
al. (Chang et al., 2013) for large area DSSCs. The device having an ac-
tive area of 2 cm2⁠ and Co9⁠ S8⁠ as a CE showed the overall PCE of 7.0%.
This PCE was slightly lower than Pt based DSSCs. Qian group (He et
al., 2015) prepared Ag2⁠ S nanoparticle as CE catalyst for DSSCs. DSSCs
with Ag2⁠ S CE showed the higher efficiency of 8.40%, and it was sur-
prisingly higher than Pt based device (8.11%). They also found that the
thickness of catalyst material affects the reduction reaction at CE. The
optimum thickness of CE for this performance was 0.53 μm. Pan group
(X. Zhang et al., 2016) prepared a flexible CE by depositing a thin film
of CuS on Polyethylene terephthalate (PET). A solar cell based on such
a flexible CE gave the PCE of 6.38%, superior to that of conventional
N.A. Karim et al.
DSSC. The mechanical stability of PET substrate was assessed by bend-
ing test. Only 10% decrease in efficiency was observed after each 100
cycles of stress and strain. It illustrates a good mechanical strength of
PET substrate. P. Sun et al. (2015) employed a hydrothermal procedure
to deposit a thin film of Sb2⁠ S3⁠ on conductive glass substrates. They used
them as a CE of cell and attained an efficiency of 5.37%, which was
equivalent to Pt based device (5.36%). Nanofibers of VS2⁠ as a catalyst
material for the CE of DSSCs were utilized by Zheng and co-workers (X.
Liu et al., 2017). They attained the overall PCE of 6.24%, which was
closed to the DSSCs with Pt as a catalyst material for CE (6.44%). Simi-
larly, the PCE values of 7.01%, 6.50% and 3.79% were obtained by us-
ing Ni3⁠ S2⁠ , Co8⁠ .4⁠ S8⁠ , and Cu1⁠ .8S, respectively (Mulmudi et al., 2011). Chen
et al. (Y.-C. Wang et al., 2013) deposited a semitransparent film of FeS2⁠
on flexible conductive substrate (ITO/PEN). DSSCs using this film as a
CE showed the PCE of 7.31%.
Metal selenides (M Se, M = Ru, Co, Cu, Ni, Co) as CEs of bifa-
cial DSSCs were extensively used by Tang group (Duan et al., 2014). M
Se based CEs e.g. Ru0⁠ .3⁠ 3Se, Cu0⁠ .50Se, Ni0⁠ .8⁠ 5Se, and Co0⁠ .8⁠ 5Se showed
the front and rear efficiencies of 9.22% and 5.90%, 6.43% and 4.24%,
7.85% and 4.37%, 8.30% and 4.63%, respectively. However, Pt based
DSSCs showed front and rear PCEs of 6.18% and 3.56%, respectively.
Thus, many M Se as catalysts of CEs show higher PCE as compared
to Pt based cells (Duan et al., 2014; Wu et al., 2017). The reasons of
higher PCE can be attributed to their high transparency, good catalytic
D
activity and low charge transfer resistance at the interface CE and elec-
trolyte. Wang group (F. Gong et al., 2012) synthesized nickel selenide
(Ni0⁠ .85Se) and cobalt selenide (Co0⁠ .85Se) for CEs of DSSCs. These mate-
rials showed outstanding catalytic activity and devices based on such
TE
materials gave the PCE of 8.32% and 9.40%, respectively. Tang (Li and
Tang, 2016) used mild solution method to synthesize CuSe catalyst ma-
terial for the CE of DSSCs. It was found that the catalytic activity of CuSe
could be changed by changing the pH of solution. At pH of 11, they at-
tained the highest PCE of 6.25%. Dai et al. (W. Wang et al., 2014) found
that the morphology of catalyst materials significantly affects their cat-
EC
alytic performance. They prepared two different structures of FeS2⁠ cata-
lyst including microrods and spherical particles for the CE of DSSC. The
devices assembled by using these structures showed the PCE of 8% and
7.38% respectively. The obtained PCE was comparable with Pt based
device (7.87%). A higher PCE of 10.19% was achieved by Jia et al. (Jia
et al., 2015). They used Ni0⁠ .8⁠ 5Se as a catalyst material for the CE of
RR
DSSCs.
5. Conclusion and future directions
The estimated manufacturing cost of this type of photovoltaic (PV)
technology is equivalent to other thin film PV technologies; conse-
quently, DSSCs are near to commercialization. According to the Grand
CO
View Research report, the estimated market share of DSSCs technology
was 49.6 million US Dollars in 2014. It is expected to grow annually
at a growth rate of 12% from 2015 to 2022 (Shakeel Ahmad et al.,
2017). Distribution of DSSC technology in different areas and its esti-
mated growth rate are shown in Fig. 17.
Furthermore, the fabrication of DSSCs is solution-based and do not
require intensive energy inputs. On the other hand, silicon-based solar
UN
cells need high purity of silicon and intensive heat treatment process to
fabricate the device. For that reason, the mass production of 1 m2⁠ mod-
ule of DSSCs require less energy (less energy payback time) compared
to silicon solar cell. In addition, the emission of harmful or toxic gasses
during the production process of DSSCs is very small compared to Si so-
lar cells (Ramasamy et al., 2008). The less cost together with environ-
ment-friendly materials, DSSCs propose a feasible approach to confront
the growing energy demand of mankind.
However, to make this technology more viable, it is crucial to fur-
ther improve the efficiency and outdoor/indoor stability of DSSCs.
17
Solar Energy xxx (xxxx) xxx-xxx
F
OO
Fig. 17. Distribution of DSSCs technology in different areas and Estimated growth rate
(“Global E-Paper Display Market Worth USD 28.87 Billion by 2022,” n.d.; Shakeel Ahmad
et al., 2017).
PR
There is also a need to further reduce the manufacturing and material
cost of DSSCs. In the present work, we briefly reviewed materials avail-
able for PE and counter electrodes CE of DSSCs. It can be said with no
hesitation that the PCE, stability and the economics of devices strongly
depend on PE and CE materials.
The massive research has been conducted to modify the PE and CE
of DSSCs, which ultimately improve the PCE of DSSCs. Following steps
can be taken to further improve the photovoltaic performance of DSSC.
I. Fundamental research is needed to disclose the charge transport
mechanisms in DSSCs, which predominantly occur at the interface
of PE and electrolyte, where the foremost light to electricity conver-
sion occurs.
II. Recombination is the main lose path in DSSCs, which significantly
reduces the PCE of DSSCs. It can be reduced by nanocomposites of
TiO2⁠ with carbon allotropes. These composites not only reduce the
recombination but also improve the conductivity of PE.
III. Low light harvesting of PE reduces the current density of devices,
which ultimately reduces the overall PCE of DSSCs. It can be im-
proved by doping of different metals on TiO2⁠ PE. Carbon allotropes
also improve the light harvesting efficiency of PE.
IV. Inefficient light scattering inside the PE is the major cause of poor
optical properties. The light harvesting efficiency of PE is restricted
by the weak light scattering ability of TiO2⁠ NPs. Light scattering can
be improved either by doping or using different morphologies of
TiO2⁠ (nanowires or nanotubes of TiO2⁠ ). It reflects the incident solar
radiation, directing to enhance the distance travel by incident light
in the PE.
V. At present, the major focus of DSSCs is to decrease the cost and
to increase the PCE. For the counter electrode part, platinum gives
the best performance, but it is also expensive and its rarity limits
its practical application in DSSCs. We have seen a series of plat-
inum-free counter electrode materials in DSSCs such as carbon ma-
terials, conducting polymers, inorganic oxides and sulfides, transi-
tion-metal nitrides and carbides, and composite materials. Among
these materials, conducting polymers show promise as alternatives
to Pt-free CE in DSSCs.
VI. Catalytic activity of CE can further be improved by using compos-
ites of materials i.e. graphene/Pt, CNTs/P and PANi/graphene etc.
Acknowledgement
The authors acknowledge the support rendered by the Polymer and
Process Engineering department, UET Lahore.
N.A. Karim et al.
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