Desalination 276 (2011) 148–153

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Desalination
j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / d e s a l

Adsorption of Pb(II) from aqueous solutions using activated carbon developed from
Apricot stone
Lotfi Mouni a,⁎, Djoudi Merabet a, Abdelkrim Bouzaza b, Lazhar Belkhiri c
a
Département de génie des procèdes, faculté de Technologie, Université de Bejaia, Targa, Ouzemour, 06000, Algeria
b
Equipe “Chimie et Ingéniérie des Procédés” UMR 6226 “Sciences Chimiques de Rennes” Ecole Nationale Supérieure de Chimie de Rennes, Avenue du Général Leclerc, 35700 Rennes, France
c
Laboratoire de génie de l'environnement, Département d'Hydraulique, Université de Batna 05000, Algeria

a r t i c l e i n f o a b s t r a c t

Article history: Low-cost activated carbon was prepared from Apricot stone material by chemical activation with sulphuric
Received 16 December 2010 acid for the adsorption of Pb(II) from dilute aqueous solution. The activated carbon developed shows
Received in revised form 10 March 2011 substantial capacity to adsorb Pb(II) from dilute aqueous solutions. The parameters studied include physical
Accepted 12 March 2011
and chemical properties of adsorbent, pH, adsorbent dose, contact time and initial concentrations. The percent
Available online 6 April 2011
removal increased with pH from 1.5 to 5. The optimum pH required for maximum adsorption was found to be
Keywords:
6.0. Adsorption kinetics data were modeled using the pseudo-first and pseudo-second-order models. The
Toxic metal removal results indicate that the second-order model best describes adsorption kinetic data. The isotherm equilibrium
Adsorption data were well fitted by the Langmuir and Freundlich models. The estimated maximum capacities of lead ions
Isotherm adsorbed by Apricot stone activated with sulphuric acid were 21.38 mg g−1. The adsorbent derived from this
Lead material is expected to be an economical product for metal ion remediation from water and wastewater.
Apricot stone © 2011 Elsevier B.V. All rights reserved.

1. Introduction
Heavy metal contamination is recognized as a priority problem at
hazardous waste sites. The contamination by metals can occur in both
soils and groundwater as a result of industrial activities such as
mining, metal plating, tanneries, and petroleum refining [1–3].
Another source of groundwater metal contamination is related to
the migration of leachates from uncontrolled landfill sites. Because of
their strong complexing capacity (because of the high concentration
of organic and inorganic ligands), metals can be strongly extracted by
the dumped wastes and move easily to the groundwater [4]. With
respect to the other categories of contaminants, heavy metals are
particularly dangerous because they are not biodegradable and
accumulate in living organisms.
Lead poisoning causes damage to liver, kidney and reduction in
hemoglobin formation, mental retardation, infertility and abnormal-
ities in pregnant women. Due to the hazardous nature of lead (II), it
directly or indirectly may cause anemia, headache, chills, diarrhea and
poisoning leading to the dysfunction of kidneys, reproductive system,
liver, brain and central nervous system also.
Available technologies for heavy metal-contaminated waste
stream and soil treatments are usually carbon adsorption, ion
exchange, precipitation, membrane filtration, reverse osmosis, and
solidification/stabilization. Sorbent-based processes are probably the
⁎ Corresponding author. Tel.: + 213 776865678.
E-mail address: lotfimouni@gmail.com (L. Mouni).
most used, although the cost of substrate materials and regeneration is
a limiting factor. Thus, great attention is given to the characterization
of the sorption properties of alternative low-cost materials that range
from natural sorbent phases to dead biomass [5]. Disposal of
agricultural by-products has become a major, costly waste disposal
problem. Produced activated carbons are used for removing organic
chemicals and metals from wastewater. A wide variety of materials
such as rice husk [6], modified cellulosic materials [7], wheat brean [8],
modified bark [9], sawdust [6] and pine bark [10], are being used as
low-cost alternatives to expensive adsorbents. Most of the activated
carbons are produced by a two-stage process carbonization followed
by activation. The first step is to enrich the carbon content and to create
an initial porosity and the activation process helps in enhancing the
pore structure. Basically, the activation can be done by two different
processes: physical and chemical. In fact, there are two important
advantages of chemical activation in comparison to physical activa-
tion. One is the lower temperature in which the process is
accomplished. The other is that the global yield of the chemical
activation tends to be greater since burn off char is not required.
Among the numerous dehydrating agents, sulphuric acid in particular
is the widely used chemical agent in the preparation of activated
carbon. In the present work the sorption of lead ion from aqueous
solution by using activated carbon produced from Apricot stone was
investigated. The adsorption capacity of adsorbent was investigated
using batch experiments. The influence of pH, contact time, metal ions
and adsorbent concentrations were investigated and the experimental
data obtained were evaluated and fitted using adsorbent equilibrium
isotherms, and kinetic models.

0011-9164/$ – see front matter © 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2011.03.038
 L. Mouni et al. / Desalination 276 (2011) 148–153
2. Experimental technique
2.1. Preparation of activated carbon
Apricot fruits are widely consumed fresh and in processed forms as
juice and jams. Apricot stone, as a by-product of the Apricot juice
industry is therefore an inexpensive materials. The Apricot stone were
washed with distilled water, dried at 105 °C and crushed in a mortar.
Sulfuric acid, as a chemical reagent, added during the activation
process help to produce more specific area. The activation procedure
was accomplished as follow: Apricot stone was impregnated with a
solution of 50% H2SO4 in water. Then this suspension (H2SO4 and
untreated Apricot stone) was heated at 200 °C for 2 h and then filtered.
The resulting chemical loaded Apricot stone was placed in a furnace
and heated (10 °C min−1) to the final carbonization temperature of
650 °C for 30 min [11]. In all experiments, the heating rate was kept
constant. After cooling, the activated carbon was washed to get it acid
free and its pH was checked. The carbonized adsorbents were dried
and rewashed many times until its pH reaches 4. After this the
activated carbon was deacidified by use of water and ammonia
solution in later stages. Deacidification was done in following manner.
After 20–25 times washing carbon was treated with liquid aqueous
ammonia solution in such a fashion that it does not affect the surface
properties. Then activated carbon was dried at 60 °C [11]. The
carbonized material was sieved (250–125 μm size) and used for
adsorption experiments. The specific surface area of the activated
carbon was measured by N2 gas adsorption at −196 °C (COULTER-
SA3100). BET equation was used to calculate the specific surface area.
The physical characteristics of the adsorbent are given in Table 1.
2.2. Method of experiment
Batch reactor tests were carried out to study the effect of various
operating parameters on the adsorption rate. Adsorption experiments
of Pb(II) on activated carbon were conducted containing different
weighted amounts of each sample with 100 ml solution of 10, 30, 50,
80 and 100 mg/l of initial concentration. The aqueous lead solutions
were prepared by dissolving known amount of corresponding nitrate
salt (Pb(NO3)2) in 1 l of ordinary water.
2.3. Adsorption experiments
Batch adsorption experiments were carried out in a series of
stoppered reagent bottles. A weighted amount (0.1 g) of adsorbent
was introduced into reagent bottles (200 ml) containing various
concentrations of lead. The total volume of the aqueous solution is
equal to 100 ml. The solution pH was adjusted to the desired value by
adding HCl or NaOH. Then, the bottles were shaked at room
temperature (20 ± 2 °C) using a mechanical shaker for a prescribed
time to attain the equilibrium. Then the solutions were filtered and
the final lead(II) concentrations of metal ions were determined by
using an atomic absorption spectrophotometer (Shimadzu AA6500)
with lead hallow cathode lamp and air-acetylene flame. The
instrument calibration was periodically checked by using standard
Table 1
Main characteristic of the adsorbent.
Parameters
Pore volume (cm3 g−1 )
a
BET surface area (m2 g−1)
Iodine number (mg g−1)
Methylene blue number (mg g−1)
Bulk density
Acidic surface functional groups (mmol g−1)
a
BET surface area corresponds to the particle size 250–125 μm.
149
metal solutions for every 15 readings. The effects of concentration
(10–100 mg/l), contact time (2–180 min), solution pH (1.5–9) and
adsorbent concentration (0.2–2 g) were studied. Blank solutions were
treated similarly (without adsorbent) and the concentration at the
end of each operation was taken as the initial one.
The percent removal of heavy metal from solution was calculated
by the following equation:
ðC0 −Ce Þ
Removal ð%Þ = 100 ð1Þ
C0
Where C0 and Ce represent initial and equilibrium concentrations
respectively; (mg/l) of lead. Isotherm studies were recorded by
varying the initial concentrations of heavy metal solutions from 10 to
100 mg/l for lead. A known amount of different activated carbons is
added into solutions followed by agitating the mixture at 150 rpm till
equilibrium. The adsorption capacity qe (mg/g) after equilibrium was
calculated by mass balance relationship equation as follows:
ðC0−CeÞ × V
qe = ð2Þ
m
Where V is the volume of the solution (L) and m is the mass of the
adsorbent (g).
3. Results and discussions
3.1. Effect of agitation time and initial concentration on Pb (II) adsorption
Fig. 1 shows the effects of agitation time and Pb(II) concentration
on adsorption capacity. We note that the adsorption of Pb (II)
increases with an increase in agitation time and attains equilibrium in
10 min for 10 mg/l Pb(II) and 20 min for 30, 50, 80 and 100 mg/l Pb(II).
This result is interesting because equilibrium time is one of the
parameters for economical wastewater treatment plant applications.
According to these results, the agitation time was fixed at 5 h for the
rest of the batch experiments to make sure that equilibrium was
reached. It also shows that increases in metal ion concentration
increased the amount of metal ion uptake per unit weight of carbon
(mg/g).
ASAC
0.192
393.2
154
91
0.81
0.78
Fig. 1. Effect of contact time for the adsorption of lead ions onto activated carbon from
Apricote stone at T = 20 °C, pH = 6, S/L = 1 g/1 l.
150 L. Mouni et al. / Desalination 276 (2011) 148–153
3.2. Effect of adsorbent concentrations
One of the parameters that strongly affect the sorption capacity is
the concentration of the adsorbents. At a fixed metal concentration, it
can easily be inferred that the percent removal of metal ions increases
with increasing weight of the adsorbents as shown from Fig. 2. This is
due to the greater availability of the exchangeable sites or surface area
at higher concentration of the adsorbent.
For the complete removal of Pb (II) from 1000 ml solution at 50
and 100 mg/l concentration, a maximum carbon concentration of 1.5
and 2.0 g/l, is required respectively.
3.3. Effect of particle size on Pb (II) removal
The percent removal of Pb (II) decreased with increasing adsorbent
particle size. The percent removal for particle size ranges of 750–500,
500–250 μm and 250–125 μm was 76.4%, 81.6% and 86.7%, respective-
ly. The adsorption of Pb (II) attains equilibrium in 120, 90 and 60 min
for particle size ranges of 750–500, 500–250 μm, and 250–125 μm with
specific areas equal to 212, 278 and 393 m2 g−1, respectively. This is
because adsorption is a surface controlled phenomenon, so the smaller
adsorbent particle size offers a comparatively larger and more acces-
sible surface and hence, higher adsorption occurs at equilibrium.
3.4. Effect of pH
The pH of the solution has a significant impact on the uptake of
heavy metals, since it determines the surface charge of the adsorbent,
the degree of ionization and speciation of the adsorbate. In order to
establish the effect of pH on the biosorption of lead (II) ion, the batch
equilibrium studies at different pH values were carried out in the
range of 1.5–9 (Fig. 3). We note that the uptake is quite low at lesser
pH. However, with the increase in pH, a significant enhancement in
adsorption is recorded. The optimum pH for ASAC-Pb system was
found to be 6.0 with the removal of about 88.3% Pb(II) from the
solution with initial lead concentration of 50 mg/l. At lower pH, Pb(II)
uptake decreased because the surface area of the adsorbent was more
protonated and competitive adsorption occurred between H+ protons
and free Pb(II) ions and their hydroxides towards the fixation sites
[12]. Therefore, H+ ions react with anionic functional groups on the
surface of ASAC and results on the reduction of the number of binding
sites available for the adsorption of Pb(II). However, a favorable
Fig. 2. Effect of adsorbent concentration for the adsorption of lead ions onto activated
carbon from Apricote stone at 20 °C, initial concentration 50 mg/l and 100 mg/l, pH = 6.
Fig. 3. Effect of pH on removal of lead from aqueous solution by activated carbon from
Apricot stone at T = 20 °C.
increase in adsorption was observed above pH 5. The amount
adsorbed increased as pH increased from 1.5 to 6.0. This increase
may be due to the presence of negative charge on the surface of the
adsorbent that may be responsible for metal binding. However, as the
pH is lowered, the hydrogen ions compete with the metal ions for the
sorption sites in the sorbent; the overall surface charge on the adsor-
bent becomes positive, and hinds the binding of positively charged
metal ions [13]. At pH 8.0, a decrease in adsorption of Pb(II) was
observed due to the formation of soluble hydroxyl complexes. So all
the experiments were carried out at pH 6.0.
3.5. Kinetic models
In order to investigate the mechanism of adsorption, two kinetic
models were considered as follows. Lagergren proposed a pseudo-
first-order kinetic model. The integral form of the model is:
lnðqe−qt Þ = lnqe–Kpf t; ð3Þ
Where qt is the amount adsorbed (mg/g) at time t (min), qe is the
amount adsorbed (mg/g) at equilibrium, and Kpf is the equilibrium
rate constant of pseudo-first-order adsorption (l min− 1). The straight
line of the plot of ln(qe − qt) versus time suggest the applicability of
the Lagergren equation for the present system [14]. The values of Kpf
were determined from the slope of the plots and are given in Table 2
(Fig. 4). Recently, Ho and Mc Kay [15] have reported that most of the
sorption systems followed a second-order kinetic model which can be
expressed as:
t 1 1
= + t ð4Þ
qt Kps q2e qe
Where Kps is the pseudo-second-order rate constant of adsorption.
The plots of t/qt versus t (Fig. 4) were used to determine the rate
constants and correlation coefficients. Table 2 shows the pseudo-
second-order rate constants and correlation coefficients for removal
of lead from aqueous solutions.
The calculated correlation coefficients are less than 0.963 for the
first-order kinetic model, whereas the values of the correlation
coefficient are greater than 0.999 for the pseudo-second-order kinetic
model. Therefore, the adsorption kinetics could be well explained and
approximated by the pseudo-second-order kinetic model for the
activated carbon from Apricot stone. These results suggest that the
 L. Mouni et al. / Desalination 276 (2011) 148–153 151

Fig. 4. Kinetics of lead removal according to pseudo-second-order model at initial lead

Fig. 6. Freundlich plots for the adsorption of lead (II) ions onto activated carbon from
concentration of 10, 30, 50, 80 and 100 mg/l.; pH = 6; S/L = 1 g/1 l.
Apricot; T = 20 ± 2 °C, S/L = 1 g/l, pH = 6.0.

system. Two kinds of several isotherms equations were tested to fit

the experimental data [16]:

Langmuir isotherm : Ce = qe = 1 = qmax b + ðCe = qmax Þ ð5Þ

Freundlich isotherm : lnqe = ln K + ð1 = nÞlnCe ð6Þ

where qe is the amount adsorbed at equilibrium (mg/g) and Ce is the

Fig. 5. Langmuir plots for the adsorption of lead (II) ions onto activated carbon from
Apricot; T = 20 ± 2 °C, S/L = 1 g/l, pH = 6.0.
pseudo-second-order mechanism is predominant and that chemisorp-
tion might be the rate-limiting step that controls the adsorption process.
Kinetic parameters for the adsorption of Pb2+ ions onto activated
carbon by Apricot stone at various initial concentrations.
equilibrium concentration of metal ions in solution (mg/l). The other
parameters are different isotherm constants, which can be deter-
mined by linear regression of the experimental data. In the Langmuir
equation, qmax (mg/g) represents the maximal adsorption capacity
under the experimental conditions and b is a constant related to the
energy of adsorption. The maximal adsorption capacity calculated
from the Langmuir isotherm is equal to 21.38 mg/g at an initial pH of
6.0. Freundlich model gives the parameters, n, indicative of bond
energies between metal ion and the adsorbent and K, related to bond
strength. The linearized Langmuir and Freundlich isotherms of lead
are shown in Figs. 5 and 6. The estimated model parameters with
correlation coefficient (R2) for the different models are shown in
Table 3. From the values of R2 summarized in Table 3 it may be
concluded that both equations fit reasonably well the experimental
data. However the Langmuir equation provides a better fit than the
Freundlich one. The essential feature of the Langmuir isotherm can be
expressed in terms of dimensionless separation parameter RL, which
is indicative of the isotherm shape that predicts whether an
adsorption system is favourable or unfavourable. RL is defined as [17]:

RL = 1 = ð1 + bC0 Þ ð7Þ
3.6. Adsorption isotherms
Where b is the Langmuir constant. The parameter RL indicates the
In order to successfully represent the equilibrium adsorptive shape of the isotherm as follows:
behavior, it is important to have a satisfactory description of the
equation state between the two phases constituting the adsorption RL value type of isotherm
RL N 1 unfavorable
RL = 1 linear
Table 2
0 b RL b 1 favorable
Kinetic parameters for the adsorption of Pb2+ ions onto activated carbon by Apricot
stone at various initial concentrations. RL = 0 irreversible

First-order kinetic model Second-order kinetic model

Metals C0(mg/l) Kpf (l min−1) R2 Kps (g mg−1 min−1) R2 Table 3

Freundlich and Langmuir constants.
+2
Pb 10 0.073 0.623 0.246 0.999
30 0.046 0.532 0.052 0.999 Metals Freundlich constants Langmuir constants
50 0.038 0.874 0.025 0.999
K 1/n R2 qmax (mg g−1) b R2
80 0.032 0.912 0.028 0.999
100 0.026 0.745 0.588 0.999 Pb+ 2 21.123 0.4385 0.984 21.38 5.69 0.999
152 L. Mouni et al. / Desalination 276 (2011) 148–153

Table 4
Different values of RL at different concentrations of lead.

Metals Concentrations (mg/l) RL

Pb2+ 10 0.0172
30 0.0058
50 0.0035
80 0.0021
100 0.0017

According to McKay et al. [18], RL values between 0 and 1 indicate

favorable adsorption. The RL values were found to be between 0.0017
and 0.0172 (Table 4) for concentrations of 10, 30, 50, 80 and 100 mg/l
Pb(II).
The calculated maximum adsorption capacity for lead was
21.38 mg g− 1. Freundlich model is characterized by 1/n heterogeneity
factor; hence, it is applicable to sorption on heterogeneous surfaces,
i.e., surface with non-energetically equivalent sites. The values of 1/n
between 0.1 b 1/n b 1.0 represent good adsorption of metal onto the
sorbent [19]. Fig. 7. Effect of concentration of NaCl on removal of P(II) from aqueous solution.
Conditions: Pb(II) = 50 mg/l; S/L = 1 g/1 l; pH = 6; temperature = 20 °C.
Values of the adsorption capacity of other adsorbents from the
literature are given in Table 5 for comparison. The value for lead sorption
observed in this work is in good agreement with values found by other 4. Conclusion
researchers. Differences of metal uptake are due to the properties of
each adsorbent such as structure, functional groups and surface area. The present investigation shows that Apricot stone activated
carbon is an effective adsorbent for the removal and recovery of
lead from wastewater. The adsorption of lead on activated carbon is
3.7. Effect of sodium chloride concentration on Pb( II) removal found to be contact time, Pb concentration, pH and adsorbent dose
dependent. The pH influence on metal ion removal was high, and was
The presence of complexing ions is one of the most important more noticeable at pH values between 1.5 and 5 in particular. The
influencing factors in solution adsorption processes. The effect of kinetic study of the sorption of lead shows that the pseudo-second-
different concentrations of NaCl on lead removal was studied. The effect order model provides better correlation of the sorption data than the
of complex formation on sorption of a metal ion depends on the relative pseudo-first-order model. This suggests that the rate-limiting step
stability of the cation–ligand in solution and the cationic surface and on may be chemical sorption rather than diffusion.
whether the surface has an affinity for the complexed form [29]. The Langmuir and Freundlich isotherm models were used to
Increasing chloride ion concentration considerably decreases the represent the equilibrium data. Results obtained indicate that the
adsorption of lead for the carbon studied (Fig. 7). In the absence of adsorption equilibrium data fitted well by the Langmuir isotherm
NaCl, maximum removal has been observed due to formation of Pb model in the studied concentration range. Maximum adsorption
(OH)2 which is higher at pH above 3.0 and it seems to be better adsorbed capacity calculated from the Langmuir isotherm is equal to 21.38 mg/
than PbCl2 [30]. At higher Cl concentrations the low adsorption is likely g at an initial pH of 6.0. In the presence of chloride ions low Pb (II)
to be due to the formation of more stable Pb–Cl complexes which are adsorption was observed.
poorly adsorbed [30]. The observed variations in Pb sorption with ionic These results show that adsorbents which have a very low
strength may be explained by the formation of outer-sphere complexes economical value may be used effectively for removal of Pb(II) ions
since Na+ in the background electrolyte. This last could compete with from aqueous systems for environmental protection purpose.
the metal ions adsorbed on the outer-sphere sorption sites and reduce
the adsorption capacity. Whereas Na+ would not have competed for the
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