Special Issue on Biological Engineering & Natural Science, May 2014

ISSN: 2347-6818 2014 | Published by The Standard International Journals (The SIJ) 1



AbstractLeachate treatment is important because of its possibility to contaminate the environment. The main
objective of this research was to investigate the efficiency of Aloe Vera (AV) and Chitosan (CS) as coagulant
and coagulant aids for removing colour and suspended solids from landfill leachate. Anaerobic leachate was
collected from Dennis Town Landfill site, located at Parit Buntar, Perak, Malaysia. Higher colour and SS
removals were recorded at FeCl
3
dosage of 1100 mg/L with 91.3% and 93.5% reduction, respectively.
Meanwhile, 10 000 mg/L of AV removed 66.7% of colour. SS reduction by CS was 18.8 % at 5 mg/L, and at
20 mg/L, 37.74 % of colour was removed. The optimum pH for FeCl
3
as main coagulant was at pH 6 and the
optimum pH for both AV and CS were at pH 9, respectively. AV as coagulant aid removed 97.3% of colour
and 97.2% of SS. On the hand, CS as coagulant aid was able to remove 98.64 % and 100 % of colour and SS,
respectively. The results showed that, AV and CS removed colour and SS better when used as a coagulant aid
compared to when it is used alone.
KeywordsAloe Vera; Anaerobic; Chitosan; Coagulant aid; Ferric Chloride; Landfill.
AbbreviationsAloe Vera (AV); Chitosan (CS); Ferric Chloride (FeCl
3
); Suspended Solids (SS).

I. INTRODUCTION
OAGULATION and flocculation is a process
commonly used in water and wastewater treatment
[Amudaa & Amoo, 2007]. The coagulation-
flocculation process is a physical-chemical method which is
more suitable to be used for old or stabilized leachate [Zainol
et al., 2012]. The efficiency of coagulation and flocculation
process can be influenced by many factors such as, type and
dosage of coagulant/flocculant, pH, mixing speed and time,
temperature and retention time. By optimizing these factors,
the process efficiency will be influenced [Rui et al., 2012].
There are three successive stages in coagulation process:
formation of coagulant, destabilization of colloid/particle, and
particle aggregation. The two earlier steps, coagulant
formation and colloid/particle destabilization are stimulated
during rapid mixing stage. Particle aggregation is taking
place during flocculation stage. At this stage, the interparticle
collisions form large flocs particle amenable to separation
from treated water [Jiang & Graham, 1998]. Coagulation
mechanism occurred depends on type of coagulant use. There
are four kinds of mechanism: double layer compression,
sweep flocculation, adsorption and charge neutralization and
adsorption and interparticle bridging.
Typically, inorganic salts of Al and Fe are used for water
and wastewater treatment [Zouboulis et al., 2007]. Among
these inorganic coagulants, iron salts are often more efficient
than aluminum [Ghafari et al., 2009]. The metal salts
commonly used as coagulants are aluminium sulfate (alum),
ferrous sulfate, ferric chloride and ferric chloro-sulfate
[Hassan et al., 2009]. Coagulants such as ferric chloride or
polymer can destabilize the colloidal materials in water and
wastewater. Addition of coagulants also caused the small
particles to agglomerate into larger settleable flocs [Amudaa
& Amoo, 2007]. Ferric Chloride (FeCl
3
) can be found in
liquid, crystal or anhydrous form. Usually the liquid form is
the most common. For liquid and crystal form, it must be
handled with similar care as hydrochloric acid because both
are extremely corrosive [Bratby, 2006]. When FeCl
3
was
added to the leachate, Fe3+ and its hydrolyzed products can
interact with negative colloids and then neutralize their
charge. These make the colloids to destabilize. The colloids
can become positively charged by absorbing cations when the
appropriate dosage is over [Rui et al., 2012].

C
*Professor, School of Civil Engineering, Universiti Sains Malaysia (USM), 14300 Nibong Tebal, Penang, MALAYSIA.
E-Mail: cehamidi{at}usm{dot}my
**School of Civil Engineering, Universiti Sains Malaysia (USM), 14300 Nibong Tebal, Penang, MALAYSIA.
E-Mail: ctfatihah88{at}gmail{dot}com
Hamidi Abdul Aziz* & Siti Fatihah Ramli**
Coagulation-Flocculation of Anaerobic
Landfill Leachate using Ferric Chloride
(FeCl
3
), Aloe Vera (AV) and Chitosan (CS)
Special Issue on Biological Engineering & Natural Science, May 2014
ISSN: 2347-6818 2014 | Published by The Standard International Journals (The SIJ) 2
There is a concern on a possibility for metal salts may
induce Alzheimer disease and carcinogenic properties.
Therefore, an alternative to use natural organic coagulants is
been proposed [Rizzo et al., 2007]. Natural coagulants are
mostly polysaccharides or protein. They have their own
advantages such as, they are cost-effective, unlikely to
produce treated water with extreme pH and also highly
biodegradable. There are many plant-based coagulant have
been reported, but the most well-known types are Nirmali
seeds, Moringa oleifera, Tannin and Cactus [Vijayaraghavan
et al., 2011].
In this research, we are focusing on Aloe Vera and
Chitosan as a plant/animal-based coagulant or coagulant aid.
Aloe Vera is a natural polysaccharides comprising of both
mono- and polysaccharides. The word aloe comes from
Arabic word alloeh which means radiance. Aloe plant
can be found in warm tropical areas and not suitable in
freezing temperature. Fresh leaves of aloe Vera can produce a
sticky colorless gel obtained from paren-chymatous cells in
the leaves. This clear sticky gel is known as aloe gel or often
called as aloe vera. The gel is composed mainly of water
(99%) and mono- and polysac-charides (25% of the dry
weight of the gel) [Wani et al., 2010].
Chitosan, which is produced by deacetylation of chitin
(one of the most simple biopolymers), has been investigated
as a coagulant/flocculant for sludge withdrawal from the
natural and waste water [Bergamasco et al., 2009] . Chitin is
a nontoxic, environmentally friendly, high polymer molecule
weight, which can be obtained from skeleton subtances of the
shell of crustaceans such as crabs, shrimp and prawns. Chitin
is also a linear polymer of chitobiose and virtually insoluble
in water and organic solvents [Sanghi & Bhattacharya, 2005].
II. MATERIALS AND METHOD
2.1. Leachate Sampling and Characterization
The leachate samples were collected from a closed landfill at
Parit Buntar, Perak, Malaysia. The collection and
preservation of samples were done in accordance with the
Standard Methods for the Examination of Water and
Wastewater (APHA, 2005) [Zainol et al., 2012]. The samples
were tested for pH, Biochemical Oxygen Demand (BOD
5
),
Chemical Oxygen Demand (COD), Suspended Solids (SS),
turbidity, ammoniacal nitrogen and colour. The
characteristics of the leachate are listed in table 2.
2.2. Preparation of Ferric (I I I) Chloride
Ferric Chloride (FeCl
3
) solution was prepared by dissolving
FeCl
3
.6H
2
O into distilled water. The solution should only be
made when it is needed in order to avoid aging. After aging
for 24 hours, the solution is kept in a cold place.
2.3. Preparation of Aloe Vera and Chitosan
Collected fresh Aloe Veras were repeatedly washed under
running water to remove dirt and other impurities. After that,
water was allowed to dry before being weighed. 100 g of
Aloe Vera were weighed and mixed with 100 mL of distilled
water. The mixture was blended by using a domestic blender
operated at high speed. Then, the mixture was filtered by
using a cloth filter. The solution was measured once again to
determine the final volume. The Aloe Vera stock solution can
be used immediately for coagulation test or after storing at
4
o
C.
The prawn shells chitosan was obtained from Chito-
Chem (Malaysia). 100 mg of Chitosan powder was weighed
and mixed with 10 mL of 0.1 M HCL in a beaker. The
solution was kept aside for about 1 hour to dissolve. Then,
the mixture was diluted with 100 mL of distilled water. This
solution was prepared daily [Patel & Vashi, 2013].
2.4. J ar Test
Coagulation test was performed by using jar test equipment
(SW6 Stuart Bibby Scientific Limited, UK). 3M NaOH and
3M HCl were used to adjust the pH sample. The study
involved rapid mixing, slow mixing and sedimentation in a
batch process. 500 mL of leachate samples were filled into
six beakers and agitated simultaneously, and the rotational
speed were varied accordingly, allowing simulation of
different mixing intensities and resulting flocculation process
[Mokhtar et al., 2011].
III. RESULTS AND DISCUSSION
3.1. Characteristics of Leachate
Value for physico-chemical parameters of landfill leachate
are listed in Table 1. Sample from the landfill is categorized
as partially stabilize leachate since its BOD
5
/COD ratio is
0.27 [Alkassasbeh et al., 2009]. Therefore, coagulation and
flocculation may work well for this type of leachate [Huang
& Chen, 1996]. Colour may be associated with organic
matter present in the leachate. COD comes from
biodegradable and non-biodegradable organics. Some of
them may be in suspension which could be settled in
coagulation and flocculation processes.
Table 1: Characteristics of Raw Leachate from Parit Buntar Landfill
No Parameters Value
1

1 pH 7.51
2 BOD
5
(mg/L) 150.6
3 COD (mg/L) 551.13
4 Suspended Solids (mg/L) 80.67
5 Ammoniacal nitrogen (mg/L NH
3
-N 292.
6 Colour (Pt.Co) 2570.83
7 Turbidity (NTU) 21.44
1
An average of 5 samples were taken from June until October 2013
3.2. Removal Rate
In order to establish a practical understanding on coagulation
performance and to find the optimum pH of coagulant,
dosage of coagulant and also dosage of coagulant aid, a
numerous number of coagulation test to treat leachate were
conducted.
Special Issue on Biological Engineering & Natural Science, May 2014
ISSN: 2347-6818 2014 | Published by The Standard International Journals (The SIJ) 3
3.2.1. Effect of pH on Coagulation
In this study, a wide pH range from 4-9 were selected. Figure
1 showed the effect of pH on Suspended Solids (SS) and
colour removal, when Ferric Chloride (FeCl
3
), Aloe Vera
(AV) and chitosan were used as main coagulants. In order to
determine the optimum pH, the dosage of FeCl
3
, AV and CS
were constant at 1100 mg/L, 4000 mg/L and 30 mg/L,
respectively. The graph showed that the optimum pH for
FeCl
3
was at pH 6. At this optimum pH, the removal rates for
SS and colour were 95.2 % and 94.2 % respectively. As pH
values increased from 4-6, the removal rate for both SS and
colour showed increment, but when pH value was higher than
optimum pH (pH 6), the removal rates of both parameters
started to decrease. In coagulation process, pH is very
important because it controls hydrolysis species. A numbers
of soluble hydrolysis species are formed when FeCl
3
is added
into sample. Depending on the pH value, the species can
either be positive or negative charge. A positively charged
species will formed at lower pH (<6) and at higher pH, it will
be negative charged. Since leachate is negative charge, the
positively hydrolysis species can absord the colloidal
particles and destabilizes them. This is called charge
neutralization mechanism [Aygun & Yilmaz, 2010]. The
optimum pH for AV was obtained at pH 9. As pH values
increase from 4-9, SS removal efficiency increased from 13
% (pH4) to 21.7 % (pH 9). On the other hand, colour removal
efficiency fluctuated throughout the pH values. A better
removal rate was found at pH 9 with 33.3 % colour removal.
The optimum pH for CS was also at pH 9. At this pH value,
the percentage removal for colour was 54.56 % and 3.53 %
for SS. From the graph, CS showed less removal of SS
compare to AV but it removed colour better than AV at both
acidic (pH 4) and basic (pH 9) condition. At pH 4 and pH 9,
CS removed 32.51 % and 56.54 % of colour compared to AV
with 27.8 % and 33.3 % removals, respectively. At acidic
solution, CS becomes a positively charged coagulant due to
the protonation of amino groups. Therefore, CS tends to
attract and bind to leachate which is negatively charged
surface via hydrogen bonding [Sakkayawong et al., 2005]. At
basic condition, the hydroxyl group in CS changed and
become deprotonated hydroxyl group and binds with the
sample by covalent bond [Boonurapeepinyo et al., 2011].

Figure 1: Percentage Removal of SS and Colour as a Function of
Coagulant Dosage
3.2.2. Effect of Dosage on Coagulation

Figure 2: Percentage Removal of SS and Colour by using Ferric
Chloride

Figure 3: Percentage Removal of SS and Colour by using Aloe Vera

Figure 4: Percentage Removal of SS and Colour by using Chitosan
Figure 2, 3 and 4 shows the effect of FeCl
3
, AV and CS
dosages on SS and colour removal rate respectively. In this
test, the pH value was constant at pH 5 for FeCl
3
, pH 6 for
AV and pH 4 for CS. The coagulation and flocculation was
conducted between ferric chloride dosages of 1000-1500
mg/L. At concentration 1100 mg/L ferric chloride, the SS
removal rate was 93.5 %. The highest colour removal rate
was also recorded at concentration 1100 mg/L, with 91.3 %.
This is the optimal concentration of ferric chloride to remove
SS and colour. Colour removal efficiency decreased by
increasing FeCl
3
dosage. This probably because, higher
concentration of FeCl
3
itself imparted colour into the leachate
-80
-60
-40
-20
0
20
40
60
80
100
3 4 5 6 7 8 9 10
R
e
m
o
v
a
l
,

%
pH
Colour
(FeCl3)
SS
(FeCl3)
Colour
(AV)
85
86
87
88
89
90
91
92
93
94
900 1000 1100 1200 1300 1400 1500
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Colour
SS
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SS
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SS
Special Issue on Biological Engineering & Natural Science, May 2014
ISSN: 2347-6818 2014 | Published by The Standard International Journals (The SIJ) 4
[Zin et al., 2013]. Compare to FeCl
3
, AV was not good
enough for SS removal, the results gave negative values
which means no removal of SS at all. This was probably
because of inadequate destabilization of colloidal particles
[Ersoy, 2005]. On the other hand, colour removal showed an
increment with the increase of AV dosages. The optimum
colour removal efficiency was found at 10 000 mg/L with
removal rate of 66.7 %. The removal of SS using CS is better
compared to AV. The highest SS removal was found to be at
5 mg/L with 18.8 % removal. As the dosage of CS increases
from 5 mg/L to 30 mg/L, the percentage removal of SS
decreases. This could happen when colloidal surfaces adsorb
the excess polymer and produced restabilized colloids. Due to
this, the particles surfaces were left with no more sites
available for the formation of interparticles bridges and
positively charged restabilized particles can cause the
electrostatic repulsion among the suspended solids [Hassan et
al., 2009]. The color removal was increased with increase of
coagulant dose until 20 mg/L with 37.74 % removal. Above
20 mg/L, the colour removal shows a decrement. At higher
concentration, particle surface received positive charges from
coagulant, thus redispersing the particles [Patel & Vashi,
2013].
3.2.3. Effect of Coagulant Aid on Coagulation
Polyelectrolytes are commercial coagulant aids. It can either
be natural or synthetic polyelectrolyte. Usually, high
efficiency can be achieved with a small amount of
polyelectrolyte dosage. The density and molecular weight of
polyelectrolyte play important role in coagulation processes.
Metal coagulant dosage can be reduced when polyelectrolyte
is use as coagulant aid [Aygun & Yilmaz, 2010]. Figure 5
and 6 showed the percentage removal of SS and colour when
AV and CS were used as coagulant aid respectively. Based
on the graph, the optimum dose for AV to act as coagulant
aid when FeCl
3
1100 mg/L at pH 6 was 4000 mg/L and the
optimum dose for CS as coagulant aid was 25 mg/L. At this
optimal dose, AV removed 97.2 % SS and 97.3 % color.
Meanwhile, CS removed 98.64 % of colour and 100 % of SS
at its optimal dose. CS removed colour and SS better than AV
because CS as coagulant aid has high positive charges
compared to AV and this condition helps the flocks to form
quickly and increase the rate of sedimentation [Hesami et al.,
2013]. When FeCl
3
was used alone, the percentage removal
of SS was 93.5 %) and color was 91.3 %. Even though the
different between main coagulant and coagulant aids was
insignificant, but AV and CS still showed it potential to be
used as coagulant aid. At higher concentration of AV (above
optimum dose), the removal rate for both SS and color
decreased. This because at optimum (4000 mg/L) AV
concentration was expected to forms a bridge between
particles and can cause a good flocculation. However, when
concentration of polyelectrolyte increase, an envelope on the
suspending particles will be formed and caused them to
remain in suspension, thus the removal rate decreased
[Aygun & Yilmaz, 2010].

Figure 5: Percentage Removal of SS and Colour by using Ferric
Chloride and Aloe Vera as Coagulant Aid

Figure 6: Percentage Removal of SS and Colour by using Ferric
Chloride and Chitosan as Coagulant Aid
IV. CONCLUSION
The optimum pH and dosage for SS and colour removal of
FeCl
3
was found to be at pH 6 and 1100 mg/L respectively.
Higher SS and colour removal efficiency of Aloe Vera was
found at pH 9. Meanwhile, varying the dosage of Aloe Vera
did not affect the removal of SS since there was no removal,
but for colour, the optimum concentration was at 10 000
mg/L. The optimum pH for CS was found to be at pH 9 and
dosage of 20 mg/L for colour removal. Meanwhile, higher SS
removal of CS was at dosage of 5 mg/L. The test also showed
that, AV and CS had a potential to be used as natural
coagulant in leachate, even though the removal was
insignificant.
ACKNOWLEDGMENT
This research was supported by the Universiti Sains Malaysia
under RU Team Research Grant (1001/PAWAM/854005).
Thanks are due to the Majlis Perbandaran Taiping, Perak for
their cooperation during the study.
0
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Special Issue on Biological Engineering & Natural Science, May 2014
ISSN: 2347-6818 2014 | Published by The Standard International Journals (The SIJ) 5
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Hamidi Abdul Aziz is a professor in
environmental engineering in the School of
Civil Engineering of Universiti Sains
Malaysia. Professor Aziz received his PhD
degree in civil engineering (environmental
engineering) from the University of
Strathclyde in Scotland in 1992. To date, he
has published over 200 refereed articles in
professional journals and proceedings, 16
chapters in refereed international books, and 8 chapters in refereed
national books. He has also published 7 research books. Dr Aziz
continues to serve as a peer reviewer for more than 30 international
journals. Professor Aziz's research focuses on alleviating problems
associated with water pollution issues from industrial wastewater
discharges and from solid waste management via landfilling, such as
landfill leachate. Advanced oxidation processes is one of his
research focuses. He also has strong interest in biodegradation and
bioremediation of oil spills.
Siti Fatihah Ramli is a degree holder and
graduated from School of Engineering,
Universiti Sains Malaysia. Currently she is
doing her Master degree in Environmental
Engineering at the same university. Her
current research is focusing on how to treat
leachate using natural coagulant.