Desalination 256 (2010) 129–135

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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 e v i e r. c o m / l o c a t e / d e s a l

Adsorption of 2,4-dichlorophenoxyacetic acid and carbofuran pesticides onto

granular activated carbon
J.M. Salman, B.H. Hameed ⁎
School of Chemical Engineering, Engineering Campus, Universiti Sains Malaysia, 14300 Nibong Tebal, Penang, Malaysia

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

Article history: Adsorption equilibrium and kinetics of 2,4-dichlorophenoxyacetic acid (2,4-D) and carbofuran using
Received 22 August 2009 commercial granular activated carbon, Filtersorb 300 (GAC F300) were studied in a batch system with
Received in revised form 2 February 2010 respect to initial concentration of 2,4-D and carbofuran. The Langmuir and the Freundlich isotherm models
Accepted 2 February 2010
were applied to the equilibrium data of 2,4-D and carbofuran adsorption. Observed results showed that the
Available online 5 March 2010
equilibrium data fitted well to the Langmuir equilibrium model in the studied concentration range of 2,4-D
Keywords:
and carbofuran. The monolayer adsorption capacities of GAC F300 were 181.82 and 96.15 mg/g for 2,4-D and
2,4-Dichlorophenoxyacetic acid carbofuran, respectively. Two simplified models, pseudo-first order and pseudo-second order kinetic, were
Carbofuran used to test the adsorption kinetics of 2, 4-D and carbofuran on GAC F300. The data was best fitted to the
Granular activated carbon pseudo-second-order kinetic model.
Adsorption © 2010 Elsevier B.V. All rights reserved.
Equilibrium
Kinetics

1. Introduction
Water pollution is any human-caused contamination of water that
reduces its usefulness to humans and other organisms in nature.
Pollutants such as pesticides, fertilizers, and hazardous chemicals
often find their way into water channels. When water supply is
contaminated, it posed a great threat to humans, animals, and plants’
health unless it goes through a costly purification procedure. Water
pollution can be considered in a number of ways but in simple terms it
is an addition of an array of unwanted contaminant elements to it [1].
Pollution of surface and ground waters causes risk to human
health because of the potential health hazards of their contents of
inorganic and organic compounds. Pesticides are group of hazardous
compounds that may pollute water due to their extensive application
in agriculture [2–4].
2,4-Dichlorophenoxyacetic acid (2,4-D) belongs to a group of
chemicals known as phenoxy compounds, which are potentially toxic
to humans [5]. The herbicide, 2,4-D is most extensively applied to
control broad-leaved weeds and pests in fields worldwide. It is
commonly preferred because of its low cost and good selectivity [6].
2,4-D is a widely used pesticide found in surface and ground water all
over the world [7].
Carbofuran is a carbamate insecticide and nematocide used for the
control of a variety of solid welling and foliar-feeding pests on many
fruit and vegetable crops [8]. The World Health Organization (WHO)
⁎ Corresponding author. Fax: +60 45941013.
E-mail address: chbassim@eng.usm.my (B.H. Hameed).
specified a standard limit of 20 and 3 μg/L for 2,4-D and carbofuran in
portable water respectively [3]. Carbofuran (2,3-dihydro-2,2-
dimethylbenzofuran- 7-yl-N-methyl carbamate) is a broad spectrum
systemic acaricide, insecticide and nematocide included in the general
group of the carbamate derivative pesticides [9]. It is widely used for
the control of soil dwelling and foliar-feeding insects including
wireworms, white grubs, weevils, stem borers, aphids and several
other insects [10]. In Malaysia, it is used in rice fields for control of
rodents and in oil palm plantations for control of rhinoceros beetles.
Carbofuran is known to be more persistent than other carbamate or
organophosphate insecticides [11]. Even though carbofuran is widely
used in Malaysia, to the best of our knowledge, no intensive research
has been carried out although there are some publications on its
behavior in tropical and temperate soils [12,13].
Adsorption is one of the most frequently applied methods because
of its efficiency, capacity and applicability on a large scale [4,14].
Activated carbon is the most effective and widely used adsorbent for
removal of organics from aqueous solutions owing to its highly
developed surface properties such as surface area, porosity and
surface chemistry [15]. A typical activated carbon particle, whether in
a powder or granular form, has a porous structure consisting of a
network of interconnected macrospores, mesopores, and micropores
that provide a good capacity for the adsorption of organic molecules
due to its high surface area [16]. Commercial granular activated
carbon, Filtersorb 300 (GAC F300) is particularly a good adsorbent
medium due to its high surface area to volume ratio. One gram of a
typical commercial activated carbon will have a surface area
equivalent to 1000 m2. This high surface area permits the accumu-
lation of a large number of contaminant molecules [17].

0011-9164/$ – see front matter © 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2010.02.002
130 J.M. Salman, B.H. Hameed / Desalination 256 (2010) 129–135

The purpose of this work was to evaluate the adsorption potential
of activated carbon, Filtersorb (GAC F300) for 2,4-D and carbofuran.
The equilibrium and kinetic data of the adsorption process were
studied to understand the adsorption mechanism of these two
pesticides molecules onto the surface of the GAC F300.
where Co and Ce (mg/L) are the liquid-phase concentrations of
pesticide at initial and at equilibrium, respectively. V (L) is the volume
of the solution and W (g) is the mass of dry adsorbent used.
2.5. Effect of pesticides solution pH

2. Materials and methods The effect of solutions pH on the pesticides removal was examined
by varying the initial pH of the solutions from pH 2 to 12. The pH was
2.1. Adsorbate adjusted using 0.1 M HCl and/or 0.1 M sodium hydroxide (NaOH) and
was measured using pH meter (Model Ecoscan, EUTECH Instruments,
Technical grade 2,4-D and carbofuran of 97.9 and 99.9% purity, Singapore). The pesticides initial concentration was fixed at 100 mg/L,
respectively were supplied by Sigma-Aldrich (M) Sdn Bhd, Malaysia. with activated carbon dosage of 0.20 g/200 mL and temperature of
Distilled water was used to prepare all solutions. Table 1 listed the 30 °C.
chemical structures, molecular weights and solubilities of pesticides.
2.6. Adsorption isotherm
2.2. Adsorbent
Two isotherm models (Langmuir and Freundlich) were used to
Commercial activated carbon, Filtersorb 300 (F300) was supplied by test the fitting of the experimental data. The linear form of Langmuir
Calgon Carbon Asia, Singapore. The activated carbon was manufactured isotherm [18] equation is given as:
from selected grades of bituminous coal, and it was used in this work
without further treatment. Ce 1 C
= + e ð2Þ
qe qm b qm
2.3. Characterization of activated carbon
where Ce (mg/L) is the equilibrium concentration of the adsorbate, qe
Characterization of the activated carbon is important to determine (mg/g) is the amount of adsorbate adsorbed per unit mass of
the physical and chemical properties. The surface area and pore adsorbent, qm (mg/g) is a monolayer adsorption capacity, and b (L/
characteristics which include the pore volume and pore size mg) is the equilibrium adsorption constant.
distribution were analyzed using Micromeritics (Model ASAP 2020, The linear form of Freundlich [19] isotherm is given by the following
USA surface area and porosity analyzer) through nitrogen adsorption equation:
isotherm at 77 K. In order to determine morphology of GAC F300  
surface, the sample was examined using a Scanning Electron 1
log qe = ln KF + log Ce ð3Þ
Microscope. The analysis was conducted using a Scanning Electron n
Microscope model Leo Supra 35 VP Field Emission SEM.
where Ce (mg/L) is the equilibrium concentration of the adsorbate, qe
2.4. Adsorption studies (mg/g) is the amount of adsorbate adsorbed per unit mass of
adsorbent, KF and n are Freundlich constants.
The adsorption experiments of pesticides onto GAC F300 were
determined in a set of 250 mL Erlenmeyer flasks. 200 mL of the adsorbate 2.7. Adsorption kinetics
with various initial concentrations was in the range of 50–300 mg/L and
50–225 mg/L for 2,4-D and carbofuran, respectively. Fixed dosage of For kinetic studies, 0.20 g of GAC F300 was contacted with 100 mL of
0.20 g of the GAC F300 was added to each flask and kept in an isothermal 2,4-D and carbofuran solutions of concentrations 50–300 mg/L and 50–
water-bath shaker with an agitation speed of 120 rpm at 30 °C. The 225 mg/L and pH 3.5 and 6.35, respectively. The experiments were
experiments were carried out for 8 h and 26 h for 2,4-D and carbofuran, conducted at 30 °C and agitation speed of 120 rpm.
respectively. The concentrations of 2,4-D and carbofuran in the solutions The rate constants of the adsorption were determined from the
before and after adsorption were determined using a double beam UV–Vis pseudo-first-order and pseudo-second-order equations. For the
spectrophotometer (Shimadzu UV-1700, Japan) at its maximum wave- pseudo-first-order, the Lagergren and Svenska [20] expression given
length of 284 nm and 276 nm, respectively. The pesticide uptake at below was used:
equilibrium, qe (mg/g), was calculated by Eq. (1).
k1 t
qe = ðCo −Ce ÞV = W ð1Þ log ðqe −qt Þ = log qe − ð4Þ
2:303

Table 1
Chemical structures, molecular weights and solubility of pesticides.

Pesticide Chemical structure Molecular weight (mg/mol) Solubility in water (g/100 g water) at 20 °C

2,4-Dichlorophenoxyacitic acid 221.04 0.09

Carbofuran 221.3 0.07

 J.M. Salman, B.H. Hameed / Desalination 256 (2010) 129–135 131

Intraparticle diffusion model based on the theory proposed by

Weber and Morris [22] was tested to identify the diffusion
mechanism. This is an empirically found functional relationship
which is common to most adsorption processes, where uptake varies
almost proportionally with t1/2 rather than with the contact time t.
According to this theory,

1=2
qt = kp t +C ð6Þ

where qt (mg/g) is the amount of pesticides adsorbed at time t (h). kp

(mg/g h1/2) is the intraparticle diffusion rate constant.

3. Results and discussion

3.1. Characterization of GAC F300

Fig. 1 shows the GAC F300 SEM image of 1000× magnification. It

Fig. 1. SEM image of GAC F300 (magnification = 1000×).
where qe and qt (mg/g) are the amounts of pesticide adsorbed at
equilibrium and at time t (h), respectively and k1 (1/h) is the rate
constant adsorption.
While in the case of pseudo-second-order, the expression of Ho
and Mckay [21] was used as stated below:
can be seen that the surface is coarse rough and porous indicating that
there is a good possibility for 2,4-D and carbofuran to be trapped and
adsorbed onto the surface of the pores. The Brunauer–Emmett–Teller
(BET) surface area and the total pore volume of pores are 731.48 m2/g
and 0.454 cm3/g, respectively.
3.2. Effect of initial concentration and contact time on pesticides
adsorption

Fixed dosage of 0.20 g GAC F300 and varied initial concentrations

t 1 1
= + t ð5Þ of 50, 100, 150, 200, 250 and 300 mg/L for 2,4-D and 50, 100, 150, 200
qt k2 q2e qe
and 225 mg/L, for carbofuran were used in this investigation. Fig. 2(a)
and (b) shows the results of the effect of initial concentrations of both
where k2 (g/mg h) is the rate constant of pseudo-second-order pesticides and contacting time on their adsorption by GAC F300. The
adsorption. results revealed that pesticide solutions with low concentrations of

Fig. 2. Effect of contact time on (a) 2,4-D and (b) carbofuran concentration (T = 30 °C, Agitation speed = 120 rpm).
132 J.M. Salman, B.H. Hameed / Desalination 256 (2010) 129–135

Fig. 3. Effect of pH on the adsorption rate of 2,4-D and carbofuran onto GAC F300.

50–150 mg/L and 50–100 mg/L attained equilibrium faster than the
high concentrations of 200–300 mg/L and 150–225 mg/L for 2,4-D
and carbofuran, respectively. At initial concntrations of 50–150 mg/L
for 2,4-D, the equilibrium was attained in approximately 3.5 h, while
at higher initial concentrations of 200–300 mg/L, it took 6.5 h to
establish equilibrium for the adsorption of 2,4-D onto the GAC F300.
On the other hand, for the adsorption of carbofuran onto the GAC F300
at low initial concentrations of 50–150 mg/L, the equilibrium time
was 10 h. When the initial concentration of carbofuran was increased
to 200–225 mg/L, it took 22 h to reach equilibrium. However, to
ensure that equilibrium is fully established, the experimental data
were measured at 8 h and 26 h for 2,4-D and carbofuran, respectively.
It was observed that the concentrations and contact time played an
important role in the adsorption of 2,4-D and carbofuran onto GAC
F300. This behavior is similar to the work of Gupta et al. [3] for the
adsorption of 2,4-D on carbon slurry.
3.3. Effect of solution pH on pesticide adsorption
The effect of solution pH was studied in the range of 2 to 12. The
experiment was conducted by adding 0.20 g GAC F300 to 200 mL each
of 2,4-D and carbofuran solutions having an initial concentration of
100 mg/L. As shown in Fig. 3, the amount of pesticides adsorbed at
equilibrium, qe decreases from 57.25 to 38 mg/g and from 38 to
28 mg/g for 2,4-D and carbofuran, respectively with increase in pH
from 2 to 12. The maximum qe was observed at pH 2. It was suggested
that the increase in adsorption depended on the properties of the
adsorbent surface and the pesticides structure, the surface functional
groups of adsorbate make the process complex by the nature of charge
characteristics of the adsorbent surface. In the acidic medium, the
pesticides uptake increase faster than the basic medium. Gupta et al.
[3] showed that an increase in pH from 2.0 to 7.5 for 2,4-D and from
2.0 to 8.0 for carbofuran resulted in a small decrease (respectively 7
and 5%) in adsorption. With further increase in pH value up to 12.0, it
was observed that the percentage adsorption becomes poor. The
decrease in adsorption per unit pH over the range of higher pH (from
7.0 to 12.0) suggests that the adsorption was dominated by the
interaction between pesticide and adsorbent surface and this also
suggested a weaker interaction of carbon surface with deprotonated
(anionic) 2,4-D than with its neutral molecular form.
3.4. Equilibrium modeling
The Langmuir and Freundlich isotherms were used to describe the
experimental results. From the linear plot of specific adsorption (Ce/
qe) against the equilibrium concentration (Ce) (figures not shown),
the Langmuir constants qm and b were determined from the slope and
intercept and are listed in Table 2. The essential characteristics of the
Langmuir isotherm can be expressed in terms of a dimensionless
constant separation factor RL:
RL = 1 = ð1 + bCo Þ ð7Þ
where Co (mg/L) is the highest initial concentration of adsorbate, and
b (L/mg) is Langmuir constant. The value of RL indicates the shape of
the isotherm to be either unfavorable (RL N 1), linear (RL = 1),
favorable (0 b RL b 1), or irreversible (RL = 0). The RL values between
0 and 1 indicate favorable adsorption. The values of RL in the present
investigation were found to be 0.9917 and 0.9852 for 2,4-D and
carbofuran, respectively.
The values of KF and n for Frendiulch isotherm were calculated
from the intercept and slope of log qe vs. Ce (figures not shown) and
are given in Table 2. The correlation coefficient (R2), which describes
the fitness of a set of data revealed that Langmuir isotherm best
describes the adsorption of the considered pesticides than the
Frendiulch isotherm with R2 of 0.992 and 0.985 for 2.4-D and
carbofuran, respectively. The monolayer adsorption capacities of
GAC F300 for 2,4-D and carbofuran were 181.82 and 96.15 mg/g,
respectively. The fact that the Langmuir isotherm fits the experimen-
tal data very well may be due to homogeneous distribution of active
sites onto GAC F300 surface, since the Langmuir equation assumes
that the surface is homogenous. Similar results were reported for the
adsorption of 2,4-D and carbofuran onto fertilizer and steel industry
Table 3
Comparison of 2,4-D and carbofuranpesticides adsorption of this work and previous
studies.

Table 2 Pesticide Adsorbent Operating conditions Adsorption Reference

Isotherm parameters for removal of 2,4-D and carbofuran by GAC F300. capacity (mg/g)

2,4-D GAC T = 30 °C, pH = 3–3.8 181.82 This study

2,4-D Carbofuran
conc. = 50–300 mg/L
Langmuir isotherm Carbofuran GAC T = 30 °C, pH = 6.0–6.5, 96.15 This study
qm (mg/g) 181.82 96.15 conc. = 25–250 mg/L
b (L/mg) 0.104 0.129 Carbofuran Carbon T = 25 °C, pH = 7.5 212 [3]
R2 0.992 0.985 slurry
Freundlich isotherm 2,4-D CAC F-200 T = 30 °C, pH = 3.2–3.9 169.49 [23]
n 1.727 2.617 conc. = 50–300 mg/L
KF 23.478 19.9 2,4-D Pristine T = 30 °C, pH = 3.8, 88.4 [24]
R2 0.963 0.928 biomass conc. = 50–300 mg/L
 J.M. Salman, B.H. Hameed / Desalination 256 (2010) 129–135 133

Table 4
Comparison of the pseudo-first-order, pseudo-second-order adsorption rate constants
and calculated and experimental qe values obtained at different initial 2,4-D
concentrations.
wastes [3]. Table 3 compares the adsorption capacities of GAC F300 for
2,4-D and carbofuran pesticides obtained in this work with other
studies [3,23,24].

Initial qe,exp Pseudo-first-order kinetic Pseudo-second-order kinetic

3.5. Adsorption kinetics
conc. (mg/g) model model
mg/L
k1 (1/h) qe,cal (mg/g) R2 k2 (g/mg.h) qe,cal (mg/g) R2 The adsorption kinetics were studied using pseudo-first-order and
50 26.08 1.020 46.16 0.993 0.045 29.07 0.970 pesudo-second-order models as given in Eqs. (4) and (5), respective-
100 50.74 0.859 65.77 0.985 0.018 58.14 0.986 ly. Values of k1 for the pseudo-first-order kinetic model were obtained
150 74.51 0.760 100.07 0.996 0.068 91.74 0.981
from the slopes of the linear plots of ln(qe − qt) versus t (figure not
200 98.29 0.632 121.87 0.995 0.004 126.58 0.986
250 121.26 0.569 153.87 0.982 0.002 169.49 0.985 shown) for all concentrations tested are listed in Tables 4 and 5 for
300 137.65 0.519 157.72 0.994 0.002 192.31 0.994 2,4-D and carbofuran, respectively. Fig. 4(a) and (b) are plots for the
pseudo-second-order kinetic for 2,4-D and carbofuran, respecitvely.
The calculated R2 and predicted equilibrium uptakes for pseudo-
second-order kinetic model are listed in Tables 4 and 5 for 2,4-D and
carbofuran, respectively. The values of the equilibrium uptake, qe
calculated for both 2,4-D and carbofuran are closer to the experi-
Table 5 mentals, hence the pseudo-second-order kinetic model describes the
Comparison of the pseudo-first-order, pseudo-second-order adsorption rate constants
adsorption of the two pesticides by GAC F300 better than the pseudo-
and calculated and experimental qe values obtained at different initial carbofuran
concentrations. first-order kinetic model. Ayranci and Hoda [2] found that the
adsorption processes for pesticides Ametryn, aldicarb, dinoseb and
Initial qe,exp Pseudo-first-order kinetic Pseudo-second-order kinetic
diuron from aqueous solution onto high specific area activated
conc. (mg/g) model model
mg/L
carbon-cloth were followed the pseudo-second-order.
k1 (1/h) qe,cal (mg/g) R2 k2 (g/mg h) qe,cal (mg/g) R2 The third model was the intraparticle diffusion model which was
50 24.25 0.301 13 0.962 0.040 25.50 0.999 tested to identify the intraparticle diffusion mechanism. Eq. (6) was
100 47.76 0.179 30.16 0.988 0.012 50.76 0.999 applied to determine the pesticide adsorption mechanism. In general,
150 63.25 0.153 46.51 0.996 0.006 68.03 0.996
the plot of qt versus t0.5 may be multilinear, which indicates that two
200 79.88 0.136 58.29 0.994 0.004 86.21 0.993
225 85.85 0.128 65.53 0.987 0.004 93.46 0.991 or more steps occur in the adsorption processes. Fig. 5(a and b)
indicates that three linear stages are involved with a moderate

Fig. 4. Pseudo-second-order kinetic for adsorption of (a) 2,4-D and (b) carbofuran on GAC F300.
134 J.M. Salman, B.H. Hameed / Desalination 256 (2010) 129–135
Fig. 5. Intraparticle diffusion plot for the adsorption of (a) 2,4-D and (b) carbofuran on GAC F300.
diffusion rate in the initial stage which are due to external surface
adsorption or instantaneous adsorption. This is followed by rapid
diffusion indicating that intraparticle diffusion is the rate-controlling
for the adsorption process. Thus, predominantly, pesticides adsorp-
tion took place rapidly by external mass transfer followed by
intraparticle diffusion. The third step corresponds to the final
equilibrium adsorption process, where the intraparticle diffusion
starts to slow down due to the extremely low solute concentration in
solution. However, the controlling step might be distributed between
intraparticle and external transport [25].
As shown in Fig. 5(a and b) the intraparticle diffusion plots for
adsorption of 2,4-D and carbofuran on GAC F-300 at 30 °C for various
pesticides initial concentrations, the first region was completed
within the first 1–2.25 and 1–5 h for 2,4-D and carbofuran,
respectively. This was the instantaneous adsorption or external
surface adsorption representing the mass transfer of adsorbate
molecules from the bulk solution to the adsorbent surface. The
second region was the gradual adsorption stage where intraparticle
diffusion was the rate limiting. The third region did not exist as most
of the pesticides molecules had already been adsorbed on the surface
of the activated carbon. The rates of adsorption observed at different
stages of the process indicated that the adsorption rate was initially
very fast and then slowed down as time progressed. Referring to all
the intraparticle diffusion plots in the figures, the linear line of the
second and third stages did not pass through the origin and this
deviation from the origin or near saturation might be due to the
difference in the mass transfer rate in the initial and final stages of
adsorption [26]. This implied that intraparticle diffusion was not the
only rate limiting mechanism in the adsorption processes.
4. Conclusion
The present investigation showed GAC F300 to be a promising
adsorbent for the 2,4-D and carbofuran over a wide range of
concentrations. Equilibrium data were fitted to Langmuir and
Freundlich isotherms and the equilibrium data were best described
by the Langmuir isotherm model with maximum monolayer
adsorption capacity of 181.82 and 96.15 mg/g for 2,4-D and
carbofuran, respectively. The adsorption kinetics was found to follow
closely the pseudo-second-order kinetic model for both pesticides.
Acknowledgement
The authors acknowledge the research grant provided by
Universiti Sains Malaysia, Penang, under short-term grant (Grant
no: 6035287) that has resulted in this article.
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