Separation and Purification Technology 22-23 (2001) 519– 528

www.elsevier.com/locate/seppur

Mechanisms of retention and flux decline for the

nanofiltration of dye baths from the textile industry
B. Van der Bruggen *, B. Daems, D. Wilms, C. Vandecasteele
K.V. Leu6en, Department of Chemical Engineering, W. de Croylaan 46, 3001 He6erlee, Belgium

Abstract

Removal of dye compounds from colour baths used in the textile industry is a possible application of nanofiltra-
tion. However, the mechanisms involved in this process are not clearly understood and the practical application of
the process is facing many problems such as fouling and flux decline. The mechanisms of retention and flux decline
were examined using two different approaches. Firstly, synthetic dye baths were prepared according to manufacterer’s
recipes. Retention of two reactive dyes (reactive blue 2 and reactive orange 16) was studied in separate baths and with
different concentrations of Na2SO4, Na2CO3, NaOH and a surfactant. Different nanofiltration membranes (UTC-60,
NF70 and NTR 7450) were used. The water flux in each of the experiments was monitored. It was found that the
retention of ions decreased with the ion concentration due to a decrease of the Donnan potential. The retention of
the dyes was high and was not influenced by the dye concentration or the ionic strength. The water flux was
dependent of the ion concentration in the feed solution: high ion concentrations caused a dramatic decrease of the
water flux. The dye concentration in the bath was found to have only a minor influence, whereas surfactants did not
change water flux or dye retention. A theoretical explanation for these effects is given. The phenomenon of flux
decline limits strongly the applicability of nanofiltration for direct treatment of dye baths. In a second step, an
industrial wastewater from a textile factory was treated biologically in an active sludge system. The effluent was used
as feed for nanofiltration with the same membranes as in the first step. The overall results for these experiments were
satisfactory. The ion concentration was much lower than in the earlier experiments due to mixing of different feed
streams. Therefore, the water fluxes were not considerably lower compared with the clean water fluxes. The retentions
were sufficiently high to make recirculation of the treated water possible, thereby providing a considerable saving of
water. © 2001 Elsevier Science B.V. All rights reserved.

Keywords: Nanofiltration; Dye baths; Textile industry; Wastewater treatment

Nomenclature

Aƒ constant= 1.8246 × 106/(mT)3/2 (if the solvent is water)

B parameter in Pitzer model

* Corresponding author. Tel.: + 32-16-322726; fax: + 32-16-322991.

E-mail address: bart.vanderbruggen@cit.kuleuven.ac.be (B. Van der Bruggen).

1383-5866/01/$ - see front matter © 2001 Elsevier Science B.V. All rights reserved.
PII: S 1 3 8 3 - 5 8 6 6 ( 0 0 ) 0 0 1 3 4 - 9
520 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528

B ƒMX interaction coefficient

C ƒMX interaction coefficient
cj concentration of component j (kg/m3)
Fƒ fugacity coefficient
I ionic strength=1/2 i miz 2i (mol/kg)
M molality (mol/kg)
M moleclar weight (g/mol)
Ms molecular weight of the solvent (g/mol)
R 8.314 (J/mol K)
T Absolute temperature (K)
6s molar volume of the solvent (m3/mol)
zm charge of positive ion
zx charge of negative ion

Greeks
h parameter in Pitzer model
i (0) parameter in Pitzer model
i (1) parameter in Pitzer model
Dy osmotic pressure difference (bar)
m dielectrical constant=78.54 for water at 25°C
w number of ions
wm number of positive ions
wx number of negative ions
ƒ osmotic pressure coefficient

1. Introduction Membranes can be used for the purification of

Because of more stringent regulations and eco-
nomical advantages, companies tend to invest
more and more time and money in water reuse.
For textile companies in particular, the large
amount of water that is needed for processes like
dyeing, rinsing and further treatment of the
textile leads to a growing importance of water
reuse [1].
Dye baths produce large wastewater streams
that can’t be discharged directly because they
would have a dramatic impact on the total
wastewater stream. Used dye baths contain high
concentrations of organic compounds, combined
with a very high concentration of inorganics.
Purification is therefore advisable, in view of the
decrease of the wastewater amount as well as the
decrease of the water consumption.
these complex wastewater streams [2,3]. The mem-
brane process that can meet the necessary stan-
dards is nanofiltration, because nanofiltration
membranes can retain ions as well as relatively
small organic molecules from an aqueous solution
[4,5]. However, it is not well understood what
mechanisms of retention and flux decline are in-
volved in this process.
Two possible solutions can be investigated. One
option is the direct filtration of dye baths. The
solution in the dye bath then goes directly to the
nanofiltration unit, where the contaminants are
retained. Hence, a clean water stream is produced
that can be recycled to the process. The advantage
of this strategy is, that the filtration can be carried
out at enhanced temperature, which results in a
significant energy saving. However, the complex-
ity of the solution makes filtration difficult in
 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528
Fig. 1. Schematical representation of the nanofiltration process
(1, feed; 2, module; 3, permeate; 4, retentate; 5, feed; 6, pump.
many ways. In this work, the parameters that
determine the possibility of (nano)filtration will be
examined for representative dye baths used in the
textile industry.
The second option is to provide a biological
treatment of the wastewater streams from the dye
baths. The biological treatment is then followed by
a nanofiltration unit, where the degradation prod-
ucts and the non-biodegradable organic com-
pounds are removed. Because many textile factories
already have an activated sludge system, this option
can be very easily implemented. However, many
degradation products are small, which could allow
them to pass the membrane pores. Furthermore, no
energy savings can be obtained.
2. Methods and materials
For the filtration experiments, a commercial
nanofiltration unit on laboratory scale was used
(Amafilter, Test Rig PSS1TZ). Flat sheet mem-
branes were used with an active surface of 0.0044
m2. Fig. 1 represents the nanofiltration unit
schematically.
Table 1
Properties of the membranes used in the experiments
NF-70
Manufacturer Dow/FilmTec
Membrane material Crosslinked aromatic polyamide
Charge (neutral pH) negative
MWC (estimate) 250
Mean pore size (nm) 0.34
Standard deviation on pore size (nm) 0.54
521
The feed solution is pumped to the membrane by
a three-stage membrane pump. The filtration in the
module occurs in cross-flow.
The pressure over the membrane can be varied
from 0 to 60 bar with manual valves. The feed flow
varies from 0 to 1000 l/h, which corresponds to a
feed velocity of 0–7.5 m/s. The temperature is set
with an electronic circuit.
The membranes that were used are NF-70 (Dow/
FilmTec), UTC-20 (Toray Ind. Inc.) and NTR 7450
(Nitto-Denko). For the research of the direct
filtration of dye baths, the UTC-60 membrane
(Toray Ind. Inc.) was also used as an alternative for
UTC-20. These membranes have also been used in
earlier research [5,6], which allows to characterize
them thoroughly. They were selected because their
retention characteristics allow to retain small or-
ganic molecules together with a part of the ions in
the solution. The extent to which these components
are retained depends of the specific membrane. The
membranes that were used reflect the range of
nanofiltration membranes from low pressure re-
verse osmosis to ultrafiltration. A summery of
membrane properties is given in Table 1.
Metal concentrations in solution were measured
by inductively coupled plasma mass spectrometry
(ICP-MS). Anions in solution were measured with
capillary ion analysis (CIA). Total phosphorus was
determined using the Molybdene-blue spectropho-
tometric method, after destruction to orthophos-
phate. Chemical oxygen demand (COD) and
biological oxygen demand (BOD, measured after 5
days), which are measures for the concentration of
organics, were determined according to their re-
spective definitions [7]. Suspended solids were mea-
sured by filtration over a glass fiber filter (Whatman
GF/C 0.45 mm).
UTC-20 NTR 7450
Toray Ind. Inc. Nitto-Denko
Polyamide Sulfonated polyethersulfone
positive negative
180 600–800
0.54 0.80
0.17 0.52
522 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528
Table 2
Composition of a reactive dye bath
Component Concentration (g/l)
Na2SO4 56.0
EDTA 0.2
Na2CO3 1.0
NaOH 2.5
Reactive orange 16 or reactive blue 2 5.0
A Shimadzu UV-210A double beam spec-
trophotometer was used for absorbance
measurements.
3. Direct filtration of dye baths
To simulate the direct filtration of dye baths,
known recipes were used to prepare synthetical
dye baths. This option is crucial to obtain infor-
mation on the scientific background of the filtra-
tion process. Hence, the retention mechanisms can
only be studied when known concentrations of
well-known molecules are applied to the process.
With the synthetic solutions, concentrations of the
different components were varied, and the influ-
ence of each component was studied by evaluating
the filtration characteristics with or without this
component.
The solutions were filtered with the NF-70,
UTC-20, NTR 7450 and UTC-60 membranes. A
bath with reactive dyes (reactive orange 16 and
reactive blue 2) was prepared. The composition of
the dye bath is represented in Table 2. Commer-
cial surfactants were not used because the molecu-
Fig. 2. Chemical structure of reactive orange 16 (a) and reactive blue 2 (b).
lar structure is in most cases not available. As an
alternative, EDTA was chosen, because it has a
known molecular structure and affects the dye
bath in a comparable way.
The solution contained one of the reactive dyes
in each experiment. The chemical structure of the
dye molecules is represented in Fig. 2.
When the feed solution was prepared according
to Table 2 and applied to the nanofiltration unit,
no measurable water flux was obtained with the
membranes mentioned above. The membranes
were strongly coloured after filtration. This is not
surprising, because the dye molecules are sup-
posed to attach strongly to a surface. However, it
can be disadvantageous for fouling effects. After
the experiment, the membranes were rinsed and
the permeate flux was measured with distilled
water as feed. This revealed that membrane foul-
ing was limited to a colour change at the surface
of the membrane. On the average the permeate
flux after the experiment was 85, 90 and 85% of
the normal permeate flux for NF-70, UTC-20
and NTR 7450, respectively. This means that
the dramatical flux decline in the experiment was
not caused by (irreversible) fouling of the mem-
brane.
The high ionic concentrations cause an impor-
tant osmotic pressure because a large part of the
ions are retained by the membrane. The concen-
tration difference on both sides of the membranes
gives rise to an osmotic pressure.
An estimate of the osmotic pressure during the
filtration can be obtained with theoretical calcula-
tions. The Van’t Hoff model calculates the os-
motic pressure as:
 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528
RT
Dy =wcj
M much lower than the value obtained with the Van’t
For a solution containing 30 g/l Na2SO4, which is
not unusual for dye baths, the osmotic pressure
would be 15.7 bar.
For the solution in Table 2, the osmotic pressure
will be even higher. However, the Van’t Hoff model
returns an overestimation of the osmotic pressure at
these high concentrations. Therefore, the osmotic
pressure was also calculated with the more precise
Pitzer model [8]. This model calculates the osmotic
pressure on the base of intercations between ions.
The osmotic pressure is expressed as:
RTMs
Dy = (wm)ƒ
1000 6s
ƒ in this equation is an osmotic pressure coefficient,
indicating the deviation from the Van’t Hoff model.
ƒ can be calculated (for a 2 – 1 electrolyte) with the
following equation:
2wmwx ƒ
523
The osmotic pressure is thus 10.3 bar; this value is
Hoff model, but is still too high to allow a permeate
flux at reasonable membrane pressures. Hence, the
osmotic pressure has to be exceeded before transport
of water can take place.
This example shows that due to the high ionic
concentrations, the dramatic reduction of the perme-
ate flux was to be expected. Moreover, in real
situations the ion concentrations can be even higher
than 30 g/l Na2SO4.
The mechanism of the osmotic pressure causes a
linear decrease of the water flux when the ion
concentration in the feed solution increases. This can
be derived from the theoretical equations of Van’t
Hoff and Pitzer and was found experimentally for the
three used membranes (Fig. 3). Omitting EDTA in
the feed solution did not influence the results.
The influence of the dye molecule on the water flux
is small. The concentration of the dye solution had no
influence on the efficiency of the nanofiltration. This
ƒ − 1= zmzxf ƒ + m B MX was examined for a feed solution where only the dye
w

+m 2
 2(wmwx)3/2 ƒ
C MX
molecule was present. The ions were omitted in order
not to influence the water flux. The permeate flux
w remained constant as a function of the concentration
of the dye, for concentrations ranging from 0 to 10 g/l
where the fugacities and the interaction coefficients
reactive orange 16 or reactive blue 2. Nevertheless, at
can be obtained from theoretical considerations and
higher concentrations the colour shift of the mem-
experimental values:
brane after the experiment was much stronger.
4 ƒ 2(5/2) ƒ The small influence of membrane fouling was also
ƒ − 1= 2f ƒ + m B XM +m 2 C XM confirmed by an experiment that examined the
3 3
influence of time on the water flux when all other
I 1/2
= 2−Aƒ settings in the membrane unit remain constant

 
1+bI 1/2 (temperature, pressure, cross flow velocity, concen-
4 (0) 4 (1) tration). During a 2 h filtration experiment with the
+m i + i exp( − hI − 1/2) UTC-60 membrane, the water flux remained con-
3 3
stant, which indicates that for a short time scale no
2(5/2) ƒ fouling occurs (Fig. 4).
+m 2 C XM
3 The retention results were satisfactory for UTC-
For the example above: Aƒ =0.51; m =0.21 mol/kg 60, UTC-20 and NF-70. In Table 3, the dye retention
and I= 0.63 mol/kg. is presented for cumulative addition of the different
Pitzer found the optimal value for h as 2 and b as components of the dye bath. From Table 3 it can be
1.2. The parameters (4/3)i (0), (4/3)i (1) and (2(5/2)/ seen that the dye retention is high enough to remove
3)C ƒXM stand for anorganic components of the 2 – 1 all colour from the feed solution. For reactive orange
16, there is an additional retention increase when
type and can be found in tables [6]. For Na2SO4 they
NaOH is added. This is caused by a shift in the
are, respectively, 0.0261, 1.484 and 0.00938. The
chemical structure of the molecule when the pH
osmotic pressure coefficient then becomes:
increases. The influence of EDTA on the dye
ƒ = 1 − 0.41+ 0.0055+ 0.064 +0.00042 =0.65 retention is negligible.
524 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528

Fig. 3. Influence of the Na2SO4 concentration on the water flux with nanofiltration, for the different membranes at 10 bar and 25°C.

Fig. 4. Influence of time on water flux for a solution of 0.5 mg/l reactive orange 16 (UTC-60, 10 bar, 25°C).

From these results, it is obvious that the reten-
tion of ions with the used membranes is too high
to allow direct filtration of the dye baths. The
pore structure of these membranes is so tight that
together with the dye molecules, the major part of
the ions is removed. This way, an osmotic pres-
sure is built up that prevents filtration at realistic
pressures. This was especially the case for the
membranes with the smallest pores (NF-70 and
UTC-20). For membranes with larger pores, such
as NTR 7450, the possibility of nanofiltration of
dye baths remains, depending of the composition
of the feed solution. However, the dye retention
for a single pass module with NTR 7450 is not
sufficient; a double pass module is needed to
provide complete colour removal.
The ion retention is high for most membranes,
as mentioned above, but due to the Donnan
mechanism [9] this retention will be lower at
higher salt concentrations.
The results for NTR 7450 are summarized in
Table 4. In this table, the water flux is indicated
with distilled water as feed (1) and with the dye
solution as feed (2). The measurement with dis-
tilled water was carried out before the filtration of
the dye solution.
 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528 525

Table 3 gathered and treated in an activated sludge sys-

Dye retention (%) for reactive orange 16 and reactive blue 2
tem, nanofiltration can provide an additional
for nanofiltration with UTC-60 (cumulative addition, / indi-
cates no retention measurable because no permeate was ob- purification that allows to reuse the filtered water
tained) as process water [6].
After biological treatment, the water still con-
Condition Reactive orange 16 Reactive blue 2
tains a significant amount of colour forming com-
1.0 g/l dye 97.9 99.9 ponents from dyes that are not or only partly
+ 2.5 g/l NaOH 99.3 99.8 degraded. A typical composition is given in Table
+1.0 g/l Na2CO3 99.7 99.6 5.
+0.2 g/l EDTA 99.7 99.7
For reuse of the treated wastewater, it is neces-
+11.0 g/l 99.6 99.3
Na2SO4 sary that the quality of the effluent is equal to or
+19.0 g/l 76.3 96.5 better than the quality of the water that is used as
Na2SO4 process water. The most important parameters are
+26.0 g/l / /
suspended solids, BOD/COD, hardness and sul-
Na2SO4
phate and chloride concentration. Another re-
quirement is that no enrichment of other
At a pressure of 10 bar the water flux is 23% components such as heavy metals occurs in the
of the water flux with distilled water as feed, while process [11].
this is typically 85 to 90%. Although this is a As a pretreatment for the membrane filtration,
significant decrease, the possibility of nanofiltra- a sand filter was used. The pretreatment removed
tion remains. The osmotic pressure is strongly suspended and settleable solids, which was neces-
dependent of the composition of the dye bath. If sary to avoid fouling of the nanofiltration mem-
salts with monovalent ions like NaCl are used branes, which would shorten the membrane
instead of bivalent salts (Na2SO4, Na2CO3) the lifetime dramatically. During the experiments on
osmotic pressure will be lower, and the water flux short terms, the membranes were somewhat
at the same pressure will increase. Moreover, the coloured after the experiment, in spite of the
osmotic pressure will me much lower when the pretreatment.
salt concentrations in the solution are lower. For The results of the nanofiltration experiments
a number of dyeing processes such as disperse are also presented in Table 5. For each of the
dyeing the problem is avoided because the salt membranes, all colour was removed in the visible
concentrations in the dye bath are lower [10].
light range (Fig. 5). For NTR 7450, a small
absorption in the UV range remained, which was
4. Nanofiltration of the effluent of activated caused by small organic compounds that were not
sludge treatment retained by the membrane. The removal of or-
ganic compounds is also expressed by BOD/COD
When the wastewater of a textile factory is removal. This shows that the remaining organic

Table 4
Overview of results for NTR 7450 with Reactive blue 2 (*, no results available)

Pressure (bar) Water fluxa (l/m2 h) Water fluxb (l/m2 h) Dye retention (%) Salt retention (%)

5 65.0 10 86.4 21.5

10 129.0 29.4 * *
20 264.0 64 92.1 87.3

a
Distilled water as feed.
b
Dye solution as feed.
526 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528

Table 5
Nanofiltration of effluent of biological treatment (NF70, NTR 7450 and UTC-20)

Parameter Feed NF-70 NTR 7450 UTC-20

pH 8.3 9.3 8.6 8.6

Suspended solids (mg/l) 18.8 B1 B1 B1
Ca (mg/l) 85.6 0.6 27.8 9.6
Cr (mg/l) 140 B10 10 B10
Fe (mg/l) 360 B10 10 B10
Zn (mg/l) 610 13 149 17
COD (mg O2/l) 231.8 17.7 31.4 33.4
BOD (mg O2/l) 5.2 B1 B1 (–)a
Conductivity (mS/cm) 3.8 0.11 2.29 1.78
SO2−
4 (mg/l) 313 0.9 93 N.D.
Cl− (mg/l) 740 17.4 587 496
Total P (mg/l) 1.0 0.2 0.34 0.17
Water flux (l/m 2 h bar) 8.1 (85b) 13.3 (85b) 15.7 (90b)

a
(–) no measurement available.
b
Percentage of the water flux with distilled water as feed

Fig. 5. Colour removal with nanofiltration membranes NF-70, UTC-20 and NTR 7450.

fraction for NTR 7450 is also larger than for both
other membranes.
The results for BOD/COD and colour removal
correspond with earlier findings about retention
of organic molecules with these membranes [5].
For NF-70 and UTC-20, retention of raffinose
and galactose was higher than the COD retention
in this experiment (Table 6). For NTR 7450,
raffinose and galactose retention was lower. This
can be explained by the assumption that the ma-
jor part of the organic material in the wastewater
has a relatively high molecular weight (and, corre-
 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528
spondingly, a large molecular size). Thus, the
wastewater contains a large amount of molecules
with a molecular size that corresponds approxi-
mately with a molecular weight of 800, the esti-
mated molecular weight cut-off of NTR 7450.
NF-70 and UTC-20 have both tight pores; only
very small molecules like ethanol can permeate
through these membranes. For these small
molecules, transport can also take place by disso-
lution in the membrane followed by diffusion
through the polymeric material. The larger the
molecules, the more difficultly they dissolve in the
membrane structure.
Because galactose retention is higher than the
obtained COD retention, the wastewater must
also contain a fraction with a relatively small
molecular size.
The removal of other components follows the
same lines. Removal of hardness is insufficient for
NTR 7450, but is more than sufficient for both
other membranes. Sulphate removal is low for
NTR 7450, but NF-70 and UTC-20 remove all of
the sulphates. Chloride concentration decreases
significantly only for the NF-70 membrane. The
removal of heavy metals is high enough to avoid
enrichment throughout the water cycle in the
process.
The findings above show that water reuse is
possible when the right membrane is used. NF-70
is a good example of such a membrane. COD,
concentrations of calcium and other metals and
concentrations of anions in the NF-70 permeate
are lower than the concentrations in the raw
waters that are used in the textile industry. How-
ever, an unknown factor is the behaviour of the
water flux on longer terms. Indeed, it is necessary
to obtain a stable flux for long periods to ensure
a good water quality and recovery in time.
Table 6
COD retention compared to retention of galactose, raffinose and the estimated molecular weight cut-off
COD Galactose (MW 180)
NF-70 92 95
UTC-20 88 95
NTR 7450 85 29
527
5. Conclusions
The results of this study show that nanofiltra-
tion can be a realistic treatment method for both
options. As seen in the light of the development of
nanofiltration as a separation process, this tech-
nique could become more important in the future,
also in this field [12,13]. When a biological treat-
ment precedes the filtration unit, not many prob-
lems occur. The nanofiltration experiments with
the effluent of activated sludge treatment yielded
an acceptable water flux. The salt concentrations
in the water treated with activated sludge are low
enough to avoid problems with build-up of an
osmotic pressure. The retentions of dyes and
other components (hardness, metals, chlorides,
sulphate, BOD/COD) are sufficient to allow reuse
of the wastewater as a process water. The condi-
tion hereby is that a membrane with small pores is
chosen so that small break down products are
also removed from the water. Retention of these
uncharged molecules is achieved through sieving.
For the direct filtration of dye baths, problems
with (too) high osmotic pressures can occur. This
is strongly dependent of the composition of the
dye bath and the right choice of the membrane.
The salt concentration should be as low as possi-
ble; monovalent ions are easier to filter than
bivalent ions. The choice of the membrane is also
important: if a membrane with too small pores is
selected, the fraction of the ions that is retained is
too large and an osmotic pressure builds up. If the
pores are too large, the dye molecule passes
through the membrane. The ideal membrane is
thus a compromise between dye retention and salt
retention.
The results with the NTR 7450 membrane show
that a membrane configuration with at least a
double pass is needed. The dye retention of 90% is
Raffinose (MW 504) Estimated cut-off
99 250
97 180
67 600–800
528 B. Van der Bruggen et al. / Separation/Purification Technology 22-23 (2001) 519–528
unsufficient to remove all colour from the water,
which is necessary for reuse. For the second filtra-
tion step, less problems are expected, because the
larger part of the components from the dye bath
is already removed in the first step.
When a water recovery of 80% is assumed,
these results prove that the amount of fresh pro-
cess water can be reduced with a factor 5. The
volume of wastewater decreases with the same
factor. However, the fraction that is left (the
retentate) contains higher concentrations and can
in many cases not be discharged without further
treatment. For the first option, ozonisation can be
applied to break down the fraction of the organic
molecules that is still left; from the ozonisation
the resulting stream goes back to the activated
sludge system. For the second option, the reten-
tate can be sent directly to an activated sludge
system.
A factor that has not been examined yet is the
influence of temperature on the water flux and the
retention of dyes. No influence of the temperature
on retention is expected, whereas the water flux
increases with 2.5% for each °C temperature rise
[14]. The effect of the high ion concentration can
be partly compensated this way.
Acknowledgements
This research was financed with a fellowship
from IWT (Vlaams Instituut voor de bevordering
van het Wetenschappelijk-Technologisch Onder-
zoek in de Industrie). Grateful acknowledgement
is made to Toray Ind. Inc. for supplying the
UTC-60 membranes, and to I. De Vreese (Centex-
bel) for cooperation and advices.
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