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Zno Based Heterostructures As Photocatalysts For Hydrogen Generation and Depollution: A Review
Zno Based Heterostructures As Photocatalysts For Hydrogen Generation and Depollution: A Review
Zno Based Heterostructures As Photocatalysts For Hydrogen Generation and Depollution: A Review
https://doi.org/10.1007/s10311-021-01361-1
REVIEW
Abstract
Energy shortage and escalating pollution are major challenges globally. Heterogeneous photocatalysis is one of the most
cost-effective methods for producing renewable energy and removing pollutants. In particular, ZnO nanostructures are prom-
ising photocatalysts that are economic, stable, and biologically safe. ZnO-based nanoheterostructures have been used for
heavy metal reduction, organic pollutants degradation, photocatalytic hydrogen production, and drug mineralization. Here,
we review ZnO-based nanoheterojunctions as photocatalysts for hydrogen production and pollutant degradation. Hydrogen
production has reached 1200 mol g−1 h−1 using Ce-doped ZnO/ZnS heterojunction, with a 8.5-fold higher efficiency than bare
ZnO. Nearly complete removal of a dye pollutant was achieved in 15 min using hybrid ethyl cellulose-modified g-C3N4/ZnO.
Moreover, ZnO/Ag2WO4/Fe3O4 showed a 152% and 143% higher antibiotic degradation rate than bare A g2WO4 and ZnO,
respectively. We present methods to modify ZnO, including coupling with other semiconductors, metal/non-metal doping,
and carbon-based materials coupling; and methods for charge divergence in binary and ternary ZnO-based nanocomposites.
Keywords Zinc oxide · Photocatalysts · Semiconductor heterojunctions · Binary and ternary nanocomposites · Hydrogen
energy · Environmental remediation
Abbreviations
BCN Boron carbon nitride
* Pooja Dhiman CB Conduction band
dhimanpooja85@gmail.com CIP Ciprofloxacin
* Amit Kumar DRS Diffuse reflectance spectroscopy
mittuchem83@gmail.com g-C3N4 Graphitic carbon nitride
1
School of Physics and Materials Science, Shoolini GO Graphene oxide
University of Biotechnology and Management Sciences, HRTEM High-resolution transmission electron
Bajhol, Solan, Himachal Pradesh 173229, India microscopy
2
International Research Centre of Nanotechnology MB Methylene blue
for Himalayan Sustainability (IRCNHS), Shoolini University, MO Methyl orange
Bajhol, India OTC Oxytetracycline
3
College of Materials Science and Engineering, Shenzhen PE-CVD Plasma-enhanced chemical vapour deposition
Key Laboratory of Polymer Science and Technology, PL Photoluminescence
Guangdong Research Centre for Interfacial Engineering
of Functional Materials, Nanshan District Key Lab RhB Rhodamine B
for Biopolymers and Safety Evaluation, Shenzhen University, R6G Rhodamine 6G
Shenzhen 518055, People’s Republic of China RGO Reduced graphene oxide
4
Center of Excellence for Green Energy and Environmental SEM Scanning electron microscopy
Nanomaterials (CE@GrEEN), Nguyen Tat Thanh SAED Selected area electron diffraction
University, 300A Nguyen Tat Thanh, District 4, TEM Transmission electron microscopy
Ho Chi Minh City 755414, Vietnam
UV Ultraviolet
5
School of Science and Technology, Glocal University, VB Valance band
Saharanpur, India
XRD X-ray powder diffraction
6
Department of Chemistry, College of Science, King Saud 4-NP 4-Nitrophenol
University, P.O. Box 2455, Riyadh 11451, Saudi Arabia
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Fig. 1 Publications on a zinc oxide as a photocatalyst and b removal as promising photocatalyst for the removal of organic pollutants and
of dyes, drugs, and heavy metals by zinc oxide from 2010 to 2021 an exponential increase in the publications is observed
(Source: Scopus, September 2021). ZnO is being effectively utilized
Fundamentals of photocatalysis
Photocatalytic mechanism
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Zinc oxide has lot of applications such as field emission rhodamine B reduction, the synthesized samples were capa-
devices (Hwang et al. 2011), medication administration (Cai ble of reducing Cr (VI) as shown in Fig. 4k. This kind of
et al. 2016), piezoelectric devices (Dagdeviren et al. 2016), experimental evidence suggests to the scientific community
photocatalysis, and so on. ZnO has wurtzite-like structure that particle shape, morphology, and size also play a major
with space group P63mc and more thermodynamically role in photocatalytic processes.
steady at adverse environmental situations (Dhiman et al. In another reported work, zinc oxide was fabricated by
2013, 2020b; Kayaci et al. 2014; Kumar et al. 2016; Sena- co-precipitation technique and this method shows high deg-
pati and Kumar 2018). This varies depending on factors radation capacity of rhodamine B dye as compared to citrate
such as doped atom concentration, flaws, external crystal technique (Giraldi et al. 2012). The precipitation approach
lattice stresses, and temperature and much more. Recently, resulted in a crystalline surface that was free of impurities
Byzynski et al. have demonstrated the impact of morphol- and favourable for catalysis process. The activity of zinc
ogy on the photocatalytic behaviour of ZnO and nitrogen- oxide in comparison with a precursor made by the citrate
doped ZnO nanoparticles synthesized by microwave-assisted approach using zinc acetate was followed by zinc nitrate and
hydrothermal (MAH) and modified polymeric precursor then zinc sulphate, but those were fabricated by the precipi-
method (MPP) (Byzynski et al. 2017). Field emission scan- tation approach were essentially identical. Some synthesis-
ning electron microscopy images of the microwave-assisted related characteristics, such as surface morphologies, aggre-
hydrothermal synthesized samples exhibit the flower-shaped gation of particles, and sintering temperature, as well as the
morphology for both bare ZnO and N-doped ZnO samples. counter anion of the zinc precursor, had no effect on the
But N-doped ones were bigger in size. Similarly, modified degradation kinetics. (Giraldi et al. 2012). In most situations,
polymeric precursor method-synthesized samples exhibited the photo-activity does not grow monotonically as particle
the nanoplate-like morphology and high-resolution images size decreases, and the interaction between size dependency
confirmed the crystalline nature of the synthesized samples and catalytic effectiveness is complex. The correct dimen-
(Fig. 4a–h). An evident impact of particle morphology can sion is required to balance the precise surface area, material
be observed on photocatalytic activity against the degrada- crystalline structure, and surface-bulk carrier recombination
tion of rhodamine B (RhB) under ultraviolet and visible- possibilities to produce optimum performance.
light irradiation (Fig. 4i, j). However, the microwave-assisted
hydrothermal-synthesized samples proved to be better cata- Influence of pH and degradation pathways
lysts than modified polymeric precursor method synthesized
catalysts. The scavenging experiments confirmed the holes/ An extremely difficult task is to interpret pH effects on
oxygen vacancies as the reactive species for the decolouri- photo-degradation efficiency. It is possible to reduce the
zation of rhodamine B (inset of Fig. 4i, j). Similar to the organic pollutant by three possible reaction mechanisms
such as radical attacks on hydroxyl, direct oxidation of
positive hole, and direct decreases of the conducting band
electron. The contribution of each is regulated by the sub-
stratum’s composition and pH (Tang et al. 1997). The pH
of the solution is also controlling the size of the aggregates
generated and the photocatalysts surface charging properties
(Qamar and Muneer 2009). In the highly acidic media, the
zinc oxide particles are also dissociated (El-Kemary et al.
2010). Relying on the solution pH, a catalyst’s surface can
be charged positively or negatively. The amphoteric char-
acteristic of most metal hydroxide surfaces explains this
fact. The zinc oxide surface is negative charged mainly with
adsorbed hydroxyl ions over the pH of 9.3 (Kansal et al.
2007; Ba-Abbad et al. 2013). The pH of the solution is thus
influenced by the adsorption of organic matter to zinc oxide.
Chauhan and his team observed that the photocatalyst has
increased its degradation efficiency with a higher pH (Chau-
Fig. 3 Basic mechanism of photocatalysis involving the role of elec- han et al. 2020b). According to Hayat and colleagues, the
tron acceptors (R) and electron donors (D). In the figure, CB refers negative charge of zinc oxide and the pH solution (pH = 9)
to conduction band and VB refers to valence band. The mechanism as well as the repulsive force between both the ZnO region
shows the possible reduction, oxidation as well as recombination pro-
cess involved in photo-degradation process which takes place when and the pollutant reduced the chances of a process consider-
photocatalyst surface is irradiated with light ably (Hayat et al. 2011). The interpretation of pH effects is
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Fig. 4 Field emission scanning electron microscopy (FE-SEM) thesized by modified polymeric precursor (ZnONp); i photocatalytic
images: a undoped ZnO sample synthesized by microwave-assisted degradation of rhodamine B by zinc oxide samples under ultraviolet
hydrothermal (ZnOm), c N-doped ZnO sample synthesized by micro- light (inset includes rate constant k for various scavengers solutions),
wave-assisted hydrothermal (ZnONm), e Undoped ZnO sample syn- f photo-degradation of rhodamine B by ZnO samples under visible
thesized by modified polymeric precursor (ZnOp), g N-doped ZnO light (inset includes degradation rate constant k for various scaven-
synthesized by modified polymeric precursor; high-resolution trans- gers solutions), k photo-degradation of Cr(VI) by ZnO samples under
mission electron images of ZnO synthesized samples for b undoped ultraviolet light (Reproduced with permission from (Byzynski et al.
ZnO sample synthesized by microwave-assisted hydrothermal 2017) (Copyright Elsevier). Figure differentiates the surface morphol-
(ZnOm), d N-doped ZnO sample synthesized by microwave-assisted ogy and dimensions of bare and doped ZnO nanoparticles synthe-
hydrothermal (ZnONm), f Undoped ZnO sample synthesized by sized by two different synthesis routes along with photo-degradation
modified polymeric precursor (ZnOp), h N-doped ZnO sample syn- graphs observed for degradation of Cr (VI)
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complex in the photocatalytic process due to the numerous (MB), crystal violet and methyl orange (MO), as compared
factors such as catalyst surface interactions, substrates, and to degussa P25 dye. So, ZnO was suggested as dye photosen-
charged radicals and the pH controls on breeding between sitization in visible light, which improve the charge carrier
species (Kansal et al. 2007; Qamar and Muneer 2009; Tale- segregation (Li et al. 2010). In the process, the excited dye
bian et al. 2012). molecules are transferred to covalent band and converting
Furthermore, a variety of processes, such as straight these dye molecules to cationic radical (Reactions 6–10).
reductions in generated electrons or holes and mediated reac- The series of active oxygen species produced by the interac-
tions to hydroxyl radicals, may lead to degradation at various tion of injected electrons with molecular oxygen adsorbed
pH values and operating conditions. The hydroxyl radicals on the surface of zinc oxide. The oxygen species are reacting
formed at the nanoparticles surface, by the reaction between with dye molecules to cause degradation (Vinu et al. 2010;
photo-induced holes and hydroxide ions, are also affected by Li et al. 2013b; Hsiao et al. 2014).
pH, which has a significant impact on photocatalytic activ-
Dye + hv → Dye∗ (6)
ity. Hydroxyl radicals are thought to be the most important
species at neutral or high pH (Jallouli et al. 2017), while
positive holes are thought to be the most important species Dye∗ + ZnO → Dye⋅+ + ZnO(e− ) (7)
that produce oxidation reactions at lower pH (Ahmad et al.
2016). In another reported work, photo-degradation rate of ZnO(e− ) + O2 → O−⋅ (8)
2
cephalexin increases with the increase in the pH from 5 to
9.2 by zinc oxide nanowires (He et al. 2019). Such results H+
are attributed to the reason that h+ are the major carriers at O−⋅
2
⟶ HO⋅2 + HO⋅ (9)
lower pH and OH· at the higher pH values.
Recent work by Le and group is also focussed on pH Dye⋅+ + reactive oxygenated radicals → products (10)
effect on photo-degradation of organic pollutant using ZnO
nanoparticles (Le et al. 2021). Photo-corrosion behaviour of Because visible radiation accounts for 45 per cent of
ZnO at various conditions of light irradiation was analysed. solar energy, while ultraviolet light contributes for less than
The results under dark conditions were prominent indicating ten per cent, any photocatalyst must absorb simultaneously
the weight loss of ZnO as 10.3%, 0.2%, and 2.1% at pH 3, ultraviolet and visible light for photocatalytic efficiency and
7 and 11, respectively. However, under the ultraviolet-light many other realistic applications (Dhiman et al. 2018; Maaz
irradiation, the weight loss of ZnO was much elevated for et al. 2009). It is critical to develop a material that really can
acidic as well as basic conditions. These results indicate the absorb simultaneously ultraviolet and visible light in order
photo-corrosion of ZnO is highly expected under ultraviolet to broaden the range of a photocatalyst.
light. The removal degradation power of ZnO against rhoda-
mine B was found to increase with the increase in pH, and
less removal efficiency in acidic medium was attributed to
the higher solubility of ZnO particles in the solution under ZnO‑based photocatalysts
ultraviolet light condition. To summarize, pH is a crucial for environmental remediation
parameter which plays a significant role in photocatalytic
activity either directly or indirectly. Limitations of ZnO as photocatalyst
Light intensity effects An ideal photocatalyst material should have some important
properties such as low bandgap structure, high redox poten-
To attain high output in photocatalytic reactions, the optimal tial, high photo-constancy, inexpensive, and abundant supply
light intensity must be chosen. At low intensity values (0–20 (Zhang et al. 2010a). The majority of traditional photocata-
mW/cm2), the reaction rate increases linearly, suggesting lyst materials have drawbacks, including poor absorption
that rising light intensity will rise the rate of nanoparticles and photo-corrosion (Lin et al. 2012). Despite its versatility,
photocatalytic reaction, while the propensity of electron and zinc oxide-based photocatalysis is endemic for a variety of
hole recombination becomes insignificant (Mozia 2010). reasons:
Since the separation of charge carriers (electron–hole pair)
competes with recombination at intermediate light intensi- 1. Since zinc oxide does not absorb visible light, it requires
ties (approximately 25 mW/cm2), the square root of light costly ultraviolet light to excite the bandgap.
intensity determines the rate of photocatalytic reaction 2. The difficulties associated with recovering ZnO powder
(Zangeneh et al. 2015). Under ultraviolet–visible light, ZnO from a suspension using traditional filtration
nanoparticles degrade different dyes such as methylene blue
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3. Photo-induced charges recombine quickly, reducing pho- Yu et al. (2016b) documented that the photocatalytic effi-
tocatalytic activity because charge carriers are unable to ciency of nitrogen-, carbon-, and sulphur-doped ZnO is far
enter the catalyst surface. advanced as compared to pure ZnO. The electronic struc-
4. During the photocatalytic reaction, holes are generated tures of pure ZnO show that the valence band is occupied by
and produce photo-corrosion of ZnO. Equation 11 shows Zn 3d (lower) and O 2p (upper) states, while the conduction
less stability and photo-corrosion of ZnO (Han et al. band is similarly occupied by Zn 4 s and 3p states. Because
2010; Chen et al. 2012; Ong et al. 2013): of their p-type structure, both N and C doping have two
main properties: increasing Fermi level electron density and
ZnO + h+ + H+ → Zn2+ + 1∕2H2 O2 (Photo - corrosion) adding vacant states into the bandgap. By adding impurity
(11) states, N and C doping can boost electron excitation, and C
In addition, zinc oxide was dissolved in both acidic and doping can also minimize the distance between the Fermi
basic environment, yielding Z n2+ and Zn(OH)4 (Han et al. level and the conduction band. The increased photocatalytic
2010). As a result, in the case of ZnO, only restrained pH efficiency of S-doped ZnO is due to direct bandgap. When
environments are favourable for the photocatalytic synthesis photo-generated electrons and holes are doped with N, C,
method. To address the aforementioned challenges, scien- or S, they become lighter or heavier, respectively. C dop-
tists are working to improve the surface-electronic struc- ing <<N doping << S doping << pure ZnO are all used
ture of ZnO, which primarily entails changing the ZnO to calculate electron–hole pair with increase in the concen-
defect chemistry to benefit photocatalysis in ambient con- tration recombination frequencies (Yu et al. 2016b). It was
ditions. As a result, in the last few years, this method has found that with increase in the concentration of dopant, the
made high progress as compared to other methods, but there bandgap of zinc oxide gets decreased (Dhiman et al. 2017).
are more problems which remain to be addressed become Photocatalytic activity is expected to be low because ZnO
more effective and broadly received, especially for indus- nanoparticles have an optical bandgap in the ultraviolet
trial applications. One of the practical challenges with this range. However, because of the small bandgap, the absorb-
technology that needs to be addressed is long-term photo- ance changes in the visible region as the Fe concentration
stability. Furthermore, surface architecture and crystallinity rise. When Fe cations are substituted in the ZnO lattice,
are examples of material design parameters are critical and the atmosphere of Zn varies, affecting the electronic struc-
must be taken into account during photocatalyst process- ture and generating oxygen vacancies. Because of trapping
ing. These parameters decide a material’s light absorption of electrons via oxygen vacancies and dopant ions, elec-
behaviour, and the key challenge for investigators is to main- tron–hole pair recombination is decreased. Electron–hole
tain absorption of light from the solar range. Various ways pairs production takes place as a result of sun exposure.
have been investigated in this area, including doping with Electrons are present in the valence band, and these elec-
metals/non-metals, interfacing with carbon-based materials, trons are energized and transferred to the conduction band.
coupling with certain other semiconductors, and so on (Ong Electron–hole recombination is predicted as the bandgap
et al. 2018). These strategies can successfully boost ultravio- narrows. The donor states caused by oxygen vacancies and
let active photocatalysts’ visible-light absorption, resulting intermediate zinc atoms are examples of defect locations,
in improved photocatalytic efficiency. as well as the acceptor states caused by zinc vacancies and
intermediate oxygen atoms are commonly due to the photo-
Doped ZnO as photocatalyst catalytic action of undoped ZnO.
A recent work was focussed on theoretical and experi-
The drawbacks of using ZnO as a photocatalyst have been mental assessment of dopant impact on photocatalytic activ-
addressed in previous parts of this study. Poor photocatalytic ity of ZnO (Mohsin et al. 2021). Response surface methodol-
performance and less stability due to photo-corrosion are ogy models were applied for the optimization of the various
the key disadvantages of pure ZnO nanomaterials. To over- reaction parameters involved in the photo-degradation pro-
come with these drawbacks, ZnO is proposed to be doped cess of humic acid using Fe-doped ZnO photo catalyst. The
with other elements (Ullah and Dutta 2008). Doped ZnO has formation of ·OH radicals via dissociation or reduction of
better photocatalytic properties as doping which can influ- H2O2 was linked to the increased rate of degradation with
ence both electrical and physical properties of the materials. increasing H2O2 concentration (Fig. 5a). The effect of pH
From this perspective, doping with non-metals is an appeal- over the humic acid degradation was checked for the syn-
ing technique for semiconductor bandgap manufacturing, as thesized catalysts (Fig. 5b, c, f). Under the acidic pH condi-
it can change the visible light field’s threshold wavelength. tions, humic acid degradation was found to increase under
Small bandgap is incredibly useful for effectively using the the sunlight illumination. In contrary, under basic condi-
solar energy spectrum (Anandan et al. 2007). tions, the phenomenon was reversed. This behaviour was
explained in terms of protonation of catalyst surface under
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Fig. 5 3-dimensional surface plots of response surface methodology from (Mohsin et al. 2021) (Copyright Elsevier). Figure shows the
models showing the impact of irradiation time and H 2O2 (a), H2O2 impact of variable reaction parameters on the photo-degradation effi-
and pH (b), irradiation time and pH (c), H2O2 and humic acid con- ciency of Fe doped ZnO for the degradation of humic acid. The deg-
centration (d), Humic acid concentration and irradiation time (e) and radation efficiency gets increased for Fe-doped ZnO deposited over
humic acid concentration and pH (f). (Reprinted with permission ceramic plate as photocatalyst
acidic conditions and accumulation of more negative charge which thereafter decreases for some specific concentration.
on the surface under basic conditions. These experiments Another experiment was also performed to study the influ-
confirmed the optimized pH of 7 for such experiments. ence of irradiation time on the photo-degradation rate of
Figure 5d shows the impact of humic acid concentra- humic acid (Fig. 5e). Experiment revealed that degradation
tion variation on the photo-degradation rate. Results indi- rate increases only for the 5-h sunlight irradiation and after
cated that initially there was increase in degradation rate that no change was observed. However, under the optimized
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reaction parameter conditions, Fe-doped ZnO deposited over Type II In type II nanohetrojunction, the bandgaps of two
ceramic plate exhibits photo-degradation efficiency two semiconductors, for example, A and B, are aligned. So, in
times higher than pure ZnO. case of B semiconductor conduction band is negative than
In a reported work, researchers have synthesized carbon- A semiconductor, and in case of B semiconductor valence
doped zinc oxide in which the C atoms were replaced with band is less positive than A semiconductor. As a result, the
Zn ions, which was confirmed by X-ray photo-electron spec- charge carriers are transferred from conduction band of A
troscopy investigation (Zhang et al. 2015). Carbon-doped semiconductor to B semiconductor and holes are transferred
ZnO is capable of absorbing more light and results into low- from valence band of A semiconductor to B semiconduc-
ering of the bandgap between 3.19 and 2.72 eV (bare ZnO). tor, and the results show the significant charge segregation
The lower bandgap energy of carbon-doped ZnO improves throughout the photocatalytic procedure (Kumar et al. 2020).
the photocatalytic efficiency. Furthermore, the reduced The p–n junction is the Type II system, which is made up
photoluminescence strength in C-doped ZnO confirms the of alternating p- and n-type photocatalysts (Moniz et al.
inhibited recombination of photo-generated charge carri- 2015; Xu et al. 2015). By virtue of the differences in elec-
ers. Carbon-doped ZnO is prepared for the degradation of tronic structures between p- and n-type materials, photo-
methylene blue dye under visible-light irradiation. By elimi- excited electrons accumulate at the n-type side’s coupling
nating the adsorbed oxygen in the photocatalytic mixture, contact and holes accumulate in the p-type component. As
photo-generated electrons from conduction band produce a result, just at the interface, electrons and holes create a
oxidizing O2·, which is suitable for the improved degrada- gradient, encouraging charge carrier transit while inhibiting
tion in case of carbon-doped ZnO nanomaterial. Because of photo-generated electron and hole recombination, therefore
doping, segregation of photo-generated charge carriers is encouraging efficient solar energy conversion. (Zhao et al.
improved, where active OH· produced from H 2O and H2O 2016).
are the region of degradation (Zhang et al. 2015). Basically, Z-Scheme system The Z-scheme system, which is based
ZnO doped with metal or non-metal catalysts shows high on the photosynthesis in plants, is a useful method for
photocatalytic performance, so they are beneficial for hydro- photo-induced charge segregation. To align the bands in
gen generation and environmental applications. Doped-ZnO this method, two semiconductors are used. To produce the
catalysts also show the absorption of broad range of solar separation of photo-induced electron–hole pairs and water
radiations. As a result, doping with metals and non-metals to splitting, a photocatalyst with water reduction or oxidation
boost visible-light activity in ZnO photocatalysts has risen in activity can be employed to one side of the Z-scheme (Ma
popularity. Recently reported various doped ZnO nanoma- et al. 2017a; She et al. 2017). Charge transfer occurs in these
terials along with their photocatalytic efficiencies, proposed heterojunctions in the same way that it does in type II hetero-
mechanisms and irradiation time are summarized in Table 1. junctions, with electrons accumulating in one semiconduc-
tor's conduction band and holes accumulating in the other,
ZnO coupled with other semiconductors favouring photocatalytic activity.
Schottky junction system In this system to arrange the
A nanoheterojunction is created when two semiconductor Fermi energy levels, electrons can move from the pho-
materials are combined, affecting the surface structure and tocatalyst to the co-catalyst over the interface (Ran et al.
charge transfer characteristics of the resulting photocata- 2017). As a result, the co-catalyst has an overabundance of
lytic system and allowing for broad spectrum absorption. negative charges, whereas the semiconductor has positive
(Liu et al. 2014b). Type I, Type II, Z-Scheme system, and charges close to the interface. As a result, a space charge
Schottky junction system are the several types of photocata- layer forms at the interface, and the semiconductor’s con-
lytic systems (Su et al. 2018). Figure 6a–d contains diagram- duction band and valence band are bent upward. The crea-
matic representation of all four types of heterojunctions. tion of a Schottky junction between the semiconductor and
Type I In a type I nanoheterojunction, the valance band the co-catalyst is caused by this space charge layer. As a
and conduction bandgap of a semiconductor having a large result, the Schottky junction can behave as an electron trap,
band are capable of enclosing the conduction band and capturing photo-induced electrons efficiently and increasing
valence band levels of a semiconductor with less bandgap. photocatalytic activity (Meng et al. 2013; Jiang et al. 2015;
Photo-generated charge carriers can flow across advanta- Xu et al. 2015; Peng et al. 2016; Wang et al. 2016b; Ma et al.
geous potentials, such as electrons down potential and holes 2017b; Ran et al. 2017).
up potential. Photo-generated charge carriers build on one
of the semiconductor materials in such nanoheterojunctions,
which is not conducive to photocatalytic activity (Jiang et al.
2015).
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Ce-doped ZnO Ultraviolet Direct 99.5% and 70 min Kumar et al. (2015)
red-23
Mn-doped ZnO Solar and Orange II 75% and 240 min Achouri et al. (2016)
visible
light
Na-doped ZnO Solar light Rhoda- 84.4% and 120 min Tabib et al. (2017)
mine B
(In-Mg-doped ZnO Ultraviolet Orange II 88.5% and 20 min Benzitouni et al. (2018)
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Table 1 (continued)
Photocatalysts Light Targeted Degradation effi- Mechanism References
source pollutant ciency/irradiation
time
Gd-doped ZnO Visible Methylene 93% and 90 min Selvaraj et al. (2019)
light blue
Na-doped ZnO Sunlight Methylene 99.5% and 1.5 h Elsayed et al. (2020)
blue
Reproduced with the permission from (Kumar et al. 2015) Copyright Elsevier, (Achouri et al. 2016) Copyright Elsevier, (Tabib et al. 2017)
Copyright Elsevier, (Benzitouni et al. 2018) Copyright Elsevier, (Dhiman et al. 2019) Copyright Elsevier, (Selvaraj et al. 2019) Copyright Else-
vier, (Elsayed et al. 2020) Copyright Elsevier. The table presents some previously reported doped ZnO nanomaterials which have been utilized
as photocatalyst for the degradation of some specific organic pollutants. The degradation efficiency and plausible mechanism involved in the
degradation process are also illustrated
CB conduction band, VB valence band, MB methylene blue, RhB rhodamine B, ORII orange II
Heterojunctions based on ZnO/carbonaceous right location of band edges implies that graphitic carbon
materials nitride is a great alternative for hydrogen production (Martin
et al. 2014). g-C3N4 nanosheets are often utilized as visible-
As we all know, carbon is a reasonably safe, inexpensive, light photocatalysts for the degradation of organic/inorganic/
and stable element in nature. Carbon nanostructures can pharmaceutical contaminants or water disassociation (Chen
be used as supports for ZnO and their co-catalysts because et al. 2014). Graphitic carbon nitride has also been investi-
they have large specific surface area, chemical stability, gated as a potential metal-free photocatalyst due to its strong
and conductivities (Low et al. 2016; Kumar et al. 2018c; absorption of visible light and a bandgap. However, the
Bahuguna et al. 2019; Sengottaiyan et al. 2019). Addition- applicability of graphitic carbon nitride (g-C3N4) is limited
ally, the dimensionally restricted carbon-based materi- by the photo-generated charge carriers’ rapid recombination
als help with semiconductor nanostructures, which is ben- rate (Mousavi and Habibi-Yangjeh 2016, 2017).
eficial for improved photocatalytic applications (Low et al. Sun et al. used a simple calcination procedure to make
2016). g-C3N4/ZnO composites with different ZnO weight ratios,
Because of features such as a good bandgap, limited which resulted in a threefold increase in methyl orange deg-
visible-light mobility, and great chemical and thermal radation (Sun et al. 2012). Yang et al. (Yang et al. 2020) pre-
robustness, graphitic carbon nitride is a unique material for pared g-C3N4/ZnO nanosheets for methylene blue dye deg-
photocatalysis (Kumar et al. 2018a, 2021a). Graphitic car- radation. Under visible-light irradiation, the optimized ethyl
bon nitride does have a bandgap of 2.7 eV that enables it cellulose-modified g-C3N4 was inserted in ZnO nanosheets
to absorb visible light efficiently (Kumar et al 2021b). The as a co-catalyst to degrade methylene blue. These optimized
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Fig. 7 Charge transmission in
a zinc oxide-graphene quantum
dot heterojunction during ultra-
violet irradiation for pollutants
deterioration (Reproduced with
permission from Kumar et al.
2018b) Copyright Elsevier.
The figure also demonstrates
the hydroxyl radical generated
through degradation of hydro-
gen peroxide as active species
taking part in mineralization
process
to pure ZnO. Additionally, it shows that to achieve an ele- hydrothermal and sequential hierarchical assembly to create
vated rate of deterioration, both the photoluminescence lifes- multi-component heterostructures (Zhou et al. 2015).
pan and the material’s surface area played a key role, and Figure 9a–c clearly shows the strong interaction between
both should be high/optimal. The rate of recombination of zinc oxide or copper oxide, according to high-resolution
produced charged carriers is inversely related to the mate- TEM images, elemental mapping, and transmission elec-
rial’s lifespan. As a result, grapheme–ZnO nanocomposites tron microscopy analysis of C ux/ZnO@Au heterostructure.
could be a promising choice for photocatalytic applications, In addition, for solar spectrum applications, a blend of wide
particularly in environmental protection. All major findings and narrow bandgap semiconductor ZnO (3.2 eV) and CuO
including complete band structure and plausible mechanism (1.4 eV) is being used. Under visible-light irradiation, the
are shown in Fig. 8a–c. hybrid nanostructures were employed for water splitting
photocatalytic applications (Zhou et al. 2015). Similarly,
zinc oxide/tin oxide (ZnO/SnO2) nanocomposites were fab-
Coupling of ZnO with metal oxides ricated by two facial approaches: sol–gel and electrospinning
approach for the photocatalytic decomposition of different
ZnO clubbed with the number of metal oxides is found to be organic contaminants. ZnO/SnO2 nanocomposites show
most promising host material for photocatalysis. Recently, high photo-degradation percentage of rhodamine B organic
methyl orange dye degradation was driven by the ternary contaminant as compared to ZnO and SiO2 nanoparticles,
nanocomposite ZnO/TiO2–SnO2 produced via sol–gel tech- because of its stability and large surface area (Zhang et al.
nique. The prepared sample was calcined at 500 °C for 3 h. 2010b). A well-known approach for improving photo-deg-
At high calcination temperatures (650–700 °C), the produc- radation activity is the combination of wide bandgap and
tion of low active phases decreased the composite’s activ- narrow bandgap structures. The n-ZnO/p-CaFe2O4 hetero-
ity (Yang et al. 2012). ZnO/TiO2, a binary nanocomposite junction nanocomposite was prepared via ball milling tech-
was synthesized via tape casting and lamination method and nique and has been proposed for photocatalytic applications.
calcined at 600 °C and 700 °C for 3 h reported by Konyar The timing of ball milling altered the photocatalytic perfor-
and team. At low temperature, i.e. 600 °C, inter-dispersal mance. The n-ZnO/p-CaFe2O4 nanocomposite showed great
between ZnO and T iO2 decreased and results into production catalytic activity as compared to pure zinc oxide nanoparti-
of binary compounds, which are very effective for photo- cles. The photo-induced electron–hole pairs were segregated
catalysis (Konyar et al. 2012). Therefore, calcinations tem- by the internal electric field as the p–n junction photocatalyst
peratures play a major factor for the fabrication of desired n-ZnO/p-CaFe2O4 was formed, and the photocatalytic activ-
material and the morphology of materials has an important ity is considerably increased (Shifu et al. 2009).
factor in regulating photocatalytic activity, as per the litera- Recently, Yu and group (Yu et al. 2019) have coupled
ture survey (Yu et al. 2014b). From this perspective, Zhou ZnO with metal oxide (CuO, F e2O3 and C o3O4) and the
and group fabricated Cux/ZnO@Au nanocomposite using films were fabricated. CuO/ZnO, F e2O3/ZnO, and C
o 3O 4/
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Fig. 8 Mechanism of photocata-
lytic reactions taking place in
a zinc oxide; b graphene-zinc
oxide; and c band diagram for
graphene-zinc oxide (Repro-
duced with permission from
Beura and Thangadurai 2017)
Copyright Elsevier. The figure
shows the band alignment of the
conduction as well valence band
along with the possible charge
flow taking part in mineraliza-
tion process. In figure, CB
refers to conduction band and
VB refers to valence band
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reports in the literature that describing the use of metal semi- from higher energy level to low energy level until the equi-
conductor nanostructures for hydrogen production and envi- librium level is reached. It means, the diminution layer is
ronmental applications such as photo-degradation of various generated when p–n interaction happened, which is separate
contaminants (Kumar et al 2022). from the development of an electric field by the junction of
Hydrothermal fabrications followed by ultrasonic n-type and p-type semiconductors (Chang et al. 2016).
treatment were used to create Pt-loaded ZnO-RGO (Zinc For that reason, the photogenerated electrons and holes
oxide-reduced graphene oxide) nanocomposites. The ideal will diffuse out of the diminution layer due to the electric
deposition of platinum nanoparticles in zinc oxide-reduced field generated by the stimulation of negative and positive
grapheme oxide nanocomposites was 5 wt.%, and the charges on the p-sides and n-sides (Mamba and Mishra
associated catalyst improved photocatalytic properties for 2016). Furthermore, the photoinduced electrons/holes cou-
4-nitrophenol reduction. Under the same testing conditions, ples are separated by the integrated electrical force. As a
the improved ZnO-RGO-Pt nanocomposite had six times result, photogenerated electrons shifted to the semiconduc-
higher photo catalytic properties as compare to its binary tor with more positive in conduction band, and on the other
counterpart. The Pt loading causes the creation of a Schottky side holes in the heterojunction arrangement shifted to the
contact between ZnO and Pt, where photogenerated charge semiconductor with more negative in valence band (Wang
transfer occurs from ZnO's conduction band to Pt nanopar- et al. 2014a). Charges are transported in a certain manner
ticles, enhancing the reduction of 4-nitrophenol as shown depending on how the two unitary semiconductors are ori-
in Fig. 10d. As a result, adding Pt nanoparticles to a hetero- ented. This inhibits photoinduced electrons/holes couples
junction improves charge transfer, which is favourable for from recombining and thereby increases the total charge
the photocatalytic activity (Kumar et al. 2018d). In another transfer performance in the reaction and increases the charge
work, Au–ZnO nanocomposites show high photo-degra- carriers’ lifespan.
dation efficiency of rhodamine B dye as compared to pure As a result, a favourable environment is created for the
ZnO nanostructures. There are several factors that indicate designing of most efficient photocatalysts for employment
that Au-ZnO nanocomposite has high photocatalytic activ- in photocatalysis reactions (Li et al. 2015d). There are
ity such as large surface area, interspaces, stability of the numbers of benefits of p-n heterojunction: charge transfer,
material, and increased charge segregation. Furthermore, the long life, segregation of spatially unsuitable reduction and
high efficiency of the Au-doped ZnO hybrid nanostructure oxidation reactions and many more, which is suitable for
is highly recommended nanomaterials for environmental many applications in the field of environment. As a result, a
applications (Ahmad et al. 2011). carefully designed ZnO-based p–n heterostructure can pro-
According to the studies discussed above, combining vide advantageous photo-electrochemical applications. ZnO
ZnO with metal nanoparticles has a synergistic impact was formerly thought to be a photocatalytic semiconductor
that improves visible-light absorption and charge carrier that responds to ultraviolet light. Broad bandgap (3.37 eV),
segregation. good catalytic activity, cheap manufacturing costs, and envi-
ronmental friendliness, all of these properties make ZnO
ZnO‑based binary nanoheterostructures suitable candidate (Verma et al. 2018). Nevertheless, by
virtue of its lack of ability to absorb visible light, which
To get the desired application from the nanoheterostructure accounts for ̴ 43% of the spectrum of the sun its applicability
depends upon the surface charge sharing (Liu et al. 2019b) is limited. The employment of ZnO as a solar-light recep-
which can control the energy bandgap of the nanohetero- tive photocatalysts is quiet restricted. As a result, modify-
structure, thus enhancing the quality photocatalytic proper- ing the ZnO surface to improve its optical characteristics is
ties of the prepared material. The amalgamation of n-type required. For the preparation nanocomposite, ZnO was com-
and p-type semiconductors for nanocomposites gives a novel bined with small-size band-gap semiconductor because this
strategy for merging distinct physicochemical properties of type of nanocomposite photoluminescence emission inten-
particular compounds into a single component system (Yu sity when increasing light absorption (Mittal et al. 2016),
et al. 2014a). The p–n-type heterojunction is a heterojunc- which is a measure of electron–hole recombination control.
tion in which n-type semiconductor serves as donor and a CuO semiconductor is believed to be an ideal choice for
p-type semiconductor is considered as acceptor (Kumar et al p–n heterojunction synthesis with ZnO (Taufik et al. 2015;
2021c). In p-type semiconductors, where holes are the domi- Wang et al. 2017a). Due to the high recombination rate of
nant carriers, and the Fermi level resides in close proximity the photogenerated electrons/holes couples, pure CuO has
of valence band and in case of n-type semiconductor the a reduced photocatalytic activity. As a result, when charge
Fermi level is close to conduction band. The concentration carriers are shifted from CuO to ZnO, the amalgamation of
of electrons as carriers is greater than that of holes (Wu et al. CuO and ZnO could result in highest catalytic efficiency.
2019). The Fermi level of these heterojunctions is changed Because ZnO’s conduction and valence bands are lower than
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Environmental Chemistry Letters
those of CuO’s, this is the case, making electron–hole pair degradation was substantially higher than that of ZnO and
transfers a thermodynamically advantageous procedure. Pal SnO2 nanofibres fabricated using electronspun. Due to their
et al. (2015) demonstrated a simple and practical technique one-dimensional nanostructural characteristics, the mixed-
for large-scale production of ZnO/CuO heterostructures and oxide samples were efficiently recycled without degrad-
used for methylene orange and rhodamine B dye degrada- ing their photoactivity (Zhang et al. 2010b). Zhang et al.
tion. Nanocomposite heterostructures produced from ZnO/ (2012) developed ZnO/CuO composite with colloidal car-
CuO nanoparticles showed higher photo-degradation activ- bon spheres. The samples were more successful than pure
ity compared to their pure counterparts. This nanocomposite ZnO hollow spheres at photocatalytic decolourization of a
could degrade 98% of methyl orange dye within 280 min, methylene blue aqueous solution (Zhang et al. 2012). There
and removal efficiency of rhodamine B dye is 98% within are number of components that influence the heterojunction
400 min when exposed to visible light. photocatalysts performances such as pH, concentration of
Cho et al. (2011) fabricated ZnO/ZnSe heterostructures pollutant, and photocatalysts concentrations. One of them is
by simple solution-based surface-modification reactions. the pH of the solution, which has a considerable impact on
When compared to pure ZnO structures, the visible-light the photocatalysts surface charge characteristics (Zeghioud
photocatalytic activities of ZnO/ZnSe heterostructures were et al. 2016). In 2019, Yi and group prepared ZnO@Ag3PO4
much greater due to the absorption of visible light by ZnSe core–shell nanocomposite by combining three methods, i.e.
nanoparticles and the enhanced charge-carrier transport of magnetron sputtering, hydrothermal growth, and stepwise
type II heterostructures. An ecologically benign semicon- deposition. Solar cells, expeditious photoelectric switches,
ductor ZnSe was discovered to be an ideal for enhancing sensors, and other fields can be accessed from ZnO@
the photocatalytic capability of ZnO, because of its nar- Ag3PO4 nanocomposite heterostructure (Yi et al. 2019).
row bandgap, i.e. 2.67 eV and its valence or conduction Chiu et al. (2010) used a seed-mediated growth approach
band arrangements. These advantages of ZnSe account for to create F e3O4/ZnO core–shell heterostructures in non-
its potential to improve ZnO-mediated photocatalysis by hydrolytic states with regulated thermal pyrolysis of zinc
increasing the use of energy source while reducing the rate acetate, allowing for the development of a ZnO layer on the
of electron–hole recombination. surface of Fe3O4 seeds. A 0.6 T magnet can simply separate
Dhiman et al. (2020b) prepared ZnO/Fe 2O 3 binary this Fe3O4/ZnO core–shell heterostructure, and it has a lot
nanocomposite by using solution combustion method and of potential as a photocatalysts.
reported that ZnO/Fe2O3 binary heterojunction nanomaterial Height et al. (2006) state that the Ag/ZnO nanocompos-
is stable and reusable as well as capable of photocatalytic ites manufactured by flame pyrolysis spray technique and
contaminations removal in both visible and natural light. wet chemical technique were investigated for photocatalytic
The junction has the best photoreduction efficiency, i.e. 88% destruction of methylene blue dye under ultra violet irradia-
within 90 min for Cr (VI) under visible light and 100% dimi- tion. The crystalline sizes of Ag/ZnO of two different meth-
nution in 45 min using tartaric acid as a conciliatory agent. ods were identified as 5–20 nm and 8–25 nm, respectively.
The effects of scavengers and sacrificial agents indicate that With the ideal condition of 3 wt.% Ag/ZnO in a 5/5 flame
photogenerated electrons were the most active species, fol- condition the Ag/ZnO manufactured by flame pyrolysis spray
lowed by super oxide radical. Under visible light and solar technique demonstrates greater photocatalytic efficiency as
light, the conduction band edges have enough capacity to compared to Ag/ZnO manufactured by wet chemical tech-
reduce hexavalent chromium. The photoluminescence and nique (Height et al. 2006). The photocatalytic performance
electrochemical impedance in the heterojunction indicate of ZnO–TiO2 nanohybrids was checked for the destruction
low recombination and high charge segregation. There is of three organic compounds, i.e. oxytetracycline (OTC),
the transport of electrons from F e2O3's conduction band to methylene blue, and rhodamine 6G (R6G). Under sunlight
ZnO's with a high sufficient negative potential to decrease irradiation, the photocatalytic performance of ZnO–TiO2
Cr (VI). In addition, flaws such as F e2O3's low conductiv- nanoheterojunctions was found to be extraordinarily high,
ity and ZnO’s high bandgap are eliminated in the junction. with 90.3% of oxytetracycline, 98.4% of methylene blue dye,
This research found that common semiconductors such as and 81.3% of rhodamine 6G dye in only 8 min, 6 min, and
ZnO and F e2O3 have sufficient possibility in double roles as 30 min, respectively. Due to extreme high density of the
electrochemical sensors or photocatalysts, with the optimum synergistic effect between ZnO and T iO2, the recombination
production when the circumstances and ratios are optimized rate is effectively reduced and the charge separation process
(Dhiman et al. 2020b). is enhanced, leading to enhanced photo-degradation activity.
A combination of the sol–gel procedure and electro- The results of this work show that diverse morphologies of
spinning technology was used to make one-dimensional ZnO–TiO2 nanohybrids modulate the heterojunction density
ZnO/SnO2 nanofibres (Zhang et al. 2010b). The compos- (Singh et al. 2020) (Fig. 11a–f). The possible mechanism is
ite nanofibres’ photocatalytic activity for rhodamine B demonstrated in Fig. 11g.
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studied for photocatalytic applications (Rong et al. 2016). In was preserved in these cases, resulting in strong materials
visible-light irradiation for 48 min, the ciprofloxacin (CIP) for photocatalytic water splitting. The enhanced capability
removal rate of ZnO/Ag2O/pg-C3N4 was 97.4%. On the other to collect catalytic synergy owing to optimistic organiza-
side, the removal efficiency of pure ZnO, pg-C3N4, Ag2O, tion between the carbon-based compounds (for example,
ZnO–Ag2O, and was 8.2, 25.4, 42.3, and 69.4%, respec- graphene oxide and g-C3N4) and analogues were credited
tively. The visible-light-assisted photocatalyst (g-C3N4) was for the ternary photocatalysts for remarkable photocatalytic
selected as the ally material of zinc oxide-silver (I) oxide— activity.
in order to establish a ternary combination system, which is Much of the present literature on photocatalysts con-
critical for improving the efficiency of photocatalytic perfor- centrates on the segregation and conveyance of photo-gen-
mance (Rong et al. 2016). ZnO/ZnS/graphene oxide (Opoku erated charge carriers. Developing the interface between
et al. 2017), ZnO/ZnCr2O4/g-C3N4 (Patnaik et al. 2017), and the used semiconductors is an excellent way to progress
ZnO/ZnS/g-C3N4 (Wang et al. 2014b) are some additional the segregation, duration, or reduce recombination rate.
newly produced visible-light-driven photocatalysts that have As a result, there are several studies which have been con-
shown high photo-activities for effective hydrogen evolution centrated for the creation of n–n or n–p heterojunctions
in the visible area. The electronic band structure of ZnO by connecting two or more than two semiconductors that
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Environmental Chemistry Letters
induce inner electric fields and they can successfully man- and much significant recombination of carriers in C u2O (Ren
age electron–hole photogeneration (Wang et al. 2017b). et al. 2015).
In recent times, investigators have found that combining a Golzad-Nonakaran and Habibi-Yangjeh (2016a, 2016b)
n–n-type heterojunction with a p-type junction or n-type fabricated ternary ZnO/Ag3VO4/AgI nanocomposite for
semiconductor junction, they get p–n–n-type or n–n–n- the photocatalytic applications. The increased activity was
type heterojunctions with much great catalytic efficiency attributable to the nanocomposite's creation of tandem n–n
as compared to p–n or n–p heterojunction. As a result, heterojunctions, which reduced electron–hole recombina-
much work is focussed on developing new and simple tion. Ultimately, superoxide ions were discovered to be the
ways for synthesizing ternary heterojunctions (Sancheti most prevalent reactive species in the degradation reaction
and Gogate 2017). As compared to single and binary (Golzad-Nonakaran and Habibi-Yangjeh 2016a). Similarly,
photocatalysts, all of the examined ternary nanocompos- to improve photocatalytic activity, researchers prepared
ites ZnO/Ag 3VO 4/AgI (Pirhashemi and Habibi-Yangjeh ternary ZnO/NiWO4/Ag2CrO4 nanocomposite with p–n–n
2016a), ZnO/Ag3VO4/Ag2CrO4 (Pirhashemi and Habibi- heterojunction. These heterojunction materials improved the
Yangjeh 2016b), ZnO/AgI/Ag 2CO3 (Golzad-Nonakaran separation between the photo-generated electron–hole pairs
and Habibi-Yangjeh 2016b), and ZnO/AgI/Ag 2 CrO 4 and increased the visible-light capability by the advance-
(Shaker-Agjekandy and Habibi-Yangjeh 2016)) demon- ment of heterojunctions (Pirhashemi and Habibi-Yangjeh
strated greater catalytic performance for the elimination 2018). It means that the electrostatic interactions of inner
of rhodamine B, methylene blue, methyl orange dyes under electric field produced n–n–n or p–n–n heterojunctions and
visible-light irradiation. Through the creation of innova- these ternary nanocomposites are highly efficient as com-
tive ternary nanocomposites, a simple ultrasonic-irradi- pared to binary heterojunction for significantly improved
ation approach was used to photosensitize zinc oxide by segregation of electron/hole pairs and charge carrier lifetime.
mixing it with AgBr and A g2CO3 particles. The as-syn- As a result, photocatalysts with n–n–n or p–n–n heterojunc-
thesized ZnO/AgBr/Ag 2CO3 nanocomposites possessed tions give better photocatalytic activity as compared to n–n
optical capacity approximately across the visible range, or p–n heterojunctions.
according to ultraviolet–visible diffuse reflectance spectra. Zinc oxide, noble metal, or another semiconductors are
The ternary nanocomposite ZnO/AgBr/Ag2CO3 was used combined with each other for the generate of plasmonic
for the degradation of rhodamine B dye and reported 99% ZnO-based ternary nanocomposites (Li et al. 2013a, 2015a;
degradation efficiency within after 70 min of irradiation Cao et al. 2014, 2015; Naghizadeh-Alamdari et al. 2015;
time. The photocatalytic performance of ternary nanocom- Zhang et al. 2016). As a result, plasmonic photocatalysts
posites is higher than ZnO, ZnO/AgBr, and ZnO/Ag2CO3 with high absorption in the visible region can efficiently con-
samples, respectively, in the degradation of methylene vert solar to chemical energy. As a result, they have been
blue, rhodamine B, and methyl orange dye. recognized as promising candidates in the area of photoca-
The ternary photocatalysts increased photocatalytic effi- talysis. Wu and group developed ZnO/Ag/ZnFe2O4 ternary
ciency by helping electron–hole pair segregation caused by nanocomposites by using hollow and porous morphologies
the creation of n–n heterojunctions and surface character- (Wu et al. 2016a, b). Within 100 min of sunlight irradia-
istics. A plausible mechanism showing the electron–hole tion, ZnO/Ag/ZnFe2O4 ternary nanocomposites had entirely
pair separation is represented in Fig. 12c (Pirhashemi and eliminated methylene blue dye. This was the newly intro-
Habibi-Yangjeh 2016a). Yu and his team utilized a two- duced plasmonic ternary nanocomposite that can be utilized
step self-assembly approach to create a heterostructure of to purify the surroundings. The ZnO nanocomposite was
CdS/Au/ZnO (Yu et al. 2013). The CdS/Au/ZnO hetero- synthesized using the co-precipitation process and showed
structure exhibit much elevated hydrogen production from the highest efficiency for methylene blue degradation when
water which is 4.5 times higher as compared to CdS/ZnO exposed to visible light. This heterostructure exhibited a
heterostructure. Ren and group prepared ZnO@Au@Cu2O high saturation magnetization of 57.2 emu/g, making mag-
nanocomposite by three steps: electro-deposition, sputter- netic recycling easy across multiple separation cycles (Chi-
ing, and second electro-deposition (Ren et al. 2015). The dambaram et al. 2016).
gold nanoparticles interposed between ZnO and C u2O sig- Shen et al. (2016) have recently manufactured a unique
nificantly increase the photocatalytic efficiency of ZnO@ ternary ZnO/Ag 2 WO 4 /Fe 3 O 4 nanocomposites, which
Cu2O; however, efficiency lowers with the enhancement in demonstrated a 152% and 143% greater rate of antibiotic
Cu2O shell thickness. The outstanding catalytic behaviour degradation than the A g 2WO 4 and ZnO photocatalysts,
of ZnO@Au@Cu2O is ensured by the quick segregation of respectively. Sharma et al. (2020) fabricated F e3O4/ZnO/
electron–hole couples in the C u2O/ZnO interface. The par- Si3N4 ternary nanocomposite and found high degradation
tial inactivation of ZnO@Au@Cu2O is caused by the damp- efficiency. For the degradation of two dyes, sunset yel-
ening of the electromagnetic field in the Au/Cu2O junction low and methyl orange, its catalytic performance has been
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Environmental Chemistry Letters
studied. Sunset yellow and methyl orange have maximum ZnO‑based materials for hydrogen
degradation efficiency of 90 and 96%, respectively. The production
·OH radicals were discovered to be the most reactive spe-
cies. Furthermore, the Fe3O4/ZnO/Si3N4 (magnetite/zinc Hydrogen production has been proposed as a viable option
oxide/silicon nitride) ternary nanocomposite shows poten- for demonstrate the high global energy demands. The pho-
tial antibacterial properties (Sharma et al. 2020). Dhi- tocatalytic splitting of water with the help of natural sun-
man and group identified the interfacial electron transfer shine appears to be a promising technique for producing
mechanism in solution combustion produced ZnO/Fe/Ni H2 in a clean and environmentally acceptable manner. The
nanocomposites and a photocatalyst for the breakdown of semiconductor excites electrons from the valence band
the methylene blue dye (Dhiman et al.). position to the conduction band position after harvesting
Cai et al. (2015) used a hydrothermal technique at low light with a greater energy in comparison with the band-
temperature to manufacture magnetically separable ZnO/ gap energy, resulting in electron–hole pairs (Kitano and
Ag2O/Fe3O4 (zinc oxide/silver oxide/magnetite) photocata- Hara 2010). The dissociation and movement of electrons
lysts. The value of saturation magnetization of magnetite and and holes into the surface of the photocatalyst for water
ZnO/Ag2O/Fe3O4 is 38.9 and 1.61 emu g −1. The greater con- splitting occur, where holes oxidize H2O into H+ and O 2
centrations of diamagnetic ZnO and Ag2O in the fabricated gas, while electrons simultaneously decrease H + to H
2 gas
photocatalyst resulted in a comparatively low level of satura- (Ran et al. 2014), as shown in Fig. 13a.
tion magnetization for the ready nanocomposites. However, As a non-polluting, renewable, and cost-effective alter-
the ZnO/(Ag 2O)0.6/Fe3O4 ternary nanocomposites were native energy source, hydrogen-based energy systems have
subjected to the magnet, demonstrating that the nanocom- a bright future. They can provide high-quality energy ser-
posite has sufficient magnetic characteristics. Because of the vices in a wide range of applications (Zhou et al. 2011).
electron–holes recombination hindrance, the photocatalytic Nevertheless, most hydrogen production technologies rely
performance was increased by the good magnetic property. on natural gas (Zhou et al. 2011), coal (Zhou et al. 2011),
After three successive runs, the nanomaterial could be mag- crude oil (Rana et al. 2007), or water electrolysis (Zeng
netically alienated and recycled with no noticeable hammer- and Zhang 2010), and most of these techniques are limited
ing in photoactivity. The ZnO/AgI/Fe3O4 (zinc oxide/silver in their use due to the need for heat and electricity. As a
iodide/magnetite) ternary nanocomposites were fabricated result of their great effectiveness in photo-driven charge
by using an ultrasonic-assisted technique. The destruction creation and segregation, heterojunction photocatalysts are
of rhodamine B under visible-light irradiation was used to particularly propitious for solar hydrogen synthesis (Kim
assess the nanocomposites catalytic performance. The ZnO/ and Yong 2021).
AgI/Fe3O4 nanocomposite had a 32-fold greater catalytic ZnO is a potential semiconductor owing to its envi-
performance than the ZnO/Fe3O4 sample. Additionally, this ronmental sustainability and low cost when compared to
nanocomposite demonstrated significantly increased activity other binary nano-sized metal oxides. There are several
in the destruction of methylene blue and methyl orange dyes applications where the ZnO surface's reactivity is affected
(Shekofteh-Gohari and Habibi-Yangjeh 2016b). Similarly, by particle size (e.g. catalysts) (Kowsari 2011). Surveys
a number of ternary zinc oxide-based magnetic nanocom- of nanocrystalline catalysts such as ZnO, CuO, T iO2, and
posites, such as F e3O4@AgBr/ZnO (Shekofteh-Gohari and SrCO3 have emphasized the importance of form for photo-
Habibi-Yangjeh 2015a), Fe3O4@ZnO/AgCl (Shekofteh- catalytic performance (Kanade et al. 2007). The majority
Gohari and Habibi-Yangjeh 2015b), ZnO/Ag3VO4/Fe3O4 of research has concentrated on high-bandgap semicon-
(Shekofteh-Gohari and Habibi-Yangjeh 2015c), and F e 3O 4/ ductor oxides like ZnO, which require more energy for
ZnO/NiWO4 were fabricated and examined their photo- photo excitation and so require ultraviolet light to form
catalytic activity under visible light (Habibi-Yangjeh and electron–hole pairs for H 2 generation. Because of their
Shekofteh-Gohari 2017). smaller bandgap, photocatalytic H 2 generation by sul-
A narrow and matching band is one of the most criti- phide photocatalysts takes less energy. As a result, com-
cal variables in the creation of a heterojunction between bining wide bandgap ZnO with narrow bandgap sulphide
ZnO and semiconductor materials. This is a great way to semiconductors has the capability to produce efficient H 2
get ZnO’s spectral sensitivity into the visible range. When (Preethi and Kanmani 2013).
we compared the single ZnO and ZnO-based binary nano- The behaviour of ZnO/ZnS nanoparticles doped with
composites, ZnO-based ternary nanocomposites show bet- cerium ions in photocatalytic hydrogen generation from
ter photocatalytic properties for degradation of different sacrificial polysulfides was examined by Chang et al.
organic/inorganic/pharmaceutical contaminants. Various 2015. From an aqueous sodium chloride solution with
recently reported ZnO-based nanostructures are listed in sacrificial polysulfides ( Na2S and Na2SO3), the optimum
Table 2.
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Table 2 Review of work on metal-/non-metal-doped ZnO, ZnO-based binary nanocomposite, and ZnO-based ternary nanocomposite as photocatalysts
Catalyst Pollutant Degradation efficiency (%) Time (min) Light source References
Metal-/non-metal-doped ZnO
Nd-ZnO Methylene blue 98 – Ultra violet light Alam et al. (2018)
Ag-ZnO Rhodamine B 90 30 Sunlight Zhai et al. (2015)
Au-ZnO Methyl orange 100 180 300-W Xe lamp Lu et al. (2016b)
N-ZnO Rhodamine 6G 81.6 80 1000-W Xe lamp Wu et al. (2014)
C-ZnO Methylene blue 99.3 30 200-W Xe lamp Osman et al. (2016)
ZnO-based binary nanocomposite
ZnO/g-C3N4 Eriochrome black T 99 90 Ultraviolet light Ahmad (2020)
MgFe2O4/ZnO Rhodamine B 100 120 500-W Xe lamp Su et al. (2014)
ZnO/Cu2O Methylene blue 100 380 150-W Xe lamp Shi et al. (2017)
ZnO/Mn2O3 Methyl orange 95 210 250-W Xe lamp Saravanan et al. (2014)
Zn/Se Methyl orange 100 80 1-W mercury lamp Cho et al. (2012)
ZnO-based ternary nanocomposite
g-C3N4/ZnO/AgCl Rhodamine B 99 270 Ultraviolet light Akhundi and Habibi-Yangjeh (2015)
ZnO/Ag/CdO Methyl orange 90 210 Visible light Saravanan et al. (2015)
Sm2WO6/ZnO/GO Ciprofloxacin 69.92 90 Sunlight Arunpandian et al. (2020)
Methylene blue 98.24 25
ZnO/Ag/ZnFe2O4 Methylene blue 87 – Visible light Wu et al. (2016a, b)
Zn/AgBr/Ag2O3 Rhodamine B 99 70 Ultraviolet–visible light Pirhashemi and Habibi-Yangjeh (2016a)
This table focuses on the utilization of ZnO-based nanostructures for the degradation of organic dyes as pollutants
Environmental Chemistry Letters
Environmental Chemistry Letters
photocatalytic hydrogen generation efficiency of Ce- and Ce4+. During multiple trials, the performance of recy-
doped ZnO/ZnS photocatalysts exceeds 1200 mol/g/h. cled cerium-doped ZnO/ZnS photocatalysts (made with
The appearance of a mixed valence state of cerium in the 0.01 M cerium nitrate) in producing hydrogen is revealed
photocatalysts was revealed by X-ray photoelectron spec- in Fig. 13c, d. The activity loss in the recycled catalyst
tra of C e 3d shown in Fig. 13b. The activity of an opti- is minimal. The fourth test produces 85% of the H 2 pro-
mized Ce-doped ZnO/ZnS photocatalyst (1200 mol/g/h) duced in the first test (Chang et al. 2015).
in an aqueous NaCl solution with electron donors ( Na2S By adding metal sulphides containing A g2S, CuS, F
e 2S 3,
and Na2SO3) is 5.2 times high as compared to bare zinc and NiS, hydrogen production using photocatalysis in the
oxide/zinc sulphide photocatalyst. The increased activity sacrificial S2−, SO32− anions was examined. CuS/ZnS/ZnO
caused by cerium doping is due to the vacant or half-filled had 8.5-fold elevated photocatalytic efficiency for H2 evo-
cerium 4f electron configuration, which allows for quick lution as compared to ZnO. The established system could
and repetitive oxidation/reduction cycles between C e 3+ be used to develop a strategy for developing stable and
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Environmental Chemistry Letters
low-cost technologies for H2 production (Gomathisankar To produce the required products, these holes and elec-
et al. 2013). Using a one-pot thermal approach, several trons might go through a series of redox reactions on the
single-material and composite photocatalysts based on semiconductor’s surface.
g-C3N4 and ZnO were produced. Doping effect of boron
was also investigated to see if it could improve photocata-
lytic hydrogen production from water photolysis. To produce Reduction mechanism
boron-doped graphitic carbon nitride/zinc oxide (g-C3N4/
ZnO), polycrystalline ZnO was immersed in amorphous This is attributed to the reason that oxygen is a quickly
g-C3N4, and boron dopants swapped carbon atoms to pro- reducible substance, which has been used as a replacement
duce B-N bonds in g-C3N4. The undoped heterojunction has for hydrogen generation. Superoxide anions are formed
a Z-scheme band structure, which is known for g-C3N4/ZnO, when electrons in the conduction band react with dissolved
whereas boron-doped carbon nitride/ZnO has a type II band oxygen molecules. These superoxide anions bind to the
alignment. The higher Fermi level of carbon nitride results oxidative reaction’s intermediate products, producing
from the low electronegativity, and boron doping causes peroxide or converting to hydrogen peroxide and finally
the charge transfer mechanism to switch. The Fermi level water. An organic material is more prone to undergoing
position of boron-doped carbon nitride exceeds that of zinc reduction than water. High quantities of organic matter
oxide, resulting in a change of band bending direction at the tend to increase positive holes. This improves photocata-
heterojunction. The electron spin resonance study confirmed lytic activity by reducing carrier recombination (Rajesh-
that Z-scheme is dominated by type II heterojunction charge war et al. 2008; Nakata and Fujishima 2012; Khan et al.
transfer mechanism, with results that were compatible with 2015; Mudhoo et al. 2020). The reduction process is seen
those established by band structure analysis. So, the effec- in Fig. 14a. As a pairing reaction, oxygen in the air is
tively boron-doped C3N4/ZnO exhibit a 2.9-fold enhance- reduced (Rajeshwar et al. 2008; Rehman et al. 2009).
ment in hydrogen production compared to the undoped sam-
ple. Because both graphitic carbon nitride and zinc oxide
have large sufficient conduction band energy to push hydro-
gen photoreduction, this demonstrates that a type II band
structure is better for hydrogen generation in this situation.
Boron-doped C3N4/ZnO also showed great photocatalytic
properties (Kim and Yong 2021).
Reaction mechanisms
The wavelength and the catalyst are the most important fac-
tors in the photocatalytic process. Semiconducting nano-
materials, because of their electronic structure, are used as
a catalyst that functions as a sensitizer for light-triggered
redox reactions (Khan et al. 2015). The following points
are the basic stages in the semiconductor photocatalysis
method (Rajeshwar et al. 2008; Rehman et al. 2009; Khan
et al. 2015).
13
Environmental Chemistry Letters
13
Environmental Chemistry Letters
7. Additionally, the photocatalytic performance of dual temperature. Colloids Surf A 538:127–132. https://doi.org/10.
phase crystal structures is a field that has yet to be stud- 1016/j.colsurfa.2017.10.074
Ajmal A, Majeed I, Malik RN, Idriss H, Nadeem MA (2014) Principles
ied. Therefore, research in this area is still in its early and mechanisms of photocatalytic dye degradation on T iO2 based
stages, and more systematic investigations, such as photocatalysts: a comparative overview. RSC Adv 4(70):37003–
structural characterization of multi-component hybrid 37026. https://doi.org/10.1039/C4RA06658H
structures with better electrical and optical character- Akhundi A, Habibi-Yangjeh A (2015) Ternary g-C3N4/ZnO/AgCl
nanocomposites: synergistic collaboration on visible-light-driven
istics for highly effective and accurate photocatalysts, activity in photodegradation of an organic pollutant. Appl Surf
are eagerly awaited. Scientists should make sure when Sci 358:261–269. https://doi.org/10.1016/j.apsusc.2015.08.149
developing and implementing photocatalytic materials Akyol A, Yatmaz H, Bayramoglu M (2004) Photocatalytic degrada-
that they should be more widely available around the tion of reactive brilliant blue X-BR in aqueous solution using
quantum-sized ZnO. Appl Catal b: Environ 54:19–24. https://
world, cost-effective, and non-toxic for clean technol- doi.org/10.1016/j.materresbull.2007.08.029
ogy, and possibly valuable in a wide range of energy and Alam U, Khan A, Ali D, Bahnemann D, Muneer M (2018) Compara-
environmental applications. tive photocatalytic activity of sol–gel derived rare earth metal
(La, Nd, Sm and Dy)-doped ZnO photocatalysts for degradation
of dyes. RSC Adv 8(31):17582–17594. https://doi.org/10.1039/
C8RA01638K
Al-Rawashdeh NA, Allabadi O, Aljarrah MT (2020) Photocatalytic
Authors' contributions PD designed the review, interpreted, and wrote activity of graphene oxide/zinc oxide nanocomposites with
the original draft. GR drew the figures and tables of the manuscript. embedded metal nanoparticles for the degradation of organic
AK contributed to the original draft. GS contributed to the original dyes. ACS Omega 5(43):28046–28055. https://doi.org/10.1021/
draft. DVNV provided the technical advice and support. MN contrib- acsomega.0c03608
uted to the revision of the draft. Anandan S, Vinu A, Lovely KS, Gokulakrishnan N, Srinivasu P, Mori
T, Murugesan V, Sivamurugan V, Ariga K (2007) Photocatalytic
Funding No funding was received to assist with the preparation of activity of La-doped ZnO for the degradation of monocrotophos
this manuscript. in aqueous suspension. J Mol Catal A Chem 266(1–2):149–157.
https://doi.org/10.1016/j.molcata.2006.11.008
Anta JA, Guillén E, Tena-Zaera R (2012) ZnO-based dye-sensitized
Declarations solar cells. J Phys Chem C 116(21):11413–11425. https://doi.
org/10.1021/jp3010025
Conflict of interest The authors declare that they have no conflicts of Arunpandian M, Selvakumar K, Raja A, Rajasekaran P, Ramalingan
interest. C, Nagarajan E, Pandikumar A, Arunachalam S (2020) Rational
design of novel ternary S m2WO6/ZnO/GO nanocomposites:
Consent to participate All authors have agreed with the content and an affordable photocatalyst for the mitigation of carcinogenic
that all gave explicit consent to submit and participate. organic pollu.tants. Colloids Surf A Physicochem Eng Aspects
596:124721. https://doi.org/10.1016/j.colsurfa.2020.124721
Consent for publication All authors have consent for publication. Ba-Abbad MM, Kadhum AAH, Mohamad AB, Takriff MS, Sopian
K (2013) Visible light photocatalytic activity of F e3+doped
ZnO nanoparticle prepared via sol–gel technique. Chemosphere
91(11):1604–1611. https://doi.org/10.1016/j.chemosphere.2012.
12.055
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