High-yield synthesis of pure ZnO nanoparticles by one-step solid-state reaction approach for enhanced photocatalytic activity

Article abstract of DOI:10.1002/jccs.201900307

Zinc oxide (ZnO) nanostructures were synthesized via a one-step solid-state reaction approach in ammonia (NH₃) gas environment with different temperature ramp rates. The so-formed nanostructures were characterized using X-ray diffraction (XRD) for phase identification, where the typical wurtzite hexagonal structure was observed. Scanning electron microscopy (SEM) confirmed the particle size to be in the range 45–50 nm, the same as calculated by the XRD pattern for the ramp rate of 10 °C/min. Energy dispersive X-ray (EDX) spectroscopy and X-ray photoelectron spectroscopy (XPS) confirmed the chemical purity of the samples. The photoluminescence (PL) spectrum indicated multiple near-band-edge emissions and energy-band emissions. Then, these ZnO nanomaterials were used for the degradation of crystal violet (CV) dye under UV light irradiation. The CV solution was completely degraded in 2 hr. The initial photocatalyst and dye amounts of 0.2 g/100 ml and 0.5 mg/L, respectively, were found to be the optimum values for maximum degradation efficiency. The ZnO-based photocatalyst was stable up to three cycles of reuse. These results indicate that the high surface area and porosity of the nanomaterials are responsible for the high efficiency, which was confirmed by specific surface area analysis.

Full text of DOI:10.1002/jccs.201900307

Received: 28 July 2019
Revised: 31 October 2019
Accepted: 22 December 2019
DOI: 10.1002/jccs.201900307
A R T I C L E
High-yield synthesis of pure ZnO nanoparticles by one-step
solid-state reaction approach for enhanced photocatalytic
activity
1
1
2
Naveed Akhtar Shad | Muhammad Munir Sajid | Yasir Javed
|
1
3
2
2
Nasir Amin | Muhammad Ikram | Kanwal Akhtar | Gulzar Ahmad
|
2
4
Faisal Ali | Aamir Razaq
1
Department of Physics, Government
Abstract
College University Faisalabad (GCUF),
Faisalabad, Pakistan
Zinc oxide (ZnO) nanostructures were synthesized via a one-step solid-state reac-
2
Department of Physics, University of
tion approach in ammonia (NH ) gas environment with different temperature
3
Agriculture, Faisalabad, Pakistan
ramp rates. The so-formed nanostructures were characterized using X-ray diffrac-
tion (XRD) for phase identification, where the typical wurtzite hexagonal struc-
ture was observed. Scanning electron microscopy (SEM) confirmed the particle
size to be in the range 45–50 nm, the same as calculated by the XRD pattern for
3
Nanobiotech Group, National Institute
for Biotechnology and Genetic
Engineering (NIBGE), Faisalabad,
Pakistan
4
Department of Physics, COMSATS
ꢀ
the ramp rate of 10 C/min. Energy dispersive X-ray (EDX) spectroscopy and X-
Institute of Information Technology,
Lahore, Pakistan
ray photoelectron spectroscopy (XPS) confirmed the chemical purity of the sam-
ples. The photoluminescence (PL) spectrum indicated multiple near-band-edge
emissions and energy-band emissions. Then, these ZnO nanomaterials were used
for the degradation of crystal violet (CV) dye under UV light irradiation. The CV
solution was completely degraded in 2 hr. The initial photocatalyst and dye
amounts of 0.2 g/100 ml and 0.5 mg/L, respectively, were found to be the opti-
mum values for maximum degradation efficiency. The ZnO-based photocatalyst
was stable up to three cycles of reuse. These results indicate that the high surface
area and porosity of the nanomaterials are responsible for the high efficiency,
which was confirmed by specific surface area analysis.
Correspondence
Yasir Javed, Department of Physics,
University of Agriculture Faisalabad,
38000, Faisalabad, Pakistan.
Email: myasi60@hotmail.com
K E Y W O R D S
ammonium carbonate, CVD, photocatalytic activity, solid-state reaction approach, Zn powder
1
| INTRODUCTION
effluent can cause serious problems for both aquatic life
[
3]
and human health.
These concerns have urged
Large amounts of dyes are generated and used in differ-
ent industries such as textiles, pharmaceuticals, cos-
metics, and nutrition. Almost 15% of the total dyes used
in textile industry is lost during the dyeing process.
The presence of even trace amount of these dyes in the
researchers in recent years to develop new techniques
and methods for the treatment of dyes in the wastewater
[
4,5]
from industries.
There are various methods employed
[
1,2]
for the removal of dyes such as adsorption, coagulation,
[6]
advanced oxidation, and membrane filtration. These
©
2020 The Chemical Society Located in Taipei & Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
J Chin Chem Soc. 2020;1–9.
http://www.jccs.wiley-vch.de
1

2
SHAD ET AL.
methods have certain advantages and disadvantages. In
recent times, degradation of dyes by using light-activated
a = 0.321 nm and c = 0.519 nm (Figure 1). The peaks
present at 2θ values 31.69 , 34.38 , 36.18 , 47.45 , 56.46 ,
ꢀ
ꢀ
ꢀ
ꢀ
ꢀ
[7–13]
ꢀ
ꢀ
ꢀ
ꢀ
ꢀ
ꢀ
catalysts has emerged as a useful method.
In this
62.76 , 66.21 , 67.50 , 68.92 , 72.47 , and 76.78 corre-
spond to the (100), (002), (101), (102), (110), (103), (200),
(112), (201), (004), and (202) planes, respectively, of the
wurtzite structure. While studying effect of the ramp rate,
a reduction in peak broadening was observed as the ramp
rate of heating was increased (Inset Figure 1). The effect
of ramp rate was studied quantitatively by calculating the
crystalline size using the Scherrer equation:
method, inorganic nanomaterial-based catalysts generate
hydroxyl radicals, which can break the complex dye
structure in the presence of ultraviolet or visible light.
The appropriate wavelength of light is very important, as
dye degradation using only the catalyst is not very effi-
[14]
cient.
There are different nanomaterials, such as metal
oxides, sulfides, tungstates, and vanadates, that have
been evaluated as potential photocatalysts for the treat-
[15]
ment of industrial wastewater.
kλ
d =
ð1Þ
Zinc oxide (ZnO) nanomaterials have attained consid-
erable attention in the last two decades owing to their
unique and multidisciplinary applications prospects such
βcosθ
where d is the mean particles size, k is the shape factor
taken as ~0.9, λ is the wavelength of X-rays used for the
analysis (λ = 0.154178 nm), β is the full width at half-
maximum, and θ is the Bragg angle, usually taken for
highest intensity peak in the spectrum.
[
16]
[17]
[18]
as sensors,
toelectron devices.
tronic, and structural applications in engineering and
catalysts,
functional devices
and pho-
[
19,20]
ZnO has specific thermal, elec-
[
21]
science.
conductor at room temperature.
is usually used for photocatalytic, photochemical,
ZnO is a wide direct-bandgap (3.37 eV) semi-
[22]
Nanostructured ZnO
It was observed that a small ramp rate resulted in
broad diffraction peaks, indicating a small crystalline
size, due to the more extensive annealing effect, because
the furnace took more time to reach the given tempera-
[
23–27]
[
28,29]
optoelectronic, and electrical applications.
Many methods are employed for the synthesis of ZnO
nanomaterials, such as combustion,
[
30,31]
ꢀ
thermal
ture, that is, 600 C, with a low ramp rate (5 hr). In the
[32]
[33]
[34]
ꢀ
decomposition,
sol–gel,
hydrothermal,
laser
beginning, when ramp rate was 2 C/min, the average
[
35]
[36]
[37]
ablation,
assisted,
electrochemical,
co-precipitation,
ultrasound,
anodization,
microwave-
crystalline size was 27 nm. This increased to 38 nm when
[
38]
[39]
[40]
ꢀ
two-step
the ramp rate was increased to 4 C/min and reached up
[41]
ꢀ
mechano-chemical thermal synthesis
retic deposition.
and electropho-
to 48 nm for 10 C/min (Figure 2). In general, the sharp-
[42]
Among these methods, chemical vapor
ness of the peaks reduced with smaller ramp rates, indi-
cating small crystal size.
deposition (CVD) works at atmospheric pressure and uti-
lizes few volatile precursors.
For further studies, the nanoparticles produced at the
ꢀ
In this paper, we report a one-step solid-state reaction
approach which was used to fabricate nano-sized ZnO
powder with high yield and purity at different ramp rates.
CVD was employed owing to its versatility, low cost, and
eco-friendliness. The as-prepared nanosized ZnO powder
was characterized using X-ray diffraction (XRD), scanning
electron microscopy (SEM), energy dispersive X-ray (EDX)
analysis, BET analysis, X-ray photoelectron spectroscopy
ramp rate of 10 C/min were utilized. Field-emission
(XPS), and photoluminescence (PL). And finally, the
photocatalytic response of the synthesized nanomaterials
was evaluated by degrading the model dye crystal violet
(CV), which is frequently used in the textile industry.
2
2
| RESULTS AND DISCUSSION
.1 | Characterization of synthesized
powder
FIGURE 1 XRD spectrum of ZnO nanostructures produced
by solid-state reaction method at the ramp rate of 10 C/min. Inset:
ꢀ
The XRD peaks matched well with the standard ZnO
pattern (JCPDS Card No. 036-1451) and showed hexago-
nal wurtzite structure having lattice parameters
Series of XRD spectra ZnO nanomaterials obtained at ramp rates
ꢀ
ꢀ
ꢀ
ꢀ
of (a) 2 C/min, (b) 4 C/min, (c) 6 C/min, (d) 8 C/min, and
ꢀ
(e) 10 C/min

SHAD ET AL.
3
scanning electron microscopy (FESEM) was used for
studying the topographical and dimensional features of
ZnO powder (Figure 3). SEM images were taken at differ-
ent magnifications, which showed the high yield in the
low-magnification image. As the magnification was
increased, clearer morphology of the nanoparticles was
observed, indicating two aspects: the particle size was
consistent with the calculated from XRD pattern
(
Figure 3d inset), and the appearance of the particles was
somewhat spherical. The chemical purity of the synthe-
sized nanomaterials was confirmed by EDX, where the
Zn and O peaks were observed (Figure 4). The Cu and C
peaks in the spectrum are due to the carbon-coated cop-
per grid used in the observations.
FIGURE 2 Graph between ramp rate and crystalline size,
indicating increase in size with ramp rate
XPS is a versatile technique for elemental and energy-
state analysis of the elements. The XPS spectrum con-
ꢀ
FIGURE 3 SEM images at different magnifications (a-d) of ZnO nanostructures synthesized at the ramp rate of 10 C/min. Inset: Size
distribution of the nanomaterials

4
SHAD ET AL.
FIGURE 4 Chemical analysis based on EDX spectrum,
showing purity of the sample
FIGURE 6 Photoluminescence spectrum of the synthesized
ZnO nanomaterials
excitation at 310 nm. There are emission bands at
3
62, 390, 451, and 466 nm. The emission band at 362 nm
[
45]
belongs to the energy bandgap of ZnO.
This value is
different from those reported (around 380 nm) and corre-
sponds to near-band-edge emission. The emission at
390 nm is defect-related and is unexpected from the usu-
ally observed green/yellow bands in ZnO-based
[
46]
nanomaterials.
This can be explained by different
mechanisms such as interband transitions, that is, from
the conduction band (CB) to the valence band (VB), and
photogenerated electron–hole recombination in Zn donor
level and holes in acceptor level. Considering our method
of preparation of ZnO nanomaterials, the emission at
3
90 nm can be attributed to electrons shifting from the
FIGURE 5 Detailed XPS spectra of the ZnO sample prepared
at the ramp rate of 10 C/min
[
47]
ꢀ
shallow donor levels of Zn to the top of VB.
blue emissions observed at 451 and 466 nm represent
zinc interstitial and/or oxygen vacancies.
i
Weak PL
[
48]
firmed the presence of Zn and O elements (Figure 5).
High-resolution XPS spectra for the binding energy of Zn
2
1
p core level showed two fitting peaks at energy values
,021 and 1,043 eV, associated with chemical Zn species,
2.2 | Photocatalytic activity and reaction
mechanism
as higher binding energy states of Zn 2p3/2 and Zn 2p1/2
,
respectively, in Zn–O bonds. This indicates the presence
Because of their semiconducting nature and a direct
bandgap of 3.37 eV, ZnO nanomaterials have received a
lot of attention to break down organic pollutants, speci-
fied dyes, and volatile organic compounds utilizing light
of +2 oxidation state of Zn on the surface of the
[
43]
nanomaterials.
The O 1s peak present at binding
2
−
energy 530.5 eV was associated with the O ion in the
Zn–O bonding structure.
[44]
[1]
The C 1s peak in the XPS
irradiation. When ZnO is irradiated by a photon with
[8]
spectrum is usually observed because of the presence of
the synthesis solvent. This peak suggests considerable
adsorption of organic solvent molecules on the surface of
the nanoparticles.
The room-temperature PL spectrum of the synthe-
sized nanomaterials (Figure 6) was recorded with
an energy equal to or greater than the bandgap of ZnO,
electron–hole pairs are generated. Electrons are pro-
moted to the CB of the ZnO, where they reduce the oxy-
gen molecules to turn into hydroxyl radicals. The hole in
the VB generates hydroxyl radicals at the surface of ZnO
[
49–53]
nanospecies.
The UV–visible absorption spectrum

SHAD ET AL.
5
FIGURE 7 (a) Gradually diminishing absorption spectra of CV dye solution under UV light irradiation. (b) Variation of CV
concentration after absorption equilibrium
FIGURE 8 Schematic and proposed mechanism of the photocatalytic degradation of crystal violet by the ZnO photocatalyst
is shown in the Figure 7, where the absorption peak of
the CV dye around 580 nm weakens gradually and van-
ishes completely in 2 hr when irradiated with UV light.
The degradation efficiency is determined using the
absorption spectra with Equation (11) in Section 3.
followed by desorption of the products. Finally, the
polluting products are removed from the interface
region. When ZnO is irradiated with light with photon
energy (hv) equal to or greater than the excitation
energy (E ), electrons from the VB are stimulated to
g
The photocatalytic mechanism of the degradation
of CV dye solution by using ZnO as a catalyst under
UV light irradiation is shown in Figure 8. The photo-
catalytic oxidation steps can be described as follows:
first, organic pollutants diffuse from the liquid phase
to the surface of ZnO; then, adsorption of the organic
pollutants takes place on the surface of ZnO. In the
next step, oxidation and reduction reactions take place
the CB. This photoinduced process produces electron–
hole pairs (ehp), as shown in Equation (2). These pairs
can migrate to the ZnO's surface and get engaged in
redox reactions, as shown in Equations (3)–(5), where
+
H
reacts with water and hydroxide ions to produce
hydroxyl radicals while electrons react with oxygen to
produce superoxide radical anions and then hydrogen
•
peroxideEquations (6) and (7). The OH radical will

6
SHAD ET AL.
then react with superoxide radicals to form hydroxyl
radicals, Equations (8) and (9). Then, the resulting
hydroxyl radicals, being a powerful oxidizing agent,
will attack the pollutants adsorbed on the surface of
ZnO to yield intermediate compounds. These interme-
diates ultimately are converted to green compounds
such as CO , H O, and minerals, as shown in Equa-
2.3 | Effect of catalyst dose, dye
concentration, and recyclability
These experiments were scaled up by utilizing different
concentrations of ZnO, that is, 0.05, 0.2 and 0.3 g/100 ml,
for the photocatalytic degradation of CV solution. Photo-
catalytic degradation of CV increased with the increase of
ZnO concentration, achieving the optimum value for
0.2 g/100 ml and then decreasing for 0.3 g/100 ml. The
decline in the efficiency of degradation action at high
dose of ZnO may be due to the increase in opacity of the
solution, which increases light scattering, reduces the
photon infiltration depth, and consequently activates less
photocatalyst. Another important factor that can hamper
the degradation efficiency at higher catalyst dose is the
agglomeration of the nanoparticles, which reduces the
number of active surface sites required for the photo-
catalytic process. The dose of ZnO of 0.20 g/100 ml yields
the optimum efficiency of 92% (Figure 9a). The effect of
different dye concentrations showed that, as the dye con-
centration increased, the degradation efficiency
2
2
tion (10). Figure 9 illustrates the redox reaction taking
place during photocatalysis. Hence, the mechanism of
photodegradation of organic compounds in the pres-
ence of light irradiation via redox reaction over ZnO
[
23,27]
surface can be summarized as follows
:
ZnO + hv ! ZnO*ðe CB + h+ VBÞ
−
ð2Þ
ð3Þ
ð4Þ
ð5Þ
ð6Þ
ð7Þ
ð8Þ
ð9Þ
+
−
ZnOðh Þ + OH ! ZnO + OH•
−
2•
ZnOðe Þ + O ! ZnO + O −
2
O + 2H+ + e ! HO
−
•
2
2
•
decreased because of the limitation of OH radicals;
moreover, the photon interaction was restricted to first
layer because of the higher concentration of dye
•
•
HO2 + HO2 ! H2O2 + O2
ZnOðe−Þ + H O ! OH• + OH−
2
2
(
Figure 9b), which reduced the number of photons
and/or reduction in path length of photons according to
•
•
−
H2O2 + O2 ! OH + OH + O2
the Beer–Lambert law and consequently decreased the
[
54]
electrons excited from the VB to the CB.
Furthermore,
•
H O + hv ! 2OH
2
2
the stability and recyclability of the ZnO photocatalyst
were evaluated by reusing the photocatalyst in the CV
solution. ZnO maintained its activity even after three
repeated runs, as depicted in Figure 9c.
•
Organic pollutants + OH ! Intermediates + CO2 + H2O:
ð10Þ
FIGURE 9 (a) Effect of ZnO catalyst dose. (b) Dye concentration effect. (c) Recyclability of ZnO catalyst over CV dye solution

SHAD ET AL.
7
FIGURE 10 BET plot of ZnO nanoparticles
FIGURE 11 Schematic CVD diagram for the synthesis of
ꢀ
ZnO nanostructures at 600 C under NH
3
flow
2.4 | BET analysis for understanding
degradation kinetics
(
HT) furnace (Figure 11). After sealing, the tube portion
Photocatalytic performance is mainly connected to the
adsorption–desorption degradation mechanism. The
amount of pollutants adsorbed at the catalyst surface is a
measure of the photoinduced response. Braunner–
Emmett–Teller (BET) adsorption studies were carried out
for the determination of the specific surface area of ZnO
nanoparticles (Figure 10). The specific surface area of ZnO
of the furnace was evacuated using a rotary pump, and
ammonia gas was flushed through the furnace for 3 min.
Then ammonia flow rate was maintained at 150 sccm
(standard cubic centimeter per minute) and the tempera-
ture of the furnace was increased to the desired values at
different ramp rates. The temperature was maintained
for 2 hr. During the reaction, zinc powder plays the role
of a precursor and a substrate and is transferred to the Si
substrate owing to the ammonia gas flow and evapora-
tion of the salt (Figure 11). The produced vapors con-
dense and settle down on the Si substrate due to its lower
temperature than central zone temperature. The top-
down process, combining microfabrication method with
deposition on a horizontal substrate with the reduction
in dimensions to nanoscale, is followed by the reactants.
After completion of the reaction, the temperature of the
furnace was lowered naturally. A light brown product
was collected. The experiment was also performed at the
2
was calculated as 101.4827 m /g. The adsorption isotherm
revealed an H -type loop with type-IV hysteresis curve,
3
asserting the mesoporous nature of the material and
ascribed to slender buildup in the channels of the meso-
pores. However, the less weighted isotherm demonstrates
the existence of micropores. The measured mean pore
diameter and pore volume were 8.3946 nm and
3
0
.034932 cm /g, respectively. The higher surface area points
to the presence of a multichannel structure within the fab-
ricated ZnO material, which facilitates fast mass transport,
scattering, absorption, and gas dispersion, resulting in
enhanced light harvesting inside the pores of the material
for the quick degradation of the dye. The existence of the
nanopores enables the material to trap more dye molecules
ꢀ
ramp rates of 2, 4, 6, and 8 C /min. The synthesized
material was gathered by a copper collector cooled by
water circulation. Hence, a temperature difference of
[55,56]
ꢀ
over the surface subjected to the degradation process.
20 C/cm was maintained between the Si substrate and
copper collector. Reaction was completed in 4 h. The col-
lector was covered with light brown powder, which was
scratched off and used for characterization.
3
3
| EXPERIMENTAL
.1 | Synthesis of nanostructures
3
.2 | Characterization
Zinc powder (1.5 g) of commercial grade (99.9%, Strem
Chemicals USA) was kept in an alumina tube and placed
at the center of a high-temperature, horizontal tube
A Philip Xpert X-ray diffractometer with Cu Kα radiation
(λ = 0.15406 nm) with 2θ range of 10–80 was used for
ꢀ

8
SHAD ET AL.
structural analysis and crystalline size estimation. Mor-
phological aspects were studied using FESEM (JEOL-
ramp rate. SEM images of the nanomaterial produced
with 10 C/min ramp rate showed good agreement of par-
ꢀ
7
500). A Nova nano EDX detector was used for chemical
ticle size with that calculated from the XRD pattern. EDX
and XPS showed that the nanomaterials were pure and
contained only zinc and oxygen. Multiple emission peaks
were observed in the PL spectrum, presenting near-band-
edge emissions and energy-band emission. The synthe-
sized nanomaterials were probed for their potential for
the photocatalytic degradation of CV dye. ZnO
nanomaterials showed good potential and stability for
the degradation of the organic dye under UV light
irradiation.
composition analysis. XPS data were recorded using an
X-ray spectrometer (8025 Best Tec), and carbon contami-
nant (C 1s = 284.6 eV) was used for all energy corrections
as internal standard. The PL spectra of the nanomaterials
were examined by using a Perklin Elmer LS 55 spectro-
photometer with 310 nm excitation wavelength at fixed
conditions. The surface area studies were made by using
a BET apparatus (ASAP-2020).
3.3 | Photocatalytic study
ORCID
Yasir Javed https://orcid.org/0000-0003-4161-3543
Photocatalytic degradation (by degrading CV dye under
UV irradiation) study was carried out to evaluate the
potential of the as-synthesized ZnO material. The optical
density and/or the gradual decrease in intensity or absor-
bance were measured using the Perkin Elmer λ 35 UV–
vis spectrophotometer, with a xenon lamp of 300 W as
the UV light source. Prior to initiation of the photo-
catalytic degradation experiment, a stock dye solution
with 0.1 g/L concentration was prepared. To begin the
experiment, 150 mg of the catalyst was ultrasonically dis-
persed in 150 ml of the CV dye solution. To acquire a
homogeneous solution, the dispersion was vigorously
stirred for 1 hr in dark. A nitrogen cooling system was
employed to avoid thermal effects that may expedite the
degradation of CV in solution. The solution was con-
stantly stirred throughout the experiment. After illumi-
nating the sample, 2 ml of the catalyst-containing dye
solution was periodically drawn every 20 min. The col-
lected sample was centrifuged for 5 min at 6,000 rpm to
isolate the catalyst. The supernatant was examined using
sptheectrophotometer to account for the residual dye
concentration in the 400–800 nm spectral range. The fol-
lowing relation was used to determine the degradation
efficiency:
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4
| CONCLUSIONS
ZnO nanoparticles were prepared using a one-step solid-
state reaction through CVD in an HT furnace with differ-
ent ramp rates. XRD analysis confirmed the wurtzite hex-
agonal structure, with the peak heights shrinking with
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How to cite this article: Shad NA, Sajid MM,
Javed Y, et al. High-yield synthesis of pure ZnO
nanoparticles by one-step solid-state reaction
approach for enhanced photocatalytic activity.
J Chin Chem Soc. 2020;1–9. https://doi.org/10.
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