Desalination 194 (2006) 110

Adsorption of Reactive Black 5 from an aqueous solution:

equilibrium and kinetic studies
Zeynep Eren, Filiz Nuran Acar*
Department of Environmental Engineering, Engineering Faculty, Ataturk University, Erzurum 25240, Turkey
Tel. +90 (442) 2314-809; email: facar@atauni.edu.tr

Received 6 October 2004; accepted 25 October 2005

Abstract
Removal of a reactive dye, Reactive Black 5, from an aqueous solution was studied by adsorption on powdered
activated carbon (PAC) and Afsin-Elbistan fly ash (Turkey). The adsorption of the dye on PAC and fly ash was
investigated during a series of batch adsorption experiments carried out to determine the effect of initial dye con-
centration and contact time. The amounts adsorbed at equilibrium were measured. The Langmuir and Freundlich
isotherm models were tested for their applicability. The equilibrium data satisfied both Langmuir and Freundlich
models. The adsorption capacity of PAC and fly ash were found to be 58.823 mg and 7.936 mg dye per gram of
adsorbent, respectively. The experimental data were analysed using the pseudo-first-order and pseudo-second-order
adsorption kinetic models. According to these models, the rate constants were evaluated for initial dye concentrations.
The experimental data fit the second-order kinetic model.

Keywords: Adsorption; Adsorption isotherms; Kinetics of adsorption; Activated carbon; Fly ash; Reactive dye

1. Introduction
Dyes usually have a synthetic origin and com-
plex aromatic molecular structures which make
them more stable and more difficult to biode-
grade. Today there are more than 10,000 dyes
available commercially [1] Dyes are used in
many industries such as food, paper, carpet,
rubber, plastics, cosmetics and textiles [2]. These
colored compounds are not only aesthetically
*Corresponding author.
displeasing but they also inhibit sunlight from
penetrating into the stream and reduce the photo-
synthetic reaction. Some dyes are also toxic and
carcinogenic [3].
Dyes can be classified as follows [4]: anionic
(direct, acid and reactive dyes), cationic (basic
dyes) and non-ionic (dispersive dyes). Different
types of reactive dyes commercially react with
textile fibers to achieve a covalent dye-fiber bond
[5]. Reactive dyes are typically azo-based
chromophores combined with different types of

0011-9164/06/$ See front matter 2006 Elsevier B.V. All rights reserved
doi:10.1016/j.desal.2005.10.022
2 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110
reactive groups. They differ from all other classes
of dyes in that they bind to the textile fibers such
as cotton to form covalent bonds [6]. The ex-
panded use of reactive dyes during the last decade
has made an impact on conventional methods for
treating textile effluents due to the generally poor
biodegredation of such dyes (especially those
containing azo-groups) under aerobic conditions
[7].
Some of dyes are toxic and carcinogenic and
require separation and advanced treatment of tex-
tile effluents before discharge into conventioanl
systems [8]. Due to low biodegradability of dyes,
a conventional biological wastewater treatment
process is not very efficient in treating dye waste-
water. Hence, investigations have been conducted
on physicochemical methods of removing color
from textile effluents [9]. These studies include
chemical oxidation [10], membrane filtration [11]
and adsorption techniques [12].
In these techniques, adsorption has been found
to be an efficient process to remove dye [12].
Activated carbon [13] and natural adsorbents
such as banana and orange peel [14], apple
pomace and wheat straw [15], waste mud [16],
and wood materials [17] have been extensively
used as adsorbents. Activated carbon adsorption
has been found to be an effective means of waste-
water treatment. Despite its importance, activated
carbon is an expensive material. This has led to a
search for low-cost materials as alternatives [18].
Fly ash is a waste material originating in great
amounts in combustion processes. Although fly
ash use in construction and other civil engineer-
ing applications is expected to increase, it is
unlikely that they will ever use all the fly ash
generated. Research is therefore needed to deve-
lop new environmentally friendly applications
that can further exploit fly ash [19]. Fly ash has
been treated for dye removal. For example, Janos
et al. have studied the adsorption of both cationic
and anionic dyes onto fly ash [19]. Wang et al.
have investigated the removal of methylene blue
(a cationic dye) on raw and modified fly ash [3].
Acemioglu investigated Congo red (anionic dye)
onto calcium rich fly ash [20]. Kumar et al.
studied modelling the mechanism involved during
the sorption of methylene blue onto fly ash [21].
In another work, the removal of Omega Chrom
Red by a homogeneous mixture of fly ash was
studied by Gupta et al. [22]. Also, Ramakrishna
and Viraraghavan investigated the removal of
acid and basic dyes by low-cost adsorbents: peat,
fly ash, bentonite, and steel plant slag [23].
The purpose of this work was to study the
mechanism of adsorption Reactive Black 5 (RB5),
a reactive dye, on another industrial waste fly ash
and PAC and to compare their adsorption capa-
cities for the removal of RB5 under optimum
experimental conditions.
2. Materials and methods
2.1. Dye characterization
The dye used in this study is Chemazol Black
B (C.I. Reactive Black 5), obtained from a textile
firm in Turkey. In Table 1 its characteristics are
summarized. Its chemical structure is shown
Fig. 1. Absorbance values were recorded at the
corresponding maximum absorbance wavelength.
2.2. Powdered activated carbon (PAC)
PAC (Merck) was used as an adsorbent. Its
surface area is 900 BET, N2, m2/g.
2.3. Fly ash
Fly ash was obtained from the Afsin-Elbistan
Thermal Power Plant, Turkey. It was used with-
out further treatment. The physical characteristics
and chemical composition [24] of Afsin-Elbistan
fly ash are reported Tables 2 and 3, respectively.
Its surface area was determined by the BET
method (Quantasorb Surface Area Analyser,
Model QS-17). The fly ash was sieved to obtain
various size fractions using sieves.
 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110 3

Fig. 1. Chemical structure of Reactive Black 5.

Table 1
Characterization of Chemazol Black B

Generic name CI Reactive Black 5

Percentage of pure dye 66
Anchor Vinylsulfone
Chromophore Azo
max, nm 598

Table 2
Physical characteristics of Afsin-Elbistan fly ash, with a
specific surface area of 3.55 m2/g

Differential particle size, m % weight

Fig. 2. SEM photograph of Afsin-Elbistan fly ash.
!355 +212 3.7
!212 +180 6.3
!180 +125 9.0
!125 +90 5.0
!90 +64 31.0 with some magnetite and calcite. Afsin-Elbistan
!63 45.0 fly ash is a C class fly ash with 23.66% lime CaO
as a major constituent [24]. According to ASTM,
Table 3 Afsin-Elbistan fly ash is suitable for a C fly ash
Chemical composition of Alsin-Elbistan fly ash [24] class (with high lime content) because the value
of SiO2 + Al2O3 + Fe2O3 is below 50%, and the
Constituent % weight value of CaO is higher than 10% [25]. A SEM
photograph of Afsin-Elbistan fly ash is shown in
SiO2 15.14
Al2O3 7.54
Fig. 2 [25].
CaO 23.66 A leaching test was not done in this study, but
Fe2O3 3.30 some researchers have been reported that leach-
MgO 4.50 ability of heavy metals from coal fly ash is rela-
Na2O 0.57 tively low. The leachates contain a very negli-
K2O 0.28 gible amount (at ppb levels) of metals like Fe, Ca,
TiO2 1.03 Mg, far below the discharge levels stipulated by
SO3 13.22
statutory regulations. The concentrations of heavy
metals in the leachate were in the range of 0.01 to
As can be seen, primary crystalline species in 0.3 mg/L and did not exceed regulatory limits
the original fly ash sample are quartz and mullite [19,26].
4 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110

2.4. Experimental run

Batch adsorption experiments were carried out
at room temperature (20EC). The stock solution
of RB5 (1000 mg/L) was prepared and suitably
diluted to the required initial concentrations
(5100 mg/L). The experiments were carried out
in 250 ml flasks containing 100 ml of synthetic
dye solution. The flasks were agitated on a shaker
at 200 rpm for 60 min. The final equilibrium con-
centrations were measured spectrophotometric-
ally at 598 nm using a Shimadzu 160 A. Various
experimental conditions such as initial dye con-
centrations and contact time were studied. The
percentage removal of dye and amount adsorbed Fig. 3a. Effect of contact time and initial dye concen-
(mg/g) were calculated using the following rela- tration on dye removal. PAC dose 1 g/L (natural initial
pH, at 20EC, agitation speed 200 rpm).
tionships [18]:

Percentage removal (%) = 100 (C0!Ce)/C0 (1)

Amount adsorbed (qe) = (C0!Ce)/M (2)

where C0 and Ce are the initial and equilibrium

concentrations (mg/L), respectively, and M is the
mass of adsorbent (g/L).

3. Results and discussion

3.1. Effect of initial dye concentrations
The initial concentration provides an impor-
tant driving force to overcome all mass transfer
resistances of the dye between the aqueous and
solid phases. The effect of concentration on
contact time was also investigated as a function
of initial dye concentration. The adsorption of
dye by PAC and fly ash were studied at several
different initial RB5 concentrations ranging from
5 to 100 mg/L. The results are shown in Figs. 3a
and 3b.
The results indicate that the rate of color
removal increased depending on the contact time.
For both adsorbents, decolorization of dye is
extremely rapid in the first 10 min. Then the rate
Fig. 3b. Effect of contact time and initial dye concen-
tration on dye removal. Fly ash dose 10 g/L (natural
initial pH, at 20EC, agitation speed 200 rpm).
of adsorption became slow in the adsorption
processes. As can be seen in Figs. 3a and 3b,
when the initial dye concentration was increased,
adsorption efficiency decreased. This was due to
the saturation of the sorption sites on the adsor-
bents as the concentration of the dye increased.
The equilibrium adsorption capacity of the adsor-
bent increased with increasing initial dye con-
centration up to 100 mg/L, while adsorption
 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110 5

removal of dye showed the opposite trend. When

the initial dye concentration increased from
5 mg/L to 100 mg/L, the adsorption capacity of
PAC increased from 7.76 mg/g to 49.9 mg/g and
the adsorption removal for PAC decreased from
100.0% to 49.9%; similarly, the adsorption capa-
city of fly ash increased from 0.93 mg/g to
7.12 mg/g, and the adsorption removal for fly ash
decreased from 97.0% to 71.2%. Fig. 4a. Effect of adsorbent dose (PAC) on dye removal.
Initial dye concentration 50 mg/L (natural initial pH, at
20EC, agitation speed 200 rpm).
3.2. Effect of adsorbent dose
Figs. 4a and 4b show the removal of RB5 by
fly ash and PAC at different doses for a dye
concentration of 50 mg/L. Increase in adsorbent
dose increased the percentage removal of dye,
which is due to the increase in adsorbent surface
area of the sorbent.

3.3. Adsorption isotherms

Using the batch technique described in the
experimental section, dependencies of the ad-
sorbed amounts of RB5 on their equilibrium con-
centrations in solution were measured. The data
obtained from equilibrium studies were analyzed
according to Langmuir and Freundlich adsorption
isotherms.
The Langmuir and Freundlich equations are
commonly used to describe adsorption isotherms
at a constant temperature for water and waste-
water treatment applications. The Langmuir
model is valid for monolayer sorption onto a
surface with a finite number of identical sites.
The distribution of dyes between the solid-
solution interface equilibrium has been described
by the Langmuir equation [27]. The well known
expression of the Langmuir model is given by
Eq. (3):
qe = QobCe /(1 + bCe) (3)
where qe (mg/g) and Ce (mg/L) are the amounts of
adsorbed dye per unit weight of adsorbent and
Fig. 4b. Effect of adsorbent dose (fly ash) on dye
removal. Initial dye concentration 50 mg/L (natural initial
pH, at 20EC, agitation speed 200 rpm).
unadsorbed dye concentration in solution at equi-
librium, respectively. Qo is the maximum amount
of the dye bound per unit weight of adsorbent to
form a complete monolayer on the surface at high
Ce, and b is a constant related to the affinity of the
binding sites (L/mg).
The empirical Freundlich equation based on
sorption onto a heterogeneous surface is given as
qe = kFCe1/n (4)
where kF and n are the Freundlich constants for
the system, which are indicators of adsorption
capacity and intensity, respectively [28].
The values of the Freundlich and Langmuir
parameters were obtained, respectively, from the
linear correlations between the values of Ce /qe
and Ce and log qe and log Ce. The adsorption
isotherm parameters along with the correlation
6 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110

Table 4
Langmuir and Freundlich model constants

Langmuir model Freundlich model

Qo, mg/g b, L/mg R2 C0, mg/L RL kF, L/g n R2

PAC 58.823 0.109 0.94 5 0.647 5.754 1.697 0.94

10 0.478
25 0.268
50 0.155
100 0.084
Fly ash 7.936 0.189 0.93 5 0.514 1.285 1.965 0.98
10 0.346
25 0.175
50 0.096
100 0.050

coefficients are presented in Table 4. The linear C RL >1 Unfavorable

relationships were evidenced by the R2 values (for
the Langmuir model, 0.94 and 0.93 for PAC and
fly ash, respectively; for the Freundlich model,
0.94 and 0.98 for PAC and fly ash, respectively).
These indicate the applicability of the two
adsorption isotherms and the monolayer coverage
on the adsorbent surface.
Afsin-Elbistan fly ash was observed to possess
a high adsorption capacity. Hence, for the re-
moval of dye, fly ash could be used as a low-cost
adsorbent as an alternative to PAC. The maxi-
mum amount of dye per unit weight of adsorbent
was 6.4 mg/g on charfines and 4.1 mg/g on lig-
nite coal [29], 6.935 mg/g on shale oil ash [30],
and 7.936 mg/g in this study. The essential char-
acteristics of the Langmuir isotherm can be ex-
pressed by a separation or equilibrium parameter,
a dimensionless constant, which is defined by
Eq. (5):
RL = 1/(1 + bC0) (5)
where C0 is the initial concentration of dye
(mg/L) and b is the Langmuir constant (L/mg). RL
indicates the nature of the adsorption process as
given below [28]:
C RL = 1 Linear
C 0 <RL <1 Favorable
C RL = 0 Irreversible
The values of RL were found to be in the range
of 01, indicating that the adsorption process is
favorable for both adsorbents. In addition, the
Freundlich adsorption constant, n, should be
among 110 for beneficial adsorption [31].
Table 4 shows that n values are in the range of
110 for both adsorbents. Based on the corre-
lation coefficient R2 shown in Table 4, fly ash can
be better described by the Freundlich model. The
Freundlich equation also yields a better fit of the
experimental data than the Langmuir equation for
fly ash.
3.4. Kinetics models
3.4.1. Pseudo-first-order kinetic model
In order to examine the controlling mechanism
of adsorption processes such as mass transfer and
chemical reaction, several kinetic models were
used to test experimental data. The experimental
data were also analyzed using the pseudo-first
and pseudo-second-order adsorption kinetic
 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110 7

models, and kinetic constants were calculated for

concentration and adsorbent dose.
The first-order rate expression of Lagergren
based on solid capacity is generally expressed as
follows:

dq /dt = k1 (qe!q) (6)

where qe and q are the amounts of adsorbed dye

on the PAC at equilibrium and at time t, re-
spectively (mg/g), and k1 is the rate constant of
first-order adsorption (1/min). After integration
and applying boundary conditions, t = 0 to t = t
and q = 0 to q = q, the integrated form of Eq (6)
becomes
Fig. 5a. Pseudo-first-order model for initial dye con-
centrations for PAC.
log (qe!q) = log qe !(k1 /2.303) t (7)

A straight line of log (qe!q) vs. t suggests the

applicability of this kinetic model. In order to fit
Eq (7) to the experimental data, the equilibrium
sorption capacity, qe, must be known. In many
cases qe is unknown, and adsorption tends to
become immeasurably slow. The amount sorbed
is still significantly smaller than the equilibrium
amount. For this reason, it is necessary to obtain
the real equilibrium sorption capacity by extra-
polating the experimental data to t = 4 or by
using a trial-and-error method. Also, in many
cases the first-order equation of Lagergren does
not fit well for the whole range of contact time
and is generally applicable only over the initial
stage of adsorption processes [28,32].
The values of first-order rate constants and Fig. 5b. Pseudo-first-order model for initial dye con-
correlation coefficient (R2 value) are given centrations for fly ash.
Table 5. These data are plotted in Figs. 5a and 5b.
The PAC linear correlations were found to be
suitable at a confidence level for to fly ash. sorption capacity of the solid phase. Contrary to
the other model, it predicts the behavior over the
whole time of adsorption and is in agreement
3.4.2. Pseudo-second-order kinetic model with an adsorption mechanism being the rate
A pseudo-second-order model may also controlling step, which may involve valency
describe the kinetics of adsorption. The pseudo- forces through sharing or exchange of electrons
second-order equation is also based on the between dye anions and adsorbent.
8 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110

Table 5
Comparision of first- and second-order-kinetic models rate constants and calculated and experimental qe values obtained
at different initial Reactive Black 5 concentrations

C0 qe k1 qe(cal) R2 k2 h qe(cal) R2
(mg/L) (mg/g) (1/min) (mg/g) (g/mg min) (mg/g min) (mg/g)
PAC 10 7.76 0.0744 10.787 0.98 0.0042 0.5210 11.099 0.95
25 19.03 0.0297 6.045 0.62 0.0121 4.5556 19.418 0.98
50 34.75 0.1221 59.306 0.88 0.0021 3.7679 42.373 0.99
100 49.96 0.0320 15.367 0.53 0.0045 12.0773 51.546 0.99
Fly ash 5 0.485 0.0537 0.398 0.92 0.0846 0.0355 0.648 0.97
10 0.93 0.0035 0.103 0.02 0.5068 0.4485 0.941 0.99
25 2.305 0.0983 0.292 0.73 1.1467 6.3816 2.359 0.99
50 3.947 0.0760 1.043 0.81 0.1398 2.3202 4.073 0.99
100 7.121 0.0152 1.796 0.57 0.0413 1.9904 6.944 0.98

The pseudo-second-order model rate equation
is expressed as:
dq /dt = k2 (qe!q)2 (8)
where k2 is the rate constant of second-order
adsorption (g/mg min). For the boundary con-
ditions t = 0 to t = t and q = 0 to q = q, and re-
arranging, the linearized form can be obtained:
t/q = 1 / k2qe2 + (1 /qe) t (9)
If the second-order kinetic is applied, the plot of
t/q against t should give a linear relationship,
from which qe and k2 can be determined from the
slope and intercept of the plot.
h = k2qe2 (10)
In these equations, h is the initial sorption rate
(mg/g min) [32,33].
The kinetic plots for Eq. (9) were made for
two adsorbents at different initial concentrations.
These plots are presented in Figs. 6a and 6b. In
Table 5, calculated qe [qe(calc)] are presented. qe(calc)
calculated for the second-order kinetic equation
is close to the initial qe for both adsorbents. For
example, when qe is 19.03 mg/L [calculated from
Eq. (2)] for 25 mg/L initial dye concentration,
qe(calc) is calculated as 6.045 mg/g for PAC
adsorption in the first-order model but is calcu-
lated as 19.418 mg/g in the second-order kinetic
model.
Good fits were observed for all data where the
adsorption reaction can be approximated with the
second-order kinetic model. The smallest cor-
relation coefficient in this case was 0.95, which is
the removal of RB5 (C0 =10 mg/L) on PAC. It
can be observed that h (initial sorption rate
mg/g.min) is generally higher for PAC adsorption
than that of fly ash. This shows that the second-
order kinetics model was found to be more suit-
able than the first-order kinetic model for either
adsorbent.
The calculated qe values also agreed very well
with the experimental qe values in the case of
second-order kinetics. These results suggest that
each of the sorption experiments is not a first-
order model and that the second-order model,
based on the assumption that the rate limiting step
may have chemisorption, provides the best corre-
lation of the data for both adsorbents. Similar
kinetic results were reported in the biosorption of
Remazol Blue dye using some yeast as the
adsorbent [28], in the adsorption of Reactive Blue
114, Reactive Yellow 64 and Reactive Red 124
 Z. Eren, F. Nuran Acar / Desalination 194 (2006) 110
Fig. 6a. Pseudo-second-order model for initial dye con-
centrations for PAC.
Fig. 6b. Pseudo-second-order model for initial dye con-
centrations for fly ash.
dyes on calcined alunite [32] and the adsorption
of Congo red onto Afsin- Elbistan fly ash [20].
4. Conclusions
The capability of PAC and Afsin-Elbistan fly
ash for removing RB5 dye was examined, in-
cluding equilibrium and kinetic studies. Experi-
ments were performed as a function of initial dye
9
concentration and effect of adsorbent dosage.
Based on the experimental data, Afsin-Elbistan
fly ash had a lower adsorption efficiency than
PAC, but fly ash was an effective adsorbent for
removal of RB5 from an aqueous solution. In
addition, it is a low-cost adsorbent. PAC, com-
monly used as an adsorbent, is an expensive
material and regeneration is essential, whereas fly
ash is found in abundance at thermal power
stations in Turkey. Also for fly ash, regeneration
is not necessary.
The Langmuir and Freundlich isotherm
models were used to investigate the adsorption
equilibrium of both adsorbents. The monolayer
adsorption capacity of PAC and fly ash were
found to be 58.823 and 7.936 mg/g, respectively.
The suitability of first- and second-order
kinetic models for the sorption of RB5 onto
adsorbents was also discussed. It was decided that
the adsorption kinetics of both adsorbents obeyed
the second-order adsorption model.
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