Inorganic Chemistry Communications 152 (2023) 110638

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Inorganic Chemistry Communications

journal homepage: www.elsevier.com/locate/inoche

Review on the progress of light harvesting natural pigments as DSSC

sensitizers with high potency
Pooja Prakash , B. Janarthanan *
Energy and Nano Research Lab, Department of Physics, Karpagam Academy of Higher Education, Eachanari Post, Pollachi Main Road, Coimbatore 641 021, Tamil
Nadu, India

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

Keywords: The generation of clean energy is one of the most pressing concerns in the upcoming future, due to the subse­
Conventional energy resources quent growing population and energy demand. For the past two decades, dye-sensitized solar cells serves as the
DSSC rudiment in the field of energy conversion. Ease availability with reasonable fabrication cost coupled with
Photosensitizers
effective efficiency and endless energy made DSSC a feasible candidate in the area of research. In this review
Derivatives
Absorption Spectra
article, the structure, primary function, key elements of DSSC, and performance parameters are observed along
Conversion efficiency with a focus on the potent photosensitizers due to charge production. DSSC fabricated using organic sensitizers
provide high durability and better efficiency even though they were suffering from significant obstacles, such as
poor conversion efficiency, degradation tendency when exposed to sunlight, high cost of fabrication, and toxic
material usage. The contradictory results about DSSC based on natural sensitizers are described according to the
published report, which could help future research. These drawbacks have opened up a bio-compatible sensitizer
that contains natural derivatives such as chlorophyll, anthocyanin, carotenoid, and flavonoid. This alternate
sensitizer was responsible for photon absorption and injection of charge carriers onto the TiO2 conduction band.
Hence, the leaves, flowers, fruits, seeds, etc. act as the source for pigment extraction in the fabrication of DSSC.
This review signifies the recent progress in the development of DSSC using photo-sensitizers viz., natural sen­
sitizers extracted as dyes present in organic plants, flowers, stems, barks, roots, etc. for absorption of solar
radiance in the visible region. Enhancement of photo-conversion efficiency by incorporating the natural dyes has
proven the activity of artificial photosynthesis of DSSC. Remarks of researchers all over the world regarding the
process of cocktailing the natural dyes for DSSC have been taken into account to investigate the challenges faced
in flourishing a radically ideal DSSC. Furthermore, plant-based DSSCs are thought to be the most propitious
sustainable energy resource for semi-arid regions in the future due to the average solar radiation as well as
technological and economic considerations.

1. Introduction challenges faced by today’s world is controlling and ceasing climate

The primary energy sources are coal, petroleum, and natural gas,
which are employed in the manufacturing, transportation, and con­
struction industries [1]. In 2017, according to the IEA, fossil fuels supply
more than 81 percent of world energy needs, which equates to 11,380
million tons of oil [2]. The global energy need is expected to increase by
28% from 2015 to 2040 and one of the major regions would be the
Middle East, with an energy demand growth of 45% [3]. Due to the
expeditious growth of the global population and the immoderate use of
fossil fuels, there has been a notable rise in the consumption of natural
resources over the last several decades [4]. One of the intricate
changes produced by the excessive use of traditional resources [5]. By
2050, 9.3 billion people are expected to inhabit the planet [5]. Thus in
the contemporary scenario, the amelioration of the world’s interest has
been reinforced using solar energy which acts as a reliable alternative
candidate that can satisfy necessitate of the global market [6-9]. Hence
solar energy is considered the most undertaken natural source to
attenuate the shortage of fossil fuels and the emission of greenhouse
gases in the near future [10,11].
Nuclear fuel is another available energy resource to meet the
growing demand. While enhancing the share of nuclear fuel in the global
market, as their trash is radioactive for years, causing major issues for all

* Corresponding author at: Professor and Head, Energy and Nano Research Lab, Department of Physics, Karpagam Academy of Higher Education.
E-mail address: janarthanan.b@kahedu.edu.in (B. Janarthanan).

https://doi.org/10.1016/j.inoche.2023.110638
Received 15 October 2022; Received in revised form 2 March 2023; Accepted 16 March 2023
Available online 20 March 2023
1387-7003/© 2023 Published by Elsevier B.V.
P. Prakash and B. Janarthanan
types of life. Thus across the globe, there are ongoing programs to
minimize the presence of unsustainable energy sources and it is pre­
dicted that the impact of renewable energy raises less serious environ­
mental concerns. Interestingly, the impact of renewable power on world
energy demand will grow from 12.4% in 2015 to 17.4% in 2017 [3]. In
2017, renewable energy sources generated 25% of the world’s elec­
tricity for the first time in recorded history, followed by natural gas at
23%, nuclear gas at 10%, and global oil production at 4% [2]. In the next
two decades, the highest production growth rate will be experienced by
solar and wind power. Although wind power and hydropower are widely
producing a remarkable amount of sustainable renewable energy in
India, there is annual sunshine of 2600 to 3200 h. India receives mor­
e than 300 days of brilliant sunshine annually, with an estimated 600
TW (i.e, 5000 PWh/yr) or about 5000 trillion kWh/yr of solar energy
being received in only its geographic region. Solar power is a promising
source of energy since the sun has provided free energy for thousands of
years when compared to wind/hydropower which is likely to be affected
by dry spells. The two main commercialized solar energy technologies
with comparable economic potential are photovoltaics (PV) and
concentrated solar power (CSP). Despite the fact that CSP appears to be
more favorable in desert regions with high average solar radiation,
photovoltaic power plants are more practical for less wealthy nations,
especially in humid regions, due to their lower investment costs [12].
India stands fourth in the world and third in Asia in terms of global solar
power production. The solar power sector emerged as a notable player
yielding 36,910 MW of solar energy as of November 2020. Today re­
searchers are in pursuit of the utilization of solar irradiation directly into
electricity using photovoltaic cells at economic and domestic levels [9]
and in 2040, solar energy is expected to reach 1.4 TWh [3].
The crystalline Si-based solar cells showed higher efficiency with the
silicon bandgap (1.12 eV) closer to the Shockley-Queisser model of 1.34
eV when compared to other solar cells [11]. However, the high fabri­
cation cost of crystalline Si-based photovoltaic devices and the high
purity of silicon have led researchers to work on alternative solar cell
technologies.
In 1991, a new hope was reported by O’Regan and Gratzel having
unparalleled photocurrent generation through DSSC developed by a
mesoporous TiO2 photoelectrode, a transparent substrate (FTO), potent
sensitizer, robust electrolyte, and a photocathode [13,14]. The fabri­
cated DSSC has a power conversion efficiency that is greater than 7%
and can absorb light up to 800 nm in the visible spectrum. The use of
nanocrystalline semiconductor electrodes in 2011 resulted in an energy
conversion efficiency of 11.4%. Due to its compatibility with architec­
ture and the environment, user-friendly preparation methods, and
effective operation in diffuse lighting, DSSC is an irreplaceable natural
source in the production of energy. Photosensitizers play an imperative
role and are a crucial component of DSSC. Recently Mathew et al. re­
ported the highest efficiency of 13% by employing mesoporous photo
electrodes and ruthenium porphyrin complexes as sensitizers. The
visible light absorption is attained through a sensitizer integrated with
the nano TiO2 architecture of the fabricated DSSC. The natural dye
sensitizer is made up of inorganic, organic metal, and organic dye
molecules. Fortunately, mesoporous semiconductors have been made
sensitive using organic dyes and organic metal complexes [9]. According
to stability and efficiency, ruthenium bipyridyl compounds are the basis
for the most potent sensitizers [10]. These natural dyes have great
metal-to-ligand electron transfer and are efficient at injecting electrons,
and they absorb the majority of light in the visible spectrum [11-13]. A
charge is transferred from metal to ligand more quickly than in the back
reaction, which results in the recombination of electrons with dye
molecules that have undergone oxidation rather than performing work
[14]. Even though the PCE of Ruthenium dyes is greater than 10%, they
require time-consuming chromatographic techniques and multi-step
procedures for preparation [15]. Geetam Richhariya et al. [11] dis­
closed DSSC as the piloted novel method having efficiency more than
thin films while less than that of monocrystalline solar cells. DSSC
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Inorganic Chemistry Communications 152 (2023) 110638
Fig 1. No of research papers published per year [38].
upgrades the economic facet, as well as creates remarkable welfare from
the environmental stance. The miscellany of DSSC components makes it
appealing because novel materials are incorporated to optimize their
effect. Recently, natural sensitizers have drawn a lot of interest due to
their natural method of harvesting sunlight and they’ve become a viable
option due to their simple extraction procedures for generating energy.
India’s diverse climate and geographical conditions have resulted in the
growth of various plants in various parts of the country. Simple prepa­
ration techniques, low cost, abundance, and sustainable characteristics
are promising stimulants for DSSC. Huizhi Zhou et al. [15] scrutinized
DSSC by the extraction of natural dyes from leaves, fruit peels, bever­
ages, Chinese traditional medicines, roots, parks, etc. have been scruti­
nized on DSSC. The photoelectrochemical stability of dye sensitizer
undergoes a redox cycle without decomposition and carries functional
groups such as phosphonate, carboxylate which act as an anchoring
group to swiftly graft it to the nanoporous TiO2 semiconductor by
chemisorption was made known by Norasikin A. Ludin et al. [16]. Cal­
ogero, G et al. revealed the advancement in the mechanism of natural
photosensitizer inspecting pigments such as anthocyanin, carotenoids,
chlorophyll, and flavonoids separately influence the efficiency of DSSC
[17]. Due to their low charge transfer absorption in the solar spectrum’s
visible region and weak binding energy with nanocrystalline TiO2 sub­
strate, organic dyes like phthalocyanine, coumarin, cyanine, xanthene,
etc. appear to be weak sensitizers [16]. These dyes frequently resemble
the pigments found in naturally occurring sensitizers such as fruits,
flowers, leaves, tree bark, roots, etc. [7-11].
Several research organizations separately reviewed the various
electrolyte types used [18-20] or components used to make electrodes
[18,21], or compounds made from natural sensitizers [11,22]. Likewise,
only a few researchers have reviewed the future development [18,31]
stability [23-30] and the application of natural dye-based DSSC [8,31-
37]. It is indispensable to know that more research needs to be done for
assessing and upgrading the performance of DSSC. Eventually, the cur­
rent advancement in DSSC and their conversion efficiency with future
development are reviewed [14]. Among all the conventional energy
sources, the attention of researchers and scientists has been focused on
the most propitious power-generating device, fabricated with an effi­
ciency of 7–8 % [18-20]. This review article consolidates all the com­
ponents employed for the fabrication of DSSC, various electrolytes
employed, types of natural plant derivatives, and parameters such as
Voc, Jsc, PCE, etc. which influence the working of dye-based DSSC. The
degradation and stability of DSSC materials together with stability-
enhancing recommendations are also discussed. The necessity of
commercialization and future prospects of natural sensitizer-based DSSC
have also been examined.
Hence, it makes more sense to concentrate on newly emerging DSSCs
P. Prakash and B. Janarthanan
Fig. 2. Schematic representation of the working principle of DSSC.
with high efficiency as a remarkable research interest for developing
countries that do not have high-tech production steps and the process for
making ultrapure silicon. In this article, the advantages, key elements,
and essential functions of DSSCs are reviewed first. Then, photosensi­
tizers, their absorption properties, purification and extraction methods,
stability, chemical structure, structural modifications, and dye blends
are discussed. Future perspectives on current challenges associated with
various solar cells are also evaluated. Fig. 1 represents the no of research
papers published per year.
2. Working Principle:
Dye-sensitized solar cells are a solar photovoltaic device that con­
verts solar radiation into electricity. It comprises various constituents
namely:
(a) Indium-doped tin oxide (ITO) or Fluorine-doped tin oxide (FTO)
are typically the two types of conducting oxide that is most
prevalent. However, there are some reports on inexpensive sub­
stitutes that can be employed as transparent conducting oxides,
such as graphene, doped TiO2, and aluminum-doped zinc oxide
(AZO).
(b) Mesoporous metal oxide coating developed from nano TiO2 acts
as a photoanode.
(c) Anchoring of dye molecules (sensitizers) into the photoanode.
(d) The commonly used iodide-tri iodide electrolyte that experiences
a redox reaction.
(e) Glass coated with platinum/graphene is generally used as a
counter cathode.
DSSC has a sandwich configuration [21] which is convenient due to
its environmental friendliness, low fabrication cost, and 100% avail­
ability [14,22]. DSSC act as a photonic device [23] in which particles of
energy from the sun bash on the surface of DSSC allowing maximum
passage of radiation to the active area. Anatase TiO2 having a wide band
gap has been chosen as the semiconductor membrane [24]. DSSC
eminently relies on the photosensitizing natural pigment. The photo­
sensitizers have a lower bandgap which allows the charge carriers to be
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Inorganic Chemistry Communications 152 (2023) 110638
transmitted to the LUMO level upon photon exposure, known as exci­
tation Photo-excitation of sensitizer [25] is followed by the electron-
stimulated transition to the LUMO level of dye molecules and elec­
trons lost by the sensitizer molecules gets oxidized [39]. The injected
electrons in the excited level transmit to the guide band of the nano­
crystalline metal oxide semiconductor, which serves as a roadway for
the charge carriers to cross from photocathode to anode [26]. The
excited electrons from the conduction band of numerous TiO2 thin films
across the whole mesoporous structure, due to higher electrical potential
travel towards the anode surface and reach the counter cathode capped
with finely split platinum islands as a catalyst. Lost electrons are
recovered by the molecules of potential dyes through the organic elec­
trolyte carrying iodide/triiodide redox mediator [40] and thus the
operation is replicated [41]. While Platinum is the frequently used
counter-electrode material, the potential substituents introduced
recently for the counter electrode are graphene, carbon nanotubes,
conducting polymer, and their composites [26-28]. The Triarylamine
(TAA) based dyes reported the best PCE for DSSC can reach above 14%
[14].
Slow electron-hole recombination based on the pace at which charge
carriers are supplied by the organic electrolyte, low structural weight,
and inexpensive raw material costs is all advantages of Si-based solar
cells [29]. Iodide-tri iodide electrolyte also goes through a redox reac­
tion, which makes it different from silicon-based solar cells and the
development of all-weather solar cells. DSSCs dyes exhibit effective
performance in low-light scenarios such as overcast skies. In interior
applications, the DSSCs concept also operates in wet, foggy, and gloomy
weather [30,31]. A schematic representation of the working principle of
DSSC is displayed in Fig. 2.
3. Parameters of DSSC:
The performance of DSSCs depends on the parameters of construc­
tion, such as TiO2′ s mesoporous structure, dye absorption properties,
TCO transparency and conductivity, cathode catalytic activity, and
electrolyte redox characteristics. The primary factors that influence dye-
sensitized solar cell’s performance are Jsc, Voc, FF, and η. A quantum
efficiency known as IPCE denotes the efficient conversion of visible light
P. Prakash and B. Janarthanan
to electricity [20] and the plotting of this transformation with respect to
wavelength. Additionally, the following equation is used to calculate the
efficiency of electrical power conversion [32].
FF = (Jm ⋅Vm )/(Jsc ⋅Voc ) (1)
FF ⋅Jsc ⋅ Voc
η% = ⋅100 (2)
Input power
where the macroscopic measures such as photovoltage (e.g., Voc) and
photocurrent (e.g., Jsc) could be used to assess DSSC performance.
Theoretically, DSSC’s maximum output current is represented by the
open circuit voltage (Voc), whereas the maximum theoretical output
voltage of a DSSC is indicated by the short circuit current density (Jsc)
[20]. The fill factor (FF) is a measurement of the device’s junction
quality and series resistance. Pmax and Pin denote the maximum power
output and the power of incident photon of DSSCs respectively.
4. DSSC constituents
Several ongoing projects are scrutinizing new concepts and practices
for producing clean energy [33]. DSSCs have a number of constructional
factors that need to be improved in order to increase the efficiency of
power conversion. Here, we provide an overview of the key components
of DSSC such as transparent conductive oxide (TCO), photosensitizers,
mesoporous TiO2 semiconductors, counter electrodes, and redox elec­
trolytes [19,20].
4.1. Transparent conductive Oxide:
A transparent conductive substrate is commonly used during the
production of solar cells as the photoanode. The incoming photons can
pass through the transparent conducting substrate with minimal ab­
sorption or reflection, while giving the substrate mechanical strength,
which possesses low cost and high transparency to solar light, providing
TCO substrates with mechanical strength. It gathers charge carriers from
mesoporous semiconductors and transports them with minimal resis­
tance to the load. TCO is the most commonly used substrate for DSSC
and is a conductive thin film substrate of eminent transparency >80%
[28]. Methodical charge transfer to curtail energy losses governs the
efficiency of DSSC [23,29]. TCO thin films typically consist of fluorine-
doped tin oxide (F: SnO2) or indium tin oxide (In: SnO2). Classic
conductive film oxide is Fluorine doped Tin Oxide (FTO) evinces 75%
transmittance with a sheet resistance of about 8.5 Ω/cm2 [28]. DSSC is
endorsed with an optically transparent electrode (FTO) due to its high
forbearance to physical erosion, stability under any atmospheric con­
ditions, and resistance to high temperature. Due to thermal stability,
proper transparency, and low cost of FTO substrate is generally
preferred for the fabrication of DSSCs [25]. ITO/FTO-coated transparent
polymer thin films, i.e. polyethylene terephthalate (PET) are a low-
density, low-cost, and flexible alternative to a glass substrate in DSSCs
[34]. Flexible film solar cells (FFSCs) are a popular choice among
portable power sources due to their autogenic transformation, promi­
nent conversion efficiency, excellent portability, and sustainable output
[35].
4.2. TiO2 photo electrode
Titanium dioxide is the most commonly used semiconductor oxide in
DSSC as an electron acceptor. The large surface area of the nano-porous
TiO2 glass substrate allows the chemisorption of sensitizers onto the
electrode surface. A mesoporous film of 10–12 μm has 50% porosity and
a particle diameter of 20 nm absorbs all the incident photons and attains
a PCEs of around 11.2% [42]. The necessity of absorbing the entire
incident light is the driving force behind the growth of mesoscopic TiO2
substrate [11,43]. TiO2, SnO2, ZnO, and chalcogenides are some of the
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Inorganic Chemistry Communications 152 (2023) 110638
oxides materials used as photoelectrode owing to their environmental
remediation and wide energy storage application. It aids in attaining the
highest values for DSSC parameters when used as a semiconductor
photo-electrode [44]. Due to the poor stability of photoelectrochemical
cell by bulky semiconductor was trounced by wide band gap nano­
particles which undergo photo-conversion efficiency of the sensitized
photo-electrode [30]. Among the various candidates, TiO2 exhibits
preferable performance owing to non-toxicity, profusion, biocompati­
bility, and large surface area for loading the sensitizer [30]. Titanium
dioxide is the naturally occurring oxide of titanium. Generally, it is
sourced from rutile, anatase, and ilmenite. The anatase phase of TiO2
has been favored due to its strong conduction band edge energy (3.2 eV),
and strong chemical stability. The anatase phase shows photo-catalytic
degradation under an ultraviolet range of organic materials [11,45,46]
while the rutile phase reduces the stability and absorbs 4% of incident
light [11].
As photo electrodes, many other semiconductors are also used in the
construction of DSSC. ZnO-coated conducting glass substrate attained an
efficiency of about 0.4% using the sol–gel method [47]. ZnO-based DSSC
fabricated by Saito et.al [48] using the squeegee technique obtained an
efficiency of around 6.58% and exhibits greater electronic mobility. ZnO
photoanode displayed a shorter life period, which was attributed to the
breakdown of organic compounds, especially sensitizers under irradia­
tion of light, with rising temperature, interface instability, oxygen ab­
sorption, and electrode chemical changes [49].
In order to enhance ZnO efficiency, a combination of ZnO / TiO2 was
employed as a DSSC electrode and a radio-frequency (RF) magnetron
sputtering technique was used for the preparation which reported the
highest photon-to-current conversion efficiency from 4.76% to 6.55% by
Wu et.al [50]. But Chou et.al [51] overcome the drawback in the de­
mand for high-priced vacuum technology with a non-vacuum solution
technique and reported an efficiency of about 6.62% when compared to
ZnO/TiO2-based electrodes with pricey vacuum technology. Tan et al.
[52] synthesized large band gap ternary oxides such as Zn2SO4 (Eg =
3.35 eV) [53] and obtained an overall efficiency of about 3.8%.
TiO2 has been acknowledged as the nonesuch of semiconductor
electrodes since 1991, despite higher charge recombination and lower
electron transport [18]. Krasovec et al. [54] in 2009, prepared a unique
TiO2 paste and yielded a conversion efficiency of 10.2% by adding Ti-
isopropoxide into a solution of citric acid and ethylene glycol. Later,
Stathatos et al. [55] fabricated DSSC using nano-crystalline TiO2 semi­
conductor at low temperatures and attained an efficiency of about 5.3%
and 3.2% respectively. Chou et al. [56] developed p-type NiO composite
particle electrodes using a spin coating technique and reported an effi­
ciency of around 3.8% whereas the conversion efficiency of the tradi­
tional DSSC was 3.27%. Thus rise in efficiency is ascribed to the n-p
junction and NiO barrier effects [51,56]. DSSC fabricated by Yang et al.
[57] introduced F doped TiO2 electrode which exhibits a high efficiency
of about 8.07%.
TiO2 semiconductor electrodes are modified by covering them with
other semiconductors or with an insulator which enhances the photo
electrical activity and PCE that could avert back reaction by developing
an energetic barrier. Thus, Zalas et al. [58] created a DSSC by incor­
porating the rare earth element gadolinium with a TiO2 layer and ob­
tained a conversion efficiency of 0.74% despite the fact that the
modified electrode adsorbed less dye. The element gadolinium enhances
the photo-catalytic properties of the modified TiO2 layer, whereas,
under 400 W/m2 irradiance from a tungsten-halogen lamp, the un­
modified TiO2 electrode had an efficiency of 0.55%.
The results of modeling with semiconductor variations in photo­
anodes show that TiO2 is the optimal material when compared to ZnO
and Nb2O5. This is influenced by the photoanode surface area, electron
mobility, and dye interactions. Nanostructure optimization has been
done by analytic modeling to obtain optimum parameters for TiO2 and
ZnO thickness at 10 µm and Nb2O5 at 20 µm. The parameters of the
absorption coefficient and diffusion coefficient have a comparable
P. Prakash and B. Janarthanan
relationship to the performance of DSSC. The next material, niobium
pentoxide received attention in the scope of DSSC research because it
can be applied to anode or cathode cells. Nb2O5 can also act as a barrier
layer that is very good at reducing electron loss due to recombination
with electrolytes. Despite the high short circuit current value, the high
recombination rate reduces the potential difference when the circuit is
open. In the same way, Nb2O5 contains a barrier layer to slow down
electron recombination processes, but the current density is low. The
surface area of a semiconductor has a significant impact, as already
mentioned [59].
Zinc oxide (ZnO) is the semiconductor that comes the closest to TiO2
in a dye-sensitized solar cell (DSSC). This is explained by the fact that
ZnO and TiO2 have similar electron affinities and band gap energies, as
well as the fact that ZnO has a higher electron diffusivity than TiO2, as
well as a higher electron mobility, a larger excitation binding energy,
and is easily accessible at a lower cost and is resistant to photo-
corrosion. ZnO’s ideal properties include stability, the best facet for
usage in DSSCs, and the best redox couple for products made from ZnO.
It is projected that a DSSC with ZnO will show fewer recombination
reactions than a DSSC with TiO2. Actually, the first oxide semiconductor
used for a DSSC’s photoanode was ZnO [60]. A cheap material with a
high excitation binding energy (60 eV) and photo-corrosion resistance is
zinc oxide. The first experimental demonstration of irreversible organic
molecule-induced electron injection into the conduction band of a large
band gap semiconductor was really made using ZnO [61] and [62].
Moreover, a variety of photoanode designs for DSSCs can be anticipated
with ZnO due to its numerous morphologies, which are possibly richer
than those of metal oxides now known. ZnO is a great option for DSSCs
with photoanodes consisting of nanorods, nanowires, or nanosheets
because, unlike TiO2, its crystalline structure is favorable to anisotropic
development [63].
In ZnO-based DSSC, Tingli Ma et al. used a quasi-solid state elec­
trolyte and were successful in solid-state synthesizing the ZnO nano­
structure to achieve an efficiency of up to 6.46% [64]. A ZnO compact
layer created using the sol–gel technique was previously injected into
the photo-electrode at the interface between a mesoporous ZnO layer
and a fluorine-doped tin oxide (FTO) substrate [65] and [66]. These cells
have a significantly poorer power conversion efficiency as compared to
cells with liquid electrolytes or quasi-solid state electrolytes. The
dissolution of ZnO into Zn2+ by the adsorbed acidic dye, the formation of
aggregates (insulating layer) of Zn2+ and dye molecules (such as N3,
N719, and black dye), and finally the blocking of the injected electrons
from the dye molecules to the semiconductor by the insulating layer are
the most likely causes of the low conversion efficiencies of ZnO-based
systems [67] and [68]. Only Sakai et al. have ever studied the photo­
voltaic performance of dye-sensitized solar cells (DSSCs) using the
electrode. No other team has investigated the connection between the
DSSCs and the size of ZnO particles in a porous semiconductor electrode.
The DSSC that used ZnO particles with a diameter of 40 nm had the
highest power conversion efficiency among those based on particles
with a size range of 20 nm to 2 m [69].
4.3. Robust electrolyte
The electrolyte has a crucial part in determining the cell’s perfor­
mance and provides conductivity of internal ions by diffusing in the
nano-porous TiO2 layer [70]. Consequently, many studies have been
carried out to investigate various electrolytes such as redox electrolytes,
polymer electrolytes, VOS electrolytes, RTIL electrolytes, and so on [39].
Volatile organic solvent (VOS) is a widely used electrolyte in the fabri­
cation of DSSC and attained an IPCE of 74–78% [71] even though it has
constraints such as the demand for complex scaling processes and
impoverished long-term cell stability [72]. In addition, they might have
degradation caused by low boiling points, and usage of VOS for practical
applications is limited due to the loss of additives [73]. As a substitute
for VOS, ionic liquids (RTIL) at room temperature have acquired more
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Inorganic Chemistry Communications 152 (2023) 110638
awareness because of their non-inflammability, non-volatility, chemical
stability, and high ionic conductivity. Non-volatile liquids usually have a
viscosity higher than VOS, leading to high PCE [71]. Despite, the ad­
vantages of [BuPyIm]Br showing high thermal stability and low vola­
tility reported by Xu et al. [73] has complications such as liquid
electrolytes volatilization and leakage, hindering its influence in DSSC.
These liquid solvents also keep restrictions on the device structure and
the risk of solvent leakage and evaporation was introduced [74]. Poly­
mer electrolytes were chosen as a good alternative in order to overcome
the problem. Polymer electrolytes contain metal salts dissolved in
polymer matrices of low lattice energy such as ether or amide linkages
[39] has several advantages namely good ionic conductivity, and high
thermal stability which also eliminate the risk of solvent leakage and
sealing [39,75]. In order to regenerate the oxidized dye molecules in
DSSC, an electrolyte of suitable redox potential is used to complete the
circuit by arbitrating charge carriers between the photo-anode and
counter electrode [28]. Among other electrolytes, the I-/I3- redox
mediator is the most efficient couple with long-term stability. The ionic
conductivity, sedate electron recombination, good solubility, and high
efficiency of redox electrolyte in DSSC affect the performance of the cell
and solvent viscosity [30].
4.4. Counter cathode
The transportation of holes in solid-state electrolytes or the reduction
reaction of the redox mediator takes place at the counter cathode. The
most promising counter electrodes have been noble metals, carbon
materials, composite materials, transition metal compounds, and
conductive polymers. Photo-cathodes exhibit efficient electron transfer
using thin film electrode material such as platinum (Pt) as a catalyst
[26]. Counter electrodes regenerate the electrolyte by collecting elec­
trons from the external circuit [28]. Pt-coated FTO substrate has
exceptional catalytic pursuit, high electrochemical activity, and stabil­
ity, even though it’s highly expensive. Consequently carbon, a viable
alternative has been introduced because of its low cost and resistance to
heat [33]. Reduction of redox electrolyte takes place in the counter
electrode and a catalytic coating is suitable for the enhancement of re­
action kinetics in the counter electrode. According to patents and pub­
lished research, carbon materials are the optimum option for the counter
cathode in DSSCs.
4.5. Potent sensitizer
The essential component of the DSSC is a dye sensitizer that absorbs
photons in the visible band with a tremendous amount of intensity and
the molecular structure of the light sensitization determines the per­
formance of DSSC [26]. Photo-excited electrons interact with TiO2
particles and the redox electrolytes in both physical and electrical ways.
Some of the vital requirements for photosensitizers are absorption of
strong electromagnetic waves in visible and near IR, intense adsorption
to the semiconductor interface, appropriate LUMO and HOMO energy
level and high stability, molar extinction coefficient, and regeneration of
dye from the electrolyte. Ruthenium dyes were the first and most
effective sensitizers having effective load transfer from metal to ligand,
stability, long agitated lifetime, and a broad absorption spectrum of light
[53]. Some drawbacks of Ru (II) polypyridyl dyes-based complexes are
high cost, toxicity, low molar extinction coefficient, scarcity, and sta­
bility problems of ruthenium when exposed to sunlight for a long
duration [55]. Natural dye sensitizers are a feasible alternative to
expensive synthetic dyes [26]. Conversion efficiency was found to be
minimum for dyes extracted from natural pigments such as anthocyanin,
betalain, carotenoids, chlorophyll, flavonoids, etc. [31]. The edge of
natural dyes is their easy extraction process, cheap cost, and environ­
mentally affable nature [32]. Industrial effluents contain heavy metals
that cause serious problems when discharged into the aquatic environ­
ment [56]. Other famous metal complexes include N719, and N749 also
P. Prakash and B. Janarthanan Inorganic Chemistry Communications 152 (2023) 110638

Table 1
PCE of different natural potential sensitizers extracted from flowers, leaves, vegetables, fruits, seeds, and tree bark.
Sensitizer solution Electrode Derivative λ max (nm) Jsc (mA Voc FF η (%) Ref
cm− 2) (V)

Jabuticaba (Plinia cauliflora) TiO2 Anthocyanin 545 0.23 0.35 0.23 0.018 [76]
Thunbergia erecta TiO2 Anthocyanin 537 0.27 0.55 0.40 0.059 [77]
Saraca asoca flowers TiO2 Anthocyanin 450 0.29 0.51 0.65 0.09 [78]
Leucanthemum vulgare TiO2 Luteolin – 0.39 0.52 0.26 0.05 [79]
Red frangipani TiO2 Anthocyanins 530 0.94 0.49 0.65 0.30 [80]
Fructus lycii TiO2 Carotene 447, 425 0.53 0.689 0.46 0.17 [81]
Marigold TiO2 Xanthophyll 487 0.51 0.542 0.83 0.23
Tangerine peel TiO2 Flavone 446 0.74 0.592 0.63 0.28
China Loropetal TiO2 Chlorophyll 665 0.84 0.518 0.62 0.27
Turmeric TiO2 Carotenoid 525 0.288 0.529 0.48 0.07
Yellow rose TiO2 Xanthophyll 487 0.74 0.609 0.57 0.26
Bauhinia tree TiO2 Anthocyanin 665 0.96 0.572 0.66 0.36
Perilla TiO2 Chlorophyll 665 1.36 0.522 0.69 0.46
Flowery knotweed TiO2 Anthraquinone 435 0.60 0.554 0.62 0.21
Begonia TiO2 Anthocyanin 540 0.63 0.537 0.72 0.24 [82]
Coffee TiO2 Anthraquinone – 0.85 0.559 0.68 0.32
Erythrina variegata TiO2 Chlorophyll 451, 492 0.78 0.48 0.55 0.20 [83]
Lily TiO2 Anthocyanin – 0.51 0.498 0.66 0.17
Petunia TiO2 Chlorophyll 665 0.85 0.616 0.60 0.31
Chinese rose TiO2 Chlorophyll 516 0.90 0.483 0.61 0.27
Broadleaf holy leaf TiO2 Chlorophyll – 1.19 0.607 0.65 0.47
Violet TiO2 Anthocyanin 546 1.02 0.498 0.64 0.33
Clitoria ternatea TiO2 Anthocyanin 580 0.37 0.37 0.33 0.05
Mangosteen pericarp TiO2 Rutin – 2.69 0.686 0.63 1.16
Rosella (Hibiscus sabdariffa L.) TiO2 Anthocyanin 520 1.63 0.40 0.57 0.37 [84]
Lithospermum TiO2 Anthocyanin 520 0.14 0.337 0.58 0.03
Rose TiO2 Anthocyanin – 0.97 0.595 0.65 0.38
Raspberries TiO2 Betacyanin 540 0.26 0.42 0.64 0.07
Nerium olender TiO2 Anthocyanin 539 2.46 0.40 0.59 0.58
Ixora macrothyrsa TiO2 Anthocyanin 537 1.31 0.40 0.57 0.30
Red Bougainvillea glabra TiO2 Betaxanthin, Betacyanin 482, 535 2.34 0.26 0.74 0.45 [85]
Hibiscus rosasinesis TiO2 Anthocyanin 534 4.04 0.40 0.63 1.02
Rosa xanthina TiO2 Anthocyanin 560 0.64 0.49 0.52 0.16
Grapes TiO2 Betacyanin 560 0.09 0.34 0.61 0.02
Red Bougainvillea spectabilis TiO2 Betaxanthin, Betacyanin 480 2.29 0.28 0.76 0.49
Hibiscus surattensis TiO2 Anthocyanin 545 5.45 0.39 0.54 1.15 [86]
Violet Bougainvillea glabra TiO2 Betaxanthin, Betacyanin 547 1.86 0.23 0.71 0.30
Sesbania grandiflora TiO2 Anthocyanin 544 4.40 0.41 0.57 1.03
Violet Bougainvillea spectabilis TiO2 Betaxanthin, Betacyanin 535 1.88 0.25 0.73 0.34
Kopsia flavida TiO2 Anthocyanin 550 1.20 0.52 0.62 0.39 [87]
Red turnip TiO2 Betalin 536 9.50 0.425 0.37 1.5
Wild sicilian prickly pear TiO2 Betalin 465 8.20 0.38 0.38 1.18 [88]
Capsicum TiO2 Carotenoid 455 0.23 0.41 0.63 0.06 [83]
Myrtus cauliflora mart (jaboticaba) TiO2 Anthocyanin 520 7.20 0.59 0.54 2.3
Solanum melongena TiO2 Anthocyanin 522 3.40 0.35 0.40 0.48
Berberies buxifolia lam (Calafate) TiO2 Anthocyanin 533 6.20 0.47 0.36 1.05 [89]
Mulberry TiO2 Anthocyanin 543 0.86 0.42 0.43 0.15
Hylocereus costaricensis (Dragon fruit) TiO2 Anthocyanin 535 0.20 0.22 0.30 0.01
Chaste tree fruit TiO2 Anthocyanin 548 1.06 0.39 0.48 0.2 [90]
Citrussinensis (Redsicilian) TiO2 Anthocyanin 515 3.84 0.34 0.50 0.65 [91]
Cheries TiO2 Betacyanin 500 0.46 0.30 0.38 0.05
Shiso TiO2 Chlorophyll 440, 600 3.56 0.55 0.51 0.99
Festuca ovina TiO2 Chlorophyll 420, 660 1.18 0.54 0.69 0.44 [92]
Ivy gourd fruits TiO2 β-Carotene 458, 480 0.24 0.64 0.49 0.08
Allium cepa (Red onion) TiO2 Anthocyanin 532 0.51 0.44 0.48 0.11
Ipomea TiO2 Chlorophyll 410 0.91 0.54 0.56 0.28
Jathopha curcas Linn (Botuje) TiO2 Flavonoid 400 0.69 0.05 0.87 0.03
Spinach TiO2 Chlorophyll 437 0.47 0.55 0.51 0.13 [93]
Cabbage- palmfruit TiO2 Anthocyanin 545 0.37 0.44 0.61 0.1
Brassica olercea (Red cabbage) TiO2 Anthocyanin 537 0.50 0.37 0.54 0.1 [94]
Vernonia amygdalin (Bitterleaf) TiO2 Chlorophyll 400 0.07 0.34 0.81 0.02
Bixa arellana L. (Achiote) TiO2 Carotenoid 474 1.1 0.57 0.59 0.37 [95]
Ficus retusa TiO2 Chlorophyll 670 7.85 0.52 0.29 1.18 [96]
Anethum graveolens TiO2 Chlorophyll 666 0.96 0.57 0.40 0.22 [97]
Walnuts ZnO Carotenoid 510 0.73 0.304 0.39 0.09
Arugula TiO2 Chlorophyll 666 0.78 0.59 0.42 0.18
Rhoeo spathacea TiO2 Chlorophyll 670 10.9 0.50 0.27 1.47
Green algae ZnO Chlorophyll 666 0.08 0.32 0.37 0.01 [97]
TiO2 0.13 0.41 0.21 0.01

Parsley (Petroselinumcrispum) TiO2 Chlorophyll 666 0.53 0.44 0.34 0.8

Lawsonia Inermis TiO2 Anthocyanin 518 1.87 0.61 0.58 0.66 [98]
Garcinia subelliptica TiO2 Chlorophyll 670 6.48 0.32 0.33 0.69
(continued on next page)

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P. Prakash and B. Janarthanan Inorganic Chemistry Communications 152 (2023) 110638

Table 1 (continued )
Sensitizer solution Electrode Derivative λ max (nm) Jsc (mA Voc FF η (%) Ref
cm− 2) (V)

Undaria pinnatifida TiO2 Chlorophyll 665 0.8 0.36 0.69 0.198

Oryzasativa L. Indica (Blackrice) TiO2 Anthocyanin 560 1.14 0.55 0.52 0.32 [83]
Sumac/ Rhus TiO2 Anthocyanin 650 0.93 0.394 0.41 0.15
Alkanet TiO2 Carotenoid 535 0.268 0.372 0.46 0.05
Curcuma longa TiO2 Carotenoid 450 0.20 0.280 0.65 0.03
Madder TiO2 Anthraquinone 540 0.540 0.389 0.69 0.14
Lemon leaves TiO2 Chlorophyll 475, 675 0.286 0.539 0.74 0.11
Yemeni henna TiO2 Chlorophyll – 0.407 0.306 0.28 0.03
Bahraini henna TiO2 Chlorophyll – 0.368 0.426 0.24 0.04
Bloodleaf TiO2 Betacyanin 460 0.260 0.267 0.46 0.03
Rhubarb TiO2 Chlorophyll 410 0.82 0.238 0.44 0.08
Khella TiO2 Anthocyanin 465, 650 0.384 0.437 0.47 0.08
Cosmos sulphureus TiO2 Flavonoids 505, 590 1.041 0.447 0.61 0.28
Tagetes erecta TiO2 Xanthophyll 465 2.891 0.475 0.606 0.83 [99]
Black carrot (Daucus carota L.) TiO2 Anthocyanin 540 1.302 0.4 0.47 0.24 [100]
Gardenia blue TiO2 Carotenoid 600 0.53 0.44 0.69 0.16
Allamanda cathartic (Golden trumpet) TiO2 Carotenoid 325, 458 0.878 0.405 0.54 0.19
Punica granatum peel TiO2 Flavonoid 400 3.341 0.716 0.776 1.86
Gardenia yellow TiO2 Carotene 450 0.96 0.54 0.62 0.32 [101]
Morinda lucida TiO2 Anthocyanin 440 1.15 0.350 0.63 0.25 [102]
Light harvesting complex II (LHCII) From Sinach LHCII
pigments 436, 473, 0.80 0.59 0.58 0.27 [103]
Chlorophyll 652,678
TiO2
430, 452, 2.26 0.53 0.69 0.82
Chlorophyll 645, 661
Raspberries, Shami-berries, Grapes, Hibiscus,
Chlorophyll and a cocktail
TiO2 Anthocyanin – – – –
3.04 [104]
Wormwood and purple cabbage Chlorophyll and Anthocyanin – 3.16 0.66 0.62 1.29
TiO2
Berberis vulgaris – – –
and Phytolacca Americana Anthocyanin, Carotenoid 3.04
TiO2 and Betacyanin –
Rosella and blue pea –
TiO2 Anthocyanin 0.82 0.38 0.47 0.15

Neem and Poinsettia TiO2 Chlorophyll – 0.52 0.39 0.46 0.1

and
Anthocyanin
Purple cabbage and Beetroot TiO2 Anthocyanin and Betalains 440, 630, 1.12 0.56 0.60 0.38
675
Carica Papaya TiO2 Chlorophyll 411 0.149 0.373 0.30 0.02
Citrus Lanatus TiO2 Chlorophyll 410 0.140 0.333 0.26 0.01
Solanum melongena TiO2 Chlorophyll 411 0.126 0.321 0.28 0.01

Flora TiO2 – 665.80 1.278 0.651 0.37 0.31

Spinacia oleracea –
TiO2 Chlorophyll 0.667 0.625 0.214 0.09
Persea americana TiO2 Chlorophyll 411 0.111 0.303 0.29 0.01
Jasminum Grandifolium TiO2 – 658.1 1.278 0.651 0.377 0.314
Petroselinum crispum TiO2 Chlorophyll – 0.33 0.610 0.076 0.015
Rosa damascena TiO2 Anthocyanin 420.5 0.276 0.617 0.069 0.011
Safflower TiO2 Carthamin 420 1.00 0.390 0.24 0.09
Calumus draca TiO2 – – 0.31 0.348 0.28 0.03
Rheum TiO2 Anthocyanin – 0.31 0.259 0.27 0.02
Senna TiO2 – – 0.37 0.371 0.30 0.04
Roselle TiO2 Anthocyanin 490, 540 0.08 0.259 0.23 0.005
Carya illinoensis TiO2 – – 0.46 0.229 0.18 0.02
Punica granatum TiO2 Anthocyanin – 0.23 0.300 0.21 0.01
Wormwood TiO2 Chlorophyll – 1.96 0.585 0.47 0.54
Carthamus tinctorius TiO2 Carthamin – 0.269 0.619 0.070 0.01
Purple cabbage TiO2 Anthocyanin 500, 650 2.08 0.66 0.53 0.73
Beetroot TiO2 Betalain 550 0.72 0.46 0.54 0.18
Olive grain TiO2 – 666 0.58 0.55 0.38 0.12
Olive leaves TiO2 Chlorophyll 432, 664 0.85 0.59 0.33 0.17
Zizyphus bark TiO2 – 662 0.42 0.50 0.35 0.07
Lycium shawii bark TiO2 – 434, 662 0.15 0.44 0.29 0.02
Lycium shawii flower TiO2 – 662 0.42 0.58 0.42 0.1
Lycium shawii leaves TiO2 Chlorophyll 412, 664 1.20 0.62 0.43 0.32
Olive root TiO2 – 636 0.45 0.53 0.35 0.08
Punica granatum TiO2 Anthocyanin 412, 665 2.05 0.56 0.52 0.59 [105]
Acanthus sennii Chiovenda flower TiO2 – 524 0.49 0.51 0.60 0.15 [106]
Melastoma malabathricum TiO2 Anthocyanin – 3.18 0.45 0.52 0.74 [107]
(continued on next page)

7
P. Prakash and B. Janarthanan Inorganic Chemistry Communications 152 (2023) 110638

Table 1 (continued )
Sensitizer solution Electrode Derivative λ max (nm) Jsc (mA Voc FF η (%) Ref
cm− 2) (V)

TiO2 – 394 0.56 0.62 0.55 0.19 [108]

Apricot leaves
Petunia TiO2 Chlorophyll – 0.85 0.61 0.61 0.32 [109]
Red sicilian orange TiO2 – 538 5.13 0.33 0.59 0.99 [110]
Codiaeum variegatum TiO2 Anthocyanins – 4.03 0.44 55 1.08 [111]
TiO2 – 432 0.85 0.59 0.33 0.17 [112]
Olive leaves
Garcinia subelliptica TiO2 Chlorophyll, carotenoids or – 6.48 0.32 33 0.69 [113]
phycobiliproteins
TiO2 – 525 1.09 0.521 0.69 0.47 [114]
Opuntia dillenii
Flowery knotweed TiO2 Rhein – 0.6 0.55 0.63 0.21 [109]
Pandanus amaryllifolius TiO2 – 415 0.40 0.55 0.61 0.1 [115]
Zizyphus root TiO2 – 664 0.37 0.49 0.24 0.04
Lycium shawii root TiO2 – 662 0.13 0.38 0.26 0.01

referred to as black dye [54]. On the other hand, the advantages of
metal-free organic dyes are diverse molecule structure, economical
synthesis processes, and high molar extinction coefficient [58]. Never­
theless, dye aggregation, instability, and narrowband absorption are the
most promising limitations of these sensitizers. In DSSC, coumarin, he­
mocyanin, indoline, polyene, hetero-polycyclic and thiophene-based
dyes are some of the vital classes of organic dyes [70]. The basic fabri­
cation requirements of an effective photosensitizer consist of (i) high
visible light-harvesting capacity (ii) strong adsorption of dye molecules
onto the TiO2 film (iii) injection of charge carriers into the conduction
band of TiO2 surface (iv) high rates of electron transfer are ensured by
anchoring = O or -H groups on the semiconductor surface [70]. Another
class of photosensitizers in DSSC are quantum dots (QDs) with large
dipole moments, multiple exciton generation features, high light ab­
sorption, and tunable energy band gaps. However, due to charge leakage
at the semiconductor/sensitizer and semiconductor/electrolyte inter­
face, efficiency parameters such as fill factor (FF) and open-circuit
voltage (Voc) of inorganic semiconductor QDs are relatively poor [75].
Halide perovskite solar cells have excellent light-absorption qualities,
and perovskite sensitizer PCEs are predicted to reach 20% in the near
future. Due to excellent molecular stability, efficient electron transfer,
simple manufacturing process, intense absorption, inexpensive nature,
and appropriate energy levels of Porphyrin dyes also attracted interest in
the fabrication of solar cells [71]. Easy extraction, environment-friendly,
non-toxicity, biodegradation, and low cost are the most [72] promising
factors of natural photosensitizers [76]. The environmental and eco­
nomic advantages of NDSSCs have resulted in various research aspects,
although the PCE attained by natural derivatives is low compared to
other sensitizers, which are reviewed in Table 1.
sensitizers. Scientists stimulate further research to intensify the effi­
ciency of cells using natural dyes as potential absorbers. The majority of
developing countries have chosen to use technology for sustainable
energy production due to climatic changes, high solar radiation, fossil
fuel consumption, and technological issues. PV is a sophisticated tech­
nique for the production of renewable energy sources without pollution.
The main drawback faced by NDSSCs in commercialization is low photo-
conversion efficiency and before large-scale production plant-based
DSSCs have several struggles to overcome. A combination of
numerous natural pigments in suitable proportions forms natural cock­
tail sensitizers that act as a viable choice to enhance the stability of
DSSC. From this critical review, improved stability in efficiency was
displayed by root and fruit of stalk of pokeweed (Phytolacca Americana)
sensitizers exploring betalain derivative with efficiency around 3.04%.
Withal photovoltaic sensitization efficiency was indicated using the
SOL-GEL method by binding of anthocyanin pigment of cocktail dyes
with an efficiency of about 3.04%. Although the photo-conversion effi­
ciencies attained with natural dyes are less expensive than synthetic
dyes on a big scale, the findings could help future research with novel
natural colors and optimizing compatible components of solar cells with
sensitizers. Overall, the marketing of this energy-harvesting technology
still offers room for our country’s future development and prosperity.
This article holds auxiliary potential for future researchers in the
fabrication of an ideal DSSC.
CRediT authorship contribution statement
Pooja Prakash: Investigation, Writing – original draft. B. Janar­
thanan: Supervision.

5. Review methodology
The literature review is mainly examined using SCOPUS and Google
search engines. The most relevant and most cited publications were
picked for future analysis based on Scopus data such as common key­
words, subjects, and citations. The natural dye-based DSSC has 506
documents with 392 articles, 16 reviews, 158 conference proceedings, 8
book chapters, and so on. In 2008, it is evident that research on DSSC
started increasing rapidly and started to become a hot topic.
6. Conclusion
This review article epitomizes the sensitizers influencing the per­
formance efficiency of DSSC. Owing to distinct hurdles, metal complex
potent synthetic sensitizers were confronted by the advent of DSSCs.
Photosensitizing elements in DSSC can bestow a tenable remedy for the
subsequent production of energy. Natural derivatives are innocuous,
facilitate disposal, and are nature-friendly as compared to synthetics
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
No data was used for the research described in the article.
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