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ORI GI NAL Open Access

Fixed-bed adsorption dynamics of Pb (II)


adsorption from aqueous solution using
nanostructured -alumina
Zahra Saadi, Reyhane Saadi and Reza Fazaeli
*
Abstract
In the present study, removal of metal ions Pb (II) using nanostructured -alumina was investigated in a fixed-bed
column. Comparison of Thomas, Yoon-Nelson, and Adams-Bohart models with experimental kinetic results was
done, and model parameters were evaluated by linear regression analysis for Pb
2+
adsorption in different bed
heights, initial concentrations, and flow rates. The obtained experimental data are in good agreement with Thomas
and Yoon-Nelson models, but in the case of Adams-Bohart model, low correlation coefficient is observed.
Keywords: Lead; Nanostructured -alumina; Adsorption kinetic models; Fixed-bed column
Background
Industrial wastewater polluted with heavy metals has en-
dangered the human health and environment. Lead is
one of the most extensive toxic metals in the environ-
ment [1], so this study has discussed on the continuous
flow removal of lead from aqueous solution.
A number of conventional methods for the removal of
heavy metals from aqueous solutions have been reported
such as precipitation as hydroxides, carbonates, or sul-
fides; subsequent liquidsolid separation by gravity set-
tling; flotation; ultra-filtration; coagulation; reverse
osmosis; ion exchange; electrodialysis; liquid-liquid ex-
traction; membrane processes; evaporation; and bio-
logical treatment.
Most of these methods have disadvantages such as high-
cost devices, toxic waste production, low efficiency, and
require high energy and space. Adsorption process has
been shown as an alternative economic method for the re-
moval of heavy metals from aqueous solutions [2-9].
A number of materials have also been used to remove
heavy metals from wastewater, such as activated carbon
[10], silica [11], titanium dioxide [11], calcium carbonate
[11], alumina [11,12], and recently, various nanomaterials
such as nanometal oxides [13], carbon nanotubes [14],
and nanozeolite composites [15].
Nanoalumina has several crystalline form and mainly
used as -alumina form.
By considering the -alumina, surface area is in the
range of 150 to 500 m
2
/g and pore radius is in the range
of 1.5 to 6 nm, so -alumina is anticipated to be more
adsorptive active than -alumina. -Al
2
O
3
nanoparticles
is a promising material as an adsorbent because of its
large specific surface area, high adsorption capacity,
mechanical strength, and low-temperature modification.
Nanoalumina is used widely as electrical insulator, catalyst,
and base catalyst in many chemical reactions, membrane
processes, microelectronics, and water and wastewater
purification [16-21].
Unuabonah et al. studied in polymer-clay-based com-
posite adsorbent to remove lead (II) ions from aqueous
solution in a fixed-bed mode. The increase in bed height
and initial metal ion concentration increased the adsorp-
tion capacity of lead (II). The Yoon-Nelson, Thomas,
and Clark models were found to give good fit to adsorp-
tion data. On the other hand, Adams-Bohart was found
to be a poor predictor for the column operation [22].
Kundu and Gupta studied in continuous fixed bed to
evaluate the efficiency of iron oxide-coated cement
(IOCC) as an adsorbent for the removal of As(III) from
* Correspondence: r_fazaeli@azad.ac.ir
Department of Chemical engineering, Faculty of engineering, South Tehran
Branch, Islamic Azad University, P.O. Box 113654435, Tehran, Iran
2013 Saadi et al.; licensee Springer. This is an Open Access article distributed under the terms of the Creative Commons
Attribution License (http://creativecommons.org/licenses/by/2.0), which permits unrestricted use, distribution, and reproduction
in any medium, provided the original work is properly cited.
Saadi et al. Journal Of Nanostructure in Chemistry 2013, :
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aqueous solution under the effect of various process pa-
rameters like bed depth, flow rate, and initial As(III)
concentrations. The dynamics of the adsorption process
was modeled by bed depth service time (BDST), mass
transfer, Thomas, and Yoon-Nelson models. The
Thomas and Yoon-Nelson model predictions were in
very good agreement with the experimental results at all
the process parameters studied, indicating that they were
very suitable for IOCC column design [23].
Rao et al. studied in Syzygium cumini L leaf powder as
a biosorbent for generating adsorption data in a fixed-
bed minicolumn. Effect of flow rate, initial Cd (II)
concentration, and bed height was the experimental pa-
rameters chosen to obtain breakthrough curves. Adams-
Bohart, BDST, Thomas, and Yoon-Nelson models were
applied to the data for predicting breakthrough curves
and to determine the characteristic parameters. Promin-
ent and unique characteristic features of the respective
models like service time (Hutchins BDST model), ad-
sorption capacity (Thomas model), and time required
for 50% breakthrough (Yoon-Nelson model) were deter-
mined [24].
Han et al. studied in continuous adsorption in a fixed-
bed column using phoenix tree leaf powder as an ad-
sorbent for the removal of methylene blue (MB) from
aqueous solution. The effect of flow rate, influent MB
concentration, and bed depth on the adsorption charac-
teristics of adsorbent was investigated at pH 7.4. Four
kinetic models, Thomas, Adams-Bohart, Yoon-Nelson,
and Clark, were applied to experimental data to predict
the breakthrough curves by nonlinear regression and to
determine the characteristic parameters of the column
that are useful for process design [25].
Purpose of this study is removal of Pb
2+
by nanostruc-
tured -alumina using fixed bed with upward flow. Effects
of parameters such as flow rate, initial concentration of
lead, and fixed bed height on lead adsorption using
Thomas, Yoon-Nelson, and Adams-Bohart kinetic models
were considered.
Materials
Nanostructured -alumina prepared from nano Pars
Lima Co. (Tehran, Iran) as adsorbent and lead nitrate as
adsorbate were obtained from Merck C. (Germany). All
materials were prepared with high purity. Double dis-
tilled water was used. Dilute HNO
3
and NaOH were
used to adjust pH.
Atomic absorption spectrophotometer with acetylene
flame (PG 990) was used for the measurement of lead
ions; digital pH meter (Sartorius (PB-11)) was used to
measure pH. Different flow rates were performed using a
peristaltic pump ETATRON DS (Rome, Italy) that is cap-
able to adjust flow rates in milliliter-per-minute range.
Continuous flow studies
Thomas model
The Thomas model is widely used in column perform-
ance modeling. Its derivation assumes Langmuir kinetics
of adsorption-desorption and no axial dispersion. The
Figure 1 Schematic diagram of the experimental column.
Table 1 Characterization of nanostructured -alumina
Step number Characteristics Value
1 Particle form Powder
2 Particle size, nm 20
3 Surface area(minimum), m
2
/g 138
4 Bulk density, g/cm
3
0.9
5 Porosity 0.5246
6 Chemical analysis
Al
2
O
3
(minimum) % 99
Ca(maximum), ppm 25
V(maximum), ppm 7
CL(maximum), ppm 315
Na(maximum), ppm 70
Mn(maximum), ppm 3
Co(maximum), ppm 2
Table 2 Thomas model parameters using linear
regression analysis for Pb2+ adsorption under various
operating conditions
Q
(mL/min)
L
(cm)
C
0
(mg/L) q
e
,
max
(mg/g)
k
Th
(mL/min.mg)
R
2
q
e,max(exp)
(mg/g)
3 10 100 49.635 0.031 0.9109 47.79
6 10 100 46.607 0.052 0.9112 42.6
9 10 100 44.457 0.094 0.9308 38.15
6 5 100 42.962 0.118 0.9182 38.62
6 15 100 48.546 0.038 0.9147 44.99
6 10 65 43.288 0.064 0.9401 39.89
6 10 150 49.181 0.049 0.9319 43.59
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expression for the Thomas model for adsorption column
is given as Equation 1 [26]:
C
t
C
0

1
1 exp
k
Th
q
e
x
Q

k
Th
C
0
t
h i ; 1
where k
Th
(mL/min.mg) is the Thomas model constant,
q
e
(mg/g) is the predicted adsorption capacity, x is mass
of adsorbent (g), Q is influent flow rate (mL/min), C
0
is
initial solution concentration (mg/L), and C
t
is effluent
solution concentration (mg/L). The linear form of
Thomas model is expressed as Equation 2:
ln
C
0
C
t
1


k
Th
q
e
x
Q
k
Th
C
0
t 2
Yoon-Nelson model
This model is simpler than other models and also re-
quires no data about the characteristics of the system
such as the type of adsorbent and the physical properties
of the adsorption bed.
The Yoon-Nelson equation is expressed as Equa-
tion 3 [27]:
C
t
C
0
C
t
exp k
YN
tk
YN
; 3
where k
YN
(1/min) is the rate constant and (min) is the
time required for 50% adsorbate breakthrough. The linear
form of Yoon-Nelson model is expressed as Equation 4:
Figure 2 Linear plot of Thomas model with experimental data at different heights. C
0
= 100 mg/L, Q
0
= 6 mL/min.
Figure 3 Linear plot of Thomas model with experimental data at different flow rates. C
0
= 100 mg/L, L
0
= 10 cm.
Saadi et al. Journal Of Nanostructure in Chemistry 2013, : Page 3 of 8
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ln
C
t
C
0
C
t
k
YN
tk
YN
: 4
Adams-Bohart model
The Adams-Bohart model is based on the assumption
that the rate of adsorption is proportional to both the
concentration of the adsorbing species and the residual
capacity of the adsorbent. The Adams-Bohart model is
only used for the description of the initial part of the
breakthrough curve and is expressed as Equation 5 [28]:
C
t
C
0
exp k
AB
C
0
tk
AB
N
0
z
U
0

; 5
where k
AB
(l/min.mg) is rate constant of Adams-Bohart
model, z (cm) is the bed depth, N
0
(mg/L) is maximum
ion adsorption capacity per unit volume of adsorbent
column, and U
0
(cm/min) is the linear velocity of influ-
ent solution. The linear form of Adams-Bohart model is
expressed as Equation 6:
ln
C
t
C
0

k
AB
C
0
tk
AB
N
0
z
U
0
: 6
Methods
A Pyrex column (Sigma-Aldrich, St. Louis, MO, USA)
30 cm in height and 1 cm in diameter was used with up-
ward flow. In order to avoid the exiting adsorbent from
column, glass wool at the top and bottom of the column
was applied. Schematic of experimental set-up is shown
in Figure 1.
In order to investigate the effect of flow rate on the
behavior of the adsorbent column, flow rates 3, 6, and 9
mL/min with constant concentrations 100 ppm, con-
stant bed height 10 cm were used. In order to investigate
the effect of height on the behavior of the adsorbent col-
umn, heights 5, 10, and 15 cm (equivalent with 3.5342,
7.0685, and 10.6028 gr) with constant concentrations
100 ppm and constant flow rate 6 mL/min were used,
and in order to investigate the effect of initial concentra-
tion of lead ion on behavior of the adsorbent column,
concentrations 65, 100, and 150 ppm with constant bed
height 10 cm and constant flow rate 6 mL/min were
used. Effluent samples from the column were collected
at specified time intervals, and remaining lead concen-
trations in the solution were measured by atomic ab-
sorption technique.
In all experiments, the temperature and pH values
were adjusted to 25C and 4.5, respectively.
Maximum adsorption capacity of the adsorbent in a
fixed-bed column is calculated by Equations 7 and 8 [22]:
q
e

Q
1000W

t
total
0
C
0
C
t
dt 7
Table 3 Yoon-Nelson model parameters using linear
regression analysis for Pb2+ adsorption under various
operating conditions
Q(mL/min) L(cm) C
0
(mg/L) (min) k
YN
(1/min) R
2
3 10 100 1,196.516 0.003 0.9109
6 10 100 549.076 0.005 0.9112
9 10 100 349.17 0.009 0.9308
6 5 100 253.067 0.011 0.9182
6 15 100 857.894 0.003 0.9147
6 10 65 777.119 0.004 0.9401
6 10 150 383.662 0.007 0.9319
Figure 4 Linear plot of Thomas model with experimental data at different concentrations. Q
0
= 6 mL/min, L
0
= 10 cm.
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q
e;max

q
total
w
; 8
where q
e,max
(mg/g) is maximum adsorption capacity of
the adsorbent, Q (mL/min) is flow rate, C
0
(mg/L) is initial
concentration, C
t
(mg/L) is concentration in specified
time, and w (g) is mass of the adsorbent.
Results and discussions
Characterization of adsorbent
Characterization of nanostructured -alumina is presented
in Table 1.
Evaluation of Thomas model parameters
To determine maximum adsorption capacity of the ad-
sorbent (q
e,max
) and kinetic coefficient (k
Th
) in Thomas
model, experimental data were fit into the Equation 2.
Linear regression results and values of R
2
are listed in
Table 2, where values of R
2
ranged from 0.9109 to
0.9401. According to Table 2, the calculated q
e
,
max
from
Thomas model is greater than experimental q
e,max
. It is
also seen in Table 2 that as C
0
and adsorbent weight in-
creased, the value of q
e,max
and k
Th
increased and de-
creased, respectively. This is because the driving force
for adsorption is the difference in concentration between
the lead on the adsorbent and in the solution [29]. As
flow rate increased, the value of q
e,max
decreased. This is
because of unavailability of reaction sites, but the value
of k
Th
increased. Linear form of Thomas model in differ-
ent heights, flow rates, and concentrations is shown in
Figures 2, 3, and 4, respectively. As can be observed, the
experimental data are in good agreement with the theor-
etical results.
Evaluation of Yoon-Nelson model parameters
Linear regression results and values of R
2
are presented
in Table 3. It was observed that rate constant (k
YN
) and
Figure 6 Linear plot of Yoon-Nelson model with experimental data at different flow rates. C
0
= 50 mg/L, L
0
= 15 cm.
Figure 5 Linear plot of Yoon-Nelson model with experimental data at different heights. C
0
= 100 mg/L, Q
0
= 6 mL/min.
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time required for 50% adsorbate breakthrough () de-
creased and increased, respectively, with increasing ad-
sorbent dose. Also, it was found that the rate constant
(k
YN
) increases as much as flow rate increases. Because
of less residence time of metal ion in adsorbent bed,
time required for 50% adsorbate breakthrough () de-
creased with increasing flow rate (Table 3). Linear plot
of Yoon-Nelson model in different heights, flow rates,
and concentrations is shown in Figures 5, 6, and 7, re-
spectively. As can be observed, the experimental data
are fit well with the model. It can be concluded that
both Thomas and Yoon-Nelson models are appropriate
models to describe fixed-bed operations.
Evaluation of Adams-Bohart model parameters
Linear regression results (Table 4) are shown that ad-
sorption capacity of the adsorbent (N
0
) and kinetic con-
stant of the model (k
AB
) increased and decreased,
respectively, with increasing adsorbent dose and initial
lead concentration. Because of more saturation of ad-
sorbent sites, adsorption capacity of the adsorbent (N
0
)
decreased with increasing flow rate. Also, kinetic con-
stant of the model (k
AB
) increased with increasing flow
rate. Linear plot of Adams-Bohart model in different
heights, flow rates, and concentrations is shown in Fig-
ures 8, 9, and 10, respectively.
The lower R
2
values relative to the other models can
be interpreted that the Adams-Bohart model is not as
appropriate a predictor for the breakthrough curve.
Conclusions
Studies on continuous adsorption using nanostructured
-alumina to remove Pb (II) indicate that this adsorbent
has high ability to remove heavy metal ions from aque-
ous solutions.
Adsorption capacity strongly depends on flow rate, in-
fluent concentration, and bed height.
Comparison of Thomas, Yoon-Nelson, and Adams-Bohart
kinetic models with experimental data was performed,
and model parameters were determined by linear regres-
sion analysis for Pb
2+
adsorption under various operating
conditions. The experimental data fit well with Thomas
and Yoon-Nelson models, but the Adams-Bohart model
predicted poor performance of fixed-bed column.
Results showed that with increasing initial concentra-
tion of lead, adsorption capacity of the adsorbent and
kinetic constant of model increased and decreased, re-
spectively, in the Thomas model. Fifty percent adsorbate
breakthrough and rate constant decreased and increased,
respectively, in the Yoon-Nelson model. Capacity of the
adsorbent and kinetic constant increased and decreased,
respectively, in the Adams-Bohart model.
Table 4 Adams-Bohart model parameters using linear
regression analysis for Pb2+ adsorption under various
operating conditions
Q(mL/min) L(cm) C
0
(mg/L) N
0
(mg/L) k
AB
(mL/min.mg) R
2
3 10 100 37,182.271 0.099 0.8699
6 10 100 30,835.733 0.206 0.8669
9 10 100 27,371.123 0.334 0.8813
6 5 100 29,346.952 0.367 0.8488
6 15 100 32,464.054 0.15 0.8733
6 10 65 30,136.07 0.207 0.9096
6 10 150 35,097.074 0.118 0.7767
Figure 7 Linear plot of Yoon-Nelson model with experimental data at different concentrations. Q
0
= 6 mL/min, L
0
= 10 cm.
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Figure 9 Linear plot of Adams-Bohart model with experimental data at different flow rates. C
0
= 100 mg/L, L
0
= 10 cm.
Figure 8 Linear plot of Adams-Bohart model with experimental data at different height. C
0
= 100 mg/L, Q
0
= 6 mL/min.
Figure 10 Linear plot of Adams-Bohart model with experimental data at different concentration. Q
0
= 6 mL/min, L
0
= 10 cm.
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Competing interests
The authors declare that they have no competing interest.
Authors contributions
ZS carried out the preparation of experimental elements. ZS and RS
participated in doing the experiments and analyzed, interpreted, and
organized the data. RF designed and coordinated the overall project.
ZS, RS and RF carried out the manuscript preparation. All authors read
and approved the final manuscript.
Acknowledgments
The authors wish to thank Mr. Bagher Biralvand for his great help in the
atomic absorption analysis.
Received: 26 May 2013 Accepted: 25 June 2013
Published:
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doi:
Cite this article as: Saadi et al.: Fixed-bed adsorption dynamics of Pb (II)
adsorption from aqueous solution using nanostructured -alumina.
Journal Of Nanostructure in Chemistry 2013 :.
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Saadi et al. Journal Of Nanostructure in Chemistry 2013, : Page 8 of 8
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15 Jul 2013
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2013, 3:48
2013, 3:48
http://www.jnanochem.com/content/3/1/48

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