Desalination 240 (2009) 151
159

Coagulation ultraltration system for river water treatment

Krystyna Koniecznya, Dorota Skolb, Joanna Ponkaa, Mariola Rajcaa,

Micha Bodzeka*
a
Institute of Water and Wastewater Engineering, Silesian University of Technology,
Konarskiego 18, 44-100 Gliwice, Poland
Tel: +48 032 232 2368; Fax: +48 032 232 2368; email: michal.bodzek@polsl.pl
b
Water and Chemical Department, PKE S.A. agisza Power Plant, Pokoju 14, 42-504 Bdzin, Poland
Received 16 August 2007; revised 25 October 2007; accepted 2 November 2007

Abstract
The in-line coagulation
ultrafiltration hybrid process has been investigated using three different coagulants,
viz. FeCl3, Fe2(SO4)3 and Al2(SO4)3. The coagulants were dosed in the amounts of 2.4 mg Fe/dm3, 2.8 mg Fe/dm3
and 2.9 mg Al/dm3, respectively. Surface water from the Czarna Przemsza river (Silesia region, Poland) was used
as raw water. The ultrafiltration membrane module with capillary polyethersulphone membranes was applied.
It has been shown that the application of coagulant in-line contributes to the improvement of the quality of
water as a result of growth of the removal of organic matter. It has also been statistically proven that the proper
choice of the coagulant is of significant importance for the degree of removal of organic matter from the water.
The highest efficiency of the process was achieved when the aluminum coagulant was used.
Furthermore, it has been shown that the application of in-line coagulation and ultrafiltration with the most
proper coagulant restricts the fouling of the membranes, so that contaminations deposited on the membrane can
easily be removed using deionized water.
Keywords: Ultraltration; In-line coagulation; Water treatment; Hybrid process

1. Introduction from the environment. Until recently wastewater

Membrane processes, often aided by conven-
tional techniques, allow for economic use of
water resources by multiple use of water taken
*Corresponding author.
was defined as water used for some special
purpose, of which the physical, biological and
chemical parameters had been changed so much
that water reuse for the same purpose was not
possible. Nowadays, thanks to the application of
membrane techniques, industrial or municipal

Presented at the Third Membrane Science and Technology Conference of Visegrad Countries (PERMEA), Siofok,
Hungary, 26 September 2007.

0011-9164/09/$ See front matter # 2008 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2007.11.072
152 K. Konieczny et al. / Desalination 240 (2009) 151
159
wastewater may be used again, even for the
production of water, the purity of which
surpasses the purity of the water used previously.
The system operated in the agisza Power
Station (Silesia region, Poland), which produces
demineralized water using blow-down water
from the cooling system, is a good example of
water reuse. The application of microfiltration
and reverse osmosis makes it possible to obtain
water whose parameters are much better than the
parameters of the blow-down water [1,2].
The growing application of membrane tech-
niques in water treatment has also contributed to
the improvement of the quality of drinking
water. Micro- and ultrafiltration permit to sepa-
rate organic and inorganic suspensions, colloids
as well as the cysts and oocysts of parastites,
such as Giardia lamblia and Criptosporidium
parvum. Thanks to additional support of mem-
brane techniques by conventional techniques, i.e.
so-called hybrid processes, the physico-chemical
parameters of the water can be improved even
further, which prevents membranes against the
irreversible process of pore blocking. Ref. [3]
subjected a suspension of white clay in deminer-
alized water to successive processes of coagula-
tion and ultrafiltration. The application of the
coagulant FeCl3 in the amount of 0.1 g/g
suspension improved the conditions of separa-
tion considerably due to the formation of
floccules sedimenting during the first stage of
the treatment. Ref. [4], on the other hand, has
proven that in case of removing organic matter, a
dose of 68 mg/L of the ferric coagulant FeCl3
permits to separate 78% of organic matter
determined as dissolved organic carbon (DOC)
in the course of coagulation, whereas ultrafiltra-
tion removes further 9.6%. A reduction of the
dose of the coagulant resulted in a gradual
increase of the removal of organic matter during
the ultrafiltration. Ref. [5] investigated the
hybrid process combining coagulation by means
of iron and aluminum compounds with micro-
filtration polypropylene and ultrafiltration
polyethersulphone (PES) membranes. The result
was considerably higher elimination of organic
matter from simulated water in comparison both
to a single coagulation process and the process
of membrane filtration, not aided by coagulation.
The elimination of organic matter determined as
TOC in the process of coagulation by means of
FeCl3 in case of water with an initial TOC
concentration of 10 mg/dm3 amounted to
81.9%
95.0%, in a single process of microfil-
tration and ultrafiltration to 95.0% and 89.3%,
respectively, and in hybrid processes with micro-
and ultrafiltration to 100%.
Increasingly, more frequent mode of combin-
ing the technique of coagulation with micro- or
ultrafiltration is the in-line process [6
9,11]. It
consists of batching the coagulant to the feed
immediately before the membrane, omitting the
stage of sedimentation, which results in reduc-
tion of the dose of the coagulant and the duration
of water treatment. This is of special importance
in case of small water treatment stations, as the
surface required by the installation can be
reduced to a minimum [8]. Ref. [6] investigated
the in-line process combining coagulation by
means of FeCl3 and applying capillary cellulose
ultrafiltration membranes carried out in dead-end
and a cross-flow mode. They have shown that
running the process in such a way results not
only in improved quality of permeate, but also
the phenomenon of fouling is slowed down.
This statement has been confirmed by the results
of investigations carried out in Ref. [8], which
tested the removal of organic matter determined
as absorbance UV254 in the in-line process
coagulation
ultrafiltration, applying the alumi-
num coagulants Al2(SO4)3 and NaAlO2 as well
as polyaluminum chloride and both PES and
cellulose membranes. The improved quality of
water can, according to the authors of Ref. [6],
be accounted for as follows: the filter cake
consisting of floccules as a result of coagulation
 K. Konieczny et al. / Desalination 240 (2009) 151
159
also takes part in the retention of organic matter.
The process is essentially affected by the pH and
the dose of the coagulant [6,8].
Research carried out by Konieczny and Bodzek
[5,9,10
12] in the system coagulation-sedimenta-
tion-microfiltration, applying ceramic and poly-
meric membranes, was aimed at the comparison of
the effectiveness of the hybrid process combining
the stages: coagulation with sedimentation and
membrane filtration with the in-line hybrid
process. The results obtained allow to state that
the first process yields better results than the
second one. This concerns both the efficiency of
the membranes and the degree of the removal of
contamination from water. Comparing, however,
the effectiveness of coagulation, as such, coagula-
tion in-line-membrane filtration seems to be a
better solution, because of the fact that the
efficiency and the quality of the permeate is
insignificantly worse but smaller doses of the
coagulant can be applied.
The aim of the present paper is to compare
the effectiveness of selected coagulants in the
processes of in-line coagulation
ultrafiltration
with the purpose of removal of organic matter
from natural river water, taking into account the
influence of the coagulants on the value of the
permeate flux.
2. Experimental
These investigations were carried out on a test
unit provided by EURO-SEP, applying an ultra-
filtration module equipped with PES membranes.
The characteristics of the membrane module
have been presented in Table 1. The raw water
was river water from the water intake PKE S.A.
of the power station agisza, situated on the
Czarna Przemsza (Silesia region, Poland).
The process of membrane filtration was
carried out in an open system. This means that
permeate was disposed outside the system, and
153
Table 1
Characteristics of membrane module
Membrane type Capillary,
hydrophilic
Nominal area, m2 0.556
Membrane material PES
Number of fibers 258
Outside diameter fiber, mm 2.1
Inside diameter of fiber, mm 1.5
Module size, mm 50 /500
Module type ULTRA-U
Transmembrane pressure (max.) 0.8 MPa
the test unit was continuously provided with
fresh river water (Fig. 1).
Direct ultrafiltration process and also the in-
line hybrid processes using the following coagu-
lants: FeCl3 (PIX 111), Fe2(SO4)3 (PIX 113) and
Al2(SO4)3 (ALS), were carried out. The doses of
coagulants, determined on the basis of a jar test,
amounted to 3.0 mg Fe/dm3 for FeCl3, 2.8 mg Fe/
dm3 for Fe2(SO4)3 and 3.6 mg Al/dm3 for
Al2(SO4)3 [5,10,12]. Hybrid processes were run
with coagulant doses amounting to 100%, 80%
and 60% of the dose attained during the jar test.
Samples of raw water and permeate were
taken every hour in the course of 6 h. For the
assessment of the effectiveness of the process the
following parameters were chosen:
Fig. 1. Schematic diagram of in-line coagulation/
ultraltration system: 1, Czarna Przemsza river; 2, raw
water tanks; 3, feed pump; 4, coagulant tank; 5, feed
tank; 6, lter; 7, process pump; 8, rotameter; 9,
membrane module; 10, permeate tank.
154 K. Konieczny et al. / Desalination 240 (2009) 151
159

. general parameters describing the properties
of the investigated water, viz. pH, conductiv-
ity and turbidity and
. parameters testifying the presence of organic
compounds in the water, viz. absorbance
UV254, chemical oxygen demand (COD),
permanganate oxygen consumption and total
organic carbon (TOC).
of the permeate flux were obtained when the
following doses of coagulants were applied:
FeCl3, 2.4 mg Fe/dm3 (80% of the dose obtained
in the jar test); Fe2(SO4)3, 2.8 mg Fe/dm3 (100%
of the dose obtained in the jar test) and
Al2(SO4)3, 2.9 mg Al/dm3 (80% of the dose
obtained in the jar test [5,10,12].

Moreover, changes of the volumetric flux of
deionized water were observed before the mea-
surements (new membrane) and during the
rinsing of the membrane with deionized water
after the single UF process and after each hybrid
process. The aim of the measurements was to
compare the reversibility of the membrane foul-
ing by compounds contained in the raw water
without a coagulant and in case of coagulant
application. Before each change of the coagulant
the membrane module was chemically cleaned
using a basic and an acid solution.
3. Results and discussion
The present paper deals only with the presenta-
tion and comparison of the results concerning the
most optimal doses of the coagulants applied. It
has been found that the highest retention coeffi-
cients of organic compounds and the lowest drop
3.1. Results of selected parameters of water
treated with the ultrafiltration module
(polyethersulphone)
The mean values of the parameters of raw
water and ultrafiltration permeate as well as their
standard deviations are shown in Table 2. The
values of standard deviations did not exceed
20% concerning the raw water and 33% con-
cerning the permeate (turbidity).
The retention coefficients obtained in case of
organic compounds contained in the water differ
and amount to 32.4% of permanganate oxygen
consumption up to 33.71% of absorbance UV254
to 55.1% in case of TOC. These differences may
be explained by the fact that each of the
presented ways of analysis concerns a somewhat
different range of organic matter. Some authors
try to prove that by means of the absorbance we
determine organic compounds characterized by
considerable molecular weights [13,14]. Others

Table 2
Average value of physicochemical parameters of water treated with only ultraltration membrane, n /6a

Parameter Raw water Permeate Difference Retention

coefficient
Average s Average s (%)

pH 7.8
8.0 7.7
7.0

Conductivity (mS/cm) 0.450
0.460 0.425
0.435


Turbidity (FTU) 15 3 3 1 12 80.0
Permanganate COD (mg O2/dm3) 7.4 0.2 5.0 0.3 2.4 32.4
Absorbance UV254 (cm1) 0.175 0.008 0.116 0.004 0.059 33.7
TOC (mg C/dm3) 6.53 1.00 2.93 0.48 3.60 55.1
COD (mg O2/dm3) 23.9 4.0 13.6 1.3 10.3 43.1

s , Standard deviation; n , number of measurements; FTU, Formazin turbidity units.

a
 K. Konieczny et al. / Desalination 240 (2009) 151
159 155

stress the fact that the presence of humic acids
gives rise to UV254 absorbance [14]. In case of
the investigated water the retention coefficient of
UV254 is comparatively small. It is, therefore, to
be supposed that organic matter dominates in the
investigated water, which is denoted as UV254
absorbance, with diameters of the molecules
below those of the pores of an ultrafiltration
membrane. The highest retention coefficient in
case of TOC may be explained by its being a
coefficient comprising the widest range of
organic matter contained in the water. Applying
the permanganate oxygen consumption and
COD we determine the substances which oxidize
under given conditions of their determination,
including some inorganic compounds, such as
iron (II) compounds or nitrates (III). The change
of these parameters indicates, therefore, not only
the retention of organic matter, but also a similar
decrease of the turbidity expressed in FTU.
The low values of the retention coefficients of
all the indices of the concentration of organic
matter, obtained in single ultrafiltration process,
suggest the presence of substances with particles
smaller than the diameter of the pores of an
ultrafiltration membrane in the investigated sur-
face water. The presence of organic matter in
surface water with a rather small molecular
weight has been confirmed by investigations
carried out in Ref. [15]. They compared the
feasibility of ultra- and nanofiltration for the
purpose of removing organic matter from the
water and found that nanofiltration is much more
effective, even in case of hybrid processes
applying FeCl3 as coagulant. This has been
confirmed by the results of analyses, gathered
in Tables 3
5, as the application of coagulants in
the ultrafiltration processes raises the value of
the retention coefficients.
3.2. Results of the decrease of the volumetric
permeate flux on the ultrafiltration module
Fig. 2 presents a diagram of the dependence
of the volumetric flux of deionized water on the
time for UF membrane before measurements and
after all investigated water treatment processes.
It means that the measurements have been made
after each hybrid process when the membranes
were rinsed using deionized water.
Before the proper measurements, the flux of
deionized water decreased significantly in the
course of the first 5 min of the process and set at a
constant level after 120 min. The overall reduc-
tion of the flux did not exceed 9.8%. During the

Table 3
Average value of physicochemical parameters of water treated with in-line process coagulation
ultraltration (FeCl3
as a coagulant with dose 2.4 mg Fe/dm3, n /6)

Parameter Raw water Permeate Difference Retention

coefficient
(%)
Average s Average s

pH 7.4
7.5 7.0
7.2

Conductivity (mS/cm) 0.425
0.440 0.400
0.430


Turbidity (FTU) 17 2 2 1 15 88.2
Permanganate COD (mg O2/dm3) 6.7 0.4 4.3 0.4 2.4 35.8
Absorbance UV254 (cm1) 0.260 0.007 0.135 0.004 0.125 48.1
TOC (mg C/dm3) 7.40 0.25 4.13 0.036 3.27 44.2
COD (mg O2/dm3) 23.8 2.2 11.8 2.2 12.0 50.4
156 K. Konieczny et al. / Desalination 240 (2009) 151
159

Table 4
Average value of physicochemical parameters of water treated with in-line process coagulation
ultraltration
(Fe2(SO4)3 as a coagulant with dose 3.0 mg Fe/dm3, n/6)

Parameter Raw water Permeate Difference Retention

coefficient
Average s Average s (%)

pH 7.7
7.8 7.0
7.1

Conductivity (mS/cm) 0.365
0.370 0.335
0.355


Turbidity (FTU) 19 2 2 1 17 89.5
Permanganate COD (mg O2/dm3) 7.4 0.2 4.1 0.2 3.3 44.6
Absorbance UV254 (cm1) 0.296 0.001 0.130 0.002 0.166 56.1
TOC (mg C/dm3) 9.36 0.77 3.83 0.77 5.53 59.1
COD (mg O2/dm3) 24.6 2.6 14.4 2.7 10.2 41.5

ultrafiltration of raw river water the flux dropped
by 22.4% with regard to the value obtained at the
end of the process, when deionized water was
used. Rinsing with deionized water prevented a
return to the initial value of the flux, so that the
ultrafiltration membrane was partly blocked by
substances occurring in raw water.
It has been observed that the susceptibility of
ultrafiltration membranes to fouling depends on
the kind of coagulant applied. The addition of
FeCl3 to raw water resulted in a considerable
decrease of the value of the flux, amounting to
41.2% in the course of 6 h (maximum value).
When Fe2(SO4)3 was added, the decrease
amounted to 11.6% (minimum value) and
rinsing with deionized water proved to be
successful in restoring the previous value of
the volumetric flux of water flowing through the
membrane. Similar results were obtained with
Al2(SO4)3. In this case the reduction of the flux
amounted to 18.0% after the end of the in-line
coagulation and after rinsing the value reached
was not much lower than the initial value of the
volumetric flux of water.

Table 5
Average value of physicochemical parameters of water treated with in-line process coagulation
ultraltration
(Al2(SO4)3 as a coagulant with dose 2.9 mg Al/dm3, n/6)

Parameter Raw water Permeate Difference Retention

coefficient
(%)
Average s Average s

pH 7.8
7.9 6.9
7.0

Conductivity (mS/cm) 0.445
0.450 0.430
0.440


Turbidity (FTU) 13 1 0 1 13 100
Permanganate COD (mg O2/dm3) 7.8 0.2 4.0 0.1 3.8 54.3
Absorbance UV254 (cm1) 0.195 0.003 0.075 0.003 0.120 61.5
TOC (mg C/dm3) 5.75 0.50 2.42 0.19 3.33 57.9
COD (mg O2/dm3) 18.5 1.4 7.8 1.7 10.7 57.8
 K. Konieczny et al. / Desalination 240 (2009) 151
159
3 4. Statistical analysis of the results of the
Deionized water flux
Jv (m3/m2s) 105
2 Four groups of results have been obtained:
1
0 water and the ultrafiltration permeate have been
0 30 60 90 120 150
Time (min)
Worth of the flux of deionized water measured:
for new membrane
after UF alone
after hybrid process (FeCl3 2.4 mg Fe/dm3)
after hybrid process (Fe2(SO4)3 3.0 mg Fe/dm3)
after hybrid process (Al2(SO4)3 2.9 mg Al/dm3)
Fig. 2. Dependence of the volumetric ux (Jv) of
deionized water on time.
As far as the choice of the membrane
techniques for the water treatment is concerned,
one should take into account the susceptibility of
the membrane to the pore blocking caused by
compounds existing in the raw water (fouling).
Particles bigger than the membrane pores are
collected on its surface forming filter cake,
whereas the smaller ones may block membrane
pores inside [16]. In case of applying coagulants
Al2(SO4)3 and Fe2(SO4)3, the phenomenon of
blocking is reversible, and the resulting filter
cake is removed by rinsing the membrane with
deionized water. For these coagulants it is
possible to rinse the membrane using deionized
water and obtain the volumetric flux insignif-
icantly different from the volumetric flux for the
new membrane. In the case of applying the
coagulant FeCl3 the situation is just the opposite.
No investigations have been undertaken con-
cerning the size of the particles which are formed
in the course of coagulation, but it is to be
supposed that the particles formed when FeCl3 is
used penetrate the pores inside the structure of
the ultrafiltration membrane.
157
removal of organic matter
unit process of ultrafiltration and three groups of
results for hybrid in-line processes with three
coagulants applied. The differences between the
concentration of the investigated matter in raw
calculated, as well as the corresponding mean
retention coefficients.
In order to find out if there are any differences
between the decrease of concentration of the
investigated substances when various coagulants
are used, the differences between the concentra-
tion of the raw water and of the permeate have
been analyzed statistically. As the results obtained
did not meet the assumptions concerning the
normal distribution (result of the Shapiro-Wilk
test: p B 0.05), Kruskal
Walliss sum rang test
/
was applied, which is a nonparametric equivalent
of the variance analysis [17]. The null hypothesis
H0 assumes an equality of the mean values in the
respective groups, whereas the alternative hypoth-
esis H1 assumes that not all mean values are
equal. The necessity of assuming the null
hypotheses would mean that there is no statisti-
cally significant difference in running the process
with various coagulants, i.e. regardless of the kind
and dose of the coagulant, the effect remains the
same. In all the tests the significance level a  /
0.05 was assumed.
The highest values of the retention coefficients
of the parameters indicating the presence of
organic matter in the water could be observed in
case of applying the aluminum coagulant (Fig. 3).
It is, therefore, to be assumed that it is the most
effective coagulant. Taking, however, into ac-
count that the differences between the retention
coefficients amount from only a few to a score of
percent, it seemed to be proper to apply the
Kruskal
Wallis test in order to determine, to what
extent these differences are statistically important.
158 K. Konieczny et al. / Desalination 240 (2009) 151
159

100
lants could be compared without faking the test
Retention coefficient R (%)

80
results.
60 The results of measurements confirmed by a
40 statistical test, permit to classify the coagulants
20
according to their effectiveness as follows:
Al2(SO4)3, Fe2(SO4)3 and FeCl3. The application
0
Turbidity COD
with KMnO4
Absorbance
254nm
TOC COD of the coagulant FeCl3 in order to remove
organic matter as TOC seems to be less effective
without coagul. FeCl3 Fe2(SO4)3 Al2(SO4)3
than the application of a single UF process. The
Fig. 3. Comparison the retention coefcients of organic
situation is similar in the process of removing
substances in water for all investigated processes. substances denoted as COD by means of the
coagulant Fe2(SO4)3. It may be caused by the
The results of such a test concerning the character of the filtrate cake formed on the
ultrafiltration membrane (PES) have been pre- membrane surface which is probably more
sented in Table 6. Taking into account the porous in case of the use of coagulants.
probability level of the test a 0.05%, it may /

be said that in almost all the cases p Ba, which /

5. Conclusions
enables to reject the null hypothesis stating the
1. Application of in-line coagulation before
lack of differences between the mean values in
ultrafiltration improve the removal of
the groups. This means that, excepting the
organics, if compare with ultrafiltration
removal of compounds denoted as COD, the
alone.
choice of the proper coagulant affects the quality
2. The intensity of membrane fouling depends
of the permeate. It ought to be stressed that only on the kind of coagulant applied.
differences of raw water-permeate for processes 3. The statistical analysis of the obtained
run with in-line coagulation have been tested, results permit to classify effectiveness of
which means that in statistical calculations the the coagulants as Al2(SO4)3 Fe2(SO4)3 
/ /

single process of coagulation was not taken into FeCl3.

account, so that the effectiveness of the coagu-

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