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Resources, Conservation and Recycling 44 (2005) 185196

Laundry wastewater treatment using coagulation


and membrane filtration
a , I. Petrini

S. Sostar-Turk
ca, , M. Simonicb
a

Faculty of Mechanical Engineering, Institute of Textile, University of Maribor,


Smetanova ulica 17, SI-2000 Maribor, Slovenia
b Faculty of Chemistry and Chemical Engineering, University of Maribor,
Smetanova ulica 17, SI-2000 Maribor, Slovenia
Received 3 November 2003; accepted 22 November 2004

Abstract
This paper presents the results obtained from laundry wastewater treatment using conventional
methods namely precipitation/coagulation and the flocculation process with adsorption on granularactivated carbon (GAC) and an alternative method, membrane filtrations, namely ultrafiltration (UF)
and reverse osmosis (RO). Chemical analyses showed that parameter values of untreated wastewater
like temperature, pH, sediment substances, total nitrogen and phosphorous, COD, BOD5 , and the
amount of anion surfactants had been exceeded in regard to Slovenian regulation. These regulations
can be used as requirements for wastewater reuse and make treated wastewater an available source
for the existing water supply.
The study of conventional treatment was based on a flocculation with Al2 (SO4 )3 18H2 O and adsorption on GAC. Membrane filtrations were studied on a pilot wastewater treatment plant: ultrafiltration
(UF) and reverse osmosis (RO) units. The membranes used in this experiment were ceramic UF membrane and spiral wounded polyethersulfone RO membranes. The quality of the wastewater was
improved by both methods and the specifications of a concentration limit for emission into water were
confirmed. The disadvantage of GAC is that there is no possibility of any kind of selection, which
is essential for recycling and re-use, while permeate coming from RO met the required regulation as
well as requirements for reusing in washing process. However, the economical analyses showed that
the membrane filtrations are more expensive compared to the GAC treatment process.
2004 Elsevier B.V. All rights reserved.
Keywords: Laundry wastewater; Chemical analyses; Coagulation; Membrane filtration; Pilot plant

Corresponding author. Tel.: +386 2 220 7906; fax: +386 2 220 7990.
E-mail address: irena.petrinic@uni-mb.si (I. Petrinic).

0921-3449/$ see front matter 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.resconrec.2004.11.002

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1. Introduction
Laundering processes, including water-washing processes and dual-phase washing, use
significant amounts of water. The cleanliness obtained when laundering is the result of synergistic actions between the so-called Sinner parameters, these being mechanical energy,
chemical energy, thermal energy and time. These factors have to perform a simple separation process in which soil is removed from a textile substrate (Warmoeskerken et al., 2002).
Bleach, water softeners and surfactants are the most important ingredients of laundry detergents (Jakobi and Lohr, 1987). The concentration, type, and amounts of chemicals added
during the water-washing process depend on the type of cleaned items, and the degree
to which the items are soiled. Surfactants have the unique ability to remove both watersoluble and non-water-soluble soils. One end of the surfactant molecule (the lipophilic or
oil-loving end) penetrates oily soils, whilst the opposite end of the molecule (the hydrophilic
or water-loving end) solubilizes the oils. This action loosens soils and disperses them in the
water.
As environmental regulations tighten, concern increases about reducing the surfactant
concentration in effluent streams. It has been reported that the wastewater from a laundry,
where very dirty items are being washed, contains mineral oils, heavy metals and dangerous
substances that have COD values of 120020,000 mg O2 /L. The wastewater from hospitals
contains fat, the remains of food, blood and urine that have COD values of 4001200 mg
O2 /L. Laundries washing items from households and hotels, pollute water with COD values
from 600 to 2500 mg O2 /L (Gosolits et al., 1999).
The most widely used systems for laundry wastewater treatment are conventional methods; such as precipitation/coagulation and flocculation, sedimentation and filtration or combination of these. Coagulation and flocculation aids are usually added to facilitate the formation of large agglomerated particles (EPA, 2000). These systems remove color insufficiently
and are clearly ineffective in decolourising laundry effluents, even when mixed and treated
together with sewage. Adsorption on the granular activated carbon (GAC) after the process
of flocculation can improve the treatment due to the large surface area that allows carbon
to adsorb a wide range of compounds. However, the level of color removal depends on the
dye type (Faria et al., 2004).
Membrane processes offer a number of advantages over conventional water and wastewater treatment processes including fulfillment of higher standards, reducing environmental
impact of effluents, land requirements and the possibility to use mobile treatment units.
Bhattacharyya et al. (1987) showed that the recycled ultrafiltrate from laundry and shower
wastewater could be used as non-potable water. Ahn and Song (1990) reported that physically filtered wastewater with various types of ceramic membranes from a resort complex
can be used effectively in creating recycled wastewater for such secondary purposes. Industrial laundries have a variety of opportunities to recycle/reuse water at their facilities (EPA,
2000).
The main problems in practical applications of membrane filtrations are the reduction
of permeate flux with time, caused by the accumulation of feed components in the pores
and on the membrane surface (Mulder, 2000). Membrane fouling involves specific interaction between the membrane or adsorbed solutes and other solutes in the feed stream
and it is characterized by an irreversible and time dependent decline in flux. Membrane


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187

needs proper feed pre-treatment and a well-developed cleaning protocol because fouling
can directly influence on membrane lifecycle costs. In a wastewater treatment, polymer
membranes have wider usage due to their lower price. However, there are limitations in
chemical, thermal and mechanical stability. For this reason, when treating wastewater from
industrial laundry, the ceramic UF membrane was used as a pre-treatment stage for RO
membrane.
The authors performed several experimental investigations concerning laundry wastewater purification (Petrinic et al., 2002, 2003). This paper includes the results of laboratory
trials on wastewater using:
conventional methods: precipitation/coagulation, flocculation and adsorption on active
carbon and
membrane filtrations: UF and RO processes.
Based on recommendation and good results achieved when treating the wastewater from
metal, textile and electronic component industry, the membrane system described in the
paper was introduced to laundry industry in Slovenia. The investments and operating costs
of membrane filtrations were estimated and compared to those of GAC.
2. Materials and methods
2.1. Laundry wastewater description
The composition of the laundry wastewater is shown in Table 1.
The measured parameters for the laundry wastewater were chosen according to the
Slovenian regulation called Decree of substance emission during removal of wastewater
from laundry and dry cleaning (Official Gazette of the Republic of Slovenia, 2002) as well
as their concentration limits of emission into water. These regulations meet the requirements
for wastewater reclamation and reuse and make it an available source for the existing water
supply.
It can be seen that the values of some parameters exceeded the outflow limit value in the
water. The exceeded parameters were: temperature, pH, sediment substances, total nitrogen
and phosphorous, COD and BOD5 , and the amount of anion surfactant. It is known, that
the presence of anionic surfactant, builder and other oil substances in the wastewater could
increase the COD concentration (Seo et al., 2001). The washing flow was 200 L/h, eight
hours per day from Monday to Friday. The wastewater was colored (green). Thus, the
wastewater treatment was needed to fulfill the regulation standards.
2.2. The washing process
Wastewater was taken from the laundry that washes hospital clothes using a tunnel washer
(type Senking, Jensen Group, Denmark). Tunnel washer is shown in Fig. 1 and consists of
12 modules. The laundry items pass automatically from one module to the next. The effluent
was collected from the third cell and used as feed. Water consumption for the prewash and
main wash was 5 L/kg (cells 19) and for rinsing process, 8 L/kg (cells 912).

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Table 1
Parameters of wastewater, standard procedure, methods and concentration limit of emission in water
Parameter

Wastewater

Temperature ( C)
pH-value

62
9.6

Suspended substances (mg/L)


Sediment substances (mL/L)
Cl2 (mg/L)
Total nitrogen (mg/L)
Nitrogen ammonia (mg/L)
Total phosphorus (mg/L)
COD (mg O2 /L)
BOD5 (mg O2 /L)

Standard

Method/apparatus

30
6.59.0

DIN 38404-C4
SIST ISO 10523

35

80

ISO/DIN 11923

2
<0.1
2.75
2.45

0.5
0.2
10
5

DIN 38409-H9
ISO 7393/2
SIST EN 25663
SIST ISO 6778

9.9

1.0

/thermometer
Electrochemical/pH-meter
Iskra MA 5740
Gravimetrical/weighing machine Mettler AE 100
Sedimentation
Reagent DPDcolourmetric
Titrimetric
Spectrophotometer/PerkinElmer Cary 1E
Spectrophotometer/PerkinElmer Cary 1E
Titrimetric
Electrochemical/oximeter
WTW
Gravimetrical/weighing machine Mettler AE 100
Colourmetric/DX-200
Dorhmann
Spectrophotometer/PerkinElmer Cary 1E

280
195

Mineral oil (mg/L)

4.8

AOX (mg/L)

0.12

Anionic surfactant (mg/L)

Concentration
limit of
emission into
water

SIST ISO 6878-1

200
30

SIST ISO 6060


SIST ISO 5815

10

DIN 38409-18

10.1

0.5

SIST ISO 9562

1.0

SIST ISO 7875-1

2.3. Description of conventional plant


Water was flocculated with 5 mg/L of Al3+ added as Al2 (SO4 )3 18H2 O. After 20 min
the water was filtered through silicic sand (Puconci, Slovenia) in a column with a diameter

Fig. 1. Tunnel washer.


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189

of 3.2 cm, the height of the sand layer was 1 m, the velocity of filtration was 10 m/h, the
granulation of sand grains was 0.52 mm and the contact time was 6 min. The filtrate was
adsorbed on GAC in a column, with a diameter of 3.2 cm, the height of the GAC layer was
1 m, the velocity of filtration was 5 m/h, the granulation of GAC was 1 mm and the contact
time was 12 min. The GAC (type Chemviron F-400, Belgium) made from selected grades
of coal to produce a high-density, durable granular carbon product with high internal surface
area up to 1200 m2 /g.
2.4. Description of the membrane pilot plant
UF and RO trials were carried out on a pilot scale. For UF a tubular module with ceramic
membrane was used. The membrane was 25.4 mm in diameter and 900 mm in length. This
membrane is a multi-channel membrane with an active surface layers made of Al2 O3 , TiO2
and ZrO2 . It has a filtrating surface area of 0.13 m2 . The nominal molecular cut-off size of
the membrane was from 20400 kDa (nominal pore diameter of 0.05 m). Figs. 2 and 3
show the test equipment.
The wastewater was poured into storage tank 1 from where it was pumped into the
UF module. The retentate circled back into the storage tank under pressure of 45 bar,
while the permeate was collected in the storage tank 2. The permeate flow velocity was
1520 m/s. Back-flushing was achieved by using pressurized air to push small amounts of
permeate through the membrane every 3 min. The pressure of the back-flushing air was
68 bar.

Fig. 2. The equipment for ultrafiltration.

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Fig. 3. The equipment for reverse osmosis.

The permeate from UF unit was introduced into the RO system from where it was
pumped under pressure of 12 bar through a prefiltration unit. The feed was then pumped
under high-pressure of 2030 bar into the spiral-wound module from where the permeate
was collected into a storage vessel, while the retentate was recycled into the feed tank. The
membrane used for the tests was made from polyethersulfone material with filtering surface
area of 1.5 m2 .
The equipment and the membrane have been cleaned with 1% Ultrasil (Ecolab, USA)
solution after filtrations. After washing, the membrane was rinsed three times with the tap
water and once with the demineralised tap water.

3. Results and discussion


3.1. Coagulation and adsorption
Analyses (Table 2, third column) show that coagulation alone could not remove anionic surfactant from wastewater, COD removal was only 36% and BOD only 51%. This
is why after coagulation, adsorption on GAC was also needed. The graphite structure
gives the carbon a very large surface area, which allows the carbon to adsorb a wide
range of compounds. Activated carbon has the strongest physical adsorption forces or the
highest volume of adsorbing porosity. The water after the GAC treatment was analyzed.
Table 2 shows the effects of GAC filtration. After GAC treatment, COD removal was 93%,
both BOD5 and anionic surfactants removals were 95%. Table 2 shows that all measured


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191

Table 2
The determination of parameters in the wastewater before and after treatment with coagulation
Parameter

Wastewater

Temperature ( C)
62
pH-value
9.6
Suspended substances (mg/L) 35
Sediment substances (mL/L)
2
Cl2 (mg/L)
<0.1
Total nitrogen (mg/L)
2.75
Nitrogen ammonia (mg/L)
2.45
Total phosphorus (mg/L)
9.9
COD (mg O2 /L)
280
195
BOD5 (mg O2 /L)
Mineral oil (mg/L)
4.8
AOX (mg/L)
0.12
Anionic surfactant (mg/L)
10.1

Measured values
in wastewater
after coagulation
22
7.9
<5
<0.5
<0.1
2.60
2.40
1.0
180
100
2.5
0.12
10.0

Measured values
in wastewater
after coagulation
and active carbon
22
6.8
<5
<0.5
<0.1
2.60
2.30
1.0
20
10
<1
<0.1
<0.5

Concentration
limit of emission
into water
30
6.59.0
80
0.5
0.2
10
5
1.0
200
30
10
0.5
1.0

parameters were below the concentration limit of emission into water after GAC wastewater
treatment.
3.2. Pilot scale investigations of UF and RO processes
Correlation of flux decline with time was conducted to obtain preliminary information
about fouling tendency of the membrane. The behavior of the permeate flux as a function
of the operation time was studied.
From Fig. 4, it can be seen that the UF permeate flux appears very stable with the operating
time. Flux versus time experiments for UF unit was performed at optimum transmembrane
pressure (35 bar). This indicates that fouling is not a problem on the UF system during
150 min operation. During the UF, the temperature increased again (54 2 C) due to the

Fig. 4. Flux vs. time for UF.

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Fig. 5. Flux vs. time for RO.

working conditions, and therefore, more favourable permeation rates can be achieved due to
the decrease in viscosity (Mallevialle et al., 1996). Permeate flux was expressed as volume
per unit membrane area per unit time, e.g. Lm2 h1 (LMH).
Results of analyses of wastewater showed that the temperatures can be up to 80 C,
the pH value is between 9 and 11 as well as the presence of some oxidants like chlorine
ions has been determined. In that case, usage of ceramic membranes is recommended because polymer membranes such as polyamide membranes can be chemically damaged.
However, the dechlorination of the feed before it enters the membrane system should still
be used. The most popular methods are carbon sorption or the addition of sodium bisulphite or gaseous sulphur dioxide for removal of chlorine from the effluent (Wakeman,
2001).
From the Fig. 5, it can be seen that no fouling was presented at the RO unit, neither.
The performance was stable; the purity and the consistency of the cleaned wastewater were
maintained.
3.3. Membrane ltrations
Chemical analyses were carried out on samples of wastewater, ultrafiltration and reverse
osmosis permeate (Table 3). Concentrated water volume discharged is 20% of the treated
one.
All measurements were done in the laboratory at room temperature, 25 C. Adequate
total phosphorous was obtained after ultrafiltration. The COD, BOD5 , mineral oil, AOX and
anionic surfactant was not reduced enough, so the reverse osmosis step was necessary. The
ultrafiltration step, however, guaranteed a good performance and duration of reverse osmosis
membrane. The RO permeate had good analytical characteristics, almost all total anionic
surfactant (99.2%) and all organic content was removed. The COD value was reduced by up
to 98.9%, BOD5 up to 99.2% and mineral oil up to 75%. Almost complete color removals
were achieved with the RO membrane.
The quality of the permeate produced by the RO module fed on the UF permeate was
satisfactory and acceptable for water reuse in the laundry industry.


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193

Table 3
The determination of parameters in the wastewater before and after treatment with membrane technology
Parameter
Temperature ( C)
pH-value
Suspended substances (mg/L)
Sediment substances (mL/L)
Cl2 (mg/L)
Total nitrogen (mg/L)
Nitrogen ammonia (mg/L)
Total phosphorus (mg/L)
COD (mg O2 /L)
BOD5 (mg O2 /L)
Mineral oil (mg/L)
AOX (mg/L)
Anionic surfactant (mg/L)

Wastewater
62
9.65
35
2
<0.1
2.75
2.45
9.92
280
195
4.8
0.12
10.06

Permeate UF
53.8
8.3
18
<0.5
<0.1
0.03
0.03
0.46
130
86
4.4
0.11
7.20

Permeate RO
27.8
7.62
8
<0.5
<0.1
0.03
0.03
0.14
3
1.5
1.2
0.08
0.91

Concentration limit of
emission into water
30
6.59.0
80
0.5
0.2
10
10
2.0 (1.0)
120
25
10
0.5
1.0

3.4. Economical analyses


Economic considerations can be drawn to foresee the economical feasibility of the implementation of both mentioned methods for a large-scale plant of 200 m3 /day. Data needed for
simulation was obtained from laboratory experiments using actual wastewater. The costs for
both techniques are based on operation costs quoted by suppliers for a full-scale treatment
plant and are reported in Table 4.
When comparing investment costs between the two kinds of water purification, GAC
seems much more promising. In our case, membranes exhibited poor economics compared
to GAC, when analyzing the total annual costs. However, due to the increasing requirements
for effluent quality and increasing fees for wastewater discharge, the need for water reuse is
increasing. Recycling of water using membrane filtrations is sustainable and environmentally friendly, because only 25% of effluent water ends in the environment and about 75%
is recycled. This means 46,800 m3 of water per year is saved which saves around 50,000
euros. Furthermore, in GAC after the flocculation process, the wastewater goes through
carbon column to remove residual color, soluble salts and surfactants. Membrane filtration
uses no carbon and produces low quantities of waste unlike GAC with 17 tons of waste
production per year.
If 75% of the water is recycled, the membrane filtration would still be around 50% more
expensive then GAC method. The main reason for that is the usage of ceramic UF membrane.
Ceramic membranes are considerably more expensive and are approximately 10 times more
expensive than polymer membranes. Ceramic UF membranes have life expectancy of 10
years and the polymer membranes 3 years. There are several reasons for use of ceramic
UF including lower chemical requirements, superior quality of the produced water and
implementation of higher standards. Today, membrane ceramic module with an area of
10.7 m2 costs 10,000 euros. It is expected that this price will drop to 5500 euros per module
mainly due to two factors: the increase of membrane surface area per module and the mass
production of membrane modules.

194

Total
GAC
Cost of plant (investment
in 10 years)
Energy
Chemicals
Membrane replacement (change
every 3 years for RO plant)
Man work
Waste deposit
Total

Annual
Membrane
plant

GAC

Cost per m3

% of total
Membrane
plant

GAC

Membrane
plant

GAC

Membrane
plant

69600

390000

6960

39000

31

46

0.11

0.63

28800

15000

1060
2880

25200
10000
5000

5
13

30
12
6

0.02
0.05

0.4
0.16
0.08

10500

10200
1050

5000

46
5

0.16
0.17

0.08

108900

405000

22150

84200

100

100

0.51

1.35

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Table 4
Investment and operating costs (evaluated in euro) for UF/RO membrane treatment of 200 m3 /day or 62 400 m3 /year (full-scale plant)


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et al. / Resources, Conservation and Recycling 44 (2005) 185196

195

Although the costs of membrane systems are higher than conventional treatment systems,
their application is suitable if the costs of land and water supply are very high.
3.5. Market analyses
The ecological and technological standards for modern laundry wastewater treatment

were enforced, within the two projects carried out (Sostar-Turk


et al., 2000; Sostar-Turk
et
al., 2003). The potential market within Slovenia was analyzed for membrane water treatment
applications. It was discovered, that out of 140 Slovenian laundries most use conventional
methods for wastewater treatment such as flocculation, sedimentation and filtration. Only
three laundries with water flows between 35,000 and 45,000 m3 per year had ultrafiltration,
which does not allow closed loops, been introduced in addition to conventional treatment.
For this reason, membrane treatment consisting of ultrafiltration followed by reverse osmosis
was performed in laboratory. This system allows up to 75% of the water to be recycled. In
Slovenia there are ten potentional laundries where such a system would be remunerative,
five of them having water flow between 35,000 m3 up and 100,000 m3 per year.
In addition, a bilateral research project is being carried out between Slovenia and Croatia

(Sostar-Turk
et al., 2002). Presently, market analysis is taking place in Croatia, similar to that
carried out in Slovenia four years ago. This country is a very interesting tourist destination
because of the long Adriatic coastline with lots of hotels, restaurants, hospitals, where
among others, laundry goods need to be washed. It is already known that their legislation
did not demand any laundry wastewater treatment at all yet.
4. Conclusions
A study of the possibility for wastewater reuse is essential because of its large quantities
in the laundering process of industrial laundries. Laundry wastewater possesses the potential
for reclamation and reuse. Such reclamation and reuse of laundry discharge is important to
save water supply and significantly improve urban environments.
Good results were achieved using the conventional methods. These methods are especially effective in the case of minimizing the organic pollutants to the point where wastewater is drained into municipal sewage or directly into a water. The disadvantage is that
there is no possibility of any kind of selection, which is essential for recycling and re-use.
The consumption of chemicals can be reduced because of better separation characteristics
of membranes compared to the coagulation and adsorption methods. No coagulators and
active carbons are used for membrane filtration. Decreased sludge production has positive ecological effects. However, membrane filtration is more expensive compared to the
GAC treatment process. Widespread use of membranes will depend on the availability of
significantly cheaper membranes, or the tightening of regulatory standards.
Acknowledgements
We are thankful to the European Commission for its financial support in preparing this
paper, through a grant from EU project EKV1-CT-2000-00049.

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et al. / Resources, Conservation and Recycling 44 (2005) 185196

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