Current Research in Green and Sustainable Chemistry 6 (2023) 100358

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Current Research in Green and Sustainable Chemistry

journal homepage: www.elsevier.com/journals/
current-research-in-green-and-sustainable-chemistry/2666-0865

A review of coagulation explaining its definition, mechanism, coagulant

types, and optimization models; RSM, and ANN
Reem M. El-taweel a, Nora Mohamed b, Khlood A. Alrefaey b, Sh Husien a, A.B. Abdel-Aziz c,
Alyaa I. Salim a, Nagwan G. Mostafa d, Lobna A. Said e, Irene Samy Fahim b, *,
Ahmed G. Radwan f, a
a
School of Engineering and Applied Sciences, Nile University, Giza, Egypt
b
Industrial Engineering Program, SESC Research Center, Nile University, Giza, Egypt
c
October High Institute for Engineering Technology, Giza, Egypt
d
Environmental and Sanitary Engineering Division, Public Works Department, Faculty of Engineering, Cairo University, Giza, Egypt
e
Nanoelectronics Integrated Systems Center (NISC), Nile University, Giza, Egypt
f
Engineering Mathematics and Physics Dept., Faculty of Engineering, Cairo University, Giza, 12613, Egypt

A R T I C L E I N F O A B S T R A C T

Keywords: The textile business is one of the most hazardous industries since it produces several chemicals, such as dyes,
Coagulation which are released into water streams with ef-fluents. For the survival of the planet's life and the advancement of
Coagulants humanity, water is a crucial resource. One of the anthropogenic activities that pollute and consume water is the
Textile effluents
textile industry. Thus, the purpose of the current effort is to Apply coagulation as a Physico-chemical and bio-
Mathematical models optimization
Textile
logical treatment strat-egy with different techniques and mechanisms to treat the effluent streams of textile in-
dustries. The discharge of these effluents has a negative impact on the environment, marine life, and human
health. Therefore, the treatment of these effluents before discharging is an important matter to reduce their
adverse ef-fect. Many physico-chemical and biological treatment strategies for contaminants removal from
polluted wastewater have been proposed. Coagulation is thought to be one of the most promising physico-
chemical strategies for removing con-taminants and colouring pollutants from contaminated water. Coagula-
tion is accompanied by a floculation process to aid precipitation, as well as the collection of the created sludge
following the treatment phase.. Different commercial, and natural coagulants have been applied as a coagulants in
the process of coagulation. Additionally, many factors such as; pH, coagulant dose, pollu-tants concentration are
optimized to obtain high coagulants removal capacity. This review will discuss the coagulation process, coagulant
types and aids in addition to the factors affecting the coagulation process. Additionally, a brief comparison be-
tween the coagulation process, and the other processes; princi-ple, advantages, disadvantages, and their efficiency
were discussed throgh the review. Furthermore, it discusses the models and optimization techniques used for the
coagulation process including response surface methodology (RSM), ar-tificial neural network (ANN), and several
metaheuristic algorithms combined with ANN and RSM for optimization in previous work. The ANN model has
more accurate results than RSM. The ANN combined with genetic algorithm gives an accurate predicted optimum
solution.

1. Introduction
Due to increased industrialization and industry releasing their efflu-
ents into water streams, water pollution has become one of the world's
most pressing issue. Dyes are considered as one of the most dangerous
pollutants that are being discharged from textile industries such as;
textile, paints, leather, cosmet-ics, food, paper, and pharmaceuticals
industries. Egypt is consider one of the countries where dyes industries
are spread very much. Dyes could be classified into different forms such
as direct, acid, base types of dyes in addition to azoic colors, reactive,
sulphur, and metal complex dyes, which can represent nearly more than
100,000 commercially available dyes of annual production over 7
105
tons. It was stated that, nearly 10–50% of these commercial dyes were
lost in the effluents through the manufacturing process [1] (see Fig. 10).

* Corresponding author.
E-mail address: ISamy@nu.edu.eg (I.S. Fahim).

https://doi.org/10.1016/j.crgsc.2023.100358
Received 26 October 2022; Received in revised form 23 January 2023; Accepted 4 February 2023
Available online 15 February 2023
2666-0865/© 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
R.M. El-taweel et al.
The major pollutants in textile industries effluents are organic and
inorganic matters such as; surfactants, active substances, salts, dissolved
solids, total solids, suspended solids, dyeing substances, total solids, in-
hibitor compounds, and chlorine. Additionally, colored matters gener-
ated from dyes and heavy met-als are one of the major pollutants
produced from textile effluents, and should be removed before dis-
charging the effluents into waterways. Discharging colored effluents
without proper treatment causes an aesthetic problem that affect gas
solubility, and water transparency. Therefore, the removal of colored
pollutants from polluted wastewater is very important due to its major
contribution to the fraction of biochemical oxygen demand. Water
contamination with colored agents; dyes, and heavy metals has a severe
effect on aquatic organisms, plants, animals, and human health with its
mutagenic, carcinogenic, and orteratogenic effects, as shown in Fig. 1.
Various treatment methods have been applied for dyes removal from
polluted wastewater which can be classified into physico-chemical,
physical, chemical, adsorption, biological and electrochemical. Howev-
er, These techniques have var-ious disadvantages such as applying toxic
chemicals, high costs, generate toxic by-products [2]. Physicochemical
techniques produce highly efficient streams, which contain organic
matter and heavy metals. Physicochemical techniques remove COD,
chlorine, phenols, and other toxic materials. The PACT mech-anism can
be applied pre-stage to protect the membranes. Some mechanisms as the
evaporation C can reduce the volume by up to 95%. The disadvan-tages
of Physicochemical techniques; it is applied just in high concentration,
difficult to manage the produced chemical sludge [3]. Physical and
chemical techniques such as membrane separation, ozonation, oxidation,
photochemical, ion exchange, and electrolysis. Membrane separation can
remove the color from various types of dyes in water, but it is an
expensive mechanism and need high pressure and energy. Ozonation can
be implemented in the gas phase but it has a short half-life and need
expensive chemicals to preserve its stability. The oxidation technique is a
rapid and highly efficient process but needs expensive chemicals and
high energy consumed and high cost required. The photochemical
technique does not produce sludge but is only applied to the secondary
pollu-tant. Ion exchange has a highly efficient regeneration process, but
not can be applied to dispense dye. The electrolysis technique is applied
to various ranges of class dye but generating undesirable by-products is
considered a big disad-vantage of this technique [4]. The adsorption
technique has a lot of advantages easy to apply, moderate cost, and high
Fig. 1. Effects of textile effluents into the environment.
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Current Research in Green and Sustainable Chemistry 6 (2023) 100358
efficiency especially for removing organic pollutants, but this technique
required periodically generated and fouling may appear as a big problem.
So, monitoring and periodic maintenance must be applied [5]. The
electrochemical technique gets high efficiencies and reasonable results
for Microbiologically Influenced Corrosion (MIC), but this technology
needs a lot of mathematical effort and evaluation [6]. Additionally,
adsorption is one of the techniques that could applied for dyes removal
where various adsor-bent materials such as nano-materials, agriculture
wastes, and algae [7,7–9] Colors can be removed from water through
different mechanisms such as physical dyes separation, dyes breakdown,
or adsorption biodegredation process. Coagu-lation fluctuation, macro-
spore, adsorption, and membrane separation processes are types of
physicochemical, and physical methods. In coagulation, there is an
electrostatic attraction between oppositely charged soluble dyes of the
effluents and coagulants molecules. Applying chemical coagulation and
the process of the flocculation in wastewater treatment includes the
chemicals addition to change the physical state of suspended and dis-
solved solids and in follow facilitates their removal after that by the
sedimentation process. Coagulation is used to remove contaminants from
suspended or colloidal forms that do not settle out on standing or settle
slowly, and it is considered the most useful pre-treatment procedure in
wastewater treatment [10]. It would be noteworthy from an
en-vironmental and solid waste management perspective to use algal
wastes. It is possible to make an algal waste-bentonite mixture. Algae is
suitable for the removal of contaminants and is easily detected and
harvested in large quantities in seawater. Due to the presence of poly-
saccharides, proteins, or lipids on their cell walls that contain functional
groups including amine, hydroxyl, carboxyl, alginic acid, and sulfate,
algae can offer appropriate sites for the adsorption of contaminants and
heavy metals. In a short amount of time, there has been rapid industri-
alization growth that has contaminated the aquatic system with heavy
metals. Lead is one of the heavy metal pollutants (Pb). Pb contamination
in the environment is thought to be due to industrial wastewater
disposal. Due to its toxicity, mobility, and nonbiodegradability, Pb ac-
cumulates [7]. Overexpo-sure to Cu(II) and Pb(II) will have negative
effects such as vomiting, stomach ulcer, colic, hypotension, liver necrosis,
and even coma. Therefore, steps should be taken to reduce the amount of
Cu (II) and Pb(II) in the water. Metal ions Pb2þ adsorbents include
powdered telescope snail and mangrove crab shells. When used to adsorb
the metal ion Pb2þ, telescope snail and mangrove crab shell powders
R.M. El-taweel et al.
achieved equilibrium after 120 min, with adsorption capacities of 9.93
mg g-1 for telescope snail shell powder and 9.50 mg g-1 for mangrove
crab shell powder, respectively [11]. From the perspective of solid waste
management and ecology, using bagasse waste would be commendable.
As a result, this data set presents an easy way for making an adsorbent
from a bagasse-bentonite mix-ture. Applying the produced adsorbent
allowed Cd2þ to be taken out of the aqueous solution. The use of bagasse
wastes is commendable from an environ-mental and solid waste man-
agement perspective. As a low-cost bio adsorbent, bagasse and bentonite
are combined. Applying the produced adsorbent allowed Pb2þ to be
taken out of the aqueous solution. With variations in the mixed mass ratio
(1:0, 1:1, 1:2, 1:3, 2:1, 3:1), pH (2, 3, 4, 5, 6, 7), and contact time (5, 10,
30, 45, 90, 120, 180 min), it was carried out on a laboratory scale using a
completely randomized design. The adsorption technique used was batch
ad-sorption. The maximum Pb2þ adsorption efficiency was 97.31% for
the mixed adsorbent with a mass ratio of 3:1. Pb2þ adsorption was most
effective at a pH of 5, and 45 min of contact time resulted in an
adsorption efficiency of 94.76% and 93.38% [7]. King Palm, Alexandrae
Palm, and Alex Palm are common names for Archontophoenix alexandrae.
Production of the king palm is somehow linked to enormous amounts of
leftovers made from leaves and leaf sheaths, with certain species-specific
differences. These residues might qualify as natural dietary materials,
however, there isn't any information in the literature about their chem-
ical makeup and use as food ingredients. The king palm has a great
connection to the environment since it relieves pressure from the palmito
industry and illegally removed species, namely Euterpe edulis. Addi-
tionally, it is simple to cultivate. Alexandrae flour's chemical analysis,
antioxidant potential, and microstructure were all recorded. The plant
has a substantial amount of fibre with minimal ash content. Since there is
no major documented use for this plant in Pakistan, a large amount of
waste is produced each year that can be used for adsorption, making it an
affordable, environmentally benign, and con-veniently accessible
adsorbent [9]. Takari sand was successfully used to create the silica
hybrid adsorbent, which was then mercapto-modified. The presence of
groups of hydroxyl(-OH), silanol (Si–OH), siloxane (Si–O–Si), methylene
(-CH2), and thiol allowed for the successful preparation of this modified
silica (-SH) [8].
Additionally, Generating mathematical models for the coagulation
Fig. 2. Graphical abstract showing the various sections discussed in the review.
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Current Research in Green and Sustainable Chemistry 6 (2023) 100358
process is essential, so the processes become predictable and can be
optimized. The mathematical model should have high accuracy so that
the predictable values would be too close to the actual values. The
mathematical model helps know the results without running the actual
experiment, saving money and time. The mathematical models can be
optimized, which implies determining the best conditions for maximising
or minimising the output. The models commonly used to model coagu-
lation process are illustrated.
The models that are commonly implemented in the coagulation
process are the response surface methodology and the artificial neural
network. RSM is the most commonly multivariate statistic technique
used to model analytical chemistry. Whereas, the response surface
methodology combines mathematical and statistical techniques used to
construct the mathematical model. RSM fits experimental data to a
polynomial equation, and it is implemented when a response or a set of
responses are affected by many factors [12]. A popular machine learning
technology for chemical wastewater treatment procedures is the artificial
neural network, and it is a dynamic model that provides control and
management of the plant [13]. Therefore, this review will explain the
process of coagulation from the start to end to be a good reference for a
young researcher to start his work in coagulation. For instance, it will
discuss coagulation floculation process definition, its mechanism, coag-
ulant types, coagulant aids, in addition to the factors affecting coagula-
tion and in follow the models, which were applied to optimize these
factors to obtain high pollutants removal efficiency. Most of the parts,
which will be discussed in this review is represented in Fig. 2.
Protein, lipids, and carbs make up natural coagulants. Amino acids
and polymers of polysaccharides are the main building blocks. The pri-
mary mech-anisms influencing coagulation activity, according to earlier
studies, are charge neutralization and polymer bridging. Coagulation,
both natural and synthetic by adjusting the electrostatic charges of par-
ticles suspended in water, the chem-ical water treatment process known
as coagulation removes solids from water. The following graphical ab-
stract illustrates the major steps of the coagulation process 3.
In order to destabilize the charges on particles, colloids, or oily ma-
terials in suspension, this procedure introduces small, highly charged
molecules into water. The treatment of wastewater as many suspended
solids as possible must be eliminated during wastewater treatment before
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Fig. 3. The graphical abstract which illustrates the main steps of the coagulation process.

the leftover water, known as effluent, is released back into the environ-
ment. As solid matter decomposes, oxygen is depleted, which is necessary
for plants and animals to survive. A lot of mechanisms and processes are
established to treat water like chemical precip-itation, ion exchange,
membrane filtration, Coagulation, electrolytic recovery, adsorption and
Reverse osmosis. The following Table 1 illustrate the differ-ent processes
which treat water in different mechanism. The table 1illustrates within
advantages and disadvantages columns the environmental and economic
aspects [14].
2. Coagulation
Coagulation was applied for the removal of dyes from different
polluted types of wastewater that can be represented in Fig. 4 and mainly
have been applied for dyes removal from many years [15]. The properties
of the coagulants used are important for determining the coagulation
performance, as they can improve or hinder the effectiveness of the
treatment [16,17]. In addition to the type of coag-ulant, several factors
were specified to promote the coagulation efficiencies, such as the vol-
ume of the coagulant dose, the pH, the speed and duration of the mix-ing,
the temperature, and the settling time [18,19]. These parameters should
be controlled, reducing performance, and pathological impur-
ities/contaminants are to be reduced and improved. Because the addition
of coagulants increases of mechanisms and processes are established to
treat water like chemical precip-itation, ion exchange, membrane filtra-
tion, Coagulation, electrolytic recovery, adsorption and Reverse osmosis.
The following Table 1 illustrate the differ-ent processes which treat water
in different mechanism. The table 1illustrates within advantages and
disadvantages columns the environmental and economic aspects [14].
The insoluble compounds in the sample being treated, coagulation
requires the process of flocculation to function efficiently where coagu-
lation alone does not aid much [20]. Therefore, a flocculation step that
allows slow mixing is essential as the key to optimal performance. The
second step is to recognize the collision and thereby improve the
agglomeration between the particles. The experiment is carried out in
two stages of mixing speed; Fast and slow mixing. Coagu-lants are usually
added during the fast mix to mix the coagulants with the water samples
before the slow mixing speed is applied at the scheduled time. For
agglomeration particle formation during the settling process, adequate
mixing time for both stages is critical [20] and is followed by separation
the solids or sludge from treated water. There are certain cationic co-
agulants such as alu-minum or iron salts that can be defined as primary

Table 1
The comparison between different processes for wastewater treatment based on advantages, disadvantages and its fabrication materials.
Processes Material Advantages Disadvantages

Chemical Lime, alkali, sulfide/flocculants, The wastewater had a low metal concentration. High chemical requirements, keeping pH at the ideal level, and
precipitation surfactants, acids, bases, stirring, mixing, Large amounts of wastewater can be handled dealing with the difficulty of disposing of colloidal particle
and fluid handling are examples of with this method. Easy to use. sludge.This approach is highly challenging because a lot of
precipitants. variables, including temperature, pH, precipitant
concentration, etc., need to be watched carefully.
Ion exchange The ion Exchange synthetic or natural High treatment capacity and greater metal Costly synthetic resins that cannot be used on a big basis.
resins. removal rates.
Membrane Surfactants and Membranes Improve and Reusing wastewater can help you meet strict Membrane fouling is expensive to instal, maintain, and operate,
filtration Support the Process effluent limitations. obtaining valuable and it is less effective when the concentration of metal ions is
material and avoiding environmental harm. smaller.
Coagulation/ Reagents such as aluminum iron salts. Applicable the large-scale treatment of Costly chemicals, extensive sludge formation, and sludge
flocculation wastewater. disposal problems.
Electrolytic electric power Fewer chemical reactions, pure metal, and Energy expenses, high capital expenditures, and poor efficiency
recovery efficient removal of the required metal. at low concentrations are all factors. Higher wastewater volume
cannot be handled with this method.
Adsorption pumps, fluid handling equipment, and Highly efficient at reducing heavy metals to Chemical regeneration needs, corrosion and fouling of the
regenerators for a steady, uniform flow acceptable levels. treatment facility, disposal of used adsorbents, high-cost
processing of adsorbents such activated carbon, and loss of
adsorption capability by the adsorbent during each cycle.
Reverse osmosis membrane-supported resins Effective wastewater metals removal. High chemical expensesand membrane fouling.

4
R.M. El-taweel et al.
coagulants. On the other hand, the treatment can also be combined with
other polymeric flocculants that support faster and more time-consuming
sediment formation in small flocs [17]. However, the excessive use of
chemical coagulants also creates an additional problem such as a large
amount of sludge formation which indicates the desire to use natural
coagulants as coagulants [21,22]. Comparison between coagu-lation
process, and the physicochemical processes of wastewater treatment
was performed in Table 2, in addition to its efficiency in contrast to other
processes as shown in Table 3.
3. Coagulation mechanism
Most solids or suspended particles are smaller and carry negative
charges in an aqueous medium (see Fig. 3). Accordingly, to facilitate the
sedimentation process, the particles must clump together to form larger
flocs, as displayed in Fig. 5. However, this process is problematic because
of the electrostatic repulsive forces that prevent negatively charged
particles from accumulating on the material [40]. Therefore, it takes
longer to settle and this problem can be solved by destabilizing the
particles using a coagulant. Destabilization can be achieved by one or
more of the following mechanisms after the addition of a coagulation
agent [41]: Electrostatic double-layer pressure, Adsorption and neutral-
ization of the charge, Adsorption and inter-molecular bridges, Immuni-
zation in the sediment with an excessive dose of coagulant.
The presence of unstable particles in the wastewater facilitates the
aggrega-tion or agglomeration of flocs after the addition of an appro-
priate fluctuation agent. The particles must eventually collide, which can
occur under normal circumstances.
4. Coagulant types
Coagulant can be classified into natural, and chemical coagulants that
were investigated as an agent through the coagulation process, as rep-
resented in.
Fig. 6. Natural coagulants are classified as plant-based coagulants
such as Guar gum, Gum Arabic, Seed Strychnos potatorum extract from,
Potato starch, and Cactus latifaria extract. Moreover, animal-based co-
agulants such as chitosan, and Micro-organisms-based coagulants as
Xanthan gum.
Whereas applied chemical coagulants were categorized into three
different classes; Hydrolyzing metallic salts as Alum, Ferric chloride,
Ferric sulfate, and Magnesium chloride. The second class is Pre-
hydrolyzing metallic salts that were represented in Polyaluminium sul-
fate, Polyaluminium chloride, Polyferric chloride, Polyaluminium ferric
chloride, and Polyferrous sulfate. Meanwhile, the third class is synthetic
cationic polymers such as aminoethyl polyacry-lamide, Polyamine Pol-
yalkylene, Polyethylenimine, Polydiallyldimethyl ammo-nium chloride.
Additionally, the most applied coagulants agents can be dis-cussed as
follow.
4.1. Chemical coagulants
Chemical coagulants fall into different classes due to their effective-
ness in removing dyes from textile effluents. The former are hydrolyzed
mineral salts such as ferric chloride, ferric sulfate, magnesium chloride,
and alum. The sec-ond is the mineral salts before hydrolyses, such as poly
ferric chloride, poly ferric sulfate, poly aluminum chloride, poly
aluminum sulfate, and poly ferric aluminum chloride. The last category
includes synthetic cationic polymers such as aminomethyl poly-
acrylamide, polyalkali, polyamine, polyethylene, and poly dia-
llyldimethyl ammonium chloride [23].
Effective and simple operation is the main reason for the widespread
use and inorganic coagulants practice such as alum (aluminum sulfate),
ferric chlo-ride, and poly aluminum chloride in wastewater treatment
[42,43]. Synthetic coagulants have also been applied in the industry of
drinking water. Conven-tional mineral coagulants such as Al (III), and Fe
5
Current Research in Green and Sustainable Chemistry 6 (2023) 100358
(III) are the most widely applied coagulants and have greater advantages,
but still cannot avoid some of the disadvantages commonly known as the
lack of green chemistry [44]. Some of the reported chemical coagulants
and their bleaching performance for tissue wastewater are summarized
in Table 4.
Fig. 7 illustrates a water treatment process of a textile industrial plant
by using a mixture of chemical coagulants. Firstly, the effluent stream
from the industrial plant is neutralized and equalized, the effluent is then
sent to a reactor where water is mixed with chemical coagulants (such as
ferric sulfate, ferrous sulfate ferric chloride, and ferric chloride sulfate in
order to destabilize colloidal and finely divided materials and cause them
to start aggregating. In the process of treating wastewater, various
chemicals such as coagulants like magnesium carbonate, hydrated lime,
etc., may also be used. The wastewater's composition affects the coagu-
lant selection and dosage. By creating extremely adsorptive multi-
charged polynuclear complexes, aluminum, and iron coagulants func-
tion. The properties of the complexes and their efficiency can be
controlled by adjusting the pH of the system. The effluent is now sent to a
flash flocculation mixer, where agitators thoroughly combine the co-
agulants with the wastewater. To set up the circumstances for efficient,
effective water treatment, this phase is crucial. It is recommended to keep
the flash mixing duration between 30 and 60 s. After 30 s, the chemicals
won't be distributed correctly. After 60 s, the mixer blades once more
tend to cut or shear the aggregating material back into smaller pieces.
After coagulation, flash mixing is necessary to neutralize the electrical
charge of tiny particles in order to cease the attraction of like-charged
particles and allow the particles to start bonding and creating larger
clumps. Following flash mixing, flocculation starts, which slowly and
gently mixes the small particles created during the coagulation step until
they come into touch with one another (approximately 30–45 min time is
needed for the process). An existing treatment plant tube settler can be
used to enhance the clarifiers and sediment basins, as well as to lessen the
solid load on the filters farther downstream. Essentially huge flocks settle
in a primary tube settler when the mixing is finished. After the sludge
settles, the liquid that remains is transported to the aeration tank and is
largely free of the suspended and dissolved solids that were previously
present in the effluent [53].
There are certain risks accompanied while using chemical coagulants
to human health and living organisms in the area, such as Alzheimer's
disease, which occurs when aluminum residues enter the human body
and accumulate in the brain [54–57]. Other risks were addressed,
including constipation, cramps, abdominal cramps, and loss of energy
[58]. The post-coagulation pro-cess also produces large amounts of toxic
sludge, which makes the removal pro-cess difficult. Toxic sludge are
usually the result of unreacted chemical residues and the reaction of
polymer by-products in the treated water [59]. The result-ing sludge
cannot be avoided because during the coagulation process the larger flocs
are formed by smaller approaches to one another [60]. The resulting
sludge requires an additional step in the treatment process, with coagu-
lation being re-ferred to only as pretreatment. In addition, due to the
effective coagulant, which only works under certain conditions, the pH of
the wastewater must first be changed. A flat-bottomed glass reactor (HS
33) with a hot-plate magnetic stirrer was used to leach a total of 25 g of
pulverized aluminum dross using 500 mL of a 16 mol/l solution. HCl for
various amounts of time (15–240 min) at various leaching temperatures
(298–373 K). It was then filtered to get rid of any undissolved materials.
The solution was added to a 25% NH3 solution to precipitate after being
separated from the solid residue. By adding 5% NaOH solution and
reprecipitating with 10% NH4Cl solution, Al(OH)3 was purified. The
leached solutions were diluted and examined using a Shimadzu AA-7000
F atomic absorption spectrophotometer [61].
4.1.1. Aluminum-based coagulants
Aluminum is a type of metallic salt chemistry that is complex where it
involves three steps; dissociation, hydrolysis, and polymerization.
Equations of these steps can be expressed as follow:
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Table 2
Various applied wastewater treatment techniques.
Process Characteristics Main Idea Mechanism Advantages Disadvantages Ref

Coagulation/ It is considered the Adding coagulants  Coagulants neutralize  Simple process  Physicochemical [23]
Floculation backbone of technology in (chemical, or natural) negative charges of  Integrated parameters should be
most wastewater to help precipitate pollutants, physicochemical optimized.
treatment plants as a first pollutants using  After that, it reduces the process.  Increased sludge volume
step in the wastewater filtration, and electrostatic repulsion of  Wide range of chemicals generation.
treatment stages. sedimentation. the electric double-layer as could be applied.  Low ability to remove
destabilization process,  Cost-effective. arsenic.
 After the destabilization of  Efficient for sludge
the particles, particles settling.
develop and gradually  Help reduction of
aggregate into large flocks, chemical oxygen.
 Under free precipitation or
air flotation, flocs are
sperated from the water.
Electrocoagulation It is widely applied to It depends on the The process of  Increases  Requires addition of [24]
drinking water supply Electrolysis process. Electrocoagulation can be biodegradability, chemicals,
treatment, and defined as the in-situ  Very effective and rapid  Sludge deposition on the
contaminants removal, coagulants generation by organic matter electrodes can inhibit the
municipal and industrial electrolytic oxidation of a separation then the electrolytic process in
wastewater treatment sacrificial anode, which was traditional coagulation, continuous operation,
such as inorganic, caused by the electric current  pH control is not  Need filtration process for
organic, and biological applied through the necessary; generation of formed flocs,
contaminants removal electrodes. coagulants in situ;  Sludge treatment cost.
from the contaminated economically feasible.
water.  very effective in
removing suspended
solids, dissolved metals,
tannins, and dyes from
paints and textile
industries.
Chemical It is popular emerging Usually needs Various activation techniques  Integrated  Require Chemicals [25]
oxidation technology, which could application of are applied to produce physicochemical  Production, transport, and
be applied effectively in oxidants such as; O3, hydroxyl radical (HO), and in process, management of the
treatment of organic Cl2, ClO2, H2O2, follow destroy organic  Simple, rapid, and Oxidants, which applied in
pollutants in wastewater. KMnO4. compounds through electron efficient process, the process.
transfer mechanisms.  Increases  Efficiency varies according
biodegradability of to the type of oxidant.
product,  Unknown intermediates
 No sludge production, could be formed.
 Applied in disinfection  Release of some volatile
from bacteria and compounds and aromatic
viruses. amines.
 Minimize the pollutants
spread and reduce
treatment costs.
Adsorption It became a very common Nondestructive Adsorption is a  Technologically simple  Requirement for several [26]
process for wastewater process Use of a solid physicochemical the (simple equipment), types of adsorbents,
treatment, lately due to material treatment process in which  Could be applied in  Need chemical
their higher removal pollutants are adsorbed many treatment formats, derivatization to improve
efficiencies over the other physically and chemically  Availability of wide their adsorption capacity,
techniques. bonded to the adsorbent range of commercial  Rapid saturation and
surface. products, clogging of the reactors,
 Highly effective process  Regeneration costs are
with fast kinetics, high,
 Treat effluents with high  Elimination of the
quality, adsorbent requires high
 Possibly selective costs processes such as
depending on the centrifugation.
adsorbent type.
Ion exchange Ion exchange is a process Nondestructive Ion exchange is a process in  Technologically simple,  Requires large columns, [27]
of purification, process which an exchange of ions  Easy control and  Rapid saturation and
separation, and of between two electrolytes or maintenance, reactor clogging,
aqueous, or ion- an electrolyte solution and a  Easy to be applied with  precipitation of metals and
containing solutions. complex. They could be in other techniques such as blocking of the reactor,
They are usually two forms, cation exchangers,  precipitation and  It requires a
identified as ion exchange which exchange positively filtration, physicochemical pre-
resins, clay, zeolites, or charged ions or anion  Produce a high-quality treatment e.g., sand filtra-
soil humus. exchangers, which exchange treated effluent, tion or carbon adsorption
negatively charged ions.  Inexpensive process, to remove large
 Efficient for metal contaminants.
removal,  Conventional resins of the
 Could be selective for process are not selective,
certain metals, and  Selective resins have
beneficial for the limited commercial use.
(continued on next page)

6
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Table 2 (continued )
Process Characteristics Main Idea Mechanism Advantages Disadvantages Ref

recovery of valuable
metals.
Membrane Membrane filtration Nondestructive It could depends on the  Availability of a wide  High costs for small and [28]
filtration could be represented in separation pressure-driven membrane range of commercial medium industries,
various forms as follows; Semipermeable processes, or direct membranes,  Require high energy,
 Microfiltration (MF) barrier membrane process in which  Require small space,  High operation costs,
 Ultrafiltration (UF) only physical separation  Simple, rabid, and highly  Limited flow rate,
 Nanofiltration (NF) occur. efficient even at high  Low throughput,
 Reverse osmosis concentrations,  Not effective at low solute
 Dialysis  No need for chemicals, feed concentrations,
 Electrodialysis (ED)  Low solid waste  Type of the membrane
 Electro-electrodialysis generation, according to the process;
(EED)  High capacity for all hardness reduction,
 Emulsion liquid types of dyes, salts, and removal of particulate or
membranes (ELM) mineral Derivatives, total organic carbon,
 Supported liquid  Produce high purified  potable water, etc.
membranes effluents.
Biological methods It is an important and Use of biological Using aerobic and anaerobic  Application of  You should create an [29]
integral part of any (pure or mixed) micro-organisms for microorganisms for the optimally favorable
wastewater treatment cultures for pollutants pollutants degradation. organic contaminants  Environment for
plant, which treats removal. biodegradation simple, microorganisms growth,
wastewater from either economically attractive  Requires management and
municipality or industry. and well accepted by the maintenance of the
It have soluble organic public. microorganisms,
impurities or a mix of the  Microorganisms produce  Low biodegradability of
two types of wastewater a wide variety of certain molecules such as
sources. extracellular enzymes, dyes,
which characterized by  Bulking and foaming of
its high biodegradability sludge,
capacity  Biological sludge and
 Efficiently eliminates uncontrolled degradation
biodegradable organic products generation,
matter.  It is important to know the
 High removal capacity of mechanism of enzymatic
biochemical oxygen processes governing the
demand and suspended decomposition of the
solids. substances, which makes
the microbiological
mechanisms complex.

Dissociation Metal cations in water are present in a hydrated form as
aquocomplexes as follow:
Al2(SO4) þ 12H2O ¼ 2Al(H2O) þ 3SO2
4 (1)
Hydrolysis The aquometal ions formed in the dissolution of alum in
water are acidic or proton donors, which would be presented by the
following equa-tions:
concentration of alum over its solu-bility in water, hydrolysis process
takes place and adding of further dosage, a variety of hydroxocomplexes
were formed that followed by hydroxometal poly-mers production and
finally the aluminum hydroxide precipitates formation. Hence, it was
found that alum dissolution in water increases the hydrogen ions con-
centration, and drops the pH or the consumption of present alkalinity
were noticed and can be described as follow:

Al(H2O) 3þ þ H2O ¼ Al(H2O) (OH)2 þ H3Oþ (2a) Al2(SO4)3.14.3H2O þ 3Ca(HCO3)2 ¼ 2Al(OH)3 þ 3CaSO414.3H2O þ 6CO2
(3)
Al(H2O) (OH)2þ þ H2O ¼ Al(H2O) (OH) þ þ H3Oþ (2b)
The previous reaction equation showed that adding 1 mol of alum
Al(H2O) (OH) 1þ þ H2O ¼ Al(H2O) (OH) þ H3Oþ (2c) dose consumes 6 mol of alkalinity and carbon dioxide that means that
2 every mg/l alum decrease alkalinity by 0.50 mg/l and produces 0.44 mg/
Al(H2O) (OH) þ H2O ¼ Al(H2O) (OH) þ H3Oþ (2d)
l carbon dioxide.
Polymerization The hydroxo complexes formed as products of hy- Furthermore, if the natural alkalinity is not sufficient, soda ash and
drolysis may combine to form a variety of hydroxo metal polymers, and lime can be added, and the reaction is as follow:
equations of the process could be presented as follow:
Al2(SO4)3.14.3H2O þ 3Ca(OH)2 ¼ 2Al(OH)3 þ 3CaSO4 þ 14.3H2O (4a)
The formed hydroxometal polymers at the end of the process are.
Al2(SO4)3.14.3H2Oþ3Na2CO3þ3H2O ¼
1. Al6(OH)3þ
15 , 2Al(OH)3þ3Na2SO4þ14.3H2Oþ3CO2 (4b)
2. Al7(OH)17 4þ,
3. Al8(OH)4þ
20 , and
Lime was considered one of the most used chemicals due to its low
4. Al13(OH)5þ
34 .
cost, although soda ash has an advantage than lime where it does not
increase water hardness. The optimum applied pH in the coagulation of
The addition of alum to an aqueous solution aids in the development alum was around 6, with an effective operational range between pH 5
of mas-sive positively charged complexes that are insoluble in water, and 8 [63].
resulting in the generation of hydrogen ions [62]. After that, the pH of
the coagulant was de-termined, and the coagulant dose should be taken 4.1.2. Ferric-based coagulants
into consideration. Increasing the coagulant dose such as increasing the Ferric salts such as ferric sulfate and ferric chlorides behave in water

7
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Table 3 Table 3 (continued )

Previous applied techniques for dyes removal from polluted wastewater and their Process Pollutant Factors Removal Ref.
capacity. efficiency (%)
Process Pollutant Factors Removal Ref.  Temperature is
efficiency (%) 25  C.
Coagulation Sulphur  Coagulant 86.1 [30] Ionic Direct  Contact time; 3 h 90 [37]
process black dye dosage is 40 mg/ flocculation Yellow 27 of contact time.
l, process by  Temperature
 Calcium dosage sing a mixture range 30–40  C.
is 6 g/l, of surfactants
 Dye Coagulation Reactive  80 ppm dosage.  Nearly 100% [38]
concentration is with organic Blue  pH of 5. color removal
200 mg/l, coagulants  Dye
 pH 4. concentration
Biological Methylene  1% adsorbent 88 [31] 0.2 g/l.
Adsorption by Blue dosage, Filtration and Methylene  Temperature  Adsorption [39]
microbial  Dye the adsorption blue from 15 to 35  C. capacity
biomass concentration of on the porous  MB 3506.4 mg/g.
300 mg/l, calcium concentration:  Removal of
 pH value 7, alginate 300 mg/l, MB adsorbed
 Temperature 30 membrane.  Time 4 h, by

C,  pH 6–10, membrane:
 2 days contact  Adsorbent 96%.
time. dosages 0.5 g/l.
Advanced Direct Blue  Dye  About 62% [32]
oxidation 86 concentration reduction in
process 100 ppm, COD. in a way similar to that explained in the alum state. The following
 pH; 11,  Dye equation can explain the process of dissociation, hydrolysis that was
 Contact time; 35 reduction; 98. noticed and was similar to that obtained through the alum process [64].
min,
 Temperature;
Dissociation process
less than 40  C.
Ion exchange  C.I. Acid  Shaking rate; 88.3 [33]
Fe2(SO4) þ 12H2O ¼ 2fe(H2O) 3¼ þ 3SO2
4 (5)
Orange 7, 180 rpm,
 C.I. Direct  Dosage is 0.5 g,
Hydrolysis;
 Contact time is 3
Fe(H2O)3þ þ H2O ¼ Fe(H2O) (OH)2þ þ H3Oþ
Blue 71,
(6)
 C.I. h,
Reactive  Dye
Polymerization; This resulted in the formation of ferric dimer Fe(OH)
Black 5. concentration is 4þ
10 mg/l,
 pH 5, Additionally, Iron salts are acidic in solutions and consume alkalinity:
 Temperature of
24  C. Fe2(SO4)3 þ 3Ca(HCO3)2 ¼ 2Fe(OH)3 þ 3CaSO4 þ 6CO2 (7)
Nano-filtration, Cibacron  Density; 33 mA/ 98 [34]
or Ultra- Yellow S-3R cm2, Whereas, in the state of adding lime, and soda ash, the reaction will be as
filtration.  Dye follow:
concentration;
0.1 g/l, Fe2(SO4)3 þ 3Ca(OH)2 ¼ 2Fe(OH)3 þ 3CaSO4 (8a)
 pH 3,
 Salt (sodium Fe2(SO4)3 þ 3Na2CO3 þ 3H2O ¼ 2Fe(OH)3 þ 3Na2SO4 þ 3CO2 (8b)
chloride)
concentration; An illustration of the production process for alumina from aluminum
60 g/l. dross is shown in Figs. 8 and 9. The following chemical reactions illus-
Reverse osmosis Anthrasol  Dye 94 [35]
trate the mechanism of Alumina production [61]:
brown IBR concentration of
30 mg/l,
AL2O3 þ 6HCl ¼ 2AlCl3 þ 3H2O (9)
 Feed
concentration of
2Al þ 6HCl ¼ 2AlCl3 þ 3H2O (10)
30 ppm,
 pH value 4,
Fe2O3 þ 6HCl ¼ 2FeCl3 þ 3H2O (11)
 Temperature of
25  C.
CaCO3 þ 2HCl ¼ CaCl2 þ CO2 þ H2O (12)
 Runs No. is 4.
Reverse osmosis Methyl  Dye 99.8 [36] AlCl3 þ 3NH4OH ¼ AL(OH)3 þ 3NH4CL (13)
orange concentration is
100 mg/l, Al(OH)3 þ NaOH ¼ NaAlO2 þ 2H2O (14) NaAlO2 þ H2O þ NH4Cl ¼
 Feed pressure is
400 psi,
AL(OH)3 þ NACl þ NH3 (15)
 Flow rate is
2Al(OH)3 ¼ AL2O3 þ 3H2O (16)
higher than 2 l/
min,
 pH between 2
and 4,
 Salt 4.1.3. Sodium aluminate coagulants
concentration is The main difference between sodium aluminate and the common
100 mg/l,
coagulants, its alkaline nature rather than acidic, where it reacts with
natural carbon dioxide and production of aluminum hydroxide as follow:

8
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Fig. 4. Different applications of coagulation processes in different types of water treatment.

Fig. 5. Coagulation, and flocculation principle.

Fig. 6. Different types of coagulants.

9
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Table 4
Different coagulant materials agents previously applied in the coagulation
process.
Coagulant name wastewater Conditions Efficiency (%) Ref.

Alum Color-dyes Optimized dose 74 [45]

5000 mg/l, pH4
Ferric chloride Color-dyes Optimized dose 71 [46]
293 mg/l, pH 6
Ferrous Sulfate Sulphur-dyes Optimized dose 90 [47]
200 mg/l, pH 9.4
Polyaluminium acid and di- Optimized dose 80 [48]
chloride rect dyes 0.1 mg/l, pH 8
Magnesium Color Optimized dose 100 [47]
chloride 120 mg/l, pH 11
Ferrous sulfate Reactive Optimized dose 90 [49]
400 mg/l, pH 12.5
Al2(SO4)3 Natural Dose 5–50 mg/l, 43.2 [50] Fig. 8. The production process for alumina from aluminum dross [61]. Copy-
water pH 4-9 right 2015, Springer.
Alum Textile Initial pH 8.6–9.9, 20 (Turbidity), [51]
wastewater Initial COD: 65 (COD), 42
1000–1200 mg/l, (COD), 74 4.1.5. Organic polymers coagulants
Initial turbidity (Color). Synthetic organic polymers are known as molecules of long-chain that
45–117 NTU, alum were composed of monomeric units and smaller subunits. Polymers,
dose 100 mg/l
which contain ionizable groups as sulfonic, carboxyl, or amino groups,
ferric chloride Textile Initial pH 6, Initial 98 [52]
effluents dye content: 0.1 g/ are identified as poly-electrolytes, whereas; polymers without ionizable
l, coagulant dose groups are identified by non-ionic. Meanwhile, polyelectrolytes could be
400 mg/l anionic, cationic, or ampholytic that contains both positive and negative
polyacrylamide Reactive Initial pH 8.8–9.4, 68.2 (COD) [47] groups. Polymers were reported as excellent coagulants due to their
þ Alum dyes Initial COD 595 76.3 (BOD5)
wastewater. mg/l, Initial TSS, 61.4 (TSS)
higher ability in the destabilization of particles by charge neutralization,
coagulant dose interparticle bridging, or both. Anionic and nonionic polymers destabi-
200 mg/l alum, 1 lize negatively charged colloidal particles through their bridging effect.
mg/l poly- whereas, cationic polymers have the ability to coagulate and destabilize
acrylamide
such particles by both charge neutralization and interparticle bridging
[67,68].
2NaAlO2þCO2þH2O ¼ 2Al(OH)3þNa2CO3 (17)

However, Sodium aluminate is most commonly used coagulants in

combi-nation with alum in the boiler water treatment technology, which
produce alu-minum hydroxide floc in a similar way of sodium aluminate
reaction with acidic carbon dioxide:
6NaAlO2þAl2(So4)314.3H2O ¼ 8Al(OH)3þ3Na2SO4þ2.3H2O
Sodium aluminate can be obtained by dissolving alumina in sodium
hydrox-ide.
4.1.4. Polymeric inorganic salts coagulants
Applying polymeric ferric and aluminum salts as a coagulant for
turbid water was increased in the last period, such as Polyaluminum
chloride that was used for the potable water treatment in different
countries such as Germany, France, and Japan with large scale [13,65].
Commercial preparation of these compounds is available; however, they
were commonly prepared in the site by adding a base to neutralize the
concentrated solutions of ferric and aluminum salts. The polymerization
process was affected by salt solution concentration, base solution type,
and concentration, temperature, and ionic strength [66].
4.2. Natural coagulants
Natural coagulants have gained popularity in recent years due to their
bene-fits and also the proven fact that they solve most of the matters
(18) associated with the chemical coagulants employment. Natural Co-
agulants are highly efficient in the coagulation process especially those
made from plant extracts that are always abundant and known to be freed
from toxins [69]. Numerous studies are conducted on the employment of
natural coagulants made or extracted from a vegetable, animal, and
agricultural wastes like moringa seeds (MO), chitosan, and cassava peels
[70]. The biodegradable properties of natural coagulants, which are
believed to be harmless to live organisms and the environment, ex-isted
primarily before the appearance of chemical salts to clarify wastewater
[69,71]. The lowering mass of natural polymers are the main reason for
the less efficient coagulation [72,73]. Natural coagulants, particularly
tannin-based (TB) ones, have been extensively studied as an alternative
to toxic chemicals over the past ten to fifteen years. The benefits of
employing these eco-friendly solutions to cleanse various water, waste-
water, and effluent types, particularly from the dairy, cosmetics, laundry,
textile, and other sectors, are highlighted in this review study. Turbidity,

Fig. 7. Schematic of a typical textile wastewater treatment plant [53]. Copyright 2017,Butterworth-Heinemann.

10
R.M. El-taweel et al.
Fig. 9. Schematic illustration of the synthesis of Modified tannin coagulant [75]. Copyright 2021, Elsevier.
Fig. 10. The primary structure and probable molecular interactions of tannin in
an aqueous solution [75]. Copyright 2021, Elsevier.
color, suspended solids, soluble organic matter (chemical/biochemical
oxygen demand), and inorganic matter (total phosphate, and heavy
metals) can all be effectively eliminated by TB coagulants. TB co-agulants
can be used as coagulant-aid to lessen the intake of chemicals and are
compatible with other treatment approaches. Due to less alkalinity being
used, infrequent pH adjustments, and the creation of less biodegradable
sludge, TB coagulants can lower water treatment running costs. Utilizing
wastes and by-products from the bark of some particular trees and the
skins and pomace of other fruits and vegetables, TB coagulants can be
created as shown in 9 and the primary structure and probable molecular
interactions of tannin, are illus-trated as shown in 10. On TB coagulants,
the strengths, weaknesses, opportu-nities, and threats (SWOT) are
reviewed. Although TB coagulants are making progress, there are still
certain obstacles to be solved, particularly regarding tannin extraction
and cationization. Other weaknesses that must be overcome include the
market competition from conventional coagulants, the viability of
application in actual waters, and the industries’ resistance to change
[74].
Natural coagulants have a similar mechanism of action to poly-
electrolytes and contain a variety of functional groups such as –OH,
–COOH, and -NH2. 11 depicts a schematic representation of the coagu-
lation mechanisms discovered by FT-IR and SEM [76].
Natural coagulants can be classified into three types and they will be
discussed as follow.
4.2.1. Plant-based coagulants
Plant-based natural coagulants coagulate either by polymer bridges or
charge neutralization and may be obtained from various components of
plants. Var-ious types of plant were applied in the polymers extraction
like starch, gum, seeds, tannin, Moringa oleifera, and cactus, etc. and
11
Current Research in Green and Sustainable Chemistry 6 (2023) 100358
were generally well docu-mented as effective coagulants [77]. Addi-
tionally, these extracted polymers have many industrial applications as
their nature is polysaccharides and possess various commercial applica-
tions like in the paper industry, or as food additives, etc. Moreover, the
effectiveness of natural polymer was stated by application of some types
Ipomoea dasysperma seed gum and guar gum as a coagulant aids with
PACl and their efficiency of removal was 86% and 87% towards dyes by
applying PACl dosage of 1 mg/l and dasysperma seed gum dosage of 5
mg/l each, at optimum pH of 9.5. Significant 73% and 80% removal of
dyestuff at an equiv-alent dosage of coagulant and coagulant aid and also
the same pH of 9.5 [78]. Moreover, Strychnos potatorum (Nirmali) seeds
were applied as polysaccharides source which may effectively could
reduce 80% turbidity of kaolin solution [79].
M. oleifera, commonly called the drumstick tree is widespread
throughout India, Asia, and a few parts of Africa and America. The bark,
root, fruit, flowers, leaf seeds, and gum of the tree also were used as
medicines. The seeds of those trees are used as a coagulant and/or floc-
culant in water and wastewater treatment. For instance, M. oleifera seeds
were applied for anthraquinone pigment removal with a 95% pigment
removed by using a coagulant dose of 100 mg/l and pH 7 [80].
Furthermore, Methylene blue was removed by employing a hydrogel
com-posed as a coagulant where modified gum, polyacrylate, and poly-
acrylamide achieved 98%of dye removal efficiency at pH 8 with a
maximum adsorption ca-pacity of 48 mg of dye per gram of hydro gel.
However, gum has not yet been applied for the color removal due to the
dyes that are widely utilized in the textile industries [81].
4.2.2. Animal-based coagulants
Chitosan is usually a linear copolymer of D-glucosamine (deacetylated
unit) and N-acetyl-D-glucosamine (acetyl unit), which was produced by
the chitin deacetylation, a natural polymer of great importance [82]. The
deacetylation degree is typically determined by nuclear resonance
spectroscopy. Chitin is the structural component of the exoskeleton of
crustaceans (crabs, shrimps, etc.) and therefore the endoskeleton of other
invertebrates. Chitosan has several intrinsic properties like non-toxicity,
biodegradability, and excellent chelating behavior, making it an efficient
coagulant for removing impurities in the dissolved state [83]. Various
studies has investigated the chitosan effectiveness in the coagulation
process and suspended solids (SS) recovery within the treat-ment of
wastes from one sort of food processing industry and located that this
new coagulant was very effective in effectively reducing the COD also as
re-moving SS and turbidity. Several papers suggested that chitosan is
involved by a dual mechanism, including charge neutralization in
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

addition to coagulation and flocculation by a bridging mechanism [84]. Table 6

Carboxymethyl chitosan has been applied for wastewater treatment in The kinetics parameters of the adsorption process of Cr (VI) by IIP@GO-Fe3O4
printing and dyeing. Experimental results have shown that carbox- and NIP@GO-Fe3O4 adsorbents [98].
ymethyl chitosan is superior to polymeric floc-culants commonly used in Kinetic models Parameters IIP@GO-Fe3O4 NIP@GO-Fe3O4
wastewater bleaching and COD reduction. Chitosan is employed to get PFO R2 0.962 0.899
rid of approximately 99% of the wastewater color from sim-ulated tissues K1 ðmin1 Þ 0.043 0.037
containing Acid Blue 92 at an optimal chitosan dose of 100 mg/l while qe ðmg:g 1 Þ 5.856 4.151
maintaining the optimal pH of 9 [85]. The efficiency of chitosan in MPFO R2 0.958 0.924
removing Acid Green 25 and Direct Red 23 was reported and it recorded Kðmin1 Þ 0.085 0.084
with approximately 75 and 95% for both of them respectively, within 10 qe ðmg:g 1 Þ 10.556 9.998
MPFO-2 R2 0.95 0.921
min at an optimum pH of 2 while maintaining a stirring speed of 200 rpm
Kðmin1 Þ 0.075 0.07
[86].
qe ðmg:g 1 Þ 1.474 1.311
PSO R2 0.99 0.993
4.2.3. Microorganism-based coagulants K2 ðg:mg 1 :min1 Þ 0.019 0.027
Microorganism-based coagulants included fungi, bacteria, and yeasts qe ðmg:g 1 Þ 9.671 5.139
[87]. Microorganism-based flocculants are called biotechnological tools MPSO R2 0.898 0.897
for their ap-plication within the wastewater treatment through the floc- Kðmin1 Þ 3128.85 6163.37
qe ðmg:g 1 Þ 3.628 1.8
culation method, which is safer and more biodegradable in contrast to
MPSO-2 R2 0.888 0.884
synthetic chemical floc-culants. The choice of microorganisms for mi- Kðmin1 Þ 16.961 8.484
crobial fouling often depends on their shape and ability to produce qe ðmg:g 1 Þ 0.062 0.098
extracellular viscous polysaccharides (EPS) [88]. Table 5 summarizes Bangham R2 0.878 0.855
some of the various plant coagulants applied in the industrial wastewater K0 ðmL2 :g 1 Þ 0.017 0.016
treatment and their effectiveness (see Table 6). Elovich R2 0.975 0.971
αðg:mg 1 : min1 Þ 5.757 0.629
βðg:mg 1 Þ 0.562 0.58
5. The kinetic modeling for the coagulation process Interparticle diffusion R2 0.981 0.984
Kid ðmg:g 1 :min0:5 Þ 8.633 8.536
The kinetic modeling for coagulation can be approached using a ki- Cid ðmg:g 1 Þ 16.847 7.975
netic model for adsorption. The goal of the kinetics models’ study is to Weber Morris R2 0.9504 0.946
identify cer-tain factors in order to define and quantify the process. It is Kint 3.278 1.001
possible to apply the pseudo-first-order kinetic model, the pseudo-
second-order adsorption kinetic model, the Elovich model, the modi-
5.2. Pseudo-second-order kinetic model
fied pseudo-first-order (MPFO), the modi-fied pseudo-first order-2
(MPFO-2), the Bangham kinetics model, the Elovich kinetics model,
The adsorption process was supposed to be a chemical reaction be-
the intraparticle diffusion kinetics model, the Weber-Morris ki-netics
tween the adsorbent and the adsorbate in this model. The determination
model, modified pseudo-second-order (MPSO), and modified pseudo sec-
of the adsorp-tion rate depends on chemical adsorption, but in some
ond order-2 (MPSO). The kinetics of adsorption is identified by using
circumstances, it is also necessary to take the movement of electrons into
various kinetic models to suit the experimental data. To determine which
account [93].
kinetic model best fits the experimental data, the computed results from
the kinetic models are contrasted with the data. Adsorption equilibrium t/qt ¼ 1/(K2.q2) þ (1/qe).t (20)
time, adsorption time, adsorption type, and the method by which the
adsorbent absorbs the pollutant are all measured as part of the adsorption Where K2: pseudo-second-order rate constant (g/(mg.min)).
kinetics study.
5.3. The elovich model

5.1. The pseudo-first-order kinetic model

Heteroatoms like oxygen (in minute amounts) can be found in the
porous structure of activated carbon. This model describes how hetero-
This model considered the process's strong dependence on mass
geneous solid surfaces operate and how the adsorption process and
transfer resistance, particularly at the start of the adsorption reaction
adsorption capacity are related indirectly [93].
[93].
qt ¼ α þ β.lnt (21)
log(qe  qt) ¼ logqe  (K1/2.303).t (19)
Where α, β:parameters of Elovish model.
Where qe: adsorbed amount at equilibrium in mg/g, qt: adsorbed amount
in mg/g at time t, K1: Rate constant (1/min), t: time (min).
5.4. The modified pseudo-first-order (MPFO) and the modified pseudo-
first order- 2 (MPFO-2)
Table 5
Natural coagulants used in industrial wastewater treatment. Yang and Al-Duri proposed the modified pseudo-first-order (MPFO)
Coagulant Removal parameters Ref. kinetic equation using empirical data. This empirical equation's ease of
Moringa oleifera seed Heavy metals; Cd, Cr, Mn (100%), respectively, and [89] use makes it a very alluring and practical tool for correlating experi-
Turbidity (98.6%), biochemical oxygen demand, mental data. By assuming the Langmuir model of adsorption and a ho-
BOD (11.7%) mogeneous solid surface, Rudzinski and Plazinski demonstrated the
Ocimum basilicum Basil as aid with alum; COD (76.4%), Color (80.4%) [90]
MPFO equation could match the behavior of the kinetic equation based
(basil)
Opunnia fcus-itdica Jebns laundrt effluent; COD (64.77%), turaidiyy [91] on the SRT approach quite well. When the system is close to equilibrium,
(91.26%), and Fabric dyenng mill efflueit; COD the statistical rate theory (SRT) method can be used to construct the
(87.19%), turbidity (93.62%) MPFO equation. The MPFO equation has previously been used to
Ribiscus Hosa- Hibiscus leaf aw aid sith PAC; COD (77.8%), [92] correlate adsorption kinetic data throughout the whole time period.
sinensis leaf extract suspended solids (99.4%), color (78.4%)
MPFO- 2 causes changes in the linear form of the integrated rate equation

12
R.M. El-taweel et al.
in the four modification models, which are obtained following respec-
tively [94].
qt/qe þ ((q * t2)/(2 * q2)) þ ln(qe  qt) ¼ k * t þ lnqe (22)
2 how well-suited NIP@GO-Fe3O4 is for the PSO model. The correlation
t/qt ¼ 1/(K * q ) þ (1/qe).t (23)
Where K:Rate constant of modified pseudo-first-order; modified pseudo-
first- order-2; modified pseudo-second-order; and modified pseudo-sec-
ond-order-2.
5.5. The bangham kinetics model
Further analysis of the pore diffusion's role as a rate-controlling phase
can be done using kinetic data. The following pore diffusion Bangham
equation limits the adsorption kinetics in this instance [95]:
log(logC0/(C0  qt.m)) ¼ log((K0.m)/(2.303.V)) þ α.logt (24)
Where m: The weight of adsorbent used per liter of solution, α: Initial
adsorption rate constant of Elovich model, Co:Initial adsorbate concen-
tration, K0:Bangham rate constant.
5.6. The intraparticle diffusion kinetics model
In this model, the diffusion resistance is neglected, and the direction
of adsorbate diffusion is random [93].
qt ¼ Kid.t0.5 þ Cid (25)
Where Kid: intraparticle diffusion rate constant (mg/(g.(min)1/2), Cid:
con-stants related to the thickness of the boundary layer.
5.7. The Weber-Morris kinetics model
Studies using highly porous adsorbents in shaken and discontinued
systems have shown that, in addition to adsorption over the particle
surface, dye diffu-sion from the external surface towards the sites inside
the pores can be seen. According to Weber and Morris, when the process
is regulated by intra-particle diffusion, the uptake of adsorbate varies as
the square root of time. The best-fit straight line's intercept should
roughly pass through the origin, which shows that the boundary layer
resistance is not very substantial. Larger intercepts, on the other hand,
suggest greater external resistance because they are inversely propor-
tional to boundary layer thickness. Diffusive transport across the exte-
rior layer and diffusion within the pores of the spherical particles are
thus taken into consideration in the empirical connection for the
adsorption process. The Weber-Morris plot, often known as the square
root dependency of the time, can be written as follows [96]:
logqt ¼ log(Kint þ 1/2.logt) (26)
Where Kint ¼ Internal mass transfer rate constant.
5.8. The modified pseudo-second-order (MPSO) and modified pseudo
second order-2 (MPSO)
Yang and Al-Duri modify the pseudo-second-order equation by add-
ing the qe/q component to the right side of the differential equation in
the pseudo-second-order model. The modified pseudo-second-order rate
equation and its integrated form (MPSO). The addition of the qe2/q2
component to the right side of the PSO equation is the other alteration.
The revised equation is known as modified pseudo-second-order-2
(MPSO-2) [97].
qt/(qe  qt) þ ln(qe  qt) ¼ qe.K.t þ lnqe (27)
qt/qe þ 2.ln(qe  qt) þ qe/(qe  qt)  1 ¼ k.t.qe þ 2.lnqe (28)
13
Current Research in Green and Sustainable Chemistry 6 (2023) 100358
5.9. The adsorption of Cr (VI) by IIP@GO-Fe3O4 and NIP@GO-Fe3O4 as
adsorbents
6 shows how Cr(VI) is adsorbed on the surface of IIP@GO-Fe3O4 and
coefficient values of R^2 ¼ 0.990 for IIP@GO-Fe3O4 and R^2 ¼ 0.993 for
NIP@GO-Fe3O4 are what make them suitable. The Cr(VI) ion's theoret-
ically predicted adsorp-tion capacity and the adsorption capacity deter-
mined through tests are highly compatible. A theoretical count using the
PSO model yielded the value itself. The PSO model's applicability leads to
the conclusion that the specific active sides located on the adsorbent
surface are responsible for the Cr(VI) adsorption on IIP@GOFe3O4.
These outcomes also permit chemisorption, which involves an exchange
of electrons between the analyte, Cr(VI), and the adsorbent. The Cr(VI)
adsorption experimental data analysis's modified equation form exhibits
less linearity than the early PFO and late PSO. The modification alters the
lin-ear form of the integrated rate equation in each of the four modifi-
cation models by multiplying the differential rate equation by the qe/q
factor for MPFO and MPSO and (qe/e)2 for MPFO-2 and MPSO-2. As
shown by the R^2 value, which reaches 0.981 for IIP@GO-Fe3O4 and R2
of 0.984 for NIP@GO-Fe3O4, which shows that there is no shape multi-
linear on the curve, the probability of intraparticle diffusion resistance to
influence and control the adsorption process as a rate control stage ap-
pears to be relatively high [98].
5.10. The elimination of MN dyes by sugarcane bagasse and peanut hulls
Various statistical indices, such as the correlation co-efficient (R), co-
efficient of determination (R2), and the performance of the three models
(RSM, ANN, and ANFIS), were used to assess each model's effectiveness.
The optimum method to predict the percentage elimination of MN dyes
by sugarcane bagasse and peanut hulls was determined using mean
squared error (MSE), root mean squared error (RMSE), mean absolute
error (MAE), and mean squared error (MSE). RSM, ANN, and ANFIS
models were used to analyze all the trained and tested data sets. If there is
more agreement between the projected and actual values, the R and R2
values are closer to unity. As can be shown from 7, ANFIS models per-
formed best for both sugarcane and peanut hulls, indicating high accu-
racy for ANFIS models, however other statistical indices should be as low
as feasible for improved model accuracy. It is obvious that the ANFIS
results using RSM and ANN models are highly excellent [99].
6. Transformation from chemical coagulants into natural coagu-
lants
The transformation from chemical to natural coagulant could be an
alter-native solution to limit the environmental pollution and the health
problems resulted from the chemical coagulants [100]. Additionally, it is
promoting the application of the green technology in the water and
wastewater. Natural coag-ulants can be obtained from natural sources
such as plants, and animals [101]. Plant-based coagulants was discovered
and applied from decades ago, where their application were stated before
chemical coagulants. For instance, in the 20th century chemical co-
agulants mechanism, which was responsible for bet-ter coagulation
techniques started to be identified by researchers [102]. However
chemical coagulants had a great interest lately, various drawbacks were
identi-fied, and noticed. Furthermore, chemical coagulants costs high
more than nat-ural coagulants, which obtained from the natural re-
sources, in addition to their environmental eco-friendly nature. for
instance, the plant wastes is the most applied plant-based coagulants,
where every part in the plants from the stem to the leaf was demonstrated
as a potential natural coagulants [103]. While, the animal-based co-
agulants could be obtained from animal wastes such as shells, and bones.
The active coagulant agents could be classified into three categories;
protein polymers, functional groups such as carboxyl and hydroxyl
groups, phe-nolic compounds in addition to the polysacharides. These
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

functional groups influence the adsorption mechanisms, charge Table 8

neutralization, and polymer bridg-ing [104]. Different coagulant aids were applied in the coagulation processes.
Both chemical, and natural coagulants show a high removal capacity Coagulant aids Importance
towards the various pollutants appear in the wastewater with almost
Alkalinity Alkalinity should be added to waters with low sufficient natural
similar removal ef-ficiency. Chemical coagulants have various disad- addition alkalinity to react with the acidic metallic coagulants and
vantages such as it could affects the environment by their high, and toxic produce a good floc. It mostly provided in the form of hydroxide
generation of sludge. Additionally, they could affect the users health ion by the addition of hydrated ime in the form of Ca(OH)2, or
because of the containing of the consumed water by the chemical re- carbonate ion in the form of soda ash, Na2CO3.
pH adjustment Acids such as sulfuric and phosphoric acids, and bases such as
siduals that causes neurodegenerative disease [105]. Neverthe-less, the lime, sodium hydroxide, and soda ash were applied to adjust the
natural coagulants could have some drawbacks such as the effect of the pH range acquired for coagulation process.
seasons, and the storage duration, which in follow affect the natural Particulate Addition of bentonite clays and activated silica (sodium silicate
coagulants production, and the continuous supply of the coagulants. addition treated with sulfuric acid or alum) is very helpful coagulating low
turbidity waters which leads to increase the particulate
Additionally, other disadvantages of the natural coagulants are the
concentrations to fast the coagulation process. They work as
release of the organic content into the treated effluents, which in turn weighing agents that produce denser and better settling floc.
increase the COD, TOC, and BOD concentrations [106]. However, in Polymers Lately, organic polymers replaced the activated silica as a
contrast to the drawbacks of the chemical coagulants, increasing the coagulant aid, which it was characterized by its application with
organic content upon the natural coagulants appli-cation, which could be much lower concentrations, and easy to apply. Polymers help
producing stronger and faster settling flocs with low metallicsalt
reduced by performing some extraction and purification processes as acid dosage.
and alkali extraction [102].
In addition to the environmental eco-friendly properties, they are
character-ized by their low costs in contrast to the chemical coagulants. coagu-lant dose and the coagulation process efficiency itself. For
Reports stated that, raw materials costs differ in terms of the type of instance, the amount of colloidal particles dispersed in the polluted so-
coagulants, the processing method, and the prices according to the lution determines the coagulant dose needed to remove these suspended
geographical areas [107]. For instance, comprehensive survey was per- particles of the solution [110]. It was stated that diluted colloidal systems
formed of the costing analysis of some natural coagulants such as; Mor- lead to a very slow coagulation rate due to the colloids’ small number
inga seed contains 40% by oil weight and its press cake remain after oil occur in the solution, and in the following, no enough contact between
extraction still contains the active coagulant. Moreover, in the Malawi the suspended particles is available. Therefore, under this condition,
African country, the residue of the press cake could be obtained at zero increasing particulate matter concentration by adding an aid or settled
net cost as oil extraction by-product. In 1993, the moringa seed price was sludge recycling would improve the coagulation rate. Large coagulant
MK. dosage application would dilute the colloidal suspension that results in
75 per 1000 m3 water treated (MK 10.07 ¼ £1 sterling in March 1993) colloids destabilization greater chance.
compared to the cost of alum and soda ash which is MK 501 per 1000 m3
water treated [108]. On the other hand, other countries such as Malaysia, 8.1.1. pH
the cultivation cost for producing kg (3400 seeds) of M. oleifera is pH is the process of measuring Hþand OHions concentration in the
approximately US $ 2 which is double the cost of alum at US $ 1 per kg, solu-tion, and these ions preset in the potential-determining layer that
and in addition 1 kg seeds reportedly costs about US $ 27 [109]. could cause particle charge to be more positive or less negative at pH
values below the iso-electric point. At high pH values above the iso-
7. Coagulation aids electric point, the reverse effect occurs where the charges of particles
became less positive or more negative. The isoelectric point is the value
Coagulation aids were applied to obtain the optimum conditions that of pH at which the charge is nearly neutralized. Aluminum hydroxide
give high coagulation and flocculation performance (see Table 7). The isoelectric point is around pH 8, and it various with the solution ionic
aim of the coagulant aids was to get faster floc formation, produce denser strength but is normally in the range from 7:9. For more explana-tion, the
and stronger flocs, decrease the dose of coagulant, broaden the influen- colloidal dispersion solubility is affected by pH value, where aluminum
tial pH band, and enhance the turbidity removal and other impurities. salt Al (OH)3 is amphoteric in nature and is soluble at high and low pH.
Coagulant aids include four typical types that were shown in Table 8. Higher adsorption rate occurs in the range of minimum solubility pH; for
instance, Alu-minum sulfate optimum pH range was reported from 4.0 to
8. Factors affecting the coagulation process 7.0, Ferrous sulfate 8.5, Ferric chloride from 3.5 to 6.5 and above 8.5,
whereas Ferric sulfate pH range from 3.5 to 7.0 and above 9.0. At the
Different factors were stated to influence the coagulation process, optimum pH, positively charged aluminum hydroxide neutralizes the
which can be discussed as follow. negative charge of pollutants suspended in the solution charged and
produces colloidal particles, resulting in zero zeta potential [111].
Whereas, in the state of polymers, their behavior and effective-ness in
8.1. Colloid concentration
coagulation is particularly important due to the interaction between the
charge on the electrolyte, and pH.
The concentration of colloidal has a significant effect on the required
8.2. Temperature
Table 7
RSM, ANN, and ANFIS models’ prediction abilities are compared using statistical
The temperature has an important effect on the coagulation process
indices [99].
by metallic salts [112]. It was stated that the temperature effect is more
Statistical Sugarcane Bagasse Peanut Hulls pro-nounced in the state of using alum and, therefore, the recommen-
parameters
RSM ANN ANFIS RSM ANN ANFIS dation to apply iron salts at low water temperatures operations [65].
R 0.9794 0.9496 0.9999 0.9501 0.9312 0.9999 Another option is adding bentonite clay as a coagulation aid, where its
R2 0.9591 0.9018 0.9999 0.9028 0.8671 0.9998 negative charge enables the co-agulation process to be proceeded as a
MSE 8.7231 23.1759 0.0071 16.9182 29.4800 0.0339 result of the neutralization process of charge rather than by sweep
RMSE 2.9535 4.8141 0.0840 4.1132 5.4296 0.1842 coagulation. In general, it can be stated that at a higher temperature,
MAE 1.9614 2.9175 0.0335 3.1501 4.6695 0.0721
higher coagulation performance was reported, and this was attributed to

14
R.M. El-taweel et al.
increasing temperature, increase the molecules velocity and hence in-
crease the kinetic energy. Additionally, increasing the temperature in-
crease the chemical reactions; in addition to that, increase temperature
decrease the time of floc formation and decrease the water viscosity.
8.3. Coagulant dosage
The dosage of aluminum and iron coagulants has an impact on the
coagula-tion process as measured by the extent of removing particles that
cause water turbidity. It was reported that the relationship between
coagulant dosage and the coagulation process had been divided into four
zones that start from the low-dosage zone and increasing the dose
gradually to higher doses will be ap-plied in four zones [66,113]. The
four zones are defined as follows:
Zone 1; in which coagulant found with insufficient amount for the
colloids’ destabilization,
Zone 2; ocuurs when coagulants were added with a Sufficient amount
to allow the occurring of the destabilization process,
Zone 3; Excess concentration of coagulants can bring about charge
reversal and particles destabilization, and.
Zone 4; The over saturation with metal hydroxide precipitate that
entraps the colloidal particles and produces very effective sweep coag-
ulation. In general, it was stated that the dosage of coagulant depends on
the colloidal particle concentration and pH.
8.4. Cations and anions in the solution
Using alum and iron as coagulant agents were considered one of the
most important factors that affect the occurrence of colloids charge
restabilization and reversal. However, the presence of a high concen-
tration of ions as silicate, sulfate, and phosphate suppressed or eliminated
this behavior. For instance, it was reported that increasing SO2 sulfate
concentration from 10 to 14 mg/l was effective in preventing restabili-
zation. Using alum in the coagulation process af-fords various types of
positively charged aluminum hydroxyoxides that possesses its lowest
charge and solubility at its isoelectric point that locates in pH range of 7:9
[114]. In consequence, by increasing the dose of alum through this pH
range, sweep coagulation occurs because of aluminum hydroxide pre-
cipitate formation. Hence, alum higher dose tend to increase the alum
species positive charge that will be adsorbed on the interface of particles
that leads to charge reversal and the restabilization of the colloidal
particles. Similar concepts and conclusions are applicable to the process
of iron coagulants. Whereas, the divalent cations presence in the solution,
as Mgþ, Ca2þ in raw water, is commonly considered not only helpful in
the clay particles colloidal negatively charged coagulation by anionic
polymers but also to it is necessary.
8.5. Colloid affinity to water
Hydrophilic colloids, "water-loving molecules," are very stable due to
their hydration shell; therefore, chemicals cannot readily replace the
sorbed water molecules, and, as a result, the molecules are difficult to
coagulate and be re-moved from suspension. Briefly, it can be said that
hydrophilic dispersions’ sta-bility depends more on their “love” for water
than on their electrostatic charge.
For instance, it was found that suspensions that contain such particles
require 10:20 times excess coagulant dose than the normal that have
been applied to destabilize hydrophobic particles [115]. The materials
that produce colors on the surface of the water are a typical example for
hydrophilic molecules, whereas metal oxides that were stated easy to
coagulate and destabilize are an exam-ple for hydrophobic. Even though
the colloidal particles bulk of turbid water mixture in usual exhibit
hydrophobic–hydrophilic properties that result in sus-pensions and make
it intermediate in the degree of their difficulty to coagulate.
15
Current Research in Green and Sustainable Chemistry 6 (2023) 100358
8.6. Zeta potential
The zeta potential showed the colloidal particles’ net charge, and as a
re-sult, the zeta potential higher value leads to greater repulsive power
magnitude between the particles and in following the colloidal system,
became more sta-ble. The zeta potential magnitude is determined from
particle mobility elec-trophoretic measurement in an electric field.
9. Modelling and optimization approaches
9.1. Response surface methodology (RSM)
RSM is a statistical and mathematical approach to explore the rela-
tionship between several independent variables called factors and one or
more depen-dent variables called responses. RSM is used to build models
by setting up a series of experiment runs and fitting empirical models to
data obtained under the chosen design [116]. The steps of applying RSM
are as follows: (1) choosing the independent variables that have major
effects on the process or the system (screening design); (2) choosing the
experimental design; (3) fitting the exper-imental data to a polynomial
function; (4) evaluating the fitness of the model; (5) finding the optimum
values of the variables [117]. The experimental design identifies the
model that the experimental data should fit; the regression model that is
used to fit the data is given by Ref. [12].
Where Y is the predicted response,xi and xj are the input variables, k is the
number of variables, β0 is the constant term, βi is the linear coefficient, βij
is the interaction coefficient, βii is the quadratic term coefficient, and ε is
the residual related to the experiments. The two-level factorial design is
used to evaluate the first-order effects β0 and βi, a center point in the two-
level factorial can be used to estimate the curvature, which are the terms
that describe the interactions between the input variables (βij). The
polynomial function must contain the quadratic term to evaluate the
maximum and the minimum points of the polynomial, so the three-factor
levels, such as Box-Behnken Design (BBD), Doehlert, three-level factorial,
and central composite design are used to evalu-ate βii [12]. The BBD was
implemented to optimize different problems. The merit of using BBD that
it optimizes the experiments with the least number of experiments [118].
Different applications was optimized by BBD such as op-timizing mi-
crowave hydrodistillation of dried patchouli leaves, and optimizing the
transesterification Process using Microwave with CaO Catalyst [119,
120]. Additionally, the microwave-assisted extraction of natural dye
from Swietenia mahagony was optimized by BBD and CCD, and the CCD
had a better results than BBD [121]. The degradation of cetirizine
dihydrochloride (C–HCl) by syn-thesized Zinc vanadate flower (ZVF) was
optimized by CCD [122] (see Fig. 11).
The central composite design (CCD) is commonly used for optimizing
the coagulation process applied in wastewater treatment. CCD is a
combination of three distinct sets of experimental runs; the first set is a
two-level factorial design implementation, the second set is the center
point, and the third set is the star points [116]. In the factorial design, the
minimum level value is coded as (1), and the maximum level value is
coded as (þ1). The second experimental set is the center point, with a
coded value (0). The third experimental set is the star points, they are
allocated outside the factorial space (which is the best prediction inside
it), and they are used to get a good estimation for quadratic terms.
However, they should be in the range of operability, and their coded
values are represented as (α) and (þα) [123]. Fig. 12 shows a scheme
for the central composite design in the case of three variables, where the
red points are from the factorial design (þ1, 1), the yellow point is the
center point, and the coaxial points are the star points (α, þα). The
number of the experimental runs is evaluated as given [124]:
R.M. El-taweel et al.
Fig. 11. A schematic illustration of the mechanisms at act in the process of natural coagulation [76]. Copyright 2022,MDPI.
N ¼ 2n þ 2n þ nc.
Where n is the number of the independent variables, 2n is the number of
the factorial points, 2n is the number of the star or axial points, and nc is
the number of the center points (they are usually six points). The pre-
vious work for the coagulation process is summarized in Table 9.
9.2. Artificial neural network (ANN)
Artificial neural network (ANN) is a mathematical model based on the
hu-man brain actions [134]. ANN is a machine learning technique, and it
is consid-ered as a black box model because no information about the
physical parameters is needed [135]. ANN has many types depending on
Current Research in Green and Sustainable Chemistry 6 (2023) 100358
the architecture; the most commonly used ANN is a backpropagation
(30) (BP) feedforward neural network, and it is known as multi-layer per-
ceptron (MLP) [136]. MLP consists of an input layer, output layer, and
one or more hidden layers, as shown in Fig. 13. Each layer consists of a
certain number of neurons; the number of neurons in the input and
output layer is the number of input and output variables, respec-tively.
The values of neurons for the hidden and output layer depend on the
weight evaluated during the training stage. A threshold signal is
weighted and added to each neuron in the hidden and output layers
[137].
Constructing ANN models consists of three stages training, validation,
and test-ing. Therefore, the data set is split into three classes: training,
validation, and testing. Most of the data is in the training data set, and it
is usually 70–80% of the data. The remaining data is divided between the
16
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Where xmin, xmax are the minimum and the maximum value of the
dataset, xnorm is the normalized value of xi, and xi is the real value.
Recently, many researchers used ANN to model the coagulation process,
as shown in Table 10.

9.3. Comparative study between RSM and ANN

Many researchers have recently implemented both ANN and RSM to

Fig. 12. A scheme of central composite design.
validation and the testing data sets. The training stage is the first step of
constructing ANN, and it is a learning process where the relationship
between the input and output is built. The weights related to each neuron
are adjusted at each epoch during the train-ing stage until the stopping
criteria are satisfied. The stopping criteria could be minimum error value,
the number of epochs, or iteration and validation checks. After the
training stage, the validation dataset is utilized to check the prediction
ability of the ANN model. Applying many validation checks helps to
make sure not to fall in the local minimum [136].
Before the training stage, the normalization process for data gua-
rantees that each input contributes equally to the output prediction. If the
input parame-ters are not normalized, the effect of numerically low range
parameters will be insignificant compared to wide range parameters. The
input and output values are usually normalized between 0 and 1 in MLP
ANN models. The input and.
model the coagulation process. The two models were compared accord-
ing to the mean square error (MSE) or the R-square value (R2). For
coagulation, a comparison is implemented as shown in Table 11, and the
ANN model shows better perfor-mance than the RSM model. The RSM of
CCD, one of the most popular ways of designing experiments employed in
the analysis of the process of optimization, served as the foundation for
the optimization strategy that was used. RSM is a technique that com-
bines statistical and mathematical methods and can be used to provide a
thorough knowledge with a minimal amount of experimental data. For
the purpose of adsorption process optimization, the impact of four factors
(starting dye concentration, sorbent dosage, temperature, and pH) was
inves-tigated. A sophisticated tool that closely mimics the operation of
the human brain is called an artificial neural network (ANN), and it has
been widely used to predict the variables affecting adsorption processes.
Input, hidden, and out-put layers are the typical components of ANN
topologies. A three-layered ANN structure is used in this study, with an
input layer made up of four neurons (starting dye concentration, sorbent
dosage, temperature, and pH), a hidden layer made up of ten neurons,
and an output layer made up of one neuron. Each bio-sorbent was given
its own pair of ANN structures. ANN models were created with the aid of
MATLAB (MathWorks Inc., USA). An ANN model was Using the experi-
mental data, the back-propagation (Marquardt-Levenberg al-gorithm)
technique was taught. The transfer function (log-sigmoid) was used to
extract all the data from the hidden layer to the output layer [99].
9.4. Metaheuristic algorithms for optimization

Nearly all the design problems in nature can be considered optimi-

zation problems. Nowadays, the classical optimization algorithms based
on the math-ematical principle cannot provide satisfactory results in a

Table 9
RSM previous work for coagulation process.
Type of coagulants and wastewater Inputs Output No. of Software Model Ref.
runs

Coagulation Alum and poly aluminum chloride combined COD. Coagulant dosage. pH. COD. 32 Design Expert Quadratic [125]
with a cationic polyacrylamide to treat paper- Flocculant dosage. Turbidity.
recycling wastewater Sludge volume index
(SVI).
polyacrylamide (PAM) as coagulant Initial heavy metals concentration. pH. TDS. TOC. 35 A statistical Quadratic [126]
polyaluminum chloride (PAC) as flocculant to HMCAs dosage. Flocculant dosage. software DPS
treat the coal gasification brine Coagulant dosage. v7.05
Alum-based coagulant (Polyaluminium Coagulant dose. pH. Flocculant Turbidity removal. 20 Design Expert Quadratic [127]
Chloride) to remove natural organic matter dose. TOC. removal UV254
from drinking water treatment plants removal.
Fenton process after coagulation by using H2O2 concentration. Fe(2þ) Color removal. TOC 20 Quadratic [128]
FeCl3 as chemical coagulant to treat swine concentration. time. removal.
wastewater.
Colloidal particles removal from paint MMC dosge. Settling time. Process The TDSP removal. 20 Design Expert Quadratic [129]
wastewater using modified Aguleri temperature.
montmorillonite clay
Coagulation-flocculation of turbid water using Coagulant dosage. Initial pH. Initial Turbidity removal 20 Design Expert Quadratic [130]
graphene oxide turbidity. efficiency
Antimony (Sb) in water Removal by Initial (Sb(III,V) concentration. Sb(III) removal 17 Design Expert Quadratic [131]
Coagulation Flocculation-Sedimentation Ferric chloride (FC) dose. pH. efficiency. Sb(V)
Process using ferric chloride (FC) removal efficiency.
The coagulation/flocculation process using The bio coagulant dosage. Initial Turbidity removal. 13 Minitab17 Quadratic [132]
cactus as bio coagulant to treat sewage pH. Removal efficiency of
wastewater from plants. COD.
Rice starch is used as a natural coagulant for The dosage of rice starch. pH. The turbidity 12 Design Expert Quadratic [133]
drinking water treatment. Settling time. reduction.

17
R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Fig. 13. The ANN structure. output data can be normalized according to Ref. [138].

Table 10
The ANN previous work for the coagulation process.
Type of coagulants and Input output Normalization No. of Data set No. of MSE R Ref.
wastewater range hidden epochs
layers
neurons

Coagulation Alyssum mucilage as pH. Coagulant dosage. The 80% 1000 0.1 0.9981 [139]
natural coagulant to Contact time. percentage of training
treat the synthesized COD removal. 10%
bilge water testing
10%
validation
poly aluminum chloride Voltage. H2O2 The 0.1 to 0.9 9 70% .0033 0.994 [140]
was used on the concentration. pH. percentage of training
Chemical coagulation- Electrode distance. COD removal. 15%
electro fenton process to Reaction time. testing
treat Dairy wastewater 15%
validation
Picralima nitida extract pH. PNE dosage. Time of The 1 to 1 3 70% 9 .0403 0.999 [141]
(PNE) as a bio-coagulant settling. percentage of training
in municipal solid waste COD removal. 15%
leachate testing
15%
validation
Novel Luffa cylindrica Dosage. pH. Stirring The 10 70% 11 .0000143 0.999 [142]
seed as coagulant to time. percentage of training
treat dye-polluted COD removal. 15%
wastewater testing
15%
validation
Ipomoea batatas leaves Initial turbidity. The turbidity 5 for two 70% 0.0287 0.9997 [77]
as natural coagulant to Coagulant dosage. Rapid removal. hidden training
treat industrial mixing time. Rapid layers 15%
wastewater mixing speed. Slow testing
mixing time. Slow 15%
mixing speed. validation
Modified Aguleri Modified The total 1 to 1 70% 6 [129]
montmorillonite clay as montmorillonite clay dissolved and training
coagulant to treat paint dosage. Time. suspended 15%
wastewater Temperature. particles testing
removal. 15%
validation

reasonable period for complex design problems. Developing new opti-
mization techniques with high efficiency, good accuracy, and improved
speed rate in dealing with complex optimization problems has been great
interest. Researchers developed new al-gorithms for solving various
optimization problems called metaheuristics [146]. The metaheuristics
use some higher-level approaches to implement a searching process that
has abilities to avoid the local optimum result and find the global opti-
mum [147].

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R.M. El-taweel et al. Current Research in Green and Sustainable Chemistry 6 (2023) 100358

Table 11
Comparison between the ANN and RSM modelling for coagulation process.
Type of coagulants and Inputs Output ANN R2 RSM R2 Performance Ref.
wastewater

Coagulation The removal of colloidal MMC dosge. Settling time. The TDSP removal. 0.9504 0.9403 The ANN model [129]
particles using modified Process temperature. predictions were
Aguleri montmorillonite clay slightly better than
from paint wastewater RSM model predictions
Bio-coagulation-flocculation pH. PNE dosage. Time of The percentage of COD 0.9982 0.9957 The ANN model [141]
(BCF) of municipal solid waste settling. removal predictions were better
leachate using Picralima nitida than RSM model
extract predictions
Pollutants removals and energy pH. Current density. Time. The COD removal 0.999 0.997 The ANN model [143]
consumption in efficiency. The TDS removal 0.988 0.889 predictions were better
electrochemical cell for efficiency. The Turbidity 0.976 0.755 than RSM model
pulping processes wastewater removal. Energy 0.995 0.995 predictions
treatment consumption.
The decolouration of dye from Moringa oleifera dose. The decolouration 0.999999 0.86 The ANN model [144]
local ‘tie and dye’ industrial Agitation time. pH. percentage. predictions were much
effluent using Moringa oleifera Agitation speed. better than RSM model
seed predictions
The turbidity removal from Dosage. Time. Temperature. The turbidity removal 0.9999 0.9997 Both ANN and RSM [145]
produced water using efficiency. models had a good
Tympanotonos fuscatus as prediction
coagulant
Ipomoea batat asleaves extract Initial turbidity. Coagulant The turbidity removal 0.9994 0.9002 The ANN model was [77]
as a green and novel coagulant dosage. Rapid mixing time. efficiency. better than RSM
for treating turbid water. Rapid mixing speed. Slow
mixing time. Slow mixing
speed.
Novel Luffa cylindrica seed Dosage. pH. Stirring time. color/total suspended 0.9999 for 0.9886 for The ANN model was [142]
extracts as coagulant for dye- particle(CTSP) removal CTSP 0.9999 CTSP better than RSM.
polluted wastewater. chemical oxygen demand for COD 0.9921 for
(COD) removal COD
Alyssum mucilage as a natural pH. Coagulant dosage. The COD removal The ANN had high [142]
coagulant for the treatment of Contact time. accuracy in predicting
synthesized bilge water COD removal efficiency
with R2 values 0.99.

9.4.1. Genetic algorithm
Genetic algorithm (GA) provides solutions for constrained and un-
constrained optimizations problems. GA is biologically inspired that in-
cludes some genetic terminologies as follows. The chromosome encodes
the optimization solution, and it is usually represented in binary. Selec-
tion is a stage where individuals are chosen to generate a new generation,
crossover and mutation both are oper-ators applied to a pair of parents
when they are reproducing a new generation [115]. The algorithm
randomly selects individuals from the current population to be parents
and uses them to produce children for the next generation. Over
consecutive generations, the population approaches the optimal solution
[148].
9.4.2. Genetic algorithm applications
GA is used to solve dynamic problems containing large numbers of
discrete or continuous variables, and its space is complex. GA provides
fast and good results for the objective function that could be a function of
several variables [149]. The wastewater treatment applications that use
GA are mentioned below: The coagulation process for the printed circuit
board manufacturing wastewater was optimized. The multiple regression
model was generated for the sludge level and the cu removal. Then, the
GA was used to optimize the regression models. The efficiency of cu
removal and sludge level was 90% and 97% respectively.
[150].
Optimization techniques are applied to the models to find the best
optimum solution. The RSM model was usually optimized using nu-
merical optimiza-tion techniques using RSM software, such as Design
Expert Software. Some researchers applied metaheuristic algorithms,
usually GA, to the RSM model. The ANN model was optimized by opti-
mizing the network's weights, imple-mented using metaheuristic algo-
rithms. Combining metaheuristic algorithms, GA with the ANN, usually
had more accurate predicting values and better optimum solutions than
RSM. Recently, many researchers implemented differ-ent optimization
techniques, and they compared the results and validated the results
experimentally.
Table 12 summarizes the recent previous work results showing which
optimization technique was better. The ANN-GA was more accurate in
predicting the best solution than RSM.
10. Conclusion
Coagulation is a technique for successfully removing colors from
textile-polluted wastewater. Coagulation process considers the backbone
of the wastew-ater treatment plants technology, where it is considered as
the first process re-sponsible for organics removal from polluted waste-
water. In the coagulation process, most of suspended particles and solids
carries negative charges that coagulate by the addition of some co-
agulants and form flocs that precipitate by the effect of gravity or the
addition of some coagulant aids. Many synthetic, and natural coagulants
were stated as an effective applied materials in the co-agulation process.
Natural coagulants were identified from decades even before the dis-
covery of chemical coagulants. However, chemical coagulants gained a
lot of popularity in the last period, various disadvantages such as their
high cost, and generation of toxic chemicals was observed. This led to the
transi-tion again from the chemical coagulants to the natural coagulants
that, they characterize by their low prices, and environmentally eco-
friendly. Additionally, there are several parameters that affect the
coagulation process such as; pH, dose, pollutant concentration, and
agitation time, zeta potential and these fac-tors should be optimized.
Many optimization models were found effective where the effect of fac-
tors interaction effect on the coagulation process were stated. Addition-
ally, a comparative study between RSM and ANN based on the results of
the recent previous work is implemented. RSM and ANN were commonly
used in the coagulation process. The ANN model shows a better

19
R.M. El-taweel et al.
Table 12
Comparison between the optimization techniques used in coagulation and adsorption processes.
Type of coagulants and wastewater
Coagulation Colloidal particles removal from paint wastewater via coagulation
method using modified Aguleri montmorillonite clay
The turbidity removal from produced water using Tympanotonos
fuscatus as coagulant
The decolouration of dye from local ‘tie and dye’ industrial effluent
using Moringa oleifera seed
Chemical coagulation/precipitation process in the treatment of
water contaminated with humic acid and processed kaolin.
Ipomoea batat asleaves extract as a green and novel coagulating
and flocculating agent for treating turbid water.
performance than RSM. Different optimization techniques were used to
find the optimum solution and validated experimentally, so this paper
summarizes the different techniques and shows which technique was
better. The ANN-GA provided an accurate predicted optimum solution.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgement
This paper is based upon work supported by the Egyptian Academy of
Sci-ence, Research, and Technology (ASRT), Project ID: Call no. 2/2019/
ASRT- Nexus # 4607.
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