Journal of Water Process Engineering 42 (2021) 102096

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Journal of Water Process Engineering

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

Revolutionary technique for sustainable plant-based green coagulants in

industrial wastewater treatment—A review
Amina Adedoja Owodunni, Suzylawati Ismail *
School of Chemical Engineering, Universiti Sains Malaysia, Engineering Campus, 14300, Nibong Tebal, Penang, Malaysia

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

Keywords: Chemical coagulants have been extensively used in wastewater treatment from industrial processes due to their
Coagulation removal efficiencies. Notwithstanding, recent studies have reported concerns over the existence of lingering or
Natural coagulant incurable diseases, resulting from residues of metals from these non-degradable chemical coagulants which
Wastewater treatment
remain in the water even after treatment. The sludge produced from the treatment has also been affirmed to be
Industrial effluent
hazardous and non-biodegradable, causing harm to the environment. The potential application of plant-based
coagulants as suitable alternatives to chemical coagulants due to their biodegradability, economical, non-
toxic, and lower sludge volume, and treatment cost; is being studied in industrial wastewater treatment. Pre­
sented in this review is the state of heart of revolutionary technique for green coagulant preparation, their
properties, and application in wastewater treatment. Highlighted is the current development on improving and
purification techniques of the coagulants, and probable use of dual or combine coagulants. The review also
critically identifies notable research gaps based on the current limitations in previous research to valorizing
potential applications.

1. Introduction Globally, the expansion of most industries has occurred due to

Water is one of the foremost requirements for human survival in this
world, as it is connected to almost all world activities. In 2018, the
United Nations (UN) provided a statistic that 2 billion people live in
countries that encounter high water stress, worsening as an increase in
population and demand for water is experienced [1]. The need for clean
water has been one of the goals that are being fought for all over the
world because inadequate access to clean water has resulted in a lot of
avoidable deaths. The quality of clean water encompasses the color,
turbidity, pH, nutrients, odor, turbidity, coliform count [2].
According to the World Health Organization (WHO), in 2017, about
2 billion people in the world drink water from sources that are likely
polluted with grease, metals, effluents, and faeces. When this polluted
water is disposed into the environment and large water bodies, they
spread infectious water-borne diseases, including; vomiting, diarrhea,
cholera, typhoid fever, dysentery, gastroenteritis, worm infections,
hepatitis virus, and trachoma [3]. It is estimated that polluted water
causes a death rate of about 485 000 each year, thus by 2025, almost half
of the world’s population will be suffering living in water-stressed re­
gions [4].
development and commercialization. It was reported that one of the
negative impacts of these developments in the industries is the height­
ened rate at which pollutants are found in the water bodies caused by
industrial pollution. Water is used for numerous activities and purposes
in all industries and most of the water up and discharged is termed as
industrial wastewater. Every process undergone in the industries makes
use of water, raw materials, energy, and soil; which are converted to
generate the products, other side products, and wastewater [5]. Based
on reports by UNESCO [6], more than 80 % of the wastewater generated
globally is likely to be discharged into the environment without proper
treatment [6]. The uncontrolled discharge of industrial wastewater
which often consists of waste generated (dissolved and fine suspended
solids, organic and inorganic particles, dyes, grease, oil, and other im­
purities) into the environment has increased the turbidity, pH, COD, and
BOD of water. These may lead to both surface and groundwater
contamination which may initiate several other hazards that are detri­
mental to human health [7].
The fertilizer industry uses water extensively as a reactant and is
reported to consume up to 270 m3 of water/ton of product. Water is used
in several activities, including the reaction of water with NO2 to produce

* Corresponding author.
E-mail address: chsuzy@usm.my (S. Ismail).

https://doi.org/10.1016/j.jwpe.2021.102096
Received 20 February 2021; Received in revised form 20 April 2021; Accepted 21 April 2021
Available online 3 May 2021
2214-7144/© 2021 Elsevier Ltd. All rights reserved.
A.A. Owodunni and S. Ismail
nitrogen fertilizers via oxidation of ammonia gas. Besides, the produc­
tion of phosphate fertilizers using the wet process also need some vol­
umes of water as a reactant. Thus, the amount of wastewater created is
high due to the water used and discharged by every process of produc­
tion [8].
Large volumes of wastes containing effluents are generated at regular
intervals by the textile industry. These effluents are highly complex as
they consist of various types of dyes, chemical additives, suspended solid
particles, COD, BOD, and high acidity [9]. It is estimated that more than
10,000 different synthetic dyes and pigments are used in the textile in­
dustry [10]. The colored wastewater discharged consists of a large
quantity of organic load, which if inadequately treated before dis­
charging into the environment, would contribute hugely to the existing
pollution of the surface water and the seawater [5]. Due to the high level
of toxicity that exhibits mutagenic characteristics, it is highly dangerous
to consume water contaminated with these dyes. The dyes present in the
water could cause risk to the human and the environment as they can be
potentially mutagenic, allergic, toxic, and carcinogenic; and the salts in
the wastewater could lead to soil infertility [11]. Its effect on the aquatic
ecosystem cannot be overlooked as it distorts the photosynthesis activity
even in low concentrations because the dye reduces light penetration
through the water surface [12].
On the other hand, the agricultural industry requires a high quality of
water for the processing of produce. An example is the milling process of
palm oil, water is consumed during washing, grinding, and sieving
processes, the untreated effluent (abundant waste) generated is disposed
into the water bodies along with the water used in the processing. Raw
palm oil mill effluent (POME) is brown-colored with high concentrations
of TSS, fat, lubricant, COD, and BOD, thus changing the properties of the
water bodies [13].
Suspended and dissolved solids introduced into the water through
the feeds, chemicals (in form of medication, disinfectants, anti-fouling),
and pathogens constitute the aquaculture effluent (containing solid
wastes, nitrogenous wastes (nitrate and nitrite) and phosphorus, organic
matter) [14,15]. Dauda et al. [15] reported that regardless of the type of
fish cultivated, a high volume of wastes is produced from the aquacul­
ture industry in Japan. One ton of fish was estimated to generate about
0.8 kg of nitrogen (N) and 0.1 kg of phosphorus (P) which equates to the
amount of waste produced by 73 people per day (if each person gener­
ates 11 g of N per day) [15]. Untreated water discharged into the
environment may lead to eutrophication; and thus, a cost-effective
treatment is required because of the large volume of water needed in
fish cultivation. The water is commonly treated using iron chloride
(FeCl3) as a coagulant which increases the meal load in the water.
Recent studies are seeking sustainable and environmentally friendly
treatments that will protect the aquatic habitats from harmful contam­
inants while using the effluent rich in nutrients as soil conditioners to
improve plant growth and yield.
Similarly, in the winery industry, the winemaking process which
includes the cleaning, crushing, and fermentation of grapefruits,
washing the fermentation tanks and other equipment used; generates
huge volumes of wastewater that is characterized by high organic and
nutrient content, acidity, and COD; thus causing contamination of the
environment and waterbody [16]. Wastewater from the food processing,
winery, and fermentation industries are characterized to be nontoxic as
they are less hazardous; however, the water has a high organic matter
content comprising carbohydrate and other sugars, these compounds
could be removed from the water to use in the production of hydrogen or
other useful products [17]. The wastewater generated from the pulp and
paper processing consists of a high percentage of BOD, COD, chlori­
nated, and suspended solids, as they exhaustively require a large volume
of water in their processes [18].
Furthermore, in the iron and steel industry, producing iron from its
ores and processing coke from coal requires a large volume of water for
cooling. It was reported that the steel industry in an Asian country
consumed 25− 60 m3 water/ton of steel, which is believed to generate
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Journal of Water Process Engineering 42 (2021) 102096
wastewater with a high level of contaminant concentrations [8]. This
water may be polluted with contaminants such as phenols, hydraulic
oils, ammonia, particulate solids, cyanide, BOD, COD, metals, and acids.
Likewise in the mining industry, recent studies reported the use of up to
40 m3 of water/ton of ore during processing [19]. The rock-washing and
other mining processes generate wastewater contaminated with rock
particles, metals, acids, oils hydraulic oils, and salts [20].
Other industries identified to generate wastewater includes; petro­
leum (consumes up to 10− 300 m3 water/ton of product), pharmaceu­
tical (generates wastewater with high organic contaminants from the
medicinal compounds, solvent, and other substances) [21], paint and
varnish [22], food and beverage processing [23], cosmetics [24,25],
chemical, leather and metallurgy industries.
Notable techniques for wastewater treatment includes, coagulation
[26], adsorption [27], ion exchange [28], membrane separation [29],
and cavitation [30]. However, this paper will be focusing on the
coagulation-flocculation method of water treatment. The separation of
the suspended particle requires them to cluster and sediment, upon the
addition of coagulants, coagulation effectively destabilizes the fine
particles by neutralizing the electrical repulsion charges between the
colloids [31]. The coagulants aid the clustering and aggregation of the
colloidal particles, they carry opposite charges to the particles and
neutralize them, allowing attraction and clustering to form macroflocs.
Chemical coagulants have been effectively used in coagulation
treatment based on their application for a vast range of wastewater. The
coagulants react in the water and hydrate to produce metal hydrate
precipitates, acting as a sweep-floc mechanism. This mechanism backs
the coagulant to effectively treat very difficult and almost impossible
colloids in water. However, the chemical coagulants have been refer­
enced to be hazardous due to the residual metals precipitates after the
reaction [26]. This has been found to cause health, social, economic, and
environmental challenges as it was discovered to be related to illness,
which includes Alzheimer’s disease, abdominal spasms dementia, in­
testinal constipation [32,33]. The large amount of hazardous sludge
containing metal salts generated after the treatment process may require
additional removal techniques before disposal, thereby increasing the
treatment cost [34].
The process flow diagram of a typical effluent treatment plant is
shown in Fig. 1, the first process involves the accumulation of the
various waste from the different sections of the industry into the
collection tank [35]. The effluent is further moved to the storage tank
where the wastewater is stored before the treatment process takes place,
there are various blower pipes present in this unit to create additional
airflow and proved enhanced aeration efficiency. A paddle mixer is used
for mixing and the mixing parameters may be varied; the cooling tower
is also used to bring down the temperatures [36].
The treatment process continues with the neutralization of pH with
chemicals that reduce the acidity or alkalinity of the medium. The
coagulation process begins with the introduction of coagulants in form
of natural (plant and animal-based) or chemical coagulants (aluminum
sulphate (alum), sodium aluminate, ferric sulphate, lime) [37]. After
coagulation, biological treatment is conducted in the biological oxida­
tion tank, the process involves the degradation of the natural organic
matter (NOM) contaminants in the wastewater by microorganisms. The
microorganisms feed on the NOM in the presence of oxygen and nutri­
ents which is aided by the establishment of an artificial ecosystem [38].
Here, the BOD of the wastewater and other toxic impurities are broken
down and converted to carbon dioxide [39].
The next process is the sedimentation of the particles and separation
of sludge before transferring the residual solution for filtration in the
pressure filter which consists of a filtration layer made up of sand rock,
filters the wet sludge to separate the remnant water from it [40]. The
final process of the effluent treatment is to check the final load of
effluent in the water before discharging it to the environment.
Recently, the inclination has shifted towards research and develop­
ment of natural coagulants for efficient wastewater treatment due to the
A.A. Owodunni and S. Ismail
Fig. 1. Process Flow Diagram of a typical Effluent Treatment Plant (ETP).
numerous limitations in the use of synthetic coagulants discovered.
Numerous review papers have been published on the use of natural
coagulants for water treatment, Gautan and Saini, [41] stated some of
the advantages and disadvantages of natural coagulant in industrial
effluent treatment, but failed to highlight the purification and methods
to improve the coagulant efficiency. Also, Saleem and Bachmaan [42],
provided the historical use, contemporary review of plant-based coag­
ulant chemistry, but didn’t address the recent techniques that are used in
purification and isolation of the active coagulant agents for improved
treatment performance. This review highlights a critical discussion on
the extraction, purification, applications, and evaluation of plant-based
coagulants for an effective coagulation process. Hence, comparative
performance evaluation between green coagulant and chemical co­
agulants in the treatment of industrial wastewater were discussed.
Furthermore, parameter optimization of factors that influence green
coagulant performance in industrial wastewater treatment was
reviewed. Several coagulants used in industrial wastewater treatments
were compared, and their optimum coagulation parameters were
highlighted in this review. Projections and prospects on valorization
green coagulant production and application were identified.
2. Coagulation process
The coagulation-flocculation process is an indispensable factor in
water treatment. It is the most used chemical treatment for both water
and wastewater as it efficiently reduces the turbidity, suspended solids,
oil, organic matter, color, and chemical oxygen demand (COD) in the
water. It requires the introduction of substances that aids the clustering
of finer particles in the water into larger flocs for effective removal from
the water. Coagulation and flocculation are inter-linked. Coagulation is
the agglomeration of suspended colloidal particles in water, it is a
chemical process that involves the neutralization of the negative charge
of the dispersed materials in the wastewater [43]. While flocculation is a
physical process, it is the formation of flocs or flakes from the suspended
colloids in the water. It is majorly conducted by high molecular weight
compounds aiding the aggregation and settling of the flocs formed
during the coagulation process. Thus, coagulation forms the larger flocs
and flocculation causes the flocs to aggregate and settle at the bottom of
the water body. After the coagulation-flocculation process, the treat­
ment process further undergoes filtration and sedimentation processes
to remove the effluent from the water [44].
However, it was also reported that the process might still require
further treatments which include filtration, sedimentation, oxidation,
and physical or chemical disinfection for complete treatment [45]. This
depends on the properties of the fine suspended particles in the water,
they vary in source, compositions, density, sizes, shape. It is important to
have a complete coagulation process as it would affect ensuing pro­
cesses, incomplete coagulation will lead to incomplete flocculation to
3
Journal of Water Process Engineering 42 (2021) 102096
further result in an ineffective sedimentation process. As shown in Fig. 2,
the untreated water undergoes coagulation when the coagulants are
introduced to it, a vigorous mixing process is required to aid the floc
formed to cluster into larger flocs, the swift mixing distributes the
coagulant uniformly through the waterbody; a slower mixing follows to
aid inter-particle bridging of the flocs [46]. The coagulation process
efficiency depends strongly on the coagulant type, mixing rate, and
settling time which determines the quality of the water; the dosage
coagulant has to be optimum and intensely mixed for proper suspension
of the solid particles; other characteristics of the coagulants include its
quality and lifespan which determines the stability during storage [47].
After the coagulation-flocculation process, the water undergoes
sedimentation, the larger solid particles sink by gravitation settling to
the bottom of the vessel, this step is often dependent on the rate of
settling of the particles (flotation or settling time) and time allowed for
sedimentation. The filtration process takes place after the sedimenta­
tion, the sediments (effluents) are separated from the clean water often
by passing them through various filters or membranes. The bulk of the
suspended solids are removed in the top portion of the filter media, the
particles trapped within the filter bed are usually removed by back­
washing the filters [48]. The rapid dual-media filter is the most
commonly used filter type in the conventional wastewater treatment
process, it is composed of sand and anthracite; nevertheless, other
filtration media which is not limited to the mono-media (sand only),
multi-media (sand, anthracite, and garnet) may also be applied in the
filtration process [49]. The solid sludge generate is transferred to the
sludge bed, dried, and prepared for disposal or recycling (in the form of
fertilizers or manures). The clean water is then transferred for further
disinfection which varies according to the intended application for the
water.
The final process is storage, the treated water is often stored before
use, it is however believed that water that contains more nitrogen,
phosphorus, and potassium elements should not be stored for too long as
it aids the production of algae and the growth of other microorganisms
[50].
2.1. Mechanism of coagulation
In removing particles from wastewater, it is inefficient and discour­
aged to remove small particles that are suspended in the water or do not
settle properly, as they might pass through the filters during the filtra­
tion process. Thus, a coagulation process is required to clog the fine
particles together to form larger flocs which will be easier to separate
from the water after settling [51]. The suspended particles averagely
larger than 1.0 μm in the water also contain colloidal particles which are
very small with an extremely large surface area, they are generally
invisible to the eyes but are larger than atoms, with a size ranging from
0.001 to 1.0 μm [52].
A.A. Owodunni and S. Ismail
Fig. 2. Schematic process flow diagram for wastewater treatment.
The coagulant added to the water destabilizes the particles, resulting
in their entrapment to form larger flocs. The four principal mechanisms
for destabilizing the colloids during coagulation include sweep floccu­
lation (particle entrapment); double layer compression; charge neural­
ization; and, polymer adsorption and interparticle bridging [31,54]. The
action of the coagulation polymers is based on either destabilization or
interparticle bridging. The mechanisms could be studied and identified
through Fourier transform infrared spectroscopy (FT-IR) and scanning
electron microscopy (SEM) analyses [55]. A schematic diagram of
coagulation mechanisms is shown in Fig. 3.
The sweep flocculation is involved with the coagulant trapping the
suspended particles and causing them to settle at the bottom. In the work
of Okuda et al. [56], a coagulant solution extracted from moringa seed
using the salt solution (1 M NaCl) was used in the coagulation of syn­
thetic (kaolin) water. The Ca2+ and other bivalent cations seemed to
have connected with the molecule of the active coagulation component
in the moringa extracted solution to form a net-like structure. Based on
the formed net-like structure, it was concluded that the sweep floccu­
lation i.e. the enmeshment of the kaolin mechanism was predominantly
operated on as it was responsible for the coagulation [56,57].
While double-layer compression is the process that aids the fine
particles to overcome the force of repulsion and cluster together. When
induced by the presence of high concentrations of salt compounds
(electrolytes) in the colloidal suspension, the added ions (divalent and
trivalent ions) carrying opposite charges penetrate the diffused double
layer that surrounds the colloids causing it to increase in density and
smaller volume [58,59]. This leads to generating repulsive electrostatic
reactions that are affected by attractive van der Waals forces, resulting
in steeper electrostatic potential gradients [60]. As the net repulsive
energy decreases and reaches elimination, the particles approach each
other and cluster.
The charge neutralization mechanism is cited to involve the desta­
bilization of the suspended particles using opposite charged electric ions
to attract them, the particle charges neutralize, and the electrostatic
repulsion lessens or reaches complete elimination. Flocculation then
occurs, as the suspended colloids cluster to form larger flocs [61]. This
mechanism is observed to be involved when aloe vera gel was used as a
coagulant in treating tannery wastewater. The presence of the gal­
acturonic acid ions ionizes to produce H+ ions which aids charge
neutralization of the anionic colloidal particles [62,63]. This mechanism
was also reported for the active coagulation agent of moringa oleifera
seed, the protein was found to have high contents of glutamine, arginine,
with positively charged amino acids of nearly low molecular weight
[64].
Furthermore, the polymer adsorption and bridging mechanism occur
when the long-chained coagulant polymers destabilize the colloidal
particles as they form bridges that extend between them. The polymer
molecules attach to the surface of multiple particles by adsorption,
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Journal of Water Process Engineering 42 (2021) 102096
producing strong clusters of macro flocs as the colloidal particles are tied
together via bridging [54]. The adsorption and bridging mechanism
were hypothesized to be the primary coagulation mechanism for cactus
(Opuntia), as well as Cassia obtusifolia seed gum which is a non-ionic
natural polymer and serves as an effective bridging coagulant in acidic
solution [55]. For cactus, notable literature reported the possibility of
carbohydrate, primarily the galacturonic acid, which is a major con­
stituent of pectin, existing primarily in polymeric form provides the
bridge for the adsorption of the colloidal particles [65,66]. Nirmali seed
extracts were also reported to be anionic polyelectrolytes that use the
interparticle bridging mechanism to destabilize the particles in the
water [67]. The colloidal particles are attached to the polymerlike ma­
terial (mucilage) from the cactus. The adsorption may occur through
hydrogen or dipole interactions, the natural electrolytes (divalent cat­
ions) from the cactus pads are believed to be highly crucial to coagu­
lation involving anionic colloidal particles, as they aid the coagulation
process [59,68].
The coagulation mechanisms explain the reactions between the
colloidal particles and the coagulant added, resulting in the destabili­
zation and neutralization of the ionic charges of the particles, and they
are reported to be dependent on coagulation dosage [69]. During the
coagulation process, a long-chain polymer or polyelectrolyte imported
as the coagulant possessed an opposite charge to the suspended particles
in the water [53]. The coagulant added is intensely mixed to dissolve
and evenly distribute throughout the water body while promoting par­
ticle collisions. Incomplete coagulation may occur when there is inad­
equate mixing, also, over-mixing (or aggressive mixing) affects
coagulation, which may break the interparticle bridging and lead to
restabilization [31]. The suspended particles begin to aggregate
together immediately the coagulants successfully neutralizes the
charges and flocs are formed. The flocculation process promotes the
clustering of the flocs in the water medium.
After the thorough rapid mixing, a moderate mixing signifies the
beginning of the flocculation process, the reduced surface charge of the
particles, and the increased electrical attraction between them results in
the flocculation [44]. The particle sizes increase as the particles cluster
and aggregate, the suspended particles are now more clearly seen. As the
particles collide and interact together, the larger flocs are formed, they
start to settle at the bottom of the water body in preparation for the
sedimentation process.
Most natural coagulants are reported to function based on the charge
neutralization mechanism, however, the zeta potential analysis and
electron microscopy images of the flocs produced could give more in­
formation on the predominant mechanism exhibited by the coagulant
[70].
A.A. Owodunni and S. Ismail
Fig. 3. Schematic diagram showing a depiction of the coagulation mechanism [53].
3. Classification of coagulants
Coagulants applied in wastewater treatments are classified majorly
into two groups; synthetic coagulants and natural coagulants [71]. They
are introduced into the coagulation system to destabilize the colloidal
particles to enhance their aggregation to form larger flocs. Other types of
coagulants include coagulant aids and enhanced coagulants, they are
applied to enhance the formation of flocs by adding density to the flocs
[72].
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Journal of Water Process Engineering 42 (2021) 102096
3.1. Synthetic coagulants
The most frequently applied chemical inorganic coagulants in water
treatments are iron and aluminium salts, and organic polymers. The iron
or aluminium based coagulants are economical, widely available, and
can be used for a large array of water and wastewater treatments due to
their effectiveness in the removal of most types of solid particles. After
its addition to the water, the chemicals which have high positively-
charged neutralizes the negatively-charged colloids, forming
aluminium or iron precipitates [43,73]. Their efficiency in coagulation
A.A. Owodunni and S. Ismail Journal of Water Process Engineering 42 (2021) 102096

is a result of their capacity to develop polynuclear complexes which
increases the coagulation performance as the ions are effectively
absorbed onto the negative surface of the colloids of the particles [31,
74]. The particles clog together and settle in the process of cleansing the
water. The chemical coagulants that have been broadly used in the in­
dustrial wastewater treatments are not limited to aluminium sulphate
(alum) [75], polyaluminium chloride [76], ferric chloride [77,78],
ferrous sulphate [79], and lime [80].
However, it has been reported that they may alter the pH of water as
they deplete alkalinity, therefore, lime or soda ash is added to maintain
the desired water pH [81]. Other disadvantages and limitations include
high volumes of sludge production, the presence of residual metals in the
sludge [44,82]. The effective application of inorganic coagulants is
greatly dependent on the dosage, an excess of the metals in the effluent
will cause harm to human health, the environment, and the ecosystem.
Because of their corrosive property, the treatment process requires using
corrosion-resistant equipment and apparatus, and the solid effluents to
be disposed of must be treated and discarded in an appropriate method.
The sludge produced after coagulation has been reported to be toxic
and while being generated in large quantities. It was also noted that
aluminium-based synthetic coagulants leave aluminium salt as a res­
idue, which is a neurotoxic product, thus continued exposure to water
containing this residue leads to Alzheimer’s disease [33]. The advan­
tages and disadvantages of notable chemical coagulants have been
highlighted in Table 1.
Organic polymer coagulants (pre-hydrolyzing metallic salts) are
widely used coagulants in water treatment, they are polymeric
coagulants with exceptional characteristics that have been made to be.
Although the coagulants are fitted from the inorganic coagulants, they
are hydrophilic compounds and have the same characteristics as natural
coagulants (environmentally friendly, and non-toxic to the humans and
ecosystem). A limitation these sets of coagulants have is that they are not
effective in all conditions of wastewater treatment, thus, they are often
mixed with inorganic coagulants for effective treatment.
The polymeric coagulants are majorly polymers that have high mo­
lecular weight and are long-chained. They can be applied as the primary
coagulant or used as a coagulant alongside inorganic (metal) coagulants
as it is in the case of negatively-charged polymers. Their basicity is one
of the most significant characteristics of polymeric coagulants [104].
Other advantages over inorganic coagulants include the fact that their
application is required in lesser dosages, they have little effect on pH as
they have lesser alkalinity absorption. A cleaner and lesser volume of
sludge is formed as the coagulants treat the water without producing
additional solids (metal hydroxide precipitate) [105,106]. However,
some of their limitations include its highly expensive cost when
compared with inorganic coagulants; also, the suitable polymer to be
used as to be selected for efficient coagulation process. Few of these
polymeric coagulants (PACl, PICI, PFC, and PFS) are highlighted and
discussed in Table 1. Other synthetic cationic polymers used as chemical
coagulants include aminomethyl polyacrylamide [107], polyalkylene
[108], polyamine [109], and polyethlenimine [110].
Overall, the applications of the chemical coagulants have been
established as they are widely used in wastewater treatment due to their
proven performance, availability, and cost-effectiveness. Their

Table 1
Notable chemical coagulants.
Coagulant Production Advantages Disadvantages Ref

Aluminum Chloride AlCl₃
Aluminum Sulfate (Alum) Al2
(SO4)3⋅18H2O
Aluminum Chlorohydrate (ACH)
Al2(OH)5Cl
Sodium Aluminate Na2Al2O4
Ferric Sulfate Fe2(SO4)3
Ferric Chloride FeCl3
Ferrous Sulfate FeSO4⋅7H2O
Lime Ca(OH)2
Polyaluminum chloride PACl
Polymeric iron chloride (PICI) and
Polyferric chloride (PFC)
Polyferric sulphate (PFS)
Poly-aluminium-silicate-chloride,
Polyferric silicate sulphate,
Polysilicate ferric, and Poly-
aluminium-ferric-silicate-chloride
They consist of aluminium and chlorine
atoms in a 1:3 ratio
Usually obtained by treating minerals
like alum schist, bauxite, and cryolite
with sulfuric acid
Commercially manufactured by reacting
aluminium with hydrochloric acid.
Manufactured by the dissolution of
aluminium hydroxide in a caustic soda
(NaOH) solution.
Produced on a large scale by adding
sulfuric acid and an oxidizing agent (e.g.,
nitric acid or hydrogen peroxide) to a hot
solution of ferrous sulphate.
Produced industrially by a process called
direct chlorination, the reaction of dry
chlorine with scrap iron at 500− 700 ◦ C
Generated as a by-product from the
pickling of steel
Obtained by the reaction of the water on
calcium oxide (hydration)
Created by partially neutralized
aluminium chlorides.
Produced by partially neutralizing ferric
chloride.
Made by partially neutralized ferric
sulphate
These groups of organic polymers are
made by joining aluminium or iron-based
polymeric flocculants with polysilicate.
Substitute to alum More expensive, hazardous, and [83]
corrosive
Commonly used; most effective between Limited pH effective range; adds [84,
pH of 5.5 and 6.5 dissolved aluminium salt residues to 85]
the water
Reduces chemical solids; higher positive Reacts with alum to form a [86,
charge and efficient coagulation (increased precipitate; adds dissolved 87]
basicity); low dosage is required; lower aluminium salt residues to the water
consumption of alkalinity
A small dosage is often required; efficient Expensive; inefficiency in treating [88,
in hard water soft water 89]
pH effectiveness between 4− 6 and 8.8− 9.2 Very caustic; it produces visible rust- [90,
colored stains associated with 91]
chemical spills and leaks; depletes a
lot of alkalinity
Most corrosive, and hazardous
[92,
Least expensive coagulant.
93]
Limited use due to safety
[94,
Not sensitive Depletes alkalinity; very corrosive
95]
pH-dependent; generates large
Very efficient; may not add salts to effluent [96]
volumes of sludge
May exhibit inefficiency in removing
particles with high molar mass and [97,
Less temperature and pH-dependent
highly hydrophobic natural organic 98]
matter (NOM)
When compared with ferric chloride, they
They have not been thoroughly used
are applicable in a wider pH range, lower
as they are still undergoing research [99]
corrosiveness, and lesser residual iron
and development.
concentration
Very similar to PICI and PFC. Lesser
sensitivity to temperature, lower
It is also at the development stage, [31,
corrosiveness, and lesser residual iron
therefore, not widely used. 100]
concentration when compared with ferric
chloride
Studies made on them showed that
wider pH range applications, large floc [101,
the large flocs formed do not settle
formation, and enhancing the bridging 102,
(no sedimentation), thus resulting in
ability of coagulants 103]
high turbidity

6
A.A. Owodunni and S. Ismail
limitations that have been recurrently stated are voluminous sludge
generated as a result of their various side reactions, which further makes
the handling, disposal, or recycling of the sludge difficult [55]. Other
common disadvantages include the residual metal salts left after the
treatment process, especially if over-dosing occurred; the consumption
of alkalinity by the coagulants especially the iron-based coagulants in­
creases the cost of treatment due to the required substances added to
balance the pH [111].
3.2. Natural coagulants
Natural (green) coagulants are commonly used for wastewater
treatment to generate and remove sludge. They have the benefits of
greatly maintain pH as they do not deplete alkalinity. Unlike the
chemical metal-based coagulants, they do not add metals to the effluents
generated, a lower volume of sludge is also formed which reduces the
cost of disposing of the sludge obtained. There are different sources of
organic coagulants, which include the plant, animals, and microorgan­
isms, which has been illustrated in Table 2 [2].
The plant-based coagulants are obtained from the seeds, leaves, bark
of trees, fruit wastes, and other sources. The plant-based coagulants have
been more researched than the other two sources because of their wide
availability. Numerous natural coagulants previously studied include,
moringa seed, jatropha curcas [112], banana peel [113], cassava peel
starch [114], pawpaw [115], watermelon [116], beans [117], okra
[118], nirmali seeds [53]. The preparation process of producing natural
coagulant powder from the seeds is shown in Fig. 4.
Examples of coagulants are sourced from animal bone shell extracts,
the exoskeleton of shellfish extracts, chitin, and chitosan. Chitosan is a
natural high molecular polymer (cellulose-like biopolymer) derived
from the deacetylation of chitin, they are obtained from shells of crabs,
shrimps, lobsters, diatoms, insects, fungi, marine and freshwater
sponges, and mollusks. The potential of chitosan as a natural coagulant
has been researched extensively [122]. It is presumed that this type of
coagulant has very minimal toxicity which makes it less harmful to be
disposed of as residue either along with the sludge or water [96]. Chi­
tosan has been studied in treating wastewater generated in the textile
industry, agricultural industry [123]; food processing [124]; soap and
detergent [23]; paper mill [125], and other industries [126,127]. Chi­
tosan is highly favored as a coagulant because when added to an acidic
solution, it reacts and emits positive charges which interact with the
negative charges of the suspended colloids [128].
Compared to the inorganic coagulant (alum), green coagulants
function better at specific pH conditions, alum could function at all pH
conditions. However, it was found that both types of coagulants needed
an adjustment to their pH before or after the coagulation process, but the
green coagulant has a lower probability of producing water with
extreme pH because pH alteration does not occur during treatment [129,
130]. The advantages of using green coagulants are quite numerous and
are not limited to their positive impact on the environment and the
ecosystem because of their low toxicity levels and high biodegradability
which ensures the safety of human health and aquatic life; they also do
not generate secondary pollution and are environmentally friendly [72].
Table 2
Natural coagulant from different sources.
NATURAL COAGULANT
PLANT-BASED NON-PLANT BASED
• Seed: watermelon, tamarind, bean, moringa oleifera, • Shell: chitosan, chitin,
pawpaw, mustard insects
• Leaves: acorn, hibiscus, oak • Gelatin: animal
• Bark (tannins): acacia, schinopsis, castanea proteins
• Peels: cassava, orange, banana • Alginate: brown
• Pads (mucilage): Cactus, aloe vera, okra seaweed
• Starch: tuber (potato, cassava), grain (wheat, corn,
rice)
7
Journal of Water Process Engineering 42 (2021) 102096
Few green coagulants are used in wastewater treatment and their opti­
mum parameters are given in Table 3. Some of the parameters varied
included pH, turbidity, coagulant dosage, reaction time, and tempera­
ture; to obtain the optimum parameters for treatment.
Other coagulants used in wastewater treatment includes; Psyllium
(Plantago ovata) seed [152]; Okra mucilage [153]; Peanut (Arachis
hypogaea) [154]; soybean (Glycine max) [53]; Cowpea (Vigna unguicu­
late) [155,156]; Banana, papaya, neem leaf powder [157].
Although various studies on using agricultural-based coagulants in
wastewater treatment gave satisfying results, its inefficiency is exhibited
in the treatment of highly turbid wastewater i.e., (>800NTU); it was
noted that the highly turbid water requires treatment with high coag­
ulant doses which invariably increases the biological and chemical load
on water, coupled with over-dosage which may further stunt turbidity
[54]. Also, for its application in the industry, the economical aspect must
be considered by studying the feasibility of designing large-scale treat­
ment plants. During studies using synthetic water,
4. Natural coagulant preparation
During coagulation, the natural coagulants are usually used directly
in powder form or as a stock solution, their methods of preparation vary
based on their sources, and their compositions [42]. As shown in Fig. 4,
the seeds or other plant parts are cleansed to remove contaminants that
would negatively affect the coagulation process; cut, chop, peeled,
soaked (from other sources), dried before grinding or milling. After the
milling process, the powder is then sieved with the desired mesh sizes
and re-blended if necessary [158,159].
Sometimes during preparation oil is extracted from the agricultural
seeds, moringa oleifera seed was reported to have a high oil content of
about 30–40 %, and 35 % for jatropha curcas seeds [160,161]. The oil
present in the material increases the organic matter in the water, hence
an oil-extraction process is required to purify the seed coagulant, the
oil-free cake is then used in the coagulation process or for further pu­
rification [162]. Several studies involving studying the effect of seed oil
extraction on the coagulation process have justified the higher perfor­
mance of oil-free seeds on turbidity removal, improved pH range, and
color removal [163]. Generally, the soxhlet extraction methods are used
in the extraction process with hexane being the most used solvent
including ethanol and acetone. Oil extraction before crude extract
preparation is highly recommended to improve coagulation activities at
lower dosages [164,165].
Results of oil-free Moringa oleifera (Mo) seed extract gave a better
coagulation efficiency of more than 30 % when compared to the oil-
contained extract. In the study done by Garcia-Fayos et al. [164],
soxhlet extraction was observed to give a higher oil extraction yield than
the batch method procedure which was used alongside. Also compared
to the other solvents (acetone and hexane), ethanol oil-free extract
required significantly lower coagulation dosage which results in its high
efficiency [164].
In a study of the removal of dye color from the textile wastewater
using basil seed mucilage by Shamsnejati et al. [144], the basil seeds
were first cleansed of foreign impurities and immersed in water at a
temperature 50 ◦ C containing 0.9 % NaCl solution. The contents were
mixed for 1 h till the seeds completely swelled. A rough plate was used
to scrape the gum layer of the seed surface, and the mucilage was
separated from the seeds with the aid of a 500-micron steel filter. It was
gathered and used as a coagulant for wastewater treatment [144].
Coagulant was produced from Tamarind Indica (TI) seed by washing
the seeds with clean water to rid them of dust and pulp. The cleansed
seeds were further dried in the shade for 24 h before removing the seed
coat by treating it with hydrochloric acid. After drying, the seeds were
ground with a grinding machine to obtain the TI powder, which was
used as the coagulant [145]. Chestnut and acorn seeds coagulant used in
the removal of turbidity were prepared by dissolving the prepared
(ground) powder in distilled water or NaCl to extract the active
A.A. Owodunni and S. Ismail
Fig. 4. Schematic diagram of the process involved in preparing the coagulant powder from the seeds [41,163].
coagulant element, the mixture was stirred for 10 min before filtering
with the aid of a filter paper [166].
In extracting pectin from orange peel to apply as a coagulant in
wastewater treatment, the peel was removed from fresh orange fruit
obtained and the pith was detached from the peel with the aid of a
laboratory knife. The pith was dried at room temperature until all
moisture is evaporated. Four spoons of lemon-sourced citric acid were
added to approximately 227 g of the dried pith, it was left in a position
for 1 h before the addition of 2 cups of water and left in that position for
the next 1 h. The combination was heated for 10 min, after which it was
left to cool and was strained using a muslin cloth. The pectin is the
filtrate extracted from the pith of the orange peel which could be used
directly as a coagulant in the wastewater treatment process [148].
For preparing coagulant from Jatropha curcas seeds, the skin on the
seeds was removed manually before selecting the seeds of good quality.
The kernel obtained was ground using an electric blender to a fine
powder (63–500 μm). In obtaining the active ingredients, the coagulant
was prepared by mixing 5 g of the powder with 100 mL of distilled water
at room temperature for several minutes before filtering the suspension
obtained using a muslin cloth [129].
Similarly, Sesamum indicum seeds were washed with de-ionized
water to remove impurities after separating and confiscating the bad
ones, the samples were dried at room temperature for 2 weeks to ensure
the preservation of the physicochemical characteristics of the seeds. It
was then ground to a particle size of almost 300 μm. In preparing the
coagulant, oil was extracted from the milled sample using n-Hexane. For
the extraction of the coagulant, 10 g of the oil-free sample was dissolved
in 250 mL of salt solution and underwent constant agitation with the aid
of a magnetic stirrer for 1 h and heated up to a temperature of 70 ◦ C.
After the reaction, the mixture was filtered and the filtrate was dried at
room temperature, it was reground and deposited in a sealed vessel for
future application [134].
In the preparation of Mo coagulant, the seed pods that are matured
and dried by natural means to a brown color were collected from the
tree, the pods were opened to extract the seeds from the pods, they
undergo sun-drying while the external shells were also removed.
Matured seeds showing the absence of discoloration and softening were
used. After the sun drying process, the seed kernel was extracted from
the external shell, which was milled using a grinder to achieve the seed
kernel. In the treatment of textile wastewater by Ramesh et al. [145]. Mo
powder was mixed with distilled water and used directly as a coagulant.
4.1. Extraction of coagulation solution
Based on studies, it was discovered that using the powdered seed
directly as a natural coagulant contributes to the sludge volume gener­
ated, as well as lowers the turbidity removal efficiency of the coagulant
[167]. Hence, to remove unwanted organic components that the natural
seed powders contribute to increased organic content in the water,
additional treatments are applied to isolate the active coagulation agents
in the seeds [168].
8
Journal of Water Process Engineering 42 (2021) 102096
Distilled water and saline solution are the commonly used suitable
methods to extract the active coagulant agent. Abidin et al. [129] ach­
ieved a turbidity removal of 99 % using distilled water extracted jatro­
pha curcas seed in treating kaolin synthetic water. The coagulant active
ingredients were extracted by mixing 5 g of the seed powder with
100 mL of distilled water at room temperature for several minutes. The
resulting suspension was filtered through the muslin cloth [129].
Studies have determined that extraction of active coagulation agents
from seed powders using salt solutions was more efficient when
compared to the distilled water extraction. Salt solutions generally
demonstrated better efficiency over distilled water in wastewater
treatment, as detected by Dalvand et al. [169], they act as a poly­
electrolyte during the coagulation The most common salts used to pre­
pare the saline solutions are sodium chloride (NaCl), potassium chloride
(KCl), sodium nitrate (NaNO3), potassium nitrate (KNO3), and ammo­
nium chloride (NH4Cl) [167,170].
In the study of coagulation activity Zygia cauliflora of seed extract by
Domingues et al. [171], the coagulants were extracted from the seed
using distilled water, and saline solutions, which were prepared at 1.0 M
and 5.0 M NaCl concentration. The most efficient extraction solution
was determined to be the coagulant prepared with 1.0 M NaCl, it
showed effectiveness of 30.4 % and 74.5 % removal of color and
turbidity, respectively [171].
ELsayed et al. [172] compared the coagulation performance of active
coagulants from the natural seeds (bean, lima bean, lentil, and fenu­
greek) extracted using different solvents (distilled water, NaCl, and
NaOH). The seeds powder (5 g) were mixed with 50 mL of the solvents
for 1 h at a temperature of 40 ◦ C. The resulting suspension was then
centrifuged with the clear solutions used the coagulant in the water
treatment. Comparing the effects of the different solvents on coagulation
activity, the coagulant extracted with 0.3 M NaCl demonstrated a higher
coagulation efficiency above 75 %. For the coagulants prepared with the
saline solutions, the increase in the concentration of the salts led to
higher extraction of the active coagulation agent, which was believed to
be protein. The coagulation performance continuously increased until a
certain point, this was supported by the increase in the solubility of the
protein in the presence of salt, and its precipitation in an excess salt
solution [172].
Birima et al., [170] demonstrated the higher performance effec­
tiveness of peanut seed coagulant extracted with NaCl (PSS) over the
coagulant extracted with distilled water (PSD). The two coagulants were
used to treat the turbid water at the same dosage of 20 mg/L, the PSS
coagulant effectively removed turbidity by 92 % while the PSD co­
agulants exhibited a lower turbidity removal performance of 31.5 % at
the same dosage [170].
Another study by de Souza et al. [82] involving the extraction of
cactus mucilage textile effluent treatment supported the effectiveness of
NaCl and KCl, over NaNO3 in turbidity removal. The effects of the three
salt solutions on the coagulation activity were studied, NaCl and KCl
achieved maximum turbidity removal of 92 % and 94 %, respectively. It
was noteworthy that NaCl when compared with KCl is more economical,
A.A. Owodunni and S. Ismail Journal of Water Process Engineering 42 (2021) 102096

Table 3
Notable natural coagulants used in treating wastewater from industries with their optimum parameters and results.
Coagulant Form of application Optimum conditions Parameters and maximum Ref.
removal efficiency

Agro-industrial wastewater (palm oil mill effluent)

Cd - 1.0 g/L
Cassia obtusifolia (seed gum) Stock solution pH - 3 TSS - 93.22 % [55]
Settling time - 45 min
COD – 68.31 %
Stock solution (0.1 M HCl and Turbidity – 98.35 %
Chitosan Cd - 400 mg/L
distilled water) TSS – 98.95 %
Color – 96 %
COD – 38.60 %
Turbidity– 88.30 %
TSS – 95.42 % [123]
Moringa oleifera Seed paste Cd - 2000 mg/L
Color – 90.15 %
Oil & grease –
87.05 %
COD – 61.89 %
Zeolite Powder Cd - 1000 mg/L Turbidity – 91.98 %
TSS – 96.82 %
Cd - 2 g/L
pH - 3
Rice starch Starch solution TSS - 84.1 % [131]
settling time - 5 min
slow stirring speed - 10 rpm
pH – 3− 6 TSS - 99 %
Chitosan Solution (1% acetic acid) [132]
Cd– 0.08–8 g/L Residue oil - 99 %
pH – 4− 9 TSS - 99.2 %
Moringa oleifera Press cake (solid) [133]
Cd – 0.5–6 g/L COD - 52.5 %

Aquaculture industry wastewater

Algae removal – 98 %
Chitosan Stock solution (0.1 M HCl) Cd – 30 mg/L [127]
Biomass recovery – 80 %
Cd – 0.4 g/L TDS removal – 82 %
Settling time – 60 min
Sesamum indicum seeds extract Stock solution [134]
pH - 2 COD – 38.60 %
Temperature – 303 K

Concrete plant wastewater

Moringa oleifera + Alum Powder Cd - 20:80 (w/w) Mo and alum Turbidity - <90 % [135]

Domestic
Cd - 600 mg/L Turbidity – 84 %
Oyster mushroom (Pleurotus
Solid Mixing rate – 150 rpm [136]
ostreatus) TSS – 90 %
pH – 6− 8

Kaolin synthetic wastewater

Cd - 120 mg/L
Jatropha curcas Press cake (solid) Turbidity – 99.7 % [129]
pH – 3
Cd - 40 mg/L
Roselle seeds Suspension TSS - 93.13 % [137]
pH - 4

Oil refinery wastewater

COD – 38.60 %
Moringa oleifera Cd – 70 mg/L Turbidity – 63.70 %
TSS – 62.05 %
Stock solution [75]
Mo and alum – 2:1 COD – 50.41 %
Moringa oleifera+ alum Turbidity – 86.14 %
Cd – Alum: 80 mg/L; Mo: 70 mg/L
TSS – 81.52 %

Petroleum industry wastewater

Cd – 1.5 mg/L COD – 95.2 %
Cicer arietinum seed Turbidity – 98.89 %
pH - 7
Oil – 83.8 %
Cd – 2 mg/L COD – 92.18 %
Eggplant seed Filtrated solution Turbidity – 99.42 % [138]
pH - 7
Oil – 81.8 %
Cd – 2 mg/L COD – 93.48 %
Radish seed Turbidity – 98.78 %
pH - 7
Oil – 88.2 %

Raw river water

Cd – 0.1 kg/m3 TSS – 96.03 %
Banana pith Powder COD – 54.3 % [139]
pH - 4
Turbidity – 98.5 %
Watermelon seed Oil-free powder Cd – 0.6 g/L Turbidity – 87.9 % [116]
(continued on next page)

9
A.A. Owodunni and S. Ismail Journal of Water Process Engineering 42 (2021) 102096

Table 3 (continued )
Coagulant Form of application Optimum conditions Parameters and maximum Ref.
removal efficiency

pH – 7.5 Color removal – 84.3 %

Mixing speed – 120 rpm Temperature – 25 ◦ C
pH – 7 TDS – 39.3 %
Cd – 0.1 g/L COD –79.5 % [140,
Watermelon seed Oil-free powder
Speed – 100 rpm Turbidity – 98.5 % 141]
Time – 8 min BOD – 91.5 %

Soap and Detergent industry wastewater

Turbidity – 97.72 %
Tamarind seed Powder Cd - 400 mg/L [142]
COD – 39.55 %
Mass loading – 50 mm Color removal - 90 %
pH – 7
Chitosan – [23]
Speed – 150 rpm COD – 83 %
Time – 5 min

Textile industry wastewater

Chitosan – Cd - 25 g/L to 30 g/L Color removal - 43 %
Color removal – 47.03 %
Maize seed (Zea mays) Powder Cd - 30 g/l
COD – 68.82 % [143]
Color removal – 62.82 %
Surjana seed Powder Cd - 25 g/l and 30 g/l
COD – 74.11 %
Colour - 68.5 %
Ocimum basilicum Mucilage Cd - 1.6 mg/L [144]
COD - 61.6 %
pH - 35 %
Turbidity - 48 %
Moringa Oleifera (Mo) Powder Cd – 60 mL
TDS - 70 %
TSS - 57 %
[145]
pH - 32 %
Turbidity - 32 %
Tamarindus Indica (TI) Powder Cd – 60 mL
TDS - 48 %
TSS - 44 %
SP (nirmali seeds): Turbidity -23.07 %
Cd – 5 g TDS - 76.72 %
Strychnos potatorum (SP) TSS - 33.74 %
(nirmali seeds) COD - 45.7 %
pH - 1.95 %
BOD - 51.21 %,
Hardness - 9.94 %
Pressed seedcake [146]
Cd – 8 g Turbidity - 53.85 %
TDS - 92.90 %
Eirchorrnia crassipes (EC) TSS - 36.49 %
(water hyacinth) pH - 2.37 % COD - 50.80 %
BOD - 51.21 %
Hardness - 33.33 %

Paper mills industry wastewater

Dolichas lablab; Cd - 16 g Turbidity - 37.45 %
Azadirachta Indica Cd - 6.5 g Turbidity - 63.01 %
Powder [147]
Moringa Oleifera Cd - 3g Turbidity - 31.47 %
Hibiscus Rosa Sinensis Cd - 1g Turbidity - 12.95 %
Turbidity - 96.02 %
Moringa oleifera seed Powder pH range – 6− 8, 150 mg/L [147]
COD – 97.28 %

Household laundry rinsing water

Turbidity- 89.5 %,
Nirmali seed and Orange peel Cd mixture of Nirmali seed (6.4 g/L) and Orange peel
Pectin filterate TSS- 81.5 % [148]
pectin pectin (1.6 mL/L) at 24 h
COD- 56 %
Turbidity – 83.63 %
Moringa oleifera seed Powder Cd - 120 mg/L [149]
COD – 54.18 %

Pharmaceutical industry wastewater

Cd - 100 mg/L
Date palm (Phoenix dactylifera) Powder Settling time - 50 min. Color removal - 99.86 % [21]
pH - 2

Dairy wastewater
pH – 4 TDS – 57 %
Chitosan [150]
Cd – 10 mg/L COD – 62 %

Concrete industry
Cd: 60 mg/L Turbidity- 87.5 %
Lemon peels
OpH range: 7.3− 7.6 COD – 9.78 %
Powder [151]
Cd: 30 mg/L Turbidity- 88.75 %
Neem leaves
OpH range: 6.80− 7.02 COD – 10.75 %
(continued on next page)

10
A.A. Owodunni and S. Ismail Journal of Water Process Engineering 42 (2021) 102096

Table 3 (continued )
Coagulant Form of application Optimum conditions Parameters and maximum Ref.
removal efficiency

Cd: 30 mg/L Turbidity- 94.16 %

Tulsi leaves
OpH range: 8.48− 9.06. COD – 40.38 %
Cd: 20 mg/L Turbidity- 96.67 %
Rambutan seeds
OpH range: 7.43− 8.68 COD – 46.18 %
Cd: 40 mg/L Turbidity- 83.75 %
Papaya seeds
OpH range: 6.8− 8.02 COD - 45.79 %

Cd: Coagulant dosage; OpH: Optimum pH; COD: Chemical oxygen demand; Mo: Moringa oleifera; TP: total phosphate; TSS: total suspended solids; TDS: total dissolved
solids.

with less toxicity, and is easily accessible [82]. Although using the
extracted active solution is highly efficient, coagulation efficiency might
decline due to the microbial decomposition of the organic materials
during storage. Thus, it is preferred to prepare and use fresh coagulants
directly to evade the aging effects on the solution [172].
Previous studies have identified a setback in the coagulation activity
of natural coagulants due to the presence of other components asides
from the active coagulation agents. These materials rich in plant tissue
tend to increase the organic load in the treated water causing a defi­
ciency to the treatment, this can be minimized or prevented by further
purifying the coagulant proteins [173].
4.2. Isolation, purification, and identification of proteins
The lower shelf life of water treated with seed crude extracts has
been attributed to the presence of high organic matter (loads). Isolation
and purification of the active coagulating agent from the crude extracts
reduce the organic loads in the treated water [174]. In the removal of
cyanobacteria from surface water by Camacho et al., [32], the dissolved
organic matter was discovered to increase irrespective of the extractions
done (both oil-extraction with ethanol, and salt solution (NaCl) extrac­
tion). However salt solution extracted Mo was able to remove aromatic
organic matter up to 50 % [32].
Previous studies have identified the purified natural coagulants
extract by protein precipitation (chemical, solvents, isoelectric, heavy
metal ions), dialysis [175,176], ion-exchange chromatography [177,
178], and membrane filtration (ultra, micro, nanofiltration, reverse
osmosis) [179–181]. These techniques are dodged because it adds to the
overall cost of water treatment. The technologies separate the active
coagulants from contaminants by their molecular weights (size), pH,
and electric charge using membranes, centrifugation, and adsorbents.
Table 4 gives some of the advantages and disadvantages of the purifi­
cation techniques.
Ion exchange techniques use molecular charge to separate the
cationic coagulant from anionic and non-ionic contaminants. The dif­
ference in the charges, charge density, and distribution on the surfaces
of the substances causes the different degrees of interaction with the ion
exchanger which leads to separation. Ionic strength and pH are condi­
tions that could be varied to control these interactions [182]. A study by
Taiwo et al. [183], discovered a significant reduction in turbidity and
organic load resulting in 58.18 % total coliform reduction. In the study,
Moringa oleifera (Mo) seed purified using the ion exchange and gel
filtration chromatography was used in water treatment. Sodium dodecyl
sulphate polyacrylamide gel electrophoresis (SDS-PAGE) and gel filtra­
tion were used to analyze the subunit and native molecular weight
which were determined as 14.2 kDa and 30.3 kDa respectively.
The lyophilization technique separates the coagulant from the
contaminant by free the crude extract, followed by extracting and drying
the supernatant at low temperatures through a vacuum. The potential of
using ultrafiltration as a purification method for natural coagulants was
studied by Prodanović et al. [181]. Ultrafiltration membranes removed
molecules that inhibited high turbidity removal, the crude extracts were
separated into 4 fractions (<5 - <30 kDa). The organic load in Phaseolus
vulgaris seed treated water was minimized up to 50 % when the 4th
fraction (the contents were predominantly protein with molecular
weight 50–60 kDa) was used as a coagulant, compared to the organic
load (66 %) of crude extract-treated water. It also had the highest
coagulation activity of 75 % similar to the crude extract coagulation
activity [181].
A combination of one or more purification technique was used by
Choudhary and Neogi [184] in the purification, isolation, and identifi­
cation of Mo protein for water treatment. Chemical precipitation using
ammonium sulphate was used for isolation of the active coagulant from
the contaminants. Purification of the isolated proteins was done using
the dialysis tube (dialysis) with molecular wight 1 kDa to remove the
ammonium sulphate. Lyophilization was finally used to achieve a stable

Table 4
Merits and Demerits of Notable Purification Techniques.
Method Means Parameter Advantages Disadvantages Ref

Choice of buffer (pH and

Ion Exchange Molecular charge: ion-exchange Simple, [177,
ionic strength), High cost of operation
Chromatography media (resin, liquids, membranes) 182]
Isoelectric point Easy to scale
Precipitation pH,
Chemical Desalination is often required because of the [184,
Ammonium sulphate Nature and Relatively simple
Precipitation high salt environment 185]
concentration of ion
Molecular weight and Low energy
Dialysis Dialysis tubes Slow process [186]
size consumption
Molecular weight and
Fractionation using membranes Fouling,
size, A promising technique
Ultrafiltration (molecular weights - 5, 10, and [173]
Pressure of inert gas, for purification Quality - overlap in molecular weights of
30 kDa)
Stirring rate natural coagulants and organic contaminants
Freezing and dehydration of the proteins
Longer shelf life, may result in the alteration of protein
[187,
Lyophilization Freeze-drying Freezing temperature structure,
188]
Maintains coagulation
High running cost.
efficiency

11
A.A. Owodunni and S. Ismail
powdered form of the proteins, the isolated samples were freeze-dried at
− 80 ◦ C and placed in the lyophilizer for 2 days. The pure protein powder
obtained was 9% of the initial 5 g of the Mo seed powder used. The
proteins had a high turbidity removal efficiency of 88 %. Identification
using SDS-PAGE analysis also showed that isolated proteins with lower
molecular weight (<36 kDa) had the highest coagulation properties
because of their 100 % turbidity removal and without increasing the
organic load in the water [184].
4.3. Composite coagulants
Reports have mentioned that solely using natural coagulants have a
slight possibility of yielding poor performance in wastewater treatment
[126,128]. The solution to this challenge has been sought by producing
composite or hybrid coagulants, the coagulants are combined with
either natural or chemical coagulants [96,189]. Several successful ap­
plications of composite coagulants in wastewater treatment has shown
improved treatment performances.
A study by Ravikumar and Udayakumar [190] developed an
environmentally-friendly composite coagulants by combining bentonite
clay (BC) and moringa oleifera (MO) seed extract, 5 g/L dose of the
coagulant was able to remove heavy metals (cadmium, chromium, and
lead) with up to 99.99 % efficiency after 40 min of rapid mixing and
15 min of slow mixing. Characterization of the composites showed that
the BC and MO biopolymer physicochemically interacted with each
other during the preparation. The biopolymer is grafted into the
bentonite clay structure, thereby introducing functional groups (O-H,
C-H, C-O, and C-N, stretches) that assist coagulation process to the
spectra. The biopolymer molecules were captured between the clay
structure layers, which protects the molecules from enzymatic reactions
of microorganism on it. Thus, the challenge of low shell-life face by the
MO biopolymer is treated as the composite shelf-life is increased to more
than two years [190].
It is irrefutable that composite coagulants have the ability to reduce
the chemical coagulant dosage which would lessen its toxic effect and
tackle other negative drawbacks. When compared with PACl, the
chitosan-based composite coagulant produced by Yang et al., [191]
showed lower dosage, wider application pH range, better removal effi­
ciency, and produced sludge with lower toxicity. The coagulant’s per­
formance were ascribed to the enhanced positive charges and higher
molecular weight [191]. The application of composite coagulant was
also able to overcome the problem of weak flocs, a positive result on the
increased floc size, growth rate, and recoverability of the flocs was
achieved [189]. The economical advantage of using the composite co­
agulants while exhibiting excellent performance makes them a good
potential for industrialization and commercialization.
5. Parameters varied to determine the efficacy of the coagulants
on the coagulation activity
In the evaluation of coagulant and its efficiency in water treatment,
several parameters are varied to determine the optimum parameter
values that will give the highest efficiency. These coagulation operating
factors have huge impacts on the reactions present during the coagula­
tion processes, as they influence the efficiency and effectiveness of the
coagulants in the wastewater treatment processes. Cheng et al. [192]
implied that total suspended solids (TSS), clear color, turbidity, total
organic carbon (TOC), temperature, and pH are parameters that are
evaluated to gauge the efficiency of the coagulation process.
5.1. Effect of coagulation dosage
A good coagulant is characterized by having a very high positive
charge to neutralize the negative charge exhibited by the fine particles
present in the water body; a comparatively low molecular weight to aid
proper diffusion of the cationic charges around the particles to intensify
12
Journal of Water Process Engineering 42 (2021) 102096
dispersion of the coagulant in the water bodies. The selection of the
optimum coagulant dosage is a very essential parameter in coagulation,
the required coagulant dose will effectively aggregate the suspended
particulates in the water. Coagulation dosage affects the efficiency of the
wastewater coagulation process in such a way that a dosage lower to the
optimum will inhibit proper removal of the effluent, while overdosage
results in increased turbidity, organic matter, and higher slurry volume,
and thus leading to a high cost of treatment [193].
Several researchers have studied the effects of varying the coagula­
tion dosages to obtain the optimum for efficient treatment. Jagaba et al.
[123] in the treatment of POME to reduce the turbidity and color varied
the coagulant dosage from 500− 5000 mg/L, obtaining an optimum
coagulation dosage of 2000 mg/L which gave turbidity, COD, TSS,
color, and oil & grease removals of 88.30 %, 38.60 %, 95.42 %, 90.15 %,
87.05 %, respectively. However, lower optimum dosage values of the
moringa seed powder have been reported by several other researchers,
Muruganandam et al. [54] reduced the turbidity of raw tannery effluent
by 59.43 % at optimum dosage of 15 mg/L, a closer value of 20 mg/L
was also reported by Ramesh et al. [194]. Dehghani et al. [75] also
achieved 70 mg/L as the optimal dosage after treating the oil refinery
wastewater, the dosage removed COD, turbidity, and TSS up to 38.60 %,
63.70 %, and 62.05 %, respectively.
Ernest et al. [116] reported the optimal dosage of watermelon seed to
be 0.6 g/L after varying between 0.2–1.0 g/L to remove the turbidity
and color of river water, the optimal dosage had an efficiency of 86 %
turbidity and 82.7 % color removals. Table 3 gives some of the optimal
coagulant dosages. As it is common with green coagulants, the per­
centage turbidity reduction increases as the coagulant dosages increase
towards the optimum coagulant dosage, and beyond which increase in
coagulant dosage leads to a decreased turbidity reduction [54]. There­
fore, it is important to use the jar test in the laboratory scale to study the
effect of varying dosages to determine the optimal.
5.2. Effect of pH
pH is the measurement of the acidity or alkalinity of the water, which
value is between 1–14, it can be measured with the aid of a pH meter.
The charge on the amphoteric coagulant molecules is often highly
dependent on the pH values in the wastewater undergoing treatment
[195]. Alkalinity is measured to determine the capacity to neutralize an
acid; in the coagulation process, it dominates the efficiency at which the
chemicals react with the water and affect the destabilization process.
Most chemical coagulants especially ferric-based salts consume a high
percentage of alkalinity. It is believed that lower alkalinity generates
poor floc formation which needs the addition of alkalinity sources some
of which include soda ash or lime or caustic soda to the water. The pH
value outside the range of the optimum pH results in the generation of a
mixture of positive and negative charges of the amino acid in the protein
which may lead to the reduction of the net cationic efficiency of the
coagulant in the coagulation process.
The pH value of the medium has a huge influence on the protein
molecule ionic charges; hence it determines the amount of coagulant
required for an efficient coagulation process and thus, pH adjustment
should be done before proceeding with the coagulation process [23].
The most commonly used chemicals for lowering and increasing acidity
are sodium chloride (NaCl) and H2SO4, respectively, other chemicals
can be used to increase the pH values such as sodium carbonate, hy­
droxides of calcium, ammonia, and magnesium, while hydrochloric acid
and phosphoric acid also highly effect decreasing the pH of the water.
However, the addition of these chemicals may increase the pH
beyond the needed value, requiring additional adjustment of the pH to
obtain proper floc formation. In the case of water with higher alkalinity,
an extremely higher coagulant dosage could be needed to low the pH to
the optimal pH for effective coagulation. Regrettably, the extra addition
of coagulant doses could lead to the exorbitant cost of treatment as a
result of disposing of the enormous sludge generated. The pH was varied
A.A. Owodunni and S. Ismail
between 5–9 when using the mucilage of cactus to remove turbidity and
COD of tannery effluent by Muruganandam et al. [54], 51.50 % and
59.35 % removal were obtained for the turbidity and COD at an optimal
pH of 7. The cactus-based coagulant was neither denatured by the acidic
nor the alkaline conditions and thus the neutral pH is the most effective
and more preferred. The optimal pH value of 7–7.5 for watermelon seed
coagulants is concluded from researches conducted [116,140,141].
The amino acid in the moringa oleifera and jatropha curcas protein
coagulants are more effective in acidic conditions. This is supported by
various studies, using moringa oleifera, Sasikala et al. [196] revealed
that the positive charges on the amino acids that constitute the coagu­
lant are dominating and effectively works as a cationic coagulant. It is
believed that almost all amino acids present in seed proteins have pos­
itive charges at pH values of less than 3 and higher than 11, which was
observed in the turbidity removal of about 99 % while using moringa
oleifera; jatropha curcas seed extract as the coagulant. They obtained a
turbidity removal of 99 % at an optimal pH value of 3 after varying from
1 to 12. Although, exceptions such as Boulaadjoul et al. [57] reported an
optimum pH range of 6− 8 after treating wastewater from paper mill
reduced the turbidity by 97 % which implies that the protein coagulant
is still relevant for treating a wide range of pH. Abidin [197] expected
that most of the amino acids present in the jatropha curcas seed protein
have isoelectric point values from 3.2 to 11, suggesting that the coag­
ulant works effectively as a positively charged coagulant agent at a pH of
relatively 3.
Another efficient removal of the petroleum industrial waste was
studied by Khader et al. [138] using cicer arietinum seed, eggplant seed,
and radish seeds. The pH of the coagulants was varied from 2 to 11 with
optimal achieved at 7, the optimal gave turbidity removal of 98.2 %,
98.7 %, 98.2 %, COD 95 %, 91.8 %, 92.6 %, and oil removals of 83 %, 80
%, 87 % for cicer arietinum seed, eggplant seed, and radish seeds,
respectively. The pH values below and above 7 caused decreased
removal efficiency [138].
5.3. Effect of initial turbidity
Turbidity is an essential factor that affects effective wastewater
treatment, it is a visual property of water due to its close association with
the color of the water. The presence of suspended solid particles in the
water induces turbidity resulting in the absence of clarity. Abundant
microorganisms, soil, organic matter, colored compounds (dye),
decaying matter, plankton, and algae cause the turbid water to look
cloudy, murky, and undesirable [198]. The increasing rate of turbidity is
simultaneous to the increase in effluent; thus, turbidity and solid par­
ticles are a challenge in wastewater treatment [199].
The effect of initial turbidity on the coagulation performance using
jatropha curcas as coagulant was studied by Abidin et al. [129]. The
kaolin wastewater samples were set at initial turbidities ranging from
Fig. 5. Process flow diagram of treatment of aquaculture effluent (Ebeling et al., 2003).
13
Journal of Water Process Engineering 42 (2021) 102096
100 to 8000 NTU. The turbidity removal for all initial turbidity values
was higher than 98.4 %, it was reported that the maximum turbidity
removal was achieved at 500 NTU at 99.5 %. There was an increase in
turbidity removal from 100 up to 500 NTU, which was followed by
slightly decreased removal performance as the initial turbidity increased
up to 8000 NTU. It was thus concluded that jatropha curcas is a natural
coagulant applicable for wastewater treatment of a wide range of initial
turbidity (Abidin et al., 2011).
5.4. Effect of stirring speed and time
Adequate stirring speed and time is an essential parameter that
contributes to effective coagulation leading to higher performance in
wastewater treatment. Two mixing speeds are used during the conduc­
tion of the coagulation-flocculation experiment comprising of slow and
rapid mixing. The rapid mixing is done immediately the coagulation
additives are added to aid uniform distribution throughout the medium
and to destabilize the colloidal particles, while the slow mixing is
introduced to enable collision of the particles to cluster, aggregate, and
form macroflocs. The efficiency of the coagulation process is highly
affected by the adequacy of both mixing times and speed because and
inadequate mixing time will hinder proper agglomeration of the colloids
leading to decreased efficiency of turbidity. The velocity gradient is the
parameter used to express the mixing intensity.
Anteneh and Sahu [23] examined the effect of mixing time on COD
removal food industry wastewater, the treatment was done using chi­
tosan as a natural coagulant with the stirring speed varied within the
range of 50− 200 rpm. It was reported that mixing speeds from 50 rpm
to 120 rpm had increasing COD and color reductions of up to 58–72 %
and 63–81 %, respectively. The further increase to 150 rpm gave the
best performance at 83 % and 90 % for COD and color reduction.
However, it was observed that upon further increase of the speeds to
200 rpm, a decrease occurred in the performance for COD and color
reduction at 74 % and 79 % [23]. The coagulation mechanism attributed
to the process is also influenced by the stirring speed and time.
For the particle settling, coagulant aids or flocculants are often added
together with the coagulant to support the aggregation and settling of
the small flocs that settle very slowly. Logically, turbidity reduction in
the water increase as the time allowed is lengthened. However, it gets to
maximum when colloids have completely settled [33]. Most coagulation
studies have been reported to set the settling time of the experiment
within 15− 60 mins [172]. A considerably high settling time of about
72 h was required for the removal of dye from dye wastewater using
Azadirachta indica as natural coagulants. Even though up to 80 % dye
removal was achieved by the coagulants, this averagely long period for
the settling time necessitates the use of a flocculant aid to improve the
sedimentation process of the biocoagulants for economic and effective
application [200].
A.A. Owodunni and S. Ismail
Fig. 6. Process flow diagram of treatment of a textile wastewater [207].
6. Natural coagulant and their applications
A shift towards the use of natural coagulants for the purification of
water and wastewater treatment has been observed in recent times. It is
believed that a yield of up to 90 % of total suspended solids is removed
from wastewater if coagulation was done before gravity settling when
compared to treatment without the coagulation process [103]. Overall,
the treatment materials are added into the wastewater and thoroughly
mixed to destabilize the suspended particles, collision occurs between
the particles as they begin to cluster and aggregate to form larger and
denser flocs enabling the flocs to settle for easier removal [201].
The coagulation process is commonly used by industries that apply
the sedimentation process in treating their wastewater effluents gener­
ated. Few of these industries are not limited to agriculture, aquaculture,
food processing, beverage production, paint and varnishes, cement,
adhesives, soap and detergent, cosmetics, leather, iron and steel, plas­
tics, textile and dyeing, pulp and paper industries.
The challenge of selecting the proper coagulant for efficient treat­
ment and the conditions for coagulation places a toll on the industries.
The effective coagulation process depended largely on the type of
coagulant, coagulant dosage, the coagulant charge, the mixing param­
eters, amount and properties of impurities present in the effluent, pH of
the water [202].
6.1. Aquaculture industry
A typical process flow diagram of an aquaculture wastewater treat­
ment plant is given in Fig. 5. Several coagulants have been applied in the
treatment of wastewater generated from the aquaculture industry, often
the coagulation treatments are done in such a way that the clean water
will be obtained for reuse, while simultaneously obtaining the nutrient-
rich sludge for further processing as a raw material for other products e.
g. soil conditioner, fertilizer or feed for microalgae. The potential of
chitosan, pawpaw, as organic coagulants were investigated in treating
the wastewater generated from this industry to encourage sustainability
and efficient treatment in the industry.
A study discovered by Yunos et al. [127] used an optimum coagulant
dosage of 30 mg/L which resulted in algae removal efficiency of 98 %.
This study used chitosan as a coagulant with the aim of harvesting
microalgae from the catfish aquaculture sample. For the treatment, a
stock solution was prepared by dissolving 100 mg of the purchased
chitosan powder from shrimp shells in 10 mL of 0.1 M HCl before stir­
ring for 10 min. till the chitosan powder dissolved completely. The stock
solution was further diluted with deionized water before use. After the
experiment, the turbidity of the wastewater was also reduced from 60
NTU to 2.2 NTU, it was further claimed that the supernatant water
14
Journal of Water Process Engineering 42 (2021) 102096
discharged could be used as recycled water or released in the water
bodies [127].
6.2. Textile industry
Large volumes of water are used in every section of the textile in­
dustry in processing various types of fabric, especially during the
scouring, bleaching, washing, dyeing, and printing processes [203,204].
Fig. 6 gives the flowchart of a typical textile wastewater treatment
process.
Huang et al. [205] claimed that the coagulation-flocculation process
is commonly used in treating this type of wastewater due to its high
effectiveness and economic advantages in removing the dyes, additives,
and salts. Nevertheless, the application of inorganic chemical coagulants
contributes more to the pollution as numerous unsolicited reactions
occur in the water producing huge volumes of sludge and residual
chemicals, thus, researchers sought for the potential of natural co­
agulants to substitute the chemical coagulants in effectively treating and
decolorizing this industrial wastewater [44,82,144–146,206].
Moringa oleifera Lam seeds were compared with aluminium sulphate
to evaluate their effectiveness in treating textile wastewater. Moringa
oleifera Lam seed of 5.0 g was titrated in 100 mL of KCl 1.0 mol/L
(MKCl) as well as 1.0 mol/L NaCl (MNaCl) to obtain the seed extract, the
mixture was consistently stirred for 30 min. and was further filtered. The
organic coagulants (MKCl and MNaCl) gave their best results at an acidic
pH value of 2, with a coagulation dosage of 20,000 mg/L. Overall, the
moringa coagulant extracted in KCl (MKCl) presented the highest effi­
ciency when compared with the other two coagulants with an 82.2 %
removal for the apparent color, removal of 83.05 %, 78.4 %, 89.7 % for
COD, RP-HE7B dye, and OP-HER dye, respectively. Though the potential
for using the extract of moringa oleifera seeds as coagulant was
confirmed, it was however noted that the cost of the treatment process is
not economical due to the high coagulation dose required for effective
treatment [33].
6.3. Agriculture industry
It is highly important to remove the pollutants generated from
several activities (washing, separating, grinding, and purification) in the
agricultural industry before disposing the water which could be poten­
tially harmful to the human, environment, and aquatic habitats. Coag­
ulation has been extensively applied in the treatment process, some of
the natural coagulants used are given in Tables 2 and 3.
The coagulation performance of some chemical coagulants
(aluminium sulphate and ferric chloride) were compared with natural
coagulants (chitosan, moringa oleifera, and zeolite) in the palm oil
A.A. Owodunni and S. Ismail
milling effluent (POME) treatment by Jagaba et al., [123]. In preparing
the chitosan stock solution, 1.5 g of the powder was dissolved in 150 mL
of 0.1 M HCl and was stirred till it was dissolved. The extraction process
of removing the effective components for coagulation from the seed
began from cleaning and grinding the seeds into powder before sieving
through a mesh size of 0.8–2.5 mm. The moringa seed oil was extracted
with the aid of a Soxhlet apparatus, while the oil-free cake was dissolved
with distilled water. After the treatment, characterization, and com­
parison were made, aluminium sulphate was recognized to require the
highest coagulant dose as its optimum was 4000 mg/L which was fol­
lowed by moringa oleifera with an optimum dose of 2000 mg/L, ferric
chloride and zeolite equally had 1000 mg/L has their optimum dosage,
chitosan required the least dosage of 400 mg/L. Overall, chitosan was
proved to be the best as it gave the best result in removal TSS at 98.95 %,
turbidity, and COD removal at 98.35 % and 68.31 %, respectively [123].
Other studies also reported the efficient treatment of POME using
natural coagulant, the wheat germ was used as a coagulant had
turbidity, TSS, and COD reduction performance of 99.1 %, 95.6 %, and
61.7 %, respectively [208]. Peanut seed coagulant, which was extracted
with 1 M NaCl solution also achieved 93.6 % and 67.0 % for the TSS and
COD reduction, respectively [209].
6.4. Efficiency of the wastewater treatment process (parameters)
During wastewater treatment, the efficiency of the coagulation
process is judged based on its percentage removal of turbidity, total
suspended solids (TSS), chemical oxygen demand (COD), chemical
phosphorus, natural organic matter (NOM), color, heavy metals, and
other pollutants. The nature and properties of the wastewater determine
the coagulants to be used and the parameters to be removed during
treatment. The coagulation-flocculation process revolves around the
destabilization of the suspended particles and clustering them to form
macroflocs to enable sedimentation and filtration. Some properties
which influence adequate coagulation activities include turbidity, pH,
and others.
6.4.1. Total suspended solids (TSS)
Total suspended solids (TSS) signifies the quality of water, it is the
overall amount of solid material (organic and inorganic matter, sus­
pended, and settleable particles) that can be filtered in the wastewater
[210]. The TSS consist of an extensive variety that is not limited to in­
dustrial wastes and effluents, mud, animal carcass, and rotting plants.
The suspended particles support the adhesion of metals and various
harmful compounds.
A high concentration of suspended solids results in high turbid water
which poses a challenge to the environment and the aquatic ecosystem.
It can reduce the penetration of sunlight into the water, negatively
affecting the photosynthesis process. The TSS is measured by filtering a
water sample, drying, and accurately weighing the solids obtained. The
quantity of TSS is recorded in a unit of mg/L. The TSS reduction per­
centage was calculated using Eq. 1.
(TSS0 − TSS)
TSS reduction (%) = × 100 (1)
TSS0
where TSS0 is the value before treatment, and TSS is the value after the
treatment process.
Tamarind indica seed powder as a coagulant achieved a 24.32 %
removal of TSS from a traditional gold mine wastewater [168]. Many
other studies on the removal of TSS from palm oil mill effluent (POME)
includes; treatment with Cassia obtusifolia seed gum removed 93.22 %
[55]; treatment with moringa oleifera and chitosan removed 95.42 %
and 98.9 %, respectively [123]; 84.1 % removal achieved after treat­
ment with rice starch [131]. Other reported studies of TSS removal in
various industrial wastewaters can be found in Table 3.
15
Journal of Water Process Engineering 42 (2021) 102096
6.4.2. Turbidity
High turbid water exhibits a cloudy appearance as a result of the
impurities present, it negatively affects the ecosystem, environment, and
aquatic habitation [211]. Turbidity experienced in aquaculture habitat
inhibits sunlight penetration and distribution of which could affect
photosynthesis and the fish breeding process. Asides from the lowered
oxygen concentration in the water which leads to stunted respiration,
the suspended particles could also clog the gills of the fish [212].
Turbidity is measured as an indicator of water quality based on its
clearness and overall suspended solids in the water; it is believed that
higher turbidity of water lowers its quality. A turbidimeter or a nephe­
lometer is used to measure turbidity with a unit of Nephelometric
Turbidity Units (NTU) [213]. The turbidity reduction percentage is
calculated using Standard Method 2130B and Eq. 2.
(Initial turbidity − final turbidity)
Turbidity removal (%) = × 100 (2)
Initial turbidity
Coagulation is a principal process for treating and reducing turbidity.
As a result of the low concentration of stable particles, water with lower
turbidity is believed to be difficult to coagulate, and thus to improve
coagulation artificial turbidity is introduced into the water to aid the
formation of denser flocs which would readily settle. Asrafuzzaman et al.
[214] studied and compared the influences of natural coagulants (ex­
tracts of Moringa oleifera, Cicer arietinum, and Dolichos lablab) on
turbidity (high, medium, and low) of synthetic water, it was found that
the biocoagulants gave better results with higher turbid water and a
turbidity reduction efficiency of 95.89 % [214]. Khader et al. [138]
treated petroleum industry water with extracted solutions of radish,
eggplant, and chickpea seed powders, achieving turbidity removal of
98.785, 99.42 %, and 95.2 %, respectively [138]. Few other natural
coagulants that removed turbidity from industrial water have been
highlighted in Table 3.
6.4.3. Biochemical oxygen demand (BOD)
Biochemical Oxygen Demand (BOD) is a principal environmental
index that analyses the dissolved oxygen required by aerobic biological
organisms (bacteria and other microorganisms) for the oxidation of
organic matter present in the water body. It is especially used in char­
acterizing the concentration of natural organic matter (NOM), in aquatic
industrial wastewater treatment, agricultural industries (poultry, animal
farming), and other industries that apply organic materials in their
processes [215]. The organic materials released into the water body
results in the generation and growth of microorganisms, thereby
depleting the oxygen necessary for other aquatic habitats.
BOD is analyzed by calculating the oxygen-depleted in a diluted
aqueous specimen incubated with microorganisms, it is expressed in
milligrams of oxygen consumed per liter of the sample used for the in­
cubation period [216]. Firstly, the oxygen of the sample collected from
the waterbody is measured at the beginning of the reaction, the tem­
perature is then set within 20− 25 ◦ C and left in the dark for 5 days for
incubation, the oxygen is remeasured after the prescribed period of in­
cubation. The limitation of the BOD test is a result of the 5-day incu­
bation period, which hinders its usage in making operational decisions.
The BOD reduction percentage can be calculated using Eq. 3.
(BOD0 − BOD)
BOD reduction (%) = × 100 (3)
BOD0
where BOD0 is the value before treatment, and BOD the value after the
treatment process.
BOD of 91.5 % was removed after the treatment of municipal
wastewater with watermelon seed, the watermelon seed was used as the
organic coagulant and microbial filter (Manyuchi et al., 2016).
6.4.4. Chemical oxygen demand (COD)
Chemical oxygen demand (COD) is the measurement of oxygen that
A.A. Owodunni and S. Ismail
is consumed by reactions in a measured sample solution. The COD test
can be efficiently used in measuring the number of organics in the
waterbody, it is an alternative test to BOD as it was established due to
inefficient analysis of BOD which required 5 days of incubation for
completion. The 5220 B-open reflux-titrimetric method is used to
determine the chemical oxygen demand (COD) measurement using the
method USEPA Method 8000. It is expressed in the mass of oxygen
(milligrams) of oxygen consumed per liter of the sample (mg/L). The
COD reduction percentage was calculated using Eq. 4.
(COD0 − COD)
COD reduction (%) = × 100 (4)
COD0
where COD0 is the value before treatment, and COD the value after the
treatment process.
The laundry wastewater treated by Al-Gheethi et al. [149] using
moringa oleifera seed powder, were found to initially contain high COD
concentrations of 423− 450 mg/L. This was reported to possibly be as a
result of the detergent compounds present, increasing the chemical
reactivity between the organic substances. A coagulant dosage of
90 mg/L was able to reduce the COD by 42.72 %. The proteins existing
in the moringa seed encourages its ability to degrade organic com­
pounds, which aid the degradation of organic matter and thus causing
the COD removal. With the aid of hydrolyses enzymes, the microor­
ganisms consume the organic compounds binded to the proteins as
carbon sources. It was observed that the degradation process requires a
long period to allow for substantial COD removal [149].
A maximum COD removal of 68.82 % and 74.11 % from textile in­
dustry wastewater was achieved by treatment with maize and surjana
seed powders, respectively [143].
6.4.5. Natural organic matter (NOM) removal
Coagulation has been used in wastewater treatment to remove nat­
ural organic material (NOM) from the water. NOM is the comprehensive
name for mixtures of organic compounds contaminating the water, they
are substances generated from the aqueous discharges and solutions
derived from rotting plant, fertilizers, dead organisms, and animal waste
[217]. NOM contaminates water by contributing repugnant color, odor,
and taste to the clear water body, they are also believed to serve as a
means of conveying harmful materials such as organic pollutants and
heavy metals; they also react with chlorine resulting in the production of
carcinogenic by-products; these substances function as a food source for
bacteria, thus, enhancing biofilm production in the water [94,218].
One of the most common and economically practicable treatment
processes of removing these NOM is the coagulation-flocculation pro­
cess. The extent to which coagulation removes NOM is largely depen­
dent on the properties of organic materials existing in the water, the type
and dosage of coagulant, and pH [34,219]. During the coagulation
process, the natural organic materials are removed simultaneously with
efficient turbidity removal. Coagulants (aluminates, ferric, and their
polymeric versions) have been effectively used, as almost all types of
NOM can be removed by coagulation [106]. However, the hydrophobic
fraction (humic and fulvic acid, tannic acid, hydrocarbons, tannins, and
resorcinol) and higher molar mass compounds of NOM are more effec­
tively removed than the hydrophilic fractions (carboxylic acids, carbo­
hydrates, and proteins) and low molar mass compounds [220,221].
Analyzing the functional and structural characterization of NOM
present in water is a problem due to the complex properties and their
differing sources. Measuring the total organic carbon (TOC) is the most
commonly and reliably used technique to analyze the quantity of the
organic material. The NOM removal process during coagulation involves
the mixture of neutralizing the charges, entrapping, adsorption, and
complexation of the particles with the coagulant ions to form insoluble
particulate aggregate [34].
Few studies have been done in taking advantage of the biodegrad­
ability and other positive attributes of natural coagulants in NOM
16
Journal of Water Process Engineering 42 (2021) 102096
removal. A recent review article highlighted the use of chemically
modifying chitosan as a coagulant in NOM removal, chitosan has been
reported to effectively remove NOM, but its application is restricted due
to its insolubility at pH values below 6.5. Chitosan modification could be
done to provide functional groups (easily done due to the abundant free
amino and hydroxyl groups present along the chain backbone) that
would aid synergic interaction with NOM to be removed, to enhance
chitosan solubility for a broader pH range, and to increase the molecular
weight for effective bridging with NOM. Modified chitosan has showing
promising characteristics as a natural coagulant in NOM removal from
wastewater [106].
6.4.6. Phosphorus capture/ removal
Domestic, industrial, and urban wastewater discharged into the
environment without treatment has caused a disastrous challenge to the
environment and human health. The accumulation of phosphorus in the
soil and water is a result of the actions of these industries processes [222,
223]. A high percentage of phosphorus in the soil and water could lead
to eutrophication which is potentially harmful to aquatic habitats. Pol­
yphosphate, organic phosphorus, and orthophosphate are the different
forms in which phosphorus appears in the surrounding [224].
The detergent and their ingredients present in untreated car wash
wastewater is a potential cause for environmental problems because of
their toxicity to the aquatic habitat [225]. Also, the phosphates and
other elements existing in the detergents could result in the growth of
excess algae in the drainage or other waterways, and thus, the impurities
should be removed before discharge. Radin Mohamed et al. [226]
examined the coagulation efficiency of using Moringa oleifera and
Strychnos potatorum as natural coagulants in the treatment of car wash
wastewater. Moringa oleifera and Strychnos potatorum seeds were able to
achieve a phosphorus removal of 75 % and 65 %, respectively [226].
6.4.7. Color removal
Colorants are materials that can transfer or impart their color to the
substance, they are used in various industries which are not limited to
textile, food, soap, cosmetic, printing, painting, photography, plastics,
leather (shoe and bags), and paper industries [203]. Their primary
application is to alter the color of material to make it more attractive,
appealing (food), beautiful, and creative. The wastewater generated
from these industries consists of a high percentage of various dyes and
pigments. While most dyes used are soluble in water as they diffuse into
the material to impart their color on the substrate; pigments are
water-insoluble compounds and do not interact with the substrate
[206]. The dye is a major pollutant and its presence in water negatively
affects the environment and ecosystem [227].
Therefore, the industries must effectively treat the wastewater pro­
duced to rid it of dye additives and other pollutants before discharging
into the water bodies [228]. The effective decolorization and decon­
tamination of wastewater generated from these industries using the
coagulation-flocculation treatment process have been reportedly stud­
ied and researched. The treatment process is an important phase in
removing suspended particles, colorants, and natural organic matter in
the wastewater [139].
Chitosan is a biopolymer that has served as a good color removal, in
the work of Jagaba et al. [123], it had the highest color removal effi­
ciency of 96.44 % which was closely followed by moringa oleifera co­
agulants [123]. Dotto et al. [33] demonstrated that the application of
moringa coagulants extracted in saline solutions KCl and NaCl removed
the color with a high performance of 82.8 % and 72.8 %, respectively
[33].
7. Limitations and potential study in the use of natural
coagulants
Although the advantages of natural coagulants are numerous, they
have some disadvantages. One of its major limitations is that it is less
A.A. Owodunni and S. Ismail
effective in the coagulation process as a result of the lack of flexibility in
regulating their characteristics, in the production of chemical synthetic
coagulants, characteristics which is not limited to molecular weight,
charge type can be adjusted to desired property [44]. Studies and re­
searches should emerge on the characteristics and behavior of the nat­
ural coagulant and the coagulation process to proffer in-depth solutions
to the challenge inflexibility of the natural coagulants to improve their
efficiency.
Another limitation is that they significantly increase the organic load
in the water after treatment which may aid microbial activities leading
to undesired implications and increasing microbial activities [166]. The
residual organic matter could alter the odor, taste, and color of the
treated water; thus, the use of a disinfectant such as chlorine is required
[126]. A high microbial activity will require additional chlorine usage
for disinfection purposes which further increases the cost of treatment,
indirectly defeating the economic advantage of using natural coagulants
[229]. The formation of trihalomethane generated from interactions
with disinfectant (chlorine) is a potential hazard. Therefore, more
research should be considered on evaluating the relationship between
natural coagulants and the influence on chlorine.
Lastly, compared to the chemical coagulant, the green coagulant has
a shorter storage life as a result of its biodegradability [44,152]. As
eloquently described by Mohd-Salleh et al. [128], this drawback in using
natural coagulant causes extreme difficulty during coagulation, and thus
stimulate more intense and insightful researches that will aid the natural
coagulants to effectively substitute the chemical coagulants and have a
longer storage life while still maintaining the biodegradability property
[128].
Although the numerous advantages and efficacy of applying natural
coagulants has been reported by several researchers conducted in the
laboratory, its inability to be applied in the industry has inhibited their
evolution on an industrial scale of treatment [230].
8. Conclusion and further works
The review of the past and current use of natural coagulants has been
critically analyzed in this study, the coagulants have great efficiency in
wastewater treatment. Plant-based coagulants go through numerous
processes before they could be used as coagulants, beginning with the
primary process which includes cleaning, drying, and sieving of the
seeds and other plant parts before further treatment or application. The
secondary processes comprising of oil extraction and solvent (distilled
water, salt solution) extraction of the active coagulation agent, however,
salt solution extraction was determined to be the most effective tech­
nique. Reduction of organic matter loading in the treated water led to
further purification of the coagulant. Ion exchange, lyophilization, and
membrane filtration techniques have been successfully used in purifying
and isolating the coagulation protein. The discharge of industrial
wastewater is a great challenge to man, the aquatic habitat, environ­
ment, and ecosystem. The complexity of their treatment further arises
from the varying properties of these wastes based on the type of mate­
rials used in the various industries. The use of chemical coagulant for the
treatment has been widely used due to its economical and effective
advantages, but due to its several limitations which is based on its
artificial nature, residual metal salts, and non-degradability has brought
up concerns over health and the environmental risks attributed in the
continual application of the synthetic coagulants. The dire need for the
substitution of chemical coagulant has been described as a necessity in
this review. Thus, green coagulants which are degradable, natural,
environmentally-friendly, and economical have been developed as a
sustainable alternative potential in the coagulation process. These co­
agulants which are not limited to pawpaw seeds, cassava, moringa,
jatropha curcas, chitosan, algae, tannin, and others have displayed
effectiveness in treating industrial generated wastewaters. The appli­
cation of the green coagulants denotes development in the sustainability
of the industries without disruption in the quality of water, human
17
Journal of Water Process Engineering 42 (2021) 102096
health, and the environment. The extraction, purification, applications,
and evaluation of plant-based coagulants for an effective coagulation
process was discussed. Comparative performance between natural and
chemical coagulants in the treatment of industrial wastewater were
evaluated. Also, the influential coagulation parameters, the current
development on improving and purification techniques of the co­
agulants, and probable use of dual or combine coagulants were
addressed. Overall, green coagulants effectively remove the odor, pH,
COD, BOD, TSS, and color in wastewater; as a result of their non-
corrosive, biodegradability, long polymer chains, ecologically benefi­
cial properties. Other characteristics such as reduced generated sludge
quantity, high positive charge, ability to upsurge floc size promote their
efficacy in the treatment of wastewater which leads to reduced cost of
production and treatment of wastewater generated in the industries.
However, notable challenges identified in the use of natural coagulant
has encouraged further research to develop effective green coagulants to
be used in large-scale industrial wastewater treatment applications.
Some of the potential future research has also been highlighted for the
possible valorization of the natural coagulants in wastewater treatment.
Further research works are required to combat the various limitations of
natural coagulants. The research should focus on improving the prop­
erties of the coagulants to efficiently and optimally cleanse the waste­
water. Additionally, very limited studies have been developed on the
industrial scale application of natural coagulants, proper testing and
optimization should be evaluated for this purpose. Future research
should also investigate the reduction of residual organic matter, cost of
disinfection, and storage time of the coagulants.
Declaration of Competing Interest
The authors report no declarations of interest.
Acknowledgement
The authors would like to acknowledge Long Term Research Grant
Scheme (LRGS/1/2018/USM/01/1/1) (LRGS/2018/USM-UKM/EWS/
01) granted by Ministry of Higher Education Malaysia for funding this
research project and Universiti Sains Malaysia for the GRA-Assist
Scheme provided.
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