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Photocatalytic Degradation of Methyl Violet and Auramine-O Dyes Using

Ni/ZnO Nanocomposites for An Environmental Solution for Dye Wastewater

Article · July 2024

DOI: 10.25163/biosensors.319940

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BIOSENSORS AND NANOTHERANOSTICS RESEARCH

Photocatalytic Degradation of Methyl Violet and

Auramine-O Dyes Using Ni/ZnO Nanocomposites
for An Environmental Solution for Dye Wastewater
Ajmal Shah1, Adnan2, Talha Sharif1, Muhammad Majid Khan1, Zain ul Abidin2, Muhammad Sohail2, Farah Muhammad
Zada2, Naseer Khan3, Fawad Ali4*, Saba Zafar5*

Abstract increasing catalyst dosage enhanced degradation by

Background: The increasing release of synthetic dyes, such providing more active sites, while degradation efficiency
as methyl violet (MV2B) and auramine O (AO), into water decreased at higher dye concentrations due to
bodies from industrial effluents poses significant competition for these sites. Kinetic analysis demonstrated
environmental and health risks due to their toxicity and that MV2B degradation followed a pseudo-second-order
persistence. Conventional wastewater treatment model, whereas AO conformed to a pseudo-first-order
methods often fail to fully eliminate these dyes, leading to kinetic model. Conclusion: The Ni/ZnO photocatalyst
a demand for advanced techniques like photocatalysis. proved highly effective in degrading MV2B and AO dyes,
This study examines the efficacy of Ni-doped ZnO with pH optimization further improving performance. This
(Ni/ZnO) photocatalysts for the photodegradation of research supports Ni/ZnO photocatalysis as a promising
MV2B and AO dyes under UV irradiation. Methods: approach for treating dye-contaminated wastewater,
Ni/ZnO catalysts were synthesized via wet impregnation, contributing to sustainable environmental remediation
followed by calcination and characterization through efforts.
SEM, EDX, and XRD to confirm morphology, elemental Keywords: Dye pollution, photocatalysis, Ni/ZnO, methyl violet,
composition, and structural changes. Photodegradation Auramine-O
experiments were conducted with various dye
concentrations, catalyst dosages, and irradiation times Introduction
under controlled pH. The removal efficiency was assessed The widespread use of synthetic dyes in various industrial
by measuring absorption changes pre- and post- applications, including cosmetics, food processing,
degradation. Results: The optimized conditions showed pharmaceuticals, paper and pulp production, textiles, leather
significant degradation efficiencies of 86.36% and 69.31% treatment, and printing, has led to significant environmental and
for MV2B and AO, respectively. The study revealed that health concerns (Qamar et al., 2021; Mosleh et al., 2016; Shojaei et
al., 2021). Despite their diverse applications, an estimated 10-15%
Significance | This study demonstrated Ni/ZnO photocatalysts as of synthetic dyes produced annually are lost to wastewater during
efficient, sustainable agents for degrading toxic dyes in wastewater, the manufacturing process of colored goods (Bouasla, Samar, &
minimizing environmental impacts.
Author Affiliation.
1
Department of Chemistry, Abdul Wali Khan University, Mardan, Khyber
Pakhtunkhwa, Pakistan.
2
Institute of Chemical Sciences, University of Swat, Swat, Khyber Pakhtunkhwa,
*Correspondence. Fawad Ali, Institute of Biotechnology and Pakistan.
3
Microbiology, Bacha Khan University Charsadda, Nutrition Division Institute of Health Islamabad, Pakistan.
4
Pakistan. E-mail: [email protected] Institute of Biotechnology and Microbiology, Bacha Khan University Charsadda,
Pakistan.
Saba Zafar,Changchun University of Science 5
Changchun University of Science and technology Changchun, R.P. China.
and technology Changchun, R.P. China.
E-mail: [email protected] Please Cite This:
Adnan, Ajmal Shah, Talha Sharif, Muhammad Mjid Khan, Zain ul Abidin, Muhammad Sohail,
Farah Muhammad Zada, Naseer Khan, Fawad Ali, Saba Zafar (2024). "Photocatalytic
Degradation of Methyl Violet and Auramine-O Dyes Using Ni/ZnO Nanocomposites for An
Environmental Solution for Dye Wastewater", Biosensors and Nanotheranostics, 3(1),1-
8,9940.
Editor Muhit Rana, Ph.D., And accepted by the Editorial Board July 18,
2024 (received for review July 18, 2024)
3064-7789 /© 2024 BIOSENSORS AND NANOTHERANOSTICS, a publication of Eman Research, USA.
This is an open access article under the CC BY-NC-ND license.
(http.//creativecommons.org/licenses/by-nc-nd/4.0/).
(https./publishing.emanresearch.org).

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BIOSENSORS AND NANOTHERANOSTICS RESEARCH
Ismail, 2010). This dye-laden wastewater presents a major challenge Given the substantial environmental and health risks posed by dyes,
to environmental safety due to the toxic and often persistent nature it is crucial to treat dye-contaminated industrial effluents before
of many synthetic dyes. discharge. Conventional dye removal methods, such as physical
Currently, over 100,000 different commercial dyes are with an adsorption, chemical coagulation, and biological treatments, often
annual global production exceeding 700,000 tons (Adegoke & Bello, fall short due to the complex chemical structures and stability of
2015; Zada et al., 2022). The demand for dyes in textile, cosmetic, many dyes (Qi et al., 2020; Kashif et al., 2024). Advanced
and paper industries has escalated, leading to increased quantities techniques, including photocatalytic degradation, electrochemical
of wastewater generated, particularly in countries like Pakistan methods, and ozonation, have emerged as promising approaches.
where textile production is a key economic activity (Shah et al., For instance, photo-degradation processes using catalysts such as
2018). Polluted wastewater from these industries is frequently titanium dioxide (TiO2) and zinc oxide (ZnO) have gained traction
discharged into freshwater bodies, introducing a range of due to their ability to decompose dyes under UV light, ultimately
hazardous organic pollutants, including dyes and other mineralizing these pollutants into non-toxic by-products (Zada et
contaminants, which contribute to environmental degradation al., 2022; Zaman et al., 2024). Such methods leverage catalysts’
(Arunagiri, 2021; Humayun et al., 2016; Senthil Kumar & surface properties—density, porosity, and surface area—to enhance
Arunagiri, 2021). This dye pollution has profound effects on aquatic radical generation and achieve effective dye degradation.
ecosystems and also poses risks to terrestrial life, including humans, Our research group has explored various catalysts for dye
plants, and animals, through bioaccumulation and degradation, focusing on enhancing efficiency through
biomagnification. modifications such as co-doping and nanostructuring. Recent
Different classes of dyes have varying toxicological profiles catalysts investigated include Pd/HAP/Fe3O4, (Al, Ni)-co-doped
depending on their chemical structures, stability, and persistence in ZnO, and Cu-ZnO photocatalysts. These materials were
the environment. Many dyes are particularly resilient to characterized through SEM, EDX, XRD, FTIR, XPS, and UV-vis
degradation, thus prolonging their environmental impact (Nazir et spectroscopic techniques, providing insights into their structural
al., 2020; Naz et al., 2021). Exposure to toxic dyes can lead to and functional properties (Safavi & Momeni, 2012; Reddy et al.,
numerous health issues, such as respiratory problems, liver and 2020). Specifically, TiO2 and UV light were successfully used for the
kidney damage, skin irritation, and even cancer (Naz et al., 2021). degradation of methyl violet, and Ni-TiO2/ACFs composite
For instance, methyl violet 2B (MV2B), a commonly used aromatic catalysts exhibited enhanced activity under microwave induction
azo dye with the chemical formula C24H28ClN3, is widely utilized for the degradation of methyl violet in water (Sun et al., 2020).
in textile and printing industries (Guzmán-Vargas et al., 2016). Additionally, Cu-Fe layered double hydroxides (LDH) have shown
While MV2B is soluble in water, it is known to cause eye and promise in sulfate radical-mediated degradation of dyes (Ma et al.,
respiratory irritation and has a reported LC-50 level of 0.047 mg/L 2018).
for the freshwater fish Pimephales promelas, indicating significant This study investigated the use of Ni/ZnO photocatalysts,
toxicity at low concentrations (Sinha et al., 2014). Human exposure leveraging their unique properties for the photodegradation of dyes
to MV2B has been linked to adverse health effects on the kidneys, under near-UV or solar light. ZnO is favored in environmental
liver, brain, and central nervous system, and it has also been shown applications due to its high UV absorption, affordability, non-
to impede bacterial growth and the photosynthesis of aquatic plants toxicity, and photostability (SivaKarthik et al., 2017; Zhang et al.,
(Humayun et al., 2016; Xu et al., 2019). 2012). Furthermore, the presence of Ni enhances ZnO’s
Auramine O (AO) is another highly toxic dye, characterized as a desulfurization performance, particularly with smaller particle
water-soluble cationic fluorescent dye. Its yellow hue makes it sizes, resulting in improved dye adsorption and degradation
popular in the paper, textile, and dyeing industries, as well as in the capabilities (Zhang et al., 2012; Xu et al., 2016). ZnO nanoparticles
treatment of leather and fisheries (Zhang et al., 1997; Zhu et al., hold significant potential for applications in transparent conductive
2015). AO is particularly hazardous due to its stability and coatings, photoanodes in dye-sensitized solar cells, and
persistence in the environment, leading to adverse effects on human environmental pollutant degradation. While Ni-doped ZnO
health, including respiratory and nervous system damage, and samples have lower band gap energies, their photocatalytic
allergic reactions. AO exposure is associated with risks of performance is affected by defects introduced by Ni, warranting
carcinogenicity and allergic reactions and is thus banned as a further investigation to optimize activity and stability (Xu et al.,
hazardous dye for use in food and medicine (Hmani et al., 2012; Qi 2016).
et al., 2020). Furthermore, AO’s environmental persistence reduces The persistent environmental and health impacts of industrial dye
water transparency, thereby inhibiting photosynthesis and primary pollution necessitate effective and sustainable treatment solutions.
production in aquatic ecosystems (Ghaedi et al., 2015). Advances in photocatalysis and the development of novel materials
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BIOSENSORS AND NANOTHERANOSTICS RESEARCH
such as Ni/ZnO hold promise for the efficient degradation of dyes, The absorption of the dye was measure twice one before the
providing a pathway towards mitigating the ecological footprint of degradation and one after the degradation in order to calculate the
industrial effluents. percent removal with the help of the following formula.
𝐶𝐶𝑜𝑜 −𝐶𝐶𝑓𝑓
% 𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅 = × 100
𝐶𝐶𝑜𝑜
2.Materials and Methods Whereas, Co is the initial concentration before degradation and Cf
2.1. Reagent and chemicals is the final concentration after the degradation.
Methyl violet 2B (MV2B), zinc oxide (ZnO) and nickel nitrate
(NiNO3), disodium hydrogen phosphate (Na2HPO4), potassium 3. Result and discussion
iodide (KI) were purchased from Sigma–Aldrich, citric acid 3.1 Characterization
(C6H8O7), hydrogen peroxide (H₂O₂). All the chemicals were of 3.1.1 Scanning 1electron microscopy (SEM)
high purity and were used as such. Figure1(a) demonstrate the result of SEM image of ZnO base. It is
2.2. Preparation of Ni/ZnO catalyst evident from the image that undoped ZnO possess a distinct
The catalyst was prepared by modified wet incipient impregnation spherical and round shaped morphology with an average size of 229
method. About 10 g of ZnO catalyst was added to considerable to 989 nm. From the SEM image of Figure 1(a) it can be seen that
amount of distilled water in a beaker, this was named solution A. the undoped ZnO having spherical nano particle without
About 5% NiNO3 solution wasprepared in another beaker, which appearance of microsphere. Figure 1(b) show the SEM image of Ni-
was termed as solution B. Solution A was poured into solution B dopped ZnO, which show alternation in the modified sample. It is
and mixed well. After mixing the mixture of NiNO3 solution and clearly seen that the morphology of ZnO got alter after Doping with
ZnO slurry was kept at room temperature until the dryness of the Ni/ZnO. The SEM image of Figure 1 (b) illustrate relatively
sample. Then the material was kept in an oven for 1 hour at 120 ºC. brighter and smaller particle as compared to that of ZnO. As can be
The sample was finally calcined in a muffle furnace for 4 hrs at 500 seen the particles are aggregated and its sizes are decreases to 88 –
ºC and then grinded to a final product of fine powder. 354 nm having high porous surface.
2.3 Characterization 3.1.2 EDX analysis of Ni/ZnO
The surface area of the Ni/ZnO catalyst was calculated using N2 The catalysts elemental composition for both ZnO and Ni/ZnO was
adsorption/desorption at 77.4 K using a Surface Area Analyzer studied using EDX. The spectrum of elements for ZnO is show in
NOVA2200e Quanta chrome, USA. A 30 KV Japan scanning Figure 2 (a), while for Ni/ZnO catalyst it is shown in Figure 2(b).
electron microscope was utilized to examine the structural The EDX spectra shows that nickel is successfully impregnated on
morphology of the manufactured Ni/ZnO catalysts. An Oxford Inca ZnO as shown by the Figure 2(b). from Table 1 it is demonstrated
EDX, Inca200, was utilized in conjunction with SEM to establish the that Zn (35.6%) is the most basic and fundamental element while
chemical composition of the produced Ni/ZnO catalyst. Using a Ni (28.9%), Na (27.8%) and C (21.1%) are the major constituents
JDX3532 JEOL, Japan diffractometer at 40 kV and 30 mA in the 2. whereas O (6.2 %) and S (0.30%) are the trace elements on material
XRD investigation was performed on a monochromatic Cu-K surface.
radiation (=1. 5418) at 40 kV and 30 mA in the 2 range of 10-800 3.1.3 XRD of Ni/ZnO
with 1.030 per minute using a JDX-3532 JEOL, Japan The XRD diffraction patterns of both supports and doped catalysts
diffractometer. were taken. In Figure 2 the chart for both XRD patterns are shown.
2.4 Application of catalyst for degradation of MY2B and The diffraction patterns of XRD present all the major peaks for ZnO
Auramine-O in Figure2(a) while for Ni/ZnO it shown in Figure 2(b). The Figure
For the photo catalytic degradation of MV2B and AO, 50 ppm of 2(a) present different phases with ICDD numbers 11136, 30888,
working solution was used. For each experiment about 10 mL of the 361451 and 11244 shows peak at 28°,31°,32°, 34°, 36°, 47°,50°, 56°,
dye solution was taken in a micro reactor and were kept under the 62°, 66°, 67° and 69° and the Figure 2(b) for Ni/ZnO and shows
UV lamp at fixed distance and intensity in the presence of pattern according to ICCD number 30888, 30891, 50664, 211486,
appropriate amounts of Ni/ZnO catalyst, buffer solution of desired 471019 and 11025.
pH and H₂O₂ with their varying concentration and/or weight
and/or volume. The degradation reactions were carried out using 4. Optimization of different parameters
different time interval. After the degradation reaction, the solution 4.1 Effect of weight of catalyst
was centrifugal at 3000 rpm for 10 min. MV2B and AO degraded It is anticipated that at high concentrations, Ni/ZnO, acting as a
dye solution was analyzed using single beam visible solid support, will accumulate a significant amount of methyl violet
spectrophotometer at 586 nm 460 nm respectively against the 2B (MV2B) and auramine O (AO) molecules. In this study, the
absorption was recorded. degradation of MV2B and AO under UV light was assessed using
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BIOSENSORS AND NANOTHERANOSTICS RESEARCH

Figure 1. SEM images of (a) ZnO and Ni/ZnO

Figure 2. EDX analysis of (a) ZnO (b) Ni/ZnO

Figure 3. XRD graph of (a) ZnO and (b) Ni/ZnO

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BIOSENSORS AND NANOTHERANOSTICS RESEARCH

Figure 4. (a) Effect of catalyst dose (b) Effect of initial dye concentration (c) Effect of time (d) Effect of pH on the degradation of MV2B
using 50 ppm dye concentration and, and irradiation time 120 min.

Figure 5. (a) Pseudo first order kinetic model for AO (b) Pseudo second order kinetics model for MV2B with the effect of catalyst
weight and time for photocatalytic degradation of AO using Ni/ZnO Photocatalyst.

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BIOSENSORS AND NANOTHERANOSTICS RESEARCH
Table 1. EDX composition of ZnO and Ni/ZnO
Element Atomic %

Zn 35.6
Ni 28.9
Na 27.8
C 21.1
O 06.2
S 0.30

Table 2. Effect of catalyst Dose on degradation of MV2B and OA

% Removal
Catalyst Dose (g/L)
MV2B AO
0.3 31.62 50.12
0.5 54.92 61.21
1.0 72.39 64.70
1.5 76.38 65.33
2.0 81.15 67.69
2.5 83.98 69.31
3.0 86.36 66.61

Table 3. Effect of initial dye concentration on degradation of MV2B and AO

%Removal
Dye Concentration
MV2B AO
10 80.21 64.72
20 82.39 65.36
30 84.59 66.03
40 86.23 67.00
50 86.36 69.31
60 87.32 72.01
70 87.22 67.88

Table 4. Effect of Irradiation time on degradation of MV2B and AO

MV2B %Removal AO %Removal
Time (min)

30 87.32 72.01
60 89.03 71.01
90 92.79 77.43
120 96.37 80.33
150 96.37 80.33

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BIOSENSORS AND NANOTHERANOSTICS RESEARCH
Table 5. Effect of pH on degradation of MV2B and AO
%Removal
pH
MV2B AO
2 80.42 80.33
4 86.70 86.37
6 96.37 99.00
8 97.21 95.70
10 96.95 93.92

Table 6. Kinetics data for decomposition of Ao and MV2B used Ni/ZnOphotocatalyst

Kinetic model Parameters Values
qe (exp) 990000
Pseudo first order (AO) K1 (min ) -1
0.1529
qe calc (mg g ) -1
900326.4311
R2 0.9499
C 5.9544
Pseudo second order (MV2B) K2 (min ) -1
6
qe calc (mg g ) -1
1000000
qe calc (mg g )
2 -1
1E+12
R2 0.9994
C 0.000006

Figure 6. (a) Shows the MV2B degradation Product and (b)AO degradation product

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 BIOSENSORS AND NANOTHERANOSTICS RESEARCH
various concentrations of the catalyst (0.3, 0.5, 1.0, 1.5, 2.0, 2.5, 3.0 The optimum time for degradation was 60 min. Where qe and qt are
g/L), an initial dye concentration of 50 ppm, and a pH of 6 for a 30- the amounts of MV2B and AO degraded photo catalytically (mg/g)
minute irradiation period. The degradation efficiency for each at equilibrium and at time t (min). K1 is the rate constant of pseudo-
catalyst concentration is presented in Table 2, with maximum first order process (min-1). Linear plot between t (time in min) and
efficiencies for MV2B and AO at 86.36% and 69.31% observed at 3 log (qe-qt) was used to determine rate constant, qe and qt Figure
g/L and 2.5 g/L, respectively, as shown in Fig. 3(a). The increase in 4(a). Where the equilibrium degradation (qe) and the second order
degradation efficiency with high doses of Ni/ZnO may result from constant K2 (min-1) which linear plot between t/qt and time to
increased adsorption site availability and the driving force for target determine K2, qe and qt Figure 4(b) (c), (d), Figure 5. The result of
pollutant accumulation (Iqbal et al., 2019; Nautiyal et al., 2016). the plots investigated that the decomposition of AO follows pseudo
Additionally, a high dose of Ni/ZnO is expected to enhance the first order model of kinetics and the decomposition of MV2B follow
degradation rate of MV2B and AO due to increased •OH radical second order kinetics because of the closeness of theoretical and
formation (Iqbal et al., 2021). experimental values of qe shown in Table 6.
4.2 Effect of initial dye concentration 4.5 Effect of pH
The degradation efficiency of MV2B and AO was also evaluated The charge distribution on the surface of the target contaminants
across a range of initial dye concentrations (10-60 ppm) while and solid adsorbent materials is found to be impacted by changes in
keeping other parameters constant (3.0 g/L and 2.5 g/L catalyst for pH of aqueous solution (Sayed et al., 2018). For this reason,
MV2B and AO, 120-minute irradiation time, and pH 6 at room degradation efficiency of MV2B and AO were investigated by
temperature) (Table 3). The findings, shown in Figure 3(b), indicate Ni/ZnO by changing pH from 2-10, employing 0 = 50 ppm,
that degradation efficiency initially increased with dye [Ni/ZnO]0 = 3 and 2.5 g/L for MV2B and AO, for 120 min,
concentration up to 60 ppm, but further increases led to a decrease respectively, depicted in Figure 4(d). It was found that removal
due to competition for active sites (Table 4 ) (Nautiyal et al., 2016; efficiency increase with increase in pH from 2 to 8 and maximum
Iqbal et al., 2021). Higher pollutant concentrations enhance degradation were 97.21% and 99% at pH 8 and 6 for MV2B and AO,
accumulation and diffusion on the sorbent surface, thus increasing respectively, as shown in Table 5.
electrostatic and Coulombic attraction forces and thereby raising Mechanism of Methyl violet (MV2V) and Auramine-O (AO):
degradation efficiency (Iqbal et al., 2021; Nasrullah et al., 2018). The possible photocatalytic degradation of Methyl violet is given
4.3 Effect of time below: first the molecules of Methyl violet dye are adsorbed on the
The study also investigated the effect of varying UV irradiation surface of the photocatalyst. Which when exposed to UV light the
times on MV2B and AO degradation, employing 50 ppm dye excitation of electron occurs from valence band to the conduction
concentrations, 3.0 g/L and 2.5 g/L Ni/ZnO catalyst for MV2B and band leaving hole (h+) in the valence band. When electron and
AO, respectively, and pH 6, over a time range of 30-150 minutes holes at the surface of photocatalyst react with dissolved oxygen,
(Figure 4 (a), (b), (c)). The results showed an increase in adsorbed water molecules and the surfaces hydroxyl groups, so the
degradation efficiency up to 120 minutes, after which the rate photo hydroxyl (OH•) and superoxide (O2) radicals are generated.
plateaued as equilibrium was reached (Table 4). The initial phase The dye molecules would be degraded by these photo-generated
(30-120 min) was characterized by rapid degradation due to radicals, resulting in intermediates that completely break down into
enhanced interaction between active sites and dye molecules, while CO2 and H2O (MV2B). The same Mechanism is for Auramine-O as
the subsequent phase showed a constant rate due to saturation of mentioned above for the MV2B. In the mechanism of Auramine-O
active sites (Iqbal et al., 2021; Samal et al., 2019). there is also the production of (OH•) and superoxide (O2) radicals
4.4 Kinetics studies of MV2B and AO occurs which are responsible for the degradation of dye.
The speed of the % photodegradation process and how this speed
impacts the equilibrium time are defined using kinetic models. Two 5. Conclusion
kinetic models were investigated: pseudo first order was fitted for The photo degradation experiments were Performed using 257.3
AO Eq. 1 and pseudo-second order was fitted for MV2B Eq. 2. nm UV irradiation. The effects of different parameters such as
log 𝑞𝑞𝑒𝑒 −𝑘𝑘1 𝑡𝑡
log(𝑞𝑞𝑒𝑒 − 𝑞𝑞𝑡𝑡 ) = (1) catalyst weight, Irradiation time, pH have been observed. MV2B
2.303
degradation without any catalyst was found to be 38.33 percent at
𝑡𝑡 1 1
= 𝑡𝑡 + (2) 120 min reaction time, while the photo catalyst showed a
𝑞𝑞𝑡𝑡 𝑞𝑞𝑒𝑒 𝑘𝑘2 .𝑞𝑞𝑒𝑒2
Substantial improvement in MV2B degradation and a maximum of
Whereas qe is the removal capacity at equilibrium time (optimum 92.83 percent with 120 min irradiation time and 300 mg catalyst
time), qt is the removal capacity at any time. weight was achieved. The initial pH of the solution was also
degraded and the limit was 97.21 percent at pH 8 and the irradiation
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BIOSENSORS AND NANOTHERANOSTICS RESEARCH
time was 120 min. The photo degradation experiments were Chandhru, M., Rani, S. K., & Vasimalai, N. J. (2020). Reductive degradation of toxic six dyes
Performed using 257.3 nm UV irradiation. The effects of different in industrial wastewater using diaminobenzoic acid capped silver nanoparticles.
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Hosseinpour, S. A., et al. (2018). Use of metal composite MOF‐5‐Ag₂O‐NPs as an adsorbent

Author contributions for the removal of Auramine O dye under ultrasound energy conditions. 32(2),
All authors made equal contributions to the study design, statistical e4007.
analysis, and drafting of the manuscript. The corresponding author, Humayun, M., et al. (2016). Enhanced visible-light activities of porous BiFeO₃ by coupling with
along with the co-authors, reviewed and approved the final version nanocrystalline TiO₂ and mechanism. 180, 219-226.
of the article prior to submission to this journal. Iqbal, J., et al. (2019). Synergistic effects of activated carbon and nano-zerovalent copper on

the performance of hydroxyapatite-alginate beads for the removal of As³⁺ from

Acknowledgment aqueous solution. Journal of Hazardous Materials, 235, 875-886.

The authors were grateful to their department. Iqbal, J., et al. (2021). Exploring the potential of nano-zerovalent copper modified biochar for

the removal of ciprofloxacin from water. Science of the Total Environment, 16,

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