Journal of Environmental Management 315 (2022) 115128

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Journal of Environmental Management

journal homepage: www.elsevier.com/locate/jenvman

Novel fabricated low-cost hybrid polyacrylonitrile/polyvinylpyrrolidone

coated polyurethane foam (PAN/PVP@PUF) membrane for the
decolorization of cationic and anionic dyes
Hala Fakhry a, Mervat El-Sonbati b, Basma Omar b, Reham El-Henawy b, Yifeng Zhang c, *,
Marwa EL-Kady d, e
a
Polymer Materials Research Department, Advanced Technology and New Materials Research Institute (ATNMRI), City of Scientific Research and Technological
Applications (SRTA-City), New Borg El-Arab City, Alexandria, 21934, Egypt
b
Department of Environmental Sciences, Faculty of Science, Damietta University, 34517, Damietta, Egypt
c
Department of Environmental Engineering, Technical University of Denmark, DK-2800, Kongens Lyngby, Denmark
d
Fabrication Technology Research Department, Advanced Technology and New Materials Research Institute (ATNMRI), City of Scientific Research and Technological
Applications, (SRTA-City), New Borg El-Arab City, Alexandria, 21934, Egypt
e
Chemical and Petrochemicals Engineering Department, Engineering Faculty, Egypt-Japan University of Science and Technology, New BorgEl-Arab City, Alexandria,
21934, Egypt

A R T I C L E I N F O A B S T R A C T

Keywords: Dyes are recalcitrait organic pollutants threatening the aquatic environment and human health. In the present
Polyurethane foam study, a novel low-cost hybrid membrane was fabricated by coating polyurethane foam (PUF) with poly­
Dye removal acrylonitrile/polyvinylpyrrolidone (PAN/PVP) via phase inversion technique from casting solutions consisting of
Wastewater treatment
PAN and PVP with Dimethyl formamide (DMF) and applied for removal of cationic (Methylene Blue (MB)) and
Adsorption
Polyacrylonitrile
anionic (Methyl Orange (MO)) dyes from aqueous solutions. The as-prepared membrane was first characterized
Polyvinylpyrrolidone by Scan Electron Microscope (SEM), Fourier Transform Infrared (FTIR), Energy Dispersive Spectrometry (EDS),
etc. Then, batch experiments were conducted to optimize the adsorption conditions, including contact time,
adsorbent dose, dyes concentration, and pH. The dye removal results fitted with pseudo first and second-order
kinetics; Langmuir, Freundlich, and Temkin isotherms’ models. The maximum dye decolorization was approx­
imately 97% and 95% within 60 and 120 min using 0.5 and 1 g of the fabricated composite for MB and MO,
respectively. The kinetic studies showed rapid sorption dynamics following a second-order kinetic model. In
addition, dye adsorption equilibrium data fitted well to the Freundlich isotherm with monolayer maximum
adsorption capacity of 6.356 and 3.321 mg/g for MO and MB dye, respectively. Thus, the novel hybrid mem­
brane is promising as a cheap and efficient adsorbent for the removal of both cationic and anionic dyes from
wastewater. The current study demonstrated a new avenue to achieve efficient management of dyes in aquatic
environments.

1. Introduction difficult to decompose and, therefore, remain in the environment for a

With the rapid urbanization, industrialization and technological
advances, water scarcity and water pollution become global problems
threatening the entire biosphere and affecting human health. Dyes are
one of the most hazardous water pollutants which are extensively used
in textile, paper, food, leather, cosmetics, plastics, printing, and phar­
maceutical industries (El-Aswar et al., 2022). The physicochemical and
thermal stability of residual dyes in industrial wastewater make them
long time and threaten the aquatic environment and human health
(Duan et al., 2020).
Various technologies have been developed for dyes removal from
wastewater, including coagulation, flocculation, photocatalysis, ozona­
tion, advanced oxidation processes, membrane filtration, and biological
treatment (Aichour et al., 2022). Among them, adsorption is a more
competitive and effective method due to its outstanding superiorities
such as high adsorption efficiency, economic viability, simple operation,

* Corresponding author.
E-mail address: yifz@env.dtu.dk (Y. Zhang).

https://doi.org/10.1016/j.jenvman.2022.115128
Received 19 October 2021; Received in revised form 13 April 2022; Accepted 18 April 2022
Available online 25 April 2022
0301-4797/© 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
H. Fakhry et al.
recyclability, vast choice of adsorbents, easily applied on a large scale,
and environmental friendship. Many traditional adsorbents (fly ash,
silica, zeolite, chitosan, clay minerals, activated carbon and carbon
nanotube) have been explored for dye removal from wastewater.
However, the drawbacks of these adsorbents, such as low adsorption
capacity, low adsorption efficiency, long equilibrium time, and low
selectivity limited their practical applications in wastewater treatment
(Fan et al., 2020).
Recently, polymeric adsorbents have been emerging as promising
alternatives to traditional adsorbents due to their outstanding advan­
tages like wide variations in porosity, simple prepared process, high
surface area, and easy modification with functional groups to enhance
the selective performance (Duan et al., 2020). Polyacrylonitrile (PAN) is
one of the most important polymers that has been used extensively in
water treatment due to its excellent thermal & mechanical stability,
chemical resistance, non-toxic nature, commercial availability, surface
functionalization and hydrophobic nature (Chabalala et al., 2021). The
porosity of PAN can be enhanced by using various pore-forming agents.
Polyvinylpyrrolidone (PVP) with CH2, C–O, and C–N functional groups,
is an excellent pore-forming agent that increases the number of pores per
unit surface area without altering the pore size and distribution. In
addition, it is a non-toxic, biodegradable polymer that can be readily
soluble in water and various non-aqueous solvents. Moreover, it has
unique properties, including high thermal & chemical stability, good
tensile strength, hydrolysis resistance and physiological compatibility
(Gouthaman et al., 2018). However, the prepared PAN particles are
difficult to separate from aqueous solutions. So, it was necessary to use it
in another form such as membrane, or as a coating for other materials to
enhance their adsorption properties.
Using renewable and low-cost resources to prepare novel polymeric
materials, specifically polyurethane (PU), has garnered increasing
attention through the last years. PU is a macromolecular polymeric
material that exhibits common rubber and rigid plastic properties, with
excellent hydrodynamic characteristics. Among the main applications,
polyurethane foam (PUF) is one of the most prominent polyurethane-
based products, with high consumption of 67% of the global PU con­
sumption. PUFs have been widely exploited as a solid phase for removal
of dyes from effluent (Zhao et al., 2021). Development of versatile
porous materials could lead to water treatment without harsh efforts and
consumption of electrical and thermal energy as these sources have
become the main integral part of other water treatment systems.
Therefore, efforts are required for developing material methodologies
for the synthesis of porous adsorbents to bring down the overall cost of
the water purification process.
The literature review revealed that there was no reported researches
on using PUF wastes as a carrier for PAN/PVP to remove cationic and
anioninc dyes from wastewater. Thus, the present study aims to fabri­
cate a novel, cost-effective adsorbent material by coating PUF wastes
with a matrix of PAN and PVP polymeric solution (PAN/PVP@PUF
hybrid membrane) for efficient removal of cationic (MB) and anionic
(MO) dyes from aqueous solutions. The fabricated composite can be
easily separated from aqueous solutions without the need for additional
operations such as filtration or centrifugation making it economically
and cost-efficient, as well as improving wastewater treatment potentials.
Thus, the proposed adsorbent can solve more than one problem in a
simple one-step by using PUF wastes and increasing the efficiency and
reusability for environmental remediation.
2. Materials and methods
2.1. Reagents and materials
All chemicals used were of analytical reagent grade quality without
further purification. Stock solutions (500 ppm) of MB (Sigma Aldrich: CI
52015, CAS 122965-43-9, purity ≥82%) and MO (Merck, CI 13025, CAS
547-58-0, purity 80–100%, Germany) dyes were prepared by dissolving
2
Journal of Environmental Management 315 (2022) 115128
an accurate weight (0.5 ± 0.05 g) of each dye in double distilled water
and completed to the mark of 1 L measuring flask. Potassium persulfate
(K2S2O8, 0.1 M), acrylonitrile monomer, ethyl alcohol, Dimethyl
Formamide (DMF) and Polyvinyl Pyrolidine (PVP) were also used
throughout. White polyurethane foam remains (PUFR) were collected
from upholstery stores and furniture factories from Damietta City,
Egypt, and cut into 0.5 cm thickness and 5.5 cm diameters surface discs.
2.2. Preparation of polyacrylonitrile (PAN) powder
Precipitation polymerization technique was adopted for the prepa­
ration of PAN in the presence of potassium persulfate, K2S2O8, as an
initiator (El-Aassar, 2013). The polymerization process was conducted
by dissolving acrylonitrile monomer in 0.1 M K2S2O8 alcoholic solution
according to a mass ratio of 1:9. The solution content was stirred in a
thermostatic water bath for 4 h at 65 C. The obtained slurry particles
◦
were filtered and washed with 10% ethanol to remove the unreacted
initiator and monomers. The obtained polyacrylonitrile powder was
dried in an oven at 45 C and finally ground to the desired mesh size
◦
(Fig. 1).
2.3. Preparation of PAN/PVP@PUF hybrid membrane
The proposed PAN/PVP@PUF membrane was fabricated via phase
inversion process (Rana et al., 2015) by combining PAN powder (12%
w/v) with 5% (w/v) PVP and 10 ml DMF as a solvent. The casting so­
lution was stirred for 4 h on a hot plate at 65 C for complete dissolution
◦
then casted on PUF disc in Petri dish. The cast polymer solution film was
immersed in a water (nonsolvent) bath to complete the phase inversion
(coagulation (gelation)) then in deionized water for 24 h to remove any
soluble water material and was dabbed between two filter papers for
drying at room temperature and finally cut into small discs (Fig. 1).
2.4. Characterization of the prepared PAN/PVP@PUF hybrid membrane
All characterization was carried out in the city of Scientific Research
and Technological Application (Alexandria City). The morphological
and chemical structure of the fabricated PAN/PVP@PUF hybrid mem­
branes were characterized using different devices such as Scan Electron
Microscope (SEM, JEOL JSM, 6360 LA Japan), Fourier Transform Infra-
Red spectroscopy (Shimadzu FT-IR 8400 S, Japan) and Energy Disper­
sive Spectrometry, EDS (ZEISS Sigma 300 VP).
The porosity of the fabricated hybrid membrane was measured ac­
cording to the following procedure: 1 cm *1 cm of the wet membrane
were cut down, the water droplets on the surface were dabbed with filter
paper, then weighted (W1) and dried at 50 C for 24 h in an oven. The
◦
membrane was reweighted (W2) and the thickness (l) was measured
using a micro-meter. The membrane porosity was calculated according
to the following equation (Heng et al., 2021):
w1 − w2
ε= (1)
A l ρw
where, ρw is the density of distilled water, l is the thickness of membrane
(m), A is the area of membrane (m2).
The swelling behavior of the fabricated membrane was investigated
by immersing the pre-weighted membrane discs (0.015 gm) in a large
excess of deionized water at room temperature for 1 week. The discs
were withdrawn from water at different time intervals and their wet
weight were measured after first blotting with a filter paper to remove
the surface water. The swelling ratio was calculated as following (Sed­
diki et al., 2020):
Mt − Mo
Swelling % = *100 (2)
Mo
where Mt is the swollen hybrid membrane discs at a given time during
H. Fakhry et al.
Fig. 1. Schematic diagram for preparation of PAN/PVP@PUF hybrid membrane.
swelling and M0 is the dry mass of the fabricated hybrid membrane discs.
2.5. Optimization of PAN/PVP@PUF membrane performance
To perform the optimum adsorption conditions (contact time,
adsorbent dose, pH and dye concentration) of MB and MO dyes onto the
PAN/PVP@PUF membrane in batch mode, the stock solution of each
dye was diluted using distilled water to make the working solutions. The
concentration of each dye tested solutions was measured with a single
beam spectrophotometer (JENWAY 7305) with quartz cells (10 mm path
length). The pH of the desired dye solutions was adjusted to the required
values using NaOH and HCl solution (0.1 M, pH: 2–11). A pH meter
(ADWA, 1000 CE, Romania) was used for pH measurements. In order to
evaluate the adsorption performance, 0.2 g of PAN/PVP@PUF mem­
brane discs were added to the working solutions containing dye (10 ml
of 10 mg/l) and stirred using lab-line Stuart Scientific Orbital mechan­
ical shaker (SO1, UK) for both MB and MO dyes at 25 C for different
◦
mixing periods. Then, the adsorbent was separated from the aqueous
solution and the absorbance of MB and MO solutions was measured at
668 and 465 nm, respectively. The effect of pH (2, 5, 7, 9, and 11), initial
dye concentration (10–100 mg/l), and adsorbent dose (0.05–1 g) were
examined at the optimum contact time. The adsorption efficiency (R, %)
of MB and MO by the fabricated membrane was determined using the
following expression (Aichour et al., 2022):
Ci − Ce
R% = *100 (3)
Ci
where Ci and Ce are the initial and final concentrations of MB and MO
(mg/l).
To study the adsorption-desorption process, 0.5 and 1 g of PAN/
PVP@PUF discs were mixed with 10 mL (10 mg/l) MB and MO solu­
tions, respectively. After equilibrium, the discs were poured into
different eluting agents, stirred for the optimum time of each dye, and
separated from the working aqueous solution. The desorption process
was performed up to 10 cycles for both dyes. All measurements were
conducted in triplicate and the average values were included in the
calculation.
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Journal of Environmental Management 315 (2022) 115128
2.6. Point of zero charge
Point of zero charge was determined according to Cardenas-Peña
et al. (2012), 0.2 gm of the hybrid membrane discs was added to 40.0 mL
of 0.1 M NaNO3 in ten 120 ml bottle. The pH was adjusted to 2, 3, 4, 5, 6,
7, 8, 9, 10 and 11 with 0.1 M HCl and 0.1 M NaOH as needed, then were
shaken for 24 h to reach equilibrium. After that, the final pH (pHf) was
measured and the initial pH (pHo) vs. the difference between the pHo
and pHf values (ΔpH) was plotted. The pzc was taken as the point where
pH = 0.
2.7. Adsorption isotherms
Adsorption isotherms was carried out by shaking various initial dye
concentrations (10–100 ppm) with 0.2 g PAN/PVP@PUF membranes for
120 min (MO) and 60 min (MB) at the optimum pH value for each dye.
After equilibrium, the amount of dye adsorbed (qe, mg/g) was deter­
mined and plotted against the equilibrium concentration (Ce, mg/l).
Three common models Langmuir, Freundlich, and Temken (Table 1)
were applied to show the well fit with the adsorbtion process.
Table 1
Langmuir, Freundlich and Temkin models’ equations for adsorption of MB and
MO onto PAN/PVP@ PUF hybrid membrane at 25 ◦ C (El-Amier et al., 2021).
Adsorption Equation Parameters
Models
Langmuir Ce/qe = 1/ qe is the MB and MO amount adsorbed at
qmKL+ Ce/qm equilibrium (mg/g), qm is the maximum
monolayer coverage capacities (mg/g), KL is
the Langmuir constant (l/mg), and Ce is the
equilibrium concentration of MB and MO (mg/
l).
Freundlich ln qe = ln KF + qe is the MB and MO amount adsorbed at
1/nF ln ce equilibrium (mg/g); Ce is the MB and MO
equilibrium concentration (mg/l); and KF and
nF are Freundlich constants related to the
adsorption capacity and adsorption intensity,
respectively
Temkin RT T (K) is the temperature, R is the universal gas
qe= ln (KT
b constant, KT is constant refer to equilibrium
Ce) maximum binding energy and constant b (J/
mol) is related to the heat of adsorption.
H. Fakhry et al. Journal of Environmental Management 315 (2022) 115128

2.8. Adsorption kinetics
Kinetic study was conducted by shaking 10 mL of both MO and MB
dyes (10 ppm) separately with 0.2 g of PAN/PVP@PUF hybrid discs for
different time intervals (5–180 min). The concentration of dye was
determined after each time interval and the amount of dye adsorbed (qt,
mg/g) was plotted against time (t, min) for kinetic modeling (Table 2).
3. Results and discussions
3.1. Characterization of the PAN/PVP@PUF membrane
3.1.1. Morphological structure identification using scanning electron
microscope (SEM)
The surface morphology and topography of the fabricated mem­
branes before and after exposure to the dye models (MB and MO) are
shown in Fig. 2. It was clear that a dense layer in the cross-section with
good coverage resulted from the coating of PUF with the mixed poly­
mers, PAN and PVP (Fig. 2a). Moreover, there were many voids on the
membrane surface, which might enhance its adsorption capabilities. The
surface morphology of the membrane loaded with MB and MO dyes
clarified the disappearance of voids and ridges due to the adsorption and
coverage of the dyes molecules (Fig. 2b and c).
3.1.2. Energy Dispersive Spectrometry (EDS)
The elemental mapping and the EDS spectrum of prepared PAN/
PVP@PUF membrane were investigated to assure the presence of the
related elements and the success of adsorption process. As shown in
Fig. S1, the W% and the amount of N, S, Cl beside the other light ele­
ments, confirm that membrane structure includes MB and MO on the
surface. EDX mapping analysis also presented to provide information
about the elemental composition of the membrane before and after
adsorption of both dyes.
with PAN solution (Mohammad and Atassi, 2020). FTIR spectrum of
PVP (Fig. 3b) showed a broad peak at 1653.59 cm− 1 which is attributed
– C and shifted to a lower wavenumber in the unloaded fabricated
to C–
membrane (Chokki et al., 2019). In addition, there was a transmittance
band at 1446.06 cm− 1 corresponding to C–H cyclic structures of pyr­
rolidone in PVP which was hypo-shifted to 1423 cm− 1 in the unloaded
membrane, confirming the coating of the fabricated membrane with
PVP (Rahma et al., 2016). Comparing of FTIR spectra before and after
MB and MO dyes adsorption (Fig. 3) revealed that the peak at 1654.62
cm− 1 attributed to –C–
– O, was shifted in the loaded fabricated mem­
branes with MB to 1628.91 cm− 1, confirming the presence of a car­
boxylic group, which could be responsible for the electrostatic attraction
between the negatively charged carboxylate ion and the positively
charged MB. Moreover, a transmittance band of ester C–O at 1037.26
cm− 1 was found in the unloaded fabricated membrane, confirming the
incorporation of PUF (Sultan et al., 2019). This peak was shifted to
1046.23, and 1053 after the adsorption of MB and MO dye onto the
membrane. All the characteristic peaks in the fingerprint zone of MB and
MO dye spectra (Fig. 3d and g) were disappeared or shifted in the loaded
fabricated membranes with MB and MO spectra (Fig. 3f and e), con­
firming the adsorption of both dyes.
3.1.4. Membrane porosity
Surface porosity is one of the crucial factor that evaluate the mem­
brane performance in a specific application (Gouthaman et al., 2018).
The calculated porosity of the fabricated hybrid membrane was 80.35%,
revealing its high porous structure and potential adsorption capabilities.
The fabricated membrane showed a high porosity compared with Chung
et al. (2008) which recorded 10% and 12% porosity for non-woven
fabrics. Chao et al. (2006) reported a porosity of 52.2%–65.5% for
chitosan membrane depending on the molecular weight of the poly
(ethylene glycol) used. Moreover, 5.7%–8.92% was achieved by
different fabricated hollow fiber membranes (Mailah et al., 2016).

3.1.3. Chemical structure identification using Fourier Transform Infrared
(FTIR)
FTIR spectra of PAN, PVP, unloaded PAN/PVP@PUF membrane, MO
dye, MO loaded PAN/PVP@PUF membrane, MB loaded PAN/PVP@PUF
membrane, and MB dye was illustrated in Fig. 3a, b, c, d, e, f, and g,
respectively. PAN FTIR spectrum (Fig. 3a) indicates a characteristics
peak at 2245.66 cm− 1 corresponding to C– – N, another peak at 1460
– temperature and reached to equilibrium state after 72 h. The same trend
cm− 1 associated with C–H scissoring, and a peak at 2927 cm− 1 corre­
sponding to C–H stretching (Mahmood and Waisi, 2021). All these peaks
were shifted to lower wavenumber in the unloaded fabricated mem­
brane spectrum, which revealed the success of the membrane coating
Table 2
Pseudo-first-order, Pseudo-second–order, Elovich, and Intra-particle diffusion
kinetics models’ equations for adsorption of MB and MO onto PAN/PVP@ PUF
membrane at 25 ◦ C (El-Amier et al., 2021).
Adsorption Equation Parameters
Kinetic Models
Pseudo-First- ln (qe-qt) = ln qt and qe is the dsorbed dye amount at time t
Order qe- K1t and at equilibrium (mg/g) respectively. k1
(min− 1) is the first-order reaction rate
constant
Pseudo-Second- t/qt = (1/ qt and qe is the dsorbed dye amount at time t
Order K2q2e ) and at equilibrium (mg/g) respectively, k2 is
the second-order reaction rate equilibrium
constant (g/mg min).
Elovich Qt = ß ln (αβ)- where Qt: the amount adsorbed at time t (mg
lnt g− 1); β: the number of sites available for
adsorption; α: the initial adsorption rate (mg
g− 1 min); and t: contact time (min).
Intra-particle Qt = kidt1/2 + kid is the intra-particle diffusion rate
Diffusion c constant, and c give prediction about the
boundary layer thickness
3.1.5. Swelling measurements
The swelling characteristics of the fabricated membrane was
measured (Fig. S2) which depicts the swelling ratio of the fabricated
membrane in water at room temperature as a function of time. It was
observed that the fabricated membrane swell and retained its original
shape when immersing in excess deionized water for a week at room
was reported by Seddiki et al. (2020) and Kowalski et al. (2019).
3.1.6. Point of zero charge (pzc)
The pzc is of fundamental importance in surface science as, it de­
termines how easily a substrate is able to adsorb potentially harmful
ions. The pzc of the prepared membrane discs was examined and the
data were displayed in Fig. S3. It was found that the final pH 2 and 3
were nearly identical to the initial values, where the pHs 4, 5, 6, 7, 8, 9
all changed to around 7.2 ± 0.2. This indicated that the membrane has
an estimated pzc value at pH = 7.2, at which the surface reaches elec­
trically neutral state and above which, the membrane is negatively
charged and adsorb positively charged MB dye, while below which the
membrane surface is positively charged and attract negatively charged
MO dye.
3.2. Performance of PAN/PVP@PUF fabricated membrane
The ability of the membrane was evaluated for MB and MO dyes
adsorption from aqueous solution at room temperature through batch
mode experiments. The influence of various parameters on the uptake of
MB and MO dyes were critically investigated.
3.2.1. Effect of contact time
The effect of contact time (5–180 min) on the uptake of MB and MO
dyes (10 ml of 10 mg/l) by the fabricated adsorbent was investigated. As

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H. Fakhry et al. Journal of Environmental Management 315 (2022) 115128

Fig. 2. SEM of a) unloaded PAN/PVP@PUF membrane, b) and c) MB and MO loaded membrane at x100, d) MO loaded membrane at x500, and e) cross-section of the
unloaded membrane.

increasing adsorbent dose above 0.5 g, as the available number of dye

molecules in solution was not enough to completely combine with all
effective adsorption sites on the adsorbent, resulting in a surface equi­
librium state (Kuang et al., 2020). Thus, a dose of 0.5 g was adopted in
the subsequent work (Elkady et al., 2018; Wong et al., 2020). The ob­
tained results agreed with that reported by Elsayed et al. (2020) and
Gagliano et al. (2020).

3.2.3. Effect of pH
The pH of the adsorption medium could greatly affect the adsorbent
surface charge and the ionization of adsorbate (Aichour et al., 2022).
The influence of solution pH (2, 5, 7, 9, and 11) on the adsorption of MB
and MO dyes onto the fabricated adsorbent was studied. The data dis­
played in Fig. 4C reveal that for MB, there is an increase in removal
percent with increasing pH and reached maximum value 89% at pH 11,
while for MO the maximum removal percent was 93% at pH 2, then
decreased with increasing pH. This fact can be explained by the
competition between the surface charge of adsorbent and solution
chemistry as two important factors, MB is a cationic dye, at pH < pHpzc,
the adsorbent surface is positively charged according to protonation of
functional groups, causing cation exchange between dye molecules and
hydrogen ions of protonated groups. The competition between dye
cations (MB+) and free positive hydrogen of acidic solution reduces the
dye uptake. At pH > pHpzc, the composite surface bear a negative
Fig. 3. FTIR Spectra of a) PAN, b) PVP, c) unloaded PAN/PVP@PUF mem­
charge. Therefore, electrostatic attraction between active sites and dye
brane, d) MO dye, e) MO loaded PAN/PVP@PUF membrane, f) MB loaded
cations will occur. On the other hand, the dye molecules on the surface
PAN/PVP@PUF membrane, and g) MB dye.
of the composite can form π-π bonds with other dye molecules (Wong
et al., 2019). The opposite behavior was recorded for the anionic MO
shown in Fig. 4a, the removal efficiency was increased with contact time
dye (Aichour et al., 2022). These results were also confirmed with other
and reached a maximum value of 94.82% and 57.57% after 60 and 120
reported data for MB and MO adsorption process (Faisal et al., 2022;
min for MB and MO, repectively (Wong et al., 2018). Within the first 5
Aichour et al., 2022).
min, significant increase in the adsorption process was observed and this
was attributed to the availability of active sites and functional groups at
3.2.4. Effect of initial dye concentration
the surface of the fabricated membrane, which became gradually satu­
The effect of initial dye concentration (10–100 mg/l) on the
rated with time, leading to slow dawn the adsorption rate. The obtained
adsorption process employing the fabricated membrane was evaluated
results were basically consistent with previous studies (Gagliano et al.,
as shown in Fig. 4D. High removal percentage of MB and MO dyes at low
2020; Boonying et al., 2019).
concentrations was observed due to unoccupied and available active
sites on the adsorbent surface. However, increasing the initial concen­
3.2.2. Effect of adsorbent dosage
tration led to decrease of the removal percentage for both dyes because
The effect of the adsorbent dosage (0.05–1 g) on MB and MO dyes’
the adsorptive sites were all occupied by dye molecules (Faisal et al.,
adsorption was critically investigated. The removal percentage of MB
2022; Aichour et al., 2022). Similar trend was obtained by Janboor­
and MO dyes increased from 75.670 to 96.97% and 53.29–94.90%,
anapinij et al. (2021) who reported that the removal efficiencies for both
respectively with increasing the adsorbent dose from 0.05 to 0.5 g as
MB and MO (10 ml of 10 mg l− 1) at pyrolyzed industrial carpet waste
obvious from Fig. 4b. This may be due to increase the number of
were 97.8% and 80.3%, which decreased with increasing initial dye
adsorbent pores and available active sites which enhanced the dye up­
concentration.
take. However, no significant increase in dye removal was observed with

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H. Fakhry et al. Journal of Environmental Management 315 (2022) 115128

Fig. 4. Significance of operating variables (A) contact time (min), (B) adsorbent dosage (gm), (C) pH, and (D) dye concentration (mg/l) on MB and MO dyes
adsorption (10 ml) at 25 ◦ C.

3.3. Adsorption isotherm

Table 3
Langmuir, Freundlich and Temkin parameters for adsorption of MB and MO (10
Adsorption isotherms explain how MB and MO molecules are
ml, 10–100 ppm) onto 0.5 gm PAN/PVP@ PUF hybrid membrane at 25 ◦ C.
distributed between the membrane surface and aqueous solution as the
Isotherm parameters MB MO
adsorption process reaches an equilibrium. This can be evaluated by
fitting the adsorption data to different isotherm models (Langmuir, Langmuir
Freundlich, and Temkin (Table 1)) to identify the best model fitting the qm (mg g− 1) calculated 3.321 6.356
KL (l mg− 1) 0.171 0.021
experimental data (Alfrhan et al., 2020). Langmuir isotherm model
R2 0.984 0.879
postulates a monolayer adsorption of adsorbate onto a homogeneous Freundlich
adsorbing surface characterized by energetically identical binding sites. KF (mg g− 1) × (l mg− 1)1/n 0.644 0.1814
The Freundlich model endorses a multilayer adsorption process onto nF 2.36 1.32
R2 0.998 0.999
heterogeneous adsorption sites (El-Amier et al., 2021). The applicability
Temkin
of the isotherm equations is compared by judging the correlation co­ B (l mg− 1) 0.564 0.926
efficients (R2). The essential characteristics of Langmuir isotherm can be KT (KJ mol− 1) 3.255 0.441
expressed in terms of dimensionless equilibrium parameter RL = R2 0.978 0.905
1/(1+bCo), where b is the Langmuir constant and Co is the initial dye
concentration (mg l− 1). The value of RL indicates the type of the
4.17) for MB and (3.45) for MO uptake by raw Algerian kaolin and
isotherm to be either unfavourable (RL > 1), linear (RL = 1), favourable
activated carbon, respectively. Temkin isotherm model (Table 1) in­
(0 < RL < 1), or irreversible (RL = 0). The logarithmic form of
corporates the effects of adsorbate–adsorbate interactions on the
Freundlich model (Table 1), the values KF and 1/nF were obtained from
adsorption process. As general, typical adsorption energies, (RT/b ln
the intercepts (ln KF) and slope (1/nF) of the linear plots of ln qe & ln Ce.
(KT)), in the range of 8–16 kJ mol− 1, are associated with chemisorption
The slope 1/nF ranging between 0 and 1 is a measure of adsorption in­
as well as b value higher than 80 kJ mol− 1 (El-Amier et al., 2021). Ac­
tensity or surface heterogeneity as the adsorbent surface becomes more
cording to the R2 value, the Temkin isotherm model did not fit well with
heterogeneous if the value of 1/nF closes to zero, meanwhile, if the value
the experimental data indicating the energetic heterogeneity of the
of 1/nF below one this indicates a normal Langmuir isotherm and if it is
adsorption sites and physicosorption process (RT/b lnKT = 0.666 and
above one this is indicative of cooperative adsorption. Via comparison of
0.76 while n = 4.392 and 2.675 kJ mol− 1 for MB and MO, respectively).
the R2 values, Freundlich equation represents a better fit of equilibrium
These results were agreed with that reported for MB adsorption onto
experimental data than Langmuir as shown from the calculated pa­
electrospun nanofibrous membranes of polylactic acid and poly­
rameters (Table 3 and Fig. 5).
acrylonitrile coated with chloride doped polyaniline and MO adsorption
The calculated adsorption intensity (nF) from the Freundlich model
onto activated carbon (Shikuku and Mishra, 2021).
was 2.36 and 1.32 (1/nF = 0.424 and 0.76) for MB and MO, respectively
confirming strong adsorbate–adsorbent bonding (Shikuku and Mishra,
2021). El Maguana et al. (2020) reported good adsorption potential (n =

6
H. Fakhry et al. Journal of Environmental Management 315 (2022) 115128

Fig. 5. Equilibrium isotherm models; (A) Langmuir, (B) Freundlich, and (C) Temkin for adsorption of MB and MO (10 ml, 10–100 ppm) onto 0.5 gm of the fabricated
PAN/PVP@ PUF hybrid membrane.

3.4. Comparison of maximum adsorption capacity with other adsorbent

Table 4
material
Comparison of the maximum adsorption capacity of the present study with
previously reported.
The adsorption capacity of the proposed PAN/PVP@PUF membrane
Adsorbents Dyes Qm (mg/ References
for removal of MB and MO dyes were compared to other adsorbents as
g)
shown in Table 4. It is obvious that PAN/PVP@ PUF composite exhibited
good adsorption capacity for dye removal compared to previously re­ AC from coconut shell MO 3.00 Islam et al. (2016)
Biofunctional BiOCl3I solid 5.000 Zhang et al. (2016)
ported materials which are either expensive or required prolonged
Cellulose acetate/polyurethane 0.185 (Iqhrammullah et al.,
chemical or thermal treatments that limit their applicability in practical 2020)
implications. However, a lot of operational conditions affect the vari­ Fe NPs/SiO2–NH2/black tea 2.970 Perrotti et al. (2019)
ances in adsorption capacities such as dosage, pH, time, concentration, extract
Chitosan/PVA/Na-titanate/TiO2 6.860 Habiba et al. (2016)
volume, etc. On the basis of those facts, the proposed composite is both
CPW-500 (CaCO3/ carbon) 1.32 Janbooranapinij et al.
efficient, practically and economically feasible. (2021)
CPW-900 (Ca(OH)2/ carbon 1.84 Janbooranapinij et al.
(2021)
3.5. Adsorption kinetics PAN/PVP@ PUF hybrid 6 This study
membrane
calcined cryptocrystalline MB 0.71 Ngulube et al. (2019)
Adsorption kinetics provide valuable information on the adsorption
magnesite - halloysite
mechanisms which may be controlled by either external or film diffu­ nanocomposite
sion, pore diffusion and adsorption on the pore surface, or a combination Phosphoric acid based 3 Khan et al. (2015)
of more than one step. To predict the mechanism of the adsorption geopolymer
process of MB and MO onto the hybrid composite, the experimental data Magnetic NaY Zeolite 2.046 Shirani et al. (2014)
Almond shell-activated carbon 1.33 Wu and Tseng (2008)
were fitted with pseudo-first-order (PFO), pseudo-second-order (PSO), 750 C
◦

Elovich, and intraparticle diffusion models (Table 2). The kinetic Fe3O4–TiO2 NPs 1.880 (Alizadeh Eslami et al.,
adsorption parameters were illustrated in Table S1 and Fig. 6. According 2018)
to the obtained R2 values, the adsorption data is better fitted to the PSO CPW-500 (CaCO3/carbon) 1.86 Janbooranapinij et al.
(2021)
(MB R2 = 0.999, MO R2 = 0.999), suggesting that the boundary layer
CPW-900 (Ca(OH)2/carbon) 2 Janbooranapinij et al.
resistance was not the rate-determing step (El Maguana et al., 2020). (2021)
The intraparticle diffusion model was used to understand the stages that PAN/PVP@ PUF hybrid 3 This study
control the adsorption rate. As shown in Fig. 6d, two separate regions membrane
with different slopes (Kid) and intercepts (Ci) revealed that the
adsorption process of MB and MO onto the fabricated membrane con­
sists of surface adsorption and intraparticle diffusion and this was
confirmed by the values of C1 and C2 represented in Table S1 (Aichour

7
H. Fakhry et al. Journal of Environmental Management 315 (2022) 115128

Fig. 6. Adsorption Kinetics Models; pseudo-first-order (A), pseudo-second-order (B), Elovich (C), and Intraparticle diffusion (D) for MB and MO (10 ml, 10 ppm)
adsorption onto 0.5 gm PAN/PVP@ PUF hybrid membrane at 25 ◦ C.

Fig. 7. Adsorption mechanism of MB and MO dyes onto the fabricated PAN/PVP@PUF hybrid membrane.

8
H. Fakhry et al.
et al., 2022).
3.6. Mechanism of interaction
The adsorption mechanism proposition (Fig. 7) is critical for clear
understanding of the adsorption process. The improved removal of MB
under basic conditions (pH > Pzc for MB and pH < Pzc for MO)
demonstrated that electrostatic attraction plays a critical role in the
adsorption of cationic MB dye onto the adsorbent surface, as stated in
the “FTIR” section. For adsorption of MO onto the fabricated membrane,
according to the FTIR data, the decrease in the strength of the OH
stretching vibration at 3443 and 3448 cm− 1 for PVP and the fabricated
membrane, respectively and the red shift observed at 3439 cm− 1 for
PAN/PVP@PUF hybrid membrane with MO after anionic dye adsorp­
tion suggests that anion exchange of dyes is involved with the removal of
the hydroxyl (OH) group from the fabricated membrane. Furthermore,
the presence of a new absorption peak (1049 cm− 1), attributed to C–N
stretching vibration, supports the incorporation of MO in the fabricated
membrane. Thus, the adsorption of both dyes by the fabricated mem­
brane may be achieved by different forces as H- bonding, Wander Val,
electrostatic attraction, ion-exchange, π-π interaction, etc. Our findings
were similar to that previously reported (Khan et al., 2021).
3.7. Recyclability of the fabricated membrane
The recyclability was investigated using 0.5 and 1 g of the membrane
discs after equilibrium adsorption of 10 ml (10 ppm) for both dyes.
Different eluting agents (HCl, H2SO4, HNO3, NaOH, and acetone) were
examined separately at different mixing ratios for dye recovery from
membrane discs. The discs were washed with these eluants for 1 h (MB)
and 2 h (MO) under continuous agitation at room temperature, washed
several times with DDW, and debated with filter papers. The most
satisfied eluting agent was 100% acetone for MB dye and a mixture of
50% acetone and 50% HCl for MO dye (Fig. S4 and S5). The regenerated
membrane discs were reused for the second cycle with previous pro­
cedures to evaluate their adsorption capacity after recovery tests. The
removal percentage of both dyes reached almost 100% after 10 cycles,
revealing the high reusability of the fabricated membrane.
4. Conclusion
There is a global need to develop effective eco-friendly technologies
to treat dye-containing wastewater and prevent adverse impacts on the
environment and human beings. A novel hybrid (PAN/PVP@PUF)
membrane was developed, characterized, and optimized to remove MB
and MO dyes from aqueous solutions. The developed adsorbent achieved
a maximum removal percentage of 94.82% and 57.57% after 60 min for
MB and 120 min for MO. Increasing adsorbent dose from (0.05–1.0 g)
lead to increase the % R from 75.670 to 96.97% and 53.29–94.90% for
MB and MO, respectively. The optimum pH for removing MB was 11.0
and 2.0 for MO. The experimental results were fitted to Freundlich’s
isotherm and following a second-order kinetic model for both dyes. The
reusability studies revealed that the most satisfied eluting agent was
100% acetone for MB dye and a mixture of 50% acetone and 50% HCl for
MO dye. The removal percentage of both dyes reached almost 100%
after 10 cycles. Thus the as-prepared PAN/PVP@PUF membrane was a
promising adsorbent for organic dye removal.
5. Future prospectives
The present study provided a new adsorbent for MB and MO dyes
removal from aqueous solutions. However, further improvement should
be applied to bridge this adsorbent with industry. These improvements
including:
9
Journal of Environmental Management 315 (2022) 115128
- Enhancing the structure of the as-prepared membrane through
incorporating in-organic nanomaterial to add more active sites for
the adsorption process.
- Imploying the modified composite in both static and dynamic mode
(fixed-bed column and ultrafiltration cell) to find the propagation of
the contaminant under different operational conditions for lab scale
application.
- Applying the modified composite for removal of organic and inor­
ganic contaminants from real wastewater samples.
This research did not receive any specific grant from funding
agencies in the public, commercial, or not-for-profit sectors.
Credit author statement
Hala Fakhry: Conceptualization, Methodology, Formal analysis,
Investigation and Writing – original draft, Mervat El-Sonbati: Resources,
Visualization, Supervision, Investigation, writing and reviewing Writing
– original draft, Basma Omar: Investigation, Visualization, writing and
reviewing Writing – original draft, Reham El-Henawy: Investigation and
Data curation, Yifeng Zhang: Provided feedback, reviewing and editing
the manuscript, Marwa EL-Kady: Resources, Supervision, reviewing and
editing the manuscript.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jenvman.2022.115128.
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