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Prof. Dr. Md. Shahin Hossain,

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Prof. Dr. Suksun

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Dr. Stefano Prof. Dr. Basir Mir, National Institute
Islamic University Syarif Hidayatullah
Stacul, University of Pisa, Italy of Technology Srinagar, India
Jakarta, Indonesia

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University, Australia Australia Sriwijawa University, Indonesia

Prof. Dr. Basuony El-Garhy, A/Prof. Ali Hassan Ali Mahfouz, Suez Dr. Noor Ul Hassan Zardari,
University of Tabuk, KSA Canal University, Egypt Universiti Teknologi Malaysia

Dr. Zeki Candan, Istanbul A/Prof. Dr. Nagaratnam Sivakugan, Prof. Dr. Ahmed Hassan, Beni-
University, Turkey James Cook University, Australia Suef University, Egypt

Prof. Dr. Paresh Vasantlal Dalal, Kavayitri

Dr. Nasser Najibi, City University Prof. Dr. Aylie Han, Diponegoro
Bahinabai Choudhari North Maharashtra
of New York, USA University, Indonesia
University, Jalgaon, India

Prof. Dr. Nazar Oukaili, Dr. Md. Nuralam Hossain, Chongqing Dr. Hidetaka Noritomi, Tokyo

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11/11/2020 Editorial Board | International Journal of GEOMATE
University of Baghdad, Iraq university, China Metropolitan University, Japan

Dr. Abdul Naser Abdul Dr. Roohollah Kalatehjari, Auckland Dr. Furqan Ahmad, Dhofar
Ghani, Universiti Sains Malaysia University of Technology, New Zealand University, Oman

Dr. Abbasali Taghavi

Dr. Mary Ann Adajar, De La Salle Dr. Md Faiz Shah, University of
Ghalesari, University of Texas at El
University, Philippines Jeddah, Saudi Arabia
Paso, TX, USA

Dr. Aria Fathi, University of Texas Dr. Melito Baccay, Technological University Dr. Duc Bui Van, Hanoi University
at El Paso, TX, USA of The Philippines of Mining and Geology, Viet Nam

Dr. Trung Ngoc Ngo, University of

Wollongong Australia
International Journal of GEOMATE, Jan., 2017, Vol. 12, Issue 29, pp. 46-52
Geotec., Const. Mat. & Env., ISSN: 2186-2982(P), 2186-2990(O), Japan

ADSORPTION STUDIES OF LEACHATE ON COCKLE SHELLS

Zawawi Daud1, Mahmoud Hijab Abubakar1, Aeslina Abdul Kadir1, Abdul Aziz Abdul Latiff1, Halizah
Awang2, Azhar Abdul Halim3, Aminaton Marto4
1
Faculty of Civil and Environment Engineering, Universiti Tun Hussein Onn Malaysia
2
Faculty of Technical and Vocational Education, Universiti Tun Hussein Onn Malaysia
3
Faculty of Science and Technology, Universiti Kebangsaan Malaysia
4
Faculty of Civil Engineering, Universiti Teknologi Malaysia

ABSTRACT: Sanitary landfills are important means of disposing municipal solid waste in developing
countries. However, these landfills are associated with the generation of leachate, which if untreated may
pose severe public health risk and may damage the ecosystem in the long term. In this study, cockle shells
were explored as an adsorbent media for the treatment of a stabilized landfill leachate. The optimum shaking
speed, pH, and dosage for chemical oxygen demand (COD) parameter removal were investigated using the
adsorbent media of particle sizes ranging from 2.00 mm to 3.35 mm. Leachate characteristics were then
determined. Results indicated that leachate is non-biodegradable with high concentrations of COD (1763
mg/L), ammonia nitrogen (573 mg/L), and biochemical oxygen demand/COD (0.09). The optimum
conditions for shaking were determined at 150 rpm according to the adsorption of COD by the media.
Optimum pH and dosage was 5.5 and 35 g/L, respectively. The adsorption isotherms indicated that Langmuir
isotherm is better fitted than Freundlich isotherm.

Keywords: Cockle shells, dosage, Isotherm, Leachate, Optimum shaking speed, pH.

1. INTRODUCTION been explored as a possible treatment of kitchen

wastewater, fruit waste has also been analyzed for
Leachate is the wastewater generated from the the removal of heavy metal in wastewater, and the
biochemical reaction that occurs inside a waste application of certain crops has been postulated for
deposit in a sanitary landfill. The process occurs the removal of heavy metal from specific
when waste undergoes physical, chemical, and contaminated soils [22–24]. Although adsorption
biological decomposition under aerobic and through activated carbon is extremely popular,
anaerobic conditions. Leachate usually contains only a few studies focus on the application of
dissolved contaminants, volatile organic acids, cockle shells (CS) as a substitute of conventional
toxic heavy elements, and high concentrations of media in landfill leachate treatment. Cockle is
organic matter, chemical oxygen demand (COD), small, edible, marine bivalve molluscs living along
ammonia nitrogen, and biochemical oxygen sandy beaches. In this study, loose CS was
demand (BOD5) [2–7]. When leachate containing experimentally investigated to determine the
high levels of dissolved contaminants is directly optimum parameter of agitation speed, pH, and
discharged into the environment, it may dosage in the removal of COD from a stabilized
contaminate soil and water bodies, seriously landfill leachate.
threatening the environment and public health [8–
13].
Many conventional landfill leachate treatments 2. MATERIALS AND METHOD
involve high-technology processes. To meet
discharge standards, the conventional methods that 2.1 Sampling
generate residues are saddled with high initial and
operational costs and low applicability to a wide The leachate sample was collected manually
variety of pollutants, among others [14–21]. In from Simpang Renggam municipal landfill site in
recent years, an increasing number of research Johor, located at latitude 10 53’41.64” N and
looks into the potential application of other
longitude 1030 22’34.68” E in Kluang District.
adsorbents (e.g., agricultural waste or natural
polymers and by-products of industrial processes) [25]. The initial size of the area was only
to achieve appropriate leachate treatment or as an approximately 8 acres, which was insufficient to
alternative approach to conventional media for the accommodate the high volume of waste being
treatment of pollutants that exist wastewater. transported.
For example, gravel sand and peat soil have The landfill receives roughly 250 tons of waste

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every day. Hence, the government has established All samples were assessed in triplicate under
a new sanitary landfill beside the existing one to identical conditions, and the average was obtained.
cater for the volume of waste transported from the The adsorbent dose was determined by applying
surrounding districts [26]. 8–64 g/L of the adsorbent. Samples were analyzed
Raw leachate samples were collected from the for COD, which is one of the major contaminants
influent of the detention pond in clean 20-L high- in leachate. The COD in mg/L was measured using
density polyethylene plastic containers, were an ultraviolet-visible spectrophotometer (HACH
transported to the wastewater research laboratory, DR6000) [27]. The quantity of the adsorbed COD
and were stored at 4 °C in a cold room at per unit CS was evaluated using Equation (1).
Universiti Tun Hussein Onn Malaysia (UTHM) to
minimize any change in their initial characteristics. (𝐶𝐶𝑜𝑜 −𝐶𝐶𝑒𝑒 )V
𝑞𝑞𝑒𝑒 = (1)
All chemical analyses for leachate characterization m

were performed within the following 24 h in

accordance with the Standard Methods for the Where Co = initial concentration in leachate (mg
Examination of Water and Wastewater [27]. All L−1),
chemicals used were of analytical grade. Ce = leachate concentration at equilibrium (mg
L−1),
2.2 Adsorbent Preparation V = leachate volume (L),
m = adsorbent mass (g).
The CS were obtained from several
commercial restaurants in Batu Pahat area in Johor. The COD percentage removal (%) was evaluated
The preparation was conducted according to the with equation (2).
procedure outlined by [28, 29]. The CS were
brushed and washed thoroughly with tap water, (𝐶𝐶𝑜𝑜 −𝐶𝐶𝑒𝑒 )
Removal (%) = x 100 (2)
rinsed with distilled water, and air-dried for 24 h. 𝐶𝐶𝑜𝑜
These samples were then oven-dried at 105 °C and
air-cooled to room temperature before being 3. RESULTS AND DISCUSSION
pulverized. Subsequently, the shells were sorted
into crushed sizes from 2.0 mm to 3.35 mm [13]. 3.1 Chemical analysis of leachate
The chemical composition of the media was
determined using an X-ray fluorescence Numerous published studies describe the
spectrometry (Model Bruker S4 Pioneer), whereas variations in leachate quality from different
its density was obtained conventionally (dry landfills [28]. Table 1 presents the characteristics
weight/volume). Table 2 indicates the composition of the leachate used in this study. The leachate has
of the CS. a high amount of COD, ammonia nitrogen, and
iron (Fe) (see Table 1). The average values of
BOD5 and COD are 164 and 1763 mg/L,
Formula Cockle shell (%)
respectively. The biodegradability ratio
CO2 0.10 (BOD5/COD) of a raw leachate ranges from 0.06
to 0.15 with an average of 0.09 (see Table 1). The
SiO2 0.30
data of the BOD5 and COD indicate that the
Fe2O3 0.80 leachate is evidently stabilized.
K2O 3.55 A stabilized leachate usually has high NH3-N
CaO 92.00 (>400 mg/L) and COD (<3000 mg/L) but low
biodegradability ratio [2]. The pH of leachate
Na2O 0.92
ranges from 7.85 to 8.26 with an average of 8.11,
and it usually increases with time, reflecting the
2.3 Batch study
decrease in concentration of the partially ionized
free volatile fatty acids [3]. A previous research
The optimum equilibrium conditions for batch
has shown that the pH of a stabilized leachate is
study were determined at ambient temperature at a greater than 7.5 [30]. Untreated samples in this
fixed time of 105 min for shaking speed and pH study indicated a stabilized leachate. The
using 8 g of media and 100 ml of raw leachate or concentrations of Fe are presented in Table 1. The
80 g/L of biosorbent concentration. The agitation Fe concentration in raw leachate ranges from 2.89
speed was changed from 50 to 200 using an orbital to 9.22, with an average value of 6.79. The amount
shaker (DAIKI), and the pH was adjusted from 2 of Fe falls outside the recommended values of the
to 10 using sodium hydroxide and hydrochloric leachate standard in Malaysia.
acid.

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Table 1 Characteristics of leachate obtained from Simpang renggam landfill.

Parameter Minimum Maximum Average *

Concentration Concentration Malaysia
in sample in sample Leachate discharge
Standard (mg/L)
COD (mg/L) 1682 1844 1763 400
BOD5at 20 °C (mg/L) 114 270 164 20
Ammonia Nitrogen (mg/L) 649 541 573 5
SS (mg/L) 585 671 633 50
Color 4615 4721 4676 100
(Platinum unit, Pt-Co) 0.06 0.15 0.09
BOD5/COD 7.85 8.26 8.11 6.0 – 9.0
pH 9.22 2.89 6.79 5.0
* Acceptable condition for discharging leachate as stated in the 2009 Environmental Quality Regulations,
Second Schedule (Regulation 13)
shaking speed. Thus, the condition after
3.2 Effect of shaking speed equilibrium is possibly caused by the extremely
high kinetic energy of the molecules and adsorbent
Figure 1 illustrates the COD percentage removal in particles that limited their interaction with each
the sample after shaking at 50, 100, 150, and 200 other [31]. Hence, 150 rpm was selected for further
rpm in an orbital shaker. The optimum removal for study.
COD by the adsorbent occurs at 150 rpm. At the
beginning of adsorption, the adsorption increases 3.3 Optimum pH
simultaneously with the agitation speed. After
reaching 150 rpm, the adsorption dissipates even Figure 2 exhibits the percentage removal rate
with a further increase in the shaking speed. in the sample after the pH is adjusted from 2 to 10
Therefore, the adsorption may have attained and at an agitating speed of 150 rpm. A gradual
equilibrium at 150 rpm (28%), such that no further increase is evident in the percentage uptake by the
improvement can be attained. adsorbent up to pH5.5 (53%), and the uptake
decreases from pH6 to pH10 (see Figure 2).

Fig.1 COD removal at 50,100, 150 and 200

shaking speeds
Fig.2 COD removal at pH,2, 3,4,5,6, 7,8,9 and 10
This adsorption behavior may be due to the fact
that the initial kinetic energy of the adsorbents and
When the pH increases in the solution, the number
that of the leachate molecules increase as the
of negatively charged sites increases, whereas that
shaking speed increases. Consequently, the
of the positively charged sites decreases, thereby
probability of interaction between the molecules
resulting in an electrostatic attraction between the
and adsorbent becomes significant; hence, the
charged particles. The uptake process increases
amount of adsorbate increases until it reaches the
until it reaches equilibrium.The decrease in the
equilibrium state. After reaching equilibrium, the
uptake with an increase in pH from pH6 may be
adsorption diminishes even with the increasing

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 International Journal of GEOMATE, Jan., 2017, Vol. 12, Issue 29, pp. 46-52

caused by the dissociation that occurs at the solid finite adsorption sites are available on the
to liquid boundary because of the acid and base adsorbent surface and that any further adsorption
interaction [32]. The optimum pH condition for the can no longer be completed after these sites are
COD removal is at pH5.5 (see Figure 2). occupied [35,36]. The Langmuir isotherm is
represented by Equation (3).
3.4 Optimum dosage
1 qm b.Ce
= (3)
qe 1+b.Ce
The effect of the adsorbent dosage on
adsorption was evaluated with an agitation speed
Where
of 150 rpm, a pH of 5.5, and an adsorbent mass
𝑞𝑞𝑒𝑒 =Equilibrium sorption capacity (mgg-1)
ranging from 8 g/L to 64 g/L. From the beginning, 𝐶𝐶𝑒𝑒 =Equilibrium concentration of the
the percentage removal increases with the increase adsorbate (mg L-1)
in the adsorbent dose until it reaches an optimum 𝑞𝑞𝑚𝑚 = maximum amount of adsorbate per unit
mass of 35 g (55%); then, the percentage removal weight of adsorbent (mgg-1)
begins to decrease with a further increment of the 𝑏𝑏 = Langmuir constant related to binding sites
adsorbent dose (see Figure 3). This behavior can affinity with adsorbate (L mg-1)
be explained considering that when the amount of
adsorbent increases, the amount of available The linearized Langmuir equation is expressed as
adsorption sites increases until the optimum mass follows:
is reached; any further increase in the adsorbent
dose may result in aggregation, which can decrease 1 1 1 1
= +� �� � (4)
qe qm qm .b Ce
the probability of molecules contacting all
available adsorption sites [33, 34].
The maximum amount of adsorbate (qm) taken in a
given system can be evaluated from the isotherm.
1 1 1
A linear plot of versus gives the slope as
𝑞𝑞𝑒𝑒 𝐶𝐶𝑒𝑒 𝑞𝑞𝑒𝑒
1
and intercept .
𝑞𝑞𝑚𝑚

3.5.2 Freundlich Isotherm.

Freundlich isotherm is an empirical model
that explains heterogeneous surface adsorption in
which the surface concentration of the adsorbate
on the adsorbent increases with the increase in the
initial concentration of the solution [36]. This
isotherm can be denoted as
𝟏𝟏�
𝒏𝒏
𝒒𝒒𝒆𝒆 = 𝑲𝑲𝒇𝒇 . 𝑪𝑪𝒆𝒆 (5)
Fig 3. Optimum dosage for COD removal
The linearized equation is as follows:
3.5 Adsorption equilibrium 𝟏𝟏
𝒒𝒒𝒆𝒆 = 𝑲𝑲𝒇𝒇 + 𝒍𝒍𝒍𝒍𝒍𝒍𝑪𝑪𝒆𝒆
𝒏𝒏
Adsorption equilibrium is usually plotted in the (6)
form of adsorption isotherm (at constant
temperature) with the amount adsorbed and mass Where
in the effluent fluid placed on Y- and X- axes, 𝑲𝑲𝒇𝒇 = freudlich constant
respectively. The isotherm study explains the 𝒏𝒏 = constant relating to adsorption intensity
process of adsorption and the interaction between
the adsorbent surface and adsorbate. Langmuir and A linear plot of 𝑙𝑙𝑙𝑙𝑙𝑙𝐶𝐶𝑒𝑒 versus 𝑙𝑙𝑙𝑙𝑙𝑙𝑞𝑞𝑒𝑒 gives the
Freundlich isotherm equations have been widely 1
slope as and intercept 𝑙𝑙𝑙𝑙𝑙𝑙𝑘𝑘𝑓𝑓 .
used for the equilibrium modeling of adsorption 𝑛𝑛
systems.
Figures 4 and 5 illustrate the Langmuir and
Freundlich isotherms, respectively. The linear plot
3.5.1 Langmuir Isotherm. of both isotherms implies that both are favorable
Langmuir isotherm analyzes the formation of a for the experimental data obtained. However, the
monolayer adsorbate onto the adsorbent surface. Langmuir model has higher coefficient of
This isotherm is based on the assumption that determination (R2) values than the Freundlich

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 International Journal of GEOMATE, Jan., 2017, Vol. 12, Issue 29, pp. 46-52

model, indicating that the former fits better than The ability of the CS adsorbent to minimize COD
the latter. The adsorption on the adsorbent is from leachate solution is investigated. The results
characterized by a monolayer coverage [26]. indicate that the optimum conditions of shaking
speed, pH, and dosage for COD removal are 150
4. CONCLUSION rpm, pH5.5, and 35 g/L, respectively.

Table 2. Langmuir and freundlich adsorption isotherm model parameters for COD on cockle shells

Dosage 𝑿𝑿 = (𝑪𝑪𝒐𝒐 − 𝑪𝑪𝒆𝒆 ) 𝟏𝟏� 𝟏𝟏�

(g/L) 𝑪𝑪𝒆𝒆 (𝒎𝒎𝒎𝒎/𝑳𝑳) (𝒎𝒎𝒎𝒎/𝑳𝑳) 𝒒𝒒𝒆𝒆 (𝒎𝒎𝒎𝒎/𝑳𝑳) 𝑪𝑪𝒆𝒆 𝒒𝒒𝒆𝒆 𝒍𝒍𝒍𝒍𝒍𝒍𝑪𝑪𝒆𝒆 𝒍𝒍𝒍𝒍𝒍𝒍𝒒𝒒𝒆𝒆
8 1128.08 634.92 79.37 0.00089 0.01260 3.05234 1.89963
16 1044.90 718.10 44.88 0.00100 0.02228 3.01907 1.65207
24 943.36 819.64 34.15 0.00106 0.02928 2.97468 1.53341
32 816.25 946.75 29.59 0.00116 0.03380 2.91183 1.47108
48 846.44 916.56 19.09 0.00135 0.05237 2.92760 1.28092

literature on alternative media for leachate

0.06000 treatment, especially in developing countries.
y = 83.781x - 0.0613 Further research is in progress at the UTHM to
0.05000
R² = 0.9909 determine other factors that may affect the field
0.04000 study.
1⁄𝑞𝑞𝑒𝑒

0.03000
ACKNOWLEDGEMENTS
0.02000
The authors acknowledge the research grant
0.01000
provided by the Office for Research, Innovation,
0.00000 Commercialization and Consultancy Management
(ORICC) of the Universiti Tun Hussein Onn
Malaysia.
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