International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.
com; ISSN: 2455-474X
Adsorption Potentials of Fadama Clays towards Heavy Metals
(Zinc and Cobalt)
*OTOBO, G. &**OKPAKO, A. C.
*Department of Pure And Industrial Chemistry, University Of Port Harcourt Rivers State Nigeria.
**Department of Integrated Science, College Of Physical Education Mosogar Delta State Nigeria.
Abstract
This study investigated the potentials of Fadama Clays (Wetland soil) in the adsorption of heavy metals such
zinc and cobalt ions .Fadama Clays collected from three different locations in Delta State were analyzed for
Physico-chemical parameters. The effect of pH, contact time and adsorbent dosage were evaluated. The
adsorption behavior was characterized using adsorption isotherms, adsorption kinetics (pseudo second
order rate equation), diffusion-chemisorptions kinetics and adsorption edge experiments. Application of
Langmuir isotherm and adsorption kinetics showed that Fadama soils adsorbed the metal ions at lower pH
values of 1to 4.Adsorption kinetics (pseudo second order rate equation) showed that FAP (Patani Fadama
clays) had the highest equilibrium rate constant K (0.277mg/l/mins and 0.147mg/l/mins) for Zn and Co
respectively and next is FAU (Uwherun Fadama clays) (0.214mg/l/mins and0.000mg/l/mins). FAK (Kokori
Fadama clays) has the lowest equilibrium rate constant (K) (0.079mg/l/mins and 0.100
mg/l/minis).Application of Diffusion-chemisorptions kinetics indicated FAK yielded maximum adsorption
capacities for the two metal ions with KDC (Zn:0.89mg/g/l Co:0.24mg/g/l) followed by FAP with KDC (Zn:
0.32mg/g/l Co:0.22mg/g/l] and FAU the least with KDC (Zn:0.15 mg/g/l Co:0.23 mg/g/l] at lower pH values
of 1 to 4. This was as a result of available surface area and reduced distance for the sorbate to travel to
reach an active sorption site.
Keywords: Fadama, Adsorption Isotherm, Adsorbent, Diffusion-chemisorptions (KDC).
1. Introduction
Soil has the ability to immobilize heavy metal ions. The immobilization is due to sorption
properties such which are determine by physiochemical properties of soil such as amount of clay and organic
fraction, pH, water content, temperature of the soil and properties of the particular metal (Ashok. K. et
al.1998). Surface charge, pH and the concentration of cation as well as its accompanying anions can affect
electrostatic adsorption of metal while organic matter, Fe and Al hydroxides clay content are recognized as
the most significant soil properties influencing sorption reaction (Barry et al., 1995 and Bokin 2003).
In acidic soil, some iron, aluminum oxides are positively charged. They tend to counteract
the electronegativity of the larger silicate clays thereby reducing the capacity to adsorbed cations.
Adsorption is the accumulation of dissolved particles from a solution on to the surface of an adsorbent.
(Ademoroti, 1996) Adsorption in general is found to occur following one or more mechanisms. Analysis of
different adsorption systems indicate that adsorption mechanism can be classified into three, namely layer
formation, micro Pore filling and capillary condensation (Adamson,1990) Fadama soil (non irrigable land
and flood plains and low lying areas underlined by shallow aquifer. (Adeyeye.2005) very rich in organic
matter and nutrients than adjacent upland soil (Turner, 1977; Kparmwang and Esu, 1990), are used for
growing crops such as maize, guinea corn, tobacco and cattle grazing with little or no addition of organic
waste.
Of a particular threat to Fadama land areas are effluents from factories and manufacturing
facilities which contaminate the irrigable channels. Consequently, interest is growing in the use of sorbents
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
made from low-cost materials such as Fadama soils which contain some amount of clay. Clay minerals play
an important role in accumulation, adsorption/desorption, as well as in exchange process of metal ions
(Apak, R. Guolu and M. H Turgut 1998). It is considered that the adsorption of heavy metal ions and
complexes on clay mineral occurs as a result of ion exchange, surface complexation, hydrophobic interaction
and electrostatic interaction (Nowack and Sigg, 1996, Jung Cho and Hahn 1998). The Adsorption of heavy
metal such as Zinc and Cobalt which have tremendous hazard effect in the environment on Fadama Soils are
discussed in this research work.
2. Materials and Methods
Soil samples of Fadama soils were collected from latitude 5 45' N and longitude 6 71' E
(Kokori, Ethiope East L.G.A), latitude 5046' and longitude 526' N and longitude 546' E (Ughelli, Ughelli
North L.G.A,) latitude 50.32'N and longitude 50 50'E (Patani, Patani L.G.A) all in Delta State., Nigeria.
The Fadama soils in the Niger Delta area are moderately acidic with PH value ranging from 5.0-6.20.
Texturally, the Fadama soils comprise of particles such as sand, silt and clay held together
by organic substances, iron oxides, carbonates, clay and or silica. The clay minerals are hydroxides
aluminum, magnesium or iron Silicate.
Fadama soil from Kokori (FAK) is a brown sandy loam soil with 65% sand, 20% silt and
15% clay and it feels a bit smooth and powdery but sticky when moist. This soil belongs to the
montimorilinite group with chemical formula Al2 (OH)2 (Si205) which expands and is having higher cation
exchange capacity.
Fadama soil from Uwheru (FAU) is grey in colour and sandy with 85% sand 5% silt and
10% clay. It feels gritty when rubbed between fingers, not plastic or sticky when moist. This soil clay
mineral belongs to the illite (clay mica) group.
Fadama soil from Patani (FAP) is a yellow grey colour with 55% clay 32% silt and 13%
sand. It feels smooth, sticky and plastic when dry and does not expand when wet. This soil belongs to the
kaolinite group with chemical formula Al2 (OH)4 Si2 O5 .
The physiochemical properties of soil which affect the sorption properties of soil are
concentrated in the lower (15-30cm) than the upper depth [Alloway 1995;Tsadilas 2000] Therefore, the
various soil samples which were collected at a depth of 15-30cm Samples were sieved with a 2mm sieve and
divided into two portions. One portion was placed in polyethylene bag and stored in a refrigerator at 40C and
the second was air dried at room temperature for 48 hours and stored in a tightly sealed bottle. A sub-sample
of air dried was ground to pass 80 mesh sieves (180m) for determination of chemical properties (Chae and
Tabatabai 1986).
1g each of soil samples were first treated with 10ml of 0.1M NaOH to precipitate some of
the dissolved ions as their hydroxide which was then separated from the clay. For example, Al (OH)2+ at low
pH block the active site of the adsorbent making exchange site unavailable. Raising the pH, ions from NaOH
form Al (OH)3 thereby releasing negative charged site. These base-treated clays were then boiled with 20ml
of 0.04M HNO3 for 1 hour to activate them. They were then washed several times with distilled water, dried
and served. The soil samples were activated with HNO3 to open up micro-pores of the adsorbent thereby
making the soil ready for adsorption
l0g of each soil sample was weighed into 200m1 beaker. 20m1 of distilled water were added
to the soil mixtures and was allowed to stand for further 30 minutes and stir occasionally with glass rod and
allow the fine soil particles to settle. The pH meter (model Kent Ek7020) which was standardized with
buffer pH 4 and pH 9 was inserted into the partly settled suspension to determine the pH (Ademoroti, 1996)
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
3. Batch Experiments
2.2032g analytical grade anhydrous Cobalt (II) Chloride (CoCl 2) was dissolved in distilled
water and made up to 1 litre mark [1ml = 1mg Co]. Standard Co was prepared by withdrawing 10 ml of Co
stock solution into 1 litre volumetric flask and made up to the mark [1ml = 10 g Co].
100mg 30-mesh analytical grade Zinc metal was dissolved in slight excess of HCl (about
1ml is required) which was distilled water and made up to I litre [1ml = 1mg Zn].To prepare standard
Zn,10ml of the stock solution was withdrawn and made up to 100ml mark :1ml = 100g Zn. (Ademoroti,
1996)
All absorption tests, namely, isotherm, kinetics and pH-edge, were performed as batch
experiments. Adsorption isotherm was generated with a fixed sorbent mass and varying initial metal ions
concentration (Co) from 5mg/l to 30mg/1 while maintaining the adsorbent dosage of l g/1.
The effect of absorbent dosage was studied by varying the adsorbent amount from 5mg/1 to 20mg/1 with
metal ions concentration of 20mg/1.
The effect of time and pH were studied at 30c with metal ion concentration of 20mg/l and
adsorbent dosage of 1g. The initial concentration of Co and Zn were prepared by serial dilution of standard
mg/1 reference solution. The pH of the solution was adjusted to pH 5.6 0.1. The sealed bottles were placed
in a shaker (model TT 12F Technical and Technical USA) for 4hour at 298k. After equilibration, the
supernatants were filtered through UM pore size MF- Millipore mixed cellulose ester membrane filter and
then analyzed for dissolved Co and Zn concentration by BUCK Scientific Atomic Absorption Spectrometer
(model 200). The uptake capacity amount of Co and Zn (qe) adsorbed were calculated by mass balance
between Co (initial conc. of metals) and (final conc.) Ce. (Wahba and Zaghloul 2007).
Adsorption kinetic experiments were performed in a solution with 1.0g of sample, pH 5.
Initial Co and Zn concentration of the solution were 20mg/l and the solution pH was maintained by using
0.1M HNO3 And 0.1M KOH. The suspension was stirred by a magnetic bar and was placed on digitally
operated high speed centrifuge (modelTGL-16G) for centrifugation. The supernatant was collected at
various time intervals during the one and half hours experiment using decantation method. The sampling
time for the experiment were 20, 40, 60, 80 to 100 minutes and the concentration of heavy metals using
atomic absorption spectroscopy were taken (Cottenie 1982).
Adsorption edge (pH effect) experiments were conducted in 40ml samples tubes containing
1g of the samples and 30m1 of 20mg/1 Co and Zn solution at different pH values of 2, 4, 6, 8. The sample
tubes were placed in a shaker for 4hrs. pH of final Co and Zn concentration in the filtrate were determined
after equilibration using pH meter (model:EL17050)
4. Results and Discussion
The study of the three Fadama soil samples (FAK, FAP and FAU) before adsorption of
metals indicated that the three Fadama soils samples were acidic with the pH values of 4.47, 4.36 and 4.35
respectively which correspond to the pH of the Niger Delta region (Isirimah, 1987; Odu et al., 1985) . It
could be suggested here that the acidic nature of the soils could be as a result of the aluminum (iii) ion which
was in the soil no longer existing as aluminum (iii) ion but has been converted to aluminum hydroxyl. This
in line with (Brady,1974) who said that exchangeable H+ ions that are released by base forming cations
move into the solution where they react with OH to form water.
At pH 2 and 4, FAK had the highest adsorption capacity for the two metal ions (Zn and Co).
This is followed by FAP and FAU had the least adsorption capacity.
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
At pH8 the three soil samples adsorption capacity decreased in this order FAK<FAU<FAP as shown in
figure 1and 2.
Increase adsorption between the pH 2 and pH 4 indicated that hydroxyl groups are the major
functional group responsible for the removal of these metals ions at that low pH values. It showed that the
hydroxyls present in the silicate particles dissociate slightly and the colloidal surface is left with a negative
charge carried by the oxygen which attracts the metal ions to itself. That is to say that the mechanism of
adsorption of these ions is the ion exchange mechanism which involves the release of light metal ion during
heavy metal uptake (Crist et al, 1999) and electrostatic interaction (Do, (1998).
Adsorbent dosage as shown in figure 3 and 4 had greater effect on the adsorption of the
metal ions in the three soil samples. It was observed that the three soil samples had good adsorption capacity
for the two metal ions with increase in the adsorbent dosage. This could be attributed to the fact that minute
silicate clay colloidal particles referred to as micelles ordinarily carry negative charges and hundreds of
thousands of positively charged ions or cations are attracted to each colloids (Buseck1993).
Adsorption of these metals was higher with FAK followed by FAU and then FAP. There was a maximum
adsorption for these metal ions at maximum dosage of adsorbent. This suggested that a good solid adsorbent
must have a combination of two pore ranges: the microspore range and the macrospore range (Do1998)
Contact time appeared to have noticeable effect on the adsorption of the metal ions. There
is similarity in adsorption of zinc and cobalt on the three Fadama soils. In a nutshell, some levels of
adsorption of zinc, and cobalt were maintained with time.
FAK had the maximum adsorption for the two metal ions at 20 and 60 minutes as shown in Fig 5 and 6.
Figure 1: Effect of pH on the Adsorption of Zinc on Fadama Soils
Figure 2: Effect of pH on the Adsorption of Cobalt on Fadama Soils.
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
Zn adsorption capacity (mg/g)
35
30
25
20
FAK
15
FAP
10
FAU
0
5
10
15
20
25
30
Adsorbent dosage
Figure 3: Effect of Adsorbent Dosage on the Adsorption of Zinc ions on Fadama Soils
Co Adsorption capacity(mg/g)
80
70
60
50
40
FAU
30
FAP
20
FAK
10
0
5
10
15
20
25
30
Adsorbent dosage
Figure 4: Effect of Adsorbent Dosage on the Adsorption of cobalt ions on Fadama Soils
Figure 5: Effect of Contact Time on the Adsorption of Zinc ions on Fadama Soils
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
Figure
6:
Effect of Contact Time on the Adsorption of Cobalt ions on Fadama Soils.
5. Adsorption Isotherm
Langmuir equation yielded a satisfactory fit. The linearized Langmuir equation has the
following form.
1
/qe = 1/qmxbCe+ 1/qmx
(1.2)
Where Ce is the equilibrium metal ion concentration in mg/l, qe is the amount of metal sorbed in mg/l, qmax
is the maximum metal sorption capacity in mg/1, b is a constant, related to the strength of adsorption l/mg.
The sorption capacities are of close range with those determined from pseudo- second order kinetics model.
20
y = 1.0884x - 1.9031
R = 0.9943
18
16
y = 0.8471x + 0.8617
R = 0.9328
Ce/qe (mg/g)
14
12
10
FAP
y = 0.8523x - 2.8343
R = 0.9783
FAU
Linear
(FAK)
Linear
(FAP)
4
2
0
-2 0
FAK
10
15
20
Ce (mg/g)
Figure 7: Langmuir Isotherm for Zinc Ions Adsorption on Fadama Clay
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
16
y = 0.8116x - 1.805
R = 0.9958
14
Ce/qe(mg/g)
12
10
y = 0.5906x - 1.565
y = 0.8528x - 3.19 R = 0.3632
8
6
FAK
FAP
R = 0.9073
FAU
2
0
0
10
15
20
25
Ce (mg/g)
Figure 8: Langmuir Isotherm for Cobalt Ions Adsorption on Fadama Clays
Table 1: Isotherm Constants for Adsorption of Zn (II) Ions on Fadama Soils
Soil sample
Langmuir Isotherm
qm(mg/g) b(mg/g)
FAK
FAP
FAU
4.41
9.01
15.87
0.227
0.111
0.063
Pseudo-Second Order Rate Kinetics
k (mg/l/mins)
qe(mg/g)
.079
.277
.214
11
6
4
Table 2: Isotherm Constants and Adsorption Kinetics of Co (II) Ions on Fadama Soils
Soil sample
FAK
FAP
FAU
Langmuir Isotherm
qm(mg/g) b(mg/g)
8.00
0.125
8.47
0.118
8.77
0.114
Pseudo-Second Order Rate Kinetics
k (mg/l/mins)
.100
.147
.222
qe(mg/g)
14
15
3
FAK = Kokori Fadama Clay
FAP = Patani Fadama Cay.
FAU = Uwheru Fadama Clay
qm =Minimum adsorption capacity (mg/g)
b = Langmuir constant
k = rate constant
qe = sorption capacities
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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t0/qt
6. Adsorption Kinetics
Data from the kinetics experiment were fitted to the pseudo second order rate equation [1.3]
to determine Zn and Co, sorption capacities (qe) and rate constant k .This model conformed that the
adsorption followed the Langmuir equation. The kinetic rate equation can be written as shown below.
dqt /t = k (qe-qt)2
(1.3)
Where qt and qe are the amount of metals adsorbed at time t and at equilibrium (mg/l/g), respectively, and k
is the equilibrium rate constant for second order sorption (mg/g/mins). By integrating equation for the
boundary condition t=o to t= t, qt=0 to qt =qt the following linearized form is obtained.
t
/qt =1/kqe2 + 1/qet
(1.4)
A plot of t versus (to/qt) was used to determine value of k as shown in Figures 9and10. This model described
the data adequately when fitted into equation (1.4)
18
16
14
12
10
8
6
4
2
0
y = 0.7776x + 0.035
R = 0.9813
y = 0.4214x + 0.515
R = 0.996
FAK
y = 0.2026x + 0.015
R = 0.9968
0
10
15
20
FAP
FAU
25
Figure 9: Pseudo-Second Order Rate Kinetics For Adsorption of Zinc (II) Ions on Fadama Clays.
25
y = 0.2816x - 0.06
R = 0.9823
t0 /qt
20
FAK
15
y = 0.1831x - 2.625
R = 0.68
10
FAU
y = 0.0716x + 0.005
R = 0.9918
FAP
0
0
20
40
60
80
100
Figure10: Pseudo-Second Order Rate Kinetics For Adsorption of Cobalt (II) Ions on Fadama Clays.
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
Diffusion-chemisorption(mg/l/g)
7. Diffusion-Chemisorptions Kinetics
Initial metal concentration of different sorbent sizes greatly affects the amount of the heavy
metal adsorbed by each soil sample. Adsorption of the metal ions (Zn, Co) increase with increase
concentration of the adsorbate
A plot Diffusion-Chemisorptions rate constant (KDC) versus initial metal concentration for
various sorbent sizes as shown in figures 13 and 14 indicated that KDC increased with increased sorbent size
.This was as a result of available surface area and reduced distance for the sorbate to travel to reach an active
sorption site.
16
14
12
10
8
6
4
2
0
y = 0.577x + 1.89
R = 0.9741
y = 0.3224x + 2.205
R = 0.9765
FAK
FAP
FAU
y = 0.293x + 1.235
R = 0.8948
0
10
15
20
25
Initial adsorbate concentration (mg/l)
Diffusion-chemisorption rate(mg/l/g)
Figure 11: Diffusion chemisorptions Rate of Adsorption of Zinc ions on Fadama Soil
10
9
8
7
6
5
4
3
2
1
0
y = 0.3406x + 2.22
R = 0.9294
y = 0.1988x + 1.57
R = 0.9189
y = 0.1884x + 1.805
R = 0.9278
FAK
FAP
FAU
10
15
20
25
Figure 12: Diffusion chemisorptions Rate of Adsorption of cobalt ions on Fadama Soil
Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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International Journal of Pure and Applied Researches; 2016 Vol. 1(2); ijopaar.com; ISSN: 2455-474X
8. Conclusion
The adsorption of Zn2+ and Co2+ ions depend on the chemistry and the surface morphology
of the Fadama clays and on the concentration of these clays as shown in Figure 9 and 10. This was in line
with fact that surface sites responsible for the adsorption are assumed to be the permanent charges, SiO 4
(silanol) group, Carboxyl group, aluminol group and phenol group (Julide and Resat, 2006),).
The isotherm model of Langmuir and the kinetic model of pseudo-second order rate
equation as well as Diffusion-Chemisorptions adsorption rate equation were found to be quite suitable to
characterize the adsorption of heavy metal ions on Fadama clays. In a nutshell, the adsorption of Zn2+ and
Co2+ ions on the soil samples decreased with increased pH and increased with increased adsorbent dosage,
contact time and the adsorbate concentration. This confirmed that the Fadama clays have good adsorption
potential. From the Langmuir Isotherm, the Chemisorption-Difussion kinetics and the kinetic model of
pseudo-second order results of the soil samples, it was seen that the soils could work as adsorbent for heavy
metals in neutral and acidic solutions.
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Paper ID: B16103; Adsorption Potentials of Fadama Clays towards Heavy Metals (Zinc and Cobalt) By OTOBO, G. and
OKPAKO, A. C.; pp. 119-128; Date of Publication: 15th May 2016; Current Impact Factor: 0.832.
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