0D, 1D and 2D Nanomaterials For Visible Photoelectrochemical Water Splitting. A Review

international journal of hydrogen energy xxx (xxxx) xxx
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Review Article
0D, 1D and 2D nanomaterials for visible

photoelectrochemical water splitting. A Review
Chingis Daulbayev a,b, Fail Sultanov a,b,*, Baglan Bakbolat a,b,

Olzhas Daulbayev c
a
Al-Farabi Kazakh National University, Almaty, Kazakhstan
b
Institute of Combustion Problems, Almaty, Kazakhstan
c
Joint Institute for Nuclear Research, Dubna, Russian Federation
highlights graphical abstract
0D, 1D and 2D nanomaterials for

solar water splitting are discussed.
Heterojunction from various
nanomaterials increased efficiency
of hydrogen production.
Water splitting mechanisms of
nanostructured heterojunctions
are highlighted.
article info abstract
Article history: Global energy problems of the 21st century have led to the search for alternative energy
Received 23 May 2020 sources, among which is hydrogen produced via photoelectrochemical solar water split-
Received in revised form ting. Photo-electrochemical water splitting using semiconductor nanostructured materials
26 August 2020 is a progressive method for producing hydrogen. The unique electronic, mechanical, sur-
Accepted 14 September 2020 face and optical properties of nanomaterials make it possible to create photocatalysts with
Available online xxx complex structures of energy zones, allowing the use of a wide range of sunlight and
exerting a positive effect on absorption and scattering of sunlight. This review contains a
Keywords: detailed analysis of current studies aimed at improving the efficiency of photocatalytic
Alternative energy sources systems by using 0D, 1D and 2D nanostructures. Special attention is paid to the mecha-
Photocatalysis nisms of photocatalytic water splitting to produce hydrogen with the help of various
Water splitting nanostructures.
Hydrogen production © 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Solar energy
* Corresponding author. 172 Bogenbay Batyr street, Almaty, 050012, Kazakhstan.

E-mail address: [email protected] (F. Sultanov).
https://doi.org/10.1016/j.ijhydene.2020.09.101
0360-3199/© 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Please cite this article as: Daulbayev C et al., 0D, 1D and 2D nanomaterials for visible photoelectrochemical water splitting. A Review,
International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2020.09.101
2 international journal of hydrogen energy xxx (xxxx) xxx
Contents
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Basic principles of photocatalytic water splitting . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Nanomaterials used in the electrochemical conversion of solar energy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
0D nanomaterials for solar water splitting . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Comparison of activity for hydrogen production by water splitting for photocatalysts based on 0D, 1D and 2D
nanomaterials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Funding . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
are costly and inefficient. Standard hydrogen production

Introduction technologies are based on the following methods: steam
conversion of methane and natural gas [8e10], coal gasifica-
Today, the global increase in the demand for energy has tion [11], electrolysis of water [12,13], pyrolysis [14], partial
brought about numerous investigations in the field of its oxidation [15] and biotechnology [16]. The main drawback of
production, storage and use. The progress achieved in energy these methods is the emission of a significant amount of
production technologies is not enough to fully satisfy demand. carbon dioxide, which negatively affects the environment and
The development of new technologies or improvement of is recognized by the world community as the main factor,
existing methods for producing sustainable sources of clean exceeding all other anthropogenic factors in terms of the
energy are some of the most complicated tasks of modern impact on the planet's climate. According to [17], after two
science [1]. The wide availability of solar energy enables its years of growth, global carbon emissions did not change in
direct use as a source of electricity and heat in various parts of 2019, with a volume amounting to 33 gigatons, despite the
the globe. Solar energy is absorbed by the earth's atmosphere growth of the world economy by 2.9%. This outcome is mainly
in the amount of 3.85 1024 J per year [2]. However, at the due to the reduction of emissions in the energy sectors of
moment, only 2% of solar energy is converted via various advanced economies, owing to the increasing role of renew-
methods [3e6]. This low rate is primarily due to the insuffi- able sources [17].
cient development of technologies for converting solar en- Creation of inexpensive, effective and stable photo-
ergy; however, it also indicates the enormous potential for its electrochemical elements for the conversion of solar energy
use in solving global energy problems. into chemical energy is a promising direction for solving both
Modern technologies for using solar energy include direct energy and environmental problems. However, the effective-
photon energy conversion to electric power (photovoltaic ness of most photoelectrochemical elements is limited owing
cell), water splitting into hydrogen and oxygen under the to their wide band gap [18e20] and the fact that ultraviolet is
action of sunlight (photo-electrochemical cell) and the so- only 5% of the spectrum of solar radiation.
called solar systems. The method of converting solar energy The properties of the photoelectrochemical element (pho-
into electric power is energy efficient; the maximum effi- tocatalyst) such as specific surface area, surface morphology
ciency of solar cells on an industrial scale is 25%. The pho- and optical properties affect the efficiency of hydrogen evo-
toelectrochemical method splits molecules of water into lution. Moreover, the range of light absorption by the photo-
hydrogen and oxygen, converting solar energy into chemical catalyst depends on the width of the band gap of the
energy. Thermal solar systems, the so-called solar collectors, semiconductor, while the location of the valence and con-
convert solar energy into heat, unlike photoelectric and duction bands characterize the potential for hydrogen
photoelectrochemical elements. The efficiency of solar col- reduction and oxygen oxidation, respectively.
lectors depends on the operating temperature and is in the A narrow band gap enables the use of a wide portion of the
range of 30e80%. solar spectrum, but at the same time reduces the redox po-
The development in 1972 [7] of the method for splitting tential and vice versa (Fig. 1) [22]. At the present stage of
water into hydrogen and oxygen using ultraviolet radiation development, hydrogen production by photocatalytic water
has great possibilities for using solar energy for hydrogen splitting has a number of unsolved problems: low catalyst
evolution. Hydrogen energy can serve as a solution for global stability, insufficient efficiency and high cost. These problems
energy problems associated with climate change and pollu- are associated with the physicochemical properties of the
tion. However, the existing hydrogen production technologies
international journal of hydrogen energy xxx (xxxx) xxx 3
photocatalysts [23]. Thus, the development of new materials photoelectrochemical conversion of solar energy into chemi-
and improvement of the existing materials used as photo- cal energy with the help of semiconductors. Photocatalytic
catalysts by changing their chemical composition and struc- water splitting under the action of sunlight using semi-
ture will allow for the efficient use of solar energy in large- conductor materials is based on the absorption of light,
scale hydrogen production. resulting in the formation and transfer of electrons and holes
Recent advances in the field of photocatalytic water split- between energy levels, also called bands: the valence and
ting are mainly associated with the use of metal oxides conduction bands. These charges, electrons (e) and holes
[24e26], sulfides [27e29], noble metal semiconductors [30,31], (pþ), which are formed at the valence band formed at the
and non-metallic semiconductors [32e34]. Titanium oxide- semiconductorewater interface, are involved in the catalytic
based photocatalysts have been widely used in the last redox reaction of oxygen and hydrogen.
decade, and as a result of numerous studies, the efficiency of Water splitting is an endothermic reaction with an
hydrogen evolution has been improved by creating composite enthalpy change of DНо ¼ 238 kJ/mol [46] The general mech-
structures. Although such structures have shown high effi- anism of water splitting is represented by Eqs. (1) and (2) [47].
ciency in the decomposition of water under the influence of Overall water dissociation reaction is
ultraviolet radiation, in the visible range, they are character-
SrTiO3 =hv 1 1
ized by low rates of water decomposition. Perovskite semi- H2 O! O2 þ 2Hþ ; 2Hþ þ 2e /H2 þ O2
2 2
conductor materials have proved to be promising
(1)
photocatalysts that can be used in photocatalytic water
splitting [35e38]. Semiconductors having a low bandgap, such Full water splitting reaction:
as g-C3N4, attract much attention for use as effective photo-
SrTiO3 =hv 1
catalysts. However, g-C3N4 is characterized by a low specific H2 O! O2 þ 4Hþ ; 4Hþ þ 4e /2H2 þ O2
2
surface area with small active centres and a low separation (2)
efficiency of photoinduced charges. Despite numerous studies
of various photocatalytic materials and the proposed methods According to Eqs. (2) and (4) electrons with a total energy of
for improving hydrogen evolution efficiency, the question of 4.915 eV are necessary for forming two hydrogen molecules.
their practical application remains open. Formation of a hydrogen molecule requires energy (2.485 eV),
To date, none of the developed photocatalysts has reached which corresponds to operation with a potential difference of
the level of industrial use for production of hydrogen. How- 1.229 V for the displacement of two electrons.
ever, several review articles [39e45] have focused on theo- According to the fundamental calculations carried out in
retical and practical research for optimization of [48e50] the study of kinetics, the photocatalytic reaction can
photocatalytic systems towards the goal of enabling these be represented as a quasi-first reaction, and its rate equation
systems for water splitting into hydrogen and oxygen at an is [49].
industrial scale. For the possible use of photocatalysts in the
kobs kr1 C1
industrial production of hydrogen, it is necessary to develop r¼ P (3)
1 þ kri Ci
new or improve the existing photocatalytic systems, taking
into account all of the requirements. From this point of view, where kobs is the rate constant, which depends only on the
we believe that the use of nanotechnologies and nano- parameters of the photocatalyst and the conditions of the
materials will not only enable the development of methods for photocatalytic reaction [49].
obtaining and synthesizing highly effective photocatalysts, At low light intensity
but will also help greatly in the development of alternative
kobs ¼ aac k1 I (4)
hydrogen energy. Therefore, in this review, we consider the
latest achievements in the application of nanotechnologies and at high light intensity
and nanomaterials in the development and creation of effec-
k1 ac I
tive photocatalysts based on 0D, 1D and 2D nanomaterials, kobs ¼ aaS kOH (5)
K1 vp
which enable the use of a wide spectrum of sunlight. Special
attention is paid to the mechanisms of photocatalytic water where C1 is the concentration of organics, a is a constant, ac is
splitting using different nanostructured materials. The influ- the surface area of the photocatalyst, k1 is the rate constant
ence of various types of nanomaterials on the mechanism of associated with the formation of electron-hole pairs, I is light
photocatalytic decomposition of water and on their effec- intensity, kOH is the reaction rate constant associated with
tiveness is analysed. In addition, the problems related to hole capture, K1 is the adsorption constant of the compound
photocatalytic water splitting and their possible solutions are on the surface of the semiconductor, and vp is the particle
discussed. In view of the high publication activity in this volume [49].
research area, this review article is not able to cover all pre- In general, a detailed study on the kinetics of photo-
viously reported results. catalytic water splitting has not been completely resolved
because all mechanisms of the photocatalytic reaction need to
be determined, and previous works [48e50] have indicated
Basic principles of photocatalytic water splitting that the kinetic analysis of photocatalytic water splitting will
aid in the creation of effective composite photocatalytic
Fujishima and Honda in their fundamental work published in systems.
1972 [7] formed the basic concepts and principles of the
To convert light into electrochemical energy efficiently, the width of the band gap (3.2 eV), which allows only ultraviolet
photocatalyst must have certain characteristics. First, in order radiation to be absorbed. In fact, the use of almost any semi-
to achieve maximum light absorption, the photocatalyst band conductor material without any modification causes certain
gap should correspond to the photon energy in the visible difficulties in the photoelectrochemical conversion of solar
spectrum of sunlight (2.0e2.4 eV) [45]. In this case, the mini- energy. In particular, for instance, CdS, having a band gap of
mum band gap thermodynamically necessary to initiate the 2.4 eV, is an excellent semiconductor for photocatalytic water
redox reaction is 1.23 eV. Moreover, in view of energy losses splitting due to its use of a wide spectrum of sunlight [109], but
caused by recombination of electrons and holes, changes in its susceptibility to photocorrosion due to the low kinetics of
entropy, kinetic losses, and other factors, the minimum water oxidation does not allow its use in its pure form [110]. In
photon energy should be higher than 1.23 eV [51]. contrast to CdS, the semiconductors Fe2O3 and Cu2O are not
Second, the potential of the bottom of the conduction band subject to photocorrosion but have a high recombination rate
must be more negative than that of Hþ to H2 reduction (0 V at of electrons and holes, thus negatively influencing the effec-
pH ¼ 0), while the top of the valence band must be more tiveness of the photocatalyst [111,112].
positive than the potential of H2O to O2 oxidation (1.23 eV at The efficiency of the existing photocatalysts can be
pH ¼ 0). This renders a positive effect on the efficiency of improved by incorporating nanomaterials such as quantum
oxygen oxidation and hydrogen reduction, providing unhin- dots, nanotubes, nanowires, nanorods and nanosheets.
dered transport of electrons and holes [52,53]. Nanostructured materials can efficiently transfer charges and
Third, the crystallinity of the photocatalysts must be of a can introduce electrons and holes at the waterenanomaterial
high degree to reduce the recombination of electron-hole interface for the oxidation and reduction process. The unique
pairs and ensure their high mobility [54e56]. Recombination properties of nanomaterials provide great opportunities for
of photoinduced charges is the main problem of most photo- the development of photocatalysts with high efficiency for
catalytic systems; electron-hole pairs can recombine, thus water splitting. The combination of different synthesis
exerting a negative effect on the efficiency of hydrogen evo- methods and different types of nanomaterials may enable the
lution. Currently, two methods are mainly used to suppress development of new, effective photoelectrochemical ele-
charge recombination: the use of sacrificial reagents (meth- ments with the desired characteristics and ability to use the
anol, ethanol, or glycerine) and the creation of physical sep- entire spectrum of sunlight.
aration on the surface of the photocatalyst [57].
Fourth, for an effective water-splitting process, the pho- 0D nanomaterials for solar water splitting
tocatalyst must be resistant to the aqueous medium, tem-
perature, and acid-based solutions [58e60]. Moreover, to The use of 0D nanostructures in the form of quantum dots
decompose water into hydrogen and oxygen effectively, the (QD) and nanoparticles as photocatalysts for producing
photocatalyst must have a high specific surface area, which hydrogen under the effect of sunlight is of great interest in
contributes to free diffusion of water molecules [61]. On the view of their unique optical, electronic, and surface properties
other hand, a decrease in the particle size enables the effective [113e115]. Based on these properties, which are largely
transfer of electrons and holes to the surface of the photo- dependent on size, QDs and nanoparticles can be used both as
catalyst [62]. a pure photocatalyst [116] and as a co-catalyst [40]. Through
Finally, from an economic perspective, the main diffi- their experimental work, Grigioni et al. [117] investigated the
culties in the practical application of photocatalysts are pho- dependence of the efficiency of hydrogen generation under
tocorrosion [63e65], the use of expensive semiconductor
materials [56,66] and low stability with multiple uses [67e69],
which all lead to an increased market price of hydrogen.
Nanomaterials used in the electrochemical

conversion of solar energy
In early studies on photocatalytic water splitting, semi-

conductor materials based on binary metal oxides were
mainly used [42,70,71]. Currently, these photocatalysts are
complex composite structures consisting of non-metallic
materials [72e75] alloyed with metal particles [76e80], alloys
of various metals [81e84], carbon structures [85e92] and other
elements. Such complex photocatalytic systems are mainly
based on noble (Pt, Rh, Ag, or Pd) [93e98] and transition (Ti, Fe,
Ni, Cu, or Co) [99e103] metals, as well as on non-metallic el-
ements (B, C, N, Si, Ga, or Ge) [33,104e108].
Historically, the first study of photocatalytic water splitting
was carried out using titanium oxide (TiO2), which still serves Fig. 1 e Processes involved in semiconductor-based
as one of the main components of some photocatalytic sys- photocatalytic water splitting; reprinted from [21] with
tems. A significant disadvantage of this semiconductor is the permission. Copyright 2015 Elsevier.
Fig. 2 e (a) Spectra of UV absorption of four QDs samples with various crystalline dimensions. (b) The rate of release of
hydrogen vs. CdS QDs size under visible light irradiation. Reprinted from [117] with permission. Copyright 2016 Elsevier.
sunlight irradiation on the size of QDs and demonstrated that QDs increased the rate of hydrogen evolution by a factor of 12
2.8 nm CdSe nanocrystals had the highest rate of hydrogen by preventing the recombination of electrons and holes.
production with a quantum efficiency of 0.23% in the visible The use of QDs as co-catalysts not only allows efficient
spectrum without the use of co-catalysts (Fig. 2). separation of charges but also decreases the energy barrier for
This efficiency of QDs as photocatalysts is primarily asso- photocatalytic water splitting. The whole series of metal oxide
ciated with their optical properties of absorption and scat- nanoparticles [120e122] and noble metal nanoparticles
tering of sunlight. Notably, a decrease in the size of QDs leads [46,123e125] serve as examples of QDs used as co-catalysts for
to an increase in the probability of recombination of charges, photocatalytic systems.
since the formed electron-hole pairs are in a localized volume. Along with the QDs of noble metals, metal oxides QDs such
In addition, the development of optimal nanocomposite ma- as CuO [126], Bi2O3 [127], Co3O4 [128], NiO [129] and WO3 [130]
terials modified by QDs will avoid the influence of QDs on were studied as co-catalysts for photocatalytic water splitting
charge recombination and thus enable their use as effective under the action of sunlight. Thus, in the experimental study
photocatalysts in the visible spectrum of sunlight. [131] it was shown that Bi2O3 QDs immobilized on a TiO2-
To that end, in [118] presented the development and cre- anatase nanostructure significantly increased the photo-
ation of a WO3/MoS2 nanocomposite on an FTO substrate for catalytic hydrogen evolution rates. Addition of 0.4% of Bi2O3
the photocatalytic decomposition of water under the action of QDs led to an increase in the rate from 4.20 mmol h1 g1 on
sunlight. This study proved that the introduction of MoS2 bare TiO2-anatase to 26.02 mmol h1 g1 when exposed to
reduced the recombination of electrons and holes in the only sunlight. The contribution of Bi2O3 QDs to the reaction
semiconductor, providing high-efficiency hydrogen evolution. mechanism is presented in Fig. 4, which shows that the
This approach to the creation of two component composite electrons generated when a quantum of light hits TiO2 pass
structures is actively used in the design and production of into the conduction band of Bi2O3 and reduce Hþ to H2.
effective photocatalytic systems. The photocatalytic properties of semiconductors can also
Lakshmana Reddy et al. [119] reported the use of a com- be improved by graphene and carbon quantum dots (GQD and
posite with a more complex structure, TiO2 nanotubes (TNT)
modified with Ni(OH)2 QDs, as an effective photocatalyst for
hydrogen evolution. They clearly presented and described the
reaction mechanism for photocatalytic water splitting on the
composite photocatalyst (Fig. 3). In this case, the presence of
Fig. 4 e The reaction mechanism of Bi2O3@TiO2

Fig. 3 e The mechanism for H2 evolution on Ni(OH)2/TNT heterostructure photocatalyst for H2 evolution under the
from crude glycerol. Reprinted with permission from [119]. action of solar light; reprinted from [131] with permission.
Copyright 2020 American Chemical Society. Copyright 2017 Elsevier.
CQD), owing to their excellent optical and electrical properties selective Pt deposition on thin g-C3N4 nanosheets allowed the
and high chemical stability. The authors of [132] studied the researchers to evenly distribute QDs (sizes ~1e2 nm) with a
photocatalytic properties of TiO2 with the addition of GQD distance of 0.23 nm between the crystal lattices. This work
and reported a 95% percent increase in the efficiency of and other studies have shown that for each type of QDs,
hydrogen evolution over bare TiO2. They showed that a small depending on their chemical composition, morphology and
graphene layer exerted a positive effect on the separation of size, it is necessary to select appropriate methods for pro-
charges when exposed to sunlight on account of the rapid ducing photocatalytic systems.
transfer of the photoinduced charges, thus leading to a high Taking the use of QDs as an example, we can clearly
current density. identify the strategy for QD use in the further development of
The excellent optical properties of CQD make it possible to photocatalytic systems for the production of hydrogen under
use it as an effective collector of sunlight. Huang et al. [133] the action of sunlight. The development of solar hydrogen
reported that modifying CdIn2S4/CdS with CQDs significantly power engineering is only possible with the development and
increases the rate of photocatalytic evolution of hydrogen creation of composites with nanoscale structures. Moreover,
under the action of sunlight. This research showed that CQD functionalized or modified 0D nanomaterials enable the
can be effectively used to improve not only light absorption change of characteristics, such as the band gap, the mobility
but also charge transfer in the photocatalyst, with a of photogenerated charges, and the absorption and scattering
maximum rate of hydrogen evolution of 3177.8 mmol h1 g1 of sunlight which determine the activity of photocatalysts.
(Fig. 5).
Owing to their excellent physicochemical properties, QDs 1D nanomaterials for solar water splitting
can be used in the development and creation of effective
photocatalytic systems for the production of hydrogen. An 1D and 0D nanostructures are widely used in the production of
analysis of the literature indicates that the photocatalytic hydrogen by photocatalytic water splitting under the action of
activity of composite photocatalysts with QDs depends on the sunlight due to the increased efficiency of absorption and
method of their preparation, their composition, the surface scattering of light, which is a consequence of the high ratio of
morphology of the obtained photocatalysts and the size of the length to diameter. Researchers are particularly interested in
QDs [134]. using these 1D structures as nanofibres [136], nanorods (NR)
Zhong et al. [134] studied the effect of QD size on the [137], nanowires [138], porous spheres [139] and hollow
photocatalytic properties of the CdSe QD/WS2 composite nanoparticles [140]. A study [141] demonstrated the possibility
photocatalyst synthesized by mixing. It was demonstrated of using ZnO nanorods, which had a band gap of 3.24 eV, as a
that the highest rate of photocatalytic hydrogen evolution was photocatalyst for water splitting using the visible spectrum of
characteristic of QDs with sizes of 7e8 nm, while an increase sunlight. The use of nanorods leads to fast phototransfer with
in size led to a significant decrease in the efficiency of a photoconversion efficiency of 0.098%.
hydrogen evolution. This size effect was primarily due to the In contrast to ZnO nanorods, the band gap for 1D TiO2
formation of energy levels of the two materials. In this case, structures is 3.2 eV; however, they have a high charge
QDs with a size of 7e8 nm had a higher photocurrent density recombination coefficient. Bashiri et al. [142] reported about
than QDs of other sizes, thus indicating a better separation use of TiO2 nanorods to create a heterostructure for efficient
efficiency of photoinduced charges. photocatalytic hydrogen production. The optimized SrTiO3@-
Zhang et al. in [135] reported the use of graphite carbon TiO2@Fe2O3 heterostructure provided a 716 mmol/cm2 photo-
nitride (g-C3N4) modified with Pt noble metal nanoparticles in catalytic hydrogen production rate and demonstrated the
quantum dot sizes. When using Pt nanoparticles, the stoi- efficient conversion of solar energy with a long charge life
chiometric ratio of released hydrogen and oxygen during (Fig. 6). According to the mechanism proposed in the article,
photocatalytic water splitting under sunlight irradiation was high photocatalytic efficiency is associated with the fast
2:1. This work indicates the influence of the preparation transfer of charges between semiconductors; photoinduced
method for composite structures with QDs. The method of electrons formed as a result of irradiation of the photocatalyst
Fig. 5 e (a) Hydrogen generation rates from photocatalytic water splitting on 1% CQDs/CdIn2S4/CdS with various sacrificial
systems; (b) experimental results of hydrogen evolution by the photolysis of water under the same conditions with different
samples; (c) 1% CQDs/CdIn2S4/CdS hydrogen evolution results for a series of experimental cycles; reprinted from [133] with
permission. Copyright 2020 Elsevier.
Fig. 6 e (a) Study of photocatalytic durability of 0.025 SrTiO3@TiO2@Fe2O3 heterostructure for 25 h. (b) Schematic diagram of
the mechanism for separation of photogenerated electrons and holes in 0.025 SrTiO3@TiO2@Fe2O3 heterostructure;
reprinted from [142] with permission. Copyright 2020 Elsevier.
were displaced in TiO2 due to the energy bands formed composite photocatalyst consists of creating a difference in
throughout the structure (Fig. 6b). the band gap of semiconductors, which significantly reduces
These results similarly proved that the combination of recombination, while TiO2 nanowires facilitate the transport
various types of nanomaterials results in a significant change of photoinduced electrons to the substrate (Fig. 7e).
in the energy zones, which renders a positive effect on the Batista-Grau et al. [145] demonstrated the influence of the
evolution of hydrogen during photocatalytic water splitting. synthesis conditions of ZnO nanowires on their photocatalytic
Similar to TiO2 nanorods, TiO2 nanofibres are actively used properties. This study showed that the hydrodynamic condi-
in preparing efficient photocatalytic systems for generating tions during the anodizing process positively affected the
hydrogen using the visible spectrum of solar radiation [143]. In photosensitivity of ZnO nanowires. However, the use of ZnO
[144], CdS-based photocatalysts were modified with TiO2 nanowires for efficient hydrogen production is limited by their
nanofibres. In this type of composite photocatalyst, CdS al- susceptibility to photocorrosion under prolonged exposure to
lows efficient conversion of a wide spectrum of visible light, sunlight and a high rate of charge recombination. These dis-
and TiO2 nanofibres efficiently separate charges, thus leading advantages can be eliminated by synthesizing a composite
to a sharp decrease in their recombination. The maximum material of nanostructured ZnO particles and carbon nano-
hydrogen release rate during photocatalytic water splitting fibres (CNF). In [146], the mechanism for producing the ZnO/
was 22.44 mmol h1 cm2. The mechanism of operation of this CNF composite photocatalyst was described in detail.
Fig. 7 e (a) Time-dependent photocurrent responses of the PEC cells with the TNA-CdS 1h and TNA-CdS 2h photoanodes
under no bias. (b) Plot of the H2 volume generated as a function of reaction time in the PEC cell with the TNA-CdS 1h and
TNA-CdS 2h photoanodes. (c) Average hourly hydrogen evolution rate as a function of irradiation time in the PEC cell with
the TNA-CdS 1h and TNA-CdS 2h photoanodes. (d) IeV and PeV curves for the PEC cell with TNA-CdS 2h photoanode under
no bias. (e) Schematic illustration of the photoelectrocatalytic production of H2 over the CdS flowers-sensitized TNA film
grown on the Ti substrate; reprinted from [144] with permission. Copyright 2020 Elsevier.
Recently, great interest has been paid to the development been achieved with the use of heteroatomic graphene [157],
of complex photocatalytic heterostructures based on 1D transition metal dichalcogenides [158], layered double hy-
nanomaterials modified with metals [147e149]. For example, droxides [159], graphite carbon nitride (g-C3N4) [160], metal
the efficiency of hydrogen evolution increased during modi- oxides [161], carbides [162], nitrides [163], and other materials.
fication of photocatalysts with metal particles of Ag and Au The main difficulties in using 2D nanostructures as pho-
[97], Cu [150] and Fe [151]. In [152], the CueIn2O3 NRs/TiO2 tocatalysts lie in increasing the efficiency of hydrogen evolu-
photocatalyst was prepared and had a hydrogen evolution tion and improving mass transfer. The efficiency of the
rate of 4390 ppmgh1 cat1. Such a high efficiency of hydrogen photocatalyst depends directly on the width of the semi-
evolution under sunlight irradiation was explained by the conductor band gap; for hydrogen reduction, it must be
photocatalyst structure. In accordance with the mechanism of greater than 1.23 eV, which makes it impossible to use light in
photocatalytic water splitting, photoinduced electrons formed the infrared range. A possible solution to this problem was
on In2O3 were transferred to TiO2 without charge recombi- discussed in [164], where multilayered structures of 2D Janus
nation due to the formed structure of energy bands (Fig. 8). Cu chalcogenides of group III elements including InGaXY, M2XY
nanoparticles captured photoinduced electrons, which then and InGaX2 (M ¼ In/Ga; X, Y ¼ S/Se/Te) were effectively used as
participated in the hydrogen reduction reaction. photocatalysts for water splitting. This study showed that an
Such complex photocatalytic systems based on 1D nano- intrinsic electric field in these multilayered materials reduced
structures have several advantages over the use of QD and the band gap to 1.23 eV for photocatalytic water splitting, thus
nanoparticles. Because of their high specific surface area, 1D increasing the range of absorbed visible light (Fig. 9).
nanostructures effectively absorb and scatter sunlight and On the other hand, separation of photoinduced charges
create active centres for photocatalytic reactions [153]. More- also affects hydrogen evolution. A number of studies have
over, 1D nanostructures provide efficient transfer of charges shown that the efficiency of photocatalytic water splitting
formed at the input of absorption of a quantum of light [154], under sunlight irradiation can be increased hundreds of times
thus positively affecting the rate of hydrogen evolution. In with the efficient separation of photoinduced charges
[66,155,156] it was reported that for 1D nanostructures such as [165e167]. Mahzoon et al. [168] showed that a new type of 1D-
nanowires, nanorods and nanotubes, the charge transfer was 2D g-C3N4 composite photocatalyst possessed a high photo-
more than 200-fold greater than that for nanoparticles. How- catalytic activity due to efficient charge separation (Fig. 10a).
ever, as in the case of 0D nanostructures, the existing methods The heterostructure induced the formation of an electric field
for producing and using 1D nanostructures as photocatalysts at the boundary of 1D and 2D g-C3N4, thus enabling the
or co-catalysts require revolutionary advances for their viable effective separation of photoinduced charges (Fig. 10b).
use in large-scale hydrogen production. The efficiency of photocatalytic hydrogen evolution can
also be increased by changing the energy levels so that the
2D nanomaterials for solar water splitting minimum of the conduction band and the maximum of the
valence band are located close to the redox potentials of
2D nanomaterials refers to a class of nanomaterials that are hydrogen reduction and oxygen oxidation, respectively.
suitable candidates for efficient photocatalytic systems owing Recently, the so-called van der Waals heterostructures formed
to their high specific surface area, remarkable mechanical by successive layer superposition have been actively used for
properties, high activity and photochemical stability. Progress photocatalytic systems [169e171]. In the experimental work of
in the use of 2D nanocatalysts for water decomposition has [172], the electronic and optical properties of a heterostructure
Fig. 8 e The scheme of photocatalytic evolution of hydrogen from methanol-water mixture under visible light irradiation
over Cu nanoparticles loaded onto 1D In2O3 NRs/1D TiO2 nanowires; reprinted from [152] with permission. Copyright 2020
Elsevier.
Fig. 9 e Janus group-III chalcogenides monolayers and bilayers electronic structures and band edge positions. (a) Band
structures of the Janus InGaSTe, Ga2SeTe and InGaSe2 monolayers calculated at the HSE06 functional level. The Fermi levels
are set to 0 eV. (b) Orbital-resolved band structures of the InGaSTe, Ga2SeTe and InGaSe2 Janus bilayers. The dimensions of
the red and blue dots indicate the weights of top and bottom layers, respectively. Band edge positions of the ten Janus
group-III chalcogenides (c) monolayers and (d) bilayers relative to the vacuum levels. The energy of the vacuum level on the
bottom side (layer) was set to zero. The dotted red and blue lines represent the hydrogen reduction potential (Hþ/H2) and the
water oxidation potential (H2O/O2) at pH 0, respectively, reprinted from [164] with permission. Copyright 2020 Elsevier. (For
interpretation of the references to colour in this figure legend, the reader is referred to the Web version of this article.)
Fig. 10 e (a) Comparison of the photocatalytic H2 generation of nano-photocatalysts C3N4 (1D), C3N4 (2D) and C3N4 (1D-2D). (b)
Scheme of the charge transfer and separation in the C3N4(1D-2D) nano-photocatalyst, reprinted from [168] with permission.
Copyright 2018 Elsevier.
based on 2D ZnO and BSe nanomaterials formed using van der and the Bethe-Salpeter equation (BSE), demonstrated superior
Waals forces were studied. The results indicated that the sunlight absorption and scattering properties. Such theoret-
heterostructure has energy bands positions that lead to both ical calculations enable the development of effective photo-
the effective reduction of hydrogen and the oxidation of ox- catalysts with improved properties due to the ability to choose
ygen (Fig. 11b). In addition, the ZnO/BSe heterostructure had a enhanced materials for the heterostructure.
high carrier mobility (2538.16 cm2 V1 s1). The morphology and chemical composition of the surface
Important contributions of the heterostructure develop- significantly affect the efficiency of hydrogen evolution by the
ment are new approaches and principles for creating com- photocatalytic decomposition of water, in particular, the ab-
posite photocatalytic systems. In [173], theoretical sorption and reflection of light and the efficient separation of
calculations of the electronic and optical properties of the photoinduced charges. In the experimental work of [174], ex-
tetragonal heterobilayer ZnS/SnO (BL) were performed. These periments were carried out to assess the effect of various
calculations, conducted on the basis of the GW quasiparticles morphologies of nanoparticles, nanofibres, and aerogels
Fig. 11 e (a) Optical absorption and (b) the band edge positions of the ZnO/BSe vdW heterostructure under applied external
biaxial strain with respect to the potentials of oxidation (O2/H2O) and reduction (Hþ/H2) at pH of 0 and 7; reprinted from [172]
with permission. Copyright 2020 Elsevier.
based on TiO2; all of them showed different photocatalytic evolution, with the exceptions being photocatalytic systems
behaviours. The data indicated that TiO2 nanoparticles were based on g-C3N4 and In2O3, which indicates that they hold
more active for photocatalytic hydrogen evolution because of promise for further development. It should be noted that,
their high specific surface area. However, TiO2 nanoparticles along with the physicochemical and optical properties of
were characterized by low separation efficiency of photoin- photocatalysts, sacrificial reagents have a significant effect; in
duced charges. Because of improved conductivity along the the case of QD Ni(OH)2/TiO2, when various reagents were
axis of the nanotubes, their characteristic morphology fav- used, different values of the hydrogen evolution rate were
oured the separation of photoinduced charges, as evidenced observed. In addition, the works referenced in Table 1 all used
by several works [175e177]. different types of lamps with different wattages for simulating
sunlight.
In contrast to 0D and 1D nanomaterials, 2D nanostructures
Comparison of activity for hydrogen production have some advantages for the development and creation of
by water splitting for photocatalysts based on effective photocatalytic systems for water splitting under
0D, 1D and 2D nanomaterials sunlight irradiation. First, 2D materials are able to effectively
absorb sunlight, which is associated with the depth of light
Composite structures based on various nanomaterials are penetration [180,181]. When interacting with photons, 2D
promising candidates for the development and creation of nanostructures repeatedly reflect and scatter them, and as
efficient photocatalytic systems. This review presents recent already noted above, there are existing photocatalysts based
advances in the application of 0D, 1D and 2D nanomaterials on 2D nanostructures that increase the range of sunlight
for the photocatalytic decomposition of water. absorbed. Second, the preparation of heterostructures from
Table 1 summarizes the hydrogen evolution rate of 2D nanomaterials makes it possible to shift the edges of the
different types of composite photocatalytic systems based on conduction and valence bands, thus leading to a shift in the
0D, 1D and 2D nanomaterials when irradiated with visible potential for hydrogen reduction and oxygen oxidation. Third,
light. Most of these systems have low rates of hydrogen in contrast to photocatalysts based on 0D and 1D
Table 1 e Comparison of various photocatalysts.

Year Catalyst Parameters Hydrogen evolution Reference
2016 CdSe QD (2.5 nm) 300 W xenon lamp, methanol/water 0.09 mmol/h [117]
2018 QD Ni(OH)2/TiO2 Solar light, crude glycerol/water 4.71 mmol/hg [119]
2020 QD Ni(OH)2/TiO2 Solar light, Pure glycerol/water 45.57 mmol/hg [119]
2020 QD Bi2O3@TiO2 Solar light, glycerol/water 26.02 mmol/hg [132]
2017 QD TiO2 Solar light, glycerol/water 4.20 mmol/hg [132]
2020 SrTiO3@TiO2@Fe2O3 NR 500 W halogen lamp, visible light, glycerol/KOH/water 358 mmol/h [142]
2020 CdS@TiO2 NW 300 W Xenon lamp, water 22.44 mmol/hcm2 [144]
2019 CueIn2O3 Nrs/TiO2 Nws 35 car-HID lamp, methanol/water 2196 mmol/hg [152]
2015 In2O3/TiO2/g-C3N4 350 W xenon lamp, visible light, methanol/water 172 mmol/hg [178]
2018 1D g-C3N4 450 W xenon lamp, visible light, triethanolamine/water 93 mmol/hg [168]
2018 2D g-C3N4 450 W xenon lamp, visible light, triethanolamine/water 241 mmol/hg [168]
2017 CdS/Graphene/MoS2 300 W xenon lamp, Na2S, Na2SO3/water 9 mmol/hg [158]
2018 g-C3N4/WO3 300 W xenon lamp, visible light, TEOA/water 1853 mmol/hg [179]
nanostructures for which the transfer of photoinduced

charges occurs in only one direction, photocatalysts based on Declaration of competing interest
2D nanomaterials have several directions for the transfer of
photoinduced charges, which can significantly contribute to The authors declare that they have no known competing
the efficiency of hydrogen evolution. However, it is note- financial interests or personal relationships that could have
worthy that thickness is a critical factor for photocatalysts appeared to influence the work reported in this paper.
based on 2D nanomaterials, as photoinduced electrons must
have sufficient mobility to reach the surface of the photo- references
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0D, 1D and 2D Nanomaterials For Visible Photoelectrochemical Water Splitting. A Review

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international journal of hydrogen energy xxx (xxxx) xxx

Available online at www.sciencedirect.com

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

0D, 1D and 2D nanomaterials for visible

Chingis Daulbayev a,b, Fail Sultanov a,b,*, Baglan Bakbolat a,b,

highlights graphical abstract

0D, 1D and 2D nanomaterials for

article info abstract

* Corresponding author. 172 Bogenbay Batyr street, Almaty, 050012, Kazakhstan.

are costly and inefficient. Standard hydrogen production

Nanomaterials used in the electrochemical

In early studies on photocatalytic water splitting, semi-

Fig. 4 e The reaction mechanism of Bi2O3@TiO2

Table 1 e Comparison of various photocatalysts.

nanostructures for which the transfer of photoinduced

nanotubes from the pyrolysis-catalysis of waste tyres. Int J 2020;261:118254. https://doi.org/10.1016/

[42] He H, Liao A, Guo W, Luo W, Zhou Y, Zou Z. State-of-the-art 2018;225:452e67. https://doi.org/10.1016/

[97] Smiljanic M, Srejic

j.colsurfa.2018.06.039. [162] Kou Z, Zhang L, Ma Y, Liu X, Zang W, Zhang J, et al. 2D

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