Industrial Crops and Products 61 (2014) 169–175

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Industrial Crops and Products

journal homepage: www.elsevier.com/locate/indcrop

Use of Plantago major L. as a natural coagulant for optimized

decolorization of dye-containing wastewater
Naz Chaibakhsh ∗ , Neda Ahmadi, Mohammad Ali Zanjanchi
Department of Chemistry, Faculty of Science, University of Guilan, Rasht, Iran

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

Article history: In this study, Plantago major L. has been evaluated as an active natural coagulant for the removal of dye
Received 10 May 2014 from a model textile wastewater containing neutral red. Response surface methodology (RSM) based
Received in revised form 24 June 2014 on a three-variable, three-level Box–Behnken design (BBD) was employed to study and optimize the
Accepted 30 June 2014
treatment process. The effect of three parameters including contact time, pH and the coagulant dose on
Available online 17 July 2014
the color and COD reduction were analyzed. A partial cubic equation could accurately model the response
surface with an R2 of 0.99. The pH was found to be the most significant parameter affecting both color and
Keywords:
COD reduction. A high color (92.4%) and COD (81.6%) reduction efficiency was obtained using P. major
Plantago major L.
Dye
L. at the optimal conditions of 49.6 min, pH 6.5 and 297.6 mg/L coagulant dose. The results also showed
Coagulant that the isothermal equilibrium could be represented by the Freundlich model with an R2 of 0.94.
Wastewater © 2014 Elsevier B.V. All rights reserved.
Neutral red

1. Introduction be achieved through removal of dye molecules, and not by partial

Wastewater is one of the major environmental concerns of the
dye-manufacturing and dye-consuming industries such as textiles,
rubber, leather, paper, plastics, printing, cosmetics and mineral
processing. Dyes have high tinctorial values and less than 1 ppm of
the dye in water is highly visible (Singh et al., 2003). In addition to
their carcinogenic, mutagenic and toxic effects, untreated dye efflu-
ents are harmful to the aquatic life due to reduced light penetration.
Of current world production of dyestuffs of nearly 10 million
kilograms per year, 1–2 million kilograms of active dye enter
the biosphere annually (Sarwan et al., 2012). However, treatment
of dye-containing wastewaters is not easy. Due to the synthetic
origin and complex aromatic molecular structure, dyes are resis-
tant to biological degradation, and are stable to light, heat and
oxidizing agents (Crini, 2006). Many techniques have been devel-
oped for the removal of dyes from wastewater effluents such as
adsorption, physico-chemical and biological techniques, advanced
oxidation processes and electrochemical degradation (Gosavi and
Sharma, 2014). Among them, coagulation–flocculation is the most
common physico-chemical treatment process frequently used for
dye-containing wastewaters (Solanki et al., 2013). The main advan-
tage of this method is that the decolorization of the effluent can
∗ Corresponding author. Tel.: +98 1313233262.
E-mail address: nchaibakhsh@guilan.ac.ir (N. Chaibakhsh).
decomposition of dyes, which could produce potentially harmful
and toxic compounds (Wong et al., 2007).
Commercially available chemical coagulants include alum, fer-
ric chloride, ferric sulphate and polyaluminium chloride, together
with synthetic organic polymers as coagulant aid. However, usage
of these chemicals has several disadvantages such as relatively
high costs, harmful effects on human health, production of large
sludge volumes as well as the fact that they considerably affect pH
of the treated water (Vijayaraghavan et al., 2011). It is therefore
desirable that other environmentally acceptable and economically
viable alternatives be developed to replace the synthetic coagu-
lants (Patale and Pandya, 2012). Natural polymeric macromolecules
extracted from plants could be promising alternatives as they are
highly biodegradable, non-toxic and non-corrosive, produce less
voluminous sludge and do not alter the pH of the water under
treatment (Šciban et al., 2009). Furthermore, since the plants can
be locally grown, the natural plant-based coagulants are more cost
effective than imported chemicals (Sanghi et al., 2006).
In recent years, there have been many reports on the usage of
plant-based coagulants for water and wastewater treatment. Four
types of plants which have received the greatest degree of attention
are Moringa oleifera, nirmali seeds, tannin and cactus (Abidin et al.,
2013; Yin, 2010; Sánchez-Martin et al., 2010).
Plantago major L. (greater plantain) is a species of the Plan-
taginacea family. It is naturalized almost throughout the world
and grows best in moist areas (Webb et al., 1988). It contains

http://dx.doi.org/10.1016/j.indcrop.2014.06.056
0926-6690/© 2014 Elsevier B.V. All rights reserved.
170 N. Chaibakhsh et al. / Industrial Crops and Products 61 (2014) 169–175
Fig. 1. The chemical structure of neutral red.
many bioactive compounds including allantoin, aucubin, ursolic
acid, flavonoids, and asperuloside, which make it one of the most
commonly used medicinal herbs in the world. P. major have been
used for treatment of a number of diseases, such as respiratory,
digestive, skin, and infectious diseases, apart from wound healing. It
also has antiulcerogenic, antiinflammatory, antioxidant, antihyper-
tensive, anticarcinogenic, antitussive and antiphlogistic activities
(Samuelsen, 2000).
So far, there are few reports on the usage of P. major as a nat-
ural coagulant for wastewater treatment. Although, Yazdani et al.
(2009) studied the efficiency of a mixture of four seeds powder
including P. major, Alyssum sp., Plantago psyllium and Ziziphora
clinopodioides in the treatment of urban sewage, no specific study
on the coagulation activity of P. major has been reported.
The aim of the present work was to evaluate the effectiveness of
mucilage obtained from P. major for dye removal. Design of experi-
ments and response surface methodology (RSM) were used to study
the effect of several parameters (contact time, pH and the mucilage
dose) and the interaction between them on the color removal. In
this study, COD (chemical oxygen demand) reduction capability
of the coagulant was also investigated and the optimal conditions
were obtained.
2. Materials and methods
2.1. Preparation of P. major mucilage extract
The seeds of P. major plant (originally grown in Iran) were
bought from a local market. In order to obtain the mucilage, the
seeds were initially dried in an oven at 100 ◦ C for 2 h and then
ground in a grinder and sieved to a 35 mesh (500 ␮m) parti-
cle size (Anastasakis et al., 2009). The powdered material was
soaked in boiling water and 0.9% NaCl solution and stirred for 2 h
(Veeramalini et al., 2012; Beltran-Heredia et al., 2009). The mix-
ture was centrifuged (10 min at 20 rpm) and the highly viscous
polysaccharide extract was obtained.
2.2. Dye removal assay
Neutral red (NR), C.I. 50040, is a basic dye of the azine series and
belongs to quinone-imine class of dyes (Fig. 1). NR was purchased
from Merck (Darmstadt, Germany) and selected as a model dye
due to its wide application range and recalcitrant nature (Sarwan
et al., 2012). A dye solution of 25 mg/L was prepared by dissolving
NR in distilled water. The pH of the solution was adjusted to be
in the range of 2.5–6.5 by addition of diluted HCl and NaOH using
a pH meter (WinLab® Data Line pH meter; Windaus, Clausthal-
Zellerfeld, Germany). This range of pH was selected based on the
fact that NR could act as a pH indicator, changing from red to yellow
between the pH 6.8–8.0 (Sharma and Sharma, 2013). Five hundred
milliliter of this initial solution was put into 1000 mL-flask, and
various doses of coagulant according to the experimental design
were added. The solution was rapidly mixed at 120 rpm stirring for
5 min, then slowly mixed for various time intervals according to the
experimental design. After that, the solution was kept undisturbed
for 30 min for settling. This optimum settling time was obtained in
our preliminary studies. The supernatant after settling was filtered
through a Whatman® filter paper (pore size 20–25 ␮m).
The reduction in color concentration was measured by using a
spectrophotometer (Model UV 2100, Shimadzu Co., Kyoto, Japan).
The color removal percentage was calculated using the following
equation:
Abs0 − Abs
Dye removal (%) = × 100 (1)
Abs0
where Abs is the average of absorbance values at maximum
absorbency visible wavelength of NR solution (533 nm), Abs0 the
value before treatment, Abs the value after treatment process. The
readings were conducted in triplicate.
In order to examine the ability of P. major to remove other dyes,
several assays were performed with four other dyes with different
structures. Methylene blue (max = 666) was purchased from Merck
(Darmstadt, Germany). Congo red (max = 499.5), Malachite Green
(max = 615) and Basic Red 9 (max = 543.5) were obtained from
Sigma Chemical Co. Photometric analysis was done at appropriate
wavelength for each dye.
2.3. COD reduction analysis
Permanganate oxidation method was utilized for measuring
COD (CODMn ) (Choi et al., 2004) before and after each run of the
experimental design. The COD reduction percentage was calculated
using the following equation:
COD0 − COD
COD reduction (%) = × 100 (2)
COD0
where COD0 is the value before treatment, and COD the value after
treatment process. Each experiment was conducted in triplicate.
2.4. Design of experiments, statistical analysis and optimization
To reduce the number of experiments and to optimize the
treatment conditions, a three-variable, three-level Box–Behnken
response surface design (BBD) was employed with 17 experi-
ments. BBD is an efficient experimental design for response surface
methodology (RSM). RSM is a well known and economical statisti-
cal technique in evaluating the effect of parameters on treatment
results (Fu et al., 2009). The variables and their levels selected
for the treatment of NR solution by natural coagulant were con-
tact/treatment time (5–60 min), pH (2.5–6.5) and coagulant dose
(10–300 mg/L) (Table 1). Color removal and COD reduction were
analyzed as the responses. The design of experiments employed is
presented in Table 1.
A software package of Design Expert Version 6.0.6 (Stat-Ease,
Statistics Made Easy, Minneapolis, MN, USA) was used in this study.
After testing increasingly complex models from linear to partial
cubic, a partial cubic polynomial model was developed to study the
effects of the variables on the responses. The partial cubic model
does not contain pure cubic terms but includes terms having cubic
interactions.
An analysis of variance (ANOVA) was used to determine whether
the developed models were adequate to describe the observed data.
Optimization was performed by the software using a desirability
function.
2.5. Equilibrium study and coagulation mechanism
Equilibrium isothermal studies were performed by adding var-
ious doses of the coagulant to the dye solution and contacted for
equilibrium time.
 N. Chaibakhsh et al. / Industrial Crops and Products 61 (2014) 169–175 171

Table 1 3. Results and discussion

Composition of various experiments of the Box–Behnken design, and color and COD
reduction responses for the treatment of NR solution by P. major L.
3.1. Model fitting and ANOVA
Exp. no. Variable Color COD
removal (%) reduction (%)
3.1.1. Color removal
Time pH Coagulant
(min) dose (mg/L) Design matrix of the variables along with obtained color
removal percentage is given in Table 1. Fitting of the data to var-
1 32.5 6.5 300.0 87.5 96.0
2 5.0 4.5 10.0 84.0 16.6
ious models and their subsequent ANOVA showed that the color
3 32.5 2.5 300.0 5.9 33.3 removal process was most suitably described with a partial cubic
4 5.0 4.5 300.0 67.9 16.6 polynomial model. The equation of the model in terms of coded
5 60.0 4.5 10.0 70.7 16.6 factors is as follows:
6 5.0 2.5 155.0 0.0 29.6
7 32.5 4.5 155.0 68.5 33.5 Color removal(%) = +69.99 − 2.27A + 42.13B − 1.21C
8 32.5 4.5 155.0 66.9 30.0 −28.24 B2 + 3.69 C 2 + 4.60 AB + 4.38 (5)
9 32.5 6.5 10.0 88.4 53.8
10 60.0 6.5 155.0 92.7 53.8 AC − 1.70BC + 6.87AB2
11 5.0 6.5 155.0 74.3 73.0
12 32.5 4.5 155.0 71.4 33.9 where A is the contact time, B the pH, and C the coagulant dose.
13 32.5 4.5 155.0 69.7 30.37 The ANOVA for the model is shown in Table 2. By using an F-test,
14 32.5 4.5 155.0 73.5 34.4
the variation of the data around the fitted model (lack of fit) was
15 32.5 2.5 10.0 0.0 29.6
16 60.0 2.5 155.0 0.0 0.0
evaluated. The model showed no lack of fit at a 95% level of signif-
17 60.0 4.5 300.0 72.1 19.8 icance. The F value of the model (183.39) with a P value less than
0.0001 implied that the model was significant at the 95% confidence
level. The small P value and a very high coefficient of determi-
Two main adsorption models (the Langmuir and Freundlich nation (R2 = 0.9958) also showed the suitability of the model for
isotherms) are usually considered for coagulation and flocculation representing the real relationship among the parameters (Lee et al.,
processes. These models were examined in the present work. 2010).
The Langmuir isotherm represents monolayer adsorption on a Adequate precision measured the signal-to-noise ratio. The ade-
set of distinct localized adsorption sites having the same sorption quate precision, which measures the signal-to-noise ratio, for the
energies (Vieira et al., 2010). The linearized form of Langmuir model developed model (37.03) was greater than 4, indicating that the
is given by Eq. (3). model could be used to navigate the design space.
The significance of each term in the model was examined by
Ce 1 Ce testing the null hypothesis. If the P-value is less than the signifi-
= + (3)
qe qmax KL qmax cance level, the null hypothesis is rejected, which means that the
term is significant (Lee et al., 2010). In this case, B, B2 , AB, AC and
where qe is the equilibrium dye concentration on adsorbent,
AB2 were the significant model terms. Negative coefficient values of
Ce equilibrium dye concentration in the solution, qmax ([mg of
the individual factors, A and C, which are also insignificant, indicate
removed dye][mg of coagulant]−1 ) maximum adsorption capacity
that the factors negatively affect the response.
corresponding to a monolayer covering the surface of the adsorbent
Eq. (5) was then used to study the effect of treatment parameters
and KL ([L][mg of removed dye]−1 ) is the Langmuir constant.
on the color removal efficiency of the coagulant obtained from P.
The Freundlich adsorption isotherm deals with surface het-
major.
erogeneity and is derived from empirical data. It assumes that
According to ANOVA, pH is the most significant parameter (F
adsorption capacity (qe ) is an exponential function of the equilib-
value = 1311.04) that affects the color removal. Fig. 2a depicts the
rium dye concentration (Ce ) and is given in the linearized form of
3-D response surface plot regarding the effect of contact time,
Eq. (4).
pH, and their interactions on the color removal at coagulant dose
1 of 155 mg/L (center point of the experimental design). Maximum
log qe = log Ce + log Kf (4) color removal was obtained at pH = 6.5 and 60 min. Prolonging the
n
contact time did not have a significant effect on the color removal at
where n is the Freundlich adsorption order (dimensionless) and Kf pH below 5.5 and the equilibrium dye concentration was achieved
is the Freundlich adsorption constant ([Ln ] [mg of coagulant]−1 [mg very fast. However, at pH = 6.5, by increasing the time from 5 to
of removed dye1−n ]). 60 min, the percentage of color removal had an increase of 20%.

Table 2
ANOVA for the partial cubic model used for the analysis of NR dye removal.

Source Sum of squares Degree of freedom Mean square F value P value

Model 17,871.76 9 1985.75 183.39 <0.0001

A, time 20.70 1 20.70 1.91 0.2093
B, pH 14,196.13 1 14,196.13 1311.04 <0.0001
C, coagulant dose 11.76 1 11.76 1.09 0.3320
B2 3366.77 1 3366.77 310.93 <0.0001
C2 57.39 1 57.39 5.30 0.0548
AB 84.64 1 84.64 7.82 0.0267
AC 76.56 1 76.56 7.07 0.0325
BC 11.56 1 11.56 1.07 0.3359
AB2 94.53 1 94.53 8.73 0.0213
Residual 75.80 7 10.83
Lack of fit 49.64 3 16.55 2.53 0.1957
Pure error 26.16 4 6.54
Corrected total 17,947.56 16
172 N. Chaibakhsh et al. / Industrial Crops and Products 61 (2014) 169–175
Fig. 2. Response surface plots showing the interaction between two parameters, pH and time (a), coagulant dose and time (b) and pH and coagulant dose (c) on the neutral
red dye removal percentage. Other variables are constant at their center points.
It was observed that the decolorization process was highly pH-
dependent and maximum color removal could be obtained at pH
range of 5.5–6.5. Usually pH changes do not affect the efficiency of
natural coagulants (Mishra and Bajpai, 2005). Hence, the increase
and decrease observed in removal of a dye could be due to the
changes in the dye structure. NR is a cationic dye; therefore, the
neutralizing of positively charged NR molecules at higher pH, leads
to their destabilization and flocculation. The natural polymer serves
as a bridge and forms netlike structures during coagulation and
flocculation processes (Beltran-Heredia et al., 2009). In addition,
in acidic medium, the solubility of freshly formed sludge could
increase which also leads to the decrease in dye removal (Patel and
Vashi, 2012). Fig. 2b shows the effect of varying coagulant dosage
and treatment time on the decolorization of NR solution at pH 4.5.
Finding the optimum amount of coagulant is important in order
to have the optimum performance in treatment and also to mini-
mize the dosing cost and sludge formation (Patel and Vashi, 2013).
Increasing the amount of coagulant up to 300 mg/L did not have
a significant effect on the color removal at different times; there-
fore, choosing a low amount of coagulant (10 mg/L) resulting in a
high percent removal of the dye would be preferable. The required
dose of coagulant depends on the initial dye concentration. An over
optimum amount of coagulant should be avoided since it would
cause the aggregated particles to redisperse and disturb particle
settling (Mishra and Bajpai, 2005). In a study performed by Mishra
and Bajpai (2005), the optimal dose of mucilage obtained from P.
psyllium (Psy) was found to be 10 mg/L for decolorization of golden
yellow and reactive black dyes with 15 mg/L dye concentration. The
color removal was also independent of dye concentration within
the range examined. Fig. 2c depicts the response surface plot as a
function of coagulant dose versus pH at 32.5 min. Maximum per-
centage removal of the dye would be obtained at the pH 5.5–6.5.
Again, it was clear that the effect of coagulant dose was not impor-
tant in the treatment process and at the pH range of 5.5–6.5, 90%
color removal would be obtained by adding 10 mg/L coagulant.
3.1.2. COD reduction
Experimental data along with obtained percentage reduction
of COD are presented in Table 1. According to ANOVA, a partial
cubic polynomial model was statistically significant to represent
the actual relationship between the response (COD reduction effi-
ciency of the coagulant) and the variables, with a very small P
value (<0.0001), not significant lack of fit, and a high coefficient
of determination (R2 = 0.9963). The ANOVA for the model is shown
 N. Chaibakhsh et al. / Industrial Crops and Products 61 (2014) 169–175
Table 3
ANOVA for the partial cubic model used for the analysis of COD reduction.
Source Sum of squares
Model 8421.48
A, time 2.56
B, pH 4236.60
C, coagulant dose 2.56
A2 897.51
B2 1896.79
AB 27.04
AC 2.56
BC 370.56
AB2 338.00
B2 C 227.91
Residual 31.56
Lack of fit 14.23
Pure error 17.34
Corrected total 8453.04
in Table 3. The equation of the model in terms of coded factors is
given below:
COD reduction = +32.23 + 0.80A + 23.01B + 0.80C
−14.58A2 + 21.20 B2 + 2.60AB + 0.80
AC + 9.63BC − 13.00AB2 + 10.68B2 C
where A is the contact time, B the pH, and C the coagulant dose.
Similar to decolourization efficiency, pH of the solution was
found to have the greatest effect on the COD reduction, with the
highest F value of 805.32, while both the contact time and coagu-
lant dose were not significant parameters. A2 , B2 , BC, AB2 and B2 C
were also significant model terms.
Fig. 3a shows the three-dimensional response surface generated
to show the effect of contact time and pH on the COD reduction. By
raising pH of the solution, COD reduction increased and maximum
response was observed at pH = 6.5 and 24 min. There was a drastic
increase in COD reduction (from 39.52 to 77.12%) as pH increased
from 5.5 to 6.5. Increase in the dye removal at higher pH values
leads to increase in COD reduction. The effect of varying coagulant
dose and contact time at pH = 4.5 is shown in Fig. 3b. The percent-
age of COD reduction increased up to an optimum contact time
(34 min) and then decreased. The decrease in removal efficiency
could be due to destabilization of the aggregated particles after the
optimum time (Mishra and Bajpai, 2005). COD removal was not sig-
nificantly influenced by coagulant dose at pH 4.5. By increasing the
coagulant amount from 10 to 300 mg/L, only 1.6% reduction in COD
was observed (from 31.4 to 33.0% COD reduction).
Fig. 3c represents the effect of varying pH and coagulant dose on
the COD reduction. There was a strong interaction between pH and
coagulant dose (F value = 70.44). At pH > 6, the effect of coagulant
dose became significant. Maximum COD reduction was observed at
pH 6.5 by adding 300 mg/L coagulant. At pH 6.5, by increasing the
coagulant dose from 10 to 300 mg/L, COD reduction was increased
from 55 to 96%, while, as mentioned previously, by adding 10 mg/L
of coagulant a high color removal percentage would be obtained. It
seems that 10 mg/L coagulant can only change or destroy the color
producing part of the molecule and do not remove the residual
moieties from the effluent. Increasing the coagulant dose leads to
removal of the complete dye molecules, so that COD reduction can
be improved by increasing the amount of coagulant.
A control experiment (using a solution of distilled water and
coagulant) performed after settling of the solution showed that less
than 10% of the remaining COD is related to the organic matter of
the coagulant. This amount is negligible in low coagulant dosage.
However, an over optimum amount of coagulant may increase the
COD of the treated effluent.
173
Degree of freedom Mean square F value P value
10 842.15 160.08 <0.0001
1 2.56 0.49 0.5115
1 4236.60 805.32 <0.0001
1 2.56 0.49 0.5115
1 897.51 170.61 <0.0001
1 1896.79 360.56 <0.0001
1 27.04 5.14 0.0639
1 2.56 0.49 0.5115
1 370.56 70.44 0.0002
1 338.00 64.25 0.0002
1 227.91 43.32 0.0006
6 5.26
2 7.11 1.64 0.3016
4 4.33
16
3.2. Optimum conditions
RSM can present the optimum combination of parameters, on
the basis of the ridge maximum analysis and the canonical anal-
ysis, to obtain the highest percentage of color and COD removal.
(6) By using the optimization function of the software, the experiment
with desirability value of 1 was selected. The desirability function
is given in the following equation:
1/n
n 1/n
D = (d1 × d2 × · · · × dn ) =( di ) (7)
i=1
where n is the number of responses in the measure and di is the
desirable ranges for each response.
The maximum color and COD reduction (93.0 and 86.0%, respec-
tively) was predicted under treatment conditions of 49.6 min, pH
6.5 and 297.6 mg/L coagulant dose. The actual experimental val-
ues obtained were 92.4% with 0.6% deviation for color removal and
81.6% with 4.4% deviation for COD reduction.
3.3. Adsorption modeling
In order to study the coagulation mechanism, a theoretical
model which explains the dye removal by the coagulant was pro-
posed. According to literature (Yin, 2010), coagulation–flocculation
by plant-based coagulants can generally occur via two mecha-
nisms: adsorption and charge neutralization; and adsorption and
interparticle bridging. Destabilization of colloids may be governed
by chemical interactions between coagulant and dye molecules.
After formation of the coagulant-dye complex, flocs begin to grow
by adsorption mechanisms, which should be the controlling stage
(Beltran-Heredia et al., 2009).
Fitting of the equilibrium adsorption data to Langmuir and
Freundlich isotherms showed that the Freundlich equation fits
slightly better than Langmuir model. A linear fitting graphic for
the Freundlich isotherm is included in Fig. 4. The R2 values were
equal to 0.94 in the case of Freundlich and 0.93 in the case of Lang-
muir. The values of n and Kf estimated respectively from the slope
and intercept of the plots for Freundlich isotherm were 1.53 and
0.0373. For Langmuir isotherm, the values of qmax and KL were 0.20
and 0.206, respectively.
3.4. Removal of other dyes
The color removal ability of P. major was tested using four other
dyes including anionic dye Congo red and cationic dyes, Methylene
blue (MB), Malachite Green and Basic Red 9 at treatment condi-
tion of 30 min, 150 mg/L coagulant dose and pH = 6. The results
are presented in Fig. 5. At this condition, the lowest color removal
174 N. Chaibakhsh et al. / Industrial Crops and Products 61 (2014) 169–175

Fig. 3. Response surface plots showing the interaction between two parameters, pH and time (a), coagulant dose and time (b) and pH and coagulant dose (c) on the COD
reduction percentage of the neutral red dye solution. Other variables are constant at their center points.

percentage was obtained for the anionic dye, Congo red. The coag-
ulant showed a relatively good performance in the removing of MB.
MB has a structure similar to NR, but a different basicity, which may
change the optimum pH for its removal. The removal percentage
of Malachite Green and Basic Red 9 is not very high, which may be
due to their non-linear structures. The coagulation process prefers
linear molecules rather than non-linear ones with steric difficulties
(Beltran-Heredia et al., 2009).

Fig. 5. Removal of dyes by means of P. major mucilage extract using 150 mg/L coag-
ulant at 30 min and pH = 6.

4. Conclusions

P. major L. has been found to be a highly effective color

Fig. 4. The linear Freundlich isotherm plot for the adsorption of neutral red dye on
P. major mucilage extract.
and COD removal agent through the coagulation of the toxic
NR dye. Response surface methodology and Box–Behnken design
were effectively applied to the modeling and optimization of the
treatment parameters. Up to 92% dye removal and 82% COD reduc-
tion were achieved at 49.6 min, pH 6.5 and 297.6 mg/L coagulant
dose, which matched well with the predicted values. The process
was highly pH-dependent and maximum decolorization could be
obtained at pH range of 5.5–6.5. P. major mucilage extract also
 N. Chaibakhsh et al. / Industrial Crops and Products 61 (2014) 169–175
showed a relatively good performance in the removal of Methylene
blue. Further optimization could lead to better results. The inter-
action between coagulant and dye could be modeled according to
Freundlich hypothesis. The ability to achieve a high percentage of
color and COD removal indicates that P. major L. has a great poten-
tial to be used as an inexpensive and easily available coagulant for
the treatment of dye-containing industrial wastewaters.
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