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Ecotoxicology and Environmental Safety ()

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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
Membrane Research Laboratory, Department of Chemical Engineering, National Institute of Technology, Tiruchirappalli 620015, India
Advanced Membrane Research Center (AMTEC), UniversitiTeknologi Malaysia (UTM), Skudai 81310, Johor, Malaysia
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
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
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-

gulation, oatation, adsorption, chemical oxidation and biological
The three major fundamental concerns of current and future treatments (Kim et al., 2008). Coagulation and occulation tech-
water resources are lack of water, poor water quality and water niques are followed to facilitate the agglomeration of large parti-
related debacles (UNESCO, 2003). Enhancing water quality and cles. However, such methods have a drawback as ineffective in the
moderating water shortage are nearly connected to the grey water decolourisation of laundry efuent (Nicolaidis and Vyrides, 2014).
management. Laundry water is one type of gray water, which Another method such as chemical treatment has propensity of
consists of high concentrations of chemicals from soap powders as generate waste, which require secondary unit operation steps.
well as bleaches, suspended solids and possibly oil, paints etc. Later, biological treatment was employed prior to chemical treat-
These have chemical oxygen demands (COD) values of 1200 ment for the effective removal of COD (Nicolaidis and Vyrides,
2014). It requires a higher time for the reclamation.
20,000 mg/l, while laundries that wash items from households
Recently, effective treatment of industrial efuents as well as
and hotels contain efuents with COD values of 4001200 mg/l
ground water can achieve using membrane separation process.
(Ciabatti et al., 2009). The toxic effects of these pollutants are lis-
Such membrane also paid in stringent regulation made by en-
ted in Table 1. These pollutants are major alarming threaten to the
vironmental agencies. The membrane separation process have
ecosystem and toxic to the humans (Gross et al., 2007). number of advantages over conventional methods including ful-
Treating laundry water before its release into aquatic frame- llment of higher standards, reducing environmental impact of
works therefore, signicantly add to ensuring the earth and en- efuents, land requirements (Janpoor et al., 2011; Braeken et al.,
hancing general wellbeing and living states of groups. Thus proper 2004). Bhattacharyya (1987) attempted the treatment of laundry
laundry wastewater treatments are mandatory to remove con- wastewater using commercial ultraltration membrane. Ramon
taminants before its discharge into the environment. The major et al. (2004) compared the ltration efciency of low load gray
water using ultraltration and nanoltration membranes. In ad-
Corresponding authors. Tel.: 91 431 2503118; fax: 91 431 2500133.
dition, Ciabatti et al. (2009) employed an ultraltration membrane
E-mail addresses: (G. Arthanareeswaran), and achieved an effective removal efciency of contaminants in (A. Ismail). laundry efuent.
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),
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 earlier publication (Thuyavan et al., in press). Initially PES was
fouling (Koh et al., 2005; Zhao et al., 2013). The general methods dried in a hot air oven at the temperature of 60 C for 8 h to re-
required to overcome fouling are the modication of membrane move moisture. The casting solutions were prepared by adding
with hydrophilic additives and optimization of operating para- PES and respective additives in DMF as solvent at room tempera-
meters. The process parameters such as transmembrane pressure ture. The casting solutions were stirred continuously for 4 h until
(TMP), stirring speed and cross ow velocity are help to enhance clear homogenous solutions were obtained. The solution then cast
the ux and improving the membrane performance (Mohammadi onto the glass plate for the thickness of about 400 m with the
et al., 2003; Sondhi et al., 2000). help of a thin lm applicator followed by evaporation for a period
Treatment of laundry water using ultraltration membranes of 30 s. The glass plate was immersed immediately into a distilled
and its studies are limited. In this study, ultraltration membranes water bath maintained at 20 C. The modied PES membranes
were used for laundry wastewater treatment by optimizing the were cut into the required area corresponding to dead-end UF
parameters of transmembrane pressure and stirring speed for its experiments employed in this study. Later, synthesized mem-
reuse and recovery. PVP modied PES membranes were compared branes were stored in 0.1% formalin solution.
with commercial PES membrane with 10 kDa as a function of the
removal and ux performance of laundry wastewater. It is ex-
2.3. Membrane water uptake capacity and porosity
pected that the result of this work will provide suitable use of
laundry water for landscape irrigation in small communities and
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
2. Materials and methods
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
2.1. Materials (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

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

Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
ultraltration membranes. Ecotoxicol. Environ. Saf. (2015),
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 Contact angle Water uptake capa- Porosity(%) Avg. pore radius (FRR) (%)
polymer) (82.5% solvent) (L/m2h) (degrees) city (%) (nm)

PES (%) PVP (%)

M1 90 10 59.2 54 83.92 46.7 19.2 59

M2 95 5 54.84 63 78.9 38.5 7 54
M3 Commercial PES 10 kDa 108.21 70.1 54.3 24.3 6.1 38.8

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

Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
ultraltration membranes. Ecotoxicol. Environ. Saf. (2015),
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

5 and 10 wt% of PVP were compared with commercial PES mem-
brane with 10 kDa for the treatment of laundry wastewater. The
Fig. 2. (a) Effect of transmembrane pressure on permeate ux. (b) Effect of stirrer effect of variation of operating parameters such as transmembrane
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
pressure and stirring speed on permeate ux was also studied. The
membranes operated at 500 KPa. 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),
6 A. Sumisha et al. / Ecotoxicology and Environmental Safety ()

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Please cite this article as: Sumisha, A., et al., Treatment of laundry wastewater using polyethersulfone/polyvinylpyrollidone
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