J O U R NA L OF EN V I RO N M EN T A L S CI EN C ES 2 6 ( 20 1 4 ) 2 1 78–2 1 8 9

Available online at www.sciencedirect.com

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Invited article

Utilization of plant-based natural coagulants as future

alternatives towards sustainable water clarification

Sook Yan Choy1 , Krishna Murthy Nagendra Prasad1 , Ta Yeong Wu1 ,

Mavinakere Eshwaraiah Raghunandan2 , Ramakrishnan Nagasundara Ramanan1,3,⁎
1. Chemical Engineering Discipline, School of Engineering, Monash University Malaysia, 47500 Bandar Sunway, Selangor, Malaysia.
E-mail: ramanan@monash.edu
2. Civil Engineering Discipline, School of Engineering, Monash University Malaysia, 47500 Bandar Sunway, Selangor, Malaysia
3. Advanced Engineering Platform, School of Engineering, Monash University Malaysia, 47500 Bandar Sunway, Selangor, Malaysia

AR TIC LE I N FO ABS TR ACT

Available online 11 October 2014 Rapid industrial developments coupled with surging population growth have complicated
issues dealing with water scarcity as the quest for clean and sanitized water intensifies
Keywords: globally. Existing fresh water supplies could be contaminated with organic, inorganic and
Chemical coagulant biological matters that have potential harm to the society. Turbidity in general is a measure
Commercialization of water cloudiness induced by such colloidal and suspended matters and is also one of the
Constraints major criteria in raw water monitoring to meet the stipulated water quality guidelines.
Fruit waste Turbidity reduction is often accomplished using chemical coagulants such as alum. The use
Protein of alum is widely associated with potential development of health issues and generation of
Turbidity reduction voluminous sludge. Natural coagulants that are available in abundance can certainly be
considered in addressing the drawbacks associated with the use of chemical coagulants.
Twenty one types of plant-based natural coagulants categorized as fruit waste and others
are identified and presented collectively with their research summary in this review. The
barriers and prospects of commercialization of natural coagulants in near future are also
discussed.
© 2014 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences.
Published by Elsevier B.V.

Contents

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2179
1. History of coagulants used in water clarification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2179
2. Downsides of chemical coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2179
3. Advantages of plant-based natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2180
4. Classification of plant-based coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2180
4.1. Fruit waste . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2180
4.2. Others . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2181

⁎ Corresponding author. E-mail: ramanan@monash.edu (Ramakrishnan Nagasundara Ramanan).

http://dx.doi.org/10.1016/j.jes.2014.09.024
1001-0742/© 2014 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
 JO U R N A L OF EN V I RO N M EN T A L S CI E NC ES 2 6 ( 20 1 4 ) 2 1 7 8–2 1 8 9 2179

5. Constraints in commercialization of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2184

6. Prospects of natural coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2184
7. Limitations and further improvements on the current natural coagulant studies . . . . . . . . . . . . . . . . . . . 2185
8. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2187
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2187
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2187

Introduction resulted in the introduction of polymerized aluminium coagu-

Water, air and food are among some of the essential elements in life.
Yet, these important commodities have been taken for granted as
continuous industrial development becomes the frontier of today's
world. As a result, environmental pollutions and the shrinkage of
precious commodities have affected the lives of many. The world
consists of a major portion (about 71%) of water but freshwater
contributes to only a minor fraction of 2.5%. However, more than
60 billion m3 a year of freshwater is needed to cope with the annual
global population growth of 80 million people. In Asia alone, urban
populations can be expected to double in the year 2000–2030
(Martine, 2007) and water scarcity is now a global pandemonium
not limited to arid zones (Wu et al., 2013). Continuous population
growth, increasing standard of living, climate change, industrializa-
tion, agriculture and urbanization are triggering the decrease in
water resource worldwide (Wu et al., 2013). The remaining propor-
tion of water sources could be contaminated to certain extents
rendering them to be unsafe for direct consumptions. The contam-
ination of raw water could be due to human intervention,
geopogenic source (water-rock interaction) or climate conditions in
one country (Nasrabadi and Abbasi Maedeh, 2014).
As such, adequate water treatment and sanitation are essen-
tial to remove turbidity, impurities and other pathogenic bacteria
which can be guided through the addition of coagulants. Due
to its simplicity and effectiveness, coagulation and flocculation
are one of the most widely adopted techniques to restore the
palatability and improve the esthetic appearance of turbid
water. This technique results in the destabilization of colloidal
particles and subsequently, the increment in particle size for the
ease of sedimentation. The figurative illustration of the coagu-
lation and flocculation process via the charge neutralization
mechanism has been shown elsewhere (Choy et al., 2013).
Despite that, 67% of the worldwide population could still be
deprived to the access of adequate sanitation in the year 2030
(World Water Assessment Programme, 2009).
1. History of coagulants used in water clarification
Coagulation and flocculation could be achieved using either
natural coagulants or chemical-based coagulants. Among the
two, natural coagulants have long been acknowledged for
their application in traditional water purification which was
evident from various ancient records cited (Dorea, 2006;
Bratby, 2006). On the other hand, the global dissemination of
alum as a coagulant for public water supply occurred back in
the 19th century (Jahn, 2001). Since then, China has become
the world's earliest alum user for the clarification of water
followed by other nations globally. In the United States, metal
coagulants such as ferric salts have their reign in water
treatment since 1880. As the performance of these customary
chemical coagulants is dubious in certain working conditions
such as low temperatures, on-going developments have
lants. Polyaluminium chloride (PACl) has garnered a growing
market owing to its higher superiority and lower consumption
of alkalinity. Organic synthetic polymer flocculants such as the
more common polyacrylamide are also available in the market;
offering a wider selection of chemical coagulants to cater for the
diverse requirements of the individual water treatment plants
(Bolto and Gregory, 2007).
With the invasion of chemical coagulants, traditional
water clarification methods using natural coagulants are no
longer practiced except in rural and developing countries
which have limited accessibility to these chemicals. This
marked the beginning of a paradigm shift towards the
dependence of chemical coagulants in treating turbid water.
Over the years, this scenario has gradually led to stagnation in
the development of natural coagulants. An infinite gap has
since existed drawing obvious lines between these two
coagulant variants as the traditional water clarification
method becomes obsolete.
2. Downsides of chemical coagulants
Despite the superiority of chemical coagulants in treating turbid
water, they are still lacking in terms of green chemistry. In the
1960s, detrimental effects of chemical coagulants on the human
health were published (Simate et al., 2012). Residual aluminium
in alum treated water has been the center of debate as it is
linked to serious health issues such as the development of
Alzheimer's disease (AD) (McLachlan, 1995; Flaten, 2001;
Gauthier et al., 2000; Walton, 2013; Rondeau et al., 2000) and
senile dementia (Rondeau et al., 2001). The results from a
number of epidemiological studies and clinical observations
have suggested at least 70% of positive correlations between the
presence of aluminium in drinking water and AD (Doll, 1993;
Flaten, 2001).
However, contradictory results have also been reported due
to the absence of substantial evidence in several instances
(Martyn et al., 1997; Forster et al., 1995; Wettstein et al., 1991).
Thus, a conclusive link between aluminium and the progres-
sion of AD could not be determined at this point of time.
Nevertheless, these positive results obtained should not be
dismissed where attention must be given to control the amount
of residual aluminium in treated water (WHO, 2011). To
minimize this risk factor over prolonged duration of consump-
tion, threshold aluminium concentration values in treated
water have been reported to be 0.02 mg/L (Doll, 1993) and
0.1 mg/L (McLachlan, 1995; Rondeau et al., 2000). While the
suggested aluminium concentration by WHO is 0.2 mg/L,
certain countries have adhered to much stricter guidelines
2180 J O U R NA L OF EN V I RO N M EN T A L S CI EN C ES 2 6 ( 20 1 4 ) 2 1 78–2 1 8 9
(Simate et al., 2012). Even so, a mean aluminium concentration
ranging from 0.01 to 0.15 mg/L is common (Doll, 1993), slightly
above the threshold values which could increase the probability
of AD incidence with respect to drinking water.
Other concerns over the presence of residual aluminium in
drinking water such as reduced water disinfection efficiency
have been well documented (Driscoll and Letterman, 1995).
Synthetic organic polymer for instance acrylamide has strong
neurotoxic and carcinogenic effects. Unreacted chemical mono-
mers and the by-products of polymers in water could also
threaten the human health (Bratby, 2006). As for iron salts,
careful process controls are necessary as excessive iron residual
in the treated water will lead to highly visible rust or blood
colored stains (Gebbie, 2005) caused by the hydrolysis of iron
salts.
Another major drawback of hydrolyzing metal coagulants is
the generation of voluminous hydrous oxide sludge which is
non-biodegradable due to the nature of the coagulant. For
instance, 99% of the alum sludge is made up of water (Gregory,
2006) and alum sludge is rather hard to dewater. Alum sludge
also has the disadvantage of causing phosphorus uptake from
plants due to inorganic phosphorus absorption which leads to
aluminium phytotoxicity (Cornwell, 1999). It has been estimat-
ed that a typical water treatment plant with the treatment
capacity of 190 million L per day using alum would result in at
least 3 tonnes of dry solid waste; accumulating to more than
1000 tonnes annually (Gruninger, 1975). This finding indirectly
translates to the excessive sludge input to existing landfills
which are currently being reported to be insufficient to cater for
the rapidly growing amount of sludge produced. Moreover,
treatment of highly turbid water requires several proteolytic
additives along with alum making it an expensive process. Such
complicated methods for treatment of highly turbid water are
difficult to adopt in poor or developing countries, where
cost-effective and simple drinking water treatment methods
are needed (Bodlund et al., 2014). Owing to the downfalls of
chemical coagulants, there is a need to consider other potential
alternatives for water clarification to minimize the environ-
mental damages and to safeguard the wellbeing of human
population.
3. Advantages of plant-based natural coagulants
In contrast to chemical coagulants, plant-based natural coagu-
lants are safe (Asrafuzzaman et al., 2011), eco-friendly and
generally toxic free (Bratby, 2006; Swati and Govindan, 2005).
Natural coagulants have been found to generate not only a
much smaller sludge volume of up to five times lower
(Ndabigengesere et al., 1995) but also with a higher nutritional
sludge value. As such, sludge treatment and handling costs are
lowered making it a more sustainable option. The raw plant
extracts are often available locally and hence, a low cost
alternative to chemical coagulants. Since natural coagulants
do not consume alkalinity unlike alum, pH adjustments can be
omitted and this provides extra cost savings. Natural coagu-
lants are also non-corrosive (Swati and Govindan, 2005) which
eliminate the concerns of pipe erosions. Fig. 1 summarizes the
benefits of using natural coagulants as an alternative to
chemical coagulants in water clarification process.
Till date, reviews on plant-based natural coagulants were
mainly focused on the four most common natural coagulants
which included Moringa oleifera seeds, Nirmali seeds, tannin and
Opuntia ficus indica cactus in the water and wastewater
treatments (Yin, 2010; Vijayaraghavan et al., 2011). In addition
to the current database of studied natural coagulants, an
extensive overview on the indigenous plants used by rural
Africans in water purification has been provided (Yongabi,
2010). Recently, an extensive review covering the studied
vegetables and legumes has provided an insight to the less
commonly known water clarifying agents (Choy et al., 2013).
Apart from the mentioned plant-based coagulants, little is
known about other plant categories with notable water
clarification properties. Hence, there is a need to account for
such coagulants and to identify the key findings obtained from
various coagulation studies conducted previously. This review
work can serve as a compendium of 21 types of plant-based
coagulants grouped under two main categories namely fruit
waste and others (cactus, cereals, fungus, nuts, shrubs and
spice). Further, the challenges which kept the commercializa-
tion of natural coagulants at bay are also highlighted.
4. Classification of plant-based coagulants
A majority of the plant-based coagulants incorporated in this
current review is made up of fruit waste which ultimately
forms a viable source of raw materials for further applications.
The remaining coagulants fall under various categories of
cactus, cereals, fungus, nuts, shrubs and spice. However, they
will be jointly reviewed as others to provide a general
overview on the coagulation studies conducted. The back-
ground information and physicochemical properties for the
respective plant-based coagulants could be beneficial to
provide an insight to its nature and the probable active
coagulation agents present (refer to supporting information).
4.1. Fruit waste
Fruits are rich sources of vitamins and nutrients which can be
consumed fresh, dried, or processed with diverse demands in
the food industries. A significant amount of up to 50% of the
total fruit weight is made up of fruit waste such as peels and
seeds that are commonly non-edible. These large proportions
of waste are generally discarded into the environment as they
lack in commercial values. In Malaysia, the habit of com-
posting and waste recycling is not yet a widely adopted
method and ultimately resorting to the easiest disposal
method; landfilling (APO, 2007). Close to 1000 million tonnes
of agricultural waste are being generated internationally in a
yearly basis and of this, about 1.2 million tonnes are being
discarded into landfills in Malaysia alone (Agamuthu, 2009).
The mishandling of fruit waste could be detrimental to the
environment due to potential leaching into soil and water
sources leading to further pollution (Hacker et al., 2009).
Although fruit waste is generally discarded, it is worth-
while to note that some waste such as seeds and barks have
diverse folkloric medicine applications. Findings till date have
suggested the use of 9 fruit waste in treating turbid synthetic
water, raw surface water and waste water. These are the
 JO U R N A L OF EN V I RO N M EN T A L S CI E NC ES 2 6 ( 20 1 4 ) 2 1 7 8–2 1 8 9
Fig. 1 – Advantages of natural coagulants (NCs) over chemical coagulants.
seeds of Carica papaya, Feronia limonia, Mangifera indica, Persea
americana, seeds and pollen sheath of Phoenix dactylifera,
Prunus armeniaca, Tamarindus indica, the peels of Citrus sinensis
and the foliage of Hylocereus undatus (Table 1). Among these,
P. armeniaca has been used as primary coagulants during the
ancient times in China and Egypt with histories dating back to
the 1100s (Jahn, 2001). Generally, turbidity reduction of greater
than 80% for most of the fruit waste coagulants can be
achieved although several exceptions exists which is likely
unfavorable for the treatment of drinking water (Table 1). The
various forms of natural coagulants used could also have
influenced the turbidity removals reported. For instance, the
blending of T. indica seeds in water (Thakre and Bhole, 1985)
could be more efficient compared to aqueous extraction using
the powdered seeds (Swati and Govindan, 2005); underlying
the importance of the pre-treatment step.
The colloids present in foliage of H. undatus are cationic
which is similar to the seeds of M. oleifera. Thus, adsorption
and charge neutralization have been proposed as the possible
coagulation mechanism leading to formation of flocs (Som et
al., 2007; Idris et al., 2013). Proteins and polysaccharides are
among some of the natural polymers present in fruit waste.
The size of these polymers can be expressed in terms of
molecular weight where a larger value would correspond to a
longer polymeric chain. This would be advantageous for
coagulation as the number of active sites available for particle
adsorption will be increased. Although the polysaccharide of
T. indica has a higher molecular weight of around 720–880 kDa,
the obtained turbidity removals were no greater than that of
M. oleifera with dimeric proteins of 13 kDa (Mirhosseini and
Amid, 2012; Ndabigengesere et al., 1995). The proximate
compositions of protein and carbohydrate between these
seed types could be the underlying factor leading to the
variations in treatment efficiencies as observed.
Apart from turbidity, commonly present bacteria notably
Escherichia coli and Staphylococcus aureus in surface water must
also be removed to meet the stipulated drinking water
standards. Some fruit waste has notable coagulation activities
2181
while others could be more superior in terms of bacteriostatic
activities. An example of such coagulants is the extracts of
P. americana which is rich in antimicrobial agents such as
saponins, phenols and flavonoids (Arukwe et al., 2012). Most
of the fruit waste coagulants were also found to exhibit potent
bacteriostatic properties which retarded the proliferation in
bacteria (Osato et al., 1993; Dubey et al., 2011; Ashok kumar et
al., 2011; Engels et al., 2009;Perveen et al., 2012; Al-daihan and
Bhat, 2012; Bhat and Al-Daihan, 2012; Yiğit et al., 2009).
Nevertheless, secondary disinfection would be crucial to
attain a fecal coliform level of zero colony forming units
(cfu)/100 mL in the treated water to meet the quality of the
drinking water standards (Yongabi et al., 2011b; Pritchard et
al., 2009). Based on the worthwhile usage of fruit waste as
potential natural coagulants along with the potency against
selected bacteria, the overall economics as well as sustain-
ability of the fruit farming and juicing industries can be
enhanced.
4.2. Others
An assortment of plants other than fruit waste has also been
discovered over the recent years for treating both raw surface
and synthetic turbid water. This 12 other plants can be further
categorized into the various classifications of cactus, cereals,
fungus, nuts, shrubs and spice (Table 2). A majority of these
plants are familiar as commercial food sources while some
are distinguished for their traditional medicine applications
such as Strychnos potatorum (Ruijter, 2008) and Cassia alata
(Aweng et al., 2012).
Table 2 shows the summary of research highlight for
each of the plant-based coagulants classified as others: cacti
mucilage and extract from the pads of Cereus repandus,
Stenocereus griseus and O. ficus indica, the seeds of Oryza sativa
and Zea mays which form the backbone of agricultural
industries, the sclerotium of Pleurotus tuber-regium or King
Tuber Mushroom which is the only fungus tested till date, the
hard nuts of Jatropha curcas and S. potatorum, several species of
2182 J O U R NA L OF EN V I RO N M EN T A L S CI EN C ES 2 6 ( 20 1 4 ) 2 1 78–2 1 8 9

Table 1 – Research summaries of fruit waste used as plant-based natural coagulants.

No. Coagulant Type of sample Initial conditions Optimized parameters

Name Form used Turbidity pH Others Dosage pH Turbidity

(NTU) (mg/L) reduction

1 Carica papaya A, F, J RSW (storm water) 119 100 seeds/100 L 90%

seeds
F, H1, K, E SW (metal 5 0.5 g/100 cm3
aqueous solution)

2 Citrus sinensis C1/C2, F RSW 32 9.4 (H4) Alkalinity: 195 mg/L 4000 ~85%
peel/skin
3 Feronia E, F, H2, I, L1 SW (clay) 100 20 8.0 ~77%
limonia seeds
E, F, H2, I, L1 SW (clay) 100 9 + 20 alum ~97.5%
(as CA which
is added first)
4 Hylocereus E, F LCE 7243 7.3 COD: 7857 mg/L 300 10 99.5%
undatus foliage BOD:
1327 mg/L
SS: 1208 mg/L
B, D, E, F LCE 7243 7.3 COD: 7857 mg/L 500 10 99.7%
SS: 1208 mg/L

5 Mangifera E, F, G RSW (Nile River) 6.5 TC: 5000 MPN/100 mL 30 54% (at clarri-
indica seeds flocculator)
Mangifera A, E, F, G SW (Kaolin) 90 0.5 mL/L 13 98.65%
indica kernels
6 Persea F, J RSW (storm water) 119 100 seeds/100 L 64.2%
americana seeds

7 Phoenix dactylifera C3, E, F, L2, G1 SW (Bentonite) 75 ± 10 30 94% (at

date seeds 120th min)
Pollen sheath C3, E, F, L2, G SW (bentonite) 300 ± 10 90 93% (at
120th min)

8 Prunus E, F, G RSW (Nile River) 6.5 TC: 7000 MPN/100 mL 30 54% (at clarri-
armeniaca seeds FC: 800 MPN/100 mL flocculator)
9 Tamarindus E, F, H2, I, L1 SW (clay) 100 mg/L 20 7.5 80%
indica seeds
E, F, H2, I, L1 SW (clay) 100 mg/L 3 + 20 alum 98% (as CA
which is
added first)
E, F, G, L1 SW (Kaolin) 76–79 5 8 69%

E, F, G, L1 RSW (Pond) 94.7 8 2 96% (as CA)

E, F TWW TSS: 425 mg/L 14,000

DO: 1.8 mg/L
A: deshelled, B: removal of thorns, C: washed with: (1. formaldehyde, 2. acid-alkaline, 3. water), D: cut, E: dried, F: pulverized, G: extracted with
water, H: soaked in: (1. HNO3, 2. water), I: blended in water, J: sprinkled onto samples, K: filtered and rinsed with water, L: added with: (1. HCl, 2.
NaOH).
RSW: raw surface water, SW: synthetic water, CA: coagulant aid, LCE: latex concentrate effluent, COD: chemical oxygen demand, BOD: biological
oxygen demand, SS: suspended solids, MPN: most probable number, TC: total coliform, FC: fecal coliform, TWW: tofu waste water, TSS: total
suspended solid, DO: dissolved oxygen.

shrubs including leaves from the ornamental shrub of Cassia
alata, juice from the roots of Maerua subcordata and seeds of
Prosopis juliflora as well as the seeds from the conventional
spice of Trigonella foenum-graecum. Among them, S. potatorum
has been used as water clarifiers since over 4000 years
according to the historical records of Sanskrit writings
(Al-Samawi and Shokralla, 1996). This marked the first
reported natural plant-based coagulant used for water treat-
ment worldwide (Yin, 2010).
Generally, turbidity reduction of at least 80% has been
reported when these plant-based coagulants are used under
optimized working conditions although few exceptional
 JO U R N A L OF EN V I RO N M EN T A L S CI E NC ES 2 6 ( 20 1 4 ) 2 1 7 8–2 1 8 9 2183

Findings/claims References

• E. coli counts reduced by 75.3% Yongabi et al. (2011b)

1 • Total heterotrophic bacterial counts reduced by 71.7%
• The maximum metal adsorptions at the optimized contact time of 90 min: Egila et al. (2011)
→Lead, Pb: 4.1 mg/100 cm3
→ Manganese, Mn: 3.6 mg/100 cm3
• Smaller ionic size of Mn resulting in faster adsorptions
2 • Highly efficient in the removal of alkalinity Sowmeyan et al. (2011)
• Not effective for the removal of iron and chlorides
3 • Maximum turbidity removal of ~88% at a dosage of 60 mg/L for initial turbidity of 1600 NTU Bhole (1995)
• Maximum turbidity removal of ~99.8% at a dosage of 30 mg/L + 60 mg/L alum for initial turbidity of 1600 NTU
• Efficiency at different sequence of coagulant addition:
→ ~95% with the addition of alum followed by coagulant aid
→ 93% with the simultaneous addition of both coagulants
4 • Removal of COD by 97.7% Som et al. (2007)
• Removal of BOD by 86.9%
• Removal of SS by 94.5%
• Efficiency removals below 90% and 80% for turbidity and SS respectively at lower pH (2–9)
• Removal of COD by 94.7% Idris et al. (2013)
• Removal of SS by 88.9%
• 2 ‘peak’ values existed at pH 3 and pH 10 indicating the higher removal efficiencies
5 • At the plant outlet, total coliform counts reduced by 99.6% Ali et al. (2008)
• Treated water has a greenish color despite the high removal of various algae groups
• Coagulation activity is comparable to alum at 99% Qureshi et al. (2011)
• Removal efficiency generally increased with pH increment of the water; lowest at pH 7
6 • E. coli counts reduced by 84.9% Yongabi et al. (2011b)
• Total heterotrophic bacterial counts reduced by 75.5%
• Coagulants exhibited antimicrobiological properties (reduction in microbes count) but insufficient to meet the
WHO standards
7 • 90% turbidity reduction at 60 mg/L for initial turbidity of 150 ± 10 NTU Al-Sameraiy (2012)
• 83% turbidity reduction at 80 mg/L for initial turbidity of 300 ± 10 NTU
• Performed better than pollen sheath at an initial turbidity of 75 ± 10 NTU
• 91% turbidity reduction at 20 mg/L for initial turbidity of 75 ± 10 NTU
• 92% turbidity reduction at 50 mg/L for initial turbidity of 300 ± 10 NTU
• More superior than date seeds at initial turbidities of 150–300 ± 10 NTU
8 • At the plant outlet, total coliform counts reduced by 99.7% Ali et al. (2008)
• Fecal coliform counts reduced by 99.5%
9 • Maximum turbidity removal of 92.3% at a dosage of 60 mg/L for initial turbidity of 1000 mg/L Thakre and Bhole (1985)
• Maximum turbidity removal of 99.8% at a dosage of 10 mg/L + 60 mg/L alum for initial turbidity of 1600 mg/L
• Efficiency at different sequence of coagulant addition:
→ 97% with the addition of alum followed by coagulant aid
→ 96% with the simultaneous addition of both coagulants
• Aging seed extracts are detected from the generation of foul smell or the formation of a floating slime layer Swati and Govindan (2005)
• Optimum shelf life of 10 days
• Bacterial reduction by 99.4%
• 1:10 is the ratio of alum to coagulant aid used
• 85% turbidity removal at 5 mg/L as primary coagulant
• Removal of TSS by 67.3% Nurika et al. (2007)
• The DO value increased by 53.9%

cases existed: O. ficus indica (Yang et al., 2007) and Z. mays
(Gunaratna et al., 2007; Subramanium et al., 2011). The presence
of active agents such as carbohydrates and proteins has been
linked to the observed purification effects in the various plants.
For instance, uronic acids; a class of sugar acids detected at
around 11% in both the mucilage of S. griseus and O. ficus indica
(Fuentes et al., 2011; Karawya et al., 1980). The mucilage which
consists of galacturonic acids is generally the predominant
active coagulation agent present in cacti mucilage regardless of
species. The enhanced turbidity removal for Opuntia cactus
could be attributed to the much higher total compositions of
arabinose, galactose and rhamnose which have been found to
2184 J O U R NA L OF EN V I RO N M EN T A L S CI EN C ES 2 6 ( 20 1 4 ) 2 1 78–2 1 8 9
have synergistic effects with galacturonic acids in promoting
coagulation (Miller et al., 2008). The coagulation mechanism
was then deduced to be adsorption and bridging based on the
characteristics of the mucilage which is an anionic polyelectro-
lyte. Also negatively charged in nature, the main functional
groups of COO− and OH− in the polyelectrolyte of the seeds of S.
potatorum have been found to be responsible for the reported
coagulation activities (Subbaramiah and Rao, 1937; Tripathi
et al., 1976).
In contrast, the coagulation mechanisms in the seeds of J.
curcas were believed to be adsorption and charge neutraliza-
tion due to close similarities of the cationic active coagulation
agent to that in M. oleifera (Abidin et al., 2011). Unlike most of
the plant-based coagulants listed (Table 2), cereal crops are
largely made up of carbohydrates with up to 94% of the total
dry weight (Oko and Ugwu, 2011; Sobukola and Abayomi,
2011). Starch which is a form of carbohydrate has been
identified as the possible active agent leading to coagulation
in such coagulants (Raghuwanshi et al., 2002). Likewise, the
excellence of M. subcordata in removing turbidity could also be
due to the presence of polysaccharides mainly amylopectin
(Mavura et al., 2008). As they served as bridges to link colloidal
particles together, the increment in floc size would improve
the overall precipitation process (Göttsch, 1992). Apart from
starch, phytochemicals such as tannins in plants have also
been recognized as active agents in promoting coagulation;
suggesting the same for P. tuber-regium which contained this
active agent (Ikewuchi and Ikewuchi, 2008; Akindahunsi and
Oyetayo, 2006).
Besides notable turbidity removal properties, selected plant-
based coagulants are also capable of removing heavy metals
(Table 2). Studies have also demonstrated that Z. mays were able
to remove at least 15% of lead, chromium and hardness from
river water with larger fractions of cadmium and zinc removals
(Subramanium et al., 2011). However, the results obtained were
less superior in comparison to M. oleifera. The formaldehyde
washed seeds of S. potatorum displayed superiority with
alkalinity removals up to 70% while the acid-alkaline washed
have successfully removed more than 25% of magnesium and
hardness (Sowmeyan et al., 2011). Much smaller removal
proportions for other contaminants such as fluoride and iron
have also been obtained. Additional treatment benefits such
as the removal of bacteria (Shilpa et al., 2012; Swati and
Govindan, 2005): E. coli (Tripathi et al., 1976) and fecal coliform
(Yongabi, 2006; Yongabi et al., 2011a; Pritchard et al., 2009)
have been demonstrated. The presence of phytochemical
constituents such as alkaloids and tannins (Ejelonu et al.,
2010; Mallikharjuna et al., 2007) could most likely have
contributed to the observed antimicrobial activities in plant-
based coagulants.
5. Constraints in commercialization of
natural coagulants
Although various indigenous plant extracts have been proven
to possess coagulative properties in removing turbidity
(Sowmeyan et al., 2011), not many has reached the phase of
commercialization. The four main constraints hindering the
commercialization of natural coagulants: financial, research
and development, market awareness as well as regulatory
approval have been well documented in the literature for the
case of M. oleifera seeds (Sutherland et al., 2001). On top of the
scientific aspects, the problems encountered with the har-
vesting and processing of the plant extracts were also
highlighted. Financial freedom is a common barrier faced as
potential investors are usually hesitant to invest in new
products. By understanding the vulnerabilities and risks
involved, the development of natural coagulants would be
improved.
The research and development area holds the key in
understanding the scientific aspects of the natural coagu-
lants of interest. It also serves as a platform and backbone for
the identification of strengths, limitations, areas which
require fine-tuning as well as process improvements. The
existing results reported are largely confined to laboratory
scale which may be lacking in terms of process scalability
for real time applications. A breakthrough in this matured
market can begin by emphasizing the blending of natural and
chemical coagulants. Natural coagulants, a kind of polymers
are more than often used in conjunction with chemical
coagulants as they exhibited restricted turbidity removal
efficiencies when used alone. Likewise, the feasibility of
using plant derived coagulants may also be questionable due
to their suitability under various working conditions.
In addition, the response and needs of the market will
affect the outlook and demands of natural coagulants as a
probable replacement of chemical coagulants. This is so as
the misconception on the feasibility of natural coagulants by
both consumers and suppliers would lead to an inaccurate
prediction of the realistic target market. An evaluation on the
economic, social and environmental aspects which could be
used as a sustainability indicator would be useful with the aid
of a pilot plant study. Approval from the local governing
bodies must also be granted for successful commercialization
of any new products. However, it may not be easy to obtain an
approval as stringent screenings and documentations could
be needed to ensure product compliance to the respective
standards (Sutherland et al., 2001). Tax rebates and subsidy
schemes could be offered as a form of driving incentive to
motivate water treatment operators to adopt the use of
natural coagulants.
While the commercialization of natural coagulants will not
be an overnight success, these small steps taken would
progressively bridge the gaps and limitations encountered.
Fig. 2 summarizes these factors which must be taken into
considerations for successful commercialization of natural
coagulants.
6. Prospects of natural coagulants
Despite the constraints faced in commercialization, tannin
extracts have been used extensively in the potable and
wastewater treatment industries (Bratby, 2006). The tannin
extract from the barks of Acacia mearnsii tree have been
successfully commercialized as Floccotan (Bratby, 2006).
Another tannin commercialization is evident under the
ECOTAN series (Servyeco Group, 2008). Tannins which are a
 JO U R N A L OF EN V I RO N M EN T A L S CI E NC ES 2 6 ( 20 1 4 ) 2 1 7 8–2 1 8 9 2185

Table 2 – Highlights of plant-based natural coagulants classified as others.

No. Plant name Highlights Reference

Cactus
1 Cereus repandus Similar residual turbidity with alum (< 10 Nephelometric Turbidity Units, NTU) but Diaz et al. (1999)
at a much
lower coagulant dosage of 20 mg/L
2 Stenocereus griseus Exhibited color reduction from 50 to 25 units in treated water Fuentes et al. (2011)
3 Opuntia ficus indica Turbidity removal lowest at pH 6 Zhang et al. (2006)
Coagulation properties might be contributed by the presence of Miller et al. (2008)
mucilage, especially by the galacturonic acid component Mane et al. (2011)
Demonstrated nickel and chromium removal by at least 65% Shilpa et al. (2012)
Reduction of bacteria up to 20%
Cereals
4 Oryza sativa Maximum turbidity removal of 96.4% is achievable for initial Thakre and Bhole (1985)
turbidity of 1000 mg/L
5 Zea mays Exhibited more than 20% of cadmium and zinc removal Subramanium et al. (2011)
Fungus
6 Pleurotus tuber-regium Extremely low sensitivity to Escherichia coli; suggesting the absence of Yongabi et al. (2011a),
notable antibacterial activity Yongabi (2006)
Nuts
7 Jatropha curcas Removal of Escherichia coli and fecal coliforms by at least 60% Yongabi et al. (2011a),
Similar turbidity removal (~ 99%) in both the conventional and Yongabi
the assisted blending methods (2006), Pritchard et al. (2009)
Abidin et al. (2013)
8 Strychnos potatorum Reduction of E. coli and bacteria by at least 40% Tripathi et al. (1976), Swati
Removal of hardness and magnesium up to 30% and
Govindan (2005)
Sowmeyan et al. (2011)
Shrubs
9 Cassia alata No potential for iron and manganese removal but commendable Aweng et al. (2012)
for suspended solids
10 Maerua subcordata Contains relatively large amounts of proteins and polysaccharides Mavura et al. (2008)
(mostly amylopectin which is responsible for the coagulation properties)
11 Prosopis juliflora Works best at pH 11 Diaz et al. (1999)
Spice
12 Trigonella Lowest suspended solids removal at pH 4 Mishra et al. (2003)
foenum-graecum Active coagulant is temperature and pH stable Ramamurthy et al. (2012)

form of natural high molecular weight polysaccharide is made
as a natural water clarifier and has been reported to work in
all types of waste waters. Hence, it is not surprising that
tannins became the first commercialized natural coagulant
instead of other plant sources.
Compared to alum, enhanced turbidity and color removal
from water sources have been reported owing to the use of a
weakly basic polymer which is formed by reacting tannin with
formaldehyde and aminoethanol (Bolto and Gregory, 2007).
Besides that, the use of tannin compounds is advantageous
over the studied natural coagulants as it requires no further
purification and isolation processes which could be both time
and economically challenged. Its relatively simple extraction
methods made it highly favored over other mucilaginous
plant extracts such as the cactus species which is beneficial to
the research and development aspect. Tannins which are
polyphenol compounds extracted from plants are also com-
monly ingested through dietary intakes and are ‘Generally
Recognized as Safe’ (GRAS) for the use as food additives in
various products (United States Environmental Protection
Agency, 2006). Despite that, contradictory effects on the
human health have been reported when tannins are consumed
in large quantities (Chung et al., 1998). However, the acceptable
daily intake (ADI) for tannins has yet to be established according
to the toxicological evaluation report (FAO, 1970).
The features highlighted could be viewed favorably as a
selling point to develop and promote tannins as a commercialized
plant-based natural coagulant in line with the urgency towards
sustainable water treatment. As potential investors, stake-
holders and suppliers discover the social-economic and envi-
ronmental values in developing tannins, the financial aspect
and market awareness are resolved easily; contributing to
successful commercialization.
7. Limitations and further improvements on the
current natural coagulant studies
Natural coagulants are known for their efficiency in reducing
turbidity but little is known about the characteristics and
properties of the resultant flocs formed. The knowledge on
these parameters such as floc strength, structure and com-
pactness could be the key in establishing the probable
coagulation theory (Li et al., 2006). The scanning of flocs
generated upon coagulation could be performed via various
microscopy imaging techniques such as Transmission Elec-
tron Microscopy. This could provide an overview on the
structure and surface characteristics which may lead to better
understanding on the bonding of colloidal particles (Idris et
al., 2013).
2186 J O U R NA L OF EN V I RO N M EN T A L S CI EN C ES 2 6 ( 20 1 4 ) 2 1 78–2 1 8 9
Fig. 2 – Factors hindering the commercialization of natural coagulants.
Extensive studies to conclude the respective coagulation
mechanism involved in each of the plant-based coagulants
are also limited. The aggregation of colloidal particles leading
to water clarification could be a result of one or more
coagulation mechanisms. Determination of the exact chem-
ical constituent responsible in inducing particle agglomera-
tions is extremely difficult owing to complexity of the process
and probable synergistic effects among the components
present. Further work involving isolation, purification and
characterization of the active agents would be beneficial to
identify the underlying compounds leading to coagulation. Only
a handful of such studies have been performed over the years
which include the studies on seeds of M. oleifera (Ghebremichael
et al., 2005; Okuda et al., 2001), Moringa concanensis (Sathiyabama,
2012), Vigna unguiculata and Parkinsonia aculeata (Marobhe et al.,
2007) and more recently, endosperm of Cocos nucifera (Fatombi
et al., 2013). Direct extraction of these compounds could
enhance the effectiveness of the overall coagulation process
owing to increased relative concentration of the agents. In fact,
the coagulant dosage required to achieve optimum coagulation
was also significantly reduced by 5 to 10 times when purified
protein of V. unguiculata was used instead of the crude extract
(Marobhe et al., 2007).
Although natural coagulants are green in nature, the use of
crude extracts has been related to the leaching of organic
matters into treated water; quantifiable in terms of total
organic carbon (TOC), dissolved organic carbon (DOC) and
others. Crude extracts contained various inorganic and organ-
ic biomolecules such as lipids which do not participate in
active coagulation (Ghebremichael, 2007). Increased levels of
organic matters in treated water would have serious implica-
tions on the subsequent disinfection process using chlorine.
These organic matters can act as precursors to the formation
of trihalomethanes (THMs) in which many are carcinogenic
(Duan and Gregory, 2003) and might also increase the required
chlorine demand for adequate disinfection (Anastasakis et al.,
2009). The use of purified active agents could tackle this
undesirable and problematic issue (Ghebremichael, 2007;
Sathiyabama, 2012). Protein purification via ion exchange
has successfully eliminated the additional nutrient and
organic loading introduced by the seeds of M. oleifera
(Ghebremichael, 2007). Partial purification of active agents in
legume; Phaseolus vulgaris has also been rewarding as the
organic loading content has been reduced by at least 16 times
in contrast to the use of crude extracts (Antov et al., 2010).
However, extraction methods that are economically feasible
would be needed for successful commercialization of natural
coagulants.
While the reviewed plant-based coagulants could be
considered as potential alternatives to chemical coagulants,
several issues such as the feasibility and sourcing of the
plants could be challenging. For instance, the toxicity of the
J. curcas seeds has raised safety issues for its application as a
natural coagulant for the treatment of drinking water
(Pritchard et al., 2009). One probable solution to counter for
the potential of poison leaching into water is to opt for the
non-toxic variety of seeds as they are safe for human
consumptions. Even so, further coagulation studies would be
necessary as this seed variety has yet to be tested for its
potential in water clarifications although both variants have
similarly high protein contents. As certain fruits are seasonal,
the availability of these plant-based coagulants throughout
the year could be dubious. The respective parts of the studied
coagulants such as foliage and pollen sheath would also be
difficult to collect for mass consumptions in real time
applications. Perhaps, plant-based coagulants that are avail-
able yearly with notable coagulation activities can be consid-
ered for industrial scale applications. The use of cereal crops
as natural coagulants could be complicated by the escalating
prices due to the growing world population and challenges in
keeping up with the agricultural productivity. In fact, the
universal rice utilization is forecasted to rise by 1.4% in years
2012 and 2013 although shrinkage by 2.7% in world cereal
production can be expected (FAO, 2012). In some cases, the
 JO U R N A L OF EN V I RO N M EN T A L S CI E NC ES 2 6 ( 20 1 4 ) 2 1 7 8–2 1 8 9
sole use of natural coagulants may be inadequate to achieve
the desired turbidity removal. However, they can certainly be
added as an aid to the latter (Bhole, 1995; Thakre and Bhole,
1985; Raghuwanshi et al., 2002; Swati and Govindan, 2005).
The blending of both coagulant types can reduce the reliance
on chemical coagulants while addressing the lower turbidity
removal and unavailability of certain plant-based coagulants
which may be seasonal.
8. Conclusions
Plant-based natural coagulants have garnered growing inter-
ests from researchers over the years due to their biodegradabil-
ity and environmental friendly nature. The diverse types of
plant-based coagulants including fruit waste and others (cac-
tus, cereals, fungus, nuts, shrubs and spice) as discussed in this
work have demonstrated promising coagulation activities in
treating turbid water. In addition, a number of these coagulants
can also provide primary disinfection against some of the
commonly present bacteria in surface water while others have
been found to be capable of removing heavy metals. For
commercialization, natural coagulants must be able to pene-
trate into the well-established market highly empowered by
chemical coagulants among the local communities. Although
natural coagulants are generally less superior in contrast to
alum, the blending of both coagulants in certain proportions
may prove beneficial in maintaining the water treatment
efficiency while gradually reducing the reliance on chemical
coagulants. Unlike chemical coagulants, studies on natural
coagulants have mainly focused on the turbidity removal from
synthetic and raw surface water with ample room for further
research. However, in-light with the health and environmental
concerns of chemical coagulants, there is an immediate need
for detailed research to identify the coagulation mechanism
and developing feasible methods for pretreating natural coag-
ulants as a sustainable alternative to chemical coagulants.
Acknowledgments
The authors are grateful to Monash University Malaysia for
providing the research scholarship and essential support for
this work. Sook Yan Choy is a recipient of the Higher Degree
by Research Scholarship (HDR) awarded by Monash University
Malaysia.
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