Chemosphere 206 (2018) 142e149

Contents lists available at ScienceDirect

Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere

A novel use of Moringa oleifera seed powder in enhancing the primary

treatment of paper mill effluent
Soumia Boulaadjoul a, Hassiba Zemmouri a, Zoubida Bendjama a, Nadjib Drouiche b, *
a
Laboratoire des Sciences et de Genie des Proc

ed

es Industriels, Facult

e de G
enie M
ecanique et de G

enie des Proc

ed

es, (USTHB), BP 32, 16111 Algiers, Algeria
b
Centre de Recherche en Technologie des Semi-conducteurs pour l’Energ
etique, 2, Bd Frantz Fanon BP140 Alger-7-merveilles, 16038 Alger, Algeria

a r t i c l e i n f o a b s t r a c t

Article history: In this study, Moringa oleifera (M. oleifera) performance as an eco-friendly coagulant in the enhanced
Received 7 October 2017 primary treatment of paper mill effluent was investigated. Its performance in terms of turbidity removal
Received in revised form and COD abatement was examined. Local M. oleifera seed powder from ADRAR-city, South of Algeria, was
17 April 2018
used. Conventional jar tests were conducted for enhancing the primary treatment of paper mill effluent
Accepted 20 April 2018
from paper factory. For this reason, comparative coagulation tests were performed using aluminum
Available online 2 May 2018
sulfate (alum). Indeed, in terms of turbidity abatement, 96.02% and 97.1% were obtained for Moringa and
Handling Editor: W Mitch alum, respectively. However, in the case of COD abatement, the abatement rate of M. oleifera seeds was
slightly higher than that of alum, 97.28% and 92.67%, respectively. Because M. oleifera is a natural resource
Keywords: that is locally available, an eco-friendly coagulant, non-toxic, and biodegradable and does not affect the
Alum pH of water; thus, its use allows to avoid numerous disadvantages of conventional coagulants like alum.
Coagulation-flocculation © 2018 Elsevier Ltd. All rights reserved.
M. oleifera
Paper mill effluent
Primary treatment

1. Introduction
Generally, paper mill wastewater contains organic and inorganic
materials that are sometimes very toxic. Such components are
dispersed (colloids) in solution, in suspension or in emulsion (polar
molecules) form. Pulp and paper is among the most polluting in-
dustries, which cause worldwide environmental damages (Guo
et al., 2016). In fact, pulp and paper mill effluent is highly toxic
and the major source of aquatic pollution. The chemical composi-
tion of the paper mill effluent forms and diversifies according to the
different stages of the paper making process: (i) during the pulping
process, effluents are enriched by tannins, resin acids, unsaturated
fatty acids, diterpene alcohols, juvaniones, chlorinated resin acids,
and other chemicals and (ii) during the bleaching stage of the pulp,
a large number of pollutants such as chlorate ions, dioxins, furans,
chlorophenols, acetone, sulfur and sulfur compounds, and many
others, considered as the more dangerous chemicals, are added to
* Corresponding author. Technology of Semi-conductor for the Energetic
Research 11 Center Department of Environmental Engineering 2, Bd Frantz Fanon
BP140 Alger-7-merveilles, Algiers, Algeria.
E-mail addresses: hassiba_zemmouri@yahoo.fr (H. Zemmouri), nadjibdrouiche@
yahoo.fr (N. Drouiche).
the paper mill effluents (Pokhrel and Viraraghavan, 2004). Some of
the pollutants, namely polychlorinated dibenzodioxins and di-
benzofurans dioxins and furans, are recalcitrant to degradation; (iii)
during the final stage, which is related to the use of dyes in printing
and staining, heavy metals such as cadmium, copper, zinc, and
chromium are added. The chemical composition of paper mill
effluent is expressed by the visual color and very high levels of
biochemical oxygen demand (BOD) and chemical oxygen demand
(COD), due to the presence of lignin and its derivatives from raw
cellulosic materials, chlorinated compounds, suspended solids
(mainly fibers, fibrils, CaCO3, clays), etc.
Actually, the elimination of such potential environmental
disturbance, in a perspective of sustainable development, is an
important target for industrial and developed countries. Indeed,
several physical, chemical, and biological techniques such as
electro-coagulation (Deepak, 2014), biodegradation (Sharma et al.,
2014), moving bed biofilm reactor (MBBR) process (Oliveira, 2014),
and nanofiltration process (Beril Go € nder et al., 2011) are used to
purify paper mill effluents. In this respect, coagulation-flocculation
remains a promising process due to its technical and economic
simplicity; coagulation-flocculation is the most frequently used
process alone or in combination with other methods for paper
effluent treatment (Choudhary et al., 2015). The coagulants most

https://doi.org/10.1016/j.chemosphere.2018.04.123
0045-6535/© 2018 Elsevier Ltd. All rights reserved.
 S. Boulaadjoul et al. / Chemosphere 206 (2018) 142e149 143

commonly used are metal salts such as iron and aluminum. removal efficiency of color, turbidity, and UV-254 nm occurred with
Although these types of coagulants are widely applied, they exhibit 1 M NaCl solution, with coagulant concentration between 100 and
some drawbacks such as they are of relatively high costs, affect 300 mg/L.
human health, produce a large volume of sludge, considerably In fact, literature reviews have demonstrated the efficiency of
affect the pH of treated water, and have a low coagulation efficiency M. oleifera seeds in the treatment of highly loaded effluents such as
in cold waters (Oladoja, 2015). Further, the residual amount of tannery (Kumar et al., 2016), textile (Vilaseca et al., 2014), and palm
aluminum in treated water can cause Alzheimer's disease (Flaten, oils (Bhatia et al., 2007). It was not worthwhile to note that, to our
2001). knowledge, the treatment of real paper mill effluent using this
In response to the global concerns in reducing the harmful ef- biocoagulant has not been carried out so far. Hence, our study is an
fects of chemical coagulants, naturally based materials appear to be attempt to investigate the potential of M. oleifera seed powder as a
an interesting solution. Many authors have reported that bio- natural coagulant for the enhanced primary sedimentation of paper
materials, extracted from microorganisms, animals, or plants, can mill effluent from paper factory. Local M. oleifera seed powder from
be used as natural coagulants, such as chitosan (Zemmouri et al., ADRAR city, South of Algeria, and alum were used as coagulants. In
2012), Jatropha curcas seeds (Abidin et al., 2013), and mucilagi- this respect, several coagulation-flocculation and sedimentation
nous seeds of Ocimum basilicum (Shamsnejati et al., 2015). These trials were carried out in the laboratory using a conventional
eco-friendly coagulants are characterized by biodegradability, flocculator “jar-test” apparatus. M. oleifera and alum efficiencies in
nontoxic nature, and abundance. Furthermore, the sludge produced terms of turbidity removal, COD abatement, zeta potential, and
by these biomaterials is not only innocuous but also four to five produced sludge volume were tested.
times less in volume than the chemical sludge produced by alum
(Katayon et al., 2006). 2. Materials and methods
Moreover, the Moringa tree (M. oleifera) belonging to the Mor-
ingaceae family, is native to the sub-Himalayan tracts of India, 2.1. Preparation of M. oleifera seeds powder
Pakistan, Bangladesh, and Afghanistan, grows throughout the tro-
pics. It includes about 14 species (Oladoja, 2015). It is named Local M. oleifera seed powder used in this work was purchased
“miracle tree” because of its many nutritional, medicinal, and in- from Adrar city (South of Algeria). The seeds were removed from
dustrial potential (Ndubuaku et al., 2014). the pods and stored at room temperature; the winged seed cover
The M. oleifera seed extract is used as a coagulant for water and was shelled just before the extraction (Fig. 1).
wastewater treatment in African and South Asian countries. Pre- Thereafter, the dried seeds were peeled, crushed using a
vious studies have reported that the active compound of M. oleifera homemade processor, and reduced to a fine powder using a labo-
is a soluble cationic protein having a molecular weight of about ratory blender. Five grams of the obtained powder was dissolved in
6 kDa and isoelectric pH value of 10 and 11 (Madrona et al., 2012; 1 L of 1 M NaCl solution.
Sengupta et al., 2012a; b). According to Ndabigengesere and
Narasiah (1998), M. oleifera seed powder may be a suitable eco- 2.2. Wastewater sampling
friendly coagulant that can replace aluminum and iron salts used
in water treatment. It does not significantly affect the pH and the The raw effluent samples were collected from the inlet of paper
conductivity of water after treatment (Ndabigengesere et al., 1995) factory, Tipaza city, West of Algiers, Algeria. This factory discharges
and has a bacterial removal range of 90e99% (Lea, 2010). Recently, its effluents into the sewer system of the Bousmail city and
many studies confirmed the efficiency of M. oleifera in water sometimes directly into the Mediterranean Sea (Fig. 2). The samples
treatment. de Paula et al. (2018) optimized the coagulant dosages of were collected in three plastic containers, mixed together, stored,
aluminum sulfate, ferric chloride, and M. oleifera for the treatment and refrigerated at 4  C. The effluent samples were analyzed by
of concrete plant wastewater. The authors indicated that the standard methods (APHA) to evaluate the pollution load of raw
optimal coagulant dosages were 0.47, 0.36, and 0.18 g L
1 of
M. oleifera, aluminum sulfate, and ferric chloride, respectively, with
99.9% of turbidity removal. In addition, Freitas et al., 2016 revealed
that the application of aluminum sulfate followed by water-soluble
M. oleifera seed lectin is a promising alternative for turbidity and
toxicity removal from polluted stream water. Moreover, the use of
water-soluble M. oleifera seed lectin showed a high decrease in
residual aluminum after treatment. Furthermore, Feria Díaz et al.
(2018) studied the influence of storage time on M. oleifera seed
coagulation activity using extracts prepared from 6-month- and
4.5-year stored seeds. As a main result, the storage time has prac-
tically no influence on the coagulation activity if M. oleifera seeds.
Patel and Vashi (2012) reported that M. oleifera seed powder is
better than maize seed powder and chitosan in the removal of
Congo red dye from aqueous solutions. Petersen et al., 2016 pointed
out that M. oleifera seed coagulant has significantly removed the
number of C. parvum oocysts in wastewater compared with a nat-
ural sedimentation of 90 min.
Several studies have shown that NaCl is the extracting agent of
M. oleifera protein (Okuda et al., 1999; Nkurunziza et al., 2009).
Moreover, Madrona et al. (2012) compared the efficacy of different
M. oleifera seed extracts obtained, using different concentrations of
NaCl solution (0.01, 0.1, and 1 M), as a natural coagulant in drinking
water treatment. The obtained results revealed that the highest Fig. 1. M. oleifera seeds.
144 S. Boulaadjoul et al. / Chemosphere 206 (2018) 142e149

subjected to a rapid stirring of 250 rpm for 3 min followed by a slow

stirring of 40 rpm for 30 min and a settling time of 30 min. After
sedimentation time, 20 mL of the supernatant, which was sampled
from a depth of 3 cm from each beaker, was collected to perform
analyses. The pH was adjusted with 0.1 M HCl and 0.1 M NaOH.
Assays were performed in triplicate at room temperature
(25 ± 1  C).

2.4. Zeta potential

The zeta potentials of raw paper mill effluent and the treated
one by alum and M. oleifera were determined using a Malvern
Zetasizer instrument equipped with the zeta potential cell DTS1060
at 20  C. At the end of the Jar test, a sample was taken to assess the
zeta potential of the treated solution.

2.5. Coagulation-flocculation efficiency

The efficiency of treatment was evaluated through turbidity

Fig. 2. Sampling point. (turbidity was mesured without any dilution) and COD removal
percentages, which were calculated by the following expressions:
wastewater. The different physicochemical parameters such as Turbidityraw
Turbiditytreated
temperature, pH, turbidity (measured without any dilution), con- Turbidity removal ð%Þ ¼
Turbidityraw
ductivity, chemical oxygen demand (COD), biochemical oxygen
demand for 5 days (BOD5), and total suspended solids (TSS) were  100ð%Þ (1)
analyzed. The average values of such parameters water are pre-
sented in Table 1. CODraw
CODtreated
COD removal ð%Þ ¼  100ð%Þ (2)
CODraw
2.3. Coagulation-flocculation tests

To investigate the coagulation activity of M. oleifera seed pow-

der, conventional jar-test (Brand: Janke and Hunkeler®) having six
agitators with variable speed and six trains was used. Each train
was equipped with a 1-L beaker for the enhanced primary treat-
ment of paper mill effluent from the paper factory. Comparative
coagulation trials were performed using aluminum sulfate (alum),
Al2 (SO4)3e18H2O (Merck). Jar-test beakers were filled with the
sample of untreated water, placed on the flocculator, and then
3. Results and discussion
Coagulant dosage and pH are among the important parameters
to evaluate the coagulation-flocculation process efficiency. In this
investigation, the effects of coagulant dosage and initial pH of the
untreated water on this process were studied. This allows us to
determine the optimal values of these parameters.

Table 1
Physicochemical characteristics of paper mill effluent.

Parameter Unit Average Instrument/Method

value

Color e Brown Visual


Temperature C 23 ± 2 Laboratory's thermometer
( C)
Turbidity NTU 1739 Nephelometric/Turbidimeter (HANNA INSTRUMENTS: HI 88 713 models)
Conductivity mScm
1 1988 Consort C861Multi-parameter analyzer
pH e 7.42 pH-meter (HANNA Instruments: pH211)
Alkalinity mg/L 753 Titration of sodium carbonate solution against sulfuric acid solution using phenolphthalein and methyl orange indicators.
TSS mg/L 20770 Gravimetric method, dried at 105  C
COD mg O2/ 10752 Determination by di-chromate reflux method through the oxidation of sample with potassium dichromate (K2Cr2O7) in sulfuric acid
L (H2SO4) solution followed by titration method.
BOD5 mg O2/ 600 5 days of incubation by the reduction of dissolved oxygen.
L
NO2 mg/L 0.1 According to the standard methods (APHA)
NO3 mg/L 0.3 According to the standard methods (APHA)
TP mg/L 8.61 According to the standard methods (APHA)
Cu mg/L 0.1 Determined by atomic absorption spectrophotometry (AAS)/(SpectrAAvarian 110)
Fe mg/L 2
Zn mg/L 0.5
Cd mg/L 0.05
Pb mg/L 81
Cr mg/L 0.2
 S. Boulaadjoul et al. / Chemosphere 206 (2018) 142e149
3.1. Effect of initial pH
Trials were carried out to investigate the performance of
M. oleifera seed powder for turbidity removal at different pH levels.
The pH was adjusted by the addition of HCl (0.1 M) or NaOH (0.1 M)
solutions. Fig. 3 shows the effect of initial pH on turbidity removal.
This figure shows that, at pH in the range of 6e8, 150 mg/L of
M. oleifera seed powder removed 97% of turbidity after 30 min of
decantation. The coagulation active agent of M. oleifera seed was
recognized to be a protein with cationic peptides of relatively low
molecular weight, and the proposed mechanism of coagulation
could be explained by neutralization charge. In fact, Gassenschmidt
et al. (1995) analyzed and sequenced the amino acids present in
M. oleifera seed. They found that this biopolymer revealed high
contents of glutamine, arginine, and proline, with a total of 60 other
residues. The protein has eight positively charged amino acids (7
arginines and 1 histidine) and 15 glutamine residues. Through
electrostatic interactions, negatively charged particles are attracted
by cationic charges of the M. oleifera protein. This leads to particle
collision, thus inducing neutralization of the charges and then
flocculation of suspended particles forming flocs.
Our results are in good agreement with those obtained by Bina
et al. (2007), we found that M. oleifera seed extract in treating
synthetic turbid water of kaolin, at 10e30 mg/L dosage and pH
ranging from 6 to 8, removed more than 90% of turbidity.
Yarahmadi et al. (2009) and Madrona et al. (2010) studied the ef-
fects of pH on the treatment of turbid water. They concluded that a
high coagulation activity is observed at pH 8 in the treatment of
superficial and deionized water containing synthetic turbidity of
kaolinite. Furthermore, Muthuraman and Sasikala (2014) reported
that among natural coagulants (M. oleifera, Strychnos potatorum,
and Proteus vulgaris), M. oleifera seed extracts had the highest
performance in turbidity removal of 99% from kaolin synthetic
turbid water at pH 7 for a dosage of 250 mg/L.
3.2. Effect of coagulant dosage
3.2.1. Turbidity removal
To compare the coagulation effectiveness of both M. oleifera seed
powder and alum, a series of jar tests were conducted. Different
Fig. 3. Effect of initial pH on turbidity removal. M. oleifera dosage- 150 mg/L; settling
time- 30 min; room temperature- 25 ± 1  C.
145
dosages of 50, 100, 150, 200, and 300 mg/L of both coagulants were
adopted. The effect of coagulant dosages on turbidity removal is
shown in Fig. 4a. It can be seen from this figure that the removal
efficiency increased with the increase in M. oleifera seed powder
dosage. Indeed, the turbidity removal reached its maximum 96.02%
for M. oleifera dosage of 150 mg/L (turbidity decreased from 1739
NTU until 69.01NTU). These results are in accordance with those
obtained by Kane et al. (2017), Madrona et al. (2010), and Sengupta
et al. (2012a,b). A further increase in the residual turbidity was
observed beyond the optimal, which may be explained by the re-
stabilization of the colloidal particles in paper mill effluent. In
fact, Yuliastri et al. (2016) reported that when M. oleifera concen-
tration exceeded the optimum dosage, turbidity increased because
all colloids have been neutralized and precipitated with an opti-
mum dosage; therefore, the excess coagulants will cause turbidity
in water as they did not interact with oppositely charged colloidal
particles.
The presence of NaCl in M. oleifera solution releases the coag-
ulant protein fraction in the solution, thus improving the coagula-
tion efficiency of M. oleifera. Okuda et al. (2001) reported that the
coagulation efficiency of M. oleifera seeds can be greatly enhanced
by the extraction of their active agents using a salt solution having
one valence electron, such as NaCl or KCl. Okuda et al. (1999)
studied the coagulation process of turbid water using M. oleifera
seed extract with 1 M NaCl. Such extraction enhanced the coagu-
lation process about 7.4 times higher than that extracted by
distilled water. Okuda et al. (1999) suggested that the improvement
of coagulation efficiency by NaCl is apparently due to the salting-in
mechanism in proteins wherein a salt increases protein-protein
dissociations, thus leading to an increase in protein solubility as
the ionic strength of salt increases.
Furthermore, the highest turbidity removal was found to be
99.53% by applying the maximum dosage 300 mg/L of alum. Ac-
cording to Guo et al. (2015), the performance of coagulation-
flocculation using alum could be explained by charge neutraliza-
tion, precipitation, bridge-aggregation, adsorption and sweep-
flocculation, one or their combination, which may be dominant at
different conditions.
During experiments, it was observed that just after the addition
of M. oleifera seed powder, many small flocs emerged in fibrous
form, which fell down the beaker like snow (Fig. 4b). A clear so-
lution rapidly appeared just after a slow stirring. After alum addi-
tion, the formation of big, round flocs, glued to one another, was
observed in the middle of the backer, which is a big ball in which
water droplets are sequestered. They well settled in less than
10 min, and the final solution became clear and limpid (Fig. 4c).
The amount of produced sludge at optimal dosages and after
30 min settling was 22.3 and 124.2 mL for M. oleifera and alum,
respectively. Therefore, it is clear that the sludge produced by alum
is almost five times more voluminous than that formed by
M. oleifera seeds. The volume collected using M. oleifera was about
five times less than that generated employing alum
Ndabigengesere et al. (1995).
3.2.2. COD abatement
Fig. 5 depicts the effects of both coagulants on COD removal at
the adopted dosages. Maximum COD abatements of 93.31% and
97.28% were obtained by applying 300 mg/L of alum and 150 mg/L
of M. oleifera, respectively. Treatments using both coagulants are
acceptable because the values related to the COD are in conformity
with the restrictions required by the discharge standard.
Subramonian et al. (2014) reported that an effective coagulation for
COD removal of pulp and paper mill effluent resulted from a
combination of various mechanisms including charge neutraliza-
tion, entrapment/sweep coagulation, and/or bridging, depending
146 S. Boulaadjoul et al. / Chemosphere 206 (2018) 142e149
Fig. 4. a: Effect of M. oleifera seed powder and alum dosage on turbidity removal. At
natural pH- 7.42; settling time- 30 min; room temperature- 25 ± 1  C. b: Paper mill
effluent before and after treatment with M. oleifera seed powder. c: Floc appearance
using alum for paper mill effluent treatment.
Fig. 5. M. oleifera seed powder and alum efficiencies in COD abatement. At natural pH-
7.42; settling time- 30 min; room temperature- 25 ± 1  C.
Fig. 6. Variation in zeta potential with respect to M. oleifera and alum dosage. At
natural pH- 7.42; settling time- 30 min; room temperature- 25 ± 1  C.
on the type of coagulant. Fedala et al. (2015) suggested that the
negatively charged organic matters can be removed from waste-
water by the sweep coagulation mechanism using a plant-based
coagulant. Renault et al. (2009) used another biopolymer, chito-
san, for pulp and paper mill wastewater treatment. They showed a
higher performance of chitosan, as flocculant agent, in the reduc-
tion of COD (more than 85%), than that found using polyaluminium
chloride (55e60%) (see Fig. 6).
Hamoda et al., 2004 suggested that COD removal is associated
with the reduction of organic suspended materials in wastewater;
this indicates that M. oleifera seed powder has a high ability to bind
the organic matters. According to Sharp and Banner (1997), COD is
composed of absorbable and nonadsorbable fractions. The COD
presenting in treated water (after the coagulation process) is the
sum of both fractions remaining at equilibrium after coagulation.
This means that for the complete elimination of COD, further pro-
cesses such as adsorption on ACP, biological treatment, and/or
emerging ones (AOP, ultrasonic irradiation) should be used to
 S. Boulaadjoul et al. / Chemosphere 206 (2018) 142e149
Table 2
Literature review on M. oleifera seed as an effective coagulant for different effluents in terms of turbidity and COD removal.
Effluent Optimal dosage
Irrigation wastewater 4-32 mL/L
Textile 30 mg/L
Superficial water 100-300 mg/L
Municipal wastewater 300 mg/L
Laundry wastewater 120 mg/L
Coffee fermentation wastewater 1e2.5 g L
1
complete the treatment of industry effluent.
It is worth noting that a disadvantage of the use of M. oleifera
seeds in water and wastewater has been identified due to the
presence of oil in large quantities and coagulant-inactive seed
material that is water soluble in M. oleifera seeds; this leads to
elevated dissolved organic materials in the form of soluble COD in
the treated water. These materials may reduce the quality of the
treatment (Nordmark et al., 2016). The residual organic matter may
also be used as a substrate by microorganisms for their growth and
proliferation, thereby increasing the contamination of treated wa-
ter. Hence, numerous research works focused on the extraction and
purification of only the coagulant-active proteins from the seed
kernel (Gassenschmidt et al., 1995; Santos et al., 2012; Camacho
et al., 2017).
M. oleifera efficiency in COD removal can be attributed to the
presence of coagulant substances in the seed powder of this plant.
Indeed, solid particles present in the paper mill effluent are
agglutinated, increased in size, and decanted in the bottom of the
backer. This means that particular COD has been removed from the
supernatant coagulated water.
Table 2 summarizes our results and those of other authors using
M. oleifera seed extract for the treatment of different effluents in
terms of turbidity and COD removal.
3.2.3. Zeta potential
Zeta potential is used to study the coagulation-flocculation
mechanism induced by both alum and M. oleifera seed powder.
Zeta potential results are presented in Fig. 7. As depicted in this
figure, the paper mill effluent has a negative zeta potential value
(
16 mV). At an optimal dosage of M. oleifera (150 mg/L), the zeta
potential of treated wastewater increased from
16 to
8.91 mV.
Beyond this dosage, the zeta potential tended to decrease again.
This variation indicates that the coagulation process is unlike
Fig. 7. Microscope photography of flocs formed by (a) alum and (b) M. oleifera. At natural pH- 7.42; settling time- 30 min; room temperature- 25 ± 1  C.
147
Results Reference
Turbidity (%) COD (%) 85-96- (Sengupta et al., 2012a; b)
- 75.6 (Patel and Vashi, 2012)
99.8- (Madrona et al., 2012)
90 75 (Kane et al., 2017)
83.63 54.18 (Al-Gheethi et al., 2017)
- 26 -100 (Garde et al., 2017)
complete charge neutralization, except the neutralization of some
charges that had occurred. Therefore, the proposed coagulation
mechanism of M. oleifera used as a primary coagulant is a combi-
nation of partial charge neutralization and electrostatic patch or
microbridging mechanism, in which negative particles of colloids
are adsorbed on the microsurface of M. oleifera charged particles,
thereby forming microbridges and resulting in the formation of
light flocs. Otherwise, the zeta potential increased with the increase
in alum dosage. It increased from
16 mV at 0 alum dosage to
7 at
300 mg/L dosage. In these conditions, the neutralization of charge
could be the involved coagulation mechanism. The obtained find-
ings are in good accordance with those previously reported by Shak
and Wu (2014) and Subramonian et al. (2014) for the treatment of
palm paper mill oil and paper mill effluent using Cassia obtusifolia
seed gum and natural coagulant, respectively.
The main focus of coagulation-flocculation is to destabilize the
colloidal particles and to agglomerate them, thereby forming flocs.
These are easily removed from water by sedimentation and/or
filtration. Characteristic evaluation of the flocs formed is indis-
pensable to determine their removal performance (Szyguła et al.,
2009). The formed flocs were observed using an optical micro-
scope (OPTIKA microscope). Fig. 7a and b illustrate the morphology
of the formed flocs after paper mill effluent treatment by alum and
M. oleifera seed powder, respectively. It can be observed from the
figure that the flocs formed by M. oleifera seed extract had a chain-
like structure. In contrast, the alum flocs had an irregular shape and
dispersed randomly. Sasikala and Muthuraman (2016) examined
dried M. oleifera seed powder surface texture and porosity by
scanning electron microscopy (SEM).
The SEM images showed that dried M. oleifera granules before
being dispersed in water are approximately spherical in shape. Each
granule was composed of a large number of small M. oleifera par-
ticles surface morphology texture. When dispersed in water, the
148 S. Boulaadjoul et al. / Chemosphere 206 (2018) 142e149
granules disaggregated easily. According to these authors, chain-
like and spherical structures contributed to lowering the turbidity
in the settled water (sludge).
4. Conclusion
Our study aimed to enhance the primary treatment of paper mill
effluent using M. oleifera seed powder as a natural coagulant
compared to that using alum. The obtained results showed that
turbidity removal efficiency reached 96.02% using 150 mg/L of
M. oleifera seed extract, while the maximum turbidity abatement
rate of 99.53% was obtained for the maximum dose of alum
(300 mg/L). Furthermore, the maximum COD abatement of 97.28%
was obtained using 150 mg/L of M. oleifera, while 93.31% was ob-
tained at 300 mg/L of alum. To this end, the main conclusion can be
drawn: M. oleifera seed powder proves to be an appropriate and
promising alternative for enhancing the primary treatment of pa-
per mill effluent with less risk to human health.
Acknowledgment
The authors are pleased to acknowledge the Faculty of Me-
chanical and Process Engineering, USTHB, for providing the facil-
ities for the research. Dr. Athmane Souad and Mr. Dahmani
Mohamed are also gratefully acknowledged for their kind permis-
sion to use their facilities for the analysis and for providing Moringa
oleifera.
References
Abidin, Z.Z., Mohd Shamsudin, N.S., Madehi, N., Sobri, S., 2013. Optimisation of a
method to extract the active coagulant agent from Jatropha curcas seeds for use
in turbidity removal. Ind. Crop. Prod. 41, 319e323. https://doi.org/10.1016/
j.indcrop.2012.05.003.
Al-Gheethi, A.A., Mohamed, R., Wurochekke, A.A., Nurulainee, N.R., Rahayu, J.M.,
Hashim, M.A., 2017. Efficiency of moringa oleifera seeds for treatment of
laundry wastewater. In: MATEC Web of Conferences. EDP Sciences, p. 6001.
Beril Go€nder, Z., Arayici, S., Barlas, H., 2011. Advanced treatment of pulp and paper
mill wastewater by nanofiltration process: effects of operating conditions on
membrane fouling. Separ. Purif. Technol. 76, 292e302. https://doi.org/10.1016/
j.seppur.2010.10.018.
Bhatia, S., Othman, Z., Ahmad, A.L., 2007. Coagulationeflocculation process for
POME treatment using Moringa oleifera seeds extract: optimization studies.
Chem. Eng. J. 133, 205e212. https://doi.org/10.1016/j.cej.2007.01.034.
Bina, B., Shasavani, A., Asghare, G., Hasanzade, A., 2007. Comparison of Water
Turbidity Removal Efficiencies of Moringa Oleifera Seed Extract and Poly-
aluminum Chloride.
Camacho, F.P., Sousa, V.S., Bergamasco, R., Ribau Teixeira, M., 2017. The use of
Moringa oleifera as a natural coagulant in surface water treatment. Chem. Eng.
J. 313, 226e237. https://doi.org/10.1016/j.cej.2016.12.031.
Choudhary, A.K., Kumar, S., Sharma, C., 2015. Removal of chloro-organics and color
from pulp and paper mill wastewater by polyaluminium chloride as coagulant.
Desalination Water Treat. 53, 697e708. https://doi.org/10.1080/
19443994.2013.848670.
de Paula, H.M., de Oliveira Ilha, M.S., Sarmento, A.P., Andrade, L.S., 2018. Dosage
optimization of Moringa oleifera seed and traditional chemical coagulants so-
lutions for concrete plant wastewater treatment. J. Clean. Prod. 174, 123e132.
https://doi.org/10.1016/j.jclepro.2017.10.311.
Deepak, S., 2014. Treatment of pulp and paper effluent by electro coagulation. Int. J.
ChemTech. Res. 6, 860e870.
Fedala, N., Lounici, H., Drouiche, N., Mameri, N., Drouiche, M., 2015. Retracted:
physical parameters affecting coagulation of turbid water with Opuntia ficus-
indica cactus. Ecol. Eng. 77, 33e36. https://doi.org/10.1016/
j.ecoleng.2015.01.007.
Feria Díaz, J.J., Department of Civil Engineering, University of Sucre, Cra. 28 #5-267,
Puerta Roja, Sincelejo, Colombia, BallutDajud, G., Department of Civil Engi-
neering, University of Sucre, Cra. 28 #5-267, Puerta Roja, Sincelejo, Colombia,
Rodriguez Miranda, J.P., Department of Environnmental Engineering, Francisco
Jos de Caldas University, Cra. 7 #40B-53, Bogot, Colombia, 2018. Influence of
Storage Time of Moringa oleifera seed on the coagulant activity efficiency for
raw water treatment. Indian J. Sci. Technol. 11, 1e4. https://doi.org/10.17485/ijst/
2018/v11i9/121221.
Flaten, T.P., 2001. Aluminium as a risk factor in Alzheimer's disease, with emphasis
on drinking water. Brain Res. Bull. 55, 187e196.
Freitas, J.H.E.S., de Santana, K.V., do Nascimento, A.C.C., de Paiva, S.C., de
Moura, M.C., Coelho, L.C.B.B., de Oliveira, M.B.M., Paiva, P.M.G., do
Nascimento, A.E., Napole~ ao, T.H., 2016. Evaluation of using aluminum sulfate
and water-soluble Moringa oleifera seed lectin to reduce turbidity and toxicity
of polluted stream water. Chemosphere 163, 133e141. https://doi.org/10.1016/
j.chemosphere.2016.08.019.
Garde, W.K., Buchberger, S.G., Wendell, D., Kupferle, M.J., 2017. Application of
Moringa Oleifera seed extract to treat coffee fermentation wastewater. J. Hazard
Mater. 329, 102e109. https://doi.org/10.1016/j.jhazmat.2017.01.006.
Gassenschmidt, U., Jany, K.D., Bernhard, T., Niebergall, H., 1995. Isolation and
characterization of a flocculating protein from Moringa oleifera Lam. Biochim.
Biophys. Acta BBA-Gen. Subj. 1243, 477e481.
Guo, B., Yu, H., Gao, B., Rong, H., Dong, H., Ma, D., Li, R., Zhao, S., 2015. Coagulation
performance and floc characteristics of aluminum sulfate with cationic poly-
amidine as coagulant aid for kaolin-humic acid treatment. Colloid. Surf. Phys-
icochem. Eng. Asp 481, 476e484. https://doi.org/10.1016/j.colsurfa.2015.06.017.
Guo, J., Zhao, L., Lu, W., Jia, H., Sun, Y., 2016. Bacterial communities in water and
sediment shaped by paper mill pollution and indicated bacterial taxa in sedi-
ment in Daling River. Ecol. Indicat. 60, 766e773. https://doi.org/10.1016/
j.ecolind.2015.08.028.
Hamoda, M., A1-Ghusain, I., AL-Mutairi, N., 2004. Sand filtration of wastewater for
tertiary treatment and water reuse. Desalination 164 (2004), 203e211.
Kane, C., Ba^, A., Mahamat, S.A.M., Ayessou, N., Mbacke
, M.K., Mar Diop, C.G., 2017.
Combination of alum and extracted Moringa oleifera bioactive molecules
powder for municipal wastewater treatment. Int. J. Biol. Chem. Sci. 10 (1918)
https://doi.org/10.4314/ijbcs.v10i4.39.
Katayon, S., Noor, M.J.M.M., Asma, M., Ghani, L.A.A., Thamer, A.M., Azni, I., Ahmad, J.,
Khor, B.C., Suleyman, A.M., 2006. Effects of storage conditions of Moringa
oleifera seeds on its performance in coagulation. Bioresour. Technol. 97,
1455e1460. https://doi.org/10.1016/j.biortech.2005.07.031.
Kumar, M.M., Karthikeyan, R., Anbalagan, K., Bhanushali, M.N., 2016. Coagulation
process for tannery industry effluent treatment using Moringa oleifera seeds
protein: kinetic study, pH effect on floc characteristics and design of a thickener
unit. Separ. Sci. Technol. 51, 2028e2037. https://doi.org/10.1080/
01496395.2016.1190378.
Lea, M., 2010. Bioremediation of turbid surface water using seed extract from
Moringa oleifera Lam. (drumstick) tree. Curr. Protoc. Microbiol. https://doi.org/
10.1002/9780471729259.mc01g02s16, 1G.2.1e1G.2.14, Wiley Interscience.
www.interscience.wiley.com.
Madrona, G.S., Branco, I.G., Seolin, V.J., Alves Filho, B.D.A., Fagundes-Klen, M.R.,
Bergamasco, R., 2012. Evaluation of extracts of Moringa oleifera Lam seeds
obtained with NaCl and their effects on water treatment. Acta Sci. Technol. 34
https://doi.org/10.4025/actascitechnol.v34i3.9605.
Madrona, G.S., Serpelloni, G.B., Salcedo Vieira, A.M., Nishi, L., Cardoso, K.C.,
Bergamasco, R., 2010. Study of the effect of saline solution on the extraction of
the moringa oleifera Seed's active component for water treatment. Water, Air,
Soil Pollut. 211, 409e415. https://doi.org/10.1007/s11270-009-0309-0.
Muthuraman, G., Sasikala, S., 2014. Removal of turbidity from drinking water using
natural coagulants. J. Ind. Eng. Chem. 20, 1727e1731. https://doi.org/10.1016/
j.jiec.2013.08.023.
Ndabigengesere, A., Narasiah, K.S., 1998. Use of Moringa oleifera seeds as a primary
coagulant in wastewater treatment. Environ. Technol. 19, 789e800.
Ndabigengesere, A., Subba Narasiah, K., Talbot, B.G., 1995. Active agents and
mechanism of coagulation of turbid waters using Moringa Oleifera. Water Res.
29, 703e710.
Ndubuaku, M., Ndubuaku, T.C.N., Ndubuaku, E., 2014. Yield characteristics of mor-
inga oleifera across different ecologies in Nigeria as an index of its adaptation to
climate change. Sustain. Agric. Res. 3 (95) https://doi.org/10.5539/sar.v3n1p95.
Nkurunziza, T., Nduwayezu, J.B., Banadda, E.N., Nhapi, I., 2009. The effect of
turbidity levels and Moringa oleifera concentration on the effectiveness of
coagulation in water treatment. Water Sci. Technol. 59 (1551) https://doi.org/
10.2166/wst.2009.155.
Nordmark, B.A., Przybycien, T.M., Tilton, R.D., 2016. Comparative coagulation per-
formance study of Moringa oleifera cationic protein fractions with varying
water hardness. J. Environ. Chem. Eng. 4, 4690e4698. https://doi.org/10.1016/
j.jece.2016.10.029.
Okuda, T., Baes, A.U., Nishijima, W., Okada, M., 2001. Coagulation mechanism of salt
solution-extracted active component in Moringa oleifera seeds. Water Res. 35,
830e834.
Okuda, T.U., Baes, A., Nishijima, W., Okada, M., 1999. Improvement of extraction
method of coagulation active components from moringa oleifera seed. Water
Res. 33.
Oladoja, N.A., 2015. Headway on natural polymeric coagulants in water and
wastewater treatment operations. J. Water Process Eng. 6, 174e192. https://
doi.org/10.1016/j.jwpe.2015.04.004.
Oliveira, D.V.M. de, 2014. Evaluation of a MBBR (moving bed biofilm reactor) pilot
plant for treatment of pulp and paper mill wastewater. Int. J. Environ. Monit.
Anal. 2 (220) https://doi.org/10.11648/j.ijema.20140204.15.
Patel, H., Vashi, R.T., 2012. Removal of Congo Red dye from its aqueous solution
using natural coagulants. J. Saudi Chem. Soc. 16, 131e136. https://doi.org/
10.1016/j.jscs.2010.12.003.
Petersen, H.H., Petersen, T.B., Enemark, H.L., Olsen, A., Dalsgaard, A., 2016. Removal
of Cryptosporidium parvum oocysts in low quality water using Moringa oleifera
seed extract as coagulant. Food Waterborne Parasitol 3, 1e8. https://doi.org/
10.1016/j.fawpar.2016.03.002.
Pokhrel, D., Viraraghavan, T., 2004. Treatment of pulp and paper mill wastewaterda
 S. Boulaadjoul et al. / Chemosphere 206 (2018) 142e149 149

review. Sci. Total Environ. 333, 37e58. https://doi.org/10.1016/ j.indcrop.2015.01.045.

j.scitotenv.2004.05.017.
Renault, F., Sancey, B., Badot, P.-M., Crini, G., 2009. Chitosan for coagulation/floc-
culation processes e an eco-friendly approach. Eur. Polym. J. 45, 1337e1348.
https://doi.org/10.1016/j.eurpolymj.2008.12.027.
Santos, A.F.S., Paiva, P.M.G., Teixeira, J.A.C., Brito, A.G., Coelho, L.C.B.B., Nogueira, R.,
2012. Coagulant properties of Moringa oleifera protein preparations: application
to humic acid removal. Environ. Technol. 33, 69e75. https://doi.org/10.1080/
09593330.2010.550323.
Sasikala, S., Muthuraman, G., 2016. A laboratory study for the treatment of turbidity
and total hardness bearing synthetic wastewater/ground water using moringa
oleifera. Ind. Chem. 2, 1e6.
Sengupta, M.E., Keraita, B., Olsen, A., Boateng, O.K., Thamsborg, S.M., Pa
lsdo

ttir, G.R.,
Dalsgaard, A., 2012a. Use of Moringa oleifera seed extracts to reduce helminth
egg numbers and turbidity in irrigation water. Water Res. 46, 3646e3656.
https://doi.org/10.1016/j.watres.2012.04.011.
Sengupta, M.E., Keraita, B., Olsen, A., Boateng, O.K., Thamsborg, S.M., Pa
lsdo

ttir, G.R.,
Dalsgaard, A., 2012b. Use of Moringa oleifera seed extracts to reduce helminth
egg numbers and turbidity in irrigation water. Water Res. 46, 3646e3656.
https://doi.org/10.1016/j.watres.2012.04.011.
Shak, K.P.Y., Wu, T.Y., 2014. Coagulationeflocculation treatment of high-strength
agro-industrial wastewater using natural Cassia obtusifolia seed gum: treat-
ment efficiencies and flocs characterization. Chem. Eng. J. 256, 293e305.
https://doi.org/10.1016/j.cej.2014.06.093.
Shamsnejati, S., Chaibakhsh, N., Pendashteh, A.R., Hayeripour, S., 2015. Mucilagi-
nous seed of Ocimum basilicum as a natural coagulant for textile wastewater
treatment. Ind. Crop. Prod. 69, 40e47. https://doi.org/10.1016/
Sharma, R., Chandra, S., Singh, A., Singh, K., 2014. Degradation of pulp and paper
mill effluents. IIOAB J. 5, 6.
Sharp Jr., J.M., Banner, J.L., 1997. The Edwards Aquifer: a resource in conflict. GSA
Today (Geol. Soc. Am.) 7, 1e9.
Subramonian, W., Wu, T.Y., Chai, S.-P., 2014. A comprehensive study on coagulant
performance and floc characterization of natural Cassia obtusifolia seed gum in
treatment of raw pulp and paper mill effluent. Ind. Crop. Prod. 61, 317e324.
https://doi.org/10.1016/j.indcrop.2014.06.055.
Szyguła, A., Guibal, E., Palacín, M.A., Ruiz, M., Sastre, A.M., 2009. Removal of an
anionic dye (Acid Blue 92) by coagulationeflocculation using chitosan.
J. Environ. Manag. 90, 2979e2986. https://doi.org/10.1016/
j.jenvman.2009.04.002.
Vilaseca, M., Lo
pez-Grimau, V., Gutie
rrez-Bouz

an, C., 2014. Valorization of waste
obtained from oil extraction in moringa oleifera seeds: coagulation of reactive
dyes in textile effluents. Materials 7, 6569e6584. https://doi.org/10.3390/
ma7096569.
Yarahmadi, M., Hossieni, M., Bina, B., Mahmoudian, M.H., Naimabadie, A.,
Shahsavani, A., Others, 2009. Application of Moringa oleifera seed extract and
poly aluminium chloride in water treatment. World Appl. Sci. J. 7, 962e967.
Yuliastri, I.R., Rohaeti, E., Effendi, H., Darusman, L.K., 2016. The use of Moringa
oleifera seed powder as coagulant to improve the quality of Wastewater and
Ground Water. In: IOP Conference Series: Earth and Environmental Science. IOP
Publishing, p. 12033.
Zemmouri, H., Drouiche, M., Sayeh, A., Lounici, H., Mameri, N., 2012. Coagulation
flocculation test of Keddara's water dam using chitosan and sulfate aluminium.
Proc. Eng. 33, 254e260. https://doi.org/10.1016/j.proeng.2012.01.1202.