Potential Use of Fruit Seeds and Plant Leaves as Coagulation Agent in Water Treatment

Journal of Environmental Treatment Techniques

2020, Volume 8, Issue 3, Pages: 971-977

J. Environ. Treat. Tech.

ISSN: 2309-1185

Journal web link: http://www.jett.dormaj.com

Potential Use of Fruit Seeds and Plant Leaves as

Coagulation Agent in Water Treatment

Khalida Muda*, Nur Shahidah Aftar Ali, Ummu Nusaibah Abdullah, Ahmad Bazli Sahir

Department of Water and Environmental, School of Civil Engineering, Universiti Teknologi Malaysia, 81310 Johor Bharu, Johor, Malaysia

Received: 19/02/2020

Accepted: 16/06/2020

Published: 20/09/2020

Abstract

The treatment of turbid water by coagulation-flocculation was found to be the most common and cost-effective method. Over the years,

chemical coagulants have been widely applied to enhance the coagulation process. However, the utilisation of chemical coagulants exhibits

several drawbacks, including generation of voluminous sludge and being non-biodegradable as well as toxic compounds to aquatic life. Due

to global concerns over the harmful effects, the application of natural coagulants is a promising solution. Therefore, this study was conducted

to investigate the potential of plant-based natural coagulants to replace chemical coagulants for water treatment. Fruit seeds (Carica papaya,

Nephelium mutabile, and Euphoria malaiense seeds) and plant leaves (Pandanus, Centella asiatica, and Cymbopogon citratus leaves) were

selected as natural coagulants in this study. A series of jar tests were performed using raw water from a water treatment plant. The effects of

pH and coagulant dosage were evaluated based on the turbidity removal and coagulation activity. Of all the examined plants, the Carica

papaya seeds appeared to be the best coagulant for water treatment. An optimum dose of 130 mg/L of this coagulant resulted in a 95.5%

turbidity removal and 94% coagulation activity, at optimum pH 7.5. Overall, this study reveals the potential use of fruit seeds and plant leaves

as coagulation agents in the water treatment process.

Keywords: Natural Coagulants, Turbidity, Coagulation Activity, Carica papaya seeds, Water treatment

Introduction¹

Water is essential to all living organisms as it is the most

generation of large volumes of sludge, are non-biodegradable,

and cause detrimental effects to human health and aquatic life (2,

). The generation of voluminous sludge which is non-

fundamental nutrient to life. Safe and readily available water is

crucial for human health to avoid various diseases due to the

presence of harmful bacteria or chemicals in water. However,

lack of access to clean water has become one of the world’s

biggest problems, especially in developing countries. According

to Vaithiyanathan et.al (1), India is suffering from water crisis

which mainly due to improper wastewater and solid waste

management, where the population only able to access 4% of

usable water sources. Thus, effective water treatment is required

to remove undesirable compounds and contaminants so that the

water is safe to use for different purposes. A common way to treat

turbid water is by using coagulation. Coagulation is a physical-

chemical process for water treatment which is typically applied

prior to the sedimentation and filtration processes. The

application of coagulants in the coagulation-flocculation process

is necessary as they are able to remove high suspended solids and

colloidal particles in the water, thus enhancing the quality of

treated water. The common chemical-based coagulants used in

water and wastewater treatment are aluminium sulphate, ferric

sulphate and iron (III) chloride (2-4). Karbassi and Pazoki (5)

noted that addition of PAC could remove 99% of turbidity in

petrochemical wastewater. Despite their efficiency, these

chemical coagulants suffer from several drawbacks such as the

biodegradable has become a major problem when chemical

coagulants are used in water and wastewater treatment. Therefore,

it is essential to replace chemical coagulants with a more

sustainable approach to counteract the drawbacks.

Recently, investigations on the usage of natural coagulants in

water and wastewater treatment have caught the attention of many

researchers. Natural coagulants exhibit many advantages when

compared to the application of chemical coagulants in many

aspects. They are highly biodegradable (4), non-corrosive(7),

generate a lower amount of sludge (8), environmentally friendly,

and cheap (7). Moreover, they are less likely to produce treated

water with high pH level. Several studies have demonstrated that

natural coagulants extracted from plants, animals and

microorganisms such as chitosan, Moringa oleifera, Quercus

robur acorn, Cicer arietinum, banana pith, Jatropha curcas seeds,

rice starch, and dragon fruit foliage have excellent efficiency in

removing high turbidity in water and wastewater treatment (9-16).

Jatropha curcas seeds, dragon fruit foliage and Sterculia

foetida seeds achieved high turbidity removals of 99%, 99.2%,

and 97%, respectively (9, 15, 17). The application of Cicer

arietinum showed high turbidity and suspended solid removals of

6% and 87%, respectively (14). Meanwhile, the addition of

orange peel as a natural coagulant was able to remove 96% of

Corresponding author: Khalida Muda, Department of Water and Environmental, School of Civil Engineering, Universiti Teknologi

Malaysia, 81310 Johor Bharu, Johor, Malaysia. E-mail: Khalida Muda. Email: khalida@utm.my.

Journal of Environmental Treatment Techniques

2020, Volume 8, Issue 3, Pages: 971-977

turbidity (18). Furthermore, the addition of natural coagulants

extracted from nature can reduce costs and produce high quality

treated water. The application of natural coagulants could

increase the formation of flocs, thus improving the removal of

suspended particles in water during the coagulation process.

Although natural coagulants have many advantages, their

application as coagulation agents has not been entirely explored

in water treatment.

promote particle collision in the water and further facilitate the

particle aggregation to form flocs (20). After slow mixing, the

flocs were then left to settle for 30 min. Residual turbidity was

measured as - 푇 . The same jar test was carried out without

푓푐

coagulants and the residual turbidity was measured as - 푇_푓_푏.

Coagulation activity was calculated as:

Coagulation activity (%): [ ( T_f_b- T_f_c) / T_f_b] x 100

(1)

In this study, selected natural coagulants extracted from the

seeds and leaves of plants: Carica papaya seeds, Nephelium

mutabile seeds, Euphoria malaiense, Pandanus leaves, Centella

asiatica leaves, and Cymbopogon citratus leaves have been

utilised for water treatment purposes. Unnisa and Bi (19) studied

the application of Carica papaya seeds as a natural coagulant to

remove turbidity and the results showed that Carica papaya were

able to remove 100% of water turbidity. However, Nephelium

mutabile seeds, Euphoria malaiense seeds, Pandanus leaves,

Centella asiatica leaves and Cymbopogon citratus leaves have

not been explored as much. Thus, this study aims to investigate

the coagulation potentials of these natural coagulants compared

to chemical coagulants for the treatment of turbid water.

.4 Analytical Methods

A pH meter and nephelometer were used to measure the pH

and turbidity of water samples. To determine the optimum

condition, the pH of water sample was kept constant at 7.5, while

natural coagulants varied between 10 mg/L to 130 mg/L, in order

to obtain the optimum dosage. The pH value was varied between

to 12 with a constant value of optimised dosage, to determine

the effects of pH on treating water. All tests in this study were

conducted according to the standard methods of water and

wastewater treatment (21).

Result and Discussions

.1 Physical Properties of Natural Coagulants

Table 1 shows the physical properties of the fruit seed and plant

Materials and Method

.1 Materials

leaf-based natural coagulants. Carica papaya seeds had the

highest initial weight of 333g, while the Cymbopogon citratus

leaves had the lowest initial weight of 74g as shown in Table 1.

After undergo the drying and grinding process, the highest yield

weights were shown by the Nephelium mutabile seeds with 240

g, followed by 201 g for the Euphoria malaiense seeds, 55 g for

the Carica papaya seeds, 14 g for the Cymbopogon citratus

leaves, 13 g for the Pandanus leaves, and 9 g for the Centella

asiatica leaves.

Among the natural coagulants, the Nephelium mutabile seeds

had the lowest moisture content of 20.5 % and this contributed to

a greater yield. In contrast, the Centella asiatica leaves had the

highest moisture content at 89.5 % and resulted in the lowest

yield. Table 1 clearly shows that that moisture content plays an

important role in determining the yield. Thus, it can be concluded

that the Nephelium mutabile seeds as natural coagulants are

efficient in terms of yield properties.

The water samples were collected from an inlet point at the

Sultan Ismail Water Treatment Plant (WTP), located near

Universiti Teknologi Malaysia, Johor. Fruit seeds and plant

leaves: Carica papaya seeds, Nephelium mutabile seeds,

Euphoria malaiense seeds, Pandanus leaves, Centella asiatica

leaves and Cymbopogon citratus leaves were collected from the

surrounding neighbourhood and local market.

.2 Preparation of natural coagulants

After collecting the materials, the whole seeds of Carica

papaya, Nephelium mutabile and Euphoria malaiense were dried

in an oven at a temperature between 103°C to 105°C for 24 hours.

After drying, they were ground into a fine powder using a grinder.

Meanwhile, the fresh Pandanus, Centella asiatica and

Cymbopogon citratus leaves were first washed using tap water,

chopped and oven dried for 24 hours at a temperature between

03°C to 105°C. The dried leaves then were crushed into a fine

powder using a mortar pestle. The powder obtained from both

fruit seeds and plant leaves were sieved with a mesh size of

Table 1: Physical Properties of Natural Coagulants

Initial

Weight Weight

Dry

Moisture

Content

(%)

Yield

.4mm and mixed with three different solutions, including

Materials

(

deionised water, sodium hydroxide, NaOH and sodium chloride,

NaCl. A 10 mg sample of powder from the fruit seeds and plant

leaves were weighed and suspended in 200 mL of each solution.

The solution was vigorously mixed for 10 min using a mechanical

stirrer to extract the coagulation active component, and then

filtered. The filtered solutions, called crude extracts, were kept in

a refrigerator at 4°C. The crude extracts then can be used as a

coagulant for water treatment without any further preparation.

(g)

Carica papaya seeds

Nephelium mutabile

seeds

333

16.5

79.5

83.5

302

240

201

20.5

38.7

Euphoria malaiense

Euphoria malaiense seeds

Pandanus leaves

Centella asiatica leaves

Cymbopogon citratus

leaves

328

61.3

16.9

10.5

81.0

89.5

18.9

83.1

.3 Coagulation Test

This study used the jar test to determine the coagulation

activity of each type of seeds and leaves. Raw turbid water (500

mL) was filled into six beakers and 5 mL of the natural coagulants

were added to each beaker. The beaker was rapidly mixed at 200

rpm for 1 minute before slow mixing was applied for about 15

minutes at 60 rpm. The purpose of rapid mixing was to properly

disperse the coagulant, while a slow speed mixing was used to

.2 Effects of Solvents on Natural Coagulants

Deionised water, sodium chloride (NaCI) and sodium

hydroxide (NaOH) were tested in the study to obtain the best

solvent to extract natural coagulants. The best solvent was chosen

based on the highest removal performance achieved by the natural

Journal of Environmental Treatment Techniques

2020, Volume 8, Issue 3, Pages: 971-977

coagulants. Fig.1(a) and Fig.1(b) show the performance of natural

coagulants in the deionised water. Based on Figure 1(a), the

Nephelium mutabile seeds had the highest turbidity removal of

coagulants when sodium chloride, NaCI was added as the solvent.

The NaCI solution achieved optimum concentration at 2.0 M as

shown in Figure 2(a). At the concentration of 2.0 M, the Pandanus

leaves had the highest turbidity removal of 59.2%. This was

followed by the Cymbopogon citratus leaves, Centella asiatica

leaves, Nephelium mutabile seeds, Carica papaya seeds and

Euphoria malaiense seeds with removal rates of 59.1%, 55.9%,

34.6%, 31.8%, and 28.6%, respectively. For coagulation activity,

based on Figure 2(b), the Pandanus leaves showed the greatest

activity at 43.1%, followed by the Cymbopogon citratus leaves,

Centella asiatica leaves, Nephelium mutabile seeds, Carica

papaya seeds, and Euphoria malaiense seeds with coagulation

activities of 40%, 38.6%, 20.8%, 18.5%, and 18.5%, respectively.

From the results, it is clearly seen that all the natural coagulants

were unable to achieve high removal performance and

coagulation activity in the NaCl solution. This means that the

NaCI solution is also not suitable to be used as a solvent in water

treatment. Figure 3(a) and Figure 3(b) show the performance of

natural coagulants in a sodium hydroxide, NaOH solution.

1.5% in deionised water compared to the Carica papaya seeds

(

31.3%), Euphoria malaiense seeds (30.1%), Pandanus leaves

11.6%), Centella asiatica leaves (9.9%), and Cymbopogon

citratus leaves (9.4%). Figure 1(b) also shows that the Nephelium

mutabile seeds had the highest coagulation activity among the

natural coagulants at 10.5%. The coagulation activity for the

Carica papaya seeds, Euphoria malaiense seeds, Pandanus

leaves, Centella asiatica leaves and Cymbopogon citratus leaves

were 10%, 8.7%, 6.8%, 4.6%, and 4%, respectively. However,

based on the results displayed in both figures, all the natural

coagulants show a low performance in turbidity removal and very

low coagulation activity when deionised water was used as the

solvent. Therefore, it can be concluded that deionised water is not

suitable to be used as a solvent due to its low capability to extract

selected fruit seeds and plant leaves compared to NaOH and

NaCI.

Figure 2(a) and Figure 2(b) show the performance of natural

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Cymbopogon Citratus leaves

0.2

0.5

0.1

0.2

0.5

Concentration of NaCI (M)

(a)

(b)

Figure 1: (a) Turbidity removal and (b) Coagulation activity of natural coagulants using deionised water

Carica

Nephelium

Euphoria

Malaiense

seeds

Pandanus

leaves

Centella Cymbopogon

Carica

Nephelium

Euphoria

Malaiense

seeds

Pandanus

leaves

Centella Cymbopogon

Papaya seeds Mutabile

Asiatica

Citratus

Papaya seeds Mutabile

seeds

Asiatica

leaves

Citratus

leaves

seeds

leaves

Natural Coagulants

(

(b)

Figure 2: (a) Turbidity Removal and (b) Coagulation Activity of natural coagulants using NaCI solution

Journal of Environmental Treatment Techniques

2020, Volume 8, Issue 3, Pages: 971-977

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Cymbopogon Citratus leaves

100

0.2

0.5

0.2

0.5

Concentration of NaOH (M)

(a)

(b)

Figure 3: (a) Turbidity Removal and (b) Coagulation Activity of natural coagulants using NaOH solution

The optimum concentration obtained by the NaOH solution

was similar to NaCI at 2.0 M.Based on Figure 3(a), among all the

natural coagulants, the Carica papaya seeds had the highest

turbidity removal of 94.5% Meanwhile, the turbidity removal

achieved by the Cymbopogon citratus leaves, Pandanus leaves,

Euphoria malaiense seeds, Nephelium mutabile seeds, and

Centella asiatica leaves were 90.2%, 87.3%, 86.2%, 84.7%, and

an increment in the dosage. In contrast, it is observed that a high

coagulant dosage has a slightly adverse effect towards removal

performance. In the case of the Euphoria malaiense seeds, the

removal performance decreased from 91.7% to 90.4% as the

dosage increased from 70 to 90 mg/L. The performance of natural

coagulants shown in Figure 4(b) are associated with the

performance shown in Figure 4(a). It is clearly seen that the

Carica papaya seeds has a higher coagulation activity of 95.4%

while the Centella asiatica leaves has the lowest coagulation

activity of 89%.

1.7%, respectively. The results in Figure 3(a) show similar

trends with Figure 3(b), where the Carica papaya seeds also had

the highest coagulation activity of 92.6%, followed by the

Cymbopogon citratus leaves, Pandanus leaves, Euphoria

malaiense seeds, Nephelium mutabile seeds, and Centella asiatica

leaves with coagulation activities of 88.9%, 84.7%, 83%, 78.9%,

and 74.6%, respectively. All the natural coagulants in the NaOH

solution show high performance when compared to the other

solutions of NaCI and deionised water. This is due to the high

efficiency of the NaOH solution in extracting more coagulant

agents from these plant-based natural coagulants, which resulted

in a high coagulation activity, thus leading to a higher turbidity

removal. Therefore, it can be concluded that the NaOH solution

is the best solvent required to extract natural coagulants in water

treatment.

3.5 Effect of pH on Natural Coagulants

The pH is another important factor for coagulation efficiency.

During the coagulation process, the surface charge of coagulants

may be affected by the pH (22). Coagulants with a low surface

charge might cause the slow growth of flocs particle, thus leading

to low removal performance in water treatment. Therefore, it is

crucial to conduct jar tests to determine the optimum pH in

treating turbid water. Figure 5(a) shows the effect of varying pH

on turbidity removal by the natural coagulants while Figure 5(b)

shows the pattern of coagulation activity occurring during the

experimental work at various pH values. The pH values varied

from 2, 4, 7.5, 10, to 12, at constant dosage (130 mg/L). Based on

the figures, the best pH value to remove turbidity was at pH 7.5,

while the lowest percentage removal of turbidity was at pH 12.

All the natural coagulants showed removal trends where the

percentage of removal increased from pH 2 and rapidly decreased

after pH 7.5. Based on Figure 5(a), at optimum pH 7.5, the Carica

papaya seeds contributed the highest turbidity removal of 95.6%,

followed by the Nephelium mutabile seeds, Cymbopogon citratus

leaves, Euphoria malaiense seeds, Pandanus leaves and Centella

asiatica leaves with removal rates of 94.1%, 93%, 91.3%, 89.2%,

and 87%, respectively. Figure 5(b) demonstrates that the

coagulation activities of all natural coagulants showed positive

effects when the pH value is increased. It is noticeable that most

coagulation occurred at pH 7.5, compared to other pH value. The

highest coagulation activity in Figure 5(b) is also shown by the

Carica papaya seeds with a value of 96.7%. In contrast, the

Centella asiatica leaves had the lowest coagulation activity of

.4 Effect of Dosage on Natural Coagulants

Coagulation efficiency can be determined by considering

several factors, including coagulation dosage (22). To achieve

excellent results in water treatment, it is important to determine

the optimum conditions during the coagulation process. This is

because a high coagulation dosage may inhibit the high removal

performance of coagulants in water treatment (19). Figure 4(a)

and Figure 4(b) show the performance of each natural coagulant,

under various dosages. The pH was kept constant at 7.5.

Based on Figure 4(a), the 130mg/L dosage was selected as the

optimum coagulant dosage as it showed the highest turbidity

removal. At the optimum dosage, Carica papaya seeds had the

highest turbidity removal of 95.5%, while the Cymbopogon

citratus leaves, Euphoria malaiense seeds, Nephelium mutabile

seeds, Pandanus leaves and Centella asiatica leaves had turbidity

removals of 93.4%, 93%, 92%, 90.5%, and 90.2%, respectively.

It is clearly shown in Figure 4(a) that the coagulant dosage

significantly affects the turbidity removal efficiencies. The

removal performance for all the natural coagulants increase with

6.1%. Of all the pH values investigated, pH 7.5 was the optimum

for all the natural coagulants as both results showed the highest

turbidity removal and coagulation activity

Journal of Environmental Treatment Techniques

2020, Volume 8, Issue 3, Pages: 971-977

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Cymbopogon Citratus leaves

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Cymbopogon Citratus leaves

Dosage (mg/L)

110

130

110

130

Dosage (mg/L)

(

(b)

Figure 4: Effect of various coagulant dosage on (a) Turbidity Removal and (b) Coagulation Activity of different natural coagulants

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Cymbopogon Citratus leaves

Carica Papaya seeds

Euphoria Malaiense seeds

Centella Asiatica leaves

Nephelium Mutabile seeds

Pandanus leaves

Cymbopogon Citratus leaves

100

7.5

pH Value

(b)

7.5

pH Value

(a)

Figure 5: Effect of various pH on (a) Turbidity Removal and (b) Coagulation Activity of different natural coagulants

Carica papaya seeds

(

Alum

Carica papaya seeds

Alum

Materials

(b)

Figure 6: Comparison performance of (a) Turbidity Removal and (b) Coagulation Activity between Carica papaya seeds and Alum

.6 Potential Use of Natural Coagulant in Water Treatment

This study further compared the performance of a natural

removal and coagulation activity. Figure 6(a) and Figure 6(b)

show the performance comparison between natural coagulant

(Carica papaya seeds) and chemical coagulant (alum). The test

was carried out at optimum conditions (coagulation dosage of 130

mg/L and pH 7.5). The results showed that the natural coagulant

acts as a better coagulant agent compared to alum.

coagulants with a chemical coagulant. The potential use of natural

coagulants in water treatment can be determined through this

comparison. In the present study, the Carica papaya seeds was

selected as the best coagulant as it produced the highest turbidity

Journal of Environmental Treatment Techniques

2020, Volume 8, Issue 3, Pages: 971-977

Based on Figure 6(a), the Carica papaya seeds managed to

remove almost 95.5% of turbidity, compared to alum which could

only remove water turbidity by up to 73%. Based on Figure 3(b),

the coagulation activity of alum was only 20.8%, lower than the

Carica papaya seeds which exhibited a high coagulation activity

of 94%. Thus, based on the results, it can be proven that Carica

papaya seeds (natural coagulant) has a tremendous potential to

treat polluted water and is superior to alum (chemical coagulant).

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Conclusions

In terms of yield properties, the Nephelium mutabile seeds are

sufficient to be used as natural coagulants. This is due to the

Nephelium mutabile seeds having the lowest moisture content of

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0.5% which resulted in a greater yield. All the natural coagulants

react the best in a sodium hydroxide solution (NaOH) compared

to deionised water and sodium chloride solution (NaCI). The

NaOH solution achieved the optimum concentration at 2 M which

contributed to higher turbidity removal and coagulation activity

in the Carica papaya seeds at 94.5% and 92.6%, respectively. At

optimum condition (130 mg/L dosage and pH 7.5), the Carica

papaya seeds appeared to be the best coagulant with the highest

turbidity removal of 95.6% and coagulation activity of 94%. This

study also proved that natural coagulants have a higher efficiency

in treating turbid water compared to chemical coagulants. At

optimum condition, the Carica papaya seeds contributed to

excellent turbidity removal of 95.6% and coagulation activity of

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Acknowledgment

This research was financially supported by Research

University Grant of Universiti Teknologi Malaysia (GUP-UTM)

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Ethical issue

Authors are aware of all the publication ethics and adhere to

the publishing requirement. The manuscript is an original work

and not under consideration for publication elsewhere and has not

been published elsewhere in the same form, in English or in any

other language. The manuscript does not involve any studies

related to human participants or animals performed by any of the

authors.

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as a Plant-based Coagulant for Treatment of Palm Oil Mill Effluent

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Competing interests

The authors declare that there is no conflict of interest that

could have appeared to influence the work reported in the paper.

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Authors’ contribution

All authors have contributed in writing, gathering

experimental data and analysis. All the authors have worked

together to complete the research and mutually agree to submit

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