ENERGY, RESOURCES AND ENVIRONMENTAL TECHNOLOGY

Chinese Journal of Chemical Engineering, 20(4) 768775 (2012)

Removal of Bi (III) with Adsorption Technique Using Coconut Shell

Activated Carbon

SARTAPE Ashish1, MANDHARE Aniruddha1, SALVI Prathmesh1, PAWAR Dattatraya1,

RAUT Prakash2, ANUSE Mansing1 and KOLEKAR Sanjay1,*
1
Analytical Chemistry Laboratory, Department of Chemistry, Shivaji University, Kolhapur-416 004, India
2
Department of Environmental Science, Shivaji University, Kolhapur-416 004, India

Abstract In present study, we report the preparation of coconut shell activated carbon as adsorbent and its appli-
cation for Bi (III) removal from aqueous solutions. The developed adsorbent was characterized with scanning elec-
tron microscope (SEM), Fourier Transform Infrared (FTIR), C, H, N, S analyzer, and BET surface area analyzer.
The parameters examined include agitation time, initial concentration of Bi (III), adsorbent dose and temperature.
The maximum adsorption of Bi (III) (98.72%) was observed at 250 mgL1 of Bi (III) and adsorbent dose of 0.7 g
when agitation was at 160 rmin1 for 240 min at (2992) K. The thermodynamic parameters such as Gibbs free
energy (G), enthalpy (H) and entropy (S) were evaluated. For the isotherm models applied to adsorption
study, the Langmuir isotherm model fits better than the Freundlich isotherm. The maximum adsorption capacity
from the Langmuir isotherm was 54.35 mgg1 of Bi (III). The kinetic study of the adsorption shows that the pseudo
second order model is more appropriate than the pseudo first order model. The result shows that, coconut shell ac-
tivated carbon is an effective adsorbent to remove Bi (III) from aqueous solutions with good adsorption capacity.
Keywords absorption, bismuth (III), coconut shell, activated carbon, isotherm

1 INTRODUCTION and economically [14]. Especially, if the adsorbent is

The level of natural resources of bismuth is about
2107. The world production of bismuth is about
5000 tones per year. Much of the bismuth produced in
the U.S. is obtained as byproduct of refining lead,
copper, tin, silver and gold ores. Bismuth and its com-
pounds are used in semiconductor, cosmetics, alloys
and metallurgical additives as well as in the preparation
and recycling of uranium nuclear fuel [1, 2]. The inor-
ganic bismuth salts are used for medical treatment.
Bismuth containing compounds are being used for
different medicinal purposes, especially for the treat-
ment of syphilis, gastritis, and ulcer. As the use of
bismuth in medicines is increasing, it has spread in the
environment, and the exposure of organisms to bismuth
increases. A number of toxic effects in humans are
attributed to bismuth compounds such as nephropathy,
osteoarthropathy, hepatitis, and neuropathology [3].
Bismuth contamination is becoming an environmental
problem [4]. Therefore, the removal of bismuth is es-
sential for elimination of its contamination.
There are several techniques for removal of Bi
(III) from water, including liquid-liquid extraction [5],
solid phase extraction [6], flotation [7] and adsorption
[8]. The experimental studies on Bi (III) adsorption by
using resins [9] and the electrode surface of metals,
such as Pt (111) and Pt (100) [10], Pt (110) [11], Au [12]
and Si (001) [13], have been reported.
Amongst the many methods available for the re-
moval of heavy metals from aqueous solutions, such
as electrochemical precipitation, ion exchange, ultrafil-
tration, and reverse osmosis, adsorption techniques
have been shown to be a feasible option, both technically
inexpensive and readily available, adsorption process
provides an attractive alternative. Activated carbons
are the effective adsorbents for many pollutant com-
pounds (organic, inorganic, and biological) of concern
in water and wastewater treatment. The major use of
activated carbon is in solution purification and for the
removal of color, odors and other objectionable impu-
rities from liquids, water supplies as well as vegetable
and animal oils [15]. Activated charcoal derived from
coconut shell was found to be a good non conven-
tional adsorbent used for the removal of Cd (II) [16],
Pb [17] and cationic dye [18] from aqueous solutions.
The green coconut shell was used, as it is, for separa-
tion of Cr (VI), Cr (III), As (V) and Cd (II) [19]. Co-
conut shell as well as coconut husk was reported for
removal of Cr (VI), Zn (II) and Ni (II) [20].
In present paper, we report the adsorption study
of bismuth on low cost, easily and abundantly avail-
able adsorbent, activated carbon developed from co-
conut shell. The influence of adsorption time, adsorb-
ent dosage, shaking speed etc. is studied. From ex-
perimental data the isotherm models, kinetic model,
and the thermodynamic parameters are investigated
for adsorption of Bi (III).
2 MATERIALS AND METHOD
2.1 Preparation of materials
All chemicals used were of S. D. Fine Chem. Ltd.
(India). The standard solution with 1 mgmL1 of Bi (III)
was prepared from bismuth nitrate and the required so-
lutions were prepared from dilutions with stock solution.

Received 2010-09-20, accepted 2011-03-18.

* To whom correspondence should be addressed. E-mail: kolekarss2003@yahoo.co.in
 Chin. J. Chem. Eng., Vol. 20, No. 4, August 2012 769

The adsorbent was prepared from dry coconut
shells. The shells were crushed into small pieces,
washed with double distilled water, and dried in oven
at 383 K for 24 h. 25 g dried sample was put in a con-
tainer and 50 ml concentrated H2SO4 was added as
impregnating reagent, then kept for 24 h. After the
acid was leached out the sample was washed with dis-
tilled water till neutral pH. For complete formation as
carbaneous material, it was kept in muffle furnace, for
1 h at 573 K. Dried coconut shell activated carbon
(CSAC) powder was then sieved through BSS-25.
2.2 Characterization of adsorbent
The developed adsorbent CSAC was character-
ized with Fourier transform infra red spectroscopy
(FTIR) (Perkin Elmer Spectrum 100), and scanning
electron microscopy (SEM) (JEOL-JSM 6360 unit,
Japan). The FTIR spectrum shows the peaks at 3310.05,
2899.46, 1703.10, 1608.48, 1167.01, and 1034.86 cm1
for functional groups O H stretch, C H, C O
stretch, C C, S O stretch, and C O stretch, respec-
tively (Fig. 1). These functional groups are responsi-
ble for the better adsorption of Bi (III).
Figure 2 shows the SEM images of CSAC before
and after adsorption confirming the porous nature. The
result of C, H, N, S analyzer (Euro EA, Elemental
Analyzer) indicates the major formation of carbon.
The adsorption depends on surface area of activated
carbon. The surface area and pore diameter of the ad-
sorbents were measured with a NOVA (Quantachrome)
surface area analyzer using a Brunauer-Emmett-Teller
(BET) nitrogen adsorption technique. The total pore
volume was also determined. The BET surface area
analysis indicates that the adsorbent has large surface
area. The percentage amount of elements, surface area
and physical properties are summarized in Table 1.

Figure 1 FTIR spectrum of CSAC

(a) SEM image of CSAC before adsorption of Bi (III) (b) SEM image of CSAC after adsorption of Bi (III)
Figure 2 SEM images of CSAC before/after adsorption of Bi (III)

Table 1 Characteristics of coconut shell activated carbon

Ash Bulk density Moisture BET surface Average pore Total pore Carbon Hydrogen Sulphur
content/% /gml1 content/% area/m2g1 diameter/nm volume/mgL1 /% /% /%
12.62 0.7685 6.75 16.05 2.856 36.64103 59.23 3.41 3.84
770 Chin. J. Chem. Eng., Vol. 20, No. 4, August 2012

2.3 Batch adsorption experiment 3.2 Effect of initial concentration

The batch experiment was carried out by using The removal of Bi (III) is dependent on the initial
orbital shaker with Erlenmeyer flasks. The agitation concentration. Fig. 4 shows that the initial concentra-
was conducted at constant temperature (2992) K for tion increases from 250 mgL1 to 1000 mgL1, the
predetermined period. The adsorption was studied by amount adsorbed increases from 17.62 mgg1 to
varying the variables such as initial concentration of 53.47 mgg1 with the pH value, temperature and other
metal ion, agitation period, and speed. The medium conditions kept constant throughout the study.
was maintained acidic, pH 2, throughout the study,
since Bi (III) precipitates at pH values higher than 2.5
in aqueous solutions [8]. The concentrations of Bi (III)
in residual solutions were analyzed by using AAS
(Perkin Elmer, A Analyzer 300). The initial concentra-
tion of Bi (III) for experiment was varied from 250 to
1000 mgL1 and an adsorbent mass from 0.1 to 0.7 g.
The kinetic and thermodynamic study was done for
different time intervals. For the thermodynamic study
temperature was varied from 303 to 323 K. The equi-
librium adsorption capacity was evaluated using the
following equation,
 C0  Ce V
qe (1)
M Figure 4 Effect of initial concentration of Bi (III) on amount
adsorbed of Bi (III) on CSAC [time 240 min, T (2992) K,
where, qe (mgg1) is the equilibrium adsorption ca- CSAC 0.7 g, 160 rmin1]
pacity, C0 and Ce are the initial and equilibrium con-
centrations (mgL1) of Bi (III) ion solution, V is the
volume, and M is the mass of adsorbent. The adsorption is rapid in the early stage and
then attains an asymptotic value for longer adsorption
time. The percentage removal of Bi (III) decreases
3 RESULTS AND DISCUSSION with the increase of initial Bi (III) concentration. It
may be due to an increase in the number of Bi (III)
3.1 Effect of time on the adsorption
ions for the fixed amount of CSAC. The amount of Bi
(III) adsorbed per unit mass of activated carbon in-
The adsorption of Bi (III) was influenced by time. creases with Bi (III) concentration, may be due to the
Fig. 3 shows the result at (2992) K, 160 rmin1 agi- complete utilization of adsorbent surface and active
tation speed, and initial Bi (III) concentration of 250 sites available.
mgL1. The maximum removal, 98.72%, is obtained
at equilibrium time 240 min and the adsorption is
3.3 Effect of adsorbent dosage and agitation speed
17.62% mgg1. There was no further adsorption as
time increased, thus further study was carried out in
240 min. Figure 5 shows the effect of adsorbent dosage.

Figure 3 Effect of time on removal and amount adsorbed Figure 5 Effect of adsorbent dosage on removal and
of Bi (III), on CSAC [C0 250 mgL1, T (2992) K, CSAC amount adsorbed of Bi (III) on CSAC [C0 250 mgL1,
0.7 g, 160 rmin1] time 240 min, T (2992) K, 160 rmin1]
 Chin. J. Chem. Eng., Vol. 20, No. 4, August 2012
The removal of Bi (III) is 98.72% with 0.7 g CSAC
and the amount adsorbed is 17.62 mgg1. Bi (III) re-
moval efficiency increases with the increase of ad-
sorbent dose. As contact surface of adsorbent particles
and adsorption sites increases, the adsorption effi-
ciency also increases.
Figure 6 shows the effect of agitation speed on
the adsorption of Bi (III) under controlled temperature
160 rmin1 is appropriate.
771
sites and adsorption energy, without interactions be-
tween the adsorbed molecules. It is in good agreement
with a wide variety of experimental data [22, 23].
Ce / qe Ce / qm  1/ qm b (2)
where qm is the maximum loading capacity, Ce and qe
are the equilibrium adsorbate concentrations in the
aqueous and solid phases, respectively, and b is the
equilibrium constant related to the energy of adsorp-
tion [24]. The essential characteristics of the Langmuir
isotherm can be described by a dimensionless equilib-
rium parameter, RL [25],
RL 1/ 1  bCe  (3)
In the present study, the computed values of RL (Table
2) are in the range of 0 to 1, indicating that the adsorp-
tion process is favorable for CSAC adsorbent for the
removal of Bi (III) ions. The values of qm and b are
evaluated from the plot (Fig. 8) and are given in Table 2.
The high value of correlation coefficient R2 indicates a
good relation between the parameters and confirms
the monolayer adsorption of Bi (III) onto the adsorb-
ent surface.

Table 2 Langmuir and Freundlich constant

Figure 6 Effect of agitation speed on removal and amount for the adsorption of Bi (III) on CSAC
adsorbed of Bi (III) on CSAC [C0 250 mgL1, time 240 min,
T (2992) K, CSAC 0.7 g] Langmuir constants Freundlich constants

qm/mgg1 b/mg1 R2 Kf n R2
3.4 Adsorption isotherm 54.350 0.1265 0.995 13.41 3.669 0.969

An adsorption isotherm, which describes the re-

lation between the activity of adsorbent and the quan-
tity of adsorbate on the surface at constant temperature,
is usually employed to describe the adsorption. The
L-shaped isotherm shows more affinity between ad-
sorbent and adsorbate [21]. The adsorption isotherm of
Bi (III) on CSAC adsorbent is shown in Fig. 7. The
Langmuir and Freundlich isotherm models were used
in this work.

Figure 8 Langmuir isotherm for adsorption of Bi (III) on

CSAC

The linear form of the Freundlich isotherm [23] is

Figure 7 Adsorption isotherm for Bi (III) adsorption on
CSAC
The Langmuir model supposes a monolayer ad-
sorption with a homogeneous distribution of adsorption
lg qe lg K f  1/ n lg Ce (4)
1
where, qe is the amount adsorbed (mgg ), Ce is the
equilibrium concentration of adsorbate (mgL1), Kf
and n are Freundlich constants. The values of Kf and n
can be calculated from the intercept and slope (Fig. 9)
and presented in Table 2. The results show that the
adsorption fits the Langmuir equation better.
3.5 Adsorption kinetics
Kinetics of sorption describes the solute uptake
772 Chin. J. Chem. Eng., Vol. 20, No. 4, August 2012

min1 and 16.17 mgg1, while the experimental value

Figure 9 Freundlich isotherm for adsorption of Bi (III) on
CSAC
rate, which in turn governs the residence time of sorp-
tion reaction. The linear form of pseudo first-order
equation (Lagergren equation) is generally expressed
as follows,
of qe is 17.62 mgg1. The correlation coefficients for
the pseudo first-order kinetic model obtained at all the
studied concentrations are low and the calculated qe
values from this model are not reasonable, indicating
that this adsorption system does not follow a pseudo
first-order reaction.
The rearranged linear form of pseudo second-order
adsorption kinetic rate equation is expressed [27] as,
t / q 1/ k2 qe2  t / qe (6)
where, k2 is the rate constant of pseudo second-order
adsorption (gmg1min1). The rate parameters k2 and
qe can be obtained from the intercept and slope of the
plot of t/qt vs. t (Fig. 11) [28]. The values obtained
from the graphs for both adsorption models are given
in Table 3. The results show that the pseudo second-order
is more appropriate than the pseudo first-order.
lg  qe  qt  lg qe  k1t / 2.303 (5)
where, qe and qt are the amount of adsorption at equi-
librium (mgg1) and at time t (min) respectively, and
k1 is the rate constant of the pseudo first-order adsorp-
tion process. When the values of lg(qe  qt) are corre-
lated with t, a linear relationship is obtained (Fig. 10),
from which k1 and qe can be determined (Table 3)
from the slope and intercept, respectively [26].
The Lagergren plot (Fig. 10) is for the adsorption
of Bi (III) at 0.7 g dosage of CSAC, at the initial con-
centration of metal ion to be 250 mgL1, constant
temperature of (2992) K and agitated with fixed 50 Figure 11 Pseudo second-order for adsorption of Bi (III)
ml quantity and 160 rmin1. on CSAC

3.6 Intraparticle diffusion

The most commonly used technique for identify-

ing the mechanism involved in the sorption process is
by fitting the experimental data in an intraparticle dif-
fusion plot. A good fit to the experimental data means
that, the sorption rate is governed by intraparticle dif-
fusion, which is the rate-limiting step. According to
Weber and Morris, an intraparticle diffusion coeffi-
cient kid is defined
qt kid t1/ 2  c (7)
1 1/2
The kid (mgg min ) value can be obtained from
Figure 10 Pseudo first-order for adsorption of Bi (III) on the slope of the plot of qt (mgg1) versus t1/2 (Fig. 12).
CSAC The slope of the linear portion of the plot is de-
fined as the intraparticle diffusion parameter kid, while
The k1 and qe values are found to be 0.66103 the intercept reflects the boundary layer effect. The

Table 3 Kinetic parameters for the effect of temperature on removal of Bi (III)

Pseudo first order Pseudo second order Intraparticle diffusion equation
1 3 1 1 3 1
qe (exp.)/mgg k110 /min qe (calc.)/mgg R2
k210 qe (calc.)/mgg R 2
kid/mgg1min1 R2

17.62 0.66 16.17 0.869 2.159 18.62 0.978 0.880 0.976

 Chin. J. Chem. Eng., Vol. 20, No. 4, August 2012 773

Figure 12 Intraparticle diffusion for adsorption of Bi (III)
on CSAC
larger the intercept, the greater the contribution of the
surface adsorption in the rate limiting step. Higher
values of the intraparticle rate constants illustrate an
enhancement in the rate of adsorption, as well as a
better adsorption mechanism. However, these plots
indicate that the intraparticle diffusion is not the only
rate controlling step because it does not pass through
the origin. The rate constant of intraparticle diffusion
is given in Table 3. The diffusion process is controlled
by the diffusion of ions within the adsorbent [2931].
3.7 Effect of temperature
Figure 13 shows that the adsorption capacity of
Bi (III) onto CSAC increase with temperature. The ad-
sorption capacity increases from 54.9 to 59.09 mgg1
for the initial concentration of 1000 mgL1 at pH 2.0.
Kc bCAe / Ce (8)
where, bCAe is the amount adsorbed on solid at equi-
librium and Ce is the equilibrium concentration.
The standard Gibbs free energy (G) is calcu-
late as,
(9)
where, T is the temperature in Kelvin and R is the gas
constant. Thermodynamic parameters such as change
in free energy (G) (kJmol1), enthalpy (H)
(kJmol1) and entropy (S) (Jmol1K1) are deter-
mined using the following equation,
(10)
where, H and S are obtained from the slope and
intercept of the vant Hoffs plot of lnKc versus 1/T as
shown in Fig. 14. Positive value of H indicates that
the adsorption process is endothermic. The negative
values of G (Table 4) reflect the feasibility of the
process and the value becomes more negative as tem-
perature increases, indicating that the adsorption is
highly favorable and spontaneous. The positive value
of standard S entropy shows the increased disorder
and randomness at the solid solution interface of bis-
muth ion and CSAC. The enhancement of adsorption
capacity of the activated carbon at higher temperatures
is attributed to the enlargement of pore size and acti-
vation of the adsorbent surface. The enrichment in the
adsorption capacity may be due to the chemical inter-
action between adsorbates and adsorbent, creating
some new adsorption sites or increasing the rate of
intraparticle diffusion of Bi (III) ions at higher tem-
peratures [32, 33].

Figure 14 vant Hoffs plot of adsorption of Bi (III) on

Figure 13 Effect of temperature on amount adsorbed of CSAC
Bi (III) on CSAC (C0 1000 mgL1, time 240 min, CSAC
0.7 g, 160 rmin1)
Table 4 Thermodynamic parameters of CSAC

Temperature plays a major role in the adsorption T/K G /kJmol1


H/kJmol1 S/Jmol1K1
of heavy metals on adsorbent. The magnitude of the 303 2.830
heat effect for the adsorption process is one of the
308 2.960
most important criteria for the efficient removal of
heavy metals from the water. The adsorption capacity 313 3.058 0.348 2.2791
of carbon increases with temperature from 303 to 323 K. 318 3.143
The equilibrium constant Kc is evaluated at each tem- 323 3.214
perature using the following relationship,
774 Chin. J. Chem. Eng., Vol. 20, No. 4, August 2012
4 CONCLUSIONS
The adsorbent was easily prepared from dry co-
conut shell, which is abundantly available waste. It
was developed as porous, effective and economically
affordable activated carbon and its formation was
confirmed with various characterizations such as C, H,
N, S analyzer, SEM, FTIR and BET surface area
analysis. The coconut shell activated carbon has a
high capacity to adsorb Bi (III) ions from aqueous
solutions with amount adsorbed from 17.62 mgg1 to
53.47 mgg1 as the initial concentration increased up
to 1000 mgL1. All adsorptions were carried out in
acidic pH and the required period was only 4 h. Re-
moval percentage was significant, i.e. 98.72%. The
adsorption isotherm is an L shaped curve, which indi-
cates less competition between adsorbent and adsorbate.
The models of adsorption, Langmuir and Freundlich
were used, among which the Langmuir equation shows
more applicability to the experimental data than the
Freundlich isotherm. The rate of adsorption was also
investigated with kinetic study and it was found that
the experimental data fits better in pseudo second or-
der than pseudo first order. The adsorption was feasi-
ble, spontaneous and endothermic, which was con-
firmed by the evaluation of thermodynamic parame-
ters viz. H, G and S. The results show that the
activated carbon from coconut shell can be effectively
applied for the removal of Bi (III) from aqueous solu-
tions. Easy and inexpensive availability and suitability
for the production of activated carbon from coconut
shell, makes it one of the biomass wastes that can be
effectively utilized for removal Bi (III) from aqueous
solutions.
ACKNOWLEDGEMENTS
The authors acknowledge the DST-FIST, UGC-SAP
facilities, Department of Chemistry, Shivaji University,
Kolhapur. Authors are grateful to Professor G. S. Go-
kavi for his valuable suggestions.
NOMENCLATURE
1
b Langmuir adsorption intensity constant, mg
CAe amount adsorbed on solid at equilibrium, mgL1
Ce equilibrium concentration of Bi (III) ion solution, mgL1
C0 initial concentration of Bi (III) ion solution, mgL1
c constant
G standard Gibbs energy of adsorption, kJmol1
H standard enthalpy of adsorption, kJmol1
Kc equilibrium constant
Kf Freundlich multilayer adsorption capacity, mgg1
kid intraparticle diffusion rate, mgg1min1/2
k1 rate constant for pseudo first-order adsorption
k2 rate constants of pseudo second-order adsorption
M mass of adsorbent, g
qe amount adsorbed on adsorbent, mgg1
qm Langmuir monolayer adsorption capacity, mgg1
qt amount adsorbed at time t, mgg1
RL dimensionless equilibrium parameter
R2 correlation coefficient
S standard entropy of adsorption, Jmol1K1
T temperature, K
t time, min
V volume of the solution, L
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