Solar Energy 233 (2022) 378–407

Contents lists available at ScienceDirect

Solar Energy
journal homepage: www.elsevier.com/locate/solener

Advancements, frontiers and analysis of metal oxide semiconductor, dye,

electrolyte and counter electrode of dye sensitized solar cell
Anupam Agrawal a, Shahbaz A. Siddiqui b, *, Amit Soni a, Ganesh D. Sharma c
a
Department of Electrical Engineering, Manipal University Jaipur, Jaipur 303007, Rajasthan, India
b
Department of Mechatronics Engineering, Manipal University Jaipur, Jaipur 303007, Rajasthan, India
c
Department of Physics, The LNM Institute of Information Technology, Jamdoli, Jaipur, Rajasthan 302031, India

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

Keywords: The Dye-sensitized solar cell (DSSC) is globally investigated technology due to their attractive characteristics
Photovoltaics such as low-cost, simple fabrication, flexible, transparent, variety of colour, sensitive to diffuse light and eco-
Dye sensitized solar cell friendly photovoltaic (PV) technology and have capabilities for commercial application. These characteristics
Photoanode
are particularly well suited for integrated PV in buildings and automotive, as well as indoor or portable light
Sensitizer
Electrolyte
applications. DSSC is a photo-electrochemical device comprises of a photo-anode consists of wide band metal
Counter electrode oxide semiconductor (MOS) layer sensitized with dye, counter electrode (CE) coated with platinum or other
material and an electrolyte which is sandwiched between the photo-anode and counter electrode. Therefore, to
enhance the DSSC’s performance, a comprehensive study to understand the fundamental and recent research
trends of MOS, dye, electrolyte, sealing material and CE employed in DSSC is necessary. This paper have pre­
sented the various design strategies, material employed and literature in the field of MOS, dye, electrolyte,
sealing material, and CE for DSSC. We illustrate the architecture, working mechanism, and brief explanation of
DSSC growth as well as necessary requirements for the DSSC components to provide a direction for the con­
struction of highly efficient DSSC. This paper also consolidated the introduction, benefits and classification of PV
technologies. We also give brief description of market growth of DSSC technology and future perspective for
efficient DSSC.

1. Introduction
One of the most amazing and life-changing innovation made by
humans is electricity generation. Electricity has many uses in our life for
example in domestic usage, commercial and industrial sectors,
communication and transportation sector, medical sectors, science and
technology centres etc. Therefore, life without electricity is unimagin­
able. The consumption of electricity varies from person to person and is
increasing day by day all over world. To meet the requirement, we have
to produce more electricity. With the prevailing situation in electricity
consumption, energy demand is expected to double and electricity will
be quadrupled (Lapillonne et al., 2007; I.E. Agency, 2013). The annual
electricity consumption data of different countries are shown in Fig. 1
and as provided by Enerdata (intelligence + consulting) company in
Global Energy Statistical Yearbook 2020 (Enerdata, 2020).
More than 80% generation of the electricity in the world is depen­
dent upon the coal (I.E. Agency, 2013). It is well proven that coal mining
has a detrimental effect on the atmosphere and the environment by (i)
discharging of several harmful gases such as CO, SO2, Hg, Se, As and dust
which reduces the air quality (ii) dispersing solid pollutants and heavy
metals, loss in water quality (iii) causing planet and green space
degradation (iv) displacement of inhabitants from their location because
of the earth’s hollowing (v) excavation degrading the soil (Khanna,
2013; Manju and Sagar, 2017). Therefore, the extraction and burning of
coal have polluted the atmosphere, reduced resources and seriously
harmed the ecosystem. It is very important to promote the production of
alternative energy resources, such as wind, solar, geothermal and tidal
energy, in order to cope with environmental issues and the need for
electricity generation. Fig. 2 displays the emission of CO2 scenario in
various countries around the globe (Enerdata, 2020). In 2019, CO2
emissions from fuel combustion decreased marginally (-0.2%) after two
years of development and a sharp decrease in CO2 emissions per kWh
generated (-3.2% or 443 g CO2/kWh) primarily due to the change in fuel
from coal to gas and renewable sources in the world power mix

* Corresponding author.
E-mail address: shahbazahmed.siddiqui@jaipur.manipal.edu (S.A. Siddiqui).

https://doi.org/10.1016/j.solener.2022.01.027
Received 26 October 2021; Received in revised form 4 January 2022; Accepted 12 January 2022
Available online 29 January 2022
0038-092X/© 2022 International Solar Energy Society. Published by Elsevier Ltd. All rights reserved.
A. Agrawal et al. Solar Energy 233 (2022) 378–407

(Enerdata, 2020). The initiation of renewable energies over the last ten systems. The market prospects of the DSSCs are significantly improved
years has generated considerable interest in understanding the eco­ while being incorporated into various products (Devadiga et al., 2021;
nomic feasibility of the new energy resource among academics, elected Yeoh and Chan, 2021).
officials and business leaders. The scenario of projected world total
electricity generation by various fuels and renewable fuels (from year
1.1. PV solar energy
2010 to 2050) given by US Energy Information Administration in their
International Energy Outlook 2019 report which is shown in Fig. 3 and
On a regular basis, we are receiving 1.7 × 105 TW amount of radi­
Fig. 4 respectively (U.S. Energy Information Administration, 2019). In
ation energy from the sun out of them only 600 TW (assumption) are
Fig. 3, most of the growth in electricity generation is fueled by renew­
nearly harvestable. If PV devices are just 10% effective then 60 TW of
ables and natural gas in year 2050. Wind and solar shares around 70% of
solar energy can be generated which is exceeding the demand forecasts
the overall generation of renewables sources by 2050 as shown in Fig. 4.
(Lau and Soroush, 2019). Though, there is a large difference in our
and interestingly solar energy dominates the overall renewable
present usage of solar energy and its immense capacity. Over the last few
generations.
decades, variety of innovative developments and ideas have been
PV technology is considered to be one of the most promising devel­
established and developed for solar energy harvesting such as thermo-
opment since it can convert sunlight energy into electrical energy
electric, photo-catalytic, PV, and photo-electrochemical technologies.
(O’regan and Grätzel, 1991). Among the different PV technologies, the
Among other technologies, PV technology is highly desirable because it
market has growing interest in the DSSC and maximum power conver­
converts sunlight into power energy. Thus, the primary goal of re­
sion efficiency (PCE) reported for DSSCs is around 14.3% (Kakiage et al.,
searchers and scientists is to generate power from sun radiation by cost-
2015a) which is less than Si-based solar cells. Fig. 5 indicates the
effective and reliable instruments (Sharma and Kar, 2015).
number of publications per year in different fields of DSSCs. But the
In 1839, Becquerel discovered the photosensitivity of selenium and
following features of DSSC make this technology exceptionally inter­
that was the starting of PV phenomena for world (Becquerel, 1839).
esting: -
Significant development in PV can be seen in 1954, when efficient sili­
con solar cell with 6% efficiency was developed in Bell laboratory
(i) easy fabrication, manufacturing at room temperature and low
(Chapin et al., 1954). This triggered the growth of the PV technology
cost.
and this performance boost the PV technology into one of the best
(ii) perform better at higher temperatures and under diffuse light
contenders to overcome the usage of traditional energy resources. At
conditions than other PV cells.
present PV technology are used in both spatial and earth applications
(iii) offers less than one-year short payback period.
such as building integrated PV systems, telecommunications, spacecraft,
(iv) less stringent requirement on materials, use of more widely
cooking & heating units, water pumping, water desalination, satellite,
available feedstock, and manufacturing versatility that can be
lightening street (Sampaio and González, 2017). Overall, PV technolo­
transformed from a basic lab setting to a large scale industrial
gies are growing at high speed in research and industrialization but they
printing production without investment of large amount.
have certain demerits which are shown in Fig. 6 (Sampaio and González,
(v) offer different variety of shapes, sizes, colours, and transparency.
2017).
(vi) printable at the flexible substrate.
(vii) their applicability to indoor facilities, building-integrated PV,
2. Progress in PV technologies
flexible devices for walls or windows, portable devices such as
solar bags, chargers, and solar keyboards.
The development of solar cells from the first crystalline silicon solar
cell to today’s solar cell, as per material point of view, architecture and
These features make DSSCs appealing technology in various fields
technological time scale, can be classified into different generations are
that are not limited exclusively to land use, but even in applications
shown in Fig. 7 and list of solar cell with their current efficiency is shown
ranging from low commercial systems to large-scale architectural
in Table 1 (NREL Best Research-Cell Efficiencies chart, 2021).

Fig. 1. Electricity consumption in different countries around the world (Enerdata, 2020).

379
A. Agrawal et al.
(i) First generation solar cell- This solar cell generation was started in
year 1954-1960 which is based on crystalline solar cell. Silicon is
the most suitable material for the manufacturing of crystalline
solar cell. This generation also includes solo junction gallium
arsenide based solar cell. Silicon based solar cell dominate the
world’s PV market and currently they own 90% of the market
shares (Solar Power Europe, 2016). This is the most reliable and
mature PV technology. However, their manufacturing cost is very
high due to large consumption of materials and complicated
fabrication process (Belfar and Mostefaoui, 2011). The efficiency
of crystalline solar cell is influenced due to change in temperature
(Tobnaghi et al., 2013). Single crystalline and multi crystalline
based solar cells come under this generation.
(ii) Second generation solar cell- This generation solar cells were
developed in the mid of 1970 and also referred as thin film solar
cell. In thin film solar cell, chemical used in the form of powder
that makes the cell lighter and more flexible. Manufacturing cost
is also less as compared to first generation solar cell. However, the
biggest challenge to the thin film solar cell is their lower effi­
ciency (Green, 2007) and limited supply of material. Cadmium
telluride, copper indium gallium diselenide, copper indium dis­
elenide, amorphous silicon and copper zinc tin sulphide are the
solar cells of this generation.
(iii) Third generation solar cell- Development of this generation started
in year 1990 when first efficient DSSC was fabricated. This gen­
eration is also known as emerging thin film solar cell. Organic
solar cell, perovskite solar cell, DSSC and quantum dot solar cell
are the various solar cells of third generation. The main advan­
tage of this generation are low manufacturing cost, simple
fabrication process, eco-friendly materials, feasible for large scale
production, transparent, colourful and flexible device. Most of
the solar cells in third-generation are still in the research stage to
overcome the limitation of short life span of solar cell, unstable
behaviour in environmental conditions and therefore they are
still not fully commercialized.
(a) Hybrid solar cell- This category of solar cell is the hybrid of first,
second and third generation solar cell. It incorporates the benefits
of all solar cell generations to boost performance, reliability and
cost optimization. Hybrid solar cell consist of Perovskite/Si-
tandem (monolithic), Perovskite/CIGS tandem (monolithic) and
Perovskite/ DSSC etc.
Fig. 2. Scenario of the CO2 emission in different countries of the world (Enerdata, 2020).
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Solar Energy 233 (2022) 378–407
3. Background of DSSC
The journey of DSSC was started after 1873 when a scientist named
Hermann Wilhelm Vogel noticed a behaviour change in silver halide
nature while working on the improvement of photographic emulsion
sensitivity. Basically, silver halides are insensitive to maximum portion
of visible light due to their band gaps (2.7–3.2 eV). However, silver
halide placed in dye solution is reactive to visible light (West, 1974;
Hagfeldt and Grätzel, 2000). In 1887, James Moser used the phenome­
non of Vogel and developed the device but voltage was too low for the
application of PV cell (Moser, 1887). Yasushi Hishiki introduced n-type
MOS ZnO with cyanine dye for the investigation of sensitization effects
at semiconductor surfaces (Namba and Hishiki, 1965). Afterward, in
1968, Gerischer developed sensitized photo electrode by replacing
synthetic organic dye with rose Bengal natural dye (Gerischer et al.,
1968). Then, ZnO based electrode sensitized by chlorophyll dye was
prepared in 1972 and shows efficient photons to electricity conversion
(Tributsch, 1972). In subsequent years Daltrozzo and Tributsch added
Rhodamine B as a novel dye for ZnO system. However, cell performance
was very poor because 1% of incident sunlight absorption was allowed
by monolayer of dye molecules on the ZnO surface (Daltrozzo, 1975).
Thus, the performance was enhanced by improving the porosity of SO
deposited on substrate. For that dye absorption on the MOS might be
improved and as a result the efficiency of light harvesting could also be
improved. In 1977, Spitler and Calvin replaced ZnO by TiO2 and
sensitized with rose Bengal dye for better performance (Spitler and
Calvin, 1977). The outstanding achievement in the field of DSSCs was
accomplished by Michael Gratzel and Brian O Regan (O’regan and
Grätzel, 1991; Kalyanasundaram et al., 1987; Kavan and Grätzel, 1989]
at EPFL lab between 1988 and 1991. Gratzel and his collaborators were
able to produce remarkable 7.1% PCE with novel ruthenium (Ru)
bipyridyl complex sensitizer and TiO2 electrode. This DSSC is also
known as Gratzel cell. By using the N3 dye, Grätzel’s group further
increased the performance to 10% in 1993 (Nazeeruddin et al., 1993).
Researchers continue to understand the behaviour of DSSC and to
improve the overall efficiency. In 2004, the N719 dye was used to obtain
an efficiency of 11.18% under 1000 W/m2 illumination, in which one
group of the carboxylic acid was deprotonated and substituted by tet­
rabutylammonium cation in each of the 4,40-dicarboxy-2,20-bipyridyl
groups (Nazeeruddin et al., 2005). The use of redox electrolyte based
on CoII/III tris (bipyridyl) and permitting it to be mixed with a custom
A. Agrawal et al.
Fig. 3. Projected overall generation of electricity across world by all fuels including renewable sources (2010–2050) (U.S. Energy Information Administration, 2019).
Fig. 4. Projected overall generation of electricity across world by all renewable
sources (2010–2050) (U.S. Energy Information Administration, 2019).
synthesized sensitizer (i.e. donor-π-bridge-acceptor zinc porphyrin)
resulted in the PCE being raised up to 12% (Yella et al., 2011). In 2014 a
device fabricated with donor- π-acceptor zinc porphyrin dyes molecu­
larly engineered to work with CoII/III redox mediator that improved PCE
to 13.0% (Mathew et al., 2014). Then, in 2015, by cosensitizing with
LEG4 and ADEKA-1 (two metal-free organic dyes) and CoII/III tri
(phenanthroline)-based electrolyte configuration was prepared by
Kakiage et al. and highest PCE of 14.3% was reported (Kakiage et al.,
2015a). Chronological development of DSSC is shown in Fig. 8.
4. Construction and working of DSSC
The working architecture of DSSC is similar to the photosynthesis
process of plants (Raturi and Fepuleai, 2010). Furthermore, in DSSC the
dye replaces the chlorophyll, the MOS layer replaces the phosphate
nicotinamide adenine dinucleotide, electrolyte replaces the water and
the electron acceptor & electron donor serve equivalent to carbon di­
oxide and oxygen respectively (Smestad and Gratzel, 1998; Lagref et al.,
2008; Efurumibe et al., 2012). In Plants, sunlight converted into energy
by photosynthesis process. Gratzel et al. imitate this prodigy to fabricate
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Solar Energy 233 (2022) 378–407
DSSC, which transforms light energy into electric energy (O’regan and
Grätzel, 1991; Grätzel and Durrant, 2008) DSSC is an architecture of
working electrode MOS layered on conductive glass substrate) soaked
with a dye and CE (catalyst layered on conductive glass substrate) sealed
by polymer material to prevent the leakage of electrolyte (filled between
working electrode and counter electrode) as shown in Fig. 9. Therefore,
MOS, dye, electrolyte, catalyst, conductive glass substrate, sealing ma­
terial are the key components of DSSC design. These components need to
be optimized to maximize the PCE. Here, we provide the characteristics
of these components of DSSC as shown in Fig. 9 for an efficient solar cell.
In order to enhance performance of DSSC, it is important to under­
stand electron behaviour and detailed process of DSSC as shown in
Fig. 10 and Table 2. The working mechanism of DSSC involves following
steps: -
1. Photoexcitation- Under the illumination of sunlight, electron of dye
ground state (Dy) is converted into dye excited state (Dy#) which
means an electron promotes from HOMO state of dye to LUMO state
of dye (Eq. (1)).
2. Injection- Then excited electron is shifted from dye LUMO to CB of
SO, left the dye molecule at MOS/dye interface in an oxidized state
(Dy+) (Eq. (2)).
3. Transportation- After injection of electron, it is transferred to the
contact phase of conductive glass substrate through the meso-porous
MOS (Eq. (3)).
4. Conduction- Electron at surface of conductive glass substrate reached
the CE with help of external circuit (Eq. (4))
5. Diffusion- An electron comes from external circuit diffuse into the
electrolyte through counter electrode. When oxidised form of elec­
trolyte received an electron it goes back to the reduction form of
electrolyte (Ered) and ready to regenerate the dye. This is the elec­
trolyte regeneration (Eq. (5)).
6. Dye Regeneration- The oxidized state (Dy+) of dye is accepting an
electron from electrolyte redox couple and returns to the ground
state (Dy) of dye. Now, dye again available to inject an electron. This
process is dye regeneration (Eq. (6)). Meanwhile, electrolyte reduc­
tion takes place in which an electron and oxidized form of electrolyte
(Eox) are produced (Eq. (7)).
For DSSC, Eqs. (1)–(7) are required reactions for converting the
photon energy into electrical energy. During this light-to-electric
A. Agrawal et al.
Fig. 5. Number of publications each year of various DSSC components during 2011–2020 (Source: www.scopus.com with keywords as mentioned).
Fig. 6. Merits and demerits of solar PV technology (Sampaio and
González, 2017).
conversion, other reactions or phenomena may have occurred which
interrupt the effective flow of electrons. These reactions are known as
recombination reactions. Due to this disruption in flow of electrons af­
fects the overall photovoltage and photocurrent of DSSC. Therefore, it is
important to understand and enhance electron flow in order to boost
DSSC efficiency as shown in Table 2.
In research articles some undesirable recombination reactions re­
ported are: - (i) from CB of SO to the HOMO level of dye (Eq. (8)); (ii)
from CB of MOS to the electrolyte redox couple (Eq. (9)); (iii) from the
dye excited state (LUMO) to the dye ground state (HUMO) (Eq. (10));
(iv) from CGS to the dye HOMO level (Eq. (11)); (v) from CGS to the
electrolyte redox couple (Eq. (12)). These recombination paths are
appeared because of following reasons: - (i) several trap states present
below the CB of MOS (Cahen et al., 2000; Ansari-Rad et al., 2012b; Jeon
et al., 2014), (ii) At each interface surface trapping area (Li et al., 2014;
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Solar Energy 233 (2022) 378–407
Yao et al., 2016), (iii) slow mechanism of dye regeneration (Zhang and
Cole, 2017), (iv) electrolyte penetration in the mesoporous layer of MOS
(Amiri et al., 2013) (v) Inappropriate concentration of electrolyte and
nature of cation species (Nakade et al., 2005). However, recently several
researchers have focused on the development and modification of the
MOS structure, surface passivation of photoanode and improving
counter electrode morphology, variation in dye molecular engineering,
and optimization & alteration of electrolyte to broaden absorption of
light (Sharma et al., 2013; Balasingam et al., 2013), scattering (Niaki
et al., 2014; Deepak et al., 2014; Li et al., 2017), charge transport (Chu
et al., 2016; Javadi et al., 2016b; Lee et al., 2017b), and enhancing the
energy of interfaces by preventing the charge recombination (Sharma
et al., 2013; Mustafa and Sulaiman, 2021). In the upcoming sections
these improvements are explored further. Recently, Ates SonmezogluIn
et al., introduced efficient thin tunneling barrier effect in DSSC that
reduces the charge recombination and improves the electron injection
by using the double helix DNA molecules at TiO2 interface (Ates Son­
mezoglu et al., 2016).
4.1. Equivalent circuit of DSSC
Kern and Bisquert have developed two distinct impedance models.
Kern’s model was focused on the continuity equations of CB and trap
states of MOS, while Bisquert model was primarily connected with the
theoretical perspective of recombination and electron diffusion in the
layer of oxide (Kern et al., 2002; Bisquert, 2002). Later, these ideas were
unified by Adachi and his team, searching method for evaluating pa­
rameters linked to the transport of electrons in the DSSC (Adachi et al.,
2006). Both groups (Bisquert’s and Grätzel’s) use these above works and
formed the foundation of the transmission line model (TLM) of the
DSSCs impedance (Fabregat-Santiago et al., 2005; Wang et al., 2005).
Fig. 11 demonstrates the TLM based equivalent circuit of a DSSC. In the
TLM, there is two parallel networks: - (i) transport of electron via MOS
(ii) transport of redox species through electrolyte. These two networks
are bound by the charge transfer mechanism associated with the reac­
tion of the electrons with the redox ions at the MOS/electrolyte inter­
face. If the thickness of MOS layer is ‘d’, then the detail of circuit
elements of the solar cell is:
• RS (Ω): series resistance, including contact resistance of the cell and
sheet resistance of the TCO glass.
A. Agrawal et al. Solar Energy 233 (2022) 378–407

Fig. 7. Different generations of PV technology (Agrawal et al., 2020).

• cμ (F/m): photoanode chemical capacitance, that stands for the

Table 1
change of electron density as a function of the Fermi level. The total
List of solar cells with their current efficiency solar cell (NREL Best Research-Cell
chemical capacitance is Cμ = cμ × d.
Efficiencies chart, 2021).
• Zd (Ω): electrolyte diffusion impedance, accounting for mass trans­
Type of Generation Type of solar cell Efficiency
port of redox species in the electrolyte.
First Generation Single Crystalline Solar cell 26.1% • RPt (Ω): counter electrode charge transfer resistance at the Pt/elec­
Multi crystalline Solar cell 23.3% trolyte interface.
Single Junction Gallium Arsenide Solar Cell 27.8%
• CPt (F): counter electrode double layer capacitance at the Pt/elec­
Second Generation Amorphous Silicon Solar Cell 14%
Cadmium Telluride 22.1% trolyte interface.
Copper Indium Gallium Diselenide 23.4% • Cí is the chemical capacitance of the MOS film.
Third Generation Dye Sensitized Solar Cell 12.3%
Organic Solar Cell 17.4%
5. Evaluation of DSSC performance
Perovskite Solar Cell 25.2%
Quantum Dot Solar Cell 16.6%
Hybrid Solar Cell The PV performance of a DSSC is measured by the power conversion
Perovskite/Si-tandem (monolithic) 29.1% efficiency (PCE or η), short-circuit current density (Jsc), open-circuit
Perovskite/CIGS tandem (monolithic) 24.2% voltage (Voc) and fill factor (FF).
(a) Short-circuit current density (Jsc)
• RCO (Ω): contact resistance of substrate at the interface between TCO JSC is the current density calculated when no external bias is applied.
and MOS layer. JSC is significantly affected by the dye light absorption, their interfacial
• CCO (F): contact capacitance of substrate at the interface between charge transfer and intramolecular charge transfer from the dye to MOS
TCO and MOS layer. (Omar and Abdullah, 2014).
• RTCO and CTCO (F): charge transfer resistance and the corresponding (b) Open-circuit voltage (Voc)
double-layer capacitance at the exposed TCO-electrolyte interface, VOC is the gap between the energy level of electrolyte redox and the
respectively. quasi-fermi level of MOS. VOC is influenced by the distribution of elec­
• Rt is the resistance of the electron transport resistance in the TiO2 trons in the CB of MOS and the quantity of electron recombination from
film is Rt = rt × d, while the interfacial charge recombination the injected dyes to the oxidized electrolyte as shown in Eq. (1)(Gong
resistance is Rct (=rct/d). et al., 2017).
• RctTCO (Ω): charge transfer resistance of substrate accounting for the ECB kT n Eredox
electron recombination from the uncovered layer of the TCO to the VOC = + ln( )− (1)
q q NCB q
electrolyte.
• rt (Ω/m): electron transport resistance in the MOS layer. The total where n is the number of electrons in the MOS, NCB the effective density
transport resistance of the film is Rt = rt × d. states in the MOS, ECB the energy level of the bottom of the CB of the
• rct (Ω⋅m): charge transfer resistance of the charge recombination MOS, Eredox the energy level of the electrolyte, and q the unit charge.
process between electrons in the mesoscopic MOS film and redox (c) Fill factor (FF)
ions in the electrolyte. FF is defined by the ratio of the maximum power of the solar cell to
the multiplication of JSC and VOC. Moreover, η is strongly affected by the

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A. Agrawal et al. Solar Energy 233 (2022) 378–407

2015 - 14.3%
TiO 2 + Dye (LEG4 + ADEKA1) +
Cobalt based electrolyte + Au/GNP
counter electrode
1991 – 7.1%
TiO 2 + Ru bipyridyl
2004 – 11.18% 2014 - 13%
complex +Iodine based
TiO 2 + N719 dye + TiO 2 +
electrolyte
Iodine based electrolyte molecularly
engineered
2011 – 12.3% Zinc porphyrin
Developme nt

1968 – <1% TiO 2 + Zinc dye + CoII/III

ZnO + Rose Bengal dye porphyrin dye based
+Cobalt based electrolyte
electrolyte
1873
Silver halide 1993 – 10%
sensitive to visible 1977 – <1% TiO 2 + N3 dye +Iodine
light in presence of TiO 2 + Rose based electrolyte
dye Bengal dye
1964 – <1%
1887 ZnO +Cyanine
Silver halide + dye dye
(low 0.04 volt)
Years

Fig. 8. Chronological development of DSSC.

Fig. 9. Structure and characteristics of key components of DSSCs for an efficient solar cell.

FF. FF depends upon the series resistance, characterization conditions
and different fabrication methods (Hamann et al., 2008).
(d) Power conversion efficiency (PCE or η)
PCE of a PV device is the most substantial parameter of solar cell,
which is defined by the incident light power (Pin) and Jsc, Voc, FF as
shown in Eq. (2):
JSC VOC FF
η=
Pin
6. Development of constructional parameters of DSSC
The material selection is the main parameter of DSSC construction to
enhance the performance of DSSC as discussed below:
6.1. Substrate
The widely accepted choice for DSSC substrate is transparent
conductive oxide (TCO) glass because it follows almost all substrate
characteristics (Shalini et al., 2016). The widely used TCO substrates in
(2) DSSCs are (i) Fluorine doped tin oxide (FTO), SnO2:F (ii) Indium doped
tin oxide (ITO), SnO2:In. FTO and ITO transmission in the visible region
is more than 75% and 80%, respectively, while sheet resistance is 18 O/
cm2 and 8.5 O cm2, respectively (Mehmood et al., 2014). FTO is widely
recommended for use in DSSC manufacturing due to its robust sheet
resistance temperature and conduction properties (Sima et al., 2010). A

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A. Agrawal et al. Solar Energy 233 (2022) 378–407

Fig. 10. Energy level diagram representing the electron transfer and illustrates the operational sequence of the DSSC.

2007). Metals such as stainless steel, tungsten, and titanium have also
Table 2
been considered as alternate substrates (Suhaimi et al., 2015). However,
Operational and recombination process indicated by equation with their time­
the metal substrates are opaque, which reduces cell efficiency (Jun et al.,
scale for charge transport (Kumara et al., 2017; Saygili et al., 2019; Bera et al.,
2021).
2007). Overall, substrate used in the DSSC should have following
characteristics: -
Equation Reaction Process Time
No.
(a) Should be transparent to allow incident light to pass through
1 Dy (at MOS) + sunlight Photoexcitation 100 fs-100 them.
→ Dy# (at SO) ps
2 Dy# (at MOS) → Dy+ (at Electron injection 1 ps
(b) Low and stable sheet resistance which is helpful for smooth flow
SO) + e− (injected at (10− 12s) of electron.
MOS) (c) Good conduction properties to collect the electron from MOS and
3 e− (at MOS) → e− Electron transport 10 ms transferred the external circuit.
(transported at CGS) (10− 3s)
(d) High optical transmittance so that minimum reflection and ab­
4 e− (at CGS) + I2Rext → Electron conduction
e− (conducted at CE) sorption of light.
5 EOx + e− (at CE) → Ered Electron diffusion or 10 µs (e) Provide mechanical strength to the device.
Electrolyte Regeneration (10− 6s)
6 Dy (at MOS) + ERed →
+
Dye regeneration 0.10–10 µs
Dy (at MOS) + EOx (10− 6s) 6.2. Metal oxide semiconductor
7 EOx + e− (free) → Ered Electrolyte Reduction 10− 5s
8 e− (MOSCB) + Dy+ (at Recombination between 1 µs − 30 ms For the first time in 1972, a wide band gap of semiconductor was
MOS) → Dy(at MOS) SOCB and DyHOMO (10− 4s) used to convert photon into electricity (Tributsch, 1972). Tributsch
9 e− (SOCB) + EOx → Ered Recombination between 1 ms
demonstrated a DSSC having chlorophyll sensitized ZnO electrode.
SOCB and electrolyte (10− 2s)
10 Dy# (at SO) + sunlight De-excitation 20 ns However, light harvesting in ZnO-based DSSCs was severely reduced
→ Dy (at SO) (10− 9s) due to insufficient dye adsorption to the MOS surface. After that, Grat­
11 e− (at CGS) + Dy+ (at Recombination between – zel’s group recorded a breakthrough PCE in 1991 with the incorporation
SO) → Dy (at SO) CGS and DyHOMO
of mesoporous TiO2 nanoparticles. The incorporation of a mesoporous
12 e− (at CGS) + EOx → Ered Recombination between –
CGS and electrolyte
MOS layer greatly expanded the inner surface area, allowing for more
dye loading without losing interaction with the dye/electrolytes (O’re­
gan and Grätzel, 1991). This significantly increased the PCE and boost
thin film of TiO2 and cadmium stannate (CTO) was coated on glass the DSSC research field.
substrates using magnetron sputtering, leading to a novel TCO (Braga TiO2 (Tennakone et al., 1999; Lenzmann et al., 2001; Ito et al., 2008;
et al., 2014). New CTO contact shows approximately 90% optical Guo et al., 2012; Hegazy et al., 2016; Agrawal et al., 2021), ZnO (Ten­
transmittance and 15 O/cm2 sheet resistance. Plastic substrates, on the nakone et al., 1999; Saito and Fujihara, 2008; Memarian et al., 2011;
other hand are highly acceptable due to their low cost and flexibility. Vittal and Ho, 2017; Shashanka et al., 2020), SnO2 (Chappel and Zaban,
However, the use of plastic is limited by its instability (Weerasinghe 2002; Birkel et al., 2012; Batmunkh et al., 2016) SrTiO3 (Burnside et al.,
et al., 2013). FTO/ITO coated transparent polymer films like poly­ 1999; Lenzmann et al., 2001; Jayabal et al., 2014), Zn2SnO4 (Tan et al.,
ethylene terephthalate are also used as glass substrates in DSSCs. Ad­ 2007; Chen et al., 2012; Shin et al., 2014; Das et al., 2017), WO3 (Zheng
vantages of this film are cheap in cost and their flexibility (Jun et al., et al., 2010; Yong et al., 2013; Patil et al., 2021), Nb2O5 (Sayama et al.,

385
A. Agrawal et al.
Fig. 11. Equivalent circuit and general transmission line model of DSSC. Reproduced from Publication (Fabregat-Santiago et al., 2005), Copyright (2005), with
permission from Elsevier.
1998; Tennakone et al., 1999; Lenzmann et al., 2001; Ou et al., 2012;
Rani et al., 2014), MgO (Jung et al., 2005; Merazga et al., 2016), Al2O3
(Choi et al., 2008; Zazpe et al., 2017) etc. are the popular metal oxides
which have been commonly used as photoanode material due to their
high tolerance to photo-corrosion and superior electronic properties.
The band positions of various MOS are shown in Fig. 12 (Highfield,
2015). Among these MOS, TiO2 (3.2 eV), ZnO (3.2 eV) and SnO2 (3.8 eV)
have shown better performance. However, TiO2 is the most preferred
option for the construction of DSCC due to its increased photo stability
under intense operating conditions, low cost, simple to produce, secure
and more chemically stable (Hagfeldt et al., 2010; Ahmad et al., 2017).
Although the high electronic mobility of ZnO and SnO2 more than 2
orders of magnitude, and ZnO has a comparable band gap (3.2 eV) to
that of TiO2. There is a high band gap of SnO2 (3.8 eV) and the CB is
around 500 mV which is more positive than that of TiO2. Therefore,
SnO2 displays a higher injection rate of charge than ZnO and TiO2
(Tiwana et al., 2011). Despite the benefits of ZnO and SnO2, have poor
PCE. Few papers are published to justify the differences in ZnO, TiO2 and
SnO2 based solar cell performance (Milan et al., 2015; Tiwana et al.,
2011; Zhang et al., 2008, 2012b). A comparative assessment of electron
movement and injection dynamics of mesoporous ZnO, SnO2 and TiO2,
sensitized with Z907 dye have been documented by Tiwana et al.
(Tiwana et al., 2011). They demonstrated that TiO2 has a quicker elec­
tron injection (a few picoseconds) than ZnO and SnO2 (10 to 100 pico­
seconds). The effective mass of an electron in TiO2 (5–10 me) is higher
than that in ZnO (~0.3me) and SnO2 (~0.3me). Hence, injection of
electron in TiO2 is fast as compared to both ZnO and SnO2. Němec et al.
reported that the slow injection of ZnO could be due to lower static
dielectric constant (~10) than TiO2 (~100) (Němec et al., 2010).
6.2.1. Modifications in metal oxide semiconductor
(a) Doping
Fig. 12. Band position of different MOS used for photoanode (Babar et al., 2020).
386
Solar Energy 233 (2022) 378–407
The doping of MOS with transition metals or ions has effectively
improved the DSSC efficiency. The effect of doping in DSSC is to widen
the absorption range of MOS in the visible area, thus changing the MOS
band gap and reducing the recombination of electron. Other develop­
ment involves surface alteration of MOS using metal oxides, coating of a
semiconductor with noble metals and introduction of carbon materials
into a semiconductor (Ye et al., 2015).
Tong et al. improved the efficiency of TiO2 after doping of W due to
the creation of the intermediate band inside the TiO2 band (Tong et al.,
2014). Zhang et al. also reported encouraging performance of Ce doped
TiO2 due to the incorporation of Ce impurity effect in the CB of TiO2
(Zhang et al., 2012a). The results of Mg doped TiO2 may be attributed to
process of band shifting and disruption of recombination of interfacial
charge (Raj et al., 2013). Improved efficiency against Ga doping in ZnO
by Kim et al. due to increase in resistance of electron recombination
(Kim et al., 2012). For ZnO, Futsuhara et al. analyzed their optical band
gap that is minimized by doping with N from 3.26 to 2.30 eV (Futsuhara
et al., 1998). Mahmood et al. showed indium-doped ZnO based DSSC
which produced significant result of 7% efficiency (Mahmood et al.,
2013). Akin et al. presented dual dopant (Ge and Te) ZnO nanoparticle
based DSSC and exhibited 7.08% of PCE for Ga0.25Te0.75ZnO, which is
greater than pure ZnO based DSSC (3.53%) (Akin et al., 2017).
The doping of SnO2 using n-type material leads to excessive va­
cancies of oxygen and decreases the band gap further. Meanwhile,
doping of SnO2 using p-type material would transfer the energy level
from Fermi to the VB and further expand the band gap. An important
structural relaxation and alteration of the charge across Sb in Sb-doped
SnO2 surface was noted by Boumeddienne et al. (Boumeddiene et al.,
2013). As a dopant, Zn2+ and Ni2+ were used by Shalan et al. in SnO2
nanoparticles and had better PCE of 4.2% and 3.6% respectively than
undoped SnO2 (3.2%) (Shalan et al., 2014). Comparable PCE (4.15%)
was achieved with Zn doped SnO2 by Li et al. which is four times greater
than PCE of simple SnO2 (1.13%) (Li et al., 2012). Table 3 shows some
A. Agrawal et al. Solar Energy 233 (2022) 378–407

Table 3 Table 4
Efficiency of the DSSCs based on differently doped MOS. Various morphologies of MOS and their efficiency.
S. Metal oxide Dopant PCE Reference S. Metal oxide Morphology PCE Reference
No. Semiconductor (%) No. Semiconductor (%)

1 TiO2 W 9.10 (Zhang et al., 2011) 1 TiO2 Nanoparticle 10.6 (Grätzel, 2003)
2 Sb 8.13 (Wang et al., 2012) 2 Nanotube 9.1 (Lin et al., 2010)
3 Cr 8.4 (Kim et al., 2008) 3 Nanorod 9.5 (Lee et al., 2009)
4 Sn 8.31 (Duan et al., 2012) 4 Nanowire 6.2 (Lee et al., 2013)
5 Ce 7.65 (Zhang et al., 2012a) 5 Nanoflakes 8.2 (Shanmugam et al.,
6 N 6.25 (Xie et al., 2013) 2013)
7 Nb 8.7 (Lü et al., 2010) 6 Nanosphere 8.44 (Kim et al., 2009)
8 ZnO N 5 (Mahmood et al., 7 ZnO Nanoparticle 6.58 (Saito and Fujihara,
2014) 2008)
9 Mg 4.19 (Raj et al., 2013) 8 Nanowire 5.7 (Barpuzary et al.,
10 I 4.5 (Zheng et al., 2011) 2014)
11 Ga 4.01 (Futsuhara et al., 9 Nanorods 4.7 (Rao and Dutta,
1998) 2008)
12 In 7 (Mahmood et al., 10 3D Sponge 6.67 (Sacco et al., 2012)
2013) 11 Nanosheet 7.07 (Lin et al., 2011)
13 Ga-Te Dual 7.08% (Akın et al., 2016) 12 Microspheres 5.16 (Li et al., 2012a)
dopent 13 SnO2 Nanocrytal 3.2 (Birkel et al., 2012)
14 SnO2 Ta 3.26 (Ramarajan et al., 14 Nanoparticles 1.66 (Lee et al., 2011)
2020) 15 Nanoroad 1.4 (Wijeratne et al.,
15 Zn 1.29, (Li et al., 2011; 2012)
4.20 Shalan et al., 2014) 16 nanotubes 1.06 (Desai et al., 2013)
16 Ni 3.60 (Shalan et al., 2014) 17 Nanograins 2.98 (Lee et al., 2011)

useful dopants and their respective PCE for various MOSs available in
the literature.
(b) Nanostructure
Research advancements have implemented improved MOS
morphology that decreases the influence of grain boundaries, acceler­
ates the transfer of electrons. The surface area improvement of MOS is
done by increasing the nanostructure’s length and by adding nano­
particles between them (Karim et al., 2019). Diverse MOS morphology
as photo-anode has been developed ranging from 1-D structure (nano­
rod, nanotubes, nanowires etc.) to 3-D structure (nanospheres, nano­
flowers etc.) to more advanced structure (hollow microspheres etc.) in
order to supress dark current formation and boost the performance of
DSSCs. The efficiency of 13% was achieved through TiO2 nanoparticle
film sensitized by porphyrin dye (Mathew et al., 2014). Lin et al. pre­
pared perpendicular oriented TiO2-nanotube onto TiO2 thin deposited
FTO substrate. Efficiency of 9.1% was achieved due to smooth interac­
tion of electrolyte with TiO2 thin film through open ended TiO2-nano­
tube (Lin et al., 2010). Kim et al. obtained PCE of 8.44% with
synthesized TiO2-nanosphere because it enhanced the dye adsorption
with MOS film (Kim et al., 2009). Javadi et al. enhanced the DSSC
performance (~8.91%) by incorporation of quasi-two-dimensional
porous TiO2 structure. As electron confinement in a porous media is a
significant strategy for effective transportation of electron toward the
collecting electrode due to this phenomenon PCE of DSSC has been
improved (Javadi et al., 2016b). Tao et al. used ZnO nanorod as pho­
toanode and gave 0.96% efficiency by increase in resistance of electron
recombination at the ZnO/electrolyte interfaces (Tao et al., 2012). Saitio
et al. achieved better short circuit current and PCE of 6.58% due to
improve dye loading of dye on ZnO-nanoparticles (Saito and Fujihara,
2008). Lin et al. prepared ZnO-nanosheet and achieved 7.07% efficiency
with TiO2- nanoparticles (Lin et al., 2011). Birkel et al. fabricated SnO2
nanocrystals based DSSC and 3.2% od PCE obtained due to efficient
charge transport in photoanode (Birkel et al., 2012). Lee et al. prepared
SnO2 nanograin and gave PCE of 2.98% in DSSC. SnO2 nanograin
improved the electron diffusion and light scattering effect in MOS layer
(Lee et al., 2011). Various morphologies of semiconductor oxides and
their efficiency are shown in Table 4.
Electron transport in nanostructured MOS materials or porous media
is a significant and relevant area from both theoretical and technical
perspective. The flow of electrons in this porous medium influences the
performance of DSSC (Smolin et al., 2015; Javadi et al., 2016a). To study
the electron transport phenomenon in porous medium, Monte-Carlo
random walk simulations was recently utilized (Anta and Morales-
Flórez, 2008; Ansari-Rad et al., 2012a). To explain electron transport in
trap-contained nanostructured media, two primary techniques have
been used (i) Multi-trapping model: transfer of charge carriers is
accomplished by the trapping and detrapping of electrons from the
localized states to the transport level (Ansari-Rad et al., 2012c) (ii)
Hoping model: charge carrier transportation done by direct transitions
between the localized states (Abdi et al., 2016, Abdi et al., 2017). Javadi
and Abdi detailed the transportation of electrons in thick layer and
columnar structure of porous TiO2 by Monte Carlo continuous time
random walk simulation (Javadi and Abdi, 2015). Naser et al. developed
equations that describe the morphological dependence of electron flow
in nanostructured solar cells (Abdi et al., 2016).
(c) Plasmonic effect
Metal nanoparticles can be used in MOS to efficiently capture light
because of their nature of optical phenomena and this effective strategy
is surface plasmon resonance (SPR). SPR is the cumulative excitation of
electrons in metal nanoparticles as they communicate with electro­
magnetic radiation and strengthens electromagnetic waves in their at­
mospheric environment. Metallic nanoparticles such as silver (Ag), gold
(Au), aluminium (Al) and copper (Cu) show SPR in the visible region and
therefore serve as suitable options for the light trapping in solar cells.
Solar cells using SPR for light-harvesting are known as plasmonic solar
cells (Jeong et al., 2011; Dhonde et al., 2017). Different types of work
reported in plasmonic nanoparticles like doping in MOS, core/shell
structure of metal nanoparticles in MOS and back scattering layer (Amiri
et al., 2018; Ganeshan et al., 2018; Ali et al., 2019).
Nahm et al. doped TiO2 with Au nanoparticles and enhanced 20%
PCE as compared to undoped TiO2 (Nahm et al., 2011). Double layer
film structure was made in DSSC through Ag doped TiO2 and Au doped
TiO2 and 10.03% of efficiency was obtained (Kim et al., 2015). Incor­
poration of Au and Pt metal nanoparticles in TiO2 based photoanode
demonstrate improved PCE than simple TiO2 based photoanode (Khan
et al., 2017). Aponsu et al. inserted Au as a dopant into photoanode
based on SnO2 demonstrated better 3.9% PCE than simple SnO2 (Aponsu
et al., 2010). The improvement is defined by moving the CB edge of
SnO2 to a higher level upon in contact with Au nanoparticles. Core@­
shell (Au@SiO2 and Ag@SiO2) structure was used by Gangishetty et al.

387
A. Agrawal et al.
and Brown et al. to improve the PCE. This core@shell structure
enhanced the efficiency by preventing the corrosion of metal nano­
particles (Brown et al., 2011; Gangishetty et al., 2013). Amiri et al.
deposited a layer of Ag nanoparticles in between TiO2 layers and
improved the PCE from 3.47% to 5.26% (Amiri et al., 2015). Recently,
Selvapriya et al. synthesised multishaped Ag nanoparticles and included
in DSSC which had enhanced the PCE of DSSC from 5.28% to 7.64% due
to coupled plasmonic effect (Selvapriya et al., 2022).
(d) Addition of metal oxide layer
The SO coated with materials like ZnO (Kay and Grätzel, 2002;
Niinobe et al., 2005; Kanmani and Ramachandran, 2012), Al2O3 (Pal­
omares et al., 2003; Law et al., 2006; Ganapathy et al., 2010; Zazpe
et al., 2017), SnO2 (Pang et al., 2014; Milan et al., 2015), SrTiO3 (Dia­
mant et al., 2003; Wu et al., 2011; Kim et al., 2013), and Nb2O5 (Chen
et al., 2001; Barea et al., 2011; Kim and Moon, 2012; Suresh et al., 2018)
called as core–shell structures. This strategy reduces recombination of
charge and moves the CB potential. For example, Lee et al. noted that
ZnO–SnO2 nanocomposite thin film exhibits outstanding electronic
conduction capabilities due to the special elecronic configuration of
amorphous nanocomposite combined by two heavy-metal Zn and Sn
cations (Lee et al., 2014b). Further analysis on the integration of SnO2
with Zn2SnO4 showed the effective separation of photogenerated pair of
electron-hole due to the lower SnO2 CB relative to Zn2SnO4 (Li et al.,
2015). Li et al. recorded a substantial increase in PCE (1.29%) of
Zn2SO4/ SnO2 over simple Zn2SO4 (0.90%) and SnO2 (0.28%) based
DSSC (li et al., 2011). Wang et al. integrates a SnO2/TiO2–ZnO bilayer in
DSSC and obtained better efficiency of 6.37% (Wang et al., 2015). The
Al2O3 coated SnO2/TiO2 electrode improved the cell performance by
37% as compared to simple SnO2/TiO2 (Liu et al., 2005).
Some others efforts are made to improve photoanode characteristics
by insertion of blocking layer before the MOS layer. For example, in
order to block recombination of electron between FTO and electrolyte, a
dense and compact layer of TiO2 can be deposited onto the FTO before
the deposition of TiO2 layer (Krüger et al., 2001; Cameron and Peter,
2003; Peng et al., 2004; Lin et al., 2009; Burke et al., 2008). While other
materials, such as Nb2O5, ZnO, CaCO3, and BaCO3 have been investi­
gated and used. TiO2 is still the most preferred material because strong
adhesion of the TiO2 mesoporous layer with the FTO substrate, while its
denser and more continuous morphology provides more pathways for
electron collection. Overall, incorporation of different technique for the
modification of MOS were found to improved absorption of dye, optical
scattering, charge collection efficiency and charge transfer dynamics
(Lenzmann et al., 2001; Green et al., 2005).
From the above discussion, it can be concluded that, MOS has sig­
nificant role in DSSC’s performance because it accelerates the transfer of
electrons, increases the surface area for dye, reduces the recombination
pathway etc. For the improvement and modification of MOS’s charac­
teristics different strategies which are crucial i.e. doping of ions, nano­
structured shapes for morphological development, use of plasmonic
metals and insertion of metal oxide layer have been discussed. Thus,
following parameters are to be included in the selection of the MOS in
the DSSC: -
(1) Transparent to eliminate the absorption of visible spectrum.
(2) CB of MOS relatively lower than that of dye LUMO for better
transport of photogenerated electrons.
(3) inexpensive, stable, eco-friendly and simple synthesis.
(4) quick conduction of electron from dye to external circuit.
(5) offer high mobility for charge carriers to effectively capture
photoelectrons.
(6) high dielectric constant that delivers effective electrostatic
shielding of the injected electron from the oxidized dye thus
preventing electron recombination until the dye is reduced by the
redox electrolyte.
388
Solar Energy 233 (2022) 378–407
(7) high refractive index enables effective diffuse scattering of the
light within the porous photoelectrode which improves light
adsorption.
(8) for good dye adsorption, porosity and surface area of MOS should
be high. Because it expands the absorption range.
(9) inert to redox electrolyte for reducing electron recombination
rate.
6.3. Dye photo-sensitizer
The Dye photosensitizer (DPS) plays a critical role in maintaining the
performance of light harvesting and the output of photo-excited elec­
trons in the DSSC. DPS is covalently anchored with the MOS, absorbs
photons from sun radiation below 920 nm wavelength and transforms
sunlight energy (standard global AM 1.5) into electrical energy. The
performance of the DSSC is primarily determined by the molecular
configuration of the DPS (Sharma et al., 2018). Fig. 13 shows the
different forms of DPS used in DSSCs (Iqbal et al., 2019; Tomar et al.,
2020; Devadiga et al., 2021). DPS can be classified into metal-complex
photosensitizer, organic photosensitizer, and natural photosensitizer,
which are described below. These photosensitizers have several ad­
vantages and disadvantages which are discussed in Table 5.
6.3.1. Metal complex photo-sensitizer
Various metal based photo-sensitizers have been used for DSSC such
as Ruthenium (O’regan and Grätzel, 1991; Bomben et al., 2012;
Colombo et al., 2014; Naik et al., 2018), Iridium (Wang et al., 2013b;
Hierlinger et al., 2018), Copper (Sandroni et al., 2016; Dragonetti et al.,
2019), Osmium (Altobello et al., 2005; Swetha et al., 2015; Juwita et al.,
2020), Platinum (Gauthier et al., 2014; Yam et al., 2015), Rhenium
(Wong et al., 2007) and Iron (Harlang et al., 2015). Anchoring and
ancillary ligands are present in metal complex sensitizers and have
significant effect on DSSC. Ancillary ligands alter the functional prop­
erties of the sensitizer because anchoring capability of sensitizers to
MOS depends upon the nature of anchoring ligands. By the modifica­
tions of these two ligands the performance of the DSSCs have been
improved. There are many papers published on these two ligands but
most of the works reported on the ancillary ligands development (Gong
et al., 2012; Mehmood et al., 2014).
Ruthenium complexes based dyes have been intensively explored
and widely used because they are the most efficient sensitizers for DSSC
(Table 6) (Nazeeruddin et al., 2001; Tomar et al., 2020). The chemical
structure of various Ru based dyes shown in Fig. 14. The origin of these
complexes occurred in 1970s, when tris(2,2′ -bipyridyl) Ru(II) was
identified as a sensitizer (Yanagida et al., 2009). Some other ruthenium
polypyridyl complexes are used as sensitizers for photo-generation and
able to transform PCE of around 11% under AM1.5 conditions. Grätzel
and his group produced a significant range of Ruthenium complex DPS,
the most prominent being N3 or red dye. Nazeeruddin et al. used N3 dye
and deliver an efficiency of 10% under AM 1.5 solar radiance (Nazeer­
uddin et al., 1993). N749 (Nazeeruddin et al., 1997; Nazeeruddin et al.,
2001; Yanagida et al., 2009; Liu et al., 2012) and N719 (Wang et al.,
2004c; Al-Alwani et al., 2016) also known as black dye were identified
by the same group and reported PCE of 11.1% and 11.18% respectively
(Nazeeruddin et al., 2005; Chiba et al., 2006). These ruthenium com­
plexes are the most powerful sensitizers due to: - (i) broad absorption
spectra in the region of visible to near-infrared (ii) carboxylate groups
that are linked to bipyridyl moiety reduces the ligand π* orbital energy
(Monari et al., 2011).
Several ruthenium-based sensitizers have been investigated to
improve the efficiency and stability of DSSCs (Bessho et al., 2009;
Vougioukalakis et al., 2011). The new amphiphilic sensitizers K19
(Wang et al., 2003, Wang et al., 2005a)and K73 (which has no amphi­
philic chains) (Kuang et al., 2006a) and K77 are introduced (Kuang
et al., 2007). The improved absorption properties of the K77, K73 and
K19 molecules are likely to derive from their more complex conjugated
A. Agrawal et al.
Fig. 13. Different types of DPSs used in DSSCs.
Table 5
Advantages and disadvantages of different types of dye.
Types of Dye
Metal based
Advantages (1) with the aid of noble metal-based sensi­
tizers, highly efficient DSSCs have been
developed.
(2) quick electron injection and strong
anchoring capacity with MOS molecules
specially with TiO2.
(3) ruthenium dye has good photochemical,
photo physical and electrochemical
properties.
(4) it has stable and usable oxidation states
from I to IV.
(5) the broad range of the absorption
spectrum can be tuned to achieve high
coefficients of molar extinction.
(6) long excited lifetime
(7) good solubility is found in all solvents.
(8) highly effective metal-to-ligand charge
transfer spectra are demonstrated by
metal complex dyes.
(9) high redox properties.
(10) broad absorption spectra from visible to
NIR.
Disadvantages (1) high cost due to restricted quantity of noble
metals.
(2) complex synthesis and purification steps
limit their use.
(3) harmful for nature.
(4) stability and degradation problem due to
water molecules penetrate the electrolyte
allowing the dye to desorb from the TiO2
layer
Solar Energy 233 (2022) 378–407
Metal Free Natural
(1) with the help of metal free-based organic sensi­ (1) eco-friendly DSSCs can be fabricated.
tizers, cost-effective DSSCs have been developed. (2) no use of noble metals
(2) compared to metal complex dyes, the organic dye (3) inexpensive and widely available
preparation process is simple, low-cost, non-toxic (4) easy to prepare and completely biodegradable
because they do not contain noble metals such as (5) with the aid of functional groups such as
Ru, Os, Ir, etc. hydroxyl groups, sulfonic acid and carboxylic
(3) dye aggregation occurs in metal-free organic acid, the amount and wavelength of light to be
dyes, resulting in intermolecular quenching. absorbed can be altered.
(4) high molar extinction coefficients (6) good photoreceptors
(5) stability under high temperature and long
illumination.
(6) comparable PCE with metal complex dyes.
(7) exhibits exceptional electronic and optical
properties
(8) strong light-harvesting capability and tunable
redox potential.
(9) large absorption coefficients produced by
intramolecular π-π* transitions
(1) on TiO2 surfaces, strong π-stacked aggregates (1) PCE reported is very poor due to easier
between D–π–A dye molecules accumulation of dye that affects layer
(2) there are less electron-injection yields from the absorption.
dyes to the TiO2 CB as compared to metal com­ (2) steric obstruction of the molecules which
plex dyes. prohibits them from being organized on the
(3) low absorption bands in contrast with metal dye, surface.
due to this potential of light absorption decreases. (3) low stability due to degradation of dye with
(4) low stability because sensitizer properties decay time.
with time.
(5) it contains chemicals that are expensive and
easily not available.
(6) long and repetitive purification process, and
needs longer time for the preparation
(7) toxic in nature and affect the environment.
(8) The observed stability was not strong as expected
under high temperature.
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Table 6 ancillary ligand and PCE of 6.22% and 6.75% was obtained, respectively
PV parameters of metal complex photosensitizer. (Paek et al., 2010).
S. Dye λmax PCE Jsc Voc FF Reference Some other heavy transitions metal such as platinum, rhenium and
No. (nm) (%) (mA/ (V) osmium are explored to develop new range of sensitizers for DSSC. For
cm2) example, Wu and co-workers replicate the design of TF1 (ruthenium
1 N3 534 10.0 18.2 0.72 0.73 (Nazeeruddin based sensitizer) to develop TF-51 and TF-52 (osmium based sensi­
et al., 1993) tizers), which comprises 4,4′ ,4′′ -tricarboxy-2, 2′ :6, 2′′ -terpyridine
2 N719 540 11.18 17.73 0.84 0.74 (Nazeeruddin (H3tctyp) and dianionic 2,6-bis (1,2-pyrazol-5-yl) pyridine chelating li­
et al., 2005)
3 N749 605 10.4 20.53 0.72 0.70 (Nazeeruddin
gands. The efficiency produced by TF-51 and TF-52 sensitizers based
et al., 2001) DSSC demonstrated efficiency of 7.40% and 8.85%, respectively (Wu
4 N945 550 9.6 16.5 0.79 0.72 (Nazeeruddin et al., 2012). Based on benzathiazole moiety a series of chlorotricarbonyl
et al., 2006) rhenium(I) complexes have been developed and achieved low PCE of
5 Z910 543 10.2 17.2 0.77 0.76 (Wang et al.,
1.72%, 1.46%, and 1.43%, respectively (Colombo et al., 2014). Plat­
2004b)
6 Z955 519 8.0 16.37 0.70 0.69 (Wang et al., inum metal also used in DSSCs as sensitizer such as square planar
2004a) platinum (II) dyes with Pt(4,4′ -dicarboxy-2,2′ -bipyridine)(quinoxalline-
7 Z907 526 7.3 14.6 0.72 0.69 (Wang et al., 2,3-dithiolate) and Pt(4,7-dicarboxy-1,10-phenanthroline) (quinoxal­
2003) line-2,3-dithiolate). DSSCs prepared by these sensitizers showed PCE of
8 K73 545 9.0 17.22 0.74 0.69 (Kuang et al.,
2006a)
2.57% and 2.33%, respectively (Islam et al., 2000).
9 K8 555 8.64 18.0 0.64 0.75 (Klein et al.,
2005) 6.3.2. Metal free dye
10 K51 530 7.8 15.4 0.73 0.68 (Kuang et al., Metal-free dyes (organic donor–acceptor (D–A)) is a second category
2006a)
of the synthetic sensitizers which can be produced by known design
11 K19 543 7.0 14.61 0.71 0.67 (Wang et al.,
2005a) strategies (Horiuchi et al., 2003; Mishra et al., 2009; Ahmad et al.,
12 C101 547 11.0 17.94 0.77 0.78 (Gao et al., 2013). The researchers developed interest in organic dye after year 2000
2008a) when efficiency is improved from 4% to 9% (Chen et al., 2007b; Ooyama
13 C106 550 10.57 18.28 0.74 0.77 (Cao et al., and Harima, 2009; Hagfeldt et al., 2010). Organic dyes have several
2009)
benefits for DSSC applications relative to traditional ruthenium dyes as
14 C104 553 10.53 17.87 0.76 0.77 (Gao et al.,
2008b) seen in Table 5.
15 CYC- 551 8.96 17.4 0.78 0.65 (Li et al., 2010) Several organic dyes, such as coumarin dyes (Hara et al., 2003; Wang
B7 et al., 2007), hemi-cyanine dyes (Chen et al., 2005); indoline dyes (Ito
16 CYC- 553 8.54 23.92 0.65 0.55 (Chen et al.,
et al., 2006; Wang et al., 2014) carbazole dyes (Wang et al., 2008),
B1 2006)
17 CYC- 554 7.9 16.1 0.71 0.69 (Chen et al., porphyrin dyes (Campbell et al., 2007; Ladomenou et al., 2014), tri­
B11 2009a) phenylamine dyes (Singh et al., 2012; Liang et al., 2007, perylenes (Li
18 SJW- 546 9.02 21.6 0.66 0.62 (Chen et al., et al., 2008) and phthalocyanine dyes (Martín-Gomis et al., 2014; Mori
E1 2007a) et al., 2010) are employed in DSSC (Table 7), and solar cell based on
19 IJ-1 536 10.3 19.2 0.74 0.72 (Yum et al.,
these dyes exceeds the PCE of 10% (Hardin et al., 2012). These sensi­
2009)
tizers are efficient and provide a way to manufacture new sensitizers
that can attain the best possible performance and address possible sta­
hydrophobic bipyridyl ligand systems relative to other molecules (Al- bility problems. Fig. 15 shows the chemical structures of some efficient
Alwani et al., 2016). Then, K51 sensitizer containing Li+ coordinating organic dyes available in literature.
was developed by Kuang et al. which has better PCE than Z907 sensitizer In DSSC, organic dye generally identified as D–π–A molecular
(non-ion-coordinating) due to efficient Li + coordination with meso­ structure. It comprises an electron donor (D)/acceptor (D) configuration
porous TiO2 MOS (Kuang et al., 2006b). Chen et al. reported CYC-B3 and connected via π-conjugated bridge as shown in Fig. 16. After light ab­
SJW-E1 sensitizer, and explored the effect of ethylenedioxy groups on sorption, the presented groups induce the separation of charge from the
the physicochemical properties & performance of the dye molecules. donor part to the acceptor part, where the dye is adsorbed to the MOS
CYC-B3 and SJW-E1 based DSSC exhibited PCE of 7.39%, and 9.02% surface (Yella et al., 2011; Yella et al., 2013; Mathew et al., 2014). The
respectively (Chen et al., 2007a). Kuang et al. showed PCE of 6.6% for a characteristics of a sensitizer depend upon the ability of the acceptor
DSSC based on K68 sensitizer (ewion-coordinating ruthenium poly­ part to accept the electron and the donor part to donate the electron, as
pyridyl) (Kuang et al., 2008). CYC-B11 (heteroleptic ruthenium photo­ well as on the electronic properties of the π bridge.
sensitizer) was designed by Chen et al. in year 2009 by adding hexylthio- Metal-free organic dyes are the best alternative option to replace the
bithiophene which are dense with electrons (Chen et al., 2009a). As a ruthenium based dyes. The first successful implementation of organic
result, the light harvesting ability increased and PCE of 11.5% was dyes done by Feldt et al. They used D35 (triphenylamine-based dye)
achieved. Bessho et al. replaced cyclometalated 2,4-difluorophenylpyr­ named organic dye with cobalt based electrolyte (Feldt et al., 2010;
idine with thiocyanate donor ligands to form the panchromatic photo­ Feldt et al., 2011; Tsao et al., 2011). Using indoline dye Horiuchi et al.
sensitizers (Bessho et al., 2009) and improved the performance of DSSC. obtained PCE of 6.1% (Horiuchi et al., 2003). For organic push–pull
In 2014, novel photosensitizers JJ7 and JJ9 were demonstrated by Kim photosensitizers in DSSCs, Peng Wang and team identified rigidified-
et al. and shown an efficiency of 4.96% and 5.07% respectively (Kim conjugated linkers (Zhou et al., 2011a; Cai et al., 2013; Dai et al.,
et al., 2014). Gao et al. introduced C101 and C102 (heteroleptic poly­ 2015). The C275 dye contains 4-Hexylphenyl moieties that result in high
pyridyl ruthenium sensitizer) and C101 sensitizer achieved remarkable molar extinction with a red-shifted absorption and exhibited efficient
PCE of 11.0-11.3% (Gao et al., 2008a). Another efficient C106 hetro­ efficiency of 12.5% (Yao et al., 2015).
leptic sensitizer was developed and reached to 11.7% efficiency. It Another sequence of organic dyes derived from the synthesis of the
comprises bipyridine ligand with thiophene moieties to boost spectral twisting electron-donor triphenylaminephenanthro carbazole. A
characteristics and hydrophobic alkyl chains to guard the SO from the mixture of planar (1,2,5-thiadiazol)benzyl and ethynyl units acceptor
redox ions (Cao et al., 2009). Paek et al. synthesized JK-91 and JK-92 moiety stabilized the sensitizer’s LUMO level without the usual
ruthenium based sensitizers by replacing the 2,2′ -bipyridyl-4,4′ -dicar­ compromise of lower photon-to-electron conversion efficiency. The
boxylate groups in N719 sensitizer into the conjugated bipyridine of the C288 dye using mixture of planar (1,2,5-thiadiazol)benzyl and ethynyl

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Fig. 14. Chemical structure of various metal based dyes (Al-Alwani et al., 2016; Tomar et al., 2020).

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Table 7 achieved by co-sensitizing system of chemically modified chlorophyll a

The PV parameters of different DSSC based on metal free dyes. and purified betanin (Al-Alwani et al., 2016). Orona et al. using cochi­
S. Dye λmax PCE Jsc Voc FF Reference neal, papaya peel and the microalga Scenedesmus obliquus as a natural
No. (nm) (%) (mA/ (V) dye, and obtained efficiency of 0.228, 0.093 and 0.064% respectively.
cm2) Cocktails of these three dyes were used to achieve 0.36% efficiency for
1 C275 545 12.5 17.03 0.95 0.77 (Yao et al., DSSC (Orona-Navar et al., 2020). Bashar et al. used extracted red dye
2015) and green dye from beetroot and spinach respectively in DSSC to yield
2 SM315 440, 13.0 18.1 0.91 0.78 (Mathew low efficiency of 0.56% (beetroot) and 0.49% (spinach). Blend of red
454, et al., 2014)
581,
and green dyes have shown better results 0.99% than that of the indi­
668 vidual red and green dyes (Bashar et al., 2019). Narayan et al. used
3 ADEKA-1 ~515 12.5 15.67 1.03 0.77 (Kakiage flavonoid from Allamanda cathartic, Bougainvillea spectabilis and
et al., Cosmos sulphurous as a sensitizer and presented the efficiency of 0.40%,
2015b)
0.54% and 0.38% respectively (Narayan and Raturi, 2011). Akin et al.
4 LEG41 – 14.3 18.27 1.01 0.77 (Kakiage
ADEKA-1 et al., extracted nine different natural dyes from various plants and reported
2015a) that them dye extracted from red cabbage (long-hydroxyl & carbonyl-
5 Y123 – 10.3 13.61 1.06 0.69 (Ahmad chain bearing anthocyanin) showed higher PCE of 1.87% (Akın et al.,
et al., 2012) 2016).
6 C219 521 10.10 17.94 0.77 0.73 (Zeng et al.,
2010)
DPS is the main component of DSSC because synthesis process, cost
7 RK1 364, 10.20 18.26 0.76 0.74 (Joly et al., of material, degradation with time etc. of dye are the key factors for the
471 2015) efficient DSSC. Recent research of metal complex based dye, metal free
8 RK2 371, 8.71 14.92 0.75 0.78 (Joly et al., dye and natural dye have been discussed and compared to understand
472 2015)
the chemical structure, chemical design strategy and proper selection of
dye. Several natural dyes are summarised and in most of these natural
units electron acceptor moiety presented outstanding intramolecular dyes, anthocyanin pigments are present in a higher proportion, with
charge splitting via its near planar electronic structure and achieved better yields and higher stability, and thus become a viable choice for
12% efficiency (Ren et al., 2016). Hanya et al. had done remarkable research. For a successful DPS in DSSC some criteria should be followed
work by altering the anchoring group from carboxylic to silyl-anchoring as:
(Kakiage et al., 2013; Kakiage et al., 2014) and achieved 12.8% effi­
ciency with cosensitization of ADEKA-1 dye and coumarine dye SFD-5 1. Wide visible spectrum that absorbs all wavelengths of sunlight.
(Kakiage et al., 2015b). Later on highest PCE of 14.3% was obtained 2. For the smooth electron injection, the LUMO of dye must be higher
by cosensitization of organic dye LEG4 and ADEKA-1 dye and ADEKA-1 than the CB of MOS.
dye system (Kakiage et al., 2015a). 3. The dye molecule must be compact since the bulky molecule will
The YD2 dye was altered by Gratzel and team, who achieved a contribute to a lower optical cross-section.
conversion efficiency of around 10.9% (Bessho et al., 2010). In 2011, 4. Optimal viscosity of dye to allow dye regeneration.
DSSC based on the YD2-o-C8 dye fabricated by a group of scientists in 5. Adsorption coefficient should be high so that dye molecules can
which the zinc atom was enclosed by a ring-shaped molecule called easily and fast adsorb on the surface of MOS.
porphyrin, produced a PCE of around 12.3% (Yella et al., 2011). Mathew 6. High coefficient of molar extinction to facilitate high adsorption of
et al. reported 13% efficiency with SM315 a molecularly engineered dye.
porphyrin dye is better compatible with electrolyte and enhances the 7. Rapid dye regeneration to prevent the recombination of electrons
light harvesting ability (Mathew et al., 2014). and high dye stability at all temperatures.
8. Separate the MOS layer from electrolyte.
6.3.3. Natural dye
The concept of natural pigments based DSSC has been created 6.4. Electrolyte
through a biomimetic approach (Hug et al., 2014). In this method,
various pigments are extracted from environment such as fruits, flowers The electrolytes are liable for (i) dye regeneration (ii) transfer of
and leaves, and used as sensitizers for the processing of DSSCs. Natural charge between the photoanode and CE of the DSSC. Electrolytes are
colourants are pigmentary molecules and dyes that are mainly obtained classified as liquid, quasi-solid, and solid-state. The different categories
from plants with or without chemical treatments. of the electrolytes developed for DSSCs are shown in Fig. 18 and, their
In DSSCs, various natural dyes are being used as sensitizers advantages and disadvantages are displayed in Table 9. The efficiencies
comprising anthocyanin (Pramananda et al., 2021; Chang et al., 2010; recorded for different DSSCs using various electrolytes are summarized
Richhariya et al., 2017), chlorophylls (Hao et al., 2006; Syafinar et al., in Table 10. The DSSCs with liquid electrolytes report the best conver­
2015), carotenoids (Liang et al., 2007; Rühle et al., 2010; Hemalatha sion efficiency till date reaching greater than 14% (Kakiage et al.,
et al., 2012), flavonoids (Rühle et al., 2010; Sinha et al., 2012; Maurya 2015a). There are various redox couples efficiently used in the liquid
et al., 2016), cyanines (Furukawa et al., 2009; Ghann et al., 2017) and electrolyte based DSSC (Mariotti et al., 2020). The first successful DSSC
tannins (Kamel et al., 2005). Natural colours are easily derived from was made with a liquid electrolyte (iodide/triiodide redox couple and
seeds, which means that they are low in cost, widely accessible and do organic solvent) and achieved PCE above 7% (O’regan and Grätzel,
not involve complicated synthesis methods. The use of natural colours is 1991). There were no extra additives in this electrolyte solution. Komiya
therefore important for the development of inexpensive and commer­ et al. also used iodide/triiodide redox couple to obtain remarkable ef­
cially available DSSCs. The moderate PCEs have been reported by nat­ ficiency of 11.9% (Hishikawa et al., 2012).
ural colors and maximum have PCEs below 2% (Al-Alwani et al., 2016, Nusbaumer et al. introduced the first complexes of cobalt as a redox
Amogne et al., 2020, Błaszczyk et al., 2021). Several natural dyes have mediator (Nusbaumer et al., 2001). Later, Sapp et al. explored the cobalt
been studied and are shown in Table 8. Fig. 17 shows the chemical complexes and developed the bipyridine, terpyridine and phenanthro­
structure of various natural dyes. line ligands (Sapp et al., 2002). In 2010, Feldt et al. used cobalt trisbi­
Purified betalain and chemically modified chlorophyll have PCE of pyridine [Co(bpy)3]2+/3+ as an alternative redox mediator to
3% and 6.5% were obtained respectively. Further, 9.5% efficiency was manufacture high-efficiency DSSCs with the organic dyes D29 and D35
(Feldt et al., 2010). In 2011, Cobalt complexes gained considerable

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A. Agrawal et al.
Fig. 15. Chemical structure of various metal free based dye (Al-Alwani et al., 2016; Jiang et al., 2019).
recognition because [Co(bpy)3]2+/3+ electrolyte with zinc porphyrin
sensitizer (YD2-o-C8) obtained PCE of greater than 12%. Nazeeruddin
et al. replaced the I−3 /I− redox couple with [Co(bpy-pz)2]2+/3+ in
conjunction with organic dye Y123 and exhibits better results (Yum
et al., 2012). Then, Co2+/3+ redox couple with SM315 achieved 13%
efficiency (Mathew et al., 2014). Later on, [Co(bpy)3]2+/3+ redox couple
obtained record breaking PCE of 14.3% at AM 1.5 sunlight irradiation
with cosensitization of ADEKA-1 + LEG4 dye (Kakiage et al., 2015a).
Fukuzumi and his team given a new series of copper complexes as a
redox mediator for DSSC ([Cu(SP)(mmt)]0/− , [Cu(dmp)2]2+/+, and [Cu
(phen)2]2+/+) in year 2005. Initially the efficiency with the copper redox
mediator and N3 dye was low due to slow rate of dye regeneration by
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Solar Energy 233 (2022) 378–407
electrolyte (Hattori et al., 2005). PCE of 2.2% using [Cu(dmp)2]2+/+ was
attained under the 20 mW/cm2 solar irradiance. Peng Wang et al. used
[Cu(dmp)2]2+/+ as redox mediator and able to reach PCE of 7% with
organic dye C218 (Bai et al., 2011). But the FF was poor due to slow
charge-transfer rates of electrolyte. There is improvement in [Cu
(dmp)2]2+/+ based DSSC efficiency upto 8.3% with LEG4 sensitizer
(Freitag et al., 2016)). Likewise, the same group was able to boost the
efficiency around 10.0% and 10.3% by [Cu(dmby)2]1+/2+ and [Cu
(tmby)2]1+/2+ based electrolyte in conjugation with organic dye Y123
(Saygili et al., 2016). Again Freitag et al. reached 11.3% efficiency with
Cu(tmby)22+/+ under standard AM 1.5G sunlight. And also reported
28.9% (power output of 88.5 µW/cm− 2) efficiency under 1,000 lx the
A. Agrawal et al. Solar Energy 233 (2022) 378–407

Fig. 15. (continued).

performance and stability of the DSSC (Saygili et al., 2016).

Cao et al. presented first thermoplastic polymer electrolytes (type of
quasi-solid) based DSSCs (Cao et al., 1995). It comprises a mixture of
PAN polymer, NaI, I2, ACN as the solvent and other additives. This cell
exhibited 3–5% PCE under full sunlight illumination. Shi et al. used a
PEO polymer to convert the liquid electrolyte into gel and achieved an
efficiency of 6.12% (Shi et al., 2009). It was observed that PEO enhance
Li+ mobility which minimized internal resistance of the cell. The PVDF-
HFP polymer was mixed with I− /I−3 redox couple and produced 10.37%
efficiency better than liquid electrolyte efficiency (9.89%) measured
under 100 mW/cm− 2 irradiation (Hwang et al., 2017). The first example
of a thermosetting polymer electrolyte produced 2.62% efficiency with
α-methacryloyl-ω-methocyocta (oxythylene) polymer matrix and liquid
electrolyte on TiO2 mesoporous layer (Matsumoto et al., 2001). Park
Fig. 16. Organic dye D–π–A molecular structure.
et al. prepared polymer film by the use of MMA and HDDA on the TiO2
film and cell showed 10.6% efficiency (Park et al., 2013). BEMA and
PEGMA type of thermosetting polymer electrolyte mixed with cobalt
indoor illumination (Freitag et al., 2017). Another redox mediator,
mediator reached the PCE of 6.4% (Bella et al., 2015). The TEMPO
ferrocene/ferrocenium Fc0/1+ also attained effective PCE of ̴ 7.5% under
polymer was applied in a liquid electrolyte by Nishide et al. PCE of
1 sun illumination with a Carbz-PAHTDTT (metal free organic sensi­
10.1% was obtained with indoline dye (Suzuka et al., 2016).
tizer) (Daeneke et al., 2011). The major drawback of liquid electrolytes
Croce et al. introduced first composite polymer electrolyte that
is the leakage from the cell’s outer boundary, which reduces the
contains TiO2 and Al2O3 nanoparticles mixed with PEO-LiCLO4 (Croce

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Table 8
Natural sensitizers used in DSSCs with relevant PV parameters.
S. Dye Plant λmax PCE Jsc (mA/ Voc FF Reference
No. (nm) (%) cm2) (V)

1 Betanin beets – 3 14 0.375 – (Treat et al., 2016)

2 Betanin beets 535 2.71 13.91 0.36 0.56 (Sandquist and Mchale,
2011)
3 Chlorophyll Spinach (leaves) 655 3.4 10.6 0.54 0.6 (Wang et al., 2006)
4 Chlorophyll a 675 6.5 14.9 0.61 0.72 (Tamiaki et al., 2018)
5 Betalain Prickly pear (fruit) 450 2.06 8.8 0.389 0.6 (Calogero et al., 2012)
6 Betalain Pokeweed (stalk) 539 3.04 9.08 0.632 0.53 (Güzel et al., 2018)
7 Anthocyanin Ixora sp. (Rubiaceae) (Flower) ~540 0.96 6.26 0.35 0.47 (Kumara et al., 2013)
8 Anthocyanin Hibiscus rosa-sinensis (Flower) ~540 1.08 3.31 0.145 0.55 (Yusoff et al., 2014)
9 Cyanidin and Malvidin derivatives Ixora sp. (Rubiaceae) ~540 0.95 3.39 0.49 0.58 (Kumara et al., 2015)
10 Xanthophyll Marigold (Flower) 487 0.23 0.51 0.54 0.83 (Zhou et al., 2011b)
11 Betacyanin Purified Red Bougainvillea Glabra 481, 535 0.49 2.33 0.26 0.79 (Hernandez-Martinez et al.,
(Flower) 2011)
12 Flavonoid Tangerine peel (Fruit) 446 0.28 0.74 0.59 0.63 (Zhou et al., 2011b)
13 Carotene Fructus lycii[fruits 425, 447 0.17 0.53 0.68 0.46 (Zhou et al., 2011b)
14 – Neem (leave) – 2.81 15.10 0.54 0.35 (Sahare et al., 2015)
15 Chlorophyll Punica granatum (Pomegranate) 412, 665 0.597 2.05 0.56 0.52 (Chang and Lo, 2010)
(leave)
16 Chlorophyll, carotenoids or Ficus reusa (leave) ̴425, 1.18 7.85 0.52 0.29 (Lai et al., 2008)
phycobiliproteins ~670
17 Chlorophyll/lutein Spinach Modified (leave) – 4.0 12.5 0.54 0.59 (Wang et al., 2006)
18 Anthocyanin Celosia Cristata 510 1.38 4.82 0.52 0.55 (Hosseinnezhad et al., 2018)
19 Flavonoid Saffron petals 468 0.52 2.77 0.36 0.52 (Hosseinnezhad et al., 2018)
20 Anthocyanin Cynoglossum 573 1.12 4.11 0.48 0.57 (Hosseinnezhad et al., 2018)
21 Anthocyanin Red cabbage 478 1.87 1.88 0.54 0.56 (Akın et al., 2016)

et al., 1998). Wang et al. employed P(VA-co-MMA) (polymer electro­ 6. Should be easily dissolved to provide high concentration of charge
lyte) with I− /I−3 redox couple mix in organic solvent ACN and MPN carriers in the electrolyte, resulting in necessary availability of redox
(Wang et al., 2013a). The addition of a TiO2 nanofiller in ACN and MPN couple needed for dye regeneration.
enhanced the PCE from 9.10% to 9.40% and 8.61% to 8.98% 7. It must be chemically stable with all components of electrolyte and
respectively. smoothly operated under expected conditions.
Solid state electrolyte based DSSC also performed well as compared
to other types of electrolyte based DSSC. For example, CuSCN thin film
6.5. Counter electrode
as a hole transport material (HTM) based DSSC showed PCE of 5.1%
(Chappaz-Gillot et al., 2014). PCE of 4.7% was achieved with Cs2SnI6 in
Counter electrode (CE) captures the electron from an outer circuit
combination with Z907 sensitizer, and 8% efficiency with use of other
and aims to regenerate the dye by reduction and oxidation of electrolyte
sensitizers such as YD2-o-C8, N719 and RLC5 (Lee et al., 2014a). In
that substantially influences the overall PCE of DSSC. There are various
2017, Chevrier et al. integrating P3HT and spiro-OMeTAD with organic
materials and methods for the preparation and deposition of CE in DSSC.
dye (D102) and, PCE of 4.78% and 3.99% was achieved respectively
A few examples of CE materials are carbon black, CoNi2S4, platinum
(Chevrier et al., 2017). Later, spiro-OMeTAD based DSSC achieved 7.2%
(Pt), activated carbon, graphite, polyaniline, PEDOT, polypyrrole, and
and 7.7% efficiency (Burschka et al., 2011; Xu et al., 2015). In contrast,
carbon nanosheets that can be used as catalysts for the electrolyte
PEDOT also obtained good PCE of 7.1% (Zhang et al., 2016). Electro­
reduction (Chen et al., 2009b; Choi et al., 2011; Ellis et al., 2013; Bu
deposited PEDOT with Y123 dye and Cu (tmby)22+/+ showed a PCE of
et al., 2013; Shi et al., 2015; Chen et al., 2016). Pt has been considered as
11.0% (Cao et al., 2017).
the most appropriate material for the CE so far. The Pt can be coated
In short, the smooth working and long life of solar cell depends upon
onto the TCO substrate by screen-printing, sputtering, vapour deposi­
the nature of electrolyte. By incorporating polymer electrolytes into
tion, electro-deposition and pyrolysis etc. The Pt coated TCO substrate
DSSC, the stability of the system may be improved without compro­
shows (i) strong electrocatalytic action which enhances the electrolyte
mising its performance. Therefore, quasi solid and solid electrolyte are
reduction by promoting electron exchange (ii) high reflection of light
the future of electrolyte. We provide a detailed analysis of the progress
due to shiny surface of Pt; therefore improving the light-harvesting ef­
in the development and use of electrolytes for DSSCs, ranging from
ficiency of the cell (Papageorgiou et al., 1997; Lee et al., 2010). Pt based
liquid electrolytes to quasi solid and solid electrolytes. Some recently
CE is not suitable for commercial production of DSSC because of limited
discovered electrolyte materials are discussed, and the composition of
availability of Pt due to its high price and scarcity. To overcome these
electrolytes in various DSSC device designs with their PCE, VOC, and JSC
problems researches are designing new Pt-free CE which is suitable for
are critically assessed. Therefore for DSSCs to work efficiently, the redox
mass production. Table 11 shows some Pt-free CE for DSSC with their PV
mediator must meet the following requirements:
parameters.
Guo et al. presented In2.77S4 conductive carbon based CE by two-step
1. Absorption of light in visible spectrum should be minimal for elec­
synthesis method and reported 8.71% PCE which is equivalent to the
trolyte to prevent the dye absorption losses.
8.75% PCE of conventional Pt based DSSC (Guo et al., 2017). Lin et al.
2. It should be chemically inert and not react with the photoanode or
reported nano-structured vertically aligned MoS2/CNT based CE with
dye.
PCE of 7.83% which is better than Pt based CE (7.15%) (Lin et al., 2017).
3. To maximizes the voltage of cell, redox pair potential needs to be
Mengal et al. improved the efficiency from 4.18% to 6.2% with new
even lower as compared to potential of dye reversible.
cationized graphite CE (Mengal et al., 2018). Miao et al. exhibited
4. Solvent used in the electrolyte should have high diffusion coefficients
excellent catalytic activity of graphene with carbon black thus leading to
to promote effective transportation of mass.
high PCE of 5.99% (Miao et al., 2013).
5. Use non-toxic and easily accessible elements.
Ma et al. prepared flexible ITO@PEN deposited PEDOT By

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Fig. 17. Chemical structure of various natural based dye (Semalti and Sharma, 2020; Kumara et al., 2017).
electrochemical deposition process for 40 sec, 80 sec, 120 sec, and 160
sec. They found that 80sec deposited PEDOT based CE showed PCE of
7.18% (Ma et al., 2018). Lee et al. demonstrated the PCE of 7.36% with
composite of graphene dot and PEDOT:PSS CE which is close to PCE of
8.46% (Pt based CE) (Lee et al., 2017a). By an electrochemical poly­
merization process Shih et al. synthesized conductive composite of
PANI/graphene nanoplates/MWCNT. They showed almost similar PCE
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Solar Energy 233 (2022) 378–407
of 7.67% (PANI/GNP/ MWCNT) than Pt based CE (7.62 %) (Shih et al.,
2017). Li et al. synthesized Pt-free CE by mixing conducting polymers
such as PANI, PPy, and PEDOT in reduce graphene oxide. They obtained
PCE of 4.41% for rGO/PPy, 2.93% for rGO/PANI, 2.05% for rGO/
PEDOT with PEN substrate (Li et al., 2016b).
Tsai et al. reported PCE of 2.73% and 3.04% with CE CuO and CuO/
Graphene nanostructured respectively (Tsai et al., 2018)). Du et al.
A. Agrawal et al. Solar Energy 233 (2022) 378–407

Table 9
Advantages and disadvantages of different electrolytes with their composition
structure and solvents.
Liquid Quasi Solid

Advantages • simple • very good ionic • no leakage

preparation conductivity, problem from
methods, • good chemical and the outer
• low viscosity, mechanical stability, boundary of
• high PCE, • excellent properties cell,
• excellent to make bond with • they do not
connectivity MOS, contain any
interaction at • high viscosity, solvents that
the electrode/ compatible for roll- make them
electrolyte to-roll deposition suitable for
interface, methods, large-area ap­
• high • low solvent plications etc.
conductivity volatility, feasible to
etc. low cost
manufacturing of
DSSC modules etc.
Disadvantages • due to leakage • low PCE as compared • low PCE as
Fig. 18. Various types of electrolytes used in DSSCs.
from to liquid based compared to
• the cell DSSCs, liquid based
prepared NiCo2O4 ternary oxide as CE with various nano-structure such assembly • less stable, DSSCs. Low
which reduces • leakage problem etc. long-term
as nanorods, nanosheets, and nanofibres. Among all nano-structure,
the stability,
NiCo2O4 nanofibers demonstrated the PCE of 8.48%, which is greater performance, • they cannot
than PCE of Pt based CE (8.11%) (Du et al., 2017). Ahmad et al. • complex form proper
exhibited the PCE of 4.1% with synthesized multiporous α-MnO2 redox bonds with
nanorod as CE in DSSC (Ahmad et al., 2017a). Wang et al. and Hou et al. chemistry the MOS
corrosive pores etc.
achieved PCE of 8.17% and 6.96% zinc oxide and α-Fe2O3 as a CE
nature etc.
respectively (Wang et al., 2013c; Hou et al., 2013). Composition Redox couple + Polymer material + HTM +
Jiang et al. synthesized Co3S4 nanosheets on reduced graphene oxide Structure solvent + Redox couple + solvent additives
surface and obtained a significant efficiency of 7.13% and 8.08% with additives + additives
Redox couple- Polymer- poly
Co3S4 nanosheets and by adding reduce graphene oxide in Co3S4
Iodine, Cobalt, (vinylidene fluoride)
nanosheets respectively (Jiang et al., 2018). Wang et al. were fabricated Copper, Nickel, (PVDF), poly
CoS/MoS2 nanosphere and reported PCE of 7.48% which is equivalent to Ferrocenium, (acrylonitrile) (PAN)),
PCE of Pt based CE (7.51%) (Wang et al., 2018). Yue et al. and Liu et al. poly(ethylene oxide)
were synthesized CNTs/VS2 and CuMnSnS4)/carbon nanotube counter (PEO), Poly(propylene
oxide) (PPO), Poly
electrodes having 0.05 g CNTs in both and exhibited the PCE of 7.72%
(vinyl pyrrolidone)
and 8.97%, respectively (Yue et al., 2017; Liu et al., 2017b). Zhang et al. (PVP), Poly(methyl
obtained p-type semiconductor FeS from n-type α-Fe2O3 through sulfu­ methacrylate) (PMMA),
rization process. This process shows enhancement of PCE from 3.79% to Poly(vinylidene
6.47%, which is equivalent to the Pt based CE (7.05%) (Zhang et al., fluoride-
hexafluoropropylene)
2017). Chen et al. deposited a composite of metal–organic framework by (PVDF-HFP)
conductive binder sulfonated poly (thiophene-3-[2-(2-methoxy ethoxy)- Solvent and Additives- Acetonitrile (ACN),
ethoxy]-2, 5-diyl) on carbon cloth substrate. They reported PCE of methoxyacetontrile (MAN) and 3-methoxy­
8.91% which is higher than the PCE of 8.21% (Pt-based CE) (Chen et al., propionitrile (MPN), ethylene carbonate
(EC), propylene carbonate (PC), Ƴ-
2017).
butyrolactone (GBL), and N-methyl-2-
A flexible CE of Pt/carbon sphere composite was fabricated by Zhu pyrrolidone (NMP), N-methyloxazolidinone
et al. and obtained PCE of 9.02% (Zhu et al., 2017). Li et al. prepared (NMO), Diethyl carbonate (DEC),
various composites of silicon (Si3N4, SiO2, SiS2, and SiSe2) with Propionitrile (PPN), 1-ethyl-3-methylimida­
PEDOT:PSS for the application CE in DSSC. They presented PCE of 8.2% zolium selenocyanate (EMImSeCN),
ammonium, guanidinium, phosphonium,
with SiS2/PEDOT:PSS composite which is comparable to 8.5% PCE (Pt pyridinium, and sulfonium, .PMImI,, DMII,
based CE) (Li et al., 2016a). Lan et al. synthesized Pt/NiO nano sheet and BMII, PMII, TPAA, TEMPO
achieved PCE of 8.40% as CE in DSSC which is similar to PCE of 9.15%
(Pt based CE). The PCE of cell improved 8.40% to 11.27% when placed
on Ag mirror (Lan et al., 2016). Hou et al. achieved PCE of 9.82% from a sulfide, metal oxide and carbon materials with their PV parameters are
transparent nanostructured CE based on cobalt sulfide/reduced gra­ presented and discussed. Designing new concepts, applying new
phene oxide (Huo et al., 2016). Rafique et al. obtained 7.1% efficiency methods, and exploring novel materials should be the emphasis of future
with Cu-PPy-FWCNTS (copper polypyyrol functionalized multiwall progress. Therefore, CE should have following characteristics for the
carbon nanotubes) nanocomposite, which is better than Pt based DSSC efficient DSSC:
(6.4%) (Rafique et al., 2021). Zhang et al. prepared transparent one step
PW11Co-n/Co0.85Se (polyoxometalates) based CE and PCE of 7.56% was 1. High conductivity so that fast redox reaction occurs which enhances
achieved (Zhang et al., 2021). the stability and avoiding the recapture of electron.
The interface between the electrolyte and the TCO electrode, i.e., CE, 2. High electron mobility allows for fast electrolyte regeneration thus
is an important aspect of the DSSC. Therefore, the CE is an essential minimizing electron recombination.
element that has a substantial impact on DSSC PV performance as well as 3. High stability towards the electrolyte’s corrosive properties.
device cost. An alternative for Pt based CEs such as polymers, metal 4. Chemically inert, which means it won’t react with the dye or MOS.
5. Low electrical resistance and high electrocatalytic action.

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A. Agrawal et al. Solar Energy 233 (2022) 378–407

Table 10
Efficiency of DSSCs employing different electrolytes with their solvent.
State Electrolyte composition Dye PCE (%) Reference
2+/3+
Liquid [Co(phen)3] + ACN ADEKA + LEG4 14.3 (Kakiage et al., 2015a)
[Co(bpy)3]2+/3+ + ACN SM315 13.0 (Mathew et al., 2014)
2+/1+
[Cu(tmby)2] + ACN D35 + XY1 11.3 (Freitag et al., 2017)
I− /I−3 + ACN + VN + PMII + TBP Z-910 10.2 (Wang et al., 2004a)
I− /I−3 + DMII + NBB + GuNCS + MPN C103 9.60 (Shi et al., 2008)
Co((MeIm-Bpy)PF6)3]2+ + NOBF4 + GuNCS + TBP + PMII/ N719 7.37 (Xu et al., 2013)
EMINCS
I− /I−3 + NMBI + GuSCN + PMImI/EMImSCN K19 7.05 (Fabregat-Santiago et al., 2007)
Quasi solid TEMPO + PVDF-HFP + MPN MD-153 10.10 (Suzuka et al., 2016)
I− /I−3 + PEO + PVDF + MPN N719 8.32 (Liu et al., 2017a)
I− /I−3 + PVA-co-MMA + ACN N719 9.10 (Wang et al., 2013a)
[Co(bpy)3]2+/3+ + BEMA-PEGMA LEG4 6.40 (Bella and Bongiovanni, 2013)
I− /I−3 + PEO + PVDF + TiO2 N719 8.91 (Liu et al., 2017a)
I− /I−3 + PAA + PEG + PEDOT-graphene N719 8.20 (Li et al., 2018)
I− /I−3 + Phtaloychitosan + PEO + TPAI + BMII N3 9.61 (Buraidah et al., 2017)
I− /I−3 + Hydrotalcite nanoclay + PMII N719 N/A 9.60 (Wang et al., 2013d)
SeCN− /SeCN−3 + POEI-IS TA 8.18 (Lin et al., 2016)
Succinonitrile + DMPII N719 7.80 (Hwang et al., 2013)
Solid state I− /I−3 + MPII + NMBI + LiI MK2 7.45 (Li et al., 2014a)
[Cu(tmby)2](TFSI)2 Y123 11.0 (Cao et al., 2017)
Fluorine doped CsSnI3 + SnF2 N719 8.5 (Lee et al., 2012)
Spiro-OMeTAD AQ310 8.0 (Li et al., 2017b)
Spiro-OMeTAD + TeCA LEG4 7.7 (Xu et al., 2015)
PEDOT with OM-TiO2 N719 6.8 (Kim et al., 2011)
For Natural Dyes I− /I−3 + KI + ethylene carbonate + acetonitrile Crocetin (Gardenia fruit) 0.56 (Yamazaki et al., 2007)
I− /I−3 + KI + water free ethylene glycol Rosella (Anthocyanin) 0.37 (Wongcharee et al., 2007)
I− /I−3 + LiI + DMII + GuSCN + TBP + ACN Mangosteen pericarp (Anthocyanin) 1.17 (Zhou et al., 2011b)
I− /I−3 + BMII + GuSCN + TBP + ACN + VN Red cabbage in addition with 0.516 (San Esteban and Enriquez,
graphene 2013)

6.6. Sealing material 7. Commercialization growth

DSSCs are required to be sealed using sealing materials. Most of the
researchers prefer to fabricate DSSCs by directly sandwiching together
two electrodes, one with MOS electrode and other with CE, by a ther­
momelt polymer that also serves as a gasket to retain the electrolyte. To
melt the polymer, optimal temperature and pressure are given to seal the
DSSC. Surlyn, an ethylene and methacrylic acid copolymer, is the most
commonly used polymer. Surlyn is the marketing term for a group of
ionomer resins that are commonly used in general packaging materials
and lamination. Importantly, it allows DSSC devices to be sealed quickly
and at lower temperature (120 ◦ C). Surlyn’s permeability to oxygen and
humidity is considered to be greater at temperatures above 60 ◦ C
(Hinsch et al., 2001). Several experiments also employ “Bynel,” an ad­
hesive resin with a higher melting temperature (190 ◦ C) and better
longevity (Ito et al., 2013). Glass frit sealing, which efficiently encap­
sulates the cell by melting the glass together, has been used for sealing
the gasket for even greater durability (Sommeling et al., 2004).
Aluminum foil laminated with polymer foil (Burnside et al., 2000),
epoxy glue (Grünwald and Tributsch, 1997) and the vacuum sealant
Torr Seal (Smestad et al., 2003) have also been used to seal DSSCs.
Overall, sealing of DSSC is a major technical obstacle for DSSC tech­
nology and directly linked solar cell long-term stability. Therefore
sealing material should have following characteristics:-
(i) Thermally stable at high temperatures to avoid leakage of
electrolyte
(ii) Chemically inert to the liquid redox couple presented in the
electrolyte to prevent corrosion
(iii) Suitable for large scale production.
(iv) Highly durable against water vapours and oxygen.
In 2014, the global market size of the DSSC technology was valued
approximately $49.6 million and it is expected to expand at a compound
annual increase of more than 12% between 2015 and 2022 (Trancik,
2006; Campillo and Foster, 2003). The global demand for DSSC is
heavily influenced by module/cell production costs and related eco­
nomics. Kalowekamo et al. estimated the manufacturing expense of
DSSC and compared it to the two generations of solar cells (Kalowekamo
and Baker, 2009). The price of DSSC is expected to be between 0.5$/W
to 1$/W for an efficiency 5% to 15%. The DSSC generates electricity at a
lower cost than the Organic solar cell, Si and amorphous Si solar cell,
perovskite solar cell (Fakharuddin et al., 2014). Several commercial
enterprises from different countries have arisen to develop this solar
technology such as 3G Solar, Solaronix, Dyesol, SHARP, Konarka, G24
Power, and Dynamo etc. from Israel, Switzerland, Australia, Japan, USA,
United Kingdom and Sweden respectively (Fakharuddin et al., 2014).
Portable solar charging unit, which was attached to backpacks, was
probably the first commercial use of DSSC devices (Duarte et al., 2012).
According to market report of 2014, portable charging unit was the most
popular application segment according to business survey of 2014 and
accounted for 33.0% of revenue share and is projected to expand. This is
due to its potential to deliver optimum energy in indoor light environ­
ment, making it appropriate for portable electronic devices (Campillo
and Foster, 2003). Recently, a portable solar powered keyboard was
shown that does not require a battery therefore it save time and cost of
battery. However, the main purpose of this technology will be to
incorporate PV into buildings (Building Integrated PV/ Building Applied
PV). Building Integrated PV/ Building Applied PV is projected to
accelerate with a net worth of more than $30 million in upcoming years
(Matiko et al., 2013). The demand for electricity consumption for resi­
dential areas, such as roof-top panels and water heating is expected to
boost market development of DSSC technology (Nielsen et al., (2010).
Building Integrated PV/ Building Applied PV, automotive, portable

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A. Agrawal et al. Solar Energy 233 (2022) 378–407

Table 11
Summary of some relevant CE in DSSC with PV parameter.
Counter Counter PCE JSC VOC FF Reference
electrode electrode (%) (mA/ (V)
material cm2)

Carbon Graphene/ 5.99 15.07 0.70 0.57 (Miao

based carbon black et al.,
C25G 2013)
In2.77S4 8.11 17.34 0.75 0.67 (Guo et al.,
2017)
MoS2/CNTs 7.83 16.65 0.74 0.66 (Lin et al.,
2017)
Si@G10% 6.42 16.63 0.706 0.546 (Mengal
et al.,
2018)
Conductive rGO/PPy– 4.41 14.2 0.589 0.527 (Li et al.,
polymer 2016b)
based PEDOT-80 s 7.18 14.17 0.788 0.64 (Ma et al.,
2018)
30 vol% 7.36 14.70 0.718 0.70 (Lee et al.,
GDS/ 2017a)
PEDOT-PSS
PANI-G1C2 7.67 18.21 0.780 0.54 (Shih
et al.,
2017)
Metal oxide ZnO/ 8.17 19.71 0.862 0.48 (Wang
based Polymer et al.,
(32:1) 2013c)
α-Fe2O3 6.96 15.92 0.784 0.56 (Hou et al.,
2013) Fig. 19. Future perspective for efficient DSSC.
NiCo2O4-NF 8.48 17.01 0.770 0.64 (Du et al.,
2017)
α-MnO2 4.10 14.70 0.655 0.38 (Ahmad 8. Conclusion and recommendation
Nano-rods et al.,
2017a) PV devices transform solar energy directly into electrical energy
CuO + GNs 3.40 15.62 0.690 0.31 (Tsai et al.,
without polluting the environment. In the last two decades, DSSC has
2018)
Metal CNTs/VS2 8.02 15.57 0.75 0.68 (Yue et al.,
become a topic of considerable research due to its fundamental and
sulfide 2017) scientific significance in the field of energy conversion. Although its
based CuMnSnS4 8.97 16.52 0.75 0.72 (Liu et al., efficiency is low as compared to other solar cells but the ability to
0.05 g CNTs 2017b) operate in several lighting situations, compatible with flexible substrate,
FeS 6.47 14.00 0.66 0.63 (Zhang
degrees of transparency, variety of colours offer DSSC a suitable choice
et al.,
2017) over its competitors. In this review, various materials utilized in DSSCs
MOF-525/S- 8.91 16.14 0.80 0.70 (Chen from photoanodes to CEs were summarized, including different MOSs,
Pt et al., electrolytes, CEs configuration, sealing materials, and DPSs. The oper­
2017)
ational mechanism along with their equations which is responsible for
CO3S4 8.08 15.70 0.75 0.67 (Jiang
nanosheet/ et al.,
the conversion of solar radiation into electrical energy and the reasons
rGO 2018) for the inhibition of cell operation were demonstrated. Various strate­
CoS/MoS2 7.48 16.50 0.74 0.61 (Wang gies to improve the performance of MOS such as nanostructures, addi­
et al., tion of metal oxide layer, and doping of anion, cation and plasmonic
2018)
metal were described. The properties and progress of three types of DPSs
Composite Transparent 9.82 18.9 0.767 0.67 (Huo et al.,
based CoS/rGO 2016) such as metal-based complex dyes, metal-free organic dyes and natural
Fe3O4@rGO- 9.04 17.01 0.760 0.71 (Zhou dye, and the advantages and disadvantages of the sensitizers for DSSCs
NMCC et al., were discussed in detail. Overview of recent trends in research on
2016) electrolytes for DSSCs, highlight the electrolyte compositions and limi­
Pt/NiO/Ag 11.27 30.1 0.810 0.462 (Lan et al.,
mirror 2016)
tation of different types of electrolyte are shown. We have also presented
SiSe2/ 8.2 16.98 0.720 0.67 (Li et al., in encapsulation and sealing of cells which enhances the stability and
PEDOT: PSS 2016a) hence life time of the DSSCs. This paper presents a systematic overview
M-AC/CNT-2 6.26 12.4 0.72 0.71 (Memon of CE in DSSCs with a focus on Pt-TCO free CEs.
PF et al.,
Many issues still require extra attention and collaborative effort. Our
2017)
Pt/CS 9.02 14.24 0.859 0.74 (Zhu et al., suggestions in this respect are as follows: - (i) To increase the absorption
flexible 2017) ability and minimize the recombination process, other strategies may be
Cu-PPy- 7.1 14.17 0.72 0.696 (Rafique explored further such as core shell layer formation at MOS, up and down
FWCNTS et al., conversion material, MOS layer passivation and of surface area modi­
2021)
fication of MOS. (ii) Novel materials like Donor-Acceptor-Acceptor DPS
configuration, hybrid perovskite DPS and amphiphilic DPS can be
charging, embedded electronics etc. are the various expected market developed to improve photothermal stability, reduce dye desorption,
segments for the development of DSSC technology (Nazeeruddin et al., and boost absorption ability in the near-infrared range. (iii) Explore or
1993). Therefore, DSSC has been identified as one of the most promising employ less volatile, quasi state and completely solid state electrolytes
technologies for the near future, but there is still need for further with stabilizing compounds. (iv) The manufacturing expenditure of a
progress in order to commercialize it (shown in Fig. 19). DSSC device can be reduced by using noble metal-free based CE and new
structural morphologies of carbon-conducting polymer composite based

399
A. Agrawal et al. Solar Energy 233 (2022) 378–407

CE. (v) Interfacial contact research has received less attention in the Ansari-Rad, M., Abdi, Y., Arzi, E., 2012c. Simulation of non-linear recombination of
charge carriers in sensitized nanocrystalline solar cells. J. Appl. Phys. 112, 074319.
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Anta, J.A., Morales-Flórez, V., 2008. Combined effect of energetic and spatial disorder on
improved by considering the interfacial interactions. (vi) Commercially the trap-limited electron diffusion coefficient of metal–oxide nanostructures. J. Phys.
feasible production technologies like as screen printing, roll to roll Chem. C 112, 10287–10293.
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solar cells of SnO2 surface modified with gold nano particles. Sri Lankan J. Phys. 9.
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can be explored for perfect encapsulation. Approach for High-Efficiency Photoelectrochemical Solar Cells by Using Bifunctional
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comprehensive review. Renewable Sustainable Energy Rev. 129.
Bai, Y., Yu, Q., Cai, N., Wang, Y., Zhang, M., Wang, P., 2011. High-efficiency organic dye-
The authors declare that they have no known competing financial sensitized mesoscopic solar cells with a copper redox shuttle. Chem. Commun. 47,
interests or personal relationships that could have appeared to influence 4376–4378.
the work reported in this paper. Balasingam, S.K., Lee, M., Kang, M.G., Jun, Y., 2013. Improvement of dye-sensitized
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