Research in Chemistry and Environment

Suresha et al. Int. J. Res. Chem. Environ. Vol. 4 Issue 4 (101-108) October 2014
International Journal of
Research in Chemistry and Environment
Available online at: www.ijrce.org
ISSN 2248-9649
Research Paper
Biosorption of Ni (II) in Aqueous Solution and Industrial Wastewater by Leaves
of Araucaria cookii
Deepa C. N. and *Suresha S.
Department of Environmental Science, Yuvaraja’s College, University of Mysore-570005, Mysore, Karnataka, INDIA
(Received 01st July2014, Accepted 10th August 2014)
Abstract: Biosorption experiments were carried out in batch process and the parameters like pH, contact time, size
variation, adsorbent dose and metal ion concentration were optimized. Maximum percent removal of Ni (II) ions in
the aqueous solution was 96.95 at pH 6 and contact time of 40 min. Langmuir and Freundlich isotherm models
were applied to describe the equilibrium data. Kinetic models like Pseudo first order and Pseudo second order
fitted well for the biosorption process. The results showed that the leaves of Araucaria cookii can efficiently remove
Ni (II) ions from the aqueous solution and also from the Metal plating wastewater. Hence it can be used as a low
cost biosorbent.
Keywords: Biosorption, Araucaria cookii, Nickel, Kinetic models, Langmuir and Freundlich isotherms
© 2014 IJRCE. All rights reserved
Higher concentration of nickel causes cancer of
lungs, nose and bone. Dermatitis is the most frequent
effect of exposure to nickel, such as coins and jewellery.
Acute poisoning of Ni (II) causes headache, dizziness,
nausea and vomiting, chest pain, tightness of the chest,
dry cough and shortness of breath, rapid respiration,
cyanosis and extreme weakness [12-14]. Although nickel is
not considered to be toxic at low levels, like other
pollutant metals, it accumulates in the food chain and
once it gets absorbed into the body it cannot be easily
excreted [13].
Introduction
In the global technological progress the
discharge of heavy metals from different industries into
the natural environment suffers the detrimental effects
caused by water pollution. The natural process of
transportation of metal ions between soil and water
consolidates metal contamination in high concentrations
that affect the natural ecosystems [1, 2]. The presence of
heavy metals in the water environment is a major concern
due to their toxic effects since they cause severe health
problems to animals and human beings [3]. Heavy metals
are most hazardous pollutants because of their nondegradable nature [4].
A number of methods are used for the removal
of heavy metal pollutants from liquid wastes when they
are in high concentrations [15]. The processes used to
remove heavy metals from industrial effluents, include
chemical precipitation, coagulation, solvent extraction,
membrane separation, and ion exchange [16,17].
Nickel (Ni) is ubiquitous in nature [5]. It occurs
naturally in soil, sea salts, and volcanic ash and as
particles in smoke from forest fires in the form of
sulphides, arsenides, antimonides and oxides [6]. Ni (II) is
more toxic and carcinogenic than Ni (IV). According to
ISI: Bureau of Indian Standard (BIS) the industrial
effluent permissible discharge level of Ni (II) into inland
water is 3.0 mg L-1[7,8]
The new technological trend is based on the
utilization of low cost biological materials as adsorbents
of heavy metals[18,19]. Biosorption is the removal of heavy
metals by the passive binding to non-living biomass from
an aqueous solution [20]. Living or dead biomass can be
used to remove metals, but maintaining a living biomass
during metal biosorption is difficult because it requires a
continuous supply of nutrients and some metals may
prove toxic to microorganisms. On the other hand, the
use of dead biomass can overcome these problems and
once used cells can be easily regenerated [21, 22].
Nickel is released into the environment by a
large number of industrial processes, such as
electroplating, leather tanning, wood preservation, pulp
processing and steel manufacturing[9,10]. The most
common application of nickel is in steel and other metal
products such as jewellery [11].
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Suresha et al. Int. J. Res. Chem. Environ. Vol. 4 Issue 4 (101-108) October 2014
In recent years, the search for low-cost adsorbents
that have metal binding capacities has intensified.
Agricultural by-products have been widely studied for
metal removal from water. These include peat, wood,
banana pith, soybean and cotton seed hulls, peanut shells,
hazelnut shell, rice husk, saw dust, wool, orange peel,
compost and leaves[23].
methods described by American Public Health
Association (APHA, APHA 1998) and the results
presented in Table 1.
Biosorption Experiments: Batch experiments were
carried out at room temperature. For experimental run 20
ml of 1000 mg/l of Ni (II) solution at pH of 1.0-7.0 were
taken in a pre- cleaned conical flask. Two g of biosorbent
were added and the mixture was stirred at constant speed
of 200 rpm in a mechanical shaker. The mixture was then
centrifuged at 6000 rpm for 15 min. The resultant
supernatant liquid was analysed by AAS. Percent
biosorption of metal ion was calculated by the following
formula
In the present study dried leaves powder of A.
cookii has been tried as biosorbent for the removal of Ni
(II) ions in the aqueous solution. Various parameters like
pH, contact time, dosage, size variation and metal ion
concentration will be optimized. Comparing to all these
factors, pH is considered as one of the ‘master parameter’
which controls in ion exchange, dissolution/precipitation,
reduction/oxidation, adsorption and complexation
reactions [24] .Experimental data would be collected by
using Langmuir and Freundlich isotherms. Kinetic
studies of Pseudo first order and Pseudo second order
reactions will also be carried out.
% Removal= (C0–Ce) x 100
Where C0 and Ce are the initial and final concentrations of
the Ni (II) solution respectively. The metal uptake
capacity was calculated using following formula:
qe= (C0–Ce) x V
(2)
M
Where, qe is the metal uptake (mg/g), C0 and Ce are the
initial and final equilibrium metal concentrations in the
solution (mg/l), respectively, V is the solution volume
(ml) and M is the mass of the Biosorbent (g).
Material and Methods
Preparation of Metal ion solution:Metal ion solution of
Ni (II) was prepared by using Nickel ammonium sulphate
A.R. grade. Stock solution (1000 mg/l) was prepared by
dissolving 6.727g in 1000 ml of double distilled water.
Table -1
Physico-chemical Characteristics of Metal plating
wastewater
Parameters
pH
Conductivity (µs/cm)
Total Dissolved Solids
Calcium
Magnesium
Chloride
Sulphate
Sodium
Potassium
Nickel (II)
Chromium (VI)
(1)
Results and Discussion
Effect of pH: The pH is an important parameter in the
biosorption process of metal ions from aqueous solution,
which is responsible for the protonation of metal binding
sites and speciation of the metal solution [23]. Figure 1
show that the percent Ni (II) biosorption increased with
increasing from pH 1.0 – 6.0 with corresponding Ni (II)
biosorption efficiency increasing from 39.0 to 96.95 %.
Further increase in pH the rate of biosorption gradually
decreased. This is due to formation of poorly soluble
hydroxyl species and precipitation of Ni (II) at higher
pH[24]. Similar results were obtained by using protonated
rice bran and using Rhizopus sp [25, 26].
Contents
(mg/l)
3.5
1883
1032
102.15
48.92
217.81
88.45
73.85
3.06
45.95
15.67
Effect of Particle size variation: The particle size effect
on biosorption of Ni (II) was studied by taking different
particle sizes ranging of 100, 200, 300 and 400 µm. The
results prescribed in the Figure 2 reveals that the
saturation capacity of Ni (II) biosorption increased with
decreasing the particle size. This shows the relationship
between the effective specific area of the biosorbent
particles and their sizes. As the surface area of the
particles increases the particle size decreases and as a
consequence, the saturation capacity per unit mass of the
adsorbent increases [27]. This can be explained by the fact
that for smaller particles a large external surface area is
available for Ni (II) in the solution which results in the
lower driving force per unit surface area for mass
transfer. This decreases the biosorption of Ni (II) from
96.95 to 68 % as the particle size increases from 100 to
400 µm. Similar results were reported for the biosorption
of Cu (II) by Valonia Tannin Resin [28].
Preparation of biosorbent: Fresh leaves of A. cookii
were collected from the trees growing in the campus of
Manasagangotri, University of Mysore, Mysore. The
leaves were washed with deionised water, cut into small
pieces sun dried for seven days. The material was
grounded and sieved into size fractions of 100 µm, 200
µm, 300 µm and 400µm. The sieved biosorbent was
washed with double distilled water for several times to
remove the dust particles and stored in dry plastic jar
until further use.
Metal plating waste water: The wastewater was
collected from Tritan-Valves Industry, Mysore,
Karnataka, India. The Physico - Chemical characteristics
of wastewater was analysed according to standard
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Suresha et al. Int. J. Res. Chem. Environ. Vol. 4 Issue 4 (101-108) October 2014
% biosorption
150
100
50
0
0
2
4 pH
6
8
% biosorption
Figure 1: Effect of pH on biosorption of Ni (II) ions by A. cookii
200
100
0
0
200
400
600
Particle size (µm)
% biosorption
Figure 2: Effect of Particle size variation on biosorption of Ni (II) ions by A. cookii
140
90
40
0
50
100
Contact time ( min)
% biosorption
Figure 3: Effect of time on biosorption of Ni (II) ions by A. cookii
200
100
0
0
2
4
6
biosorbent dose (g)
Figure 4: Effect of biomass on biosorption of Ni (II) ions by A. cookii
Effect of contact time: The biosorption capacity of Ni
(II) by A. cookii was studied by allowing different time
intervals of 5 – 90 min. Figure 3 shows that maximum Ni
(II) biosorption (96.95%) was achieved at 40 min. There
was rapid increase in Ni (II) biosorption during the initial
30 min and further absorption was achieved at a slower
rate. The uptake of heavy metal ions by biosorbent takes
place in two stages such as a rapid and quantitatively
predominant stage followed by a slower and
quantitatively insignificant stage. The rapid stage may be
due to abundant available sites on the biomass and in the
slower stage the occupancy of these sites becomes less
efficient [29]. Similar results were reported on biosorption
of copper, cobalt, and nickel by marine brown alga
Sargassum sp in fixed- bed column [30].
103
% biosorption
Suresha et al. Int. J. Res. Chem. Environ. Vol. 4 Issue 4 (101-108) October 2014
150
100
50
0
0
100
200
300
400
Initial metal ion concentration (mg/l)
Figure 5: Effect of metal ion concentration on biosorption of Ni (II) ions onto A. cookii
Table- 2
Comparison of Various Biosorbents with some latest literature of Ni (II) biosorption
Biosorbents
qmax
Reference
Ficus Religiosa(peepal) leaves
25.71 mg/g
[36]
Tamarind bark
15.34 mg/g
[37]
Rice straw
35.08 mg/g
[38]
38.4 mg/g (algal beads)
[49]
29.54 mg/g
313(k)
36.03 mg/g
[40]
Chitosan- immobilized Brown Algae
Loquot bark (Eriobotrya japonica)
Araucaria cookii
Present study
* qmax is equilibrium and maximum adsorption capacity (mg/g)
log (qe- qt)
3
2
1
0
-1 0
10
20
Time (min)
30
40
Figure 6: Pseudo first- order Kinetic reaction of Ni (II) ions onto A. cookii
Effect of biosorbent dosage: The biosorbent was studied
at dosages of 0.5 to 4.0 g/l. The results show that
biosorption efficiency increases from 50.0- 96.95 % with
increase in the biosorbent dose. Figure 4 shows the
maximum removal of Ni (II) was attained at 2.0 g/l. The
removal capacity of Ni (II) increased due to increase in
the number of binding sites with increase in biosorbent
dose [31, 32]. Further beyond 2.0 g/l the rate of adsorption
becomes constant. This is due to attainment of
equilibrium between liquid and solid phase. Similar
results were reported for biosorption of lead by
Saccharomyces cerevisiae [33].
This is one of the important parameters. The Ni (II)
removal efficiency decreases from 99.4 to 64.63 % with
increase in the Ni (II) ion concentration from 25 to 300
mg/l. Maximum (96.95 %) removal of Ni (II) has
occurred at 200 mg/l. It was reported that increase in the
metal ions, the biosorption percent decreases due to lack
of sufficient surface area to accommodate available sites
from metal in the solution [34]. The results are comparable
to the reported by biosorption of Cr (VI) and Co (II) ions
from fresh water green algae, Cosmarium panamense [35].
Comparison of Various Biosorbents: From Table 2 the
present biosorbent is compared with the recently reported
qmax value of Ni (II) biosorption from various
biosorbents. It shows that the present biosorbent has its
highest qmax value (36.03 mg/g) which is competitive to
Effect of metal ion concentration: Figure 5 shows the
biosorption rate with varying initial metal ion
concentration of Ni (II) in aqueous solution by A. cookii.
104
Suresha et al. Int. J. Res. Chem. Environ. Vol. 4 Issue 4 (101-108) October 2014
other reported biosorbents.
Where, t shows time in min, qt (mg/g) shows uptake
capacity at t and K (g mg -1 min -1) shows the equilibrium
rate constant of pseudo- second order adsorption. In the
integrated form it is represented as
t/dt = 1/ kq2eq + t/qe
(6)
Kinetic study: Kinetics of heavy metal ions are used to
analyse the biosorption process in relation to contact
time. Kinetic sorption of heavy metals from wastewater
was studied using pseudo first order and pseudo second
order models [41, 42]
.
Pseudo first order reaction: The first order rate
equation of Lagergren is most widely used for the
sorption of a solute from liquid solution and is given by
[43]
.
ln (qe – qt) = ln qe – K1ads t
(3)
The sorption rate, h (mg/g. min) is defined as
h= K2 qe2
K2 and h values were determined in Figure-7 for the slope
and intercept of the plots t/q against t. The linear pseudosecond order equation shows good agreement of
experimental data for different initial metal ion
concentrations. The values of pseudo second order
equation parameters together with correlation coefficients
are shown in Table-3 and Figure-7. The correlation coefficient for the equation is R2= 0.999. The qe values also
agree well with the experimental data. Thus pseudo
second order models suitably describe the biosorption of
Kinetic data in the present study. For evaluation of
sorption rate, h has been widely used. In the present
study, the value of h is 0.362 and K2 is 0.120 (g/mg/min).
Similar performances have been reported in the
biosorption of Pb (II) and Cu (II) by pomegranate peel
[45]
.
Where, qe is the mass of metal adsorbed at equilibrium
(mg/g), qt is the mass of metal adsorbed at time mg/g,
K1ads is the first order reaction rate constant, and the
linearized form is:
log (qe – qt) = log qe – K1 t / 2.303
(7)
(4)
A graph is plotted between log (qe-qt) versus t at the rate
constant K1 can be obtained by slope and intercept
(Figure 6). The slope is calculated from the Pseudo first
order rate constant K1. The calculated values of K1 and
their corresponding linear correlation coefficient (R 2)
values are shown in Table 3. The R2 value is 0.9496 for
Ni (II) in aqueous solution. This model shows that the R2
value can be applied for the biosorption process.
Adsorption isotherms: The equilibrium of the
biosorption process is often described by fitting the
experimental points with models which are used to
represent the equilibrium adsorption isotherm [46].
Pseudo second order reaction: The Pseudo second
order model considers that the rate of occupation of
biosorption sites is proportional to the square of the
number of unoccupied sites [44].
dqt / dt = K (qeq- qt)2
(5)
In order to describe the adsorption mechanism
of low-cost adsorbents used for water and waste water
treatment experimental equilibrium data are most
frequently modelled as per the relationship developed by
Langmuir isotherm [47].
Table 3: Pseudo first-order and Pseudo second –Order constants for Ni (II) biosorption by A. cookii
Pseudo first order
qe (mg/g-1 )
K 1(min-1)
1.511
0.006
R2
qe (mg/g-1)
0.949
1.74
Pseudo second order
K2 (g mg-1min)
R2
0.120
0.999
0.3
t/ qt
Metal
Ni (II)
0.2
0.1
0
0
20
40
60
Time (min)
Figure 7: Pseudo second- order Kinetic reaction of Ni (II) ions onto A. cookii
Table 4: Langmuir and Freundlich constants for Ni (II) biosorption by A. cookie
Metal
Langmuir
Freundlich
2
q max
b
R
Kf
1/n
R2
Ni (II)
36.03
0.026
0.996
33.11
0.948
0.998
105
h
0.362
Suresha et al. Int. J. Res. Chem. Environ. Vol. 4 Issue 4 (101-108) October 2014
Ce/qe
1.5
1
0.5
0
50
150
250
350
Ce
Figure 8: The linearized Langmuir adsorption isotherms of Ni (II) by A. cookii
log qe
2.5
2
1.5
1
1
1.5
2
2.5
log Ce
Figure 9: The linearized Freundlich adsorption isotherm for Ni (II) by A. cookii
Figure-8 shows the Langmuir model based on
the assumption that maximum biosorption occurs when
saturated monolayer of solute molecules is present on the
adsorbent surface, the energy is constant, and there is no
migration of adsorbate molecules on the surface plane
[48]
.
Langmuir model is represented as follows:
Ce / qe = 1 /(b q max) + Ce / qmax
wastewater and 2.0g of biosorbent in a pre cleaned
conical flask. The solution was adjusted to pH 6.0, with
contact time 40 min, centrifuged and the resultant
supernatant Ni (II) solution was analysed by AAS. The
result showed that there was decrease of 80.32% of Ni
(II) from the metal plating wastewater due to biosorption
by A.cookii leaves compared to that of aqueous solution.
This may be due to the presence of other ions and
impurities present in the wastewater as indicated in table
1 which compete with Nickel for binding sites. The
removal of Nickel is less due to unavailable of Ni (II) in
wastewater.
(8)
Where, Ce is the equilibrium concentration (mg/L), qe and
qmax are the equilibrium and maximum adsorption
capacity (mg/g), respectively and b is the equilibrium
constant.
Conclusion
The effective removal of Ni (II) ions from the
aqueous solution by the leaves of Araucaria cookii has
been shown. The other parameters like pH, contact time,
size variation, adsorbent dose and metal ion
concentration. The metal uptake was effective for the
removal of Ni (II) at pH 6. The maximum percentage
removal attained was 96.95% at initial concentration of
200 mg/l. The adsorption isotherms onto Araucaria
cookii easily fitted with Langmuir and Freundlich
equations. Kinetics was described best by Pseudo- second
order model.
The graph of Ce / qe vs. Ce is plotted on contact
time where, intercept and the slope can be obtained. The
Coefficient correlation R2 is 0.996 and q max is 37.03 as
shown in Table 4.
The Freundlich adsorption isotherm is an
empirical model that is based on sorption on a
heterogeneous surface [49]. The equation is as follows:
ln qe = ln Kf + 1/n ln Ce
(9)
The constant n is an empirical parameter that
with the degree of heterogeneity and Kf is a constant
related to adsorption capacity. The values of n and Kf
which are constant can be determined by the plot Ce and
qe (Slope = 1/n, Intercept = Kf) .The results are presented
in Table 3.
Acknowledgement
The authors would like to acknowledge
University Grants Commission, New Delhi, for financial
support under Rajiv Gandhi National Fellowship.
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