Journal of Cleaner Production 262 (2020) 121267

Contents lists available at ScienceDirect

Journal of Cleaner Production

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

Review

State of the art and sustainability of natural coagulants in water and

wastewater treatment
Wei Lun Ang a, b, *, Abdul Wahab Mohammad a, b
a
Centre for Sustainable Process Technology (CESPRO), Faculty of Engineering and Built Environment, Universiti Kebangsaan Malaysia, 43600, Bangi,
Selangor, Malaysia
b
Chemical Engineering Programme, Faculty of Engineering and Built Environment, Universiti Kebangsaan Malaysia, 43600, Bangi, Selangor, Malaysia

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

Article history: Natural coagulants have shown its coagulation efficiency as reported in a substantial number of research
Received 25 December 2019 articles. However, the acceptance and widespread application of natural coagulants in water industry is
Received in revised form still low. It is necessary to conduct a review to boost the potential of using natural coagulants by
28 February 2020
highlighting the current development and the efforts for improving the capability of natural coagulants,
Accepted 20 March 2020
Available online 23 March 2020
including showing the compatibility of natural coagulants with other treatment technologies in inte-
grated/hybrid treatment process; the modification of natural coagulants for marked improvement in
Handling editor: Prof. Jiri Jaromir Kleme
s coagulation performance efficiency; the possibility of hybridizing natural coagulants with other types of
coagulants; the improvement of extraction and purification approaches for high purity of natural co-
Keywords: agulants; and the synthesis of multifunctional natural coagulants. Though the current progress of natural
Natural coagulant coagulants is quite encouraging, perspectives from sustainability assessment showed that the acceptance
Water and wastewater treatment and commercialization of natural coagulants are hindered by two main challenges: practicality and
Sustainability feasibility of real field application and sustainability of using natural coagulants overlooking technical,
Coagulation
environmental, economic, and social aspects. Future research focusing on these issues may help to clarify
Hybrid
the uncertainties shrouded on natural coagulants and at the same time shifting the water industry to be
Integrated
more sustainable.
© 2020 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Emerging of natural coagulants and its associated challenges in application . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3. Improvement in natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1. Integrated/hybrid process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.2. Improvement of extraction and purification of coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.3. Modification for improved performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.4. Hybridization with inorganic or other types of coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.5. Multifunctional natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
4. Sustainability of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
5. Challenges of acceptance of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
5.1. Practicality and feasibility of real application . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
5.2. Sustainability of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
6. Future prospects of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
6.1. Up scaling study on the feasibility of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
6.2. Sustainability of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14

* Corresponding author. Centre for Sustainable Process Technology (CESPRO),

Faculty of Engineering and Built Environment, Universiti Kebangsaan Malaysia,
43600, Bangi, Selangor, Malaysia.
E-mail address: wl_ang@ukm.edu.my (W.L. Ang).

https://doi.org/10.1016/j.jclepro.2020.121267
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
2 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267

6.3. Multifunctional coagulant . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15

6.4. Quality control of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
6.5. Circular economy & bioeconomy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
7. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15

1. Introduction flocculant market are estimated to reach USD 6.01 billion by 2022
(USD 4.35 billion in 2016), observing a compound annual growth
Water scarcity has grown at an alarming rate and has now rate of 5.9% between 2017 and 2022 (MarketsandMarkets Research
become a global concern for sustainable development (Food and Private Ltd., 2017). These figures indicate that the interest and
Agriculture Organization of the United Nations, 2017). It is esti- importance of coagulation are expected to witness significant
mated that more than 2 billion people are affected by water scar- growth in the coming years and thus it is worth to gain insight into
city, with this figure projected to rise driven by the exponential this topic. The strong demand and interest in the coagulation
population growth and disruptive climate change. An equally process has boosted the exploration of new generation of co-
worrisome fact is that around 80% of wastewater goes into water- agulants with better coagulation performance and efficiency. This
ways without adequate treatment, further polluting and dwindling includes the search for natural coagulant as alternative option over
the clean water resources (United Nations Development chemical-based coagulants in the wake of sustainable
Programme, 2019). In response to the alarming state of water development.
scarcity, various water treatment technologies have been devel- Despite the proven treatment efficiency of inorganic and syn-
oped to ensure the production of adequate water supply and thetic organic coagulants, the associated drawbacks have motivated
quality to meet the demand and to conserve the availability of clean the search for natural coagulants which are generally claimed to be
water resources. A wide range of water and wastewater treatment more environmentally friendly in terms of production and usage.
technologies has been developed and improved in the past few This was reflected by the significant growth in the number of
decades. Generally, these technologies can be classified into three publication number as shown in Fig. 1. The main attractive advan-
main categories: physical (settling, media filtration, membrane, tages of natural coagulants lie in their renewability (feedstock can
adsorption, UV), chemical (coagulation, electrochemical, ion ex- be obtained easily), biodegradability, nontoxicity, and relative cost-
change, oxidation, catalytic reduction, disinfection, softening), and effectiveness (sludge handling and coagulant cost) (Saleem and
biological (phytoremediation, constructed wetlands, microbial Bachmann, 2019a). Natural coagulants can come from a variety of
biodegradation, digester, bioreactor) processes, with some pro- natural sources, such as plants, seeds, marine crustaceans and
cesses being the hybridization of more than one category (Ang and shellfish biomasses (shrimps and crabs), and microbial organisms,
Mohammad, 2019; Hamzah et al., 2017; Kumar and Chowdhury, with a majority of the research focused on plant-based and marine
2018; Yi Hong et al., 2018). biomass-based natural coagulant (Oladoja, 2015; Renault et al.,
Of these technologies, coagulation is one of the oldest processes 2009; Saleem and Bachmann, 2019a; Wei et al., 2018). The pre-
that continues to be widely employed in many water and waste- dominant coagulation mechanism of natural coagulants differs
water treatment plants. Coagulation is a process that removes the from the inorganic and synthetic organic coagulants as natural
impurities (especially suspended particles and colloids) in water by coagulants do not form hydroxide precipitates in water. Instead,
destabilizing and agglomerating the particles into larger aggre-
gates. This enables the aggregates to settle down quickly and sub-
sequently can be easily separated from the water (Jiang, 2015).
Technologies may come and go, but the demand and application of
coagulation in water and wastewater treatment processes never
wane. Indeed, it is being considered as one of the simple and cost-
effective approaches that can efficiently accelerate the removal of
suspended impurities in water. Today, even after a few millenniums
of development and technological advancement, coagulation re-
mains as one of the most important treatment processes for the
removal of impurities (mainly suspended particles) in water
treatment plants. In addition, coagulation has been widely
employed in wastewater treatment where it has been used as
pretreatment to remove the suspended impurities such that the
treated water is of desirable quality for subsequent purification
processes (Jiang, 2015). This trend indicates the indispensable role
played by the coagulation process in supplying clean water for
human consumption and treating the wastewater for reclamation
or safe discharge.
Owing to its indispensable role in various water and wastewater
treatment processes, coagulation is also a popular research subject
for many researchers to investigate the capability of coagulation in Fig. 1. Number of research publications* of natural coagulants in water and waste-
improving the treatment efficiency. The global coagulant and water treatment. *Data obtained from Scopus database with searching keywords
“natural coagulant” and “water and wastewater treatment”.
 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
due to the polymeric structures of the natural coagulants with
charged functional groups, charge neutralization and bridging are
the two dominant mechanisms for the formation of flocs and
removal of impurities (Saleem and Bachmann, 2019a). To date, the
commercially available natural coagulants are mainly derived from
shellfish (chitosan) and plants (moringa and tannin) (Graham et al.,
2008). The rest of the natural coagulants have not been commer-
cialized, remain in lab-scale trials or are only employed in small-
scale or case-specific applications.
2. Emerging of natural coagulants and its associated
challenges in application
In the past few years, a paradigm shift in water and wastewater
treatment industries has changed the culture of water operators to
adopt and implement sustainable development in the operation.
One of the realistic practices is to replace the chemicals used in the
treatment processes with “green” chemicals that cause lesser
environmental impacts in terms of production, consumption, and
secondary waste management. In this context, natural coagulants
appear to fit into the picture and can be an alternative option over
the conventional inorganic coagulants. It has been generally re-
ported that natural coagulants can be obtained from renewable
feedstock with ease, produce biodegradable sludge at lesser
quantity (potentially cutting down expenses associated with sludge
disposal), and less affected by water pH (Mohd-Salleh et al., 2019;
Saleem and Bachmann, 2019a). Numerous review articles have
reportedly proved the effectiveness of natural coagulants (mainly
chitosan and plant-based coagulants) in various water and waste-
water treatment application (Choy et al., 2015, 2014; Mohd-Salleh
et al., 2019; Oladoja, 2015; Renault et al., 2009; Saleem and
Bachmann, 2019b; Villasen ~ or-Basulto et al., 2018; Yin, 2010).
These review articles also presented the extraction of natural co-
agulants and highlighted some of the application challenges of
natural coagulants. However, the acceptance of natural coagulants
in actual water and wastewater treatment plants is low. The
commercialization of natural coagulants has encountered few
critical challenges that hinder its transition from lab or bench-scale
coagulation study to widespread actual water and wastewater
treatment application.
The main obstacle is the lack of industrial confidence to adopt
natural coagulants in the treatment processes. Though the perfor-
mance and benefits of natural coagulants as mentioned above have
been proven in lab or bench-scale studies, concern arises about its
cost-effectiveness and performance consistency in actual treatment
processes. In some articles, the dosage of natural coagulants was
less than conventional coagulants. In contrast, a number of articles
have revealed that to obtain the equivalent performance (impu-
rities removal) as conventional coagulants (inorganic coagulants), a
larger dose of natural coagulants is required due to its weaker
coagulation capability (Hoa and Hue, 2018; Katalo et al., 2018; Moa
Megersa et al., 2019b). This could potentially be linked to additional
costs associated with the increase of dosage consumption, such as
extraction, storage, transportation, and handling of natural co-
agulants. In view of this, doubts have arisen over the claim and
practical use of natural coagulants as an alternative compound for
sustainable development. To clarify these uncertainties, and to
boost the confidence of acceptance of natural coagulants, the
practices and signs of progress that could showcase the value and
usefulness of natural coagulants should be explored.
Unfortunately, a considerable number of research articles have
focused only on performance evaluation study. Hence, this review
paper aims to look into this matter and highlight what has been
done in academia that could improve the perception towards nat-
ural coagulants in water and wastewater treatment application.
3
These will be discussed in a few sections as followed: application of
natural coagulants in integrated/hybrid process; modification of
natural coagulants for improved performance; hybridization of
natural coagulants with other types of coagulants; improvement of
extraction and purification of natural coagulants; and the synthesis
of multifunctional coagulants. In addition, in alignment with the
sustainable development goals, the sustainability aspects of natural
coagulants application will be discussed.
3. Improvement in natural coagulants
3.1. Integrated/hybrid process
One of the viable strategies to boost the use and to exhibit the
usefulness of natural coagulants is to integrate it with other treat-
ment technologies, just like the integration of conventional inor-
ganic coagulants with other processes. The common practice in
water and wastewater treatment plants is to integrate various
technologies to achieve the treatment goals by utilizing the
strength of each process and to minimize the shortcoming of
others. A similar strategy can be adopted where the coagulation
process (using natural coagulants) can be integrated to enhance the
efficiency of subsequent treatment processes at par with conven-
tional inorganic coagulants.
The biological treatment unit is an indispensable process in a
typical municipal wastewater treatment plant. Attempts have been
made to reduce the working volume and demand for oxygen (en-
ergy through aeration requirement) for better treatment efficiency.
One of the methods is to reduce the organic load in the wastewater
through coagulation process. Hameed et al. (2018) incorporated
coagulation and flocculation prior the conventional biological
treatment process by employing Tanfloc, a commercialized tannin-
based coagulant (Hameed et al., 2018). It was shown that coagu-
lation process enhanced the removal efficiency of primary clarifier
by agglomerating the suspended solids for sedimentation. With the
decline of organic load, the dissolved oxygen level in aeration tank
had doubled, indicating the opportunity of cost-saving through
lower aeration requirement or the use of smaller air blower. This
demonstrates that natural coagulants are useful as conventional
inorganic coagulants as pretreatment in improving the perfor-
mance of subsequent treatment process.
Coagulation has been frequently adopted as pre-treatment prior
to membrane filtration process with the intention to mitigate
membrane fouling issues. Numerous articles of integrated
coagulation-membrane process have been reported with positive
outcomes, where the membrane fouling propensities have been
successfully minimized (Jiang, 2015). Though natural coagulants
can perform well in removing the foulants which are responsible
for membrane fouling, there are a few concerns that need to be
considered when operating such integrated process. Chitosan
natural coagulant reportedly improved the fouling propensity of
nanofiltration membrane towards the natural organic matter,
although the mitigation effectiveness was not as good as ferric
chloride inorganic coagulant (Ang et al., 2015). This could be
attributed to the charge neutralization as the predominant mech-
anism for chitosan coagulation that produced neutrally charged
particles and subsequently weakened the antifouling capability
(electrostatic repulsion) of membrane. On the other hand, Katalo
et al. (2018) reported that there was no obvious difference in
membrane fouling propensity for a microfiltration process
receiving supernatant from Moringa oleifera or alum coagulation,
although the turbidity removal efficiency of the latter was better
(Katalo et al., 2018). The use of Moringa oleifera had slightly
increased the load of organics in the treated river water, yet its
advantage over alum coagulant was that the water pH did not vary
4 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
much after the coagulation process, saving the need for pH
adjustment after the treatment process. All these showed that even
though natural coagulants possess the potential as an alternative
coagulant to mitigate membrane fouling, its impacts and compat-
ibility with the water sources and membrane performance should
be properly studied before decision is made.
Barbosa et al. (2018) showed that Moringa oleifera extracted
from the seeds was capable to treat the water-based paint waste-
water and render it suitable for reuse in the plant (Barbosa et al.,
2018). Interestingly, the quality of the treated water using Mor-
inga oleifera was on par with the treated water using aluminum
sulphate (inorganic coagulant). Integrating the coagulation with
electrolysis process further refined the quality of the supernatant
(by degrading the organic compounds in the effluent), making it
suitable for discharge into water bodies. This case study indicated
that by integrating the coagulation with other treatment technol-
ogy, the quality of the treated industrial wastewater can be further
enhanced to be safely discharged to the environment in compliance
with regulations.
Solar disinfection is a feasible process that could provide
drinking water in the rural communities of developing countries.
However, solar disinfection alone does not result in complete
disinfection of microorganism, mostly due to the turbidity (sus-
pended and organic matters) in water that blocks the penetration of
ultraviolet radiation in water and leads to low bacterial inactivation.
To resolve this issue, Megersa et al. (2019a) employed extracts from
plants as natural coagulants (Moringa stenopetala and Maerua
subcordata) to reduce the turbidity through coagulation process
(Moa Megersa et al., 2019a). The results revealed that with the use
of coagulants prior to the solar disinfection process, complete
bacterial inactivation was achieved. This could be attributed to the
removal of turbidity that increased the penetration of ultraviolet
rays which killed off the bacteria in water sources. Such case proves
that natural coagulants can be useful in the effort to supply clean
and adequate drinking water in the rural communities, where the
natural coagulants can be obtained easily and locally, without
having the financial and logistic constraints of using inorganic
coagulants.
Adjeroud et al. (2018) showed that the inclusion of Opuntia ficus
indica natural coagulant in the electrocoagulation-electroflotation
process helped to achieve 100% copper removal efficiency
(100 mg/L) in a shorter operating duration (Adjeroud et al., 2018).
The natural coagulant provided a large number of carboxyl and
hydroxyl groups for the enhanced removal of copper through
precipitation reaction. Apart from the improvement of pollutant
removal efficiency, the addition of Opuntia ficus indica had sped up
the sludge settling rate (as much as 15%) and reduced the specific
energy consumption of the electrocoagulation-electroflotation
process. The addition of natural coagulant, which consists of
various polyelectrolytes, assisted in the removal of copper (cutting
down the consumption of aluminum electrode) and reduced the
ohmic resistance of the wastewater. Consequently, the natural
coagulant improved the economic feasibility of the
electrocoagulation-electroflotation process. Hence, it can be seen
that natural coagulants can not only enhance the removal of pol-
lutants, but in certain cases can bring additional benefits as well.
There is a long list of integrated processes using natural co-
agulants. Basically, coagulation using natural coagulants can be
integrated with other treatment technologies as displayed in Fig. 2.
It can be concluded that natural coagulant is as competent as
conventional inorganic coagulant in the integrated process for a
wide variety of water sources (surface water and wastewater from
various industrial sources). The integration of natural coagulant as
pre or post-treatment of other treatment technologies will benefit
the overall process, even on par with using inorganic coagulant.
Fig. 2. Integrated/hybrid coagulation process (natural coagulants) for water and
wastewater treatment (Ahmad et al., 2015; Al-Gheethi et al., 2016; Bergamasco et al.,
2011; Bongiovani et al., 2016; da Conceiça ~o et al., 2015; Hoong and Ismail, 2018;
Mateus et al., 2017; Moa Megersa et al., 2019a; Nascimento et al., 2019; Nishi et al.,
2012; Noyma et al., 2017; Olugbade et al., 2017; Rajca, 2018; Rasool et al., 2016;
Santos et al., 2016; Vasic et al., 2013; Wang et al., 2019; Zaman et al., 2017).
Pilot-scale or real application of integrated treatment process
should be explored to affirm the competency of natural coagulants.
3.2. Improvement of extraction and purification of coagulants
Generally, majority of the natural coagulants can be categorized
into two groups based on the main compounds with coagulation
activity: polysaccharides and proteins (Choy et al., 2014;
Shamsnejati et al., 2015). Examples of the first group are chitosan,
starch, and mucilage while for protein-based natural coagulants
normally originated from plants (Moringa). The presence of hy-
droxyl and amino functional groups on these compounds
contribute to coagulation capability. Unlike the conventional
metallic inorganic coagulants where the characteristics (quality) of
the coagulants can be controlled precisely, the quality of some
natural coagulants is difficult to control. Such incident could be
ascribed to the green synthesis of these natural coagulants, where
the coagulants are extracted through various simple processes and
sources (especially plant-based coagulants where the compounds
might vary according to growth conditions).
In addition, it is inevitable that non-coagulating impurities will
also be included in the extracted natural coagulants if further pu-
rification is not conducted. However, extensive purification will
incur additional cost and render the “cost-saving” aspect of natural
coagulants unattractive. The presence of impurities that possess no
coagulation capability would severely affect the coagulation effi-
ciency, as past literatures have shown that these impurities
contributed to dissolved organic substances and subsequently
degraded the quality of the treated water (Ding et al., 2018; Gidde
et al., 2012). These give rise to uncertainties in quality control as the
performance of the natural coagulants might vary according to the
sources and extraction approaches. Subsequently, the varyingly
quality and efficiency of the natural coagulants are rather confusing
and not appealing to convince the water utilities to adopt natural
coagulants in their treatment operations. To clarify these issues,
this section will discuss the improvement of extraction approaches
and the influence on the quality and performance of natural
 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
coagulants in treating water and wastewater.
Moringa is one of the most popular plant-based natural co-
agulants that has received extensive research coverage. Various
extraction approaches of useful compounds with coagulation ac-
tivity from Moringa have been reported. The simplest method of
extraction is through the use of clean water. The powdered Moringa
seed kernel was mixed with water and stirred to release the
coagulating compounds (positively charged proteins) from the seed
kernel (Jung et al., 2018). However, coagulation efficiency of this
extraction approach is normally unsatisfactorily due to the pres-
ence of non-coagulating impurities and low number of coagulating
compounds. Water as solvent could not extract the proteins in the
seed kernel effectively. Furthermore, it was reported that together
with the protein compounds (with coagulation capability), the
lipids and carbohydrates (impurities) would also appear in the
extracted natural coagulant. Lipid content may inhibit the contact
between the coagulants and impurities, rendering the flocs for-
mation ineffective while the carbohydrates may increase the
organic matter level in the solution (Baptista et al., 2017; Gidde
et al., 2012; Megersa et al., 2017). Consequently, the coagulation
performance from the proteins has been diminished with the
adverse effects arising from the impurities.
To resolve these issues, improvement in the extraction method
and inclusion of purification step can be adopted. The amount of a
substance’s possessing coagulation capability can be increased by
using salt solutions (such as NaCl and CaCl2) during extraction step
(Carvalho et al., 2016; Moa Megersa et al., 2019b). For instance,
Megersa et al. (2019b) showed that the use of salt solutions (NaCl,
KNO3, and NH4Cl) could increase the coagulation performance as
compared to the Moringa coagulant extracted with water (Moa
Megersa et al., 2019b). The optimum dosage of coagulant extracted
using 0.5 M NaCl solvent was 2 mg/mL with turbidity removal ef-
ficiency of 91%. In comparison, the turbidity removal performance
of coagulant extracted using deionized water was much lower
(37%), even though its dosage was higher (4 mg/mL). Such
improvement was due to the effect of salting in as explained by
Debye-Huckel theory (increasing solvating power). The presence of
salt ionic strength increased the solubility of the proteins by
breaking down the protein-protein bond of natural coagulants
(Moa Megersa et al., 2019b; Noor et al., 2015). Subsequently, the
number of active compounds with coagulation capability (proteins)
in the extracted coagulants was higher when extracted using salt
solutions and resulted in lower optimal dosage with improved
performance. At lower coagulant dosage, the risk of residual
organic compounds in treated water would also be reduced (Moa
Megersa et al., 2019b). The type of solvent used in the extraction
process would also bring additional benefits to the coagulation
process. Carvalho et al. (2016) observed that Moringa coagulant
extracted with CaCl2 attained higher turbidity removal efficiency as
compared to NaCl solvent, which could be attributed to the
participation of calcium ions in coagulation process (Carvalho et al.,
2016). The positively charged calcium ions compressed the diffuse
layer of the electric double layer of impurities present in water,
weakening the repulsion between impurities and facilitating better
coagulation process.
Apart from increasing the yield (number of compounds with
coagulation capability) of extraction, the purity of the natural co-
agulants can also be improved to reduce the impurities and coag-
ulant dosage. The organic compounds in the natural coagulants
that do not take part in coagulation process will possibly end up in
the treated water as dissolved organic matter (Sa nchez-Martín
et al., 2010). The presence of these organic residues is unwanted
as it will cause bacteria regrowth in the water and serve as sub-
strate for the formation of hazardous disinfection by-products (Jerri
et al., 2012; Kalibbala et al., 2009). Hence, the extracted natural
5
coagulants must be purified to avoid such undesirable effects from
using natural coagulants. The first step of purification is removing
the oil content in the natural coagulant extract through the use of
suitable solvents such as hexane and ethanol (Hoa and Hue, 2018;
Megersa et al., 2017). Hoa and Hue (2018) have shown that purifi-
cation with n-hexane solution managed to reduce the lipid content
of Moringa oleifera seed extract down from 35% to 2% (Hoa and Hue,
2018). The decrease in lipid content enhanced the turbidity and
COD removal efficiencies of the purified natural coagulant since the
oil component did not help in coagulation process and would, on
the other hand, add to the impurities in the water.
After the removal of oil content, the natural coagulant extract
can be further purified to obtain final product concentrated with
active coagulation compounds via various purification processes
such as dialysis, ultrafiltration, lyophilization, chemical precipita-
tion, and ion exchange (Baptista et al., 2015; Choudhary and Neogi,
2017; Dezfooli et al., 2016; M. Megersa et al., 2019; S
anchez-Martín
et al., 2010). S
anchez-Martín et al. (2010) investigated the impact of
purification extent (ion exchange chromatography using NaCl so-
lution) on the coagulation performance of Moringa extract
nchez-Martín et al., 2010). It was discovered that the optimum
(Sa
dosage of the single-step purified (elution with 0.6 M NaCl) coag-
ulant was two times higher than the two-step purified (first elution
with 0.3 M NaCl followed by second elution with 0.6 M NaCl)
coagulant in terms of turbidity removal. It was postulated that
during the first elution, proteins without coagulation capability
were removed. This led to the production of more purified coagu-
lant containing active coagulant proteins after the second elution.
Interestingly, the purified coagulant via ion exchange process per-
formed at par with the conventional alum coagulant in terms of
dosage required (1 mg/L) and turbidity removal efficiency (83%) for
natural river water (M. Megersa et al., 2019). Without further pu-
rification, the Moringa extract could only achieve 50% removal of
turbidity at the similar dosage or required four times higher dosage
for removal efficiency of 83%. This indicated that purification pro-
cess can produce natural coagulant with higher proportion of active
coagulation compounds, which subsequently leads to better per-
formance even at lower optimal dosage.
Due to the high cost associated with ion exchange chromatog-
raphy, researchers have sought alternative purification approaches
that are more economically viable at industrial level. A relatively
simple chemical precipitation (using ammonium sulphate) of
compounds possessing coagulation activity have been proposed for
the purification of Moringa extract (Choudhary and Neogi, 2017;
Dezfooli et al., 2016). Choudhary and Neogi (2017) reported that the
natural Moringa extract isolated using 30e60% and 60e80% satu-
rated ammonium sulphate exhibited superior turbidity removal
efficiency with a slightly better performance as compared to alum
(Choudhary and Neogi, 2017). In addition, the purified natural
coagulant did not affect nor change the pH of the treated water, an
observation that alum coagulant failed to uphold since it reduced
the pH to acidic condition. Hence, the presence of a simple and
effective isolation and purification method for natural Moringa
extract could potentially help to produce natural coagulant with
great coagulation activity.
Similarly, extraction conditions such as temperature, acidity,
and solvent will affect the yield of the compounds responsible for
coagulation from the natural sources (e.g. garden cress, Basil seeds,
and cactus) (Adjeroud et al., 2018; Lim et al., 2018; Nazir et al.,
2017). Generally, these compounds are originated from the poly-
saccharides that normally formed the plant cell wall or are present
in the form of mucilage. To release the polysaccharides during the
extraction process, the plant cell wall has to be broken. Extraction
conducted at high temperature may promote the solubilisation of
the compounds that are holding the polysaccharides and increase
6 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
the yield (Lim et al., 2018; Nazir et al., 2017). However, the tem-
perature must be controlled at the optimal level, otherwise
excessive heat might destroy the polysaccharides present in the
natural coagulant and subsequently reduce the mucilage yield.
Acidic extraction environment may also facilitate the breakdown of
cell wall and release the coagulating compounds (Colodel et al.,
2017). The use of appropriate solvent such as acetone can
enhance the extraction efficiency of mucilage and enable the
extraction yield in larger quantity be carried out with minimal
amount of solvent used (Kilor, 2014; Lim et al., 2018). Judging from
the variance of extraction conditions, investigation on the influence
of these factors should be conducted to ensure the maximum
extraction of active coagulation compounds from the natural
sources.
The extraction and purification processes of natural coagulants
from other plant sources (e.g. seeds of Plantago, Phaseolus vulgaris,
chestnut, Ocimum basilicum, Quercus robur, and Hibiscus or cactus
pads from Opuntia species) are almost similar with the procedures
involved in the production of Moringa coagulant (Antov et al., 2018,
2012, 2010; Chaibakhsh et al., 2014; Ndahi and Bridgeman, 2019;


Sciban et al., 2009; Shamsnejati et al., 2015; Taylor et al., 2014; Wan
et al., 2019). In general, the extraction and purification of all plant-
based natural coagulants (including Moringa) are based on three
stages, as shown in Fig. 3 (Yin, 2010). The first stage involves pre-
processing of the sample where it is cleaned and converted into
the form (normally in fine powder) suitable for second stage. In the
second stage, the compounds possessing coagulation activity are
extracted using water, salt solution, or appropriate solvent. The
third stage is the purification where only the compounds truly
contributing to coagulation process are purified. Regardless of the
plant, the compounds contributing to coagulation activity are
either polysaccharide or protein present in the extract. The coag-
ulation performance efficiency depends on the purity of the active
compounds. However, the extent of study for the natural coagulant
stated above is not as intensive and thorough as compared to
Moringa coagulant. The influence of the extraction and purification
factors on the coagulation performance for those natural co-
agulants is not being covered in depth. Indeed, extracts taken from
numerous number of natural plants reportedly possess coagulation
capability, as reported in the past literature reviews (Choy et al.,
2014; Oladoja, 2015; Saleem and Bachmann, 2019b). Most of
these studies stopped at showing the coagulation capability, and
further pursuit for optimization and in-depth understanding on the
natural coagulants has been scarce. Having said that, to promote
the widespread use of natural coagulant, intensive study on the
exploration of suitable method of extraction and purification of the
crude extract is required to eliminate the non-active components
and to know the nature and characteristics of the active component
in the natural coagulants.
In comparison to natural coagulant from plant-based sources,
chitosan is commercially extracted from crustacean shells (shrimp,
crab, crayfish, and krill) (Kumari et al., 2017). To separate chitin
(chitosan is deacetylated derivative of chitin) from crustacean
shells, chemical processing steps such as demineralization (with
hydrochloric acid) and deproteinization (with sodium hydroxide)
are usually applied to remove calcium carbonate and proteins (the
Fig. 3. General processing steps in the production of natural coagulant from plant-based sources (Yin, 2010).
main components of shells), respectively (Bakshia et al., 2019).
However, these processes normally take a long duration and
require high operating temperature which might decrease the
quality of the chitosan. Also, chemical processing steps cause sec-
ondary waste from the excessive usage of acid and alkali solutions
(Abdou et al., 2008). Physical auxiliary methods (such as ultra-
sound, irradiation, compressional puffing-pretreatment, micro-
wave radiation, and freezing/thawing) have been proposed to
minimize the adverse impacts of chemical processing steps while at
the same time improving the quality and purity of extracted chi-
tosan (Huang et al., 2018, 2019; Nouri et al., 2016; Rashid et al.,
2012; Soria and Villamiel, 2010). For instance, ultrasound applied
to the solution during demineralization increased the contact be-
tween crustacean shells and acid, helping to shorten the extraction
time and produce less crystalline chitin for better conversion to
chitosan (Soria and Villamiel, 2010). Microwave radiation on the
other hand accelerated the reaction time during deproteinization
which could potentially cut down the extraction cost of chitosan
(Nouri et al., 2016). Though the proposed auxiliary methods
exhibited advantages including simple, environmentally friendly,
and improvement of product quality, the large-scale extraction
remains as chemical processing since it is less complicated and has
been well-established. Hence, further upscaling study on the
costing associated with auxiliary methods should be conducted to
verify the benefits of advanced extraction and purification of chi-
tosan from crustacean shells.
3.3. Modification for improved performance
Although natural coagulants possess several advantages as
compared to conventional coagulants, there remains few issues
that need to be resolved before the water and wastewater utility
industries are convinced to adopt it in their operation. The concerns
include low solubility in water, narrow working window of pH
range, undesirable isoelectric point, weak surface charge, low sta-
bility (shelf life), and moderate efficiency (translated to higher
working dosage and cost) (Lee et al., 2014; Salehizadeh et al., 2018).
Unlike inorganic coagulants (e.g. FeCl3 and alum), natural co-
agulants do not have the ability to hydrolyze in water to form
strongly charged hydroxides for the removal of impurities. How-
ever, the reactive functional groups (e.g. hydroxyl, amino, and
carboxyl) of the natural coagulants itself offer the opportunity for
modification that could help to resolve the aforementioned con-
cerns (Ghimici and Nichifor, 2018). Various compounds that could
significantly enhance the coagulation performance of natural co-
agulants can be introduced onto the coagulants through interaction
with these functional groups. Plentiful of modification efforts
(incorporation of useful compounds) have been carried out to
remedy the weaknesses of natural coagulants. Promising results
have been reported where the synthetically modified natural co-
agulants possess greater versatility and capability in coagulation
process. In general, chemical reactions such as graft co-
polymerization, crosslinking with aldehyde, esterification, ether-
ification, amination, carboxyalkylation, hydroxyalkylation, and
condensation have been adopted to improve the characteristics of
natural coagulant (Salehizadeh et al., 2018). In this section,
 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
examples of natural coagulants modification will be discussed
where highlight is given to how the modification could lead to
improvement of coagulation performance. Details of modification
(synthesis methodology and reaction conditions) are not within the
review scope of this manuscript and thus would not be discussed
in-depth.
Among the natural coagulants, chitosan has received much
attention for modification studies. Chitosan is a polysaccharide
polymer which is soluble only in dilute acidic solutions (pH
5). Its
coagulation performance is also greatly affected by pH where the
efficient removal of negatively charged impurities is limited within
a narrow pH range (pH
6) (Renault et al., 2009). Poor water-
solubility and limited working pH range have restricted the appli-
cation of raw chitosan in coagulation process since the pH of water
and wastewater may be neutral or alkaline, reducing the removal
effectiveness of negatively charged impurities. To overcome these
weaknesses, modification on the structures and functional groups
of chitosan can be conducted. Past studies have revealed that the
introduction of certain functional groups onto the chitosan not only
improved the solubility and broadened the working pH range in
water, but also enhanced its adsorption capacity to bind the im-
purities in water sources (Yang et al., 2016).
Dong et al. (2014) reported several interesting findings on
quarternized carboxymethyl chitosan, a modified chitosan for
coagulation/flocculation process (Dong et al., 2014). The introduc-
tion of carboxymethyl and grafting of quarternary ammonium
groups ((3-chloro-2-hydroxypropy)-trimethylammonium chlo-
ride) onto the chitosan backbone has destroyed the ordered
structure of chitosan, giving the new coagulant an amorphous
feature. Apart from the morphological changes, the presence of
positively charged quarternary ammonium groups has shifted the
isoelectric point of modified chitosan coagulant to beyond pH 9, as
compared to pristine chitosan at pH 6.0e6.5. This indicated that the
applicability of modified chitosan coagulant has been extended to
alkaline water sources (e.g. algal bloom water), eliminating the
need for pH adjustment. Also, the water solubility of the modified
chitosan was remarkably improved, covering almost the whole pH
range (except near its isoelectric point). The combination of
elevated isoelectric point, improved water solubility, and presence
of abundant positively charged functional groups (-NH2, eOH, and
eCOOH) has granted the modified chitosan coagulant better per-
formance in the removal of algal as compared to unmodified chi-
tosan and commercial coagulants such as aluminum sulphate and
ferric chloride. The modified chitosan coagulant reportedly out-
performed the rest with lower optimal dosage (as much as 200
times lesser than aluminum sulphate to achieve the same removal
efficiency) and better flocs quality (faster growth rate and larger
flocs size). All these improvements can be literally translated to
potential minimization of water treatment cost. Hence, appropriate
modification on the structures of chitosan can overcome the
drawbacks normally associated with natural coagulant while at the
same time is as competent as conventional coagulant.
On another note, the coagulation capability of chitosan can be
fine-tuned by modifying its structural properties during the syn-
thesis process. The two most important structural factors that have
significant influence on the coagulation mechanism and perfor-
mance of chitosan coagulant are the degree of deacetylation and its
molecular weight (Yang et al., 2016). The degree of deacetylation
will affect the number of eNH2 functional groups present on chi-
tosan backbone polymer, which determines the charge density and
thus directly influences the efficiency of charge neutralization
(coagulation mechanism). The molecular weight of chitosan is
accounted for the morphology and conformation of the polymer
chain in aqueous medium, which contributes to the capability of
bridging and sweeping coagulation mechanisms. In general, the
7
higher the degree of deacetylation and molecular weight, the better
the coagulation capability of chitosan. For instance, the removal of
turbidity was reported to be increased with the degree of deace-
tylation and molecular weight of chitosan (Chung, 2006; Li et al.,
2013). The increase in the number of eNH3þ functional groups
enabled the chitosan to interact and bind with the negatively
charged suspended solids through charge neutralization while the
longer polymer chain contributed to the flexibility and conforma-
tion of chitosan, allowing it to entrap more suspended particles and
subsequently form larger flocs for removal. Nonetheless, the sig-
nificance of these structural properties might vary depending on
the constituents of water (inorganic and organic pollutants, and
microorganism) and environmental factors (e.g. pH, ionic strength,
and temperature), given that the charge density and conformation
of the chitosan polymer may be heavily affected by those factors.
Similar to chitosan, starch is considered as one of the low-cost
natural polymeric materials that possesses great potential as nat-
ural coagulant for water treatment. Yet, starch coagulant faces the
same issues as chitosan: low water solubility and weak negative
surface charge. The precedent success of chitosan modification can
also be applied for starch-based coagulant. Huang et al. (2017) has
shown that the positive surface charge of starch could be signifi-
cantly elevated by grafting quaternary ammonium salt groups ((2-
methacryloyloxyethyl) trimethylammonium chloride) onto the
starch polymer backbone (Huang et al., 2017). The cationic qua-
ternary ammonium salt groups significantly elevated the surface
charge of starch from negatively charged (less than 0 mV within pH
range of 2e12) to positively charged (>30 mV within the same pH
range). The highly positively charged characteristics is desired for
many coagulants, given that most inorganic suspended colloidal
particles possess negative surface charge. Additional improvement
associated with the grafting on starch was the extension of soluble
pH range and creation of comb-like polymer structures. These
indicated that the number of effective coagulant sites exposed to
the suspended solids would also be increased, and the removal
capability of suspended particles through charge neutralization and
enmeshment would also be strengthened. Consequently, only low
doses (0.5e0.7 ppm) of the modified starch coagulant was required
for the efficient removal (>98%) of kaolin suspension solution
(1000 ppm; pH 2e11) (Huang et al., 2017).
Apart from the ubiquitous use of plant-based natural co-
agulants, dextran, a bio-polysaccharide-based coagulant produced
with sucrose as substrate and dextransucrase enzyme (extracted
from bacteria) has emerged as an environmentally friendly coag-
ulant in wastewater treatment. However, dextran coagulant en-
counters the same issues as chitosan, where its low solubility and
hydrophilicity has limited its application potential. To improve the
water solubility of dextran, Li et al. (2016)a,b grafted acrylamino
and carboxyl groups onto the dextran backbone (Li et al. 2016a,b).
The introduction of hydrophilic groups (-CONH2 and eCOO-)
improved the water solubility of the modified dextran coagulant
(>40 times better than pristine dextran) and at the same time
granted the coagulant negative surface charge. Interestingly, this
anionic coagulant was effective in removing positively charged
pollutant, where 96% of turbidity (hematite; 2500 ppm concen-
tration) was successfully removed as compared to 30% removal
with unmodified dextran coagulant. This indicated that with the
right formulation of modification, the natural coagulant can be
fine-tuned to remove positively charged pollutants, effectively
broadening the application window of coagulation since most of
the suspended solids for removal are negatively charged (Sillanpa €€
a
et al., 2018).
One interesting work conducted by Ge at el. (2016) has shown
that crystalline nanocellulose could be modified with 1-(3-
aminopropyl)imidazole to possess reversible capability for
8 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
harvesting of microalgae (Ge et al., 2016). The introduction of CO2
into the solution would lower the water pH and subsequently
protonate the imidazole functional groups to become positively
charged, which would then interact with the negatively charged
microalgae. After the CO2 treatment, the water sources would be
exposed to air sparging to trigger the gelation between the modi-
fied nanocellulose coagulants (removal of CO2 would reduce the
dispersibility of the coagulants), which would also enmesh the
adjacent microalgae and/or aggregates of microalgae-modified
nanocellulose. The CO2 and air sparging altered the characteris-
tics of the modified coagulants to facilitate the interaction between
the coagulants and microalgae, formation of agglomerates, and
removal via settling. It was reported that the modified nano-
cellulose coagulants had little effect on microalgae cells growth,
indicating its biocompatibility. Also, the coagulants could be re-
dispersed in the suspension through CO2 sparging and reused for
microalgae harvesting. This implied that the modified coagulants
has the potential to provide a sustainable solution for microalgal
harvesting or removal as it can be recycled by controlling the CO2/
air sparging treatment that has direct impact on the interaction
between coagulants and microalgae.
The modification of natural coagulants is not limited to the
production of cationic coagulants (extending the pH range of pos-
itive charge beyond neutral pH) for the removal of anionic impu-
rities (e.g. natural organic matter) but also catering for the cationic
impurities (e.g. cationic heavy metals and dyes) (Chaouf et al., 2019;
Song et al., 2011; Yang et al., 2013). For instance, acrylamide has
been successfully grafted to the cellulose and hydroxyethyl cellu-
lose (modified form of cellulose) and granted it negative charge at
pH above 3, which easily exceeded 45 mV above pH 7 (Chaouf
et al., 2019; Song et al., 2011). Such a negatively charged property
enabled the modified natural coagulants to remove positively
charged pollutants. Chaouf et al. (2019) showed that the
acrylamide-modified hydroxyethyl cellulose could remove 99% of
positively charged ferric hydroxide colloidal particles and achieve
excellent removal capacity of copper (II) ions heavy metal at
400 mg g1, which was difficult for the unmodified cellulose nat-
ural coagulant to remove (Chaouf et al., 2019). The improvement of
coagulation capability could be attributed to the saponification of
the amide group on the modified natural coagulant, which led to
the formation of carboxylate that could deprotonate to become
negatively charged in solution. This development enabled the
modified cellulose coagulant to acquire positive charge and sub-
sequently favoring it for the removal of cationic impurities through
strengthened charge neutralization coagulation mechanism.
Table 1 presents a few examples of modified natural coagulants
with various modifying agents. As can be observed from the table,
chitosan is the trendy natural coagulant that has been frequently
modified for coagulation performance evaluation. Indeed, a quick
search in SCOPUS database revealed that majority of the modified
natural coagulants involved chitosan. This article did not intend to
downplay the role and potential of other natural coagulants, as
modification studies have also been conducted on oatmeal, sodium
alginate, xylan, agar, and seed gum (Bharti et al., 2013; G. U. Rani
et al., 2013; P. Rani et al., 2013; Sanghi et al., 2007; S. Wang et al.,
2015a,b). However, the fact that chitosan attracted most of the re-
searchers’ attention reveals the versatility of chitosan as natural
coagulant. As shown in Fig. 4, chitosan possesses eOH and eNH2
functional groups that could readily react with modifying agents to
obtain improved characteristics for more efficient coagulation
process (Momeni et al., 2018). The long polysaccharide backbone
provides numerous active sites for modification, in which other
natural coagulants are found either to be falling short or the exact
components responsible for coagulation have been difficult to be
identified. This explains the shortage of modification studies on
certain natural coagulants since they do not own the plentiful
active sites for interaction with modifying agents. On the other
hand, though starch, dextran, and cellulose comprised long poly-
saccharide chain, both are deficit of eNH2 functional group (as
shown in Fig. 4). Subsequently, the versatility of those materials as
natural coagulants has been discounted and less effective as
compared to chitosan. The few popularly modification agents that
frequently used to enhance the performance of natural coagulants
are displayed in Fig. 5. Some modifications involve several modi-
fying agents while some only need one. Overall, the functional
groups on the natural coagulants (eOH and eNH2 functional
groups) are responsible to react with the modifying agents for
improved performance.
3.4. Hybridization with inorganic or other types of coagulants
As previously mentioned, under certain circumstances, natural
coagulant might not be as effective as compared to conventional
inorganic coagulants. However, the environmental benefits of
natural coagulants could not be neglected. To harness the benefits
of natural coagulants without sacrificing the treatment efficiency,
apart from the chemical modification discussed in the previous
section, the natural coagulants could be mixed or used together
with other types of coagulants (normally inorganic types). This
strategy can be accomplished in two ways: dual coagulant or
composite coagulant and coagulant aid (Mohd-Salleh et al., 2019;
Oladoja, 2016). The former is produced by combining two types of
coagulants as a single working composite coagulant, while coagu-
lant aid is the materials used as an auxiliary to the primary coag-
ulant (adding some time after the dosing of primary coagulant).
These approaches will help to enhance the treatment efficiency,
speed up the formation and improve the strength of flocs, and thus
minimizing the consumption of non-renewable counterpart co-
agulants (especially chemical coagulants) as well as its associated
adverse environmental and cost impacts (Mirroshandel et al.,
2016). Hybridization between synthetic or non-natural coagulants
have been widely reported but the focus in this section is the hy-
bridization that involves the use of natural materials (Lee et al.,
2012).
Ma et al. (2016) prepared a composite coagulant comprised
chitosan and aluminum chloride by mixing the two coagulants
together in solution Ma et al. (2016). The composite coagulant
outperformed the individual coagulation process by achieving the
optimal removal efficiency of M. aeruginosa (a harmful cyanobac-
terium that can produce toxins which adversely affect aquatic
ecosystems and human) with lower dosage. It was reported that the
polymer chains of chitosan and the steric crowding of aluminum
hydroxide precipitates gave rise to entrapment and bridging
mechanisms for the removal of M. aeruginosa. Both the components
of the composite coagulant exerted little or probably no stress on
the cells, indicating that negligible of cell damage occurred during
the coagulation process. In addition, the composite coagulant could
effectively remove extracellular organic matter. This was beneficial
as it indicates that the risk of disinfection by-products formation
during subsequent disinfection process would also be lessened.
Overall, the combination of natural coagulant (chitosan) with the
conventional coagulant (aluminum chloride) has proven to be an
effective treatment process for the removal of harmful cyanobac-
teria which is normally found in highly eutrophic (polluted) water.
Apart from being combined into composite coagulant, the
popular natural coagulant e chitosan e has also been used as
coagulant aid for wastewater treatment. The use of chitosan as
coagulant aid to aluminum-based primary coagulant has enhanced
the removal efficiency of dye pollutants by 5e60%, especially at
lower dosage of aluminum coagulant (Wang et al., 2017). This could
 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267 9

Table 1
Modified natural coagulants with various modifying agents and associated improvement in performance.

No. Natural coagulants Modifying agents Remarks & Improvement Ref.

1 Chitosan
2 Cellulose (flocculation
characteristics of
polyacrylamide grafted)
3 Guar gum (Flocculation Acrylamide
properties of polyacrylamide
grafted)
4 Starch (flocculation of both
kaolin and hematite)
5 Chitosan (preparation of
mercaptoacetyl)
6 Starch (graft copolymeric
flocculant)
7 Dextran (dextran derivatives Cationic: Pendent quaternary
application)
8 Chitosan (synthesis and
characterization of chitosan)
Acrylamide
Acrylamide
(2-hydroxypropyl)
trimethylammonium chloride
Mercaptoacetic acid
Acrylamide and 2-
(methacryloyloxy) ethyl
trimethylammonium chloride
ammonium groups
Anionic: Monobasic phosphate
groups, acrylamide and sodium
acrylate
N-methyl piperazinium chloride
Grafted chitosan possessed rough, porous, and loose structures. Meanwhile, the Ma et al. (2016)
isoelectric point has been shifted to pH 8. All these changes were favorable for
improved contaminants removal through charge neutralization. The highly-
branched grafted polymer also promoted the formation of larger and shear-
resistance flocs, facilitating better sedimentation process.
The polyacrylamide chains were grafted onto the rigid polysaccharide backbone Das et al. (2013)
of cellulose, which gave rise to branching structures with larger hydrodynamic
volume for the modified cellulose-based coagulant. This structure made the
capture of contaminants (kaolin and iron ore) easier and more efficient for the
modified coagulant (two to three times better than pristine cellulose).
The grafting of polyacrylamide on the guar gum increased the molecular weight Pal et al. (2011)
and gyration radius of the coagulant as compared to pristine guar gum. These
two features improved the approachability of the contaminants (municipal
sewage wastewater and synthetic water consisted of kaolin suspension and
methylene blue dye) towards the coagulant, thereby increasing the removal
efficiency (three to four times better than pristine guar gum).
The starch was chemically modified into cationic and anionic modified starch- Li et al. (2015)
based coagulant using the same modifiers but with different ratio (amount). The
structural characteristics differences between both coagulants (carboxymethyl
and anionic groups on the starch backbone) acted oppositely under different pH
conditions. Consequently, the cationic coagulant showed excellent removal of
negatively charged kaolin particles while performing poorly in the removal of
positively charged hematite suspension. Similar observation was encountered
by anionic starch coagulant but the effective removal was towards the positively
charged hematite.
The incorporation of mercaptoacetic acid improved the water solubility of Zhang et al.
chitosan up to pH 11 and enhanced the removal of copper (several times better (2015)
than pristine chitosan). This could be associated to the presence of mercapto-
group that helped to chelate the copper on top of the reaction between eNH2
and copper.
Owing to the branching nature and high gyration radius (3226 nm), the binary- Das et al. (2019)
grafted starch coagulant acquired improved approachability of contaminants
(blast furnace effluent), resulting in better removal efficiency as compared to
commercial product.
Charge neutralization is one of the most important mechanisms for Ghimici and
contaminants removal in coagulation process. Often, coagulants are modified to Nichifor (2018)
possess charge opposite of contaminants for efficient removal. In this case, the
versatility of dextran was demonstrated where it can be modified with different
compounds to possess the desired cationic or anionic charges.
High cationic charge N-methyl piperazinium chloride was grafted on the Dharani and
chitosan backbone, resulting in improved water solubility, irregular structure Balasubramanian
(which could be attributed to the branching effects) and improved thermal (2015)
stability of chitosan (up from 270  C to 440  C). The grafted chitosan recorded
lower (up to 50%) optimal dosage for the removal of bentonite (500 ppm) over a
wide range of pH (4e10). The modified chitosan performed well even under
alkaline solution, which could be attributed to the presence of cationic
quaternary ammonium groups in N-methyl piperazinium.

be attributed to the strong interaction between chitosan and
aluminum-dye aggregates. The long chain structure of chitosan
with abundance of amino groups could interact with the aluminum
aggregates through charge neutralization mechanism, which
would bind the small aggregates to form larger flocs. The bridging
between the flocs via chitosan would increase the flocs size and
strength, the characteristics desired for effective coagulation and
sedimentation processes.
Alum, being one of the most widely used inorganic coagulants in
water and wastewater treatment, has been a concern for public as it
is tied to the dispute of whether or not it causes Alzheimer disease.
Natural coagulant aid can be used to reduce the consumption of
alum coagulant as part of the effort to phase out the use of alum in
the future. Natural seed gum extracted from Cassia obtusifolia seeds
has shown promising potential as a coagulant aid to cut down the
consumption of alum in the treatment of palm oil mill effluent, an
abundant agricultural effluent discharged from the oil palm
extraction mills. Shak and Wu (2015) reported that the amount of
alum used for optimal treatment efficiency has been cut down by
55% (2.57 g/L to 1.15 g/L) with the inclusion of natural seed gum as
coagulant aid (Shak and Wu, 2015). Owing to the high molecular
weight and polymeric structure of natural seed gum, more impu-
rities would be adsorbed onto the coagulant aid while at the same
time the formation of larger aggregates would be promoted
through bridging mechanism. These characteristics have made it
possible to compensate for the reduction of alum consumption. The
combined treatment revealed that the use of natural coagulant aid
could significantly reduce the consumption of chemical coagulants
and similar trend should be explored for other types of water
sources.
Study conducted by Wu et al. (2012) had shown the benefits of
having coagulant aid (sodium alginate) for the treatment of dying
wastewater (synthetic and real) with alum as the primary coagu-
lant (Wu et al., 2012). Their findings showed that not only had the
addition of sodium alginate as coagulant aid improved the overall
color removal efficiency, but the synergistic improvement (with
1 ppm of sodium alginate) decreased the dosage of alum (4.5 ppm)
required for the same treatment efficiency when alum (6 ppm) was
used alone. The reduction of alum consumption could potentially
cut down the costs (coagulant and sludge handling) and minimize
10 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267

Fig. 4. Molecular structures of (a) chitosan, (b) cellulose, (c) starch, (d) dextran (e) guar gum (f) lignin (Ghimici and Nichifor, 2018; Gupta and Variyar, 2018; Li et al., 2015; R. Li et al.
(2016)a,b; Momeni et al., 2018; Vuoti et al., 2018).

Fig. 5. Molecular structures of various modifying agents: (a) (3-chloro 2-hydroxypropyl) trimethylammonium chloride (Momeni et al., 2018); (b) acrylamide (Hasan and Fatehi,
2018) (c) (2-methacryloyloxyethyl) trimethylammonium chloride (Hasan and Fatehi, 2018) (d) sodium acrylate (Li et al., 2016a,b) (e) mercaptoacetic acid (Zhang et al., 2015) (f)
N-methyl piperazine (Dharani and Balasubramanian, 2015) (g) methyl methacrylate (P. Rani et al., 2013) (h) N,N-Dimethylacrylamide (Kolya and Tripathy, 2013) (i) 2-acrylamino-2-
methyl-1-propanesulfonic acid (Tang et al., 2020) (j) poly (N-vinylcaprolactam) with carboxyl end.
 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
the environmental impacts arising from alum coagulant. The
bridging ability of sodium alginate reportedly facilitated the for-
mation of larger flocs with greater resistance to breakage. This
indicated that with the addition of coagulant aid, the flocs would
settle down quicker than the smaller flocs formed when alum was
used alone. The short retention time coupled with larger floc size
can lead to footprint reduction of coagulation-sedimentation units
(more compact). Treatment with real dying wastewater also
observed 5e10% improvement of color removal efficiency when
sodium alginate was used as coagulant aid to alum as primary
coagulant.
In another study conducted by Wang et al., (2015)a,b, sodium
alginate was coupled with polyaluminum chloride for the removal
of copper oxide nanoparticles and humic acid (Y. Wang et al.,
2015a,b). The impacts of the presence of sodium alginate as coag-
ulant aid on the removal efficiency and subsequent ultrafiltration
membrane performance were evaluated. Generally, the addition of
coagulant aid improved the contaminants removal efficiency up to
20e30% while slightly minimizing the membrane flux decline. The
initial coagulation process involved the formation of aggregation
between the positively charged aluminum coagulant and nega-
tively charged copper oxide and humic acid contaminants. These
microflocs will then be bridged with the alginate polymers through
the carboxyl functional groups to form “egg-box” structures. These
gel networks would then sweep across the solution to entrap
remaining contaminants, which explained the improved removal
efficiency when coagulant aid was present. At the same time, the
addition of sodium alginate enlarged the floc size and minimized
the blocking of membrane pores by small particles. This showed
that natural coagulant aid can perform well in enhancing the
coagulation performance while at the same time benefiting the
downstream treatment process.
Though Moringa-based coagulant is as popular as chitosan with
numerous publications citing the usefulness as natural coagulant in
water and wastewater treatment, its hybridization use with other
types of coagulants has not been widely reported. From the few
articles relevant to this topic, Moringa-based coagulants can be
used together with aluminium sulphate in both ways, either mixed
together or dose prior or after the dosing of alum. Ghebremichael
et al. (2009) reported that dosing the natural coagulant prior
alum would result in better removal of turbidity (20% increment)
and dissolved organic carbon (Ghebremichael et al., 2009).
Exposing the Moringa coagulant to high turbidity water would
facilitate the formation of micro-flocs, which would then be
entrapped and adsorbed easily to the aluminium hydroxide pre-
cipitates. Furthermore, the use of natural coagulant aid reduced the
alum dosage by about 50e75%.
Similar benefits (higher turbidity removal and reduced alum
consumption) can also been achieved by dosing both alum and
Moringa coagulants together (De Paula et al., 2014). In contrast,
Freitas et al. (2016) highlighted that dosing the Moringa coagulant
after alum would result in better turbidity reduction capacity
compared to dosing both together (Freitas et al., 2016). It was
postulated that when both were dosed together, the natural coag-
ulant would interact with both suspended particles and aluminium
ions. This reduced the available aluminium ions for the formation
and removal of suspended particles. On the other hand, dosing the
Moringa coagulant after alum would not disrupt the coagulation
activity by alum. Instead, the natural coagulant helped to promote
the formation of larger flocs for removal and at the same time
reduce the amount of aluminium residue in the treated water
(0.3 mg/L as compared to 35.5 mg/L using alum only). This dem-
onstrates that the dosing sequence and hybridization mode for the
incorporation of natural coagulants with conventional coagulants
have to be designed properly as the combination may perform
11
differently according to the type of water sources.
Alternative to chemical-dosing coagulation process is the elec-
trocoagulation that generates coagulating compounds from
oxidation of metallic electrodes. Electrocoagulation has also been
studied extensively for the treatment of various wastewater and it
shares the same concern as chemical coagulation process e highly
reliant on ferric and aluminum-based electrodes that form hy-
droxides for the removal of impurities in water sources. The sludge
produced and the excessive coagulants in the treated water will
then become an issue for the plant operators due to the presence of
metallic compounds. Hence, to reduce the consumption and pro-
duction of excessive coagulating compounds, natural coagulant aid
can also be applied to assist the operation of electrocoagulation
process. Adjeroud et al. (2015) evaluated the performance of elec-
trocoagulation process with and without the presence of cactus
juice (coagulant aid) for the removal of turbidity in synthetic
wastewater (Adjeroud et al., 2015). It was found that the cactus
juice significantly enhanced the turbidity removal by 15% as
compared to 72% of removal efficiency without the coagulant aid.
The improvement was made possible through adsorption mecha-
nism where the charged sugars content in cactus juice could
potentially interact with cations (coagulants from electrodes) that
were binding the suspended particles in the solution. This shows
that not only natural coagulants can be coagulant aid for chemical
coagulation but also can benefit the electrocoagulation process,
indicating the versatility of natural coagulants.
Apart from the popular natural coagulants such as chitosan and
Moringa, other natural materials that do not perform well as
coagulant individually still possess the potential to be used in water
and wastewater treatment process as coagulant aid or in the form
of composite coagulant. Few common examples of these materials
include, but not limited to, lignin, starch, green algae, and cactus
mucilage (Guo et al., 2018; R. Li et al., 2016a,b; Luo et al., 2018;
Mirroshandel et al., 2016; Xue et al., 2019; Zhou et al., 2019).
Basically, these coagulant aids strengthened the flocs through
charge neutralization and bridging interactions with the flocs
formed by primary coagulant. Subsequently, the treatment effi-
ciency has been improved and the dosage of primary coagulant has
been reduced too. This could bring a significant benefit as the re-
sidual coagulant such as Al could be minimized. Overall, natural
coagulant aids or composite coagulants demonstrate the way to
utilize the natural materials while at the same time resolving the
issues of excessive dependent on inorganic coagulants. As ex-
pected, chitosan still monopolizes the field of coagulant aid or
composite coagulant due to its versatility (structures and functional
groups) to work together with inorganic coagulants.
3.5. Multifunctional natural coagulants
There are plenty of reports on the use of natural coagulants for
the removal of suspended particles and natural organic matter
€€
(Sillanpa a et al., 2018). However, the application of natural co-
agulants for the removal of dissolved pollutants such as heavy
metals, nutrients, and trace organic compounds or emerging con-
taminants has not received as much attention as suspended solids
and natural organic matter. This could be attributed to the nature of
coagulants, which is effective for the removal of larger particles
through charge interaction and bridging mechanism. Unlike ad-
sorbents, coagulants do not possess a solid medium that provides
an abundance of surface areas for entrapment of soluble impurities
through physical or chemical adsorption mechanisms via van der
Waals forces of interaction, electrostatic attraction, p-p in-
teractions, hydrophobic interactions, and electron sharing (Sophia
A. and Lima, 2018). Hence, natural coagulants normally recorded
poor removal performance of dissolved contaminants (Teh et al.,
12 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
2016; Xue et al., 2019).
Another unneglectable fact is that real water sources contain a
vast amount of impurities, which typically requires several treat-
ment technologies to remove all the pollutants since conventional
treatment processes normally possess single functionality (target-
ing single type of pollutant). This has resulted in the need for high
capital and operation costs, complicated devices, lengthy process,
and energy and labor-intensive operations (Pintilie et al., 2016). In
conjunction with process intensification, incorporating other rele-
vant functionalities capability onto the coagulants may produce a
new generation of multifunctional coagulants that are capable to
remove various types of pollutants and at the same time perform
several functions, making the water and wastewater treatment
processes more compact and efficient in terms of performance and
costs (Tayalia and Vijaysai, 2012). Also, highlighting the capability
of natural coagulant in removing multiple pollutants coexisting in
the water sources will help to convince the water operators about
the real potential of natural coagulant. In view of this, the study on
the synthesis of multifunctional natural coagulants and the
demonstration of multi-functionality of natural coagulants could
help to achieve these targets.
Heavy metals are dissolved ions normally found in industrial
wastewater and required to be removed during the treatment
process. Coagulation process, regardless of conventional metallic
coagulants or natural coagulants, has poor capability to remove the
soluble heavy metals efficiently from the water sources (Lee et al.,
2014; Sun et al., 2019). Consequently, the coagulation process
must be integrated with other treatment units to ensure the total
removal of heavy metals (or any dissolved pollutants) from the
wastewater (Lee et al., 2014). To improve the capability of the
natural coagulant in removing multiple pollutants, certain func-
tional groups possessing high heavy metals affinities can be
incorporated into the molecular chain of coagulant. For instance,
dithiocarboxy group (eC (¼S)eS-) has a strong affinity for heavy
metal ions and can form stable chelate precipitates for the removal
heavy metal ions from water sources (Zhu et al., 2019). Yang et al.
(2018) introduced the dithiocarboxy group to the eOH functional
group on chitosan to produce xanthated chitosan with both coag-
ulation and chelation capabilities. It was reported that both the
coexisting copper (heavy metal) and kaolin (turbidity) were suc-
cessfully removed, with the presence of turbidity helping to in-
crease the removal rate of copper ions from 92% to 94%. This
observation could be attributed to the formation of flocs (coagu-
lation) that swept across the solution (sweeping mechanism) and
captured more insoluble chelating precipitates (formed between
the negatively charged dithiocarboxy groups and positively
charged copper ions through coordination/chelation mechanism).
Similar observation has been reported by Sun et al. (2019) where
heavy metal chelating functional groups grafted onto chitosan
enabled it to remove copper, chromium, nickel ions coexisting in
the synthetic water through chelation process (Sun et al., 2019). The
chelated heavy metals would form precipitates which were then
removed via coagulation sweeping mechanism in the form of flocs.
Antibiotic is another contaminant that coagulants have limited
removal efficiency due to the weak interaction between both
components. Past study has shown that in the co-existence of
copper ions, antibiotic could be removed indirectly by chitosan
coagulant. The antibiotic was embedded in copper hydroxides via
coordination effect where this composite was subsequently
removed by chitosan through charge neutralization and coordina-
tion between chitosan and copper hydroxide (Zhang et al., 2014). Jia
et al. (2016) introduced functional groups with large p-electron
clouds onto chitosan with the aim to establish direct interaction
between antibiotic (many antibiotics possess aromatic rings with
large p-electron clouds molecular structures) and chitosan
coagulant (Jia et al., 2016). It was discovered that the modified
chitosan recorded much better removal efficiency for both copper
ions and antibiotic coexisting in the solution as compared to pris-
tine chitosan under the same experimental conditions. It was
postulated that the improvement was due to the presence of p-p
stacking between the positively charged triazine rings in the
modified chitosan and the negatively charged aromatic rings in
antibiotics. The establishment of this interaction enhanced the
removal of antibiotics, in addition to being removed through
embedment in copper hydroxide.
The bacteria present in the water are required to be disinfected,
with higher bacterial density requiring larger dosage of disinfec-
tants. The dosage of large amount of disinfectants may increase the
risk of the formation of disinfection byproducts, which is harmful to
human health (Yang et al., 2014). Hence, it may be helpful if the
natural coagulant can remove both suspended solids and bacteria,
which to a certain extent may reduce the dosage requirement of
disinfectants and potentially simplify the whole treatment process.
Hoa and Hue (2018) reported that the use of Moringa natural
coagulant removed 100% of the E. coli in lake water while sustaining
99% reduction of turbidity and COD (Hoa and Hue, 2018).
Conversely, polyaluminum chloride coagulant only achieved
40e60% removal of these impurities. The high removal of bacteria
could be associated with the high removal of suspended solids and
the cationic protein of Moringa that can potentially destroy the
E. coli cells (Shebek et al., 2015). Though the potential of natural
coagulant as bactericidal or bacteriostatic is still a disputed case, the
antibacterial property of unmodified or modified natural coagulant
(apart from being used for the removal of non-living pollutants) is
worth exploring (Huang et al., 2017; Liu et al., 2017).
The functional groups that give rise to different functionalities
can significantly improve the application efficiency of the process
and reduce the costs associated with chemical consumption. For
instance, anionic groups such as carboxyl groups and sulfonic
groups are typically present on scale inhibitors and anionic co-
agulants. These similarities in structure indicate the potential for
the development of multifunctional coagulants with not only
coagulation functionality but also scale inhibition. Du et al. (2018)
have shown that the modified natural coagulant, poly (acrylic
acid) grafted starch exhibited both effective scale-inhibition per-
formance and high turbidity removal efficiency (Du et al., 2018). In
terms of coagulation performance, the natural coagulant as coag-
ulant aid for polyaluminum chloride reduced the dose of the latter
chemical by more than 30% while improving the flocs formation
and settling efficiency. On the other hand, the carboxyl groups on
the modified natural coagulants have a good chelating effect with
the calcium ions in the solution, which directly reduced the avail-
ability of free calcium ions for the formation of calcium carbonate
scales. However, both coagulation and anti-scaling studies were
conducted separately. Further study on both functionalities in one
study will provide more practical results and application potential.
The concept of multifunctional coagulant capable of removing a
broad spectrum of contaminants can be inspired by looking at
nature. Liu and his team have synthesized innovative biomimetic
micellar multifunctional nanocoagulant for single-step removal of
several water contaminants (Liu et al., 2019). Though the coagulant
was not synthesized from natural material, the concept idea can be
taken and implemented in natural coagulant. The multifunctional
coagulant imitated the structure of Actinia, a marine predator that
uses its tentacles to ensnare food. This living organism has a cy-
lindrical or spherical body with tentacles that could be retracted
while resting or extended while preying. The multifunctional
coagulant has a core-shell structure, where the core was respon-
sible for capturing dissolved contaminants while the shell would
hydrolyze to destabilize and enmesh colloids and suspended
 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
particles. The performance of the multifunctional coagulant was
very encouraging where it outperformed the commercial co-
agulants (alum, ferric chloride, and poly (dia-
llyldimethylammonium chloride)) especially for the removal of
dissolved organic carbon, total phosphorus, nitrate, and multiple
emerging contaminants. A remarkable observation was that the
commercial coagulants recorded low removal efficiency (generally
lower than 30%) of those dissolved contaminants but the multi-
functional coagulant acquired more than 90% removal efficiency.
This core-shell biomimetic multifunctional coagulant demon-
strated its great potential in carrying out the functionality of
coagulation (targeting suspended particles) and adsorption (tar-
geting dissolved contaminants) in one single process.
4. Sustainability of natural coagulants
Although performance efficiency is one of the most important
factors being emphasized in water and wastewater treatment
processes, other criteria answering the long-term reliability of the
technologies are equally important, especially with the call for
sustainable development by the United Nations. In general, sus-
tainable development can be defined as “the development that
meets the needs of the present without comprising the ability of
future generations to meet their own needs” (Brundtland, 1987). In
the context of water and wastewater treatment processes, the
sustainability can be considered from the integration of environ-
mental, social, economic, and technical aspects (Kamali et al.,
2019a). Since the focus of this review is on natural coagulants
and its performance in water and wastewater treatment, the sus-
tainability criteria have been adjusted from past literature to meet
the purpose of this review (as shown in Fig. 6). The sustainability
aspects of the natural coagulants will be discussed according to the
criteria and presented in Table 2.
5. Challenges of acceptance of natural coagulants
The sustainability assessment and the main topics discussed in
this article have highlighted few main challenges on the application
of natural coagulants in water and wastewater treatment processes.
The main challenges of the acceptance of natural coagulants by
water industry were summarized as below.
Fig. 6. Sustainability criteria commonly considered for water and wastewater treatment process (Kamali et al., 2019b).
13
5.1. Practicality and feasibility of real application
Most of the reported performance results of natural coagulants
have been confined to lab-scale studies and the transition to field
trials and real industrial applications has been scarce. The capa-
bility of natural coagulants in bracing the real application chal-
lenges such as fluctuating feed water quality, steady supply of
natural coagulants with consistent quality, and storage and
handling of natural coagulants has not been confirmed. To what
extent the benefits of using natural coagulants over conventional
coagulants in the real application has yet to be justified. The good
concepts of natural coagulants improvement such as multi-
functionality, hybridization with other types of coagulants,
enhancement through chemical modification, and integration with
other treatment technologies have been shown in numerous
experimental studies. However, the practicality of using these types
of natural coagulants has not been well understood. The challenges
of mass-production, technical issues, and toxicity of these co-
agulants coupled with the impacts on the other treatment pro-
cesses are the main concerns that require real application for the
revelation of application feasibility of natural coagulants.
5.2. Sustainability of natural coagulants
As discussed earlier, the use of natural coagulants met few of the
sustainability criteria and a few more aspects could not be verified
due to the lack of data. The main concerns of technical criteria are
the quality, stability, and safety aspects of natural coagulants, which
will control the consistency of performance and feasibility of the
coagulation process. The challenge lies in the continuous supply of
sufficient amount of natural coagulants with desired properties
without being affected by the various differences in the extraction
and purification or synthesis of natural coagulants. From the
environmental perspective, the secondary wastes after coagulation
process and during the synthesis/extraction processes as well as
the residual of natural coagulants in treated water could pose a
safety challenge to the environment and consumers. For economic
sustainability, the costs incurred or saved due to the use of natural
coagulants have received some mixed opinions. Further detailed
economic study is required to clarify the confusion arising from
various speculations. In social sustainability, the low industry
acceptance of natural coagulants could be attributed to the lack of
14 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267

Table 2
General assessment of natural coagulants according to different sustainability criteria.

No. Criteria Remarks

1 Technical
 Treatment efficiency
 Materials availability
 Compatibility with other Natural coagulants generally did not cause major problems for other treatment technologies, though more study looking at various
technologies
 Product stability
 Safety
2 Environmental
3 Economic
4 Social
 Industrial acceptance
 Public health improvement
Natural coagulants have proven track record in removing colloidal matters and suspended particles from water sources. The proper
selection of natural sources and modification of natural coagulants could lead to promising coagulation performance, offering an
opportunity as alternative options with competent performance over non-biodegradable conventional coagulants.
Past research articles showed that natural coagulants can be acquired and extracted from various sources ranging from waste biomass
to natural products or even can be synthesized from microorganisms (Kanmani et al., 2017; Lee and Chang, 2018; Saleem and
Bachmann, 2019b). Hence, it can be concluded that certain natural coagulants have reliable and easily available sources.
integrated or hybrid process using natural coagulants should be conducted.
Natural coagulants are susceptible to degradation where the active compounds (proteins and polysaccharides) may age during
storage or be altered due to microbial attack and external environmental factors during extraction and purification steps (Abidin et al.,
2019; Ho et al., 2014). This poses a challenge for the long-term storage of natural coagulants as deterioration of active compounds will
adversely affect the coagulation efficiency. This also has severe impacts on the commercialization potential of natural coagulants, as it
will affect the integrity (performance) and cause logistic (transportation and storage) problems for the natural coagulants.
Natural coagulants are generally regarded as nontoxic and safe due to its natural origin. However, toxicological study of natural
coagulants and its broader effect on living organisms remains unclear. This is especially compelling for the modified natural
coagulants since it involves the grafting of chemicals onto the coagulant. More detailed evaluation of the toxicity of natural coagulants
(modified or unmodified) on environment and human is needed to confirm the safe use of natural coagulants.
Using biodegradable natural coagulants which could reduce the amount of sludge and at the same time do not contribute to the
toxicity of the sludge might appeal to the water utilities (dos Santos et al., 2018). The organic sludge generated from natural
coagulants may offer environmental sustainability if the sludge could be reused for other purposes, such as in the civil engineering
industry (cement, concrete, and mortar), agricultural practice and land-based uses, and wastewater treatment (Ahmad et al., 2016).
The secondary waste generated during the extraction and purification or the synthesis of natural coagulants that involve the use of
chemicals has rarely been discussed.
The residues of natural coagulant are considered as organic substances that might possibly interact with disinfectants (from
downstream disinfection process) to form carcinogenic disinfection byproducts (Oladoja, 2015; Teh et al., 2016). Hence, precautions
should be taken when using natural coagulants if downstream disinfection process is available. Also, the purity of active compounds
in the natural coagulants can be elevated to reduce and eliminate the impurities (Barbosa et al., 2018; Dezfooli et al., 2016).
Natural coagulants have always been considered to be cheap since it can be extracted from low-cost biomass. However, this claim has
been misleading and generalized as it does not take into account other factors (costs of processing and variation due to geographical
regions) that place equally significant weight on the cost of the coagulants. Hence, the cost advantage of natural coagulants over
conventional coagulants has not been truly justified.
On another note, the benefits of using natural coagulants such as production of lesser sludge and without the need of pH adjustment
have been difficult to be converted into cost benefits since most reported claims were made from lab-scale observation. More detailed
evaluation at pilot-scale or real application is required to justify the cost reduction indirectly associated with the benefits of using
natural coagulants.
Another way to improve the economic aspect of using natural coagulants is to hybridize it with other coagulants to reduce its
consumption and cost. Alternatively, exploring the multi-functionality of natural coagulants may also lower the overall cost since
multiple treatment functionality can be conducted with single material in one treatment unit.
To sum up, the economic aspect of natural coagulants is inconclusive due to the lack of proper study evaluating the overall costs of the
coagulation process ranging from extraction to the impacts on other treatment unit.
The bottom line of acceptance is that the alternative process using natural coagulants can deliver similar (or better) treatment
performance at comparable (or reduced) cost when compared with existing established process (coagulation with chemical
coagulants). The lack of pilot-scale or real application of natural coagulants in water and wastewater treatment processes is one of the
main reasons why the industry hesitates to adopt natural coagulants. Another factor that hinders the acceptance of natural coagulants
by industry is the lack of regulatory guidelines and approval on the use of natural coagulant especially in potable water treatment
process.
Natural coagulants that can be obtained locally and extracted via simple process could be useful for people without clean water
access, especially those that stay in rural area or regions that have financial constraints for proper clean water supply. Consumption of
treated water will improve their health and subsequently lead to elevation of living conditions.

pilot-scale or real application of natural coagulants and the lack of
regulatory support from the government agency. On the other
hand, the niche application of natural coagulants in rural areas or
regions facing with economic water scarcity may be helpful in
improving the living conditions of those people. Overall, clarifica-
tion and justification of the above concerns could shed the light on
the sustainability potential of using natural coagulants in water and
wastewater treatment processes.
6. Future prospects of natural coagulants
The challenges faced natural coagulants are also opportunities
where future study can be carried out to clarify the uncertainties
associated with the feasibility of natural coagulants in real appli-
cation. Summarized below are the future research that can be
focused to enhance the acceptance of natural coagulants in water
and wastewater treatment processes.
6.1. Up scaling study on the feasibility of natural coagulants
Natural coagulants (modified or unmodified) that have shown
promising performance in lab-scale study should be upgraded to
pilot-scale or field applications. Through this, the practicality and
feasibility (especially performance, costs, and technical issues) of
the natural coagulants in water industry can be evaluated more
thoroughly. The findings will be able to provide a more compre-
hensive insight into the advantages of using natural coagulants and
highlight the aspects for improvement. In addition, the potential of
natural coagulants in rural areas and regions hit by economic water
scarcity should be explored. The natural coagulants can be derived
from locally available sources.
6.2. Sustainability of natural coagulants
Research aligned with the sustainability criteria (technical,
 W.L. Ang, A.W. Mohammad / Journal of Cleaner Production 262 (2020) 121267
environmental, economic, and social) will help to clarify many of
the lingering uncertainties of natural coagulants. To be able to
compete with conventional coagulants, steady supply of sufficient
raw materials for the extraction or synthesis of natural coagulants
is a must. Though it has been generally claimed that natural co-
agulants can be obtained easily from various sources, verification of
this claim has not been properly done. In addition, a comprehensive
costing study can be conducted to give a clear picture of the eco-
nomic feasibility of natural coagulants, encompassing the costs of
raw materials, extraction/synthesis and purification processes, and
during the operation. In-depth study on the consequences of using
natural coagulants (especially modified natural coagulants that
recorded marked improvement in coagulation performance) on
health and environment (toxicity) could also be studied to clarify
the safety issues. Sustainability assessment and life cycle assess-
ment can be conducted to provide an insight of the aspects that can
be improved for coagulation process using natural coagulants.
6.3. Multifunctional coagulant
The concept of multi-functionality is an interesting idea that
might revolutionize the coagulation process. Coagulants with the
capability to remove both undissolved and dissolved impurities can
intensify the treatment process and lead to several benefits such as
cost saving and reduced footprint. Innovative design and synthesis
of coagulants mimicking nature can materialize this aim.
6.4. Quality control of natural coagulants
On one hand, natural sources offer a great opportunity for the
ease of availability of natural coagulants. On the other hand, the
constituents of natural sources could be a problem for quality
control of natural coagulants due to the variances in growth con-
ditions and species. Furthermore, the identification of active com-
pounds possessing the coagulation capability in natural extract is
also a challenging task. More study on these aspects can help to
clarify the issues related to extraction of natural coagulants. With
the identification of active coagulation compounds, a better
extraction and purification approach can be developed to increase
the purity of natural coagulants. Biosynthesis of natural coagulants
from microorganism could be an alternative way of securing nat-
ural coagulants with quality control and mass production potential.
6.5. Circular economy & bioeconomy
The concepts of circular economy and bioeconomy could help to
support the sustainability of natural coagulants in water and
wastewater treatment. The former emphasizes enhancing the
coagulation process efficiency without increasing the consumption
(dosage) and exploring the potential to recover and reuse the co-
agulants. Bioeconomy highlights the production and application of
coagulants from natural sources. Research and development of
natural coagulants could take these calls into consideration to move
towards a sustainable water industry.
7. Conclusion
Nature has gifted humans with solutions to obtain clean water
and to remove the pollutants discharged into the water body from
anthropogenic activities. The materials possessing coagulation
capability can be obtained from various natural sources. It is
therefore dependent on the wisdom of humanity uncover ways to
fully utilize the natural materials for water and wastewater treat-
ment purposes. Literature has proven the capability of natural co-
agulants in removing impurities (especially colloidal particles and
15
suspended solids) that cause problem for subsequent treatment
process and health issues for consumers. Unfortunately, the wide-
spread application of natural coagulants in water industry is still far
from reality and the acceptance of natural coagulants over the
conventional coagulants is still low. Hence, efforts in raising the
confidence of water utility by showcasing the capability of natural
coagulants should be emphasized. Among these are: the compati-
bility of natural coagulants with other treatment technologies in
integrated/hybrid treatment process; the modification of natural
coagulants for marked improvement in coagulation performance
efficiency; the possibility of hybridizing natural coagulants with
other types of coagulants; the improvement of extraction and pu-
rification approaches for high purity of natural coagulants; and the
synthesis of multifunctional natural coagulants. Coupled with the
sustainability assessment of natural coagulants, the direction of
future research for further improving the capability of natural co-
agulants and boosting the confident of industry players can be
obtained.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgement
The authors would like to thank the Ministry of Education
Malaysia for funding this work through Malaysian Research Uni-
versity Network (MRUN) under the grant code KK-2019-001 at
Universiti Kebangsaan Malaysia.
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