Water Air Soil Pollut (2013) 224:1682

DOI 10.1007/s11270-013-1682-2

Ultrafiltration Combined with Coagulation/Flocculation/

Sedimentation Using Moringa oleifera as Coagulant to Treat
Dairy Industry Wastewater
Dalila Maria Formentini-Schmitt & Álvaro Cesar Dias Alves &
Márcia Teresinha Veit & Rosângela Bergamasco &
Angélica Marquetotti Salcedo Vieira & Márcia Regina Fagundes-Klen

Received: 3 April 2013 / Accepted: 26 July 2013 / Published online: 13 August 2013
# Springer Science+Business Media Dordrecht 2013

Abstract Direct ultrafiltration and its combination with
pretreatment by coagulation/flocculation/sedimentation
using Moringa oleifera as coagulant to treat dairy in-
dustry wastewater were investigated. A single-channel
tubular ceramic membrane with an average porosity of
0.1 μm was used at transmembrane pressures of 1, 2,
D. M. Formentini-Schmitt : Á. C. D. Alves : M. T. Veit :
M. R. Fagundes-Klen
Department of Chemical Engineering, Postgraduate
Program, NBQ, Western Paraná State University,
Campus de Toledo, Rua da Faculdade, 645, Jd. Santa Maria,
85903-000 Toledo, Paraná, Brazil
D. M. Formentini-Schmitt
e-mail: dalila_formentini@hotmail.com
Á. C. D. Alves
e-mail: alv_dias@yahoo.com.br
M. T. Veit
e-mail: marcia_veit@yahoo.com.br
M. R. Fagundes-Klen
e-mail: fagundes.klen@gmail.com
and 3 bars, using the cross-flow filtration principle in
a membrane filtration unit. Process efficiency was eval-
uated in terms of chemical oxygen demand (COD),
apparent color, and turbidity removal, along with ma-
jor requirements such as average permeate flux, per-
centage of fouling, and contribution of different resis-
tances (resistances in series model) to the total resis-
tance of the membrane. The highest removals for the
evaluated parameters occurred in the combined coag-
ulation/flocculation/sedimentation/ultrafiltration pro-
cess. At a pressure of 2 bar, the removal of turbidity
and apparent color was 99.9 % and that of COD was
98.5 %. For the combined process, the lowest percent-
age of fouling was 59.8 %, which occurred at 1 bar.
The fraction of resistance due to fouling, which may
indicate irreversible damage of the membrane, was
lower in the process of coagulation/flocculation/sedi-
mentation using M. oleifera as coagulant followed by
ultrafiltration than in the process that treated dairy
wastewater with direct ultrafiltration for all pressures.

R. Bergamasco Keywords Moringa oleifera . Coagulation/

Department of Chemical Engineering, flocculation . Ultrafiltration . Dairy
State University of Maringá, wastewater . Membrane fouling
Av. Colombo, 5790, 87020-900 Maringá, Paraná, Brazil
R. Bergamasco
e-mail: rosangela@deq.uem.br
1 Introduction
A. M. S. Vieira (*)
Department of Food Engineering,
State University of Maringá,
The requirements regarding control of environmental
Av. Colombo, 5790, 87020-900 Maringá, Paraná, Brazil pollution have grown exceptionally in many countries
e-mail: angelicamsalcedo@hotmail.com in recent years. Therefore, wastewater treatment is very
1682, Page 2 of 10
important and deserves special attention in industry.
Wastewater from dairy industry contains milk residues,
proteins, carbohydrates, fats, and residual cleaning
agents (László et al. 2009).
In the dairy industry, process water produced in the
starting, equilibrating, stopping, and rinsing of the
processing units generate a large volume of effluents,
which contain diluted fractions of the products pro-
cessed by this type of industry, and contribute signifi-
cantly to the total wastewater production (Balannec
et al. 2002). According to Tchamango et al. (2010),
the volume may vary from 0.2 to 10 L of wastewater
per liter of processed milk.
Dairy industry wastewater is considered highly pol-
luting not only due to the large volume, but also due to
its physicochemical characteristics, such as high chem-
ical and biochemical oxygen demand (COD and
BOD), high concentration of nutrients and solids in
suspension (Kushwaha et al. 2010), and a considerable
variation in pH from 2 to 12 (Sengil and Özacar 2006).
All the aforementioned factors demonstrate the com-
plexity required for the treatment of this wastewater and
the need for studies using modern and innovative treat-
ment techniques, considering environmental sustain-
ability, as the treatment techniques applied to this type
of wastewater are usually associated with treatment
processes that combine traditional physical or physico-
chemical treatment with biological treatment, presenting
disadvantages such as high energy demand and difficul-
ty of operation (Kushwaha et al. 2010). This justifies the
increasing search for systems that meet the standards
regarding the quality of treated wastewater.
Another disadvantage of the conventional treatment
based on a physicochemical step using inorganic co-
agulants is the generation of large volumes of nonbio-
degradable sludge due to the presence of metals such as
aluminum and iron. For this reason, alternatives have
been researched for these inorganic coagulants, like the
use of natural coagulants (Vieira et al. 2010).
The use of the extract of Moringa oleifera seeds, a
plant from India, as natural coagulant for water treat-
ment has been widely studied. This coagulant shows
turbidity removal ranging from 80 to 99 % (Bhatia
et al. 2007); 90–99 % of bacteria can be removed
(Muyibi and Evison 1995).
The coagulating effect of M. oleifera seeds is asso-
ciated with the presence of densely charged cationic
proteins with molecular weight from 6 to 16 kDa and
isoelectric pH of 10 (Ndabigengesere et al. 1995). M.
Water Air Soil Pollut (2013) 224:1682
oleifera practically does not change pH and conductiv-
ity of the treated water and produces smaller volume of
sludge, whose disposal poses no problem (Bhatia et al.
2007).
If the coagulant is extracted from the seeds using
concentrated salt solutions (1 mol L−1), its efficiency in
terms of residual turbidity is about seven times higher
than that of the coagulant extracted with distilled water
(Okuda et al. 2001).
The physicochemical step of coagulation/floccu-
lation/sedimentation alone is not enough to remove
the amount of pollutants necessary to meet the stan-
dards for releasing treated wastewater into receiving
water bodies, thus the study of a subsequent step is
required.
Ultrafiltration (UF) is a membrane separation pro-
cess that has been widely studied for water and waste-
water treatment. Its main feature is the retention of
suspended solids, colloids, and macromolecules, in
addition to constituting a complete barrier for microbi-
al species of human health concern (Ravazzini et al.
2005), and therefore the quality of the water obtained is
higher than that from conventional processes.
The implementation of environmental legislation
with more and more restrictive emission standards
and the shortage of drinking water leading to the need
for water reuse are important enough reasons for using
an advanced technique like UF for wastewater treat-
ment (Sánchez-Sánchez et al. 2010).
Purified water produced by membrane treatment
could be reused in the dairy industry as heating/cooling
water, boiler make-up water, or for cleaning purposes
(Vourch et al. 2008). Membrane filtration is an effec-
tive method of COD reduction, but the proteinaceous
material in this type of residue causes severe mem-
brane fouling, reducing dramatically the permeate flux
(László et al. 2009).
According to Bergamasco et al. (2011), factors
such as concentration polarization, cake formation,
solute adsorption, and plugging of the pores are also
responsible for the decline in permeate flux by intro-
ducing additional resistance during the ultrafiltration
process. Resistance-in-series models that consider in-
trinsic membrane resistance, adsorption resistance,
concentration polarization resistance, and cake resis-
tance have been applied in the description of such
processes.
There are few studies that use pretreatment for waste-
water from the dairy industry prior to the membrane
Water Air Soil Pollut (2013) 224:1682
separation process (László et al. 2009; Sarkar et al.
2006) in order to mitigate the effects of fouling on the
process, so this study aims to assess the combined
process of coagulation/flocculation/sedimentation using
coagulant extracted from M. oleifera followed by ultra-
filtration in the treatment of wastewater from dairy
industry and to compare this process with direct
ultrafiltration.
The efficiency of the processes was evaluated in
terms of apparent color, turbidity, and COD reduction,
and percentages of fouling and resistances in series for
the combined and direct processes at different working
pressures in ultrafiltration.
2 Materials and Methods
2.1 Wastewater Characterization
The wastewater used in the experiments came from the
washing of the pasteurizers and was collected at the
entrance of the treatment plant of a typical dairy indus-
try in the western region of Parana State, Brazil. A
single sample was collected and then homogenized,
fractionated, and suitably stored under refrigeration
for subsequent use. The sample was characterized by
physicochemical parameters—apparent color and
COD (HACH DR/2010 spectrophotometer) and tur-
bidity (HACH 2100 P turbidimeter)—immediately af-
ter collection and after the coagulation/flocculation/
sedimentation/ultrafiltration and direct ultrafiltration
tests.
All experiments to determine the physicochemical
parameters were performed in triplicate and followed
the methodology of the Standard Methods for the Ex-
amination of Water and Wastewater (APHA 1994).
Table 1 presents the characteristics of a sample of the
dairy industry wastewater.
Table 1 Physicochemical characteristics of dairy industry
wastewater
Parameter Value
Apparent color (mgPt-CoL−1) 5,544
Turbidity (NTU) 897
COD (mgO2L−1) 3,190
Page 3 of 10, 1682
2.2 Coagulation/Flocculation/Sedimentation
Experiments
The coagulant solution was prepared by grinding 5 g of
M. oleifera seeds with 100 mL of 1 mol L−1 potassium
chloride solution in a blender. The mixture was kept
under magnetic stirring for 30 min for the extraction of
the active compounds from the seeds and then filtered
under vacuum and used immediately in the coagula-
tion/flocculation tests. This procedure followed an
adapted methodology (Beltrán-Heredia et al. 2009).
The coagulant dose was taken directly from the
extract (filtered mixture). In the coagulation/floccul-
ation/sedimentation step, the following conditions were
applied: coagulant concentration of 1,500 mg L−1, rapid
mixing speed of 100 rpm for 2 min, slow mixing speed
of 20 rpm for 10 min, and settling time of 60 min (Bhatia
et al. 2007; Bhuptawat et al. 2007). The temperature was
25 °C. This treated wastewater was named coagulation/
flocculation/sedimentation (CFM) and the volume used
in the experiments was 1.2 L.
2.3 Ultrafiltration Experiments
The tests were carried out in an ultrafiltration module
(Netzsch, Fig. 1) using cross-flow filtration with a
tubular single-channel ceramic membrane of average
porosity of 0.1 μm, surface area of 0.005 m2, and
molecular weight cutoff of 4 kDa. Al2O3/ZrO2 ceramic
membranes (TAMI, France) were used in the filtration
process. The filtration module was made of stainless
steel. The system was equipped with manometers at the
inlet and outlet to control the transmembrane pressure
and connected to a thermostatic bath for temperature
control of the solution contained in the feed tank. The
output of permeate was collected by opening the valve
and the concentrate was returned to the feed tank by the
hose.
Temperature was maintained at 25 °C for the tests,
with transmembrane pressures of 1, 2, and 3 bars. The
tests were conducted using the raw dairy industry
wastewater (RDW) and that pretreated by coagulation/
flocculation/sedimentation using M. oleifera as coagu-
lant (CFM). For the combined experiments, RDW
underwent coagulation/flocculation/sedimentation in
jar test before being subjected to ultrafiltration. A peri-
staltic pump was used to transfer 10 L of CFM from the
jar test to the ultrafiltration module. Then, the
1682, Page 4 of 10 Water Air Soil Pollut (2013) 224:1682

suspension was allowed to percolate through the mem-
brane system as shown in Fig. 1.
The initial permeability of the membrane at different
pressures (1, 2, and 3 bars) was determined, as well as
the filtration profile that was divided into three stages:
initial flux (reverse osmosis water (ROW)), flux of the
solution to be treated (RDW or CFM), and final flux
(ROW). Each step had an estimated time of 180 min.
Lastly, the final permeability was determined.
The permeate flux (J) was calculated in predeter-
mined time intervals. It depends on the mass of permeate
(m) collected during a certain period of time (Δt), the
density (ρ) of the solution to be treated at 25 °C, and the
membrane area (Am) according to Eq. (1):


J L: h−1 :m−2 ¼ ½ðm=ρ25 C Þ=Δt: Am ð1Þ
membrane clogging and consequent reduction of per-
meate flux. The total resistance (Rt) is obtained by
adding the different resistances, that is, Rm, concentra-
tion polarization resistance (Rc) due to the deposition
of a layer of solute on the membrane surface, and
fouling resistance (Rf), which is caused by solute ad-
sorption in the membrane pores and walls. The resis-
tances were calculated through Eqs. (4) to (7):
Rt ¼ Rm þ Rc þ R f ð4Þ
Rm ¼ ΔPT =ðη: J initial Þ ð5Þ

ROW flux (Jinitial and Jfinal) was assessed at the

beginning of the experiment and after determining the
flux with RDW or CFM. Time intervals after stabiliza-
tion of the permeate flux (from 70 to 180 min) were
used to determine membrane fouling according to
Eq. (2).
% fouling ¼ ½1–ð J final =J initial Þ  100
The resistance in series model used by Bergamasco
et al. (2011) was applied to evaluate the filtration
characteristics. The intrinsic membrane resistance
(Rm), also known as hydraulic resistance, was calculat-
ed from data obtained during ROW filtration. ROW
flux (Jinitial) is shown in Eq. (3), where ΔPT is the
transmembrane pressure (working pressure), and η is
the dynamic viscosity of the permeate.
J initial ¼ ΔPT =ðη: Rm Þ
Fouling and concentration polarization of the solute
at the surface of the membrane are responsible for
R f ¼ ΔPT =ðη: J final Þ–Rm ð6Þ


Rc ¼ ΔPT =ðη: J Þ– Rm þ R f ð7Þ
ð2Þ
In order to better understand the permeate flux pro-
files, the relative flux was calculated by Eq. (8)
according to Reddy et al. (2005). The relative flux
allows rapid evaluation of how much the permeate flux
of RDW and CFM has decreased in comparison with
the initial ROW flux.
% relative flux ¼ ð J = J initial Þ  100 ð8Þ
ð3Þ The percentage of membrane fouling, as well as its
resistances, related with the process efficiency in terms
of apparent color, COD, and turbidity removal, were
used to determine the best working condition.

Fig. 1 Schematic diagram

of the micro/ultrafiltration
experimental unit. 1 Ther-
mostatic bath, 2 feed tank, 3
pump, 4 manometers, 5
membrane filtration module,
6 flowmeter (rotameter), 7
permeate, 8 concentrate
Water Air Soil Pollut (2013) 224:1682
3 Results and Discussion
Table 2 shows removal efficiencies in terms of appar-
ent color, turbidity, and COD reduction for the raw
dairy industry wastewater directly subjected to ultrafil-
tration (RDW-UF) and for the wastewater pretreated by
coagulation/flocculation/sedimentation prior to ultra-
filtration (CFM-UF) at different transmembrane pres-
sures (1, 2, and 3 bars). The efficiency of the coagula-
tion/flocculation/sedimentation pretreatment using the
coagulant extracted from M. oleifera seeds (CFM) is
also shown.
According to Table 2, the coagulation/flocculation/
sedimentation pretreatment with M. oleifera showed
high efficiencies of turbidity and apparent color remov-
al. However, it is apparent that this process was not
efficient for COD removal as the COD value obtained
after pretreatment was 1,933.1 mg L−1, which is too
high for disposal into receiving water bodies, justifying
the need for a subsequent treatment such as ultrafiltra-
tion to fit this parameter to the current disposal stan-
dards. The results also showed that separation by ul-
trafiltration provided removals exceeding 96 % for all
evaluated parameters and at all conditions studied. It
should be highlighted the significant increase in COD
removal, from only 39.4 % in the CFM process to more
than 96 % in the ultrafiltration processes.
Similar results of COD removal were obtained by
Sarkar et al. (2006) who used wastewater from dairy
industry in their experiments, testing chitosan
(10 mg L−1) at pH 4 for the coagulation/flocculation
step, followed by adsorption with powdered activated
charcoal (1.5 g L−1), which has improved color and odor
removal. The pretreated wastewater subsequently
underwent a tertiary treatment of reverse osmosis, in
which a reduction of 98 % in COD was achieved.
In the present study, pH adjustment was not neces-
sary for the coagulation/flocculation/sedimentation
pretreatment with M. oleifera. Therefore, fewer steps
were used (CFM-UF or RDW-UF); ultrafiltration is a
Table 2 Removal efficiencies
for CFM, CFM-UF, and RDW- Parameter CFM %
UF at different pressures
Apparent color 93.3
Turbidity 97.6
COD 39.4
Page 5 of 10, 1682
cheaper separation process as it uses lower pressures
than reverse osmosis.
In the process of direct UF of the wastewater with-
out pretreatment (RDW-UF), apparent color and tur-
bidity removal was above 99.3 % even with pressure
variation. COD reduction varied between 96.1 and
98 %.
Figures 2, 3, and 4 present filtration profiles
obtained during the experiments showing a reduction
in the permeate flux over time. These profiles showed a
steep decline in permeate flux at the initial period of
ultrafiltration. After a certain time, which was charac-
teristic of each test, permeate flux remained stable until
the end of the test.
Increasing the pressure enabled an increase in flux
for all tests (CFM-UF and RDW-UF). This result is in
accordance with Bergamasco et al. (2011), who have
reported that an increase in flux is expected when
pressure is increased, particularly at the beginning of
ultrafiltration when there is no formation of a gel layer
on the membrane.
ROW is only subject to the intrinsic resistance when
passing through the membrane during the initial ultra-
filtration process as it is pure water. RDW and CFM, on
the other hand, have particles that must be removed
and that accumulate on the membrane surface or ob-
struct membrane pores, so the flux of these substances
is much lower than that of ROW.
Table 3 shows the relative flux values obtained by
Eq. (8) after certain time intervals during the ultrafil-
tration tests. The relative fluxes of RDW and CFM at
the beginning of the experiments ranged between 40
and 64 %. Stabilized fluxes occurred after 25 min, on
average, and remained between 14 and 26 %.
The observation of the relative fluxes shown in Ta-
ble 3 aided in the evaluation of data presented in Figs. 2,
3, and 4 as they clearly demonstrated the decrease in
permeate flux of RDW and CFM in comparison with
ROW flux. According to Reddy et al. (2005), this is
due to blocking of the larger pores of the membrane
CFM-UF % RDW-UF %
1 bar 2 bar 3 bar 1 bar 2 bar 3 bar
100.0 99.9 99.8 99.9 99.3 99.7
99.9 99.9 99.8 99.9 99.6 99.8
96.1 98.5 98.3 96.1 97.2 98.0
1682, Page 6 of 10
Fig. 2 Filtration profiles for
CFM-UF and RDW-UF at
1 bar
caused by solute molecules present in RDW and CFM.
Higher relative flux was expected for CFM—as it was
pretreated—than for RDW, but this was only observed
in the first minutes of the experiments.
The increase in pressure allowed an increase in
permeate flux, but did not significantly alter the rela-
tive flux as RDW and CFM fluxes increased propor-
tionally to the ROW fluxes of the respective tests. The
largest relative flux occurred in the experiment with
CFM at 1 bar.
The average permeate flux of RDW-UF (calculated
between 50 and 150 min) was higher than that of CFM-
UF for the three pressures studied as shown in Table 4.
The major difference between the average permeate
fluxes was observed at the pressure of 1 bar in which
the RDW-UF flux was approximately 27 % higher than
that of CFM-UF. The increase in pressure increased the
average fluxes and decreased the difference between
Fig. 3 Filtration profiles for
CFM-UF and RDW-UF at
2 bar
Water Air Soil Pollut (2013) 224:1682
RDW-UF and CFM-UF, which reached approximately
9 % at 3 bar.
Membrane fouling is an inevitable drawback of the
separation process. However, it can be minimized, and
the lower the fouling rate, the more advantageous the
process.
The different pressures and solutes used in the tests
had a significant influence on the characteristics of
membrane fouling. Figure 5 shows the percentage of
fouling for the RDW-UF and CFM-UF processes, with
different transmembrane pressures (1, 2, and 3 bars).
It is clear from Fig. 5 that the increase in membrane
fouling was not proportional to the increase in pres-
sure. These results are in disagreement with
Bergamasco et al. (2011) who found in their studies
that the increase in pressure promoted an increase in
permeate flux and intensified the effect of fouling.
Turan (2004) also observed that the permeate flux
Water Air Soil Pollut (2013) 224:1682 Page 7 of 10, 1682

Fig. 4 Filtration profiles for

CFM-UF and RDW-UF at
3 bar

increased with the increase in transmembrane pressure.
However, this positive effect was reduced when the
feed solution had higher COD and therefore, according
to the author, higher concentration of pollutants that
cause fouling.
The percentages of fouling observed in Fig. 5 were
lower for CFM-UF than for RDW-UF at all pressures.
COD removal (Table 2) was higher for CFM-UF than
for RDW-UF at 2 and 3 bars; at 1 bar, it was the same
for both processes. As for the average permeate flux,
the values shown in Table 4 were lower for CFM-UF
than for RDW-UF at all pressures.
Nevertheless, the above observation represents an
advantage for the combined CFM-UF process. In a
similar study by Katayon et al. (2007), using M.
oleifera as a coagulant followed by microfiltration for
wastewater treatment, the combination of the methods
improved permeate flow and reduced membrane foul-
ing, but no further removal of the evaluated parameters
was obtained. On the other hand, Bergamasco et al.
Table 3 Relative flux for RDW-UF and CFM-UF over time at
different pressures
Relative flux (%)
(2009), studying surface water treatment, observed that
although the quality of treated water was improved, no
gain was obtained in the performance of the mem-
brane, as in this case there was an increase in mem-
brane fouling.
In ultrafiltration, the mechanism of membrane ob-
struction must be taken into account. This mechanism
causes a drop in permeate flux and is the result of phe-
nomena (Bergamasco et al. 2011) that are mainly re-
lated to the characteristics of the membrane (hydropho-
bicity, charge, surface roughness, and porosity), oper-
ating conditions of the membrane system (constant
working pressure and flux), and quality of the feed
water (physicochemical and microbiological character-
istics), as well as the hydrodynamics of the membrane
system which is characterized by the permeate flux and
the cut surface. Among the most relevant physico-
chemical characteristics is the amount of organic mat-
ter present in the feed water which is a primary con-
tributor to membrane fouling (Guo et al. 2010).
The mechanisms commonly attributed to organic
matter removal by ultrafiltration are sieve retention—
particles are retained on the membrane surface and
form a cake that grows in thickness as the filtration

RDW-UF CFM-UF
Table 4 Average permeate flux for RDW-UF and CFM-UF at
Time (min) 1 bar 2 bar 3 bar 1 bar 2 bar 3 bar different pressures

0.25 49 40 40 64 41 40 Process Average permeate flux (L h−1 m−2)

10 34 24 23 26 28 25
1 bar 2 bar 3 bar
25 27 20 24 28 19 19
50 26 18 23 23 16 19 RDW-UF 80.4 96.4 132.3
150 26 15 22 16 14 18 CFM-UF 59.0 85.4 120.1
1682, Page 8 of 10 Water Air Soil Pollut (2013) 224:1682

resistance observed in ultrafiltration using RDW and

CFM at 1, 2, and 3 bars. Comparing Rf at different
pressures in Table 5, it can be observed that it was
higher for RDW-UF than for CFM-UF. As for Rc, it
was higher for CFM-UF than for RDW-UF at all pres-
sures. As stated by Guo et al. (2009), concentration
polarization resistance is more easily removed than
fouling resistance, which can be irreversible. There-
fore, the combined CFM-UF process was found to be
appropriate to increase membrane lifetime.
As shown in Table 5, total resistance increased with
Fig. 5 Percentage of fouling for the tests with RDW-UF and increasing transmembrane pressure. This is due to the
CFM-UF at different pressures higher compression according to Bergamasco et al.
(2011). Table 6 shows the contributions of the different
progresses—and adsorption sequestration, which in- resistances to the total resistance of the membrane in
volves input and capture of particles into the membrane the RDW-UF and CFM-UF processes at 1, 2, and
matrix, allowing the removal of particles smaller than 3 bars. Rf had the greatest contribution to total resis-
the pores of the membrane (Guo et al. 2009). tance in the case of direct ultrafiltration of raw dairy
For Guo et al. (2009), the direct filtration of natural wastewater. In the combined process, Rc contributed
organic matter by ultrafiltration is through adsorption the most to the total resistance, except at 2 bar when Rf
sequestration, which causes severe membrane fouling had a slightly greater contribution.
that is not easy to remove and is often irreversible. If Tables 5 and 6 demonstrated that the use of M.
coagulation is combined with ultrafiltration, the fine oleifera for coagulation prior to ultrafiltration de-
particles are deposited on the membrane surface by creased Rf and increased Rc. Rc is easier to remove than
concentration polarization, which is considered as re- Rf and contributed with 60.1 % of Rt at 1 bar, 40.9 % at
versible fouling and is easy to clean by physical methods 2 bar, and 50.8 % at 3 bar in the CFM-UF process.
as the filtration progresses. Therefore it is important to Cross-flow filtration prevents excessive concentra-
note in Tables 5 and 6 the influence of different resis- tion of material on the membrane surface as most of the
tances on the ultrafiltration of RDW and CFM at differ- feed stream just passes along the membrane and is
ent pressures (1, 2, and 3 bars) and the relative contri- recirculated to the feed tank. The shear stress tangential
butions of each resistance to the total resistance in each to the membrane surface helps to reduce fouling phe-
process. nomena (Ravazzini et al. 2005). This can also be seen
Table 5 shows the results obtained through the re- in Tables 5 and 6, as the contribution of Rc to Rt for
sistances in series model for the different types of CFM was greater at 1 bar than at the other pressures.
Possibly due to different physicochemical characteris-
Table 5 Membrane resistances during ultrafiltration of RDW
and CFM at 1, 2, and 3 bars
tics of RDW and CFM solutes, the pressure of 1 bar
allowed a greater accumulation of material on the
Process Resistance×1012 (m−1) membrane for CFM than for RDW, and this effect
was minimized by increasing the pressure, that is, a
Rm Rf Rc Rt
higher pressure increased the flux and did not allow the
RDW-UF formation of such a thick cake layer on the membrane.
ΔP=1 bar 1.36 2.16 1.63 5.15 Lee et al. (2009) stated that permeability reduction
ΔP=2 bar 1.37 4.53 3.31 9.21 in ultrafiltration, when mainly attributed to cake for-
ΔP=3 bar 1.91 4.08 3.93 9.92 mation on the membrane surface, exhibits dual func-
CFM-UF tions while acting as a protective barrier for membrane
ΔP=1 bar 1.36 1.93 4.96 8.25 fouling in that it provides additional resistance to per-
ΔP=2 bar 1.37 4.26 3.90 9.53
meation. A similar behavior was observed in the pres-
ΔP=3 bar 1.91 3.30 5.38 10.58
ent study as the relative contribution of Rf to Rt at 1 bar
for CFM was the lowest in all experiments, and
Water Air Soil Pollut (2013) 224:1682
Table 6 Relative contributions
of the different resistances to the ΔP (bar) RDW-UF
total membrane resistance during
ultrafiltration of RDW and CFM %Rm
at 1, 2, and 3 bars
1 26.4±0.3
2 14.9±0.2
3 19.2±0.2
consequently the permeate flux under these conditions
was also the lowest one.
Stoller (2009) pointed out that the flocculation
process—due to reduction of solute concentration by
sedimentation and particle size shifts—can significantly
influence fouling. Therefore, the author suggests that the
flocculation process as pretreatment for membrane op-
eration must be optimized to not produce aggregates
whose dimensions are similar to the pore size. Different
coagulants perform different particle size shifts; this
should be considered in any membrane filtration process
using coagulation/flocculation as a pretreatment.
The results obtained in the ultrafiltration processes
using RDW and CFM were similar, although superior
performance was expected for the ultrafiltration pro-
cess combined with coagulation/flocculation using M.
oleifera when compared with direct ultrafiltration
according to some reports (Turan 2004; Sarkar et al.
2006; Katayon et al. 2007; László et al. 2009; Stoller
2009; Bergamasco et al. 2011).
As dairy industry wastewaters contain particles of
high molecular weight (milk proteins, fat, and whey
protein) and minerals like calcium and phosphorus,
milk-derived substances (which had been coagulated
and settled) may have been partially substituted for
substances from the M. oleifera. The use of a M.
oleifera coagulant dosage of 1,500 mg L−1 with a
highly concentrated saline solution (1 mol L−1) and a
membrane with molecular weight cutoff of 4 kDa
could explain the similar performance of both process-
es (RDW-UF and CFM-UF), in which despite the
increase in pressure, there were no significant changes.
With the evaluation of data such as average perme-
ate flux and total resistance, the direct ultrafiltration
process with RDW was found to be more effective. In
contrast, the better removals obtained with CFM-UF,
the lower percentage of fouling, and the Rc values,
which provided important information about the type
of fouling that can occur (reversible or irreversible), are
advantages of the CFM-UF process.
Page 9 of 10, 1682
CFM-UF
%Rf %Rc %Rm %Rf %Rc
41.9±0.5 31.7±0.6 16.5±0.1 23.4±0.3 60.1±1.6
49.2±0.0 35.9±0.1 14.4±0.2 44.7±0.4 40.9±0.8
41.2±0.4 39.6±0.6 18.0±0.4 31.2±0.3 50.8±1.0
Importantly, M. oleifera emerged as a natural coag-
ulant for this type of wastewater, as the sludge gener-
ated in the coagulation/flocculation/sedimentation pro-
cess is biodegradable, unlike the sludge generated in
the processes that use inorganic coagulants. Coagula-
tion/flocculation using M. oleifera can be a pretreat-
ment for a biological treatment or ultrafiltration. The
choice should be based on the quality required for the
treated water, which may be disposed into a receiving
body of water or reused (irrigation, industrial water).
For reuse purposes, regardless of the process
(RDW-UF or CFM-UF), ultrafiltration stands out as
an alternative to conventional treatments used for
wastewater from the dairy industry, because the quality
of the treated water is much higher than that obtained
with conventional treatments.
4 Conclusions
Direct ultrafiltration and its combination with pretreat-
ment by coagulation/flocculation/sedimentation using
M. oleifera as coagulant under the optimum conditions
determined in the coagulation/flocculation tests achieved
good results regarding COD removal, exceeding 96 % at
all pressures (1, 2, and 3 bars).
The highest removals for the evaluated parameters
were obtained in the coagulation/flocculation/sedimenta-
tion process combined with ultrafiltration, especially at
higher pressures. At 2 bar, the removal of turbidity and
apparent color was 99.9 % and that of COD was 98.5 %.
& For the combined CFM-UF process, the lowest
percentage of fouling was obtained at 1 bar.
& The fraction of resistance due to fouling (%Rf),
which may cause irreversible damage of the mem-
brane, was lower in the CFM-UF process than in
the RDW-UF process at all pressures.
The combined CFM-UF process showed many ad-
vantages over conventional processes, as besides
1682, Page 10 of 10
ensuring superior quality of treated water, it enables the
reuse of treated water for purposes other than potable
water within the dairy industry, reducing the consump-
tion of drinking water, which is a major environmental
problem of this type of industry.
Acknowledgments The authors thank CNPq–National Coun-
cil for Scientific and Technological Development and Araucaria
Foundation for Support to Scientific and Technological Devel-
opment of Paraná for the financial support.
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