Environmental Nanotechnology, Monitoring & Management 10 (2018) 331–338

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Environmental Nanotechnology, Monitoring

& Management
journal homepage: www.elsevier.com/locate/enmm

Piper betle leaves mediated synthesis of biogenic SnO2 nanoparticles for T

photocatalytic degradation of reactive yellow 186 dye under direct sunlight
Jagpreet Singha,1, Navneet Kaura,1, Pawanpreet Kaura, Sukhmeen Kaura, Jasneet Kaura,
⁎ ⁎
Preeti Kukkarb, Vishal Kumarc, Deepak Kukkara, , Mohit Rawata,
a
Department of Nanotechnology, Sri Guru Granth Sahib World University, Fatehgarh Sahib, 140406, Punjab, India
b
Department of Chemistry, Sri Guru Granth Sahib World University, Fatehgarh Sahib, 140406, Punjab, India
c
Department of Physics, Sri Guru Granth Sahib World University, Fatehgarh Sahib, 140406, Punjab, India

A R T I C LE I N FO A B S T R A C T

Keywords: Development of benign and efficient approaches towards abatement of industrial grade toxic organic dyes from
Green synthesis the fresh water resources is an evolving challenge. To this end, current study was focused on the removal of
Photocatalysis reactive yellow 186 dye (RY-186) dye using green synthesized SnO2 nanoparticles prepared from Piper betle leaf
Piper betle extract. As synthesized nanoparticles were characterized by pertinent spectroscopy and microscopy tools, which
Reactive yellow 186
ascertained the formation of highly crystalline, spherical, and ultrafine nanoparticles of 8.4 nm diameter with
SnO2
tetragonal rutile structure. Nanoparticle catalyzed photolysis of RY-186 dye in presence of sunlight revealed
degradation efficiency and apparent rate constant (K’app) values as 92.17% and 1.3 × 10−2 min−1, respectively.
Kinetic analysis of the dye degradation process rendered manifestation of pseudo-first order kinetics. Current
study demonstrated the application of biogenic SnO2 NPs as a heterogeneous catalyst towards the purification of
industrially polluted water for the savage of the environment.

1. Introduction
In the quest of achieving rapid economic growth, mankind has fo-
cused on unregulated anthropogenic activities such as urbanization,
malfunctioned agricultural practices, and industrialization. These devel-
opmental processes have substantially utilized aquatic resources as a sink
for the discharge of untreated effluent materials (Cassano et al., 2001;
Chowdhury et al., 2013). The polluted effluents released from the in-
dustries, domestic sewage, and agriculture run off hold many poisonous
materials including pesticides and unprocessed organic dyes (F, 2015;
Naidoo and Olaniran, 2013). These toxic effluents pose a significant
threat to the biotic as well as abiotic components of the ecosystem.
Among various industrial effluents, reactive are one of the most toxic by-
products of textile industry (Rhind, 2009). In the world wide survey re-
port (Gürseset al., 2016), it was observed that more than 10,000 distant
pigments and dyes are used in textiles industries. Also, 15% of the whole
world production of these synthetic and non-biodegradable dyes is re-
leased into natural water bodies, which is the primary reason of water
pollution (Lavanya, 2014). In terms of commercial usage, organic dyes
act as coloring agents on various substrates like clothes, leather, and re-
lated products. An extended conjugation system in the structure of these
dyes accounts for their recalcitrant nature (Holkaret al., 2016). Their
toxicity and resistant nature offers a great challenge for waste water
treatment plants and other remedial technologies. In addition, they are
also held responsible for increased biological and chemical oxygen de-
mand in the aqueous environment (Brillas and Martínez-Huitle, 2015).
Conventionally, effluent removal/remediation processes can be categor-
ized into three classes including physical, chemical, and biological
methods (Ahmad et al., 2015; Holkar et al., 2016). Physical methods
employ adsorbent, flocculation, precipitation, and coagulation processes
for removal of organic dyes (Ahmad et al., 2015). Many materials such as
activated carbon (Ahmad et al., 2014; Yagub et al., 2014), magnetic
nanoparticles (Asfaram et al., 2017; Babaei et al., 2017), and zeolites
(Khanday et al., 2017; Liu et al., 2014), have been extensively utilized for
adsorption based removal of organic dyes. Chemical approach relies on
disinfection agents such as chlorine, oxidation and reduction reactions,
flocculation, and froth floatation process for treatment of dyes. However,
there is accumulation of concentrated sludge which leads to a disposal
problem (Ahmad et al., 2015). On the other hand, biological methods
involve the use of microorganisms, where extracellular enzymes lead to
decolorization of the dyes (San Keskin et al., 2018). This method also
includes treatment with aerobic and anaerobic sludge blanket reactor in

⁎
Corresponding authors.
E-mail address: mohitnano.nit@gmail.com (M. Rawat).
1
These co-authors equally contributed as first authors.

https://doi.org/10.1016/j.enmm.2018.07.001
Received 4 April 2018; Received in revised form 28 June 2018; Accepted 5 July 2018
2215-1532/ © 2018 Elsevier B.V. All rights reserved.
J. Singh et al. Environmental Nanotechnology, Monitoring & Management 10 (2018) 331–338

which dye is adsorbed onto the surface of sludge biomass (Singh et al.,
2015). All the aforementioned methods barely transfer the pollutants
from one phase to another without complete elimination from the solu-
tion. In addition, treatment of organic dyes through any of the above
mentioned methods yield toxic 2° pollutants such as aromatic com-
pounds, for e.g., benzidine (Olivo-Alanis et al., 2018). These 2° pollutants
are highly mutagenic and may cause cancer and other life threatening
disorders. Moreover, these toxic effluents are responsible for many ha-
zardous health effects such as cancer, skin irritation, and allergic response
(Beydilli et al., 1998; Ventura-camargo and Marin-morales, 2013). Fur-
ther, biomagnification of these dyes in the water resources prevent the
traversing and capturing ofthe solar radiations by the aquatic autotrophs,
thereby limiting their dissolved oxygen content (Holkar et al., 2016). In
light of these life threatening disorders of toxic industrial effluents, it
become shighly essential to remove them from waste water before being Fig. 1. Chemical structure of RY-186 dye showing presence of π-conjugated
released into the fresh water resources (Singh and Chadha, 2016). In view ring systems with various functional groups.
of these health hazardous effects of organic dyes, there is an urgent need
to develop innovative solutions for their elimination from the waste water biogenic SnO2 NPs towards photocatalytic degradation of industrial dye
(Wong et al., 2015). Apart from the conventional methods, now a days RY-186 under solar radiations. The facile synthesis and photocatalytic
the use of advanced oxidation process (AOP) is of considerable interest removal of RY-186 dye under ambient conditions in this study provides
for the complete removal of dyes (E.Castro, A. Avellaneda, 2014). It in- new insight into the efficacy of biogenic SnO2 NPs as green photo-
cludes several processes such asozonation, photocatalysis, and photolysis catalyst for removal of organic pollutants from water.
with the aid of oxidants, light, and semiconductors. The process includes
the generation of highly reactive free radicals that can actively participate 2. Experimental
in effective elimination of organic pollutants from the waste water. These
free radicals rapidly react with electron-rich organic dyes leading to their 2.1. Materials
complete mineralization and decolorization by generating nontoxic
compounds such as CO2 andwater (Dewil et al., 2017; Zhang et al., 2015). P. betle leaves were collected from the nearby garden. SnCl2 (99%
In the recent years, metal oxide semiconductor (MOS) based photo cat- Pure) was purchased from Sigma-Aldrich, USA. RY-186 dye was pur-
alytic methods have gained considerable attention for the breakdown of chased from a textile industry in Ludhiana. Deionized (DI) water
organic dyes (Vidya et al., 2016; Gupta et al., 2017). Among various MOS (Siemens, Singapore) was used in all the solutions throughout the
types, nanoscale tin dioxide (SnO2) has emerged as a potent photocatalyst course of the study. All the other chemicals were of analytical grade and
owing to many exciting features such as size-tunable electronic properties were used without any purification.
(band gap = 3.6 eV), economic pricing, exceptional photocatalytic po-
tential, high electrical conductivity, benign chemical nature, and sub-
2.2. Methodology
stantial chemical and photochemical stability (Chen and Liu, 1999; Fukai
et al., 2007; Leite et al., 2000; Nayral et al., 1999; Yu et al., 2008; Zhu
2.2.1. Preparation of P. betle leaves extract
et al., 2000). SnO2 NPs are typically synthesized by various methods
The collected P. betle leaves were washed thoroughly with DI water to
including sol-gel synthesis (Aziz et al., 2013), precipitation (Nasir et al.,
remove the dust particles and dried under sunlight. 10 g of dried leaves
2017), electrochemical (Lavanya and Sekar, 2016), sonochemical (Zhu
were subsequently grinded to obtain fine powder and dissolved in 100 ml
et al., 2000), solid-state reaction (Li et al., 2002), and microwave irra-
DI water. The suspension was boiled for 4 h at 60 °C and cooled down to
diation approach (Krishnakumar et al., 2008). However, these ap-
room temperature (RT). Eventually, the solution was filtered by
proaches suffer from many limitations such as high production cost, so-
Whatman No. 1 filter paper to obtain brown colored leaf extract.
phisticated apparatus, and non-toxic by-products a. In light of these
challenges, it becomes eminent to develop facile, economically feasible,
and environmentally benign approaches for fabrication of SnO2 NPs. To 2.2.2. Preparation of SnO2 NPs
this end, biological resources such as plants are gaining much attention In typical process 3.5 g SnCl2 was solubilized in 40 ml DI water and
towards fabrication of the SnO2 NPs. Extracts obtained from plants serve was stirred for 15 min. Subsequently 20 ml of prepared P. betle leaf
the dual purpose of reducing and capping agents (Singh et al., 2017, extract was added to the SnCl2 solution, followed by heating at 60 °C for
2011). In a recent study, green synthesis of SnO2 NPs using Persia 4 h. Then resultant mixture was kept on hot plate until jelly was formed.
Americana seed extract and its application towards photodegradation of The jelly was finally calcinated at 400 °C for 4 h in muffle furnace to
phenolsulfonphthalein dye was reported by Elango et al. (2015). Taking obtain white powder of SnO2 NPs. The step wise procedure for synthesis
inspiration from this study, we investigated the synthesis of SnO2 NPs of SnO2 NPs is described in Fig. 2.
from Piper betle (P. betle) leaf extract under ambient conditions. This plant
belongs to the Piperaceae family and is well known for remediation of 2.2.3. Photocatalytic activity of SnO2 NPs
many hazardous health effects such as eye and skin disorders. It must be The photo catalytic potential of as prepared NPs was investigated by
noted that the phytoextract of P. betle consists of many chemical com- the decomposition of RY-186 dye under sunlight (630 W/m2 on pyr-
pounds such as monoterpenes, alcohols, esters, aldehydes and phenols, anometer) on a hot sunny day. In a typical experiment, 20 mg of dried
which account for their antifungal, antiseptic, anthelmintic, detoxifica- SnO2 NPs was added to 0.1 M aqueous solution (50 ml) of the dye. The
tion, antioxidation, and antihypertensive properties (Fig. 1) (Evans et al., suspension was allowed to stir in order to ensure adsorption/desorption
1984). Moreover, these phytochemicals also justify the reducing and equilibrium of the dye on the NPs’ surface. Subsequently the suspension
capping characteristics of the leaf extract. was placed under direct sunlight and 2 mL of samples were collected by
By considering the modern prerequisite of photocatalysts, we syn- every 20 min. The collected sample was centrifuged at 10,000 rpm for 10
thesized SnO2 NPs using the P. betle leaves and evaluated their potential min, and the supernatant was analyzed by a UV-visible spectro-
for photodegradation of RY-186 dye. To the best of our knowledge, this photometer. The degradation efficiency of RY-186 dye was determined
is the first study on P. betle mediated synthesis and application of by Lambert Beer's Law (Soltani et al., 2012) : R = {(C0-C)/

332
J. Singh et al.
Fig. 2. Stepwise procedure for the synthesis SnO2 NPs by P. betle leaves extract.
C0) × 100 = {(A0-A)/A0} × 100 where the variables A0 and C0denote
the initial absorbance and concentration of the dye (at time t = 0)re-
spectively. Similarly, A and C designate the absorbance and concentra-
tion of dye at time t= t. To assess the precision analysis and experi-
mental validation, the degradation experiment was performed by three
times at same time and similar experimental conditions. The relative
standard error (RSE) value of dye from triplicate experiments was found
to be 1.5 % as shown in Fig. 3.
2.3. Characterization techniques
Optical absorption spectra were recorded over Shimadzu UV 2600
Spectrophotometer fitted with double beam optical facility. Fourier
transform infra-red (FTIR) spectra were recorded on Bruker Alpha FTIR
spectrometer. The XPERT PRO, PAN analytical X-ray diffractometer
was used to obtain the powder X-ray diffraction (PXRD) pattern of the
NPs. The topography and morphology of NPs was observed on field
Fig. 3. Photocatalytic degradation efficiency of SnO2 based catalyst for RY-186
dye (error bars: relative standard error (RSE)).
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Environmental Nanotechnology, Monitoring & Management 10 (2018) 331–338
emission scanning electron microscope (JXA-8200, JEOL). The che-
mical composition of the sample was analyzed using energy dispersive
X-ray (EDX) spectroscopy (Oxford instruments (X-Max 51 –XMX0004)).
The fine structure and particle size distribution of the NPs were ana-
lyzed with the help of transmission electron microscope (TEM) using
Hitachi HF 3300 equipment. Solar flux was calculated by pyranometer
(LP02-LI19 pyranometer, Hukseflux) with operating temperature range
−40 to +80 °C and 15 × 10−6 V/(W/m2) sensitivity.
3. Result and discussion
3.1. Physicochemical characterization of the SnO2 NPs
3.1.1. PXRD observations
The PXRD patterns of calcinated SnO2 NPs were analysed by PXRD
spectrometer as described in Fig. 4, which shows numerous broad dif-
fraction peaks of the SnO2 NPs corresponding to (110), (101), (200),
Fig. 4. PXRD pattern of green synthesized SnO2 NPs. Presence of sharp peaks
designate crystalline nature of the NPs.
J. Singh et al.
Fig. 5. FTIR spectra of green synthesized SnO2 NPs showing characteristic
peaks at 3848 (OeH stretching), 3738 (OeH stretching), 1648 (amide C]O
stretching), 622 cm−1 (Sn-O bond stretching) and, 546 cm-1 (Sn-O bond
stretching), respectively.
(211), (220), (002), (310), (112), (301), (202) and (321) planes, with
their respective 2θ angles at 26.69°, 33.93°, 38.06°, 51.75°, 54.77°,
57.92°, 61.91°, 64.73°, 66.00°, 71.28° and 78.60° (ICDD No: 14-1445).
These peaks can be assigned to the tetragonal structure and in complete
agreement with the previously reported literature (Vidhu and Philip,
2015). The crystalline size (D) of SnO2 nanoparticles was calculated
using Scherrer's equation(Rehani et al., 2006; Singh et al., 2018):
Kλ
D=
βcosθ
Fig. 6. FESEM images (a and b) of the green synthesized agglomerated SnO2 NPs. Scale bar in ‘a’ and ‘b’ corresponds to 100 and 200 nm, respectively; (c) EDX spectra
of synthesized SnO2 NPs showing their elemental composition.
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Environmental Nanotechnology, Monitoring & Management 10 (2018) 331–338
where k is constant with value 0.9, λ is the wavelength of incident X-
ray beam, β is full width half maxima and θ is Bragg angle. The average
crystalline size of SnO2NPs as determined from the above mentioned
equation was calculated to be 12 nm.
3.1.2. FTIR studies
The FTIR spectrum of the NPs was recorded over the range of 4000-
500 cm−1 and presented in Fig. 5 The spectrum shows characteristic
peaks at 3848, 3738, 1648, 622 cm−1, and 546 cm−1, respectively. The
peaks observed at 541and 622 cm−1 are attributed to Sn−OH con-
jugation and Sn-O bond vibrations. (Elango et al., 2015). The bands at
1648 and 3738 cm−1 were due to the stretching of amide C]O bond
and of OeH absorbed at the surface of SnO2 respectively. All the peaks
were in accordance with the earlier reported literature and thus con-
firmed the chemical composition of the SnO2 NPs (Farrukh et al., 2010;
Tatsuda et al., 2009). Thus, this study indicates the strong capping SnO2
NPs by of phytochemicals present in P. betle leaf extract.
3.1.3. Morphological studies
The morphology of the SnO2 NPs was ascertained by FESEM ana-
lysis and presented in Fig. 6. The NPs exhibited spherical morphology
with small aggregates as shown in Fig. 6(a–b). Elemental composition
of the NPs was verified by EDX analysis and presented in Fig. 6c. The
sharp peaks of Sn (57.40%) and O (31.35%) were observed while ex-
istence of C (7.96%), N (1.63%), Si (0.41%) and Cl (1.25%) is also
indicated which can be assigned to the presence of other biomolecules
(Fig. 6c). The fine structure of the SnO2 NPs was determined by TEM
analysis and presented in Fig. 7As shown in the figure, the SnO2 NPs
were characterized by hollow spherical appearance and uniform size
distribution with an average size of 8.4 nm. Hence, the TEM observa-
tion was in accordance with the PXRD observations and confirmed the
synthesis of crystalline SnO2 NPs.
J. Singh et al.
Fig. 7. TEM image of green synthesized agglomerated SnO2 NPs. Scale bar corresponds to 20 nm.
3.2. Photocatalytic studies
The as-prepared SnO2 NPs were investigated for the degradation
application of RY-186 dye in the presence of sunlight. The RY-186 dye
is a major pollutant in the wastewater of textile industries due to its
recalcitrant nature. The aqueous dye solution shows a characteristic
absorption peak at 417 nm in UV–vis spectroscopy (Fig. 8). In the
presence of SnO2 NPs, the characteristic absorption of the dye showed
considerable decline as a function of irradiation time (Fig. 8). The in-
tensity of the dye absorption peak diminished completely over the
160 min of experimental duration, thereby indicating complete photo-
degradation in presence of SnO2 NPs.
3.2.1. Kinetics Study
The dye degradation kinetics follows the pseudo-firstorder rate law
ln(A/A0) = -kt, where k and A0 arethe rate constant and initial ab-
sorbance (at time t=0), respectively, while Ais the dye absorbance at
any time t during the course of the photocatalyticoxidation. The ap-
parent rate constant (K’app)for the degradation process was observed to
be 1.3 x 10-2min-1asshown in Fig. 9. TheSnO2catalyzed
Fig. 8. UV–vis spectra of photocatalytic degradation of RY-186 dye green
synthesized SnO2 NPs.
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Environmental Nanotechnology, Monitoring & Management 10 (2018) 331–338
photodegradation efficiency of RY-186 dye was determined as 92.17%,
which signified the potential of these NPs for environmental remedia-
tion applications
3.2.2. Mechanism of dye degradation
The photocatalytic degradation of dye in presence of SnO2 NPs oc-
curs as a consequence of light dependent free radical generation on
their surface. The light dependent excitation of SnO2 NPs renders the
generation of superoxide (O2−) ions and hydroxyl (OH.) radicals, which
react with the dye molecules to initiate their photo oxidation process.
The incidence of solar radiations on the surface of SnO2 NPs led to the
generation of electron-hole pairs as described in equation (Eq. (1)).
These photogenerated electrons in the conduction band interact with
molecular oxygen (O2) to produce superoxide radical anion (O2− %) (Eq.
(2)). Likewise, the photogenerated holes oxidize the water to produce
hydroxyl radicals OH (eq. 3). These O2− % and OH radicals are very
strong oxidants and account for photo oxidation of the dye molecules
(Elango et al., 2015). The possible mechanism of dye degradation is
illustrated in Fig. 10.
Sn O2 + hν → Sn O2 (e−) + Sn O2 (h+) (1)
SnO2 (e−) + O2 → O−2 · (2)
Fig. 9. Plot of ln(Ct/C0) versus irradiation time, t, for SnO2 catalyzed photo
degradation of RY-186 dye.
J. Singh et al.
Fig. 10. Schematic shows the mechanism of photocatalytic degradation of RY-186 under direct sunlight irradiation.
SnO2 (h+) + H2 O→ OH. (3)
O2−· or OH · + Dye (RY − 186) → deg raded product (4)
3.2.3. Effect of dark period on dye degradation profile of SnO2 NPs
In addition, control experiments in the dark were further carried to
verify the efficacy of the SnO2 NPs. However, negligible abatement in
the dye absorbance was observed in the dark period, which suggested
insignificant adsorption or degradation of the dye in the absence of
sunlight (Fig. 11). In contrast, under direct sunlight RY-186 were al-
most completely degraded over160 min of experimental duration.
These experiments evidently demonstrated that dye degradation was
driven by a photocatalytic process.
3.2.4. Selectivity studies
The selectivity of the SnO2 NPs was also determined by in-
vestigating the photocatalytic degradation of the RY-186 dye in
Fig. 11. Schematic showing the normalized concentration as a function of time
for RY-186 RR-120 and 19 RG-19, respectively under dark and sunlight reac-
tion. conditions.
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Environmental Nanotechnology, Monitoring & Management 10 (2018) 331–338
presence of two other textile grade dyes (including reactive red-120
(RR-120) and reactive green-19 (RG-19)). The cumulative percentage
degradation of the RR-120 and RG-19 under identical experimental
conditions was determined as 38.2% and 61.7%, respectively (Fig. 11),
which was lower in comparison to the RY-186 dye as discussed in
section 3.2.1. Our findings thus proved the selective potential of SnO2
NPs towards photocatalytic degradation of RY-186 dye over other dyes.
3.2.5. Stability and reusability of photocatalyst
For practical applications, reusability of the photocatalyst is a
factor of paramount importance. To this end, dye treated SnO2 NPs
were washed thrice times with water to remove the residual dye
molecules and/or degradation products from their surface. Finally, the
NPs were suspended in water and again investigated for photo-
catalytic degradation of RY-186 dye to check any variation in their
degradation potential. The percentage degradation of RY-186 dye over
five successive experiments was determined as 92.1%, 92%, 92%,
91.53, and 91.18%, respectively (Fig. 12). These observations
Fig. 12. Reusability of the SnO2 NPs photocatalyst in five successive runs.
J. Singh et al.
Fig. 13. PXRD pattern of SnO2 NPs after photocatalytic application. Depicting
the photostability of SnO2 NPs.
demonstrated negligible variation in the photocatalytic potential of
the SnO2 NPs. The minor depreciation in the photocatalytic activity of
NPs can probably be ascribed to the loss incurred during the cen-
trifugation process. Eventually, PXRD of the SnO2 NPs after five
rounds of photocatalytic degradation experiments was carried out to
measure any variation in the crystal structure of the SnO2 NPs. As
shown in Fig. 13, except minor decline in peak intensities, no variation
in the PXRD profile of the SnO2 NPs NPs was observed compared to
the naïve NPs. Hence the NPs exhibited substantial stability and reu-
sability for photocatalytic degradation of RY-186 dye. In light of our
comprehensive and methodical experimental data, it is evidently
proved that the SnO2 NPs are an effective photocatalyst for degrada-
tion of RY-186 dye.
3.2.6. Zero point charge pH study of SnO2 NPs
The zero charge point pH was investigated by determining the
zeta potential at various pH values of the SnO2 NPs’ suspension. As
shown in Fig. 14, the zero zeta potential value of the NPs was found
to be at pH 6.5. Thus, it is suggested that the acidic pH causes sub-
stantial aggregation of the NPs, which results in zero charge point
pH.
Fig. 14. Schematic shows zeta potential values of SnO2 NPs at different pH.
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Environmental Nanotechnology, Monitoring & Management 10 (2018) 331–338
4. Conclusion
The study highlighted the potential of green approach for fabrication
of SnO2 NPs by using P. betle leaves and SnCl2 as the precursors. The
comprehensive analysis of SnO2 NPs using relevant characterization tools
revealed their crystalline nature, spherical morphology, and uniform size
distribution with an average diameter of 8.4 nm. The photocatalytic po-
tential of the NPs was evaluated for the removal of textile grade pollutant
RY-186 dye. The as-prepared biogenic SnO2 degrades the dye with ap-
preciable degradation efficiency of 92.17% and the degradation process
followed the pseudo first order with the rate constant of 1.3 × 10−2 min-1.
The NPs also exhibited substantial selectivity towards photocatalytic de-
gradation of the RY-186 dye in a mixture comprising two other dyes in-
cluding RR-120 and RG-19, respectively. In addition, the NPs were char-
acterized by exceptional stability and reusability for cyclic photocatalytic
degradation of the RY-186 dye. Current study thus explored a facile, eco-
friendly, efficient, and economical approach for the application of green
synthesized SnO2 NPs in the abatement of RY-186 dye from water.
Conflict of interests
The authors declare that there is no conflict of interests regarding
the publication of this manuscript.
Acknowledgements
Authors are thankful to Vice-Chancellor, SGGSW University for
providing necessary laboratory facilities. DK acknowledges the support
of SERB, Government of India for providing financial assistance under
the early career research scheme (No. YSS/2015/000212).
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