A Review On Zno Nanostructured Materials: Energy, Environmental and Biological Applications

Nanotechnology
TOPICAL REVIEW
A review on ZnO nanostructured materials: energy, environmental and

biological applications
To cite this article: J Theerthagiri et al 2019 Nanotechnology 30 392001
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Nanotechnology
Nanotechnology 30 (2019) 392001 (27pp) https://doi.org/10.1088/1361-6528/ab268a
Topical Review
A review on ZnO nanostructured materials:

energy, environmental and biological
applications
J Theerthagiri1,9 , Sunitha Salla2, R A Senthil3, P Nithyadharseni4 ,
A Madankumar5 , Prabhakarn Arunachalam6 , T Maiyalagan7 and
Hyun-Seok Kim8,9
1
Centre of Excellence for Energy Research, Sathyabama Institute of Science and Technology (Deemed to
be University), Chennai 600119, India
2
Department of Chemistry, Sathyabama Institute of Science and Technology (Deemed to be University),
Chennai 600119, India
3
State Key Laboratory of Chemical Resource Engineering, Beijing Engineering Center for Hierarchical
Catalysts, Beijing University of Chemical Technology (BUCT), Beijing 100029, People’s Republic of
China
4
Energy Centre, Council for Scientific and Industrial Research (CSIR), Pretoria 0001, South Africa
5
Cancer Biology Lab, Molecular and Nanomedicine Research Unit, Centre for Nanoscience and
Nanotechnology, Sathyabama Institute of Science and Technology (Deemed to be University), Chennai
600119, India
6
Electrochemical Sciences Research Chair, Department of Chemistry, Science College, King Saud
University, Riyadh, King Saud University, Riyadh, Saudi Arabia
7
Electrochemical Energy Laboratory, Department of Chemistry, SRM Institute of Science and Technology,
Kattankulathur-603203, India
8
Division of Electronics and Electrical Engineering, Dongguk University-Seoul, Seoul 04620, Republic of Korea
E-mail: [email protected] and [email protected]
Received 27 November 2018, revised 26 April 2019

Accepted for publication 3 June 2019
Published 11 July 2019
Abstract
Zinc oxide (ZnO) is an adaptable material that has distinctive properties, such as high-sensitivity,
large specific area, non-toxicity, good compatibility and a high isoelectric point, which favours it to
be considered with a few exceptions. It is the most desirable group of nanostructure as far as both
structure and properties. The unique and tuneable properties of nanostructured ZnO shows
excellent stability in chemically as well as thermally stable n-type semiconducting material with
wide applications such as in luminescent material, supercapacitors, battery, solar cells,
photocatalysis, biosensors, biomedical and biological applications in the form of bulk crystal, thin
film and pellets. The nanosized materials exhibit higher dissolution rates as well as higher
solubility when compared to the bulk materials. This review significantly focused on the current
improvement in ZnO-based nanomaterials/composites/doped materials for the application in the
field of energy storage and conversion devices and biological applications. Special deliberation has
been paid on supercapacitors, Li-ion batteries, dye-sensitized solar cells, photocatalysis,
biosensors, biomedical and biological applications. Finally, the benefits of ZnO-based materials for
the utilizations in the field of energy and biological sciences are moreover consistently analysed.
9
Authors to whom any correspondence should be addressed.
0957-4484/19/392001+27$33.00 1 © 2019 IOP Publishing Ltd Printed in the UK

Nanotechnology 30 (2019) 392001 Topical Review
Keywords: battery, biosensor, biomedical applications, dye-sensitized solar cells, photocatalysis,

supercapacitor, ZnO
(Some figures may appear in colour only in the online journal)
1. Introduction namely precipitation, the wetchemical technique, the sol-gel

process, the hydrothermal method, the solvothermal process,
The design and synthesis of nanoscale materials are the key and microwave techniques, etc [17, 18]. As of late, various
innovation of the 21st century in an extensive range of applica- investigations have accounted on the advancement of ZnO
tions in numerous fields such as catalysis, energy storage and nanostructures for uses of energy and biological application
conversion devices, biosensors and biomedical applications by research. The gathering of such investigations is scarce in the
using metals, metal oxides, chalcogenides and carbon allotropes present literature, which makes the present review significant.
[1–5]. Especially, semiconducting metal oxides like ZnO, TiO2 In the present review, the current improvement in ZnO-
and SnO2 have been investigated and widely used because of based nanomaterials/composites/doped materials for the uses
their unique size and shape-based physiochemical properties. in the major area of energy and biological applications have
Among these, ZnO shows an excellent stability in chemically as been engaged. Special consideration has been focused on ZnO-
well as thermally stable n-type semiconducting material with based materials for energy storage and conversion devices such
wide applications such as luminescent material, solar cells, bat- as Li-ion batteries, supercapacitors and dye-sensitized solar
tery, supercapacitors, photocatalysis, biomedical, biosensors cells, as well as photocatalysts for the treatment of organic
piezoelectrics and optoelectronic in the form of bulk crystal, thin pollutant and biological applications such as biosensors and
film and pellets [6–12]. The rising technology has given new biomedical applications. Finally, the advantages of ZnO-based
prospect to the micro and nano structures ZnO in order to materials for the uses in the field of energy and biological
broaden its applications. For example, the designing of nanos- sciences are likewise steadily examined.
tructured ZnO with proscribed size, structure, porosity, and
morphological features have made extraordinary progress in
enhancing their activities for different applications. Recently, 2. Applications of ZnO nanostructured materials
nanostructure of ZnO (nanowires, nanorods, nanorings, nano-
tubes and nanospheres) have gained paid attention owing to their 2.1. Supercapacitor
high-sensitivity, large specific area, non-toxicity, good compat-
The electrochemical supercapacitor is widely recognized as an
ibility and high isoelectric point. The nano-sized materials exhibit
environmental friendly energy storage device and has the
higher dissolution rates as well as higher solubility when com-
potential to replace the existing energy-related devices. In recent
pared to the macroscopic counterparts [13]. The activity of years, it has been considered as a suitable energy storage device
energy storage devices is identified to be firmly influenced by the due to its greater power density as well as its stability and also it
shape, structural and physical properties of the active samples of provides greater performance than existing energy-related
the electrodes. For instance, fabricated electrodes using flake- or devices [19, 20]. The supercapacitors (SCs) find uses in plug-in
plate-like structured samples of LiFePO4 and graphite exhibit hybrid electric vehicles and backup power systems. In recent
ordered orientation which influence the flow of Li-ions [14, 15]. years, transition metal oxides as well as phosphates have been
In another report by Ye et al [16] the size of the sample impacts widely used as potential electrode material in supercapacitors
on the electrochemical activity of Au/TiO2 core/shell. In any and other energy-related applications [21, 22]. Among the
case, in spite of the significance of geometrical production of transition metal oxides, ZnO is widely recognized as a battery
metal oxide-based electrodes for the electrochemical energy active material with superior energy density of 650 A h g−1.
storage applications, which provide details regarding the impacts Additionally, ZnO has good electrical conductivity (up to
of morphology and structure of the metal oxides on their elec- 230 S cm−1), which is larger than those of other metal oxide
trochemical activity, especially of supercapacitors and batteries. materials. In this regard, there are few reports about electrode
Fortunately, the remarkable morphological features of materials of SCs based on ZnO-based materials. Ridhuan et al
ZnO make it a striking material that is widely used as a [23] reported the hydrothermally synthesized ZnO electrode
counterpart of a significant scope of energy and biological materials for SCs. However, the low specific surface area (SSA)
applications. As far as morphological perspectives of ZnO are as well as poor electrical conductivity of ZnO, remains a major
concerned, the synthesis and fabrication procedures also play task and confines rate capability for great power performance,
a significant role. The different parameters used (namely thus hampering its wide use in an energy storage system. To
surfactant, temperature, concentration, and time, etc) play a overcome this issue, composite materials have been loaded to
vital function in the growth of various types of synthetic ZnO electrode materials. It is evident that creating a hybrid
process. An expansive number of different methods were composite electrode will be an efficient way to increase the
reported worldwide for the synthesis of well surface struc- specific capacitances. The observed enhancement is credited to
tured ZnO nanopowder, composites and films. The notable the synergetic effect of individual ones in the composites via
techniques for the syntheses of various ZnO nanomaterials/ reducing particle size, increasing SSA, as well as more porosity
composites/doped heterostructures are commonly carried out, and increasing the quantity of active sites. ZnO-based composite
2
materials provide several benefits such as cost-effectiveness, properties of graphene-ZnO construction to meet large-scale
eco-friendliness, decent electrochemical reversibility, superior application necessities in SCs is still a task. Consequently,
specific capacitance, greater power density as well as energy because of the large amount of defects and the making of a
density, good cycling stability and easier fabrication, which chemical part in the synthesis approach and it gravely limits the
provides them with a favourable contender for electrochemical capabilities of graphene-based SCs. However, it is still required
supercapacitors. Herein, we present recent outcomes of several to develop the more advanced synthetic approach to fabricate
kinds of ZnO-based composite materials, such as ZnO/gra- the graphene-ZnO nanostructures; graphene always reveals
phene, ZnO/carbon, ZnO/NiO, ZnO/MnO2, and other reduced electrical conductivity.
composites. In recent years, 3DG has fascinated a lot of considera-
tion. It is also favourable to the rapid transmission of
electrical ions and have great potential to overcome the
2.1.1. ZnO/graphene. During the last few decades, graphene above-mentioned problems [34]. Recently, Li et al [35]
has fascinated and been given massive consideration owing to synthesized 3DG/ZnO nanorods with lacunaris structures via
its distinctive 2D nanostructure, extraordinary theoretical SSA, a hydrothermal route and achieved a maximum specific
exceptional electrical conductivity, thermal conductivity, capacitance value of 554 F g−1 at 5 mV s−1, whereas only
unique mechanical strength, and decent electrochemical 6.6% of the available capacity was attenuated at more than
stability. Consequently, graphene nanosheets have been the 2300 cycles. Figure 1 illustrates that the electrochemical
most encouraging material for their potential electrode properties of 3DG/ZnO composite electrodes are investigated
supporting materials in SCs and other electrochemical energy in detail. In comparison with other composited ZnO-graphene
storage devices. However, the inhibition of aggregation and materials, the electrochemical properties of the 3DG/ZnO
restacking is of utmost significance to progress the application composite materials are more electrochemically stable with
of graphene in energy storage systems [24, 25]. In particular, enriched specific capacitance as SC electrodes.
reduced graphene oxide (RGO) is mainly used in the place of
graphene, generally due to its cost-effectiveness and great
production capacity approach for developing good-sized 2.1.2. ZnO/Carbon. The limitations in ZnO electrode
graphene materials [26]. Additionally, it is also evidenced materials may be overcome by using various composites
that RGO is mostly exposed to accumulation and comprising of carbon material and ZnO as electrode materials
agglomeration problems owing to the van der Waals for SCs. Advantages of both the Faradaic capacitance of the
interaction, which effects in a considerable loss of effective metal oxide and the double layer capacitance of the carbon-
SSA, thereby reducing capacitance. Currently much interest based materials with great SSA, thereby enhance the
has been focused on improving the SSA of graphene capacitance and cycling stability [36]. More research works
considering the large-area application in SCs. are focused on developing ZnO/carbon-based materials
Recently, Lu et al pointed out that the graphene-ZnO thin (carbon aerogel (CA), activated carbon (AC), carbon
film fabricated through the ultrasonic spray pyrolysis method nanotubes (CNT) and so on) and composite electrode
and achieved the maximum specific capacitance of 635 F g−1 materials for SCs. In this regard, Zhang et al pointed out the
[27]. Lately, Haldoraia et al [28] reported the graphene-ZnO ZnO/CNT composite electrode material and achieved specific
composite materials with enhanced specific capacitance of capacitances of 324 F g−1 [37]. Lately, Kalpana et al developed
314 F g−1 for G-ZnO nanocomposite. Further, Du et al a ZnO/CA composite electrode and achieved a maximum
successfully fabricated honeycomb-like ZnO/rGO composites specific capacitance of 500 F g−1 [38]. Selvakumar et al
materials with improved capacitive property of 231 F g−1 at fabricated the ZnO/AC composite materials via the sol-gel
0.1 A g−1 because of the presence of spacers [29]. Saranya et al approach and achieved a specific capacitance of 160 F g−1 with
[30] reported the graphene-ZnO nanocomposites fabricated stability up to 500 cycles [39]. In their synthetic approach,
through the solvothermal approach and have a higher specific sucrose has been applied as the capping agent as well as a
capacitance of 122 F g−1 at 5 mVs−1. Lately, Li et al [31] carbon source to fabricate the ZnO/C nanocomposites in a
fabricated the sandwiched hybrid structure of ZnO/rGO/ZnO cost-effective green chemistry route. Afterwards, Sasirekha
materials and achieved a specific capacitance of 275 F g−1 at et al [40] synthesized the ZnO/C composite electrode materials
5 mV s−1. Moreover, the hybrid ZnO/rGO/ZnO assembly via the green chemistry route for SCs and achieved a maximum
display an exceptional rate capability and admirable long-term specific capacitance of 820 F g−1 at 1 A g−1. Further, ZnO/C
cycling stability related to rGO. It is expected that that the electrode materials retain the 92% of capacitance retention up
grouping of graphene with ZnO can effectively enhance the to 400 cycles and its symmetric SC device exhibits the
global specific capacitance related to the individual ones. maximum specific capacitance of 92 F g−1 at 2.5 A g−1 with an
Jayachandran et al [32] reported the rGO-ZnO via ultrasonic energy density of 32.78 Wh kg−1. Recently, Li et al [41]
approach and achieved a higher specific capacitance of reported the AC/ZnO composites via walnut-derived
312 F g−1 with improved cycling stability up to 1000 cycles. hydrothermal routes and its showed specific capacitance of
Rajeshwari et al [33] reported the rGO-ZnO nanocomposite 117 F g−1 at 0.5 A g−1. Kim et al [42] fabricated a ZnO/AC
materials via the hydrothermal approach for SCs and achieved nanofiber via the electrospinning/sol-gel process and exhibits a
a maximum capacitance value of about 719.2 F g−1 at a scan maximal specific capacitance of 178 F g−1, and high energy
rate of 5 mV s−1. Moreover, improving the electrochemical densities of 22.71–17.77 Whkg−1 in the power density range of
3
Figure 1. Electrochemical performance of the 3DG/ZnO electrodes. (a) The capacitance of 3DG/ZnO evaluated at a current density of
10.0 A g−1 of 2300 cycles, (b) GCD profile of the composite electrode at different current density, (c) CD profile of the composite electrodes
at a current density of 10.0 A g−1 and (d) Nyquist plot of the 3DG/ZnO composite and 3DG electrode. Reprinted from [35], Copyright 2015,
with permission from Elsevier.
400 to 4000 W kg−1. Xiao et al [43] successfully fabricated the morphology of ZnO–MnO2 electrode materials through
carbon sphere (CS)@ZnO core-shell nanocomposites through anodic electrochemical deposition and colloidal pretreatment
the facile low temperature water-bath method and achieves a and demonstrated volumetric energy density of 0.234 mW h
specific capacitance of 630 F g−1 at the current density of cm−3 and volumetric power density of 0.133 W cm−3. Quite
2 A g−1. recently, Radhamani et al [49] reported the ZnO–MnO2 core-
shell nanofiber electrode materials for SCs and acquired a
2.1.3. ZnO/metal oxide. Among the available transition maximum specific capacitance of 907 F g−1 at 0.6 A g−1.
metal oxides, MnO2 is a potential electrode candidate for Further, the packaged ZnO–MnO2 device delivered a high
SCs owing to its high theoretical capacitance (∼1370 F g−1), energy density of 17 Whkg–1and a power density of
multiple oxidation states of Mn, rich natural resources and 6.5 kWkg–1. Figure 2 displays the assymentric SCs device
low cost [44]. However, poor conductivity of MnO2 values were superior to numerous symmetric SCs and
(10−5–10−6 Scm−1) have to be rectified to be used in SCs assymetric SCs built from MnO2.
application. Electrochemical performances suffered from the NiO has been widely explored as electrode materials for
poor conductivity of MnO2. To overcome these limitations, SCs with cost-effectiveness, huge theoretical capacity
MnO2 have to be combined with multifunctional materials (2573 F g−1) and possess high power density [50, 51].
such as ZnO, which provides a pathway for electron transport Nevertheless, the poor surface area and sluggish electrical
as well as strong mechanical support [45]. In recent years, conductivity of NiO limits its applications in energy-related
Yang et al developed ZnO–MnO2 nanocables through a high devices. To overcome these shortcomings, 3D nanostructured
temperature annealing/hydrogenation method and achieved electrode materials have been widely investigated to shorten
an enhanced capacitance of 138.7 mFcm−2 at 1 mAcm−2 diffusion distance of electrolytes into pseudocapacitor
[46]. Further, Sun et al fabricated core-shell structured 3D electrodes [52]. In this regard, Pang et al successfully
ZnO–MnO2 nanocomposites and attained a specific areal fabricated porous ZnO–NiO nanocomposites bythe calcina-
capacitance of 31 mFcm−2 [47]. Li et al reported a ZnO tionof mixed oxalate precursors and attained a maximum
nanorod/MnO2 nanowired electrode structure and acquired a specific capacitance 649.0 F/gwith good cycle stability up to
maximum specific capacitance of 747 F g−1 at 2 mVs−1 [48]. 400 cycles [53]. Lately, Zheng et al [54] reported the Au
Zilong et al [45] reported the core/shell structural nanoparticles embedded ZnO-NiO core/shell nanocomposites
4
Figure 2. (a) Illumination of a red LED by a lab-scale prototype ASC device and (b) power density versus energy density for
ACǁZnO@MnO2-AC asymmetric SC in a Ragone plot with conventional capacitors, SCs, conventional batteries and fuel cells. Reprinted
with permission from [49]. Copyright (2016) American Chemical Society.
Table 1. Comparison of electrochemical performances of ZnO-based electrodes in the literature.
Capacitance Scan rate (mV s−1)/current density Potential win-

Electrodes (F g−1) (A g−1) dow (V) Electrolytes Ref./Year
−1
rGO/ZnO 635 5 mVs −0.6 V to 0.3 V 1.0 M KOH [27]/2018
RGO/ZnO 314 100 mVs−1 −0.6 V to 0.3 V 2.0 M KOH [28]/2017
ZnO/RGO 231.3 0.1 Ag−1 — 6.0 M KOH [29]/2011
3DG/ZNO 554 5 mVs−1 −0.9 V to 0.1 V 1.0 M KOH [35]/2015
ZnO/CNT 324 50 mVs−1 −0.5 V to 0.5 V 2.0 M KOH [37]/2015
ZnO/CA 500 100 mA cm−2 — 6.0 M KOH [38]/2017
ZnO/C 820 1 Ag−1 0 V to 0.8 V 1.0 M Na2SO4 [40]/2014
CS@ZnO core shell 630 2 Ag−1 0 V to 0.4 V 6.0 M KOH [43]/2014
ZnO/MnO2 nanowire 747 2 mVs−1 0 V to 0.9 V 1.0 M Na2SO4 [48]/2012
ZnO/NiO 649 5.8 Ag−1 0 to 0.5 V 3.0 M KOH [53]/2016
nanocomposite
electrode materials for SCs with good long-term cycle oxides-MnxOx, ZnO, TiO2, CoO, NiO, VxOxand FeOx) and
stability and exhibits a maximum specific areal capacitance of SnO2 due to their high theoretical capacity [59–68]. ZnO has
4.1 F cm−2 at 5 mA cm−2. Comparison of specific capacitance been especially considered as a promising potential anode due
of various kinds of ZnO nanocomposites for electrochemical to its high theoretical capacity (978 mAh g−1), high Li ion
supercapacitors are presented in table 1. diffusion coefficient, natural abundance, low toxicity and low
cost. However, its practical exploitation is impeded by its
2.2. Lithium-ion batteries rapid capacity fading initiated due to the huge volume
expansion during the electrochemical lithiation/delithiation
Energy storage technology, such as batteries and super-
process leading to the loss of electrical disconnection between
capacitors, is the authoritative power source towards the
forthcoming, owing to its ease maintenance, long cycle life, the anode powders [69, 70].
flexible power and energy features. Rechargeable lithium-ion Consequently, several efforts, i.e. various surface
batteries (LIBs) have attracted great attention due to their morphologies, nano-architectures (1, 2 and 3D dimensional),
increasing energy demands in various fields such as, elec- doping with different elements and addition of conductive
tronics, hybrid electric vehicles and renewable energy gen- agents, have been made in order to defeat the capacity decay
eration systems. LIBs remain the most dominant power and enhance the long cycle life. Concerning cathode materi-
sources for a plethora of applications because of their high als, ZnO can be mixed with various lithium storage (LiMn2O4
power and energy density. Although, the limitations of car- and LiFePO4) [71] materials in order to obtain high and stable
bonaceous anodes have been completely overcome by the use capacities. Therefore, in this review part deliberated about the
of various alloys (Sn, Sb, Si and Ge) [55–58] and metal-oxide recent progress on ZnO oxides with various structures syn-
based anode materials such as TMOs (transition metal thesized by several methods for LIB applications. Moreover,
5
this part desperately discussed its insights between the that 71.45 wt% (ZnO-HG) graphene added ZnO exhibits high
synthetic strategies for ZnO-based nanomaterials, and their reversible specific capacity and good rate performance than that
functional applications in lithium storage batteries. of other composites. Moreover, it delivers a high reversible
capacity of 240 mAh g−1 at a low cut-off voltage (0.01–1.0 V),
which is evident as an anode for Li-ion full cells. This excellent
2.2.1. ZnO/Graphite composite. Dall’Asta et al [72] performance was attributed to the graphene, which could buffer
synthesized different types of nanorods (1D), single- and the volume expansion during the cycling process. Likewise,
multi-layered nanosheets (2D) and nanobrushes (3D) and Ning et al [76] fabricated binder-free and self-supported core/
finder free ZnO nano-architectures as the anode for lithium shell structured ZnO/carbon nanofiber (ZnO/CNF) composites
ion batteries. In this method, different types of nano-architecture by single-nozzle electrospinning with different mass ratios of
were prepared on Pt-coated stainless steel (SS) substrates by a CNFs (0, 0.25, 0.5, 1.0 and 1.5). Among them, ZnO/CNF-0.5
simple and low-impact wet chemistry approach. It was noticed exhibits high capacity and good cycling stability, it could be
that the 2D single-layered nanosheets revealed high reversible ascribed to the CNFs, which enhances the electronic
capacity than that of other nano-architecture materials. This conductivity and fastens the kinetic process during the
could be due to the small nanoparticles and the presence of electrochemistry. Also the CNFs can suppress the volume
mesoporous texture which maximize the specific area to favour expansion of ZnO during lithiation and de-lithiation processes.
alloying formation and allows large room to accommodate the
volume changes during cycling. Eliana et al [73] reported
binder-free novel graphite-coated ZnO nanosheets (NS) for high 2.2.2. ZnO/Carbon composite. Xiao et al [77] fabricated ZnO
capacity and stable anode material for lithium ion battery nanoparticles encapsulated in a 3D hierarchical carbon
applications. The hybrid ZnO NS grown on a stainless steel disk framework novel material by a hydrothermal process followed
by hydrothermal process at 60 °C for 6 h, followed by annealing by post-heat treatment under N2 atmosphere of polydopamine
at 350 °C for 1 h under air. Subsequently, two different (G110 coated Zn3(C6H5O7)2 intermediate material. Raw ZnO and
and G350) graphite layer thicknesses were coated on ZnO NS by ZnO@C has been prepared by the calcination of Zn3(C6H5O7)2
a thermal evaporation process. The G350 thickness graphite layer under air and under N2 at 600 °C for 4 h, in order to compare the
coated ZnO NS reveals superior capacity of ∼600 mAh g−1 ZnO@CF. Compared to raw ZnO and ZnO@C spheres,
with minimized capacity fading at 1 A g−1 upon 100 cycles. ZnO@CF composite exhibits enhanced specific capacity,
This is attributed to the peculiar microporous structure with longer lifespan and improved rate performance. It is
well-interconnected nanoparticles (<15 nm) which allows concluded that the encapsulated 3D carbon framework can
enormous room for accommodating the volume changes upon stimulate effective electronic contacts by supplying electron
lithium insertion/de-insertion. Also, graphite plays a crucial role pathways and also the stable and flexibility structure of the 3D
in order to stabilize the morphology during the lithiation and de- carbon framework contributes greatly to buffering the stress and
lithiation process upon cycling, resulting in enhanced specific volume changes that occur in electrode materials during Li+
capacity and improves the reversible capacity of the ZnO NS. insertion/extraction. Yin et al [78] fabricated three-dimensional
Kim et al [74] developed hierarchically self-assembled ZnO ordered macro-/mesoporous carbon (3DOM-mC) from a silica
(SAZO@GO) by a modified Hummer’s method by using GO. sphere array and phenol/formaldehyde by the typical dual-
Doughnut-like ZnO (DLZO@GO) was also synthesised by templating method, and a ZnO nanoparticle encapsulated/
which the solution ratio of GO solution was varied in the range supported 3DOM-mC composite (ZnO/3DOM-mC) was
0.25−4 of DMF: distilled water ratio. For comparison, ZnO synthesized through a simple in situ solution growth approach.
nanoparticle clusters (ZONC), DLZO and ZnO were fabricated It is noticed that 3DOM-Mc supported ZnO revealed excellent
without the addition of GO. Here in this method, GO plays a electrochemical properties, which could be attributed to the
leading role to create a self-assembled structure to improve the unique hierarchical porous structure of the 3DOM-mC. Also,
electronic conductivity of ZnO. Therefore, hierarchically self- the ordered interconnected macroporous remains stable after
assembled ZnO (SAZO@GO) exhibits high reversible capacity loading the ZnO nanoparticles in it, which could facilitate the
with excellent stability and a better rate capability performance rapid kinetic properties of Li-ion. Furthermore, the confinement
than that of DLZO@GO, ZONC and ZnO materials. This effect of the mesoporous on the macropore walls of the 3DOM-
enhanced performance was attributed to the self-assembled mC can provide more space to accommodate the volume
structure in which it develops high electrical conductivity, changes during lithiation/de-lithiation and the 3D connected
shortens the Li ion diffusion path length, stabilises the SEI layer carbon skeleton enhances the strength of the electrodes.
and creates more room to accommodate the volume changes. Similarly, Zhao et al [79] demonstrated novel 3D
Followed by this report, Feng et al [75] reported different interconnected nanofiber films by intercalating petroleum
amounts of graphene incorporated (0.2 g (43.08 wt%), 1.0 g asphalt (PA) into ZnO/carbon nanofibers (ZnO/CNFs-PA)
(60.11 wt%) and 1.8 g (71.45 wt%)) ZnO-graphene hybrid via the one-step electrospinning method. In order to explore the
materials synthesized by a hydrothermal process for lithium influence of PA addition into ZnO/CNFs, films were prepared
ion battery applications. In order to further investigate the anodic by solvent impregnation and subsequent two-step thermal
performance for the commercial use of Li-ion batteries (Full Li- treatments by adjusting the PA amount to 0.4 g, 0.6 g, 1.0 g,
ion cell), the ZnO-graphene hybrid materials were tested at 1.3 g and 3.0 g. Among them, ZnO/CNFs-PA-1.0 showed
different cut off-voltages such as 0.01 to 3.0 V. It is concluded excellent electrochemical performance. This could be ascribed
6
to the special 3D conductive network structure, which can for lithium ion batteries. In order to obtain the carbon-coated
effectively accommodate the volume expansion and facilitate ZnO microspheres, the different amounts of dopamine hydro-
the kinetics of Li-ion. Followed by that report, Yang et al [80] chloride (20, 30 and 50 mg) were added to the ZnO
designed a core-shell-structured ZnO@C nanosphere by a facile microspheres and followed by a thermal treatment in N2. This
route-extended Strober method. The enhanced specific capacity process has been proved a confined crystallization strategy to
of ZnO@C nanosphere could be due to the core-shell structure, enhance the degree of crystallinity of carbon-coated ZnO
which can effectively shorten Li-ion diffusion pathways and microspheres. It was noticed that ZnO@C-30 showed superior
also prevent the pulverization originated from the large volume electrochemical performance than other materials and could be
change during the Li insertion/extraction process resulted in ascribed to the enhanced degree of crystallization, which could
reduced capacity fading. Similarly, Li et al [81] a constructed accommodate the volume changes during the cycling process.
ZnO/ZnO@C composite was synthesized by facile solution Songtao et al [86] synthesized nanostructured ZnO-carbon black
reaction followed by a simple carbonization process of ZnO/ (ZnO-CB) as the anode material for lithium-ion battery
ZnO@ZIFs-8. When evaluated as anode for lithium ion applications by atomic layer deposition (ALD). The ALD
batteries, the ZnO/ZnO@C composite presented high capacity method was used to create more oxygen vacancies in ZnO
with good capacity retention, outstanding cycling stability and structure and also strengthen the molecular bonding between the
excellent rate capability. This enhanced electrochemical ZnO and carbon surfaces, which enhances the electrical contact
performance mainly attributed to the carbon framework during the lithiation and de-lithiation processes, resulting in a
derived from ZIF-8, which improves the electronic stabilized SEI layer. Youlan et al [87] reported the series
conductivity and suppresses the volume change effect. structure of ZnO/MWCNTs nanocomposites as the anode
Taegyeong et al [82] reported ZnO-embedded N-doped material for lithium ion batteries. ZnO/MWCNTs nanocompo-
porous carbon/carbon foam (ZnO/N-CF) composites sites were synthesized through a facile self-assembly method,
synthesised by a vapour-assisted method followed by a two- therein the ZnO polyhedrons are well attached and array orderly
step thermal treatment. For comparison of ZnO/N-CF, raw ZnO along the MWCNTs to form the series structure. This unique
and ZnO/CF samples were prepared by a vapour-assisted structure can significantly enhance the capacity, electrode
method and etched N-CF was prepared by dissolving out the stability and facilitate the kinetic properties of Li-ions. Followed
ZnO from the ZnO/N-CF using 25 ml of 0.1 M HCl solution. by this report, Youlan et al [88] developed hierarchical porous
Among them, the ZnO/N-CF composite reveals superior ZnO/MWCNTs (MCZO) nanocomposites synthesized by using
reversible capacity, rate performance and long-term the well-studied zeolitic imidazolate framework-8 (ZIF-8)/
cycliability. The enhanced electrochemical performance MWCNTs (MCZF) nanocomposite as the template and
attributed to the N-doped CF matrix, which could improve the precursor followed by heat treatment at different temperatures
intimate contact between ZnO particles and N-CF matrix. Also, (300, 400 and 500 °C). When tested as the anode material for
it prevents the aggregation and severe volume changes during lithium ion batteries, the MCZO-400 °C revealed improved
the long term cycling. Similarly, a novel confined growth of lithium storage performance with high reversible capacity, good
small ZnO in N-rich mesoporous carbon nanospheres (ZnO/ rate capability and cycling stability. This could be attributed to
NMPCS) [83] has been synthesized as an anode material for the synergetic effect between the MWCNTs and the porous
lithium ion battery applications. NMPCS has been synthesized ZnO polyhedron structure. Similarly, Yonghai et al [89]
by an aerogel-assisted co-polymerization process followed by developed a novel hybrid hollow porous ZnO/C nanocages,
carbonization and washing treatment. In order to obtain a novel which were synthesized via a one-step pyrolysis of metal
ZnO/NMPCS material, a hydrothermal method was used and organic framework derived (MOF-5) as both the precursor and
followed by the calcination process. This sort of ZnO/NMPCS template under N2 atmosphere. It is concluded that hollow
has offered several merits such as interconnected spherical porous ZnO/C nanocages presented excellent electrochemical
framework with large surface area, N-rich carbon lattice and to performance, compared to hollow ZnO and commercial ZnO.
acquire a homogeneous distribution of ZnO nanoparticles. The This significant performance was attributed to the hollow
schematic diagram for preparation of SEM and TEM images of structure and carbon, which could effectively accommodate the
NMPCS and ZnO/NMPCS composites are shown in volume variation of nanocomposite and improve the electronic
figures 3(a)–(g). With the influence of such merits during conductivity. Wang et al [90] reported that carbon nanotu-
electrochemistry, it can provide sufficient Li+ storage space/ be@ZnO (CNT@ZnO) composite has been prepared via a
sites and fasten the kinetic reaction process, which resulted in liquid-phase method as an anode for lithium-ion batteries. In
high capacity with excellent cycliability and fast rate capability. order to study the influence of CNT content in ZnO, different
Yu et al [84] designed a peapod-like ZnO@Cwith internal amounts of CNTs such as CNT-20@ZnO and CNT-30@ZnO
void space as the anode and it was synthesized by a were synthesized by the same method. The electrochemistry
hydrothermal process followed by calcination of ZnO/ results indicated that the CNT-20@ZnO composite exhibits a
ZnOHF@polydopamine nanorods. The designed internal void more superior electrochemical performance than pure CNTs,
space and external carbon shell can suppress the large volume commercial ZnO and CNT-30@ZnO.
change during the electrochemistry process, resulting in
enhanced cycling stability and rate capability performance.
Liang et al [85] reported nanostructured ZnO microspheres as 2.2.3. ZnO/metal/metal oxide composite. Junfei et al [91]
the anode material and it was prepared by a hydrothermal route synthesized ZnO/N doped carbon/Cu (ZnO/NC/Cu)
7
Figure 3. (a) Schematic representation of formation process of NMPCS and ZnO-NMPCS. (b) Low magnification of SEM image of NMPCS.
(c) Low magnification SEM image of ZnO-NMPCS. (d) High-magnification SEM image of NMPCS. (e) Representative TEM image of a
single NMPCS particle. (f) TEM image of a single ZnO-NMPCS particle. (g) HRTEM image of ZnO-NMPCS (the inset shows the
corresponding SAED pattern). Reprinted from [83], Copyright (2017), with permission from Elsevier.
composites with different amounts of ZnO:Cu loading of (1:1, material for lithium ion batteries. In this work, they studied the
1:2 and 2:1) by a one-step process of the pseudo-solid-state influence of different amounts of ZnO (1, 2.5 and 5 wt%)
method using copper phthalocyanine as carbon, nitrogen and doped on the LiFePO4/C composite, named LFP, LFPZ1,
copper sources. For comparison, a Nc:Cu hybrid has been also LFPPZ2.5 and LFPZ5. The electrochemistry results reveal that
prepared under identical reaction conditions. Compared to all LFPZ2.5 has the superior performance (high specific capacity
the ratios and its pristine materials, ZnO/NC/Cu (1:1) reveals and rate capability) compared to the other ratios. Schematic
high specific capacity, good cycle stability and high rate illustrations of the charge transport mechanism for a solid-
capability, which could be attributed to its specific structure. liquid interface of a ZnO-doped LFP electrode and cycling
There, metallic Cu tightly bonded with ZnO can improve the performance are shown in figures 4(a) and (b). Li et al [93]
electronic conductivity of ZnO and also acts as catalysts to fabricated a series of ZnO-coated (1, 2 and 5 wt%) LiMn2O4
improve the reversible conversion of the SEI layer. Also, the cathode materials that were successfully synthesized through a
bounded N-doped carbon layer can prevent the detachment and combustion method using glucose as fuel. Among them, 2 wt%
aggregation of possibly pulverized ZnO nanoparticles during ZnO-coated LiMn2O4 exhibits the improved electrochemical
the cycling process. Rakesh et al [92] reported a surface- performance than that of pristine and other ratios. This could be
modified ZnO-doped LiFePO4/C composite as the cathode due to the ZnO coating on the surface, which could effectively
8
Figure 4. (a) Schematic illustration of charge transport phenomenon for a solid-liquid interface of ZnO-doped LFP electrode and (b) cycling
performance of synthesized samples at 170 mA g−1 for 50 cycles. Reprinted from [92], Copyright (2017), with permission from Elsevier.
minimize the electrochemical polarization and charge transfer recognised as a potential candidate for photoanode materials
resistance during charge-discharge cycling, resulting in to achieve high performance DSSCs [109–113]. Therefore,
improved electrochemical performances of LiMn2O4. A this section mainly focuses on recent progress in the devel-
comparison of specific reversible capacities of various opment of ZnO nanostructure-based photoanodes for high
structured/doped ZnO nanocomposites prepared by different efficient DSSCs.
methods for lithium-ion cell and characteristics is presented in Marimuthu et al [114] deposited ZnO nanorods onto a
table 2. Here, there are the NS-(nano-sphere), 1D–2D–3D ZnO-seeded FTO substrate by an electrochemical deposition
(dimensional), CNFs (carbon nanofibers), NC (N-rich carbon), method in the solution containing the different concentrations
CB (carbon black), DLZO (donut-like zinc oxide), ZONC (zinc of hexamethylenetetramine (HMTA). The obtained ZnO thin
oxide nanoparticle cluster), SAZO (self-assembled zinc oxide) films were used as a photoanode to fabricate the DSSC. The
and MWCNTs (multi-walled carbon nanotubes)). DSSCs fabricated with ZnO photoanodes obtained from
0 mM and 9 mM of HMTA solutions exhibited the power
conversion efficiency (PCE) of 1.79 and 3.75%, respectively.
2.3. Dye-sensitized solar cells
The observed improvement in DSSC after addition of HMTA
The developments of clean and renewable energy resources is mainly due to the ZnO nanorods. Wang et al [115]
are a very essential factor for solving the energy demands developed the novel ZnO nanosheets (NSs)/nanocrystalline
owing to the rapid depletion of fossil fuels such as oil, natural aggregates (NAs) composite films via a facile dip-coating
gases and coal [94–98]. Solar energy has a great potential method. They observed that the DSSCs assembled with ZnO
application to fulfil a significant part of sustainable demand NSs/NAs composite film was displaying the PCE of 7.95%
for future generations because it is the most rich permanent which was 81.51% higher than that of pure ZnO NSs. The
energy resource on earth [99, 100]. In recent times, the dye- higher efficiency of ZnO NSs/NAs composite film was due to
sensitized solar cells (DSSCs) have received considerable the large specific surface area and good electron transport.
attention as a promising alternative photovoltaic technology Saleem et al [116] assembled the flower-like ZnO nanos-
due to the low manufacturing cost, simple fabrication pro- tructures with hexagonal nanorods through a simple hydro-
cedure, eco-friendly nature, good stability and high power thermal method at low temperature using polyethyleneimine
conversion efficiency [101–103]. Generally, a DSSC con- (PEI) as a surfactant in the seed sole. They obtained two kinds
structed with an electrolyte contains a redox couple dissolved of morphology, such as rod-like flower and the blade-like
in an organic solvent, which is sandwiched between a dye- flower nanostructures by FTO substrates cleaning with etha-
sensitized nanocrystalline titanium dioxide (TiO2) as a pho- nol and distilled water, respectively. These flower-like
toanode and a Pt counter electrode [104–106]. In DSSCs, the nanostructures were further utilized as photoelectrodes in
dye-sensitized nanocrystalline semiconductor photoanodes DSSCs. It showed that the blade-like flowers provided the
play an important role in the conversion of solar energy into increased PCE of about 2.23% as compared to rod-like flower
electrical energy. The TiO2 nanoparticles are the most fre- nanostructures (1.08%). This increase in DSSC performance
quently used photoanode materials in DSSCs so far of the blade-like-flower photoelectrodes was mainly attributed
[107, 108]. However, the TiO2 nanoparticles suffer from the to the synergistic effect of the enhanced surface area for larger
high recombination and low electron transport properties. dye loading and the efficient light harvesting from efficient
Hence, it is necessary to develop the semiconductor nanos- light scattering. The schematic representation of the feasible
tructures to further improve the performance of DSSCs. More growth mechanism for obtaining the different ZnO flower-
recently, the zinc oxide (ZnO) nanostructures have been like nanostructures are presented in figure 5.
9
Nanotechnology 30 (2019) 392001
Table 2. Comparison of specific reversible capacities of various structured/doped ZnO nanocomposites prepared by different methods for the lithium-ion cell.
Initial capacity Cyclic Current density

Materials Synthesis method (mAh g−1) performance (mA g−1) Voltage window Ref/year
ZnO nanorod (1D) Simple and low-impact wet chemistry approach 311 100 100 0.0–3.0 V [72]/2017
165 30
1212 400
∼300 105 at 100th
cycle
ZnO brush (3D)
ZnO nanosheets (2D)
ZnO multilayer-nanosheets (2D)
ZnO-NS Hydrothermal synthesis ∼1200 ∼390 ∼177 0.0–3.0 V [73]/2016
∼590 ∼380
∼1480 ∼600
G110-ZnO NS
G350-ZnO NS
DLZO Modified Hummers method ∼1010 ∼90 100 0.02–3.0 V [74]/2016
∼1360 ∼90
∼1585 753
∼1390 518 at 65th cycle
ZONC
10
SAZO@rGO
DLZO@rGO
ZnO Hydrothermal method ∼1280 105 100 0.01–3.0 V [75]/2017
∼1580 ∼500
ZnO-43 wt%G
∼1580 ∼600
ZnO-61 wt%G ∼1950 ∼765 at 100th
cycle
ZnO-71.5 wt.G
ZnO/CNF-0.5 Single-nozzle electrospinning method 1233 723 at 100th 100 0.005–2.8 V [76]/2017
cycle
ZnO Hydrothermal process and subsequent thermal ∼980 ∼10 at 60th cycle 100 0.01–3.0 V [77]/2016
treatment
ZnO@C ∼1185 403
ZnO@CF ∼1480 850 at 200th
cycle
ZnO/3-dimensionally ordered macro-/mesopor- Typical dual templating method used silica opal 1966 1397 at 300th 97.8 0.01–3.0 V [78]/2018
ous carbon (ZnO/3DOM-mC-40 wt% ZnO and phenol followed by simple in situ solu- cycle
loading) tion growth
[79]/2018
Topical Review
ZnO/CNFs Electrospinning method 1188 403 200 0.01–3.0 V
∼1175 520
∼600 552
ZnO/CNFs-PA-0.4 ∼1680 702
Table 2. (Continued.)

ZnO/CNFs-PA-0.6 ∼1480 600 at 200th
cycle
ZnO/CNFs-PA-1.0
ZnO/CNFs-PA-1.3
ZnO@C NS Extended Stober method 1234 496 at 200th 82.5 0.01–3.0 V [80]/2016
cycle
ZnO Simple carbonization process used ZIFs-8 as a 1442 172 100 0.01–3.0 V [81]/2017
template and precursor
ZnO/ZnO@C
1442 839 at 50th cycle
ZnO ZIF-8 framework with water vapour-assisted 979 310 98 0.01–3.0 V [82]/2017
method followed by thermal treatment
1922 1177 at 100th
cycle
ZnO/N/CF
ZnO-N-rich mesoporous carbon Nanospheres Aerosol-assisted copolymerization 2627 1059 at 100th 200 0.01–3.0 V [83]/2017
(ZnO-NMPCS) cycle
ZnO nanorods Hydrothermal synthesis and subsequent ∼420 88 at 50th cycle 200 0.01–3.0 V [84]/2018
11
calcination
∼900 464
905 565 at 200th
cycle
ZnO@C nanorods
Peapod-like ZnO@C
ZnO Hydrothermal synthesis followed by a thermal 2953 ∼300 100 0.05–3.0 V [85]/2018
treatment under N2
2384 338
2414 527
2379 410 at 100th
cycle
ZnO@C-20
ZnO@C-30
ZnO@C-50
ZnO Atomic layer deposition (ALD) method ∼1100 ∼50 100 0.01–3.0 V [86]/2017
2096 1026 at 500th
cycle
ZnO-CB
[87]/2017
Topical Review
ZnO/MWCNTs Facile self-assembly method 1253 437 at 100th 100 0.01–3.0 V
cycle
Table 2. (Continued.)

ZnO Zn-based metal organic framework template ∼1130 ∼160 200 0.01–3.0 V [88]/2017
(ZIF-8) followed by heat treatment at 300,
400 and 500 °C
MWCNTs/ZnO-400 °C (MCZO-400) ∼1215 420 at 100th
cycle
Commercial ZnO One-step pyrolysis of hollow metal organic 1300 248 100 0.01–3.0 V [89]/2017
framework (MOF-5)
1514 289
1928 750 at 100th
cycle
Hollow ZnO
Hollow ZnO@C nanocages
Commercial ZnO Liquid-phase method 1128 25 at 30th cycle 100 0.01–3.0 V [90]/2018
CNT-20@ZnO 1327 709
1391 598 at 50th cycle
CNT-30@ZnO
ZnO Pseudo-sold-state method ∼1200 193 at 25th cycle 100 0.01–3.0 V [91]/2017
ZnO/NC/Cu (1:1) ∼1040 602
12
∼1110 415
∼1230 370 at 100th
cycle
ZnO/NC/Cu (1:2)
ZnO/NC/Cu (2:1)
LiFePO4/C (LFP) Sol-gel assisted ball-milling route ∼30 ∼30 170 2.8–4.2 V [92]/2017
∼90 ∼82
LiFePO4/C-ZnO-1 (LFPZ1) ∼135 ∼130
∼80 ∼70 at 50th cycle
LFPZ2.5
LFPZ-5
LiMn2O4 Combustion method 120 69 74 3.0–4.5 V [93]/2016
116 ∼82
113 ∼95
103 ∼50 at 500th
cycle
1 wt% ZnO/LiMn2O4
2 wt% ZnO/LiMn2O4
5 wt% ZnO/LiMn2O4
Topical Review
Figure 5. Schematic representation of the feasible growth mechanism for obtaining the different ZnO flower-like nanostructures. Reprinted
from [116], Copyright (2017), with permission from Elsevier.
In addition, Zamiri et al [117] reported the DSSCs with the electrode/electrolyte and supplied the direct electron
ZnO nanoparticles as a photoanode and graphene quantum transportation. Therefore, the TiO2-ZnO core-shell can be a
dots (GQDs) as a green photosensitizer. They fabricated the potential material as the photoanode for DSSC application.
DSSCs with different thicknesses of ZnO photoanodes from More recently, Hussein et al [120] prepared a ZrO2 surface
10–50 μm. The highest PCE of 1.26% was observed when modified ZnO/TiO2 composite film as a photoanode in
DSSC fabricating with 40 μm thickness of ZnO photoanode DSSCs and compared this with un-passivated ZnO/TiO2
due to the more photosensitizer molecules available in the DSSC performance. The obtained photovoltaic results show
semiconductor layer in order to absorb efficient sun-light. that the DSSC with the ZrO2 surface modified ZnO/TiO2
Marimuthu et al [118] investigated the effect of the light composite film exhibited the PCE of 6.97% with open circuit
scattering layer in the photoanode on the performance of voltage (Voc) of 0.87 V, short circuit current (Jsc) of
DSSCs. First, the TiO2-ZnO thin films were coated onto the 13.6 mA cm−2 and fill factor (FF) of 0.65 under simulated
FTO substrate via a spin coating method. Then, the flower- AM 1.5 solar irradiation, which was much higher than the un-
shaped ZnO nanorods were potentiostatically developed on modified ZnO/TiO2 composite film (3.41%). This higher
TiO2-ZnO films as a light scattering layer. The DSSCs con- photovoltaic performance might be due to the back electron
sisting of TiO2-ZnO thin film with a scattering layer exhibited transfer from the conduction band of the hetero-phase junc-
a PCE of 1.81% which is much higher than the TiO2-ZnO tions to the oxidized species in the electrolyte. Han et al [121]
thin film without the scattering layer (0.79%). The photo- reported that the well-crystalline ZnO nanoflakes via the
anode containing the light scattering layer possesses an hydrothermal process as the photoanode in DSSCs. In addi-
excellent light scattering effect and more dye loading, tion, the DSSC assembled with a ZnO nanoflake photoanode
resulting in an increase of the overall performance of DSSC. demonstrated an excellent PCE of 3.39% with Voc of 706 mV,
Recently, the spherical-shaped TiO2-ZnO core-shell nano- Jsc of 8.84 mA cm−2, and FF of 0.54 under sunlight intensity
particles were synthesized via a facile combined hydrolysis of 100 mW cm−2, which was due to the unique flake-like
and refluxing method by Manikandan et al [119]. After that, morphology and large surface area of the ZnO nanoflake
the DSSC fabricating with the TiO2/ZnO core/shell photo- photoanode.
anode displayed the enhanced PCE of 0.55% as compared Kim et al [122] developed the Ga-doped ZnO (GZO) thin
with the pure TiO2 anode (0.36%). This enhancement may be films and used this as the photoanode in DSSCs. Moreover,
attributed to the reduced interfacial electron recombination in the TiO2 blocking layer was deposited on the surface of GZO
13
Figure 6. J-V and IPCE curves for the fabricated DSSC with small and large ZnO platelets. Reprinted from [124], Copyright (2017), with
permission from Elsevier.
in order to protect the GZO and to improve the photovoltaic photoanodes. Manthina et al [127] developed a novel nano-
performance. The DSSCs assembled with the GZO/TiO2 thin composite structure consisting of ZnO nanorods coated with
film exhibited the PCE of 4.02% which was higher than that of TiO2 nanoparticles using an electrostatic layer-by-layer
pure GZO thin film (3.36%). This improved performance of deposition method. They found that the designed ZnO-TiO2
DSSC could be attributed to the decreased charge recombination composites exhibited an improved electron transport along
and series resistance caused by the influence of the TiO2 with nanorods and surface area provided by the nanoparticles,
blocking layer. Thereby, it revealed that the GZO/TiO2 thin which was favourable for good charge collection and light
film was an outstanding electrode to achieved high-efficiency harvesting. Moreover, the ZnO-TiO2 composite film-based
DSSCs. Kao et al [123] depositing the ZnO nanowires with DSSC provided the better current values than the conven-
different lengths from 1–4 μm on to ITO substrates by a facile tional TiO2 films. The SEM images at 1 μm of ZnO nanorods
solution phase deposition method and utilized this as the pho- coated with TiO2 with different immersion periods of 0, 1, 3
toanode in DSSCs. The obtained results revealed that the and 5 min are given in figure 7.
increases in length of ZnO nanowires can increase the adsorp- Liu et al [128] synthesized ZnO nanowires via a facile
tion of the dye molecule through ZnO nanowires to enhance the ZnO nanoseed-mediated microwave heating growth method.
Jsc and Voc, resulting in better photovoltaic performance of They obtained the vertically aligned ZnO nanowire arrays with
DSSC. The highest PCE of 1.49% was noted for DSSC fabri- a length of 3.4, 7.3, 10.8, 14.7, and 17.2 μm after growing for
cated with the ZnO nanowires length of 3 μm. Marco et al [124] 1, 2, 3, 4, and 5 h, respectively. These synthesized ZnO
synthesized the single crystal mesoporous ZnO platelets with nanowires were further used as the photoanode in DSSCs. The
small and large sizes in order to employ the high performance PCE of ZnO nanowire-based DSSCs were found to be
DSSCs. They noted that the DSSC fabricating with small-sized increased with increasing the length of the nanowires, which
ZnO platelets attained the highest PCE of 5.63% with Voc of was due to the dye-loading amount enhancement in the longer
774 mV, Jsc of 12.42 mA cm−2 and FF 0.59 as compared with ZnO nanowires by enlarged internal surface area. The DSSCs
that of DSSC with large-sized ZnO platelets (4.88%). In addi- based on ZnO nanowires reached a maximum PCE of 1.25%
tion, the J-V and IPCE curves for the fabricated DSSC with when the length of the nanowires was up to 17.2 μm. Gao et al
small and large ZnO platelets are shown in figure 6. [129] fabricated the DSSC based on ZnO nanowire-structured
Moreover, Martinson et al [125] developed the ZnO photoanodes. They observed that the enhanced PCE of 1.7%
nanotubes with large surface area and used this as the pho- for DSSC with ZnO nanowire obtained from 5 ml of ammonia,
toanode in DSSCs. This obtained ZnO nanotube-based DSSC which was much higher than the ZnO nanowire obtained from
displayed the high PCE of 1.6% with Voc of 739 mV, Jsc of 2 ml of ammonia (0.5%). Afterwards, Abraham et al [130]
3.3 mA cm−2 and FF 0.64. Marczak et al [126] studied the synthesized the CuO-ZnO nanocomposite using a simple co-
effect of calcination temperature of ZnO nanoparticle-coated precipitation method using oxalic acid and used this as the
FTO substrates on photovoltaic performance of DSSCs. They photoanode in DSSCs. The DSSC fabricated with a CuO-ZnO
prepared four different ZnO nanoparticle-coated FTO photo- nanocomposite exhibited an enhanced PCE of 3.2% than that
anodes with different calcination temperature of 400, 425, of pure ZnO (2.1%). Cheng et al [131] assembled the DSSC
450, and 475 °C. Also, the photovoltaic results demonstrate based on branched ZnO nanowires with PCE 1.51%, which
that the DSSC fabricated with the ZnO photoanode obtained was much higher than the DSSC based on a bare ZnO nano-
from 425 °C showed a higher PCE of 1.07% than the other wire (0.75%). The improvement might be attributed to the
14
was noted that the good synergetic effect between ZnO and
TiO2 increased the dye absorption, electron transport and
electron lifetime, resulting in the improvement of the overall
performance of DSSCs. Therefore, the designed ZnO/TiO2
nanocomposite can be a potential electrode material in
DSSCs. Additionally, Zhou et al [138] synthesized the ZnO/
NiO composite photoanodes for DSSCs. The ZnO/NiO
composite-based DSSC showed higher PCE of 6.60% than
the pure ZnO-based DSSC (5.04%). The enhanced perfor-
mance of the DSSCs in a ZnO/NiO composite was mainly
attributed to the energy level potential difference between
NiO and ZnO, which accelerated the electron transfer at the
ZnO/dye/electrolyte interface. In addition, the saturated
Zn(Ac)2 ethanol solution-processed ZnO/NiO composite
photoanodes attained a superior PCE of 7.01% as compared
with isolated ZnO/NiO photoanodes. Hence, this study
indicated that the obtained Zn(Ac)2 ethanol solution-pro-
Figure 7. SEM images at 1 μm of ZnO nanorods coated with TiO2 cessed ZnO/NiO composite is a promising candidate as a
with different immersion periods of (a) 0, (b) 1, (c) 3 and (d) 5 min. photoanode in DSSC applications. Also, the schematic dia-
Reprinted with permission from [127]. Copyright (2012) American gram for the charge transfer mechanism of the ZnO/NiO
Chemical Society. composite photoanode in DSSCs is shown in figure 8.
Raj et al [139] synthesized the banyan root-like Mg-doped
enlargement of the internal surface area within the photoelec- ZnO with different mole ratios of Mg, which was used as the
trode that increased the dye adsorption and hence, enhanced photoanode in the DSSCs. The DSSC fabricated with 5% of
the overall performance of the DSSCs. Chandiran et al [132] the Mg-doped ZnO photoanode presented the outstanding PCE
deposited the mesoporous ZnO with different thicknesses by of 4.11% with Voc of 710 mV, Jsc of 9.98 mA cm−2 and FF of
atomic layer deposition (ALD) on mesoporous insulating alu- 0.58 under 1 AM sun illumination than that of a pure ZnO
mina performs, which were used as photoanodes in the DSSCs. photoanode (1.97%). The enhanced performances might be
Also, they achieved 4.4% of PCE for the DSSC made with a due to the high electron transport, retardation of interfacial
5 nm ultrathin ZnO overlayer on a 3 μm mesoporous alumina charge recombination and enhanced light harvesting efficiency
film. Sonker et al [133] obtained the ZnO spherical nanos- of the Mg-doped ZnO photoanode. Qiu et al [140] constructed
tructure (SNSs) film using the sol-gel route and used this as the the hierarchical ZnO nanorod-nanosheet structures on the ITO
photoanode for DSSCs. Furthermore, the DSSC fabricated substrate using a two-step electrochemical deposition process
with ZnO SPSs photoanode displayed the PCE of 1.3% with for the application in DSSCs. The hierarchical ZnO nanorod-
Jsc of 3 mA cm−2, Voc of 0.62 V and FF of 0.66 at 1 AM sun nanosheet photoanode-based DSSC showed a higher PCE of
condition. 4.11% when compared to the DSSC based on bare ZnO
El-Shazly et al [134] prepared the Sn2+-substituted ZnO nanosheet arrays (2.85%). An increased DSSC performance in
nanopowders with different content of Sn2+ using a co-pre- the ZnO nanorod-nanosheet photoanode might be ascribed to
cipitation method for DSSCs application. The DSSC assem- the enhancement of dye loading by the large internal surface
bled with 5% weight ratio of a Sn2+ ions-substituted ZnO area within the nanostructure photoelectrode. Chen et al [141]
photoanode gave a superior PCE of 4.3% as compared with reported a glucose-modified hierarchical ZnO with a 3D micro-
the pure ZnO photoanode (3.0%). Meng et al [135] synthe- flower (MF) structure as the photoanode for the DSSCs. They
sized the 3D nanoparticle-based ZnO hierarchical spheres prepared the glucose-modified ZnO MFs with the different
(ZnO-HS) via a simple hydrothermal method. These synthe- modification times from 1 to 8 min through a facile and simple
sized ZnO-HSs were further utilized as the overlayer for light immersion method in glucose solution at room temperature.
blocking in DSSCs with ZnO nanoparticles (ZnO-NP). The Among them, the DSSC constructed with glucose-modified
obtained results clear that the DSSC made with ZnO-NP/ ZnO MFs with an immersion time of 2 min attained the best
ZnO-HS double-layered showed the highest PCE of 3.40% PCE of 5.31% as compared with pure ZnO MFs, which might
than the bare ZnO-NP (1.68%). In another study, Thambi- be due to the prevention of the dye aggregation and the high
durai et al [136] reported the ZnO nanorods using a chemical recombination resistance resulting of glucose molecules on
bath deposition method as the photoanode in DSSCs. The ZnO surfaces. Furthermore, the glucose-modified ZnO photo-
obtained ZnO nanorod-based DSSC showed the PCE of anodes had a large electron lifetime and long electron diffusion
0.71% with Voc of 270 mV, Jsc of 4.08 mA cm−2 and FF of length, which might be the reason for the enhanced photo-
0.32. Shalan et al [137] designed the ZnO/TiO2 nano- voltaic performance of DSSCs.
composites supported on the FTO substrate as the photoanode In addition, Puyoo et al [142] developed the ZnO
in DSSCs. The DSSC constructed with ZnO/TiO2 nano- nanowire/nanoparticle composite through a simple and low-
composite displayed an excellent PCE of 6.5%, which was cost wet-chemical route. The as-prepared ZnO nanowire/
much higher than that of bare ZnO nanoparticles (3.8%). It nanoparticle composite served as the photoanode in the
15
Figure 8. Schematic diagram for the charge transfer mechanism of the ZnO/NiO composite photoanode in DSSCs. Reprinted from [138],
Copyright (2018), with permission from Elsevier.
DSSC. They observed that the ZnO nanowire/nano-particle (1.50%). Yu et al [147] reported the ZnS/ZnO hetero-
composite-based DSSC showed a much better photovoltaic nanostructures as the photoanode for DSSCs. They synthe-
performance with a PCE of 4.7% than that of those bare ZnO sized with two different nanostructures like ZnS/ZnO coaxial
nanowires (0.6%) and ZnO nanoparticles (2.1%). Wu et al nanowires and ZnS/ZnO hierarchical nanowires by chemical
[143] prepared the low-density ZnO micron rods (MRs) on a bath deposition and chemical etching processes, respectively.
ITO/PEN substrate using a hydrothermal method, which was The ZnS/ZnO coaxial nanowires showed a higher PCE of
mixed with ZnO nanoparticles to make ZnO composite 0.76% than the ZnS/ZnO hierarchical nanowires (0.33%).
photoelectrode under pressures 418 kg cm−2 for DSSCs The coaxial nanostructures possess high capability on the
application. They noted that the DSSC fabricated with ZnO prevention of electron back transfer, resulting in higher power
composite structure exhibited the better PCE of 3.46% than conversion efficiency. Meng et al [148] synthesized 2D ZnO
that of pure ZnO nanoparticles (2.21%). In another invest- nanosheet-structures using a simple citric acid-assisted
igation, Lu et al [144] prepared hierarchical ZnO micro- hydrothermal route. The DSSC made with ZnO nanosheets as
architectures using a simple and economical citrate-mediated the photoanode exhibited a PCE of 1.82% which was about
hydrothermal route for DSSCs. They found that the hier- 1.5 times higher than ZnO nanorods. The enhancement in
archical ZnO microarchitecture-based DSSC showed an DSSC performance of 2D sheet-like ZnO nanostructures was
improved PCE of (0.54%) when compared with ZnO nanor- mainly due to the increased light scattering and dye loading
ods (0.41%) and ZnO nanoparticles (0.19%). This improve- properties.
ment in ZnO microarchitectures was mainly ascribed to the Yin et al [149] synthesized the ZnO nanocrystals via a
large surface area for dye loading and the rapid transportation one-step solid state reaction at room temperature and this was
of electrons. used as the photoanode in the DSSCs. The as-synthesized
Furthermore, Yi et al [145] deposited the randomly ZnO nanocrystal-based DSSC exhibited the PCE of 3.76%
oriented ZnO microsheets on TiO2 nanoparticle film as the with Voc of 688 mV, Jsc of 8.55 mA cm−2 and FF of 0.64. In
scattering layer by a cathodic electrodeposition method. The another study, Bu et al [150] synthesized the ZnO-decorated
photovoltaic results indicate that DSSC fabricated with SiO2 nanosheets via a sol-gel deposition process followed by
ZnO/TiO2 composite showed higher PCE of 2.58% as the photoelectrode prepared at three different annealed tem-
compared with pure TiO2 (1.79%). Yun et al [146] investi- peratures of 400, 500 and 550 °C for DSSCs. The DSSC
gated the influence of the heat treatment of well-aligned ZnO fabricated with the ZnO-decorated SiO2 composite electrode
nanorods on the photovoltaic performance of DSSCs. The obtained by an annealed temperature of 500 °C showed the
heat treatment of well-aligned ZnO nanorods was carried out highest PCE of 0.98% than the other electrodes. Lee et al
at 200–500 °C for 1 h. The dye adsorption ability of ZnO [151] designed the Al-doped zinc oxide (AZO) layer as a
nanorods were found to be increased with increasing temp- transparent conducting oxide (TCO) layer for making ZnO
erature, yielding an enhanced photovoltaic performance. The nanowire (NW) photoanodes for DSSCs. The well-aligned
DSSC assembled with ZnO nanorods with heat treatment at single crystalline ZnO NW arrays grown on the AZO films
500 °C presented a maximum PCE of 1.97% when comparing showed an outstanding DSSC performance with a PCE of
the DSSC with ZnO nanorods without heat treatment 0.6% when compared with ZnO NW arrays grown on FTO
16
films (0.4%). Du et al [152] fabricated TiO2/ZnO core-sheath nanoparticle aggregates using a facile wet chemical method.
nanofibers (NFs) films as the photoanode for DSSCs by a These nanostructures were tried for their photocatalytic
coaxial electrospinning method. The fabricated TiO2/ZnO activity on RhB, Mb and malachite green (MG) and it was
composite film exhibited a good PCE of 5.17% which was demonstrated that ZnO nanoplates displayed improved pho-
higher than the DSSCs based with TiO2 NFs film (4.47%). tocatalytic activity for the degradation of all three dyes. The
Liu et al [153] prepared the ZnO nanoflowers via a facile observed enhanced photocatalytic activity of ZnO nanoplates
solution phase method at room temperature. After that, they for the degradation of organic dyes under sunlight exposure
had made ZnO nanoflowers/TiO2 nanocomposite photo- was credited to their larger surface area and higher defect
anodes by a doctor blade method with different mass ratios of concentration leading to enhanced dye adsorption, improved
100:0, 75:25, 25:75 and 0:100 of ZnO/TiO2. Among these, sunlight utilization capability and high photocatalytic activity
the DSSC based on ZnO/TiO2 with mass ratios of 25:75 of the uncovered aspects. ZnO nanocrystalline materials with
achieved a higher PCE (2.82%) as compared with pure ZnO various crystallite and particle sizes were synthesized by the
(1.59%) and pure TiO2 (1.82%). Sonker et al [154] reported
solvothermal approach by John Becker et al [168]. It was
the ZnO with nanoneedle-like morphology for DSSCs
observed that the particle size of ZnO could be constrained by
application. They demonstrated that the DSSC fabricated with
changing the solvent and reaction conditions. The catalytic
a ZnO nanoneedle showed the PCE of 4.2% with Voc of
function was assessed by the degradation of the RhB under
480 mV, Jsc of 20 mA cm−2, and FF of 0.44, which was much
higher that the DSSC based on a ZnO nanoparticle (1.7%). visible light illumination. Commonly, the well crystalline
ZnO sample displayed higher rate constants for the degrada-
tion of RhB.
2.4. Photocatalysis
In recent years, effort has been made for developing highly

active heterogeneous photocatalysts for environmental appli- 2.4.1. ZnO/Carbon composite. Graphene has attracted
cations. Among various semiconductor metal oxides used in tremendous attention because of its exceptional properties in
photocatalysis, ZnO is the most extensively studied photo- the preparation of graphene-based composites for different
catalyst for its low toxicity, wide bandgap (3.37 eV), long-term applications. Kanika et al [169] developed two different
stability, high photostability, and high efficiency [155–157]. strategies to load ZnO nanorods onto reduced graphene oxide
However, the application of the ZnO semiconductor is limited (RGO) sheets, i.e., in situ growth and a self-assembly
due to the fast recombination rate of the photogenerated elec- approach. Significantly improved photocatalytic activity of
tron–hole pairs [158, 159]. This diminishes the efficiency of RGO/ZnO nanocomposites in contrast to bare ZnO
photocatalytic reaction. The substantial amount of work was nanoparticles was revealed by the degradation of MB under
already done to clarify the structure property relationship in irradiation, which could be attributed to the inhibition of
heterogeneous photocatalysis and to reveal the valuable data to electron–hole pair recombination and enhanced adsorption due
design and the working of effective photocatalysts. The surface to the presence of RGO sheets. Suneel Kumar et al [170]
morphology, crystallinity, size and oxygen defects are a few synthesized graphene QD-incorporated ZnO composites by a
factors that impact the catalytic activities and long-term stabi- simple hydrothermal method and used them as photocatalysts
lity of the ZnO catalysts. Hence, efforts have been made to for the degradation of MB and CZ under visible light. Under
improve the photocatalytic performance of ZnO via various illumination, ZnO-GQD composites show extremely improved
strategies, such as synthesis of ZnO nanorod arrays, combi- photocatalytic performances for the photodegradation of MB
nation with other components including noble metals, doping and CZ when compared to its pure sample. The optimized
and the inclusion of carbon materials [160–164]. sample with 2 wt% of GQD exhibited improved catalytic
Chiling et al [165] synthesized ZnO and applied it to the
activities. The enhanced photocatalytic activities of ZnO-GQD
photocatalytic degradation of acid blue 1 (AB1). To obtain a
might be due to more utilization of solar spectrum, fast charge
better understanding, the mechanistic details of this ZnO-
separation over the ZnO-GQD interface and high active surface
assisted photodegradation of the AB1 dye with low Watt UV
sites. The possible mechanism of ZnO-GQD heterojunction
irradiation was carried out. The degradation progresses
through competitive reactions such as N-de-ethylation, towards photocatalytic degradation is depicted in figure 9.
destruction of the conjugated structure, hydroxylation on the Carbon/ZnO nanocomposites were designed by Xiao et al
benzene ring, hydroxylation on the sulfonylated benzene ring, [171] using a low temperature precipitation process and
and substitution. ZnO nanoparticles were prepared by a TEMPO-oxidized (2,2,6,6-Tetramethyl-1-piperidinyloxy as
hydrothermal method using zinc chloride and ammonium TEMPO) cellulose as a reactive template. It was found that
hydroxide by Kumaresan et al [166]. The pH of the precursor the formation of carbon/ZnO nanocomposites with various
solution was varied to 7, 9, 11 and 13 by the addition of the morphologies not only involved the structure of TEMPO-
ammonium solution and the solution was hydrothermally oxidized cellulose but also depended on the content of the
treated at 150 °C for 3 h. Photocatlytic activity of the prepared carboxyl groups of TEMPO-oxidized cellulose. In this
ZnO nanoparticles was evaluated for rhodamine B (RhB) dye, approach, TEMPO-oxidized cellulose was not only a
which showed 94% of degradation and good stability for five template provider but also a C-provider leading to compound
cycles. Kavitha et al [167] synthesized ZnO nanoplates and ZnO nanocrystals, which decreased the band gaps of the
17
Figure 9. Schematic diagram of energy level diagram and a possible mechanism ZnO-GQD heterojunction of the charge carrier transitions for
the photocatalytic degradation of organic pollutants under visible light irradiation. Reprinted from [170], Copyright (2018), with permission
from Elsevier.
samples. ZnO-T12 exhibited a significant photodegradation on activity on RhB compared to that of P25 and ZnO. It was proved
MO with 96.11% within 120 min and for better reusability. that the degradation efficiency did not change after the three
cycles. Ahmed et al [176] fabricated Ag-doped ZnO (Ag/ZnO)
2.4.2. Metal-incorporated ZnO photocatalysis. Zahra et al
thin films and utilized them for the photodegradation of three
[172] prepared undoped ZnO and Mn-doped ZnO nanostructures different azo dyes (RR 195, RO 122, and RY 145). At a higher
with different doping concentrations through a simple chemical amount of photocatalyst, the active surface area is more for OH
method. The photocatalytic activities of the samples were radicals and therefore enhances the degradation rate. When the
investigated by the degradation of orange G solution under concentration of dye molecules increases, the degradation rate
sunlight irradiation. The results showed that doping Mn greatly was decreased due to the photons entering the solution and this
improved the photocatalytic efficiency of ZnO and 6% Mn- can be interrupted by the more number of dye molecules. As a
doped ZnO nanostructured exhibited the highest photocatalytic result of their investigation, the optimum amount of H2O2
activity under an irradiation time of 1 h. Na-doped ZnO (45 mg l−1) helps to improve the degradation performances and
nanocrystals (NCs) were effectively synthesized using a sol-gel also adding more amounts of H2O2 decreases the degradation
process by Asma Tabib et al [173]. The ZnO NCs were used as a rate. Thejaswini et al [177] synthesised potassium co-doped
photocatalyst to degrade RhB in solution, under solar irradiation. aluminium-doped ZnO nanoparticles (NPs) through a thermo-sol
Na doping enhances the photocatalytic activity of ZnO NCs until gelation process. The co-doping of K on Al–ZnO NPs was found
an optimum concentration of 0.5%, where a full degradation was to have a significant influence on the bandgap narrowing of ZnO,
observed after 120 min of sun light irradiation. Based on to an extent that the entire light absorption was shifted towards
scavangers test, it was found that both superoxide and hydroxyl the visible-light spectrum. The bandgap energy levels for bare
oxidizing radicals are mainly active. A high-performance visible- ZnO, Al-doped ZnO, and K co-doped Al–ZnO NPs were 3.26,
light-active (Al, Ni) co-doped ZnO catalyst was successfully 3.03 and 2.88 eV, respectively. The photocatalytic properties of
synthesized by Neelakanta et al [174] using high-energy ball the K co-doped Al–ZnO photocatalyst through direct green 6
milling. The doping of Ni did not significantly upgrade degradation studies was compared with well-known Al–ZnO
absorption but additionally enhanced the photo-induced charge NPs. They found that under optimized conditions, the K co-
separation, which extraordinarily enhanced catalytic activity. The doped Al–ZnO photocatalyst could induce complete dye
performances of the photocatalyst were evaluated by considering degradation within 0.5 h under visible light.
the degradation of MO and CR as targeted organic pollutants
under visible light. Furthermore, trapping tests expressed that 2.4.3. ZnO/metal oxide composite. Fe3O4-doped ZnO
O2− assumes a noteworthy role in the dye degradation in the nanospheres were synthesized by a sol-gel process and
photocatalytic framework. A series of Ag/ZnO nanocomposites compared with pristine ZnO nanospheres towards photo-
were prepared by microwave-assisted hydrothermal synthesis by catalytic properties [178]. Implantation of Fe3O4 in ZnO
Xin et al [175]. The results proved that the crystal structure did nanospheres modifies the UV absorption edge, and it
not alter significantly and light absorption by the composite was displays near-bandgap emission and deep-level emission.
clearly enhanced. The composite was tested for its photocatalytic The photocatalytic activity of Fe3O4-doped ZnO nanospheres
18
under visible light irradiation. It achieved degradation

efficiency of 86.93%, 89.3%, and 93.3% for CV, BPB and
EY, respectively, in 50 min. The nanocomposites exhibit
higher activity relative to pure ZnO. This excellent
photocatalytic performance might be attributed to the
efficient separation of photogenerated electron–hole pairs
compared to pure ZnO.
2.5. Biosensor
In recent years, ZnO-based nanostructured materials were

shown to be a suitable candidate for binding biological sub-
stances. Recent research reveals that the inspiration behind
the use of nanostructures for biosensing applications are
increasing the surface-to-volume ratio, which enhances their
reactivity and allows them to translocate more easily through
Figure 10. Absorbance spectra of pure ZnO, Bi2O3 and ZnO/Bi2O3 the cell membrane and efficiently bind analytes. Researchers
bilayers deposited on glass and spectral emission of visible light developed electrochemical sensors based on nanostructures of
lamp used in the photocatalytic measurements. Reprinted from ZnO and its composites for biosensing and environmental
[179], Copyright (2018), with permission from Elsevier.
applications. The ZnO has been reflected as a transductor/
transduction material for the development of biosensors. It
was studied against RhB dye, which was found to have higher has an inbuilt ability to form anisotropic nanostructures that
photocatalytic activity than that of pristine ZnO nanospheres have the aptitude to deliver drugs, in cancer treatment,
and revealed that Fe3O4-doped ZnO nanospheres are a detecting biomolecules as well as creating novel bioelec-
promising photocatalyst. Medina et al [179] reported a tronics devices [182]. These ZnO nanostructures have specific
novel way to fabricate supported ZnO/Bi2O3 heterostructures surface selectivity that is favourable in biosensing applica-
for the visible-light photocatalytic degradation of organic tions. An independent molecule of ZnO crystallizes in three
compounds. This 2D-heterojunction was produced by forms of zinc blende, wurtzite and rocksalt, among which the
depositing Bi2O3 dots by sputtering onto a ZnO thin film hexagonal wurtzite form is more unwavering thermo-
deposited on glass substrates by spray pyrolysis. It was found dynamically [183]. It has been observed that the anisotropic
that the ZnO/Bi2O3 bilayers with heterojunctions showed structure of ZnO exhibits higher electron mobility and a dif-
enhanced photodiscoloration and mineralization under visible fusion coefficient when compared with other metal oxides.
light compared to the ZnO and Bi2O3 films separately. This This feature makes the ZnO nanostructure highly desirable as
might be due to the positive synergistic impact in which an electrochemical biosensor [184]. The ZnO nanorod, in the
Bi2O3 extends the absorption range of the film to the visible area of biosensing has revealed many benefits, which includes
region and the proper alignment of the electronic band edges biological compatibility, fast electron transfer rates and the
initiates charge separation with the consequent decrease in the ease of preparation [185]. The collection of ZnO nanos-
recombination rate. Figure 10 shows the absorption spectra of tructures prepared under controlled reaction conditions by a
pure ZnO, Bi2O3 and ZnO/Bi2O3 bilayers spectral emission thermal evaporation method is displayed in figure 11.
of visible light lamp used in the photocatalytic experiments. Nanolaminates are yet another achievement ZnO has
The Ag2S/g-C3N4/ZnO nanoarray heterojunction with accomplished in relation to optical biosensors. These share the
different amounts of Ag2S was synthesized using a simple characteristics of a typical nanomaterial by having inbuilt
chemical method by Yimeng et al [180], in which a core-shell properties like biocompatibility, non-toxicity and chemical
structure was formed. ZnO acts as the core while g-C3N4 and stability [187]. Three methods were reported so far, through
Ag2S are the shells in order to absorb visible light and to which ZnO nanomaterials can be efficiently synthesized,
restrain photo-corrosion. The photocatalytic performance of vapour phase methods, electrochemical deposition synthesis,
g-C3N4/ZnO was 2 times higher than that of pure ZnO NRs. and synthesis by electrospinning each having their own pro-
Layered-structure g-C3N4 offers the opportunities for rapid minence [188]. It was reported that ZnO has also been inves-
electron transfer process to enhance photocatalytic tigated as a luminescent material for almost over 70 years
performance. The photocatalytic performance of optimal [189]. So far, various forms of ZnO nanomaterials have been
material, as Ag2S/g-C3N4/ZnO, was 6 times than that of reported of their synthesis. Some of them are nanohelixes,
pure ZnO NRs. The broader and stronger absorption of visible nanobows, nanopropellers, nanowires, and nanocages of ZnO.
light makes a great contribution to enhancing photocatalytic
performance. ZnO and AgBr–ZnO nanocomposites were 2.5.1. Biosensors associated with ZnO. Quantitative
prepared through a simple precipitation method by Ahmed detection of a few parameters that takes place through
et al [181]. The photocatalytic activity of AgBr–ZnO was complex biochemical reactions is regulated by a biosensor
investigated for the degradation of three dyes: crystal violet system. Biosensors have evolved through a span of three
(CV), bromophenol blue (BPB), and Eosin Y (EY) dyes, generations, each generation having its own perspective of the
19
Figure 11. A collection of ZnO nanostructures prepared under controlled reaction conditions by a thermal evaporation method. Reproduced
from [186]. © IOP Publishing Ltd. All rights reserved.
concept. The first generation normal reaction products diffused demonstrated in cancer treatment. Biosensor research had a
to the transducer, leading to an electrical response [190]. The boost since there was a rapid prevalence of diseases and an
second-generation biosensors involved a mediator that increase in the demand for a sophisticated healthcare
performed a redox reaction mediator between the enzyme infrastructure for reliable and stable disease detection [196].
and its substrate and the eventual oxidation of the mediator by These biomarkers, since then were considered to be specific
the electrode. Co-immobilization was introduced in the third cues for diagnosing diseases along with a wide range of
generation at the bio-recognition component, which makes the therapeutic management for numerous diseases. The detection
electrode transducer provide direct electrical contact between of a disease, analysing it and monitoring it has gained its pace
the enzyme and the electrode [191]. The promising prodigy for since biomarkers proved to be gainful in offering crucial
a bioimaging probe is photoluminescent ZnO QD. ZnO information regarding various facets of it [197].
nanostructured materials have been a rapidly developed pH-
responsive drug carrier [192]. Many types of biosensors have 2.5.3. Biosensers applied to treatment of meningitis.
been reported to be in activity, but a few prominent types are Meningitis is a severe case of bacterial infection caused by
hydrogen peroxide biosensors, enzymatic biosensors, non- the Neisseria meningitides, commonly called meningococcus. It
enzymatic biosensors, glucose biosensors etc [193]. has different modes of infection like bacterial, viral and fungal,
but a high percentage of deaths are seen in people with bacterial
2.5.2. Nanomaterials allied with cancer treatment and other interference [198]. Since it is a gram negative bacteria, its
disease detection. Patients inflicted with cancer have diagnosis includes a gram-staining technique followed by many
chemical substances in their body fluids and tissues called other diagnostic tests, like the latex agglutination test, PCR etc.
cancer biomarkers which have a relation to malignancy of the Even after we run these tests for diagnosing the infection, these
tumour [194]. Biosensors are effectively used for the early cannot be deemed as confirmatory tests as they just give the
diagnosis of cancer as they are cost-effective, easily and outline of the condition. On top of that, these tests are very time-
readily detectable, have good portability, and there is an consuming and expensive. Hence, an alternate method should
absence of side-effects once used etc. The paratope and be proposed with lesser time consumption and more
the epitope interaction provides an initiation for the affordability. This is where DNA biosensors come into the
biosensors for the detection of cancerous molecules in the picture. A DNA biosensor is a revolutionary improvement in the
body [195]. A mesoporous ZnO nanofiber (nF)-based label- field of nanomaterials. As discussed above, biosensors have
free immunosensor provides a befitting platform for detecting been contributing a huge deal of research lately, and this DNA
breast cancer diagnostics and also facilitates many such biosensor has been the intriguing and fascinating part of it. It is
applications efficiently for detecting other biomarkers. The widely used in disease diagnosis and therefore contributes to the
fabrication of rapid detection and highly sensitive label-free detection and, to some extent, the treatment of it. Sometimes,
immunosensors, which was carried out by anchoring ZnO alone will not be able to fulfil its function in the need for
eletrospun mesoporous ZnO nanofibers, have been efficiently better biocompatibility. In such cases, ZnO can be doped with a
20
nickel compound, to enhance its intrinsic nature and developing recognized as safe’ (GRAS) by the US Food and Drug
its biosensing properties. Since, nickel and ZnO share similar Administration (21CFR182.8991). This has been used as a
ionic sizes, this Ni doped ZnO complex matrix becomes a food additive and also as the most common zinc source in the
promising biosensing tool [199]. fortification of cereal-based foods. One of the reasons to
choose this is based on its antimicrobial properties, ZnO has
2.6. Biological applications been incorporated into the linings of food cans in packages
for meat, fish, corn, and peas to preserve colours and to
ZnO-based nanostructures possess various properties like prevent spoilage majorly in the food industries [212].
optical, semiconducting, piezoelectric, and thus ZnO nanos- ZnO is recognized as safety material by US Food and
tructures were studied for various biological applications such Drug Administration. ZnO QD treated mice exhibited no
as bioimaging, inorganic antimicrobial agents, antibacterial haemolysis even at high concentration 1600 μg ml−1 [213]. It
activity, cosmetics and drug delivery, etc [200]. showed an antibacterial effect towards gram-positive and gram-
negative bacteria. The antibacterial activity of ZnO nanopar-
2.6.1. Bioimaging. Intrinsic fluorescence property and the ticle might be due to the accumulation of NPs on the outer
penetration ability of ZnO material was used to image in vitro membrane of bacterial cells which induces excess ROS and
and in vivo. The optical property of ZnO materials are able to releases Zn2+ [214]. To understand the molecular mechanisms
tune using different dopants, such as Co, Cu and Ni [201]. ZnO of the ZnO nanoparticle action against bacterial cells, the study
coated with polymer exhibited stable luminescence under UV was executed as a set of C. jejuni genes involved in general and
and showed no toxic effect [202]. The nanoparticle exhibited a oxidative stress responses, motility, pathogenesis, and toxin
fluorescence signal after 90 min of intra dermal injection and production. Based on the expressed genes, especially oxidative
after 30 min of intravenous injection in mice model. The stress genes, katA (encoding catalase) and ahpC (encoding
nanoparticle does not exert any toxic effect in mice [203]. Gd- alkyl hydroperoxide reductase), and one general stress gene,
doped ZnO QDs having 6 nm size exhibited maximum dnaK (encoding a chaperone), were found to be upregulated
intensity at 550 nm does not induce toxicity on HeLa cells 52-, 7-, and 17-fold, respectively in response to the treatment
and is used to image with confocal microscopy and MRI with ZnO nanoparticles [215].
in vitro [204]. Similarly, Fe3O4-ZnO core shell nanoparticles
were studied for cancer imaging and therapy [205]. Green
fluorescent ZnO nanowire tagged with RGD peptide showed 2.6.3. Toxicity. ZnO nanocrystal encapsulated in phospholipid
better biocompatibility, no toxicity towards U87MG human micelles and conjugated with folic acid were found to
glioblastoma cells, water solubility and exhibited fluorescence biocompatible and accumulate throughout cytoplasm in KB
signal under a fluorescence microscope [206, 207]. cells. ZnO nanocrystals conjugated with transferrin was reported
to image cancerous cell with minimal toxicity [216]. ZnO and
HAuCl4 nanocomposites exhibit good biocompatibility and
2.6.2. Antimicrobial agents. ZnO-based nanostructures have
were found to internalize into endosomes and cytosol.
varied ranges of applications that include tissue regeneration
SiO2-coated ZnO nanoparticles having 200 nm diameter were
purposes. Tissue transplants and implants face a major threat
used to stain E. coli and exhibited a toxic effect to leukaemic
on contamination by microbes. This is when the antimicrobial
cells due to the dissolution of the ZnO surface [217]. A DOX-
and antibacterial biomaterials/nanomaterials come into the
loaded ZnO polymer matrix was up taken by cancerous cells and
picture. These are classified as organic and inorganic
released Zn2+ and ROS to induce a toxic effect to the cells.
antimicrobial agents. Inorganic antimicrobials/antibacterial
Thus, the nanoparticle can be used for chemotherapy [200]. The
agents have a little delayed reaction to contamination while,
size of the nanoparticle also plays a role in toxicity effect.
organic antimicrobials/antibacterial agents are very fast in
Surface-modified ZnO nanoparticles also showed variation in
their action [208]. There are few drawbacks for organic
toxic effect [218]. After the interaction with cell membrane, a
antimicrobials such as unstable at higher temperatures. This
release of Zn2+ causes lysosomal damage, mitochondrial
caused the microbes to develop drug resistance against the
perturbation, ROS production, excitation of pro-inflammatory
organic antimicrobials and thus the main concept of it has not
cytokine and chemokine production. Cytotoxicity of
been established. On the other hand, inorganic bacteria
nanoparticles is evaluated by MTT assay to detect
like metal oxides, though slow in action, are capable of
mitochondrial activity, LDH assay to estimate LDH release,
establishing an appropriate disinfection without any kind of
fluorimetric detection, etc. Few studies reported that ZnO
byproduct outburst. This indicated that inorganic
nanoparticles induce apoptosis by a p53 signalling pathway or
antimicrobial biomaterials are more stable and secure when
NF-kB signal way [219–221].
compared with the later one [209]. Figure 12 represents the
schematic illustration of the antimicrobial mechanism of
composite CS/nano-ZnO [210]. The ZnO nanoparticles act 2.6.4. Drug delivery. In the last few decades, ZnO quantum
on sensitively to the organism Campylobacter jejuni. This dots have been shown to have excellent luminescent
proved better MIC of around 0.05 to 0.025 mg ml−1, which is properties, together with their low-cost, low-toxicity and
8- to 16-fold lower than that for Salmonella enterica serovar biocompatibility. These properties of ZnO have turned into
Enteritidis and Escherichia coli O157:H7 (0.4 mg ml−1) one of the main candidates for bioimaging and drug delivery
[211]. ZnO is one of the listed materials as ‘generally application [222, 223]. Apart from imaging, ZnO nonmaterial
21
Figure 12. Schematic illustration of the antimicrobial mechanism of composite CS/nano-ZnO. Reprinted from [210], Copyright (2012), with
permission from Elsevier.
is also used for drug delivery application. ZnO nanomaterial major challenge in gene therapy is to prevent DNA from
encapsulated with doxorubicin showed 75% efficiency and it degradation and to increase the efficiency of cellular uptake.
released quickly at pH 7.4, which further needed to improve for ZnO nanoparticles showed a promising effect in gene
chemotherapy application. Chitosan-tagged ZnO nanoparticle delivery in various reports. 3D ZnO nanostructure was
increases the stability of nanoparticles and helps to deliver studied to deliver pEGFPN1 DNA to A375 human melanoma
doxorubicin to cancer cells [224]. Fe3O4-ZnO core shell cells. ZnO QD coated with poly(2-(dimethylamino)ethyl
nanoparticles, having a diameter of 16 nm, help to deliver methacrylate) used for pDNA delivery and it showed no
carcinoembryonic antigens into dendritic cells,which was used toxic effect on COS-7 cells [231].
as an imaging agent. The ZnO shell facilitates the cell
internalization and could easily detected by MRI in the
lymph nodes of mice [225]. Aminopolysiloxane-tagged ZnO
nanoparticles suppressed K562/A02 cell proliferation by UV 3. Summary and outlook for future directions
irradiation after incubation with nanoparticles [226]. Generally,
the use of organic dye molecules has allowed us to detect and Nanostructured materials associated with ZnO have a vast
observe a variety of substances, such as drugs, amino acids, range of properties to list. The major properties are optical,
nucleotides or materials, both outside and inside of the living high isoelectric point, large specific area, non-toxicity,
cells. They have also been mostly used to study the process of mechanical properties, bending strength and flexibility etc.
life chemistry to identify various diseases [227]. ZnO, with Each property is remarkable and diverse in an individual way
small particle size, makes zinc more easily absorbed by the as far as functioning and application. Extensive investigations
body. Thus, the nano-ZnO is commonly used as a food on the fundamental aspects of development, modification and
additive. Moreover, ZnO is graded as a ‘GRAS’ substance by utilization of ZnO-based nanostructures in the area of energy
the US Food and Drug Administration (FDA) [228]. With such and biological applications have received enormous attention
properties, ZnO nanoparticles have achieved major attention in by several researchers because of their fascinating properties.
medical biological and clinical applications. Compared to other In this review, we have focused on and presented a summa-
metal oxides, ZnO with the comparatively inexpensive and tive view on ZnO-based nanostructures with special promi-
relatively less toxic property exhibit excellent clinical and nence on its applications in the quest of supercapacitors, Li-
biological applications, such as anticancer, drug delivery, ion batteries, dye-sensitized solar cells, photocatalysis, bio-
antibacterial, and diabetes treatment; anti-inflammation; wound sensors, and the biomedical and biological fields. The key
healing; and bioimaging [229]. difficulties we tended to, in numerous examinations, talk
about in this review are identified with the advancement of
ZnO-based materials for its superior execution in various
2.6.5. Gene delivery. The drug delivery system helps gene applications.
delivery for various application. The plasmid containing ZnO-based nanostructures were found to demonstrate
genes of interest helps to target the specific tissue [230]. The excellent energy storage performances, which have staggering
22
potential as electrode materials in supercapacitors and Li-ion their performance in an interdisciplinary science. Hence, more
batteries. ZnO is generally perceived as an active material for examinations are as yet expected to investigate the tuneable
batteries with prevalent energy density of 650 A h g−1. Fur- properties of ZnO-based materials in the field of energy,
thermore, ZnO has great electrical conductivity (up to environment and biology.
230 S cm−1), which is higher than that of other oxide mate-
rials. In DSSCs, the dye-sensitized nanocrystalline semi-
conductor photoanodes play an important role in the Acknowledgments
conversion of solar energy into electrical energy. The TiO2
nanoparticles are most frequently used as photoanode mate- Dr J Theerthagiri is grateful to the authorities of Sathyabama
rials in DSSCs so far. However, the TiO2 nanoparticles suffer Institute of Science and Technology (deemed to be Uni-
from the high recombination and low electron transport versity), Chennai, for their support. Prof. Hyun-Seok Kim
properties. These properties TiO2 have been focused on by would also like to thank for the support from the Ministry
researchers to develop an alternative semiconductor ZnO of Trade, Industry and Energy (MOTIE, Korea) under the
material as the photoanode for DSSCs. Sensor Industrial Technology Innovation Programme (No.
ZnO-based materials can likewise be the potential pho- 10063682).
tocatalysts for the degradation of dye molecules under visible
light illumination. The structural morphology, crystal orien-
tation, particle size and oxygen defects are few factors that ORCID iDs
influence the photodegradation activities and long-term sta-
bility of the catalysts. The photocatalytic performance of ZnO J Theerthagiri https://orcid.org/0000-0002-5746-5541
could be improved by various strategies, such as the synthesis P Nithyadharseni https://orcid.org/0000-0001-8960-6735
of ZnO nanostructured arrays, combination with other com- A Madankumar https://orcid.org/0000-0003-0567-7857
ponents including noble metals, doping and inclusion of Prabhakarn Arunachalam https://orcid.org/0000-0002-
carbon materials. 6293-1631
ZnO-based nanostructured materials are shown to be a
suitable candidate for binding biological substances. Recent
research reveals that the inspiration behind the use of
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A Review On Zno Nanostructured Materials: Energy, Environmental and Biological Applications

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Nanotechnology

A review on ZnO nanostructured materials: energy, environmental and

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This content was downloaded from IP address 154.59.124.171 on 19/07/2019 at 07:42

Nanotechnology 30 (2019) 392001 (27pp) https://doi.org/10.1088/1361-6528/ab268a

A review on ZnO nanostructured materials:

E-mail: [email protected] and [email protected]

Received 27 November 2018, revised 26 April 2019

0957-4484/19/392001+27$33.00 1 © 2019 IOP Publishing Ltd Printed in the UK

Keywords: battery, biosensor, biomedical applications, dye-sensitized solar cells, photocatalysis,

1. Introduction namely precipitation, the wetchemical technique, the sol-gel

Table 1. Comparison of electrochemical performances of ZnO-based electrodes in the literature.

Capacitance Scan rate (mV s−1)/current density Potential win-

Initial capacity Cyclic Current density

Initial capacity Cyclic Current density

Initial capacity Cyclic Current density

In recent years, effort has been made for developing highly

under visible light irradiation. It achieved degradation

In recent years, ZnO-based nanostructured materials were

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