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https://doi.org/10.1007/s00267-020-01407-0
Received: 18 May 2020 / Accepted: 30 November 2020 / Published online: 12 January 2021
© The Author(s), under exclusive licence to Springer Science+Business Media, LLC part of Springer Nature 2021
Abstract
Cactus has shown great capabilities as a bio coagulant/flocculent in the treatment of wastewater and as a factor for
sustainable development of the environment, due to its abundance and non-toxicity for human health. This has encouraged
the present study based on the design of experiments to optimize the two operating factors: the bio coagulant dosage and
initial pH. The effect of these considered factors on turbidity and chemical oxygen demand (COD) reduction performances
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was investigated to treat sewage wastewater from plants by the coagulation/flocculation process using the response surface
methodology (RSM) based on a central composite faced design (CCFD). The effect of the pH on the supernatant turbidity
removal and the COD reduction was very significant whereas that of the coagulant dosage was insignificant on the COD
removal efficiency. Experimental results revealed that the maximum reduction of turbidity and COD could be reached at a
coagulant dosage of 28 mg/l and a pH of 12. At these optimal conditions, the removal efficiency of turbidity and COD was
98.33% and 96.55% respectively. By the end of the treatment, final values of 0.84 NTU and 20.8 mg/l were obtained for
turbidity and COD, respectively. A notable decrease of orthophosphate (O- PO4−2), nitrite (N-NO3−), ammonium (N-NH4+)
and suspended matter (SM) was observed. The study also showed that the quadratic regression model could be used as a
theoretical basis for the process based on a high coefficient of determination R2 value > 0.96, obtained from the analysis of
variances (ANOVA).
Keywords Wastewater Bio coagulant Sustainable development Response Analysis of variance
● ● ● ●
Introduction of ecosystems and water resources all over the world (Choi
et al. 2008; Uğurlu et al. 2008; Zheng et al. 2009; Thee-
Public health, protection of the environment, and socio- pharaksapan et al. 2011).
economic interests are the ultimate goals in industrial was- Palatable clean drinking water is becoming scare, and the
tewater management (Mahrouz et al. 2016). Continuous cost of water treatment is increasing (Varsha and Jay 2012;
population growth, increased economic activity and indus- Nharingo et al. 2015). In recent years, water treatment has
trial development, on the one hand, and water exploitation become the focus of considerable research attention and a
and poor management, on the other, have caused degradation pronounced challenge to society. This has encouraged
numerous researchers to test new methods for water treat-
ment including affordable, eco-friendly, and more effective
processes (Alila and Boufi 2009; Antov et al. 2012).
Supplementary information The online version of this article (https:// Several wastewater treatment plants (WWTPs) use the
doi.org/10.1007/s00267-020-01407-0) contains supplementary
coagulation/flocculation process to limit the release of cer-
material, which is available to authorized users.
tain pollutants to the receiving water course. The coagula-
* Asma Ayat tion/flocculation process is an essential and critical step in
ayat_asma@hotmail.fr both drinking water and wastewater treatment with a large
1 range of applications in treatment technology. Coagulation/
Faculty of Process Engineering, Environmental Process
Engineering Laboratory (LIPE), Salah Boubnider University flocculation process enables the removal of colloids and
Constantine 3, Constantine, Algeria particles. It also enables the removal of colloids and
490 Environmental Management (2021) 67:489–497
particles, and eliminates all bacteria and a part of viruses as limitations of the conventional method can be overcome by
well (Miller et al. 2008; Nharingo et al. 2015). applying statistical experimental design techniques using the
As typical chemical coagulants, hydrolyzing metal salts RSM. This method has been successfully applied in various
based on aluminum or iron are widely used. Colloidal may scientific and technical fields such as applied chemistry and
be subject to an instability caused by aluminum or iron physics, biochemistry and biology, chemical engineering,
salts, which lead the small particulates to form large environmental protection, membrane science, and technology
aggregates, which will be removed by sedimentation and (Khayet et al. 2011).
filtration to purify water and wastewater (Jiang and Lioyd The main objectives of using RSM is to develop models,
2002; Duan and Gregory 2003). Inorganic coagulants that improve process optimization and evaluate the relative
are extensively used may have the following disadvantages: significance of several influential factors even in the pre-
they require large dosage, low effect and they are noxious to sence of complex interactions. RSM uses an experimental
humans. Likewise, synthetic organic coagulants are toxic, design such as the CCFD to fit a model by least squares
have a high cost and require corrosion-resistant storage and techniques. The adequacy of the proposed model is then
feed equipment, limiting their application (Lu 2002). assessed using the diagnostic checking tests provided by the
In recent years, the wastewater treatment research has analysis of variance (ANOVA) (Montgomery 2001).
focused on the use of biomaterials to deal with various Likewise, another objective is to treat sewage wastewater
pollutants including heavy metallic ions pollutants, dyes, from plants using the bio coagulation/flocculation process,
phosphates, nitrates, chlorides, phenolic compounds, pesti- modeling and optimizing the key operating parameters of
cides, detergents and particulates, among others. This has this bio process using RSM based on CCFD. Two inde-
led to the identification of natural and environmentally pendent factors were investigated in this study: cactus
benign agents that purify water through the coagulation/ powder dosage and pH which might decrease supernatant
flocculation process (Li et al. 2009). Biomaterials are turbidity, and COD.
rapidly gaining interest due to their inherently renewable
character, low toxicity, lower sludge volume compared to
alum, inessential requirement for pH adjustment, biode- Material and Methods
gradability, low commercial cost, relative abundance, high
treatment efficiency, harmlessness to humans, unfound Wastewater Sampling
contamination by-product released into treated water, and
overall smaller environmental impact compared to inor- The wastewater samples used in this study were collected from
ganic and synthetic polymers (Sharma et al. 2006). Ferdjioua WWTP, located in the municipality of Mila,
In this context, the use of plant-based coagulants for water Algeria. The WWTP is intended to operate at a capacity of
treatment represents a more sustainable development strategy 9600 m³/day. It was designed in 2013 to receive municipal
of the environment. Cactus (opuntia ficus indica), commonly wastewater in order to protect “Beni Haroun” dam. This
called ‘nopal’ in Mexico, prickly pear or cactus leaf in USA WWTP is established to face various forms of water-borne
(Nharingo et al. 2015), has long been associated with its diseases and to contribute to the irrigation of agricultural lands.
medicinal proprieties and has been regarded as a dietary food A sampling from the wastewater was carried out on 08/
source, and it can be propagated in most parts of the world. It 03/2019 followed by temperature and pH measurements of
has been used as a bio sorbent (Mane et al. 2011; Bouatay and the samples, which were immediately delivered to the
Mhenni 2014), and its high coagulation capability has been laboratory and kept at 5 °C without adding any chemicals.
proven in terms of its potential for the elimination of heavy The averages of the physical and chemical characteristics of
metals, dyes, organic materials, and bacteria (Vijayaraghavan wastewater samples are shown in Table 1.
et al. 2011). The presence of the mucilage stored in cactus
inner pads, which is a viscous complex carbohydrate, is Bio Coagulant Preparation
attributed to the high coagulation capability and to its effi-
ciency for wastewater treatment (Yin 2010). In this study, cactus (powder) was used as a natural coagulant/
The significant parameters optimization in the coagula- flocculent. The cactus pads were collected from a wild
tion/flocculation process through the classical method relies plantation near Constantine, Algeria and were washed with
on varying a single factor while keeping the remaining distilled water to remove dust, impurities and all thorns.
factors constant at specific set of conditions. The biomaterial was cut into small pieces, dried at 45 °C
This is extremely time-consuming (it requires many for 48 h and then crushed using a domestic grinder. Finally,
experimental runs), expensive, and is unlikely to reach the true it was sieved to obtain solids with the diameter of 63 μm in
optimum value due to the negligence of interactions between diameter. The solids were used as a raw coagulant to treat
variables (Adinarayana et al. 2003; Ahmad et al. 2007). These wastewater without any chemical pre-treatment.
Environmental Management (2021) 67:489–497 491
Table 1 Characteristics of investigated wastewater samples Table 2 Experimental range and levels of independent variables
Parameters Units Average values Variables Range and level
pH / 7.6 −1 0 +1
Turbidity NTU 50 A: coagulant dose (mg/L) 10 25 40
Temperature °C 14.7 B: (pH) 2 7 12
Conductivity μs/cm 1961
Dissolved oxygen mg/L 9.17
Ortho Phosphate (PO4-2) mg/L 0.626
nitrate (N-NO3-) mg/L 0.91 SM. They were determined in laboratory according to the
Suspended matter mg/L 338 methods given in the series of standard methods for the
Ammonium (N-NH4+) mg/L 2.7 examination of water and wastewater (APHA 2003).
Chemical oxygen demand (COD) mg/L(O2) 602.88
Biochemical oxygen demand (BOD5) mg/L(O2) 100 Experimental Design and Data Analysis
Where Ym is the response variable to be modeled, Xi and Xj experimental design matrix along with observed and pre-
the independent variables which influence Ym, b0, bi, bii and dicted turbidity removal and COD removal efficiencies in
bij are the offset terms, the ith linear coefficient, the quadratic coded values.
coefficient and ijth interaction coefficient, respectively.
Statistical Analysis of Turbidity Removal
Results and Discussion The effects and interaction diagrams of bio coagulant
dosage and pH on turbidity reduction are shown in Fig. 2
Statistical Analysis and Modeling and the main effects plot was used to examine differences
between level means for one or more factors (Fig. 2a).
Experiments according to the CCFD were carried out in the There is a main effect when different levels of a factor affect
laboratory for different combinations of the parameters and the response dissimilarly. A main effects plot shows the
the obtained results are presented in Table 3, which shows mean response for each factor level connected by a line.
The Figure shows clearly that the bio coagulant dosage
and the pH influenced the process of coagulation and had a
very significant effect. While the interaction had no effect
on the removal performance of suspended solids, the
interaction between factors occurred when the change in
response from the low level to the high level of one factor
was different from the change in response at the same two
levels of a second factor. From the graph of Fig. 2b, no
significant interaction between all factors could be noted
(the interaction curves were almost parallel). It was
observed that the cactus powder could generate higher
turbidity elimination at high initial pH values and the
maximum removal was obtained when the initial pH of the
solution was 12.
Based on results presented in Table 3, the RSM was
applied to develop a regression polynomial equation which
provided a relationship between the output (the responses)
and the input (independent factors). By means of a regres-
sion, the turbidity removal (%) was expressed in terms of
Fig. 1 Study domain in coded values
coded values of bio coagulant dosage (A) and pH (B) by the
Table 3 CCFD matrix for turbidity removal and COD removal efficiencies
Run Coagulant dosage(A) pH (B) Turbidity removal (%) COD removal (%)
Experimental values Predicted values Experimental values Predicted values
100 100
90 90
80 80
P re d i c te d tu rb i d i ty re m o v a l e ffi c i e n c y (% )
P r e d i c te d C O D r e m o v a l e ffi c i e n c y (% )
70 70
60
60
50
50
40
40
30
30
20
20
10
10
0
0 10 20 30 40 50 60 70 80 90 100 0
Experimental turbidity removal efficiency (%) 0 10 20 30 40 50 60 70 80 90 100
Experimental COD removal efficiency (%)
Fig. 3 Predicted values vs. experimental values for turbidity elimina-
tion efficiency Fig. 4 Predicted values vs. experimental values for COD removal
efficiency
Fig. 5 3D surface graphs for turbidity removal efficiency (a) and COD In order to assess the impact of the bio coagulant use, it was
removal efficiency (b) judicious to examine the quality of the treated water, after
having had obtained the optimal conditions for the elim-
and a pH between 9 and 12. It was noted that the effect of ination of turbidity and COD and confirmed the predicted
the initial pH upon the output responses was the most values of the two responses considered. The optimal values
important. (dose of bio coagulant = 28.8 mg/L and pH = 12) were
used to test the ability of the bio coagulant to eliminate
The Optimal Values other pollution parameters such as phosphate, nitrates,
ammonium, and suspended solids. Figure 7 shows a sig-
Upon optimization, a unique solution was found bycarrying nificant decline of the pollution parameters using the cactus
out Response Optimizer multi objectives to ensure the powder in the coagulation/flocculation process: a reduction
496 Environmental Management (2021) 67:489–497
Table 4 Confirmation
pH Dose (mg/L) Predicted values Experimental values Error
experiments for optimum region
TUR (%) 12 28.78 99.00 98.33 0.67
COD (%) 97.87 96.55 1.32
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