Accepted Manuscript

Title: Sequestering of Pollutants from Public Market

Wastewater using Moringa oleifera and Cicer arietinum
Flocculants

Authors: Rosmawanie Mohd, Radin Mohamed, Adel

Al-Gheethi, Fadzilla Pahazri, Amir Hashim, Shaylinda Mohd
Zin

PII: S2213-3437(18)30156-8
DOI: https://doi.org/10.1016/j.jece.2018.03.035
Reference: JECE 2276

To appear in:

Received date: 8-12-2017

Revised date: 15-3-2018
Accepted date: 16-3-2018

Please cite this article as: Rosmawanie Mohd, Radin Mohamed, Adel Al-
Gheethi, Fadzilla Pahazri, Amir Hashim, Shaylinda Mohd Zin, Sequestering
of Pollutants from Public Market Wastewater using Moringa oleifera
and Cicer arietinum Flocculants, Journal of Environmental Chemical
Engineering https://doi.org/10.1016/j.jece.2018.03.035

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Sequestering of Pollutants from Public Market Wastewater using Moringa

oleifera and Cicer arietinum Flocculants

Rosmawanie Mohd, Radin Mohamed*, Adel Al-Gheethi*, Fadzilla Pahazri, Amir Hashim,

Shaylinda Mohd Zin

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Micro-pollutant Research Centre (MPRC), Department of Water and Environmental

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Engineering, Faculty of Civil and Environmental Engineering, Universiti Tun Hussein Onn

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Malaysia (UTHM), 86400 Parit Raja, BatuPahat, Johor, Malaysia

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*Corresponding author E mail: adel@uthm.edu.my; maya@uthm.edu.my;

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Research highlight
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 The use of M. oleifera resulted in the highest removal for BOD5, COD and O&G from
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the public market wastewater

 Adsorption of COD by M. oleifera was fitted to both the Langmuir and Freundlich
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isotherms, while the Freundlich isotherm was the best model to study COD and O& G
removal by C. arietinum.

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The natural coagulants are applicable for improving the quality of public market

wastewater.
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Abstract

The present study aimed to investigate potential of Moringa oleifera and Cicer arietinum seeds
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for the treatment of public market wastewater in comparison to Alum and FeSO4. The

flocculation process was assessed as a function of adsorbent dose (60-360 mg/L), pH (4 to 9)

and mixing rate (50 to 300 rpm). The adsorption study was performed to find out the removal

of biological oxygen demand (BOD5), chemical oxygen demand (COD), total suspended solids

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(TSS), oil and grease (O&G), colour, and turbidity in a lab-scale plant system (6 L). The results

revealed that the use of M. oleifera resulted in the highest removal for BOD5, COD and O&G

(68.08%, 79.1 % and 83.3 % respectively) at 180 mg /L, pH 7 to 8, and a mixing rate of 150

rpm. The use of Alum resulted in the highest removal percentage for TSS, colour and turbidity

(87.17, 90.83 and 81.06% respectively) at 120 mg/L, pH 7 to 8, and a mixing rate of 150 rpm.

The Langmuir adsorption isotherm was the best model for the removal of turbidity by M.

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oleifera and C. arietinum (R2=0.91 and 0.93) compared to the Freundlich model (R2=0.81 and

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0.82). Moreover, the adsorption of COD (R2= 0.91) by M. oleifera was fitted to both the

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Langmuir and Freundlich isotherms. In contrast, the Freundlich isotherm was the best for

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studying the removal of COD (R2= 0.96) and O& G (R2=0.99) by C. arietinum. The findings

obtained indicated that natural coagulants are applicable for improving the quality of public

market wastewater. U
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Key words: Langmuir model, Freundlich model, Alum, Natural coagulants, lab-scale plant
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system
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1. Introduction
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The public market is an open food market selling poultry, fish, meat, fresh fruits and
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vegetables. These activities are associated with huge amounts of wastewater generated from the

cleaning of the market floor (Jais et al., 2017). Market wastewater is normally discharged into
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open drainage channels. The high content of nutrients and organic matter in this type of
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wastewater is associated with high concentrations of 5-day Biochemical Oxygen Demand

(BOD5), chemical oxygen demand (COD) and total suspended solids (TSS) as well as oil and
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grease (O&G). The high levels of O&G in wastewater contribute effectively to the attraction of

insects and thus the distribution of infectious agents which are harmful to both humans and

animals. Therefore, public market wastewater should be treated properly before disposal.

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 The current methods used for the treatment of public market wastewater include aerobic

and anaerobic sequencing batch reactors, flow anaerobic sludge blanket (UASB), multi stage

bubble column reactor, sequential batch reactor (SBR), fixed film anaerobic filter (AF),

expanded granular sludge bed (EGSB), flow septic tank/baffled reactor (USBR) and submerged

membrane hybrid system (Rahimi et al., 2011). These techniques are effective for the reduction

of COD, BOD5, and TSS in wastewater. Nevertheless, the challenge normally associated with

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these techniques is the high cost of operation and maintenance which limits the application

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these systems for each public market centre. These gaps offer opportunities for researchers to

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find low-cost and highly efficient alternatives which do not have secondary effects on the

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environment. In the few last years, scientists have been turning to the use of natural products

for the treatment of wastewater. This idea has been taken from the fact that nature has a high
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potential to repair itself if humans stop polluting the environment. Therefore, it is very
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important for researchers to discover natural resources which can be utilised for water treatment
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(Mohamad et al., 2016). In the water treatment process, the utilisation of natural coagulants has
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various advantages in comparison to the chemical agents and other traditional treatment
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processes particularly in terms of biodegradability, low toxicity and low residual sludge

production (Antov et al., 2012; Thakur and Choubey, 2014).

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The coagulation/flocculation process is a stage used during the treatment process of

wastewater after primary and secondary steps for removing soluble organic matters. They are
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effective for the reduction of BOD5, COD, and TSS (Muralimohan et al., 2014). Hence, in the

absence of solid matters in wastewater such as public market wastewater, the

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coagulation/flocculation process might be efficient for the improvement of wastewater quality

without the need for the primary and secondary processes. Moringa oleifera is one of the natural

coagulants with high adsorption potential due to the high contents of carboxyl, phosphate and

amino acid function groups which play an important role in the adsorption process of pollutants.

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Besides, the rapid growth of Moringa trees in subtropical and tropical areas make more

applicable for water and wastewater treatment. It known that leaves, seeds, roots and flowers

of M. oleifera with high contents of protein, minerals, β-carotene and antioxidant compounds

can be used for different application such as animal nutrition and traditional medicine (Hauwa

et al. 2016). Liu et al. (2008) revealed that the C. arietinum has high concentrations of essential

amino acids and sulphur containing amino acids in both fractions (albumins and globulins).

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These components make C. arietinum more efficiency in removing the suspended solids and

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heavy metals ions from the water and wastewater.

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The efficiency of M. oleifera as an alternative coagulant in place of conventional

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chemical coagulants in water treatment has been reported in the literature (Hamid et al., 2014;

Atiku et al., 2016). The usage of M. oleifera is much more effective compared to chemical
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coagulants since it has less sludge mass and produces no harmful effects on the surrounding
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environment (Pahazri et al., 2016). This alternative coagulant offers a number of advantages
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including easy implementation as individual treatment units for each public market, low cost in
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terms of available raw materials, less energy required for the operation in comparison to the
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traditional treatment system and high efficiency for the reduction of organic and inorganic

pollutants from different types of wastewater as revealed in previous studies. However, the use
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of natural coagulants such as M. oleifera seeds and Chickpea (Cicer arietinum) for public

market wastewater treatment has not investigated before which emphasises the novelty of the
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current work.

The removal of pollutants by coagulants through a process called adsorption is one of

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the most important discoveries in the environmental field. The mechanism of natural coagulants

is depends on the adsorption process which lead to adsorb the suspended solids as well as the

metal ions as a function of functional group available in their chemical composition (Al-Gheethi

et al. 2016b). It has a wide range of applications in wastewater treatment (Jodeh et al., 2016;

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Rahim and Garba 2016; Maher, 2016). The method is a cost-effective technology for treating

wastewater (Al-Gheethi et al., 2017). The adsorption technique is a process which depends on

the surface phenomenon which takes place through chemisorption and physisorption,

depending on the characteristics of the adsorbent surface and adsorbate (Adeleke et al., 2017).

The adsorption isotherms are used to describe the equilibrium between the adsorbate and the

adsorbent (Muthukumaran et al., 2016).

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Four different isotherm models namely Langmuir, Freundlich, Redlich-Peterson and

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Koble-Corrigan models have been reported for describing the relationship between the

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adsorbate on the adsorbent materials and the solution (Hor et al., 2016). Freundlich and

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Langmuir models are most commonly used to provide significant parameters for predicting

adsorption capacities. The widely used Langmuir and Freundlich isotherm models can be
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applied to explain the sorption mechanism in a different way. Regression equations of the
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converted Langmuir isotherm model are characterised by significantly higher values of the
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determination coefficient (Desta, 2013).

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However, the effectiveness of M. oleifera and C. arietinum as natural coagulants for the
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flocculation of public market wastewater has not investigated with the details of the Langmuir

and Freundlich model in a lab scale system yet. In the current study, the adsorption isotherms
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of COD, colour and turbidity from public market wastewater on M. oleifera and C. arietinum

seeds as the adsorbent were investigated using Freundlich and Langmuir models to explain the
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adsorption process as a response for adsorbent dosage, pH and mixing rate.

2. Materials and Methods

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2.1 Sample Collection and Materials

Public market wastewater samples were collected from Rengit Public Market located in Batu

Pahat, Johor, Malaysia (coordinate 1°40’46.4”N 103°08’48.1”E) (Appendix 1). Rengit Public

Market was selected as a sampling location because it represents a model for the wet public

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market which has different types of fresh foods. This market has operation hours between 8 am

to 1 pm. The grab samples were taken at five separate times from 8 am until 1 pm to cover the

average daily flow rate. The samples were collected in plastic containers and then transported

to the laboratory for chemical analysis. The characteristics of public market wastewater samples

which included BOD5, COD, TSS, O&G and colour were determined after filtering it through

a 0.45 micron membrane according to APHA (2005). Turbidity of the water sample was

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determined using a turbidimeter Model HACH 2100N-turbimeter based on the procedure

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described in Method 180.1. pH of the wastes samples was measured by using calibrated pH

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meter model session 3-P/N 51750-60. The characteristics of raw public market wastewater are

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illustrated in Table 1.

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2.2 Preparation of Coagulants

The Moringa oleifera seeds used in this study were acquired from India while C. arietinum was

obtained from a local supermarket at Batu Pahat, Malaysia. Both M. oleifera and C. arietinum

seed pods were allowed to mature and dry naturally until they turned brown. The seeds were

removed from the pods and dried in the sun while the external shells were removed. Dry seeds

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were obtained from a commercial seed supplier. Good quality seeds (not rotten) were shelled

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by hand and reduced to a fine powder using a laboratory blender (Appendix B). The seed kernels

were grounded into a fine powder which measured approximately 600 µm in size to achieve the

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solubilisation of active ingredients in the seeds (Muyibi et al., 2004; Al-Gheethi et al. 2016;

Mojad et al., 2017). Ferrous sulphate (FeSO4.7H2O) and aluminium sulphate (alum)

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[Al2(SO4)3.18H2O] salts (Fisher Scientific) were prepared in stock solutions with a
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concentration of 3% (w/v).
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2.3 Adsorption Experimental set up
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Factorial Complete Randomized Design (CRD) (5*3*𝒙) in triplicate was used to study the
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factors affecting the adsorption process of BOD, COD, TSS and O& G from public market

wastewater. Two natural coagulants (M. oleifera and C. arietinum), two chemical coagulants
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(Alum and FeSO4) and one (1) control for the adsorption process made a total of five (5) groups.

Three (3) factors included adsorbent dosage, pH and mixing rate while the value, 𝒙,wasused for
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each factor.
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A lab-scale plant system was designed to simulate the treatment of public market Rengit
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wastewater. The system was fabricated in rectangular shape tank with a dimension measuring

0.3 m in width, 0.3 m in length and 0.6 m in depth, a storage tank and 2 effluent collection tanks

(6 L in capacity for each) made of 2 pieces of acrylic board, 2 submersible water pumps, 1

paddle, 3 PVC pipes with control valves and 3 PVC pipes for inlet and outlet (Fig. 1a).

2.4 Operating System

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 Public market wastewater (4 L) was transferred into Tank 1 (Storage tank) and then into

the coagulation /flocculation treatment tank (Tank 2) (Fig. 1a). The coagulant dosage ranged

between 60 and 360 mg/L with a rapid mixing rate between 50 and 300 rpm for 5 mins and pH

values ranging between 4 and 9. After pH adjustment using NaOH (0.1 M) and HCl (0.1 N),

the desired adsorbent dosage was added and then kept at room temperature for a fixed duration.

The rapid mixing was followed by slow mixing of 30 rpm for 60 mins to ensure equilibrium

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conditions. The coagulants were separated after each experiment by the natural sedimentation

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process for 30 mins (Fig. 2b). The concentrations of BOD5, COD, TSS, O & G, colour, and

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turbidity in the supernatant were determined according to APHA (2005). The control sample

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was not treated with coagulants. The reduction efficiency (E %) was calculated according to

Eq. (1) (Adeleke et al., 2017).

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(𝐶𝑖−𝐶𝑒)
𝐸= × 100 (1)
𝐶𝑖
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Where Ci and Ce are the initial and equilibrium values of evaluated parameters of BOD5, COD,
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TSS, O&G, colour and turbidity

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2.5 Equilibrium study

The isotherm study of the adsorption process for COD, TSS, O&G and turbidity by M.
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oleifera and C. arietinum was done on a sample which consisted of 4 L of public market

wastewater. The initial concentration ranged from 650 to 5121 mg/L of COD, 42 to 350 mg/L
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of TSS, 154 to 2500 mg/L of O&G and 40.9 to 187 NTU for turbidity. The experiment was
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conducted at the best conditions determined in Section 2.4 (180 mg/L of dosage; pH 7 and 150
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rpm of mixing rate). In each tank, M. oleifera and C. arietinum were added separately into the

wastewater with a pH value of 7. The samples were rapidly mixed at 150 rpm for 5 min and

then slowly mixed at 30 rpm for 60 min.

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 The adsorption equilibrium was analysed using Langmuir and Freundlich isotherms to

find out the relationship between the pollutants adsorbed by M. oleifera and C. arietinum in the

wastewater samples. The linearised equations used in the isotherm model analyses are the

following;

Langmuir equation:

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𝐶𝑒/𝑞𝑒 = 1/𝑄𝑚𝑎𝑥 𝐾𝑙 + 𝐶𝑒/𝑄𝑚𝑎𝑥 (2)

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Where:

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qe is Equilibrium sorption capacity (mg/g)

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Ce is Equilibrium of concentration (mg/L)
Qmax is The maximum amount of pollutants from a complete monolayer on the surface (mg/g)

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k is Constant related to the affinity of binding sites (l/mg)
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Qmax was calculated according to Eq. 3
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𝐶𝑖 − 𝐶𝑓
𝑄𝑚𝑎𝑥 = 𝑉 × (3)
𝑀
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Where;
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V is the wastewater sample volume (L)

𝐶𝑖 is the initial pollutant concentration (mg L-1),

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𝐶𝑓 is the remaining pollutant concentration (mg L-1),

𝑀is the amount of coagulant on a dry basis (g).

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Freundlich equation:
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𝑙𝑜𝑔𝑞𝑒 = 1/𝑛𝑙𝑜𝑔𝐶𝑒 + 𝑙𝑜𝑔𝐾𝑓 (4)

Where:
Kf is Freundlich constants denoting the adsorption capacity (mg/g)
qe is Uptake of pollutant per unit weight of biosorption (mg/g)
Ce is Equilibrium of concentration (mg/L)

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n is Empirical constant indicating adsorption intensity (l/mg)

2.6 Scanning Electron Micrograph (SEM) Image

In order to determine the surface morphology of M. oleifera and C. arietinum seeds

before and after the coagulation/flocculation process. The scanning electron microscopy (SEM)

SUI510 was used as described by Ribeiro et al. (2016). The SEM was operated at an

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accelerating voltage of 5 kV and a magnification of 500 x. The samples were gold coated and

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then inserted into the SEM system for the scanning process (Teng et al., 2012).

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3. Results and Discussion

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3.1 Characteristics of raw public market wastewater

The characteristics of raw public market wastewater are illustrated in Table 1. It can be noted

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that the pH of raw samples ranged from 6.8 to 7.4 which is within the EQA 1974 (Standard A
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and B). These finding are in consistence with that reported by Sankararamakrishnan et al.
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(2007) who found that the pH of wastewater sample was between 6 and 8. However, Zulkifli et
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al. (2012) revealed that the pH of the wet market wastewater obtained from Pasar Ampangan
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ranged from pH 5.6 to 5.8. Jais et al., (2015) revealed that the pH of the Public Market

wastewater in Parit Raja was pH 6. The differences between pH of different wet market
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wastewater might be related the activities of the wet market which are differ seasonally and

geographically. BOD5 and COD concentrations were between 635 and 2350 mg/L and between
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710 and 5120 mg/L, respectively. These concentrations are higher than that reported by Jais et

al. (2015) for a public market wastewater at Parit Raja where BOD5 was 89 mg/L and COD
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was 456 mg/L. The high concentration recorded in this study might be due to the presence fresh

products of seafood. The high values of BOD and COD indicate to the high pollution level of

the investigated samples and thus the potential for increasing the pollution level of the

environment after the direct discharge is more possible. Therefore, these wastes should be

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treated before the final disposal process. Moreover, TSS was ranged from 42.7 to 350 mg/L.

These values were more than that revealed by Jais et al. (2015), where 132.3 mg/L was noted.

The characteristics of raw public market wastewater samples in the current work were exceeded

the standard EQA (2011).

3.2 Factors affecting the flocculation process

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3.2.1 Coagulant dosage

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The removal efficiencies of BOD5, COD, TSS, O&G, colour and turbidity from public

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market wastewater by M. oleifera and C. arietinum as well as Alum and FeSO4 at different

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adsorbent doses are presented in Fig. 2. The highest reduction of BOD5 was 65.59% and 60.46%

using 180 mg/L of M. oleifera and C. arietinum respectively. However, Alum exhibited a higher

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efficiency (72.78 %) at 120 mg/L (Fig. 2a). The reduction of COD by M. oleifera and C.
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arietinum was more than that recorded for BOD5 at the same dosage. It was also higher than
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the values recorded by Alum and FeSO4. The reductions were 85.39% and 70.38 % for M.
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oleifera and C. arietinum respectively and 75.59 % at 180 mg/L of alum and 67 % at 240 mg/L
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of FeSO4 (Fig. 2b). It has to mention that BOD is more specific than COD, and is a more reliable

measure of organic load reduction than COD which is a general and non-specific measure of
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oxidizable pollutants in water and wastewater. These values were higher than the ones reported

in previous studies on domestic wastewater in which the maximum reduction of BOD5 and
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COD using150 mg/L of M. oleifera were 32% and 48 % respectively (Asmawy et al., 2012).
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Alum has also been shown to be effective for the improvement of water quality. Therefore, it

may be used as a solution for clean water. However, it poses potential health hazards for both
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humans and biological diversity (Hayder and Rahim, 2015).

The optimum removal of TSS was noted at 240 mg/L of M. oleifera and C. arietinum

(84.07 and 81.16 % respectively). In contrast, Alum exhibited similar efficiency (84.73 %) at

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180 mg/L (Fig. 2c). These findings are similar to that reported by Asmawy et al. (2012) in

which Alum and M. oleifera showed similar efficiency in the removal of TSS from the

wastewater which ranged between 83.33 % and 91.43 %.

The natural coagulants appeared to be highly efficient in removing O&G. M. oleifera

reduced 98.47 % of O&G at 180 mg/L which was more than Alum (97.49 %) at the same

concentrations. On the other hand, C. arietinum reduced O&G by 94.81 % at 240 mg/L which

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was more than that recorded by FeSO4 (92.24%) (Fig. 2 d). The efficiency of M. oleifera in

achieving a high reduction in O&G might be related to the preparation procedure of M. oleifera

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coagulants. Muyibi et al. (2004) mentioned that the extraction of oil content from M. oleifera

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seeds using the method in this study contributed to the removal 83% of the oil contents which

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represents 25% of kernel weight. The studies conducted on M. oleifera without oil extraction
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indicated that the M. oleifera coagulant has limited efficiency in the removal of pollutants from
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wastewater (Daud et al., 2015).
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The highest reduction in colour was achieved by 180 mg/L of M. oleifera and C.

arietinum (83.23 % vs. 72.72 %) in comparison with chemical coagulants where the maximum
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reduction was 72.41 % by Alum at 120 mg/L and 61.66 % by FeSO4 at 180 mg/L (Fig. 2e). The

turbidity was reduced by 86.24% and 80.02 % using180 mg/L of M. oleifera and 180 mg/L C.
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arietinum respectively, while the highest reduction in turbidity was 81.5% at 120 mg/L of Alum
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and 56.33 % at 180 mg/L of FeSO4 (Fig. 2f). Colour and turbidity are one of the main problems
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of wastewater where the finely dispersed, suspended and colloid particles are responsible for

the colour of the wastewater (Rao, 2005). Therefore, both turbidity and colour should be
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removed from wastewater before the final disposal (Viera et al., 2009). The results obtained

here indicated that M. oleifera and C. arietinum are effective coagulants for reducing colour

and turbidity without the need for chemical additives.

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 The findings obtained in this study indicated that the natural coagulants are more

effective than the chemical substances in the reduction of public market wastewater parameters

except for BOD5. M. oleifera was more efficient than C. arietinum in the reduction of the

parameters. Nonetheless, the results noted that dosage concentrations should be considered

when the coagulants are used in the flocculation process. These findings are in agreement with

those reported by Reddy et al. (2011). Increasing adsorbent dosage is associated with the

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availability of more active sites for the adsorption process. However, the high concentrations

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of adsorbent might have negative effects due to the agglomeration between adsorbent molecules

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and the destabilisation of colloidal particulates when coagulants are used in high dosages.

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Another side effect of the increase in dosage is the rise of BOD5 due to the suspension of

particles. Asrafuzzaman et al. (2011) concluded that M. oleifera and C. arietinum show high
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percentages of turbidity removal (87.3% and 92.8% respectively) for dairy wastewater. This
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efficiency might be due to the chemical composition of the natural coagulants which contains
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high starch content that have the ability to coagulate with TSS and settle at the bottom of the
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tank.
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3.2.2 pH

The results for the reduction of public market wastewater using natural and chemical
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coagulants as a response to pH are depicted in Fig. 3. The results revealed that the optimum pH
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for achieving high-efficiency reduction for BOD5 by M. oleifera was 8 (69.65 %) while a value
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of 7 was the optimum pH for C. arietinum (68.08 %), Alum (69.61 %) as well as FeSO4 (53.91

%) (Fig. 3a). The reduction of BOD5 observed here was more than that reported by
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Sarparatzadeh et al. (2007) where the reduction was 60 % at a pH value of 8.

The optimal pH for the reduction of COD using M. oleifera and C. arietinum was 7

(84.49 % and 75.78 %, respectively).The same applies for FeSO4 but the maximum reduction

was 61.45%. In comparison, the optimum pH for Alum was 8 with a reduction efficiency of

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80.22% (Fig. 3b). The highest reduction of TSS by M. oleifera and Alum was noted at pH 8

(88.30 vs. 86.30 %) whereas the highest reduction was recorded at pH 7 for C. arietinum and

FeSO4 (83.64 vs. 80.71 %) (Fig. 3c).

A pH of 7 was found to be the best for the high reduction in O&G by M. oleifera and C.

arietinum (96.37 % vs. 93.93 %). In contrast, a pH of 8 was preferred for Alum and FeSO4

(94.25 % vs. 84.75 %) (Fig. 3d). M. oleifera was showed to be more effective in terms of colour

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reduction (85.70 %) at pH 8, at which FeSO4 also exhibited a maximum reduction in colour

(84.17%). Among different pH values, C. arietinum and Alum appeared to exhibit maximum

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efficiency at pH 7 (80.03 % and 90.08 % respectively) (Fig. 3e). The maximum reduction of

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turbidity by M. oleifera (83.71%) and C. arietinum (81.09 %) was recorded at pH 8. Alum was

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the most effective (94.36 %) at pH 8 while FeSO4 showed the highest efficiency (70.29 %) at
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pH 7 (Fig. 3f).
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The optimum pH value depends essentially on the properties of the water treated, type
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of coagulant used and its concentration (Sharma and Lee 2015). The pH of the wastewater

increases from 5.81 to 7.03 after the addition of different coagulants (Mohamed and Hashim,
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2014), indicating the role of coagulant type in raising the pH value. pH affects the network of

negative charge on the surface of the adsorbing surface, as well as the physical chemistry and
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hydrolysis of metal (Amuda and Ibrahim, 2006). The addition of M. oleifera has no effect on
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wastewater pH. Thus, no adjustment is required and this is a major advantage of M. oleifera as
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a coagulant. A pH between 7 and 8 for wastewater during the flocculation process is more

acceptable due to the present charge density on the surface of coagulants (Anteneh and Sahu,
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2014). The pH of wastewater should be between 7 and 8 to be free from substances that could

impair the treatment process or cause a violation of water quality standards of the receiving

waters (Muralimohan et al., 2014). Viera et al. (2010) revealed that M. oleifera keeps its

adsorption capacity at a pH around 7.2. In this study, the pH of the public market wastewater

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ranged between 6.8 and 7.4 which is required for an optimal flocculation process without the

need for chemical additives.

3.3 Application of Lab-scale Experiments for the Treatment System

The lab-scale experiment for public market wastewater treatment exhibited effective

results. These experiments were conducted under optimal operating parameters determined in

Section 3.1. The removal of BOD5, COD, TSS, O&G, colour and turbidity using chemical and

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natural coagulants is presented in Fig. 4. It can be noted that the use of M. oleifera resulted in

the highest removal for BOD5, COD and O&G (68.08%, 79.1 % and 83.3 % respectively) while

R
SC
the use of Alum resulted in the highest removal percentages for TSS, colour and turbidity (87.17

%, 90.83 % and 81.06 % respectively). FeSO4 was more effective for the removal of BOD5 and

U
COD compared to C. arietinum (61.29 vs. 56.64 % and 70.99 vs. 66.05 %, respectively) which
N
exhibited more efficiency for the removal of TSS, O&G, colour and turbidity (77.36 vs. 41.34
A
%, 69.45 vs. 52.8 %, 81.59 vs. 54.32 % and 70.08 vs. 60.12 %, respectively).
M

According to Malhotra et al. (2000), alum has the potential to remove 98% of turbidity

from wastewater and 65 % of COD. In contrast, the efficiency of M. oleifera seeds is due to the
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seed content (1% active polyelectrolyte’s) that neutralises the negatively-charged colloids in

dirty water (Mangale et al., 2012). Therefore, the use of natural coagulants may provide a safe
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solution for the treatment of wastewater. Moreover, it has to mentioned that the sludge resulted
E

from the utilization of natural coagulants such as M. oleifera and C. arietinum are quite different
CC

from that resulted from the chemical coagulants. The sludge generated from the natural

coagulants has no toxicity on the human or environment and then it can be recycle for different
A

applications. It can be used as a biofuel source due to the level of oils available in their

composition, these lipids contribute effectively in the removing of pollutants.

The characteristics of treated public market wastewater by using chemical and natural

coagulants are illustrated in Table 2. It can be noted that none of the chemical or natural

15
coagulants have reduced BOD5 to meet the standards limits required by EQA 1974 (regulation

2010). However, both alum and M. oleifera have achieved the standards limits for COD which

dropped to less than 200 mg/L. In contrast, only M. oleifera has reduced O&G to meet the

standards limits required by EAQ 1974, which indicate the high efficiency of natural coagulants

in reducing of O&G in comparison to chemical coagulants.

3.4 Adsorption Isotherms models

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Isotherm studies for the reduction of COD, TSS, O&G, colour and turbidity were

conducted in public market wastewater with different initial concentrations for each parameter.

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The experiments were performed under optimised conditions as reported in the previous section

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in which the dosage was 180 mg/L of M. oleifera and C. arietinum at a pH of 7. The mixing

U
time was chosen according to previous studies which indicated that 60 min is required for the
N
adsorption process to reach the equilibrium phase (Desta, 2013). Viera et al. (2010) revealed
A
that the removal of COD and turbidity from wastewater through the adsorption process is 99 %
M

with a contact time of 60 min. The adsorption equilibrium relationship for the reduction of

COD, TSS, O&G, colour and turbidity by M. oleifera and C. arietinum seeds as analysed using
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Langmuir and Freundlich adsorption isotherms is presented in Figs. 5-8.

Straight lines were obtained by plotting Ce/qe versus Ce, showing the Langmuir model
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applicability to sorption data (Fig. 5a). The correlation coefficient value was more significant
E

for M. oleifera (R2 = 0.91) than C. arietinum (R² = 0.88). The plots of Loqqe versus Log Ce of
CC

COD was used for the application of the Freundlich model for the adsorption efficiency (Fig.

5b). The coefficient (R² = 0.96) of C. arietinum was more than that of M. oleifera (R² = 0.91).
A

The coefficient of C. arietinum (R² = 0.99 and R² = 0.99) was more than that of M. oleifera (R²

= 0.90 and R² = 0.97) in both Langmuir and Freundlich isotherms respectively (Figure 6 a and

b). The results for O&G isotherms revealed that the adsorption coefficient of C. arietinum (R²

= 0.95 and R² = 0.99) was higher than M. oleifera (R² = 0.88 and R² = 0.94) based on both

16
models (Figure 7 a and b). The study of adsorption coefficient via the Langmuir isotherm

showed that the coefficient of C. arietinum (R² = 0.94) was more than M. oleifera (R² = 0.91)

while the coefficients were similar for the Freundlich isotherms (R² = 0.82 and R² = 0.82

respectively) (Fig. 8a and b).

The constant of the Langmuir isotherm is tabulated in Table 3. The values of Qmax and

KL were estimated respectively from the slope and intercept of the plots Ce/qe versus Ce,

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IP
showing the Langmuir isotherm applicability to sorption data. The Qmax values of M. oleifera

and C. arietinum to adsorb COD, TSS, O&G and turbidity from public market wastewater

R
samples were 147.06 vs. 47.39 mg/L, 6.97 vs. 9.20 mg/L, 37.59 vs. 54.64 mg/L and 3.10 vs.

SC
2.97 NTU respectively. These findings indicate that M. oleifera is more effective for the

U
adsorption of COD and turbidity compared to C. arietinum which exhibited more adsorptive
N
capacity for TSS and O&G. The coefficient (R2) for the adsorption of COD, TSS and turbidity
A
by M. oleifera as well as for the adsorption of TSS, O&G and turbidity by C. arietinum was
M

greater than 0.90. Viera et al. (2010) and Hor et al. (2016) reported that the Langmuir model

has fitted R2 values more than 0.99, indicating the all parameters adequately describe the
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experimental data from the adsorption experiments by the Langmuir model.

The constant of the Freundlich isotherm is illustrated in Table 4. The values of n and Kf
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(g/L) were estimated respectively from the slope and intercept of the plots Log qe versus Log
E

Ce. The Kf values corresponding to the adsorption capacity of M. oleifera and C. arietinum were
CC

2.62 vs. 1.43 for COD, 2.24 vs. 3.19 for TSS, 2.04 vs. 6.67 for O&G and 1.92 vs. 1.08 for

turbidity. The large value of Kf is an indication of greater adsorbent capacity (Tohidi and Cai,
A

2016). Therefore, M. oleifera has more adsorptive capacity for COD and turbidity while C.

arietinum has more adsorptive capacity for TSS and O&G. The n values for M. oleifera and C.

arietinum were 1.94 vs. 2.11, 2.10 vs. 1.64, 1.65 vs. 1.71 and 3.122 vs. 1.98 for COD, TSS,

O&G and turbidity respectively. According to the literature, the Freundlich constant n obtained

17
for the present systems indicated favourable adsorption as it lies between 1 and 10 (Viera et al.,

2010; Fulazzaky et al., 2014; Jabari, 2016). These results confirm the effectiveness of M.

oleifera and C. arietinum for the removal COD, TSS, O&G and turbidity from public market

wastewater.

These results revealed that the selection of isotherm models depends on the wastewater

parameters as well as the adsorbent. The Langmuir adsorption isotherm was the best model for

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the removal of turbidity from public market wastewater by M. oleifera and C. arietinum

(R2=0.91 and 0.93) compared to the Freundlich model (R2=0.81 and 0.82). Viera et al. (2010)

R
found that the Langmuir model (R2=0.99 and 0.99) was more fitting than the Freundlich model

SC
(R2=0.87 and 0.92) for the removal of colour and turbidity from dairy industry wastewater by

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adsorption using M. oleifera. Moreover, both Langmuir and Freundlich isotherms were fit for
N
the adsorption of COD (R2= 0.91) from public market wastewater by M. oleifera. The Langmuir
A
model was also the best for studying the removal of TSS (R2= 0.99) by M. oleifera. In contrast,
M

the Freundlich isotherm was the best for studying the removal of COD (R2= 0.96) and O & G

(R2=0.99) by C. arietinum.
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3.5 Textural Characterisation of natural coagulants

The microstructures of the prepared composite are shown in Fig. 9. The images revealed
PT

that the surface texture of M. oleifera and C. arietinum was rough and no pores were found.
E

Both M. oleifera and C. arietinum became softer, irregular, homogeneous and porous after the
CC

flocculation process (Figure 9a and b). They appeared to have a large specific surface area. The

pore size distribution affects the efficiency and selectivity of adsorption and kinetic reactions
A

(Alias et al., 2012). The efficiency of the sorbent is increased by increasing the number of pores

and surface area (Maina et al., 2016). These findings are used to explain the effect of the

coagulation and flocculation on the surface morphology of the coagulants, which indicate that

the accumulation pollutants from the wastewater on the surface of the coagulants make it more

18
softer. However, the flocculation mechanism is relies on the interactions between the negative

charges of the coagulants surface due to the many functional groups and positive charges of the

pollutants in the wastewater (Al-Gheethi et al., 2016). In The natural flocculants such as M.

oleifera and C. arietinum investigated in this study, the polymer structure of the coagulants act

as a bridge between the coagulants and chelating metal ions and can increase the floc size as

well as improve the sedimentation of pollutants (Atiku et al. 2016).

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Conclusions

The experimental investigation concluded that M. oleifera and C. arietinum seeds could

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be used as potential natural adsorbents for the removal of BOD5, COD, TSS, O&G, colour and

turbidity from public market wastewater. The factors including adsorption dose, pH and mixing

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rate play important role in the adsorption process. The adsorption data were fitted to Langmuir
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and Freundlich isotherms.
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Conflict of interest: The authors declared that they have no conflict of interest
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Acknowledgement
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Special gratitude goes to the laboratory technicians at the Micropollutant Research

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Centre, Faculty of Civil and Environmental Engineering, Universiti Tun Hussein Onn Malaysia

(UTHM) for providing the facilities for this research. The authors also wish to thank the
A

Ministry of Higher Education (MOHE) for supporting this research under FRGS vot 1574 and

also the Research Management Centre (RMC) UTHM for providing grant IGSP U682 for this

research.

19
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Figures captions

Tank 1 Tank 2 Tank 3

Influent

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Effluent Paddle

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Fig. 1a Lab-scale treatment system
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A
M
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Tank 1 Tank 2 Tank 3

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A

Before After

Fig. 1b Operating system of public market wastewater treatment process

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 T
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SC
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N
A
M
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Fig. 2 Efficiency of natural (M. oleifera and C. arietinum seeds) and chemical coagulants (Alum
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and FeSO4) for reducing pollutants from public market wastewater as a function of
dosage 60-360 mg L-1, A) BOD5; B) COD; C) TSS; D) O&G; E) colour; F) turbidity
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A

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 T
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SC
U
N
A
M
ED

Fig. 3 Efficiency of natural (M. oleifera and C. arietinum seeds) and chemical coagulants (Alum
and FeSO4) for reducing pollutants from public market wastewater as a response for pH
(4-9), A) BOD5; B) COD; C) TSS; D) O&G; E) colour; F) turbidity
E PT
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A

29
 Alum FeSO4 M. oleifera C. arietinum

90.83
87.17
100

86.88
81.59

81.06
83.3

79.57
79.01

80.9
77.36
90

74.05
70.99

70.82

70.08
69.45
68.08
80

66.05
65.56
Removal Percentage (%)

61.29

60.12
70
56.64

54.32
52.8
60

41.34
50

T
40

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30
20

R
10

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0
BOD5 COD TSS O&G Colour Turbidity
Parameters

Fig. 4 Removal of public market wastewater parameters by flocculation process using chemical U
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and natural coagulants in the lab scale system
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M

30
A
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20
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Ce/qe

10 y = 0.0068x + 3.3406
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R² = 0.9134
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0
0 500 1000 1500 2000 2500 3000 3500
Ce
A

30
 120
B
100

80
Ce/qe

60

40 y = 0.0211x + 27.546
R² = 0.8761
20

T
0
0 1000 2000 3000 4000

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Ce

Fig.5a Linearized Langmuir isotherm plot for adsorption of COD by M. oleifera seeds (A) and

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C. arietinum seeds (B)

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3.5 2.0
B
3.0
1.5 U
N
2.5

2.0
log qe

Log qe
A
1.0
1.5
y = 0.4739x - 0.1566
M

y = 0.5147x + 0.4184
1.0 R² = 0.9058 R² = 0.957
0.5
0.5
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0.0 0.0
2.2 3.2 4.2 5.2 6.2 2.0 2.4 2.8 3.2 3.6 4.0
Log Ce Log Ce
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Fig.5b Linearized Freundlich isotherm plot for adsorption of COD by M. oleifera seeds (A) and
C. arietinum seeds (B)
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A

31
 40 30
A B
35 25
30
20
25

Ce/qe
Ce/qe

20 15
15 y = 0.1434x + 8.7771
R² = 0.9885 10 y = 0.1087x + 7.985
10 R² = 0.9945
5 5

T
0 0

IP
0 50 100 150 200 0 50 100 150 200
Ce Ce

R
SC
Fig. 6a Linearized Langmuir isotherm plot for adsorption of TSS by M. oleifera seeds (A) and
C. arietinum seeds (B)

U
N
A
M
ED

Fig. 6bLinearized Freundlich isotherm plot for adsorption of TSS by M. oleifera seeds (A) and
PT

C. arietinum seeds (B)

E
CC
A

32
 T
R IP
Fig. 7a Linearized Langmuir isotherm plot for adsorption of O&G by M. oleifera seeds (A) and

SC
C. arietinum seeds (B)

U
N
A
M
ED

Fig. 7b Linearized Freundlich isotherm plot for adsorption of O&G by M. oleifera seeds (A)
PT

and C. arietinum seeds (B)

E
CC
A

33
 T
R IP
Fig. 8a Linearized Langmuir isotherm plot for adsorption of Turbidity by M. oleifera seeds (A)
and C. arietinum seeds (B)

SC
U
N
A
M
ED

Fig. 8b Linearized Freundlich isotherm plot for adsorption of Turbidity by M. oleifera seeds
PT

(A) and C. arietinum seeds (B)

E
CC
A

34
 A

T
R IP
SC
U
N
B
A
M
ED
E PT
CC
A

Fig.9a: SEM of M. oleifera seeds before (A) and after flocculation process(B)

35
 A

T
R IP
SC
U
N
B
A
M
ED
E PT
CC
A

Fig.9b: SEM image of C. arietinum before (A) and after flocculation process (B)

36
Tables

Table 1: Characteristics of raw public market wastewater compared with the Standard Effluent
(EQA, 2011). Sampling was conducted at 8 am to 12 pm on 10 August, 15 December
2015, 21 December and 5 January 2016, n=12.

EQA1974 (Regulation
2009)
Parameter (unit) Range
Standards Standards

T
A B

IP
pH 6.8-7.4 6.0-9.0 5.0-9.0

BOD5 (mg/L) 635-2350 20 50

R
COD (mg/L) 710-5120 120 200

SC
TSS (mg/L) 42.7-350 50 100

O&G (mg/L) 63.3-2500 1 10

Colour (Pt.Co) U
11.5-95.8 100 200
N
Turbidity (NTU) 9.96-187 NR NR
A
Biochemical oxygen demand (BOD5), chemical oxygen demand (COD), total suspended
solids (TSS), Oil & grease (O&G); (
M
ED
E PT
CC
A

37
Table 2. Characteristics of treated public market wastewater by using chemical and natural

coagulants

Chemical coagulants Natural coagulants EQA, 1974

(Regulation 2009)
Alum Ferrous M. oleifera C. Standar Standar
sulphate arietinum dA dB
BOD5 218.69±23 241.81±42.1 202.69±33.2 275.33±18.3 20 50
2
COD 184.24±42.1 241.47±27.3 200.47±27.3 241.04±12.3 120 200

T
2 2 2 4
TSS 5.49± 1.77 25.04± 2.51 8.16± 0.3 9.67± 0.04 50 100

IP
O&G 18.47± 2.08 29.87± 0.52 10.19± 1.05 19.34± 0.32 1 10

R
Colour 1.05± 0.29 5.25± 1.29 1.51± 0.79 2.12± 0.52 100 200
Turbidit 1.89± 1.30 3.97± 1.03 2.034±0.67 2.98± 1.76 NR NR

SC
y
Biochemical oxygen demand (BOD5); chemical oxygen demand (COD); total suspended
solids (TSS); Oil & Grease (O&G); Non-reported (NR)

U
N
A
M
ED
E PT
CC
A

38
Table 3: Langmuir isotherm for adsorption of COD, TSS, O&G and turbidity from public
market wastewater by M. oleifera and C. arietinum.

Parameters Qmax KL R2

M. oleifera C. M. oleifera C. M. oleifera C.

arietinum arietinum arietinum

COD 147.0590 47.3934 2.0350 0.0765 0.9134 0.8761

T
TSS 6.9734 9.1996 0.0163 0.0136 0.9885 0.9945

IP
O&G 37.5940 54.6448 1.7480 0.0421 0.8827 0.9461

R
Turbidity 3.0950 2.9735 0.0329 0.0652 0.9061 0.9344

SC
U
N
A
M
ED
E PT
CC
A

39
Table 4 Freundlich isotherm adsorption of COD, TSS, O&G and turbidity from public market
wastewater by M. oleifera and C. arietinum.

n Kf(g/L) R2

Parameters C. M. C. C.
M. oleifera M. oleifera

T
arietinum oleifera arietinum arietinum

IP
COD 1.9429 2.1100 2.6206 1.4342 0.9058 0.9570

R
TSS 2.0674 1.6364 2.2387 3.1871 0.9737 0.9852

SC
O&G 1.6480 1.7062 2.0359 6.6664 0.9380 0.9904

Turbidity 3.1221 1.9794 1.9235 1.0844 0.8142 0.8174

U
N
A
M
ED
E PT
CC
A

40