Ecotoxicology and Environmental Safety ()

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Ecotoxicology and Environmental Safety

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

Treatment of laundry wastewater using

polyethersulfone/polyvinylpyrollidone ultraltration membranes
A. Sumisha a, G. Arthanareeswaran a,n, Y. Lukka Thuyavan a, A.F Ismail b,n, S. Chakraborty c
a
Membrane Research Laboratory, Department of Chemical Engineering, National Institute of Technology, Tiruchirappalli 620015, India
b
Advanced Membrane Research Center (AMTEC), UniversitiTeknologi Malaysia (UTM), Skudai 81310, Johor, Malaysia
c
Department of Informatics, Modeling, Electronics and Systems Engineering (DIMES),University of Calabria, Via P. Bucci, Cubo 42a, 87036 Rende, CS, Italy

art ic l e i nf o a b s t r a c t

Article history: In this study, laundry wastewater ltration was studied using hydrophilic polyvinylpyrollidone (PVP)
Received 9 January 2015 modied polyethersulfone (PES) ultraltration membranes. The performances of PES/PVP membranes
Received in revised form were assessed using commercial PES membrane with 10 kDa in ultraltration. Operating parameters The
1 April 2015
inuence of transmembrane pressure (TMP) and stirring speed on laundry wastewater ux was in-
Accepted 6 April 2015
vestigated. A higher permeate ux of 55.2 L/m2h was obtained for modied PES membrane with high
concentration of PVP at TMP of 500 kPa and 750 rpm of stirring speed. The separation efciencies of
Keywords: membranes were also studied with respect to chemical oxygen demand (COD), total dissolved solids
Laundry wastewater (TDS), turbidity and conductivity. Results showed that PES membrane with 10% of PVP had higher
Ultraltration
permeate ux, ux recovery and less fouling when compared with other membranes. Higher COD and
Total dissolved solids
TDS rejection of 88% and 82% were also observed for modied membranes due to the improved surface
Turbidity
Chemical oxygen demand property of membranes. This indicated that modied PES membranes are suitable for the treatment of
surfactant, detergent and oil from laundry wastewater.
& 2015 Elsevier Inc. All rights reserved.

1. Introduction conventional treatment of laundry wastewater methods are coa-

The three major fundamental concerns of current and future
water resources are lack of water, poor water quality and water
related debacles (UNESCO, 2003). Enhancing water quality and
moderating water shortage are nearly connected to the grey water
management. Laundry water is one type of gray water, which
consists of high concentrations of chemicals from soap powders as
well as bleaches, suspended solids and possibly oil, paints etc.
These have chemical oxygen demands (COD) values of 1200
20,000 mg/l, while laundries that wash items from households
and hotels contain efuents with COD values of 4001200 mg/l
(Ciabatti et al., 2009). The toxic effects of these pollutants are lis-
ted in Table 1. These pollutants are major alarming threaten to the
ecosystem and toxic to the humans (Gross et al., 2007).
Treating laundry water before its release into aquatic frame-
works therefore, signicantly add to ensuring the earth and en-
hancing general wellbeing and living states of groups. Thus proper
laundry wastewater treatments are mandatory to remove con-
taminants before its discharge into the environment. The major
n
Corresponding authors. Tel.: 91 431 2503118; fax: 91 431 2500133.
E-mail addresses: arthanaree10@yahoo.com (G. Arthanareeswaran),
fauzi.ismail@gmail.com (A. Ismail).
gulation, oatation, adsorption, chemical oxidation and biological
treatments (Kim et al., 2008). Coagulation and occulation tech-
niques are followed to facilitate the agglomeration of large parti-
cles. However, such methods have a drawback as ineffective in the
decolourisation of laundry efuent (Nicolaidis and Vyrides, 2014).
Another method such as chemical treatment has propensity of
generate waste, which require secondary unit operation steps.
Later, biological treatment was employed prior to chemical treat-
ment for the effective removal of COD (Nicolaidis and Vyrides,
2014). It requires a higher time for the reclamation.
Recently, effective treatment of industrial efuents as well as
ground water can achieve using membrane separation process.
Such membrane also paid in stringent regulation made by en-
vironmental agencies. The membrane separation process have
number of advantages over conventional methods including ful-
llment of higher standards, reducing environmental impact of
efuents, land requirements (Janpoor et al., 2011; Braeken et al.,
2004). Bhattacharyya (1987) attempted the treatment of laundry
wastewater using commercial ultraltration membrane. Ramon
et al. (2004) compared the ltration efciency of low load gray
water using ultraltration and nanoltration membranes. In ad-
dition, Ciabatti et al. (2009) employed an ultraltration membrane
and achieved an effective removal efciency of contaminants in
laundry efuent.

http://dx.doi.org/10.1016/j.ecoenv.2015.04.004
0147-6513/& 2015 Elsevier Inc. All rights reserved.

Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
ultraltration membranes. Ecotoxicol. Environ. Saf. (2015), http://dx.doi.org/10.1016/j.ecoenv.2015.04.004i
2 A. Sumisha et al. / Ecotoxicology and Environmental Safety ()

Table 1
Toxic effects of laundry water constituents.

Source of pollutants Effects References

Surfactant  The surfactants had both high or moderate toxicity and most toxic (mmol/L) Warne1 and Schifko (1999), Braga and Varesche (2011),
components. They contributed between 10.4% and 98.8% of the toxicity of the de- Morel and Diener (2006)
tergents with a mean contribution of 40.7%.

 Surfactants create a bacterial population rise, transmitting through the food chain
to protozoa, which are more sensitive to laundry wash toxins

 Linear alkyl benzene sulfonate (LAS) is the most widespread anionic surfactant and
its concentration may vary from 17 to 1024 ppm. It is derived from petroleum bi-
products, is quite rapidly degraded aerobically, but only very slowly or not at all
under anaerobic conditions. It generate carcinogenic and toxic by-products.

Detergents  All detergents will destroy sh mucus membranes and gills to some degree. The Zaneti et al. (2011)
gills may lose natural oils, interrupting oxygen transfer. Damaged mucus mem-
branes leave sh susceptible to bacteria and parasites. Detergents are toxic to sh
near 15 ppm, killing sh eggs at 5 ppm and cause endocrine disrupting and es-
trogenic effects in sh.

Oil/grease  Laundry water contains 835 mg/l of oil/grease. It adversely affect the esthetic ChristovaBoal et al. (1996), Brasino and Dangler (2007)
merit, water transparency and Dissolved Oxygen (DO) content in the water

However, the major disadvantage of membrane process is
fouling (Koh et al., 2005; Zhao et al., 2013). The general methods
required to overcome fouling are the modication of membrane
with hydrophilic additives and optimization of operating para-
meters. The process parameters such as transmembrane pressure
(TMP), stirring speed and cross ow velocity are help to enhance
the ux and improving the membrane performance (Mohammadi
et al., 2003; Sondhi et al., 2000).
Treatment of laundry water using ultraltration membranes
and its studies are limited. In this study, ultraltration membranes
were used for laundry wastewater treatment by optimizing the
parameters of transmembrane pressure and stirring speed for its
reuse and recovery. PVP modied PES membranes were compared
with commercial PES membrane with 10 kDa as a function of the
removal and ux performance of laundry wastewater. It is ex-
pected that the result of this work will provide suitable use of
laundry water for landscape irrigation in small communities and
households.
2. Materials and methods
2.1. Materials
earlier publication (Thuyavan et al., in press). Initially PES was
dried in a hot air oven at the temperature of 60 C for 8 h to re-
move moisture. The casting solutions were prepared by adding
PES and respective additives in DMF as solvent at room tempera-
ture. The casting solutions were stirred continuously for 4 h until
clear homogenous solutions were obtained. The solution then cast
onto the glass plate for the thickness of about 400 m with the
help of a thin lm applicator followed by evaporation for a period
of 30 s. The glass plate was immersed immediately into a distilled
water bath maintained at 20 C. The modied PES membranes
were cut into the required area corresponding to dead-end UF
experiments employed in this study. Later, synthesized mem-
branes were stored in 0.1% formalin solution.
2.3. Membrane water uptake capacity and porosity
Both modied and commercial membrane samples were cut
into 2 cm  2 cm size and immersed in distilled water for 24 h at
30 C. The weight of the wet membrane samples (W1) were cal-
culated after removing the surface water by blotting with tissue
paper. It was dried at a temperature of 75 C in an oven for 24 h
and again weighed (W2). The water uptake (%) was calculated by
(Srivastava et al., 2011)

Commercial grade Polyethersulfone (PES 3000) was purchased W1 W2

Water uptake (%) = 100
from M/s solvay chemicals India Ltd. and polyvinyl pyrollidone W1 (1)
(PVP) from M/s Central drug house, India Limited. The solvent
The porosity of the membranes was analyzed by considering
dimethyl formamide (DMF) was obtained from M/s Loba Chemie
the weight of membranes at dry and wet states. It was calculated
Pvt Ltd. Sodium Lauryl sulfate (SLS) were purchased from M/s.
Qualigens ne chemicals, India Ltd. The commercial membrane by the following equation (Gohari et al., 2013)
Polyethersulfone with 10 kDa molecular weight cutoff (MWCO) W1 W2
Porosity (%) = 100
was received from M/s Orelis Environmental SAS, France. w A l (2)

2.2. Membrane synthesis where, w density of water at room temperature (1 g/cm3); A

The modied membranes were fabricated by phase inversion
method using PES as base polymer and water as non-solvent. PVP
as modier was added in varying concentration of 5% and 10%. The
procedure for the membrane fabrication was followed by our
area of membrane (cm2); l thickness of wet membrane.
2.4. Ultraltration membrane process
The membrane ltration experiment was studied using a

Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
ultraltration membranes. Ecotoxicol. Environ. Saf. (2015), http://dx.doi.org/10.1016/j.ecoenv.2015.04.004i
 A. Sumisha et al. / Ecotoxicology and Environmental Safety () 3

pressure and stirring speed on laundry water ux has studied. The

permeate ux was measured by varying the transmembrane
pressure from 100 to 600 kPa and stirrer speed from 250, 500 and
750 rpm. The membrane efciencies in removing pollutants from
laundry wastewater are determined using Eq. (5).
Cp
R (%) = 1 100
Cf (5)

where R is the percentage rejection, Cf is the initial concentration

of feed and Cp is the permeate concentration. Unit used for each
parameter i.e. COD, TDS, turbidity and conductivity is mg/l, mg/l,
NTU and S/cm respectively. Analysis of COD of the sample and
Fig. 1. Dead-end mode ultraltration experiment setup. (1) Stirred ultraltration permeate solutions was performed according to titration method.
cell (2) Permeate (3) Magnetic stirrer (4) Selector; (5) Reservoir Turbidity analysis was conducted by using a Turbidity meter
(Model- Hach 2100 Q, India). The TDS and conductivity were
measured using conductivity meter (Eutech, Instruments PCD 650,
constant volume, variable pressure dead-end mode ultraltration
Singapore).
stirred cell (Model XFUFO76, Millipore, USA). Fig. 1 shows the
schematic diagram of the process. The membrane samples with
2.5. Fourier transform infrared spectroscopy (FTIR)
effective surface area of 37.5 cm2 cut into circular shape and placed
into the cell. Membranes were compacted in the ultraltration
A batch adsorption study was conducted to compare the
module using distlled water at the TMP of 500 kPa until a steady
binding efciency of efuent on both modied PES commercial
ux. During the compaction, the membrane structure was com-
PES 10 kDa. An airtight bottle lled with laundry water and small
pressed under a high transmembrane pressure difference to form
pieces of (2 cm  2 cm) membranes were kept in shaker for two
closer, denser and uniform pores resulting in the reduction of pore
days at 150 rpm. The presence of chemical functional groups over
size and ux (Chakraborty et al., 2003). Then the pure water ux
the membrane surface after the adsorption process was identied
( Jw1) of the membranes was determined using the following
by FTIR spectra (Model 2900, U.S). The scans for each membrane
equation. specimen were collected in the spectral range from 4000 to
V 400 cm  1.
Jw1 =
A t (3)

where Jw1 is the pure water ux in L/m2 h, V is the volume of water

3. Result and discussion
permeated in liters, A is the area of membrane in m2 and t is the
time for permeate collection in hours.
3.1. Pure water ux of membranes
The sample of wastewater collected from a laundry center lo-
cated in National Institute of Technology campus, Tiruchirappalli,
The membrane pore size and hydrophilicity are the two major
Tamilnadu, India. The efuents were analyzed with respect to
factors inuencing the pure water ux performance of mem-
chemical oxygen demand (COD), Total dissolved solids (TDS),
branes. Table 3 displays the properties of ultraltration mem-
conductivity and turbidity and characteristics of wastewater are branes PES(90%)/PVP(10%) (M1), PES(95%)/PVP(5%) (M2) and
shown in Table 2. Prior to feed of solution to the ltration module, commercial PES 10 kDa (M3) in terms of pure water ux, water
pure water ux ,. was measured at 500 kPa. The permeate ux of uptake capacity, porosity, contact angle and average pore radius
laundry wastewater was also calculated similarly to water ux in a (Thuyavan et al., in press). Among the modied membranes, PES
15 min interval of time using Eq. (3). with 10% PVP showed high water ux than PES with 5% PVP. It is
In order to calculate the antifouling characteristics of the due to the addition of PVP that affects the development of porous
membrane, the membranes were cleaned with 0.2 wt% sodium structure on the surface of membrane at the time of membrane
lauryl sulfate (SLS) solution by running it for 20 min after the fabrication. The M1 membrane has the higher average pore size of
treatment of laundry water. The pure water ux Jw2 was evaluated 19.2 nm when compared with M2 (7 nm). The similar increasing
again using Eq. (3). Then the ux recovery ratio (FRR) is calculated trend was observed for porosity of modied membranes. The
using Eq. (4) lower contact angle value (54) conrms hydrophilic property of
Jw2 membranes containing PES and PVP in ratio of 90/10 wt%. The
FRR = 100 polar amide group of PVP enhances the hydrophilic character of
Jw1 (4)
modied membranes and allows water to ow through the pores
where Jw1 and Jw2 are the water ux before and after the UF of the membrane owing to capillary forces (Liu et al., 2005). The
process. results of water uptake capacity also owing to the hydrophilic
The effect of operating parameters such as transmembrane character of modied PES membranes (Arthanareeswaran and
Starov, 2011). The membrane with higher concentration of PVP
Table 2 shows maximum water uptake capacity of 83.92% and it decreased
Characteristics of laundry waste water. to 78.9% as the PVP concentration decreased to 5%. This higher
water uptake and porosity of modied membranes offered the
Parameter Waste water
enhancement of laundry water ux. Whereas in the case of com-
pH 7.68 mercial PES 10 kDa membrane, all the properties except water ux
COD (mg/l) 753 were lower than modied membranes. However, overall proper-
Turbidity (NTU) 41.4 ties showed that modied membranes also hold a better water
Conductivity (S/cm) 1.2
TDS (mg/l) 603.3
ux and thus, it is expected to separate laundry efuent very
effectively.

Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
ultraltration membranes. Ecotoxicol. Environ. Saf. (2015), http://dx.doi.org/10.1016/j.ecoenv.2015.04.004i
4 A. Sumisha et al. / Ecotoxicology and Environmental Safety ()
Table 3
Properties of commercial and modied PES membranes
Membrane code Polymer and additive composition (17.5% Pure water ux
polymer) (82.5% solvent) (L/m2h)
PES (%) PVP (%)
M1 90 10 59.2
M2 95 5 54.84
M3 Commercial PES 10 kDa 108.21
3.2. Inuence of operating parameters
3.2.1. Effect of transmembrane pressure
To study the effect of transmembrane pressure on permeate
ux, experiment was conducted at different TMP ranging from 100
to 600 kPa and at constant stirring speed (250 rpm). The results
were illustrated in Fig. 2a and it is observed that the ux is in-
creasing with increase in the transmembrane pressure. The in-
crease in ux with TMP was due to higher driving force applied on
the membrane surface, which overcomes the membrane re-
sistance and the pressure drop of the solution on the membrane
surface (Datta et al., 2009; Arthanareeswaran and Thakur 2012). At
500 kPa, the ux was stabilized around 57.2, 50.8 and 46.3 L/m2h
for PES membrane M1, M2 and M3 respectively. However, beyond
500 kPa, solutes (detergents and surfactants) accumulate on
membrane surface and enhances the boundary layer formation
which causes blockage of inside pores by solutes. Hence the
permeate ux became independent of TMP and it was controlled
by mass transfer (Sarkar et al., 2009). A high ux of 57.2 L/m2h was
obtained for modied membrane of PES with 10% PVP at 500 kPa.
This is because of the high hydrophilic character of amide groups
in PVP, which improve of hydrophilicity on modied PES mem-
branes (Arthanareeswaran and Ananda Kumar, 2010).
3.2.2. Effect of stirring speed
Effects of stirring speed of 150, 500 and 750 rpm on permeate
ux was studied at 500 kPa and ux behavior of membranes are
shown in Fig. 2b. From Fig. 2b permeate ux of laundry waste
water was increased with increasing stirring speed in ultraltra-
tion. The enhanced turbulence of laundry waste water on mem-
brane surface in ultraltration with stirring speed was reduced the
formation of cake layer on surface of the membrane. The possible
causes of higher permeate ux at 750 rpm stirring speed and it
takes solutes away from the membrane surface and bulk layers
concentration increased in ultraltration system. Which results a
decrease in concentration polarization and fouling and lead to
increase in permeate ux (Datta et al., 2009). In addition, PES
membranes with 10 wt.% of PVP shows maximum ux at a speed
of 750 rpm. This also supports the effect of PVP on hydrophilicity
and porous structure of the modied membrane. The minimum
ux of commercial PES membrane is due to its high hydro-
phobicity and it leads to the adsorption of contaminants on the
membrane surface and cause fouling.
3.2.3. Constant pressure ltration
The membrane permeability with respect to time at 500 kPa
and 750 rpm of stirring speed is illustrated in Fig. 2.c. The
permeate ux was higher for initial period and gradually declined
after 2 h of ultraltration. The rapid ux decline for membranes
M2 and M3 is due to the contaminants present in the laundry
wastewater, which plugged the pores of the membrane and forms
concentration polarization layer on the surface. This layer causes
total resistance to the uid ow through modied membranes.
The variation in the ux of modied membrane M1 is due to the
Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
ultraltration membranes. Ecotoxicol. Environ. Saf. (2015), http://dx.doi.org/10.1016/j.ecoenv.2015.04.004i
Contact angle Water uptake capa- Porosity(%) Avg. pore radius (FRR) (%)
(degrees) city (%) (nm)
54 83.92 46.7 19.2 59
63 78.9 38.5 7 54
70.1 54.3 24.3 6.1 38.8
higher porosity and hydrophilicity by addition of PVP and gives
better performance including less fouling, than neat commercial
PES membrane. FRR is an important parameter used to measure
the antifouling characteristic of membranes. Table 3 represents the
ux recovery ratio along with water ux. From Table 3, It is in-
dicated that the FRR value increased from 38.8% to 59% for com-
mercial PES membrane and 10% PVP added in PES membrane re-
spectively. For membrane with 5% PVP had a 54% ux recovery,
which was higher than that of commercial membrane. This high
FRR value of modied PES is due to the surface modication of
membrane with PVP, which retard the adsorption of solute on the
membrane surface and increases the antifouling property of the
membrane. The low FRR value commercial PES membrane with
10 kDa indicates that water washing with pure water after
permeate ux is ineffective due higher adsorption of detergents
and surfactants on membrane surface.
3.2.4. Rejection efciency of membrane
Fig. 3.a. represents the separation efciency of the membranes
for the treatment of laundry wastewater. The ultraltration pro-
cess is carried out under a controlled pressure of 500 kPa and a
stirring speed of 750 rpm. The efuent is characterized with re-
spect to COD, TDS, turbidity and conductivity. COD values mea-
sures the quality of laundry wastewater as it contain organic
matters and reducing substances.
The PES membrane with 10% addition PVP attained 88% of COD
removal. However, PES membrane with 5% addition PVP attained
85% of removal efciency. The commercial PES membrane with
10 kDa had 83% of removal efciency. Laundry water is containing
detergents, carbonate and bicarbonate in wash water. In the wash
water bicarbonate level was signicantly increased with the use of
powder detergents. The laundry waste water collected was the use
of powder detergents. The rejection is brought down in commer-
cial PES 10 kDa membrane and it might be due to the higher ad-
sorption of solutes (bicarbonate) on the membrane surface. In
addition, modied membranes greatly removed turbidity with
greater than 90% removal efciency. In this case, PES with 10% PVP
achieved appreciable separation of 98% turbidity followed by PES
(95%)- PVP(5%) and commercial membrane with removal ef-
ciency of 96% and 93% respectively. PVP is a water-soluble polymer
and due to the micro Brownian motion of the polymeric segments
resulting in an increase of DMF solubility in polymer casting so-
lution. Under the inuence of the solubility a solvent (DMF/PVP)
poor phase and polymer (PES) rich phase takes place in different
order within the membranes structure that inuences the rejec-
tion of laundry water. The total dissolved solids (TDS) were also
removed signicantly. The removal efciency of 82%, 81% and 79%
were obtained respectively for PES-10% PVP, PES-5% PVP and PES-
10 kDa. The PES membrane with 10 wt% PVP had better rejection
efciency of chemical contamination from detergents during the
washing of clothes which can useful to minimize water pollution
and protect our health.
3.2.5. FTIR
The FTIR spectra of modied and neat commercial PES
 A. Sumisha et al. / Ecotoxicology and Environmental Safety () 5

Fig. 3. (a) Separation efciency of membrane in treating laundry wastewater, M1:

PES(90%)/PVP(10%); M2: PES (95%)/ PVP(5%); M3: PES- 10 kDa. (b) FTIR spectra of
membranes after adsorption.

membranes after adsorption have shown in Fig. 3b. The carbox-

ylates groups were present in laundry wastewater shows peaks in
the range of 15501610 cm  1 wave number. Both commercial
membrane and membrane with 5% PVP show the same peak at the
wave number of 1577 and 1576.9 cm  1 respectively. In the case of
PES (90%)-PVP(10%) the peak corresponding to carboxylate group
is vanished. Similarly, C CH2 groups are present in three mem-
branes at the wave number of 800900 cm  1 with different in-
tensities. It shows that adsorption carboxylate group from laundry
waste water in surface of the membrane

4. Conclusion

The performances of PES modied membranes with addition of

Fig. 2. (a) Effect of transmembrane pressure on permeate ux. (b) Effect of stirrer
speed on permeate ux for different membranes at constant pressure 500K Pa, M1:
PES(90%)-PVP(10%); M2: PES(90%)-PVP(10%); M3: PES- 10 kDa (c) Permeate ux of
membranes operated at 500 KPa.
5 and 10 wt% of PVP were compared with commercial PES mem-
brane with 10 kDa for the treatment of laundry wastewater. The
effect of variation of operating parameters such as transmembrane
pressure and stirring speed on permeate ux was also studied. The
experimental results shows that by increasing stirring speed and
TMP can enhance the permeate ux. The COD, TDS and turbidity of
laundry wastewaters was appreciably removed by ultraltration

Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
ultraltration membranes. Ecotoxicol. Environ. Saf. (2015), http://dx.doi.org/10.1016/j.ecoenv.2015.04.004i
6 A. Sumisha et al. / Ecotoxicology and Environmental Safety ()
through modied PES membranes. The laundry wastewaters pol-
luted by addition detergents, which causes water pollution with
dissolving of carbonate and bicarbonate. The modied PES mem-
brane with 10 wt% PVP can apply successfully to treat laundry
waste water to minimize chemical contamination of water.
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