Journal of Hazardous Materials 142 (2007) 340–347

Removal of lead from aqueous solution using Syzygium cumini L.:

Equilibrium and kinetic studies
P. King ∗ , N. Rakesh, S. Beenalahari, Y. Prasanna Kumar, V.S.R.K. Prasad
Environmental Pollution Control Engineering Laboratory, Department of Chemical Engineering, A.U. College of Engineering,
Andhra University, Visakhapatnam 530 003, India
Received 23 May 2006; received in revised form 11 July 2006; accepted 11 August 2006
Available online 18 August 2006

Abstract
The biosorption of lead ions from aqueous solution by Syzygium cumini L. was studied in a batch adsorption system as a function of pH, contact
time, lead ion concentration, adsorbent concentration and adsorbent size. The biosorption capacities and rates of lead ions onto S. cumini L. were
evaluated. The Langmuir, Freundlich, Redlich–Peterson and Temkin adsorption models were applied to describe the isotherms and isotherm con-
stants. Biosorption isothermal data could be well interpreted by the Langmuir model followed by Temkin model with maximum adsorption capacity
of 32.47 mg/g of lead ion on S. cumini L. leaves biomass. The kinetic experimental data were properly correlated with the second-order kinetic model.
© 2006 Elsevier B.V. All rights reserved.

Keywords: Syzygium cumini L.; Adsorption; Adsorption isotherm; Kinetic studies

1. Introduction techniques described, adsorption is generally preferred for the

removal of heavy metal ions due to its high efficiency, easy han-
The removal of toxic metal ions and recovery of valuable ions dling, availability of different adsorbents and cost effectiveness
from mine wastewaters, soils and waters have been important in [8].
economic and environmental problems [1–4]. Heavy metals and Earlier studies demonstrated that the living systems had been
other metal ions exist as contaminants in aqueous waste streams often unreliable because there were many problems to maintain
of many industries, such as tanneries and mining. Some metals active microbial populations under highly variable conditions
associated with these activities are Pb, Hg, Cr and Cd. Some of of wastewaters [9]. Therefore, some types of biomass served as
these metals are accumulated in living organisms and produce biosorbents to remove heavy metals [9–11]. Biosorption, a term
diseases and disorders. that describes the removal of heavy metals by the passive binding
Heavy metals such as lead, mercury, arsenic, copper, zinc to non-living biomass from an aqueous solution [12], is consid-
and cadmium are highly toxic when adsorbed into the body [5]. ered as an alternative to conventional methods of metal recovery
They can cause accumulative poisoning, cancer, brain damage, from solutions [13]. Although freely suspended biomass may
etc. Lead is a general metabolic poison and enzyme inhibitor. It have better contact with adsorbates during biosorption process,
can cause mental retardation and semi permanent brain damage the suspended biomass is normally not the practical form for the
in young children [6]. Lead has the ability to replace calcium direct use in the removal of heavy metals. Since cell immobiliza-
in the bone to form sites for long-term release. Toxic metals tion can enhance its stability, mechanical strength, reusability
are released into the environment in a number of ways. Coal and the ease of treatment, the technique has been well used to
combustion, sewage wastewaters, automobile emissions, battery remove toxic heavy metals [9,14–16]. Usually a fixed bed reac-
industry, mining activities, and the utilization of fossil fuels are tor, in which a certain type of immobilized biomass is packed, is
just a few examples [7]. Among the various water-treatment designed for effective and continuous removal of heavy metals
[9,16–19].
The effectiveness of biosorption for the removal of heavy
∗ Corresponding author. Tel.: +91 891 2844894. metals has been shown in a number of studies. However, only
E-mail address: p [email protected] (P. King). when the cost of the biosorption process can complete with the

0304-3894/$ – see front matter © 2006 Elsevier B.V. All rights reserved.
doi:10.1016/j.jhazmat.2006.08.027
 P. King et al. / Journal of Hazardous Materials 142 (2007) 340–347 341

existing technologies will it be accepted commercially. Kuyucak V the solution volume (mL); M is the mass of biosorbent (g). The
indicated that the cost of biomass production played an impor- pH of the solution was adjusted by using 0.1N HCl and 0.1N
tant role in determining the overall cost of a biosorption process NaOH.
[20]. Therefore, low cost biomass becomes a crucial factor when The Langmuir [21] sorption model was chosen for the estima-
considering practical application of biosorption. tion of maximum lead sorption by the biosorbent. The Langmuir
The present work investigates the potential use of untreated isotherm can be expressed as
Syzygium cumini L. biomass as metal sorbent for removal of lead
Qmax bCeq
from aqueous solution. S. cumini L. was chosen as a biosorbent q= (2)
because of the relative lack of information about its sorption 1 + bCeq
ability. Environmental parameters affecting the biosorption pro- where Qmax indicates the monolayer adsorption capacity of
cess such as pH, contact time, metal ion concentration, adsorbent adsorbent (mg/g) and the Langmuir constant b (L/mg) is related
concentration and adsorbent size were evaluated. The equilib- to the energy of adsorption. For fitting the experimental data, the
rium adsorption data were evaluated by Langmuir, Freundlich, Langmuir model was linearized as
Redlich–Peterson and Temkin isotherm models.
1 1 1
= + (3)
2. Materials and methods q Qmax bQmax Ceq

2.1. Preparation of biosorbent The Freundlich [22] model is represented by the equation:

q = KCeq
1/n
(4)
The green S. cumini L. leaves were collected from Andhra
University College of Engineering campus of Visakhapatnam, where K (mg/g) is the Freundlich constant related to adsorption
Andhra Pradesh, India. Leaves were washed with deionized capacity of adsorbent and 1/n is the Freundlich exponent related
water several times to remove dirt particles. The dried leaves to adsorption intensity (dimensionless). For fitting the experi-
of 75–212 ␮m particle size were used as biosorbent without any mental data, the Freundlich model was linearized as follows:
pretreatment for lead adsorption.
1
ln q = ln K + ln Ceq (5)
n
2.2. Chemical
The Redlich–Peterson [23] model is represented by the equation:
Analytical grades of Pb(NO3 )2 , HCl and NaOH were pur-
ACeq
chased from Merck, India. Lead ions were prepared by dissolv- q= g (6)
ing its corresponding nitrate salt in distilled water. The pH of 1 + BCeq
solutions was adjusted with 0.1N HCl and NaOH. where A (L/g) and B (L/mg) are the Redlich–Peterson isotherm
All the experiments were repeated five times and the aver- constants and g is the Redlich Peterson isotherm exponent,
age values have been reported. Also, blank experiments were which lies between 0 and 1. The linearized form of equation
conducted to ensure that no adsorption was taking place on the is given by
walls of the apparatus used.  
ACeq
ln − 1 = g ln(Ceq ) + ln(B) (7)
2.3. Biosorption experiments q
Redlich–Peterson isotherm equation contains three unknown
Biosorption experiments were performed at room temper-
parameters A, B, and g. Therefore a minimization procedure is
ature (30 ± 1 ◦ C) in a rotary shaker at 180 rpm using 250 mL
adopted to maximize the coefficient of determination, between
Erlenmeyer flasks containing 30 mL of different lead concentra-
the theoretical data for q predicted from the linearized form of
tions. After 1 h of contact (according to the preliminary sorption
Redlich–Peterson isotherm equation and the experimental data.
dynamics tests), with 0.1 g S. cumini L. leaves biomass, equi-
The Temkin [24] isotherm has generally been applied in the
librium was reached and the reaction mixture was centrifuged
following form:
for 5 min. The metal content in the supernatant was determined
using Atomic Absorption Spectrophotometer (GBC Avanta Ver RT
1.32, Australia) after filtering the adsorbent with 0.45 ␮m filter q= ln(AT Ceq ) (8)
bT
paper. The amount of metal adsorbed by S. cumini L. leaves was
calculated from the differences between metal quantity added where AT (L/mg) and bT are Temkin isotherm constants.
to the biomass and metal content of the supernatant using the
following equation: 2.4. Biosorption kinetics
V
q = (C0 − Cf ) (1) The kinetics studies were carried out by conducting batch
M biosorption experiments with different initial lead concentra-
where q is the metal uptake (mg/g); C0 and Cf the initial and tions. Samples were taken at different time periods and analyzed
final metal concentrations in the solution (mg/L), respectively; for their lead concentration.
342 P. King et al. / Journal of Hazardous Materials 142 (2007) 340–347

3. Results and discussion

3.1. The effect of contact time

The data obtained from the biosorption of lead ions on the S.

cumini L. showed that a contact time of 10 min was sufficient
to achieve equilibrium and the adsorption did not change sig-
nificantly with further increase in contact time. Therefore, the
uptake and unadsorbed lead concentrations at the end of 10 min
are given as the equilibrium values (qeq , mg/g; Ceq , mg/L),
respectively (Fig. 1).

3.2. Effect of pH

It is well known that the pH of the medium affects the sol- Fig. 2. Effect of pH on lead adsorption by S. cumini L. for 20 mg/L of metal and
ubility of metal ions and the concentration of the counter ions 0.1 g/30 mL of adsorbent concentration.
on the functional groups of the biomass cell walls, so pH is an
important parameter on biosorption of metal ions from aqueous
solutions [25–29]. 3.3. Effect of metal ion concentration
S. cumini L. presents a high content of ionizable groups (car-
boxyl groups from mannuronic and gluronic acids) on the cell Fig. 3 shows the effect of metal ion concentration on the
wall polysaccharides, which makes it, very liable to the influ- adsorption of lead by S. cumini L. The data shows that the
ence of the pH. As shown in Fig. 2, the uptake of lead increased metal uptake increases and the percentage adsorption of lead
with the increase in pH from 2.0 to 6.0. Similar results were also decreases with increase in metal ion concentration. This increase
reported in literature for different biomass systems [30–33]. At (5.23–21.77 mg/g) is a result of increase in the driving forces,
pH values lower than 2.0 lead removal was inhibited, possibly as i.e. concentration gradient. However, the percentage adsorp-
a result of the competition between hydrogen and lead ions on tion of lead ions on S. cumini L. was decreased from 87.18
the sorption sites, with an apparent preponderance of hydrogen to 72.57%. Though an increase in metal uptake was observed,
ions, which restricts the approach of metal cations as in conse- the decrease in percentage adsorption may be attributed to lack
quence of the repulsive force. As the pH increased, the ligands of sufficient surface area to accommodate much more metal
such as carboxylate groups in S. cumini L. would be exposed, available in the solution. The percentage adsorption at higher
increasing the negative charge density on the biomass surface, concentration levels shows a decreasing trend whereas the equi-
increasing the attraction of metallic ions with positive charge librium uptake of lead displays an opposite trend. At lower
and allowing the biosorption onto the cell surface. concentrations, all lead ions present in solution could interact
In this study, these lead cations at around 6 would be expected with the binding sites and thus the percentage adsorption was
to interact more strongly with the negatively charged binding higher than those at higher lead ion concentrations. At higher
sites in the adsorbent. As a result, the optimum pH for lead concentrations, lower adsorption yield is due to the saturation
adsorption was found as 6 and the other adsorption experiments of adsorption sites. As a result, the purification yield can be
were performed at this pH value. increased by diluting the wastewaters containing high metal ion
concentrations.

Fig. 1. Effect of contact time on lead uptake by Syzygium cumini L. for 20 mg/L Fig. 3. Effect of metal concentration on the adsorption of lead by S. cumini L.
of metal and 0.1 g/30 mL of adsorbent concentrations. at 0.1 g/30 mL of adsorbent concentration.
 P. King et al. / Journal of Hazardous Materials 142 (2007) 340–347 343

dosage from 0.1 to 0.5 g at an initial concentration of 20 mg/L.

The increase in the adsorption of the amount of solute is obvious
due to increasing biomass surface area. Similar trend was also
observed for lead removal using Azadirachta indica as adsorbent
[34].

4. Biosorption equilibrium

The equilibrium biosorption of lead on the S. cumini L.

as a function of the initial concentration of lead is shown in
Figs. 6–10. There was a gradual increase of adsorption for
lead ions until equilibrium was attained. The Langmuir, Fre-
undlich models are often used to describe equilibrium sorption
isotherms and Redlich–Peterson and Temkin models are also
applied to describe equilibrium sorption isotherms. The calcu-
Fig. 4. Effect of S. cumini L. particle size on adsorption of lead for 20 mg/L of
metal and 0.1 g/30 mL of adsorbent concentration.
lated results of the Langmuir, Freundlich, Redlich–Peterson and
Temkin isotherm constants are given in Table 1.
It is found that the adsorption of lead on the S. cumini L.
3.4. Effect of adsorbent size was correlated well with the Langmuir equation and Temkin
equation as compared to Freundlich and Redlich–Peterson equa-
The effect of different adsorbent particle sizes on percentage
removal of lead is investigated and showed in Fig. 4. It reveals
that the adsorption of lead on S. cumini L. decreased from 87.18
to 76.42% with the increased particle size from 75 to 212 ␮m at
an initial concentration of 20 mg/L. The smallest size obtained
was 75 ␮m due to the limitation of available grinder configura-
tion. It is well known that decreasing the average particle size of
the adsorbent increases the surface area, which in turn increases
the adsorption capacity.

3.5. Effect of adsorbent dosage

Fig. 5 shows the effect of adsorbent dosage on the % removed

at equilibrium conditions. It was observed that the amount
of lead adsorbed varied with varying adsorbent dosage. The
amount of lead adsorbed increases with an increase in adsor-
bent dosage from 0.1 to 0.5 g. The percentage of lead removal
Fig. 6. Langmuir adsorption isotherm for lead at 0.1 g/30 mL of adsorbent con-
was increased from 87.18 to 98.03% for an increase in biomass centration.

Fig. 5. Effect of S. cumini L. dosage on adsorption of lead for 20 mg/L of metal Fig. 7. Freundlich adsorption isotherm for lead at 0.1 g/30 mL of adsorbent
concentration. concentration.
344 P. King et al. / Journal of Hazardous Materials 142 (2007) 340–347

Table 1
Langmuir, Freundlich, Redlich–Peterson and Temkin isotherm constants and
correlation coefficients
Langmuir
Q (mg/g) 32.47
b (L/mg) 0.0746
R2 0.9997
Freundlich
Kf (mg/g) 3.1761
n 0.606
R2 0.9834
Redlich–Peterson
A (L/mg) 1.08
B (L/mg) 13.1129
g −1.2261
R2 0.3259
Fig. 8. Redlich–Peterson adsorption isotherm for lead at 0.1 g/30 mL of adsor- Temkin
bent concentration. AT (L/mg) 0.7584
bT 356.72
R2 0.9938

5. Kinetics of adsorption

The prediction of adsorption rate gives important informa-

tion for designing batch adsorption systems. Information on the
kinetics of solute uptake is required for selecting optimum oper-
ating conditions for full-scale batch process. Fig. 1 shows the
plot between amount adsorbed, q (mg/g) versus time, t (min)
for different initial solute concentrations. From the figure it
was observed that q value increased with increase in initial
lead concentration. The adsorption rate within the first 5 min
was observed to be very high and thereafter the reaction pro-
ceeds at a slower rate till equilibrium and finally a steady state
was obtained after equilibrium. The kinetics of the adsorption
Fig. 9. Temkin adsorption isotherm for lead at 0.1 g/30 mL of adsorbent con- data was analysed using two kinetic models, pseudo-first-order
centration.
and pseudo-second-order kinetic model. These models corre-
late solute uptake, which are important in predicting the reactor
tions under the concentration range studied. Examination of volume. These models are explained as follows:
the Freundlich and Redlich–Peterson data shows that these two
isotherms are not modeled as well across the concentration range 5.1. The pseudo-first-order equation
studied.
The pseudo-first-order equation of Lagergren and Kungliga
[35] is generally expressed as follows:
dqt
= k1 (q − qt ) (9)
dt
where q and qt are the sorption capacities at equilibrium and
at time t, respectively (mg/g) and k1 is the rate constant of
pseudo-first-order sorption (1/min). After integration and apply-
ing boundary conditions, qt = 0–qt at t = 0–t; the integrated form
of Eq. (9) becomes
k1
log(q − qt ) = log(q) − t (10)
2.303
The equation applicable to experimental results generally differs
from a true first-order equation in two ways [36]:

• The parameter k1 (q − qt ) does not represent the number of

Fig. 10. Equilibrium curves for lead onto S. cumini L. available sites;
 P. King et al. / Journal of Hazardous Materials 142 (2007) 340–347 345

this model can be applied to predict the adsorption kinetic

model.

5.2. The pseudo-second-order equation

If the rate of sorption is a second-order mechanism, the

pseudo-second-order chemisorption kinetic rate equation is
expressed as
dqt
= k(q − qt )2 (11)
dt
where q and qt are the sorption capacity at equilibrium and at
time t, respectively (mg/g) and k is the rate constant of pseudo-
second-order sorption (g/mg min). For the boundary conditions
qt = 0–qt at t = 0–t; the integrated form of Eq. (11) becomes:
Fig. 11. Pseudo-first-order adsorption of lead by S. cumini L. for 20 mg/L of
metal and 0.1 g/30 mL of adsorbent concentration. 1 1
= + kt (12)
q − qt q
• The parameter log(q) is an adjustable parameter which is often
not found equal to the intercept of a plot of log(q − qt ) against which is the integrated rate law for a pseudo-second-order reac-
t, whereas in a true first-order sorption reaction log(q) should tion. Eq. (12) can be rearranged to obtain:
be equal to the intercept of a plot of log(q − qt ) against t. t
qt = (13)
1/kq2 + (t/q)
In order to fit Eq. (10) to experimental data, the equilibrium
sorption capacity, q, must be known. In many cases q is unknown which has linear form:
and as chemisorption tends to become unmeasurably slow, the t 1 1
= 2+ t (14)
amount sorbed is still significantly smaller than the equilibrium qt kq q
amount [37]. In most cases in the literature, the pseudo-first-
where t is the contact time (min), q (mg/g) and qt (mg/g) are the
order equation of Lagergren does not fit well for the whole
amount of the solute adsorbed at equilibrium and at any time,
range of contact time and is generally applicable over the initial
t. Eq. (14) does not have the problem of assigning as effective
20–30 min of the sorption process. Furthermore, one has to find
q. If pseudo-second-order kinetics are applicable, the plot of
some means of extrapolating the experimental data to t = ∞, on
t/qt against t of Eq. (14) should give a linear relationship, from
treat (q) as an adjustable parameter to be determined by trial and
which q and k can be determined from the slope and intercept
error. For this reason, it is therefore necessary to use trial and
of the plot (Fig. 12) and there is no need to know any parameter
error to obtain the equilibrium sorption capacity (q), in order to
beforehand.
analyse the pseudo-first-order model kinetics. In over 50% of
The pseudo-second-order rate constant k2 , the calculated q
literature references, based on analyzing sorption kinetics, the
value and the corresponding linear regression correlation coeffi-
authors did not measure an equilibrium isotherm.
cient values R22 are given in Table 2. At all initial copper concen-
The pseudo-first-order rate constant k1 can be obtained from
trations, the linear regression correlation coefficient R22 values
the slope of plot between log(q − qt ) versus time, t. Fig. 11 shows
the Lagergren pseudo-first-order kinetic plot for the adsorption
of lead onto S. cumini L. The pseudo-first-order rate constant k1
values were calculated from the slope of Fig. 11. The calculated
k1 values and their corresponding linear regression correlation
coefficient values are shown in Table 2. The linear regression
correlation coefficient R21 found as 0.9633, which shows that

Table 2
Kinetic constants for lead onto Syzygium cumini L.
Initial concentration (mg/L) 20
Pseudo-first-order
Rate constant, k1 0.3901
Amount of lead adsorbed on adsorbent, qe (mg/g) 2.8661
Correlation coefficient, R21 0.9633
Pseudo-second-order
Rate constant, k2 0.2498
Amount of lead adsorbed on adsorbent, qe (mg/g) 5.3242
Correlation coefficient, R22 0.9995 Fig. 12. Pseudo-second-order adsorption of lead by S. cumini L. for 20 mg/L of
metal and 0.1 g/30 mL of adsorbent concentration.
346 P. King et al. / Journal of Hazardous Materials 142 (2007) 340–347

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