289

Adsorption of Alizarin Red S onto Nano-sized Silica Modified with

γ-Aminopropyltriethoxysilane

Deliang Li*, Qing Liu, Shuanglong Ma, Zhixian Chang and Ling Zhang Institute of
Environmental and Analytical Sciences, College of Chemistry and Chemical Engineering, Henan University, Kaifeng
475004, P. R. China.

(Received 20 October 2010; accepted 7 April 2011)

ABSTRACT: The adsorption of Alizarin Red S (ARS) dye onto nano-sized

silica modified with γ-aminopropyltriethoxysilane (AMNS) was studied. The
effects of the initial pH and concentration of the ARS solution, the AMNS
dosage, the contact time and temperature on the removal and adsorption
capacities have been investigated. The experimental isotherm data were
analyzed using the Langmuir and Freundlich equations. The adsorption of ARS
onto AMNS followed the Langmuir model, the maximum adsorption capacity
being estimated as 200 mg/g. The application of three kinetic models, viz.
pseudo-first-order, pseudo-second-order and intra-particle diffusion, to the
experimental kinetic data was discussed. It was shown that the sorption
processes were better fitted by the pseudo-second-order equation. From
thermodynamic studies, the values of the Gibbs’ free energy (∆G0), standard
enthalpy change (∆H0) and standard entropy change (∆S0) were calculated as
–3.78 kJ/mol, –90.05 kJ/mol and –289.34 J/(mol K), respectively, thereby
indicating that the adsorption process was spontaneous and exothermic.

INTRODUCTION

Large amounts of wastewater containing dyes originate from dyeing industries such as textile,
leather, printing and plastics, etc. These dyes are commonly considered to be hazardous and toxic
to living organisms. In addition, such dyes are invariably resistant to degradation by light, chemical,
biological and other exposures. Dye wastewater has caused serious pollution to water resources and
hence the removal of dyes from industrial wastewaters has become a major problem.
Technologies such as coagulation and flocculation (Majewska-Nowak et al. 1989), ultrasound
oxidation (Vončina and Majcen-Le-Marechal 2003), ozonation (Galindo and Kalt 1999),
membrane-based separation processes (Purkait et al. 2006), electrochemical (Shendrik 1989) and
biological degradation (Walker et al. 2003) have already been investigated extensively, but these
methods possess drawbacks such as the use of substantial amounts of energy and chemicals.
Adsorption is a well-known and popular physicochemical method for dye removal. The most
common adsorbent employed is activated carbon because of its high effectiveness and capacity;
however, its large-scale application is still limited by its high cost and difficult regeneration.
Over the past two decades, many low-cost adsorbent materials, e.g. clay minerals (Turabik
2008; Nandi et al. 2009), biomaterials (Hameed et al. 2008), fly ash (Lin, X.J. et al. 2008),
bagasse pith (Nassar and El-Geundi 1991), alumina (Asok et al. 2005), activated sludge (Pagga

*
Author to whom all correspondence should be addressed. E-mail: lideliang@henu.edu.cn.
290 Deliang Li et al./Adsorption Science & Technology Vol. 29 No. 3 2011

and Taeger 1994), nanotubes (Fugestu et al. 2004; Lee et al. 2008) and modified silica (Pavan et
al. 2008; Cestari et al. 2009; Andrzejewska et al. 2007), have been examined with a view to their
use in the removal of dyes from aqueous solutions. Modified silica has been widely examined as
a promising material because of its high specific surface area, high reactivity, high stability and
non-toxicity. Thus, for example, Pavan et al. (2008) investigated the removal of Congo Red by
anilinepropyl-silica xerogel, Cestari et al. (2009) discussed the adsorption behaviour of Reactive
Yellow GR and Reactive Red RB onto a mesoporous aminopropyl-silica and Andrzejewska et al.
(2007) studied the adsorption of C.I. Reactive Blue 19 onto precipitated Syloid® 244 silica
modified with 3-aminopropyltriethoxysilane. However, such silicas have usually been prepared in
the laboratory and their sizes have often been in the micrometre range. In addition, their shape,
stability and reproducibility remain to be validated.
Nano-sized silica modified with γ-aminopropyltriethoxysilane (AMNS) is a novel type of
material developed in our laboratory involving surface modification via in situ polymerization of
nano-sized silica and γ-aminopropyltriethoxysilane (APS). Alizarin Red S (ARS) is a
hydroxyanthraquinone dye with a superior colour performance but with strong carcinogenic
toxicity. In the present work, we were particularly interested in the adsorption of ARS onto
AMNS, with the principal factors affected the adsorption equilibrium including the initial pH and
concentration of the ARS solution, the AMNS dosage, the contact time and the temperature being
examined. The equilibrium data were analyzed using the Langmuir and Freundlich models, while
attempts were made to fit the kinetic data by the pseudo-first-order, pseudo-second-order and
intra-particle diffusion models. In addition, the various thermodynamic parameters were also
calculated in an attempt to reveal the nature of the adsorption process. The results obtained could
be helpful in the further application of AMNS, as well as for designing new approaches for the
treatment of dye-containing wastewaters.

MATERIALS AND METHODS

Materials

AMNS was obtained from the Henan Province Nanomaterial Engineering & Technology Research
Center. This pilot silica was modified with APS according to the method employed by Li, X.H. et
al. (2006). A.R. grade Alizarin Red S (ARS) was supplied by the Merck Chemical Company
(Germany). All the other reagents were of A.R. grade and high-purity water was used throughout.

Methods

Working solutions of ARS were prepared by diluting a stock solution containing 1000 mg/
ARS.
All experiments were performed by taking 15 m
of the ARS working solution in a glass beaker
under variable conditions and stirring at 200 rpm. These variables were the initial pH (1–10), the
AMNS dosage (20–300 mg), the initial ARS concentration (50–1000 mg/
), the contact time
(2–60 min) and the temperature (10–40 ˚C). The pH value of the ARS working solution [as
measured by a pH 211 Microprocessor pH meter (HANNA, Italy)] was adjusted by adding small
amounts of HCl or NaOH solutions as appropriate. The final AMNS/ARS mixture was centrifuged
at 4000 rpm for 30 min to disperse the AMNS particles. A known volume of supernatant solution
was then taken, diluted with phosphate buffer (pH
7.0) and the ARS remaining therein
determined spectrophotometrically at a wavelength of 520 nm using a LabTech Bluestar UV–vis
Adsorption of Alizarin Red S onto Nano-sized Silica Modified with γ-Aminopropyltriethoxysilane 291

spectrophotometer (LabTech Ltd., Beijing, P. R. China). The amount of ARS adsorbed onto
AMNS was calculated via material balance while the percentage removal of ARS was calculated
via equation (1):

c0 − c
% Re moval = × 100 (1)
c0

where c0 and c are the initial and residual concentrations of ARS (mg/
), respectively, in the
aqueous solution. The adsorption capacity of ARS onto AMNS (q) was calculated via equation (2):

q =
(c 0 − c )V
(2)
m

where q is the adsorption capacity of ARS on AMNS (mg/g), V is the volume of the ARS working
solution (
) and m is the dosage of AMNS employed (g).

RESULTS AND DISCUSSION

Characterization of AMNS

Generally, the functional groups on the adsorbent play a very important role in the adsorption of the
adsorbate. Thus, knowledge of the nature of the functional groups on the adsorbent surface would
be helpful in understanding the adsorption process. Figure 1 shows the IR spectra of AMNS and
silica. Compared to the silica spectrum, the absorptions corresponding to the stretching vibration at
3000–3800 cm1 and the deformation vibration at 1636 cm1 and 963 cm1 of the silanol
functionality in AMNS are significantly diminished, thereby demonstrating a significant decrease in

70
SiO2
60

50
Transmittance (%)

40
AMNS
30

20 2873
1569
2936
10

−10
4000 3500 3000 2500 2000 1500 1000 500
Wavenumber (cm−1)

Figure 1. IR spectra of AMNS and nano-sized silica.

292 Deliang Li et al./Adsorption Science & Technology Vol. 29 No. 3 2011

the silanol content after modification of silica with APS. The new peak in the spectrum of AMNS at
1569 cm1 is attributed to the deformation vibration of the N–H group, those at 2873 and 2936 cm1
are assigned to the C–H stretch of the –(CH2)n– group, while the peak at 691 cm1 is attributed to
the –CH2– rocking vibration of Si–CH2R. There is no obvious vibration corresponding to C–O in the
AMNS spectrum, which indicates that APS was grafted onto silica via chemical bonding rather than
physical adsorption. This suggests that AMNS possesses a relatively stable structure.

Effect of pH

To study the effect of pH, experiments were undertaken with initial pH values varying within the
range 1–10. As shown in Figure 2, the percentage removal of ARS increased slightly from 95.3%
to 99.1% as the pH of the system was increased from 1 to 2.2, followed by decreases to 33% at
pH
4 and to 21% at pH
10. This result can be explained if account is taken of the charged
states of AMNS and the existing forms of ARS. At lower pH values, AMNS may readily receive
a proton to form a positive group ( − NH 3+ ) while ARS could lose a proton to form a negative group
−
( −SO 3 ). As a consequence, the interaction between AMNS and ARS is dominated by electrostatic
attraction between the corresponding − NH 3+ and −SO 3− groups. In addition, lower pH results in
the number of − NH 3+ and −SO 3− reaction sites increasing, thereby enhancing the adsorption of
ARS onto AMNS. However, such adsorption decreases sharply when the pH value is greater than
2.2, probably as a result of a reduction in the number of − NH 3+ reaction sites. Over the pH range
4–10, the removal extent slowly decreases, possibly as a consequence of a further reduction in the
number of − NH 3+ reaction sites and the secondary ionization of ARS. However, removal did not
decrease to zero until the pH value had increased to 10 (at such a pH value, the AMNS functional
groups are mainly in the –NH2 form while ARS is mainly present as the multiple negatively
charged form), suggesting that the interactions between AMNS and ARS might involve both
electrostatic attraction and hydrogen bonding. The different removal extents recorded at lower and

105

90

75
% Removal

60

45

30

15

0
0 2 4 6 8 10
pH

Figure 2. Effect of initial pH on the percentage removal of ARS from aqueous solution by AMNS. Experimental
conditions employed: initial ARS conc., 500 mg/
; AMNS dosage, 0.15 g; contact time, 60 min; temp., 20 C.
Adsorption of Alizarin Red S onto Nano-sized Silica Modified with γ-Aminopropyltriethoxysilane 293

100

98

96

% Removal 94

92

90

88
0 10 20 30 40 50 60
Time (min)

Figure 3. Effect of contact time on the percentage removal of ARS from aqueous solution by AMNS. Experimental
conditions employed: initial pH, 2.2; ARS concentration, 500 mg/
; AMNS dosage, 0.15 g; temp., 20 C.

higher pH values indicate that about 78% of ARS could be recovered by changing the pH value
of the aqueous medium.

Effect of contact time

The uptake of adsorbate increased with increasing contact time, the short time period necessary
for adsorption to attain an equilibrium value being of value in any practical application. Figure 3
shows a plot of the percentage removal versus the contact time. This indicates that the removal of
ARS rapidly increased to 89% within 2 min and to 97% within 5 min; thereafter, further increase
proceeded slowly, with equilibrium being approached after 40 min.

Effect of the initial ARS concentration

The percentage removal of ARS at different initial concentrations within the range 50–1000 mg/

is shown overleaf in Figure 4, as well as the corresponding adsorption capacity at equilibrium (qe).
As shown overall, the removal of ARS increased rapidly to 98% as the initial concentration of
ARS increased from 50 mg/
to 250 mg/
, then increased slowly to 99% as the initial ARS
concentration was increased up to 500 mg/
, and finally decreased slightly to a value of 97% for
an initial ARS concentration of 1000 mg/
. At the same time, the value of qe increased linearly
from 4 mg/g to 98 mg/g. These results indicate that the adsorption of ARS increased as the initial
concentration of ARS increased. This could be attributed to the greater number of ARS molecules
present in the system at higher initial ARS concentrations, thereby providing a higher driving
force for the adsorption of ARS onto AMNS.

Effect of AMNS dosage

The effect of different adsorbent dosages within the range 0.02–0.3 g on the removal of ARS is shown
overleaf in Figure 5. It will be seen that the percentage removal of ARS initially increased rapidly to
more than 98% as the AMNS dosage was increased up to 0.15 g, which may be attributed to the
294 Deliang Li et al./Adsorption Science & Technology Vol. 29 No. 3 2011

102
100
99

96 80

% Removal

qe (mg/g)
93
60
90
40
87

84 20

81
0
0 200 400 600 800 1000 1200
Initial dye concentration (mg/ℓ)

Figure 4. Effect of the initial ARS concentration on its percentage removal from aqueous solution by AMNS together with
the corresponding adsorption capacity at equilibrium (qe). Experimental conditions employed: initial pH, 2.2; AMNS
dosage, 0.15 g; contact time, 60 min; temp., 20 C.

102 350

300
99
0.05
250
96 0.04
% Removal

1/qe (g/mg)

qe (mg/g)

0.03 200
93
0.02
150
0.01
90
100
0.00
0 100 200 300
87 Adsorbent dosage (mg)
50

84 0
0 50 100 150 200 250 300
Adsorbent dosage (mg)

Figure 5. Effect of AMNS dosage on the percentage removal of ARS from aqueous solution by AMNS together with the
corresponding adsorption capacity at equilibrium (qe). The inset shows the linear relationship between 1/qe and the AMNS
dosage. Experimental conditions employed: initial pH, 2.2; ARS conc., 500 mg/
; contact time, 60 min; temp., 20 C.

greater availability of adsorption sites with increasing amounts of AMNS in the system. However,
after the attainment of a critical dosage (0.15 g), the percentage removal slowly decreased. Over the
same range of AMNS dosage, the value of qe diminished in a regular manner. The inset in the figure
shows the plot of 1/qe versus AMNS dosage. This exhibits a good linearity, revealing that smaller
dosages of AMNS led to the supply of a greater number of adsorption sites. At higher dosages, it is
possible that AMNS agglomerates, thereby resulting in some adsorption sites being encapsulated.
Adsorption of Alizarin Red S onto Nano-sized Silica Modified with γ-Aminopropyltriethoxysilane 295

100 52

96
50

% Removal

qe (mg/g)
92
48
88

46
84

80 44
8 16 24 32 40
Temperature (°C)

Figure 6. Effect of temperature on the percentage removal of ARS from aqueous solution by AMNS together with the
corresponding adsorption capacity at equilibrium (qe). Experimental conditions employed: pH, 2.2; ARS conc., 500 mg/
;
AMNS dosage, 0.15 g; contact time, 60 min.

Effect of temperature

Temperature is an important parameter in any adsorption process. To observe the effect of

temperature in the system under study, plots of the percentage removal of ARS and qe as a function
of temperature (over the range 10–40 C) are shown in Figure 6. This shows that both the percentage
removal and the value of qe decreased with increasing temperature. The extent of adsorption at lower
temperature was greater than that at higher temperature, thereby implying that the adsorption process
was exothermic. The percentage removal of ARS at room temperature (25 C) was ca. 97%,
confirming the potential use of AMNS for the adsorption of ARS. The fact that such removal
decreased with increasing temperature also suggests the possibility of recovering ARS by changing
the temperature.

Adsorption isotherms

Adsorption isotherms are of fundamental importance in designing a given adsorption system,

since they provide valuable information for understanding the interaction between the adsorbate
and the adsorbent. Hence, it is essential to establish a theoretical or empirical isotherm equation
for interpreting a given adsorption process and for predicting the extent of such adsorption.
In the present work, the most commonly used isotherm equations, viz. those of Langmuir and
Freundlich, were used to interpret the experimental adsorption data obtained. The linearized
Langmuir model may be expressed as in equation (3) (Alkan et al. 2005):

ce 1 ce
= + (3)
qe q max K L q max

where qmax is the maximum adsorption capacity of the adsorbent (mg/g) and KL is the Langmuir
constant (
/mg). The values of qmax and KL may be obtained from the respective slope and
intercept of the linear plot of ce/qe versus ce. The essential features of the Langmuir isotherm can
296 Deliang Li et al./Adsorption Science & Technology Vol. 29 No. 3 2011

be expressed in terms of a dimensionless constant, called the separation factor or the equilibrium
parameter (RL), which may be defined by equation (4) (Purkait et al. 2006):

1
RL = (4)
1 + K Lc0

The value of RL, which is related to the isotherm shape, indicates that the adsorption is either
unfavourable (RL  1), linear (RL
1), favourable (0  RL  1) or irreversible (RL
0).
The linearized Freundlich isotherm (Khenifi et al. 2007) is commonly expressed as in equation (5):

log q e = log K F + 1
n log c e (5)

where KF is the Freundlich constant. The slope, 1/n, which ranges in value between 0 and 1, is a
measure of the surface heterogeneity and the adsorption intensity. The lower the value of 1/n, the
more heterogeneous is the adsorption process. The values of KF and 1/n may be determined from
the linear plot of log qe versus log ce.
Table 1 lists the values of the parameters (qmax, KL, KF, n and R2) obtained from the application
of the Langmuir and Freundlich models to the experimental data obtained in the present study. It
will be seen from the data that the regression coefficient, R2, for the application of the Langmuir
isotherm model was higher than 0.99, whilst that for the application of the Freundlich isotherm
was only about 0.92. Figure 7 shows plots of qe versus ce, allowing a comparison of the
experimental data with the respective values of qe predicted by the Langmuir and Freundlich
isotherm equations. It is obvious from the data depicted that the adsorption process was better
described by the Langmuir model than the Freundlich model. This suggests that the adsorption
process may have been limited to monolayer coverage. This would accord with the view
expressed above that adsorption occurred because of the electrostatic interaction between AMNS
and ARS. The electrostatic field would be badly weakened if a monolayer of ARS formed on the
surface of AMNS, leading to the retardation of any further ARS adsorption. Furthermore, RL was
calculated as 0.048, implying that the adsorption of ARS onto AMNS was very favourable.

Adsorption kinetics

To determine the mechanism and effectiveness of the adsorption of ARS onto AMNS, a study of
the kinetics of the process was undertaken. Three kinetic models, i.e., the pseudo-first-order,
TABLE 1. Langmuir and Freundlich Model
Parameters for the Adsorption of ARS
onto AMNS

Parameters Magnitude

Langmuir
qmax (mg/g) 200
KL (
/mg) 0.04
RL 0.048
R2 0.9968
Freundlich
n 1.92
KF (mg/g) 16.2
R2 0.9197
Adsorption of Alizarin Red S onto Nano-sized Silica Modified with γ-Aminopropyltriethoxysilane 297

180

150

120

qe (mg/g) 90

60

30

0
0 20 40 60 80
ce (mg/ℓ)

Figure 7. Application of the Langmuir and Freundlich adsorption models to the experimental data obtained in the present
study for the adsorption of ARS onto AMNS. The various plots of qe versus ce correspond to the following: ,
experimental data; , application of Langmuir model; , application of Freundlich model.

pseudo-second-order and intra-particle diffusion models, were examined to see which provided
the best fit to the experimental data. The pseudo-first-order model may be expressed as in equation
(6) (Purkait et al. 2006):

= k1( q e − q t )
dq t (6)
dt

After integration applying the conditions that qt
0 at t
0 and qt
qt at t
t, equation (6)

becomes:

log ( q e − q t ) = log q e −
k1
t (7)
2.303

where k1 is the pseudo-first-order rate constant (min1) and qt is the amount of dye adsorbed at
time t (mg/g).
The pseudo-second-order model is based on the assumption that the rate-limiting step involves
chemisorption of the adsorbate onto the adsorbent. This may be expressed as in equation (8) (Ho
and McKay 1999), viz.:

= k 2( q e − q t )
dq t 2
(8)
dt

By integrating and applying the above conditions, equation (8) can be written as:

t 1 t
= 2
+ (9)
qt k 2q e qe
298 Deliang Li et al./Adsorption Science & Technology Vol. 29 No. 3 2011

The intra-particle diffusion model may be expressed as in equation (10) (Weber and Morris
1963):

q t = k i t 1/ 2 + C (10)

where ki is the intra-particle diffusion rate constant [mg/(g min1/2)] and C is a constant (mg/g). The
plot of the intra-particle diffusion model has the same general features, viz. an initial curved
portion, a linear portion and a final plateau. The parameters of this model are often calculated by
fitting the data corresponding to the linear portion.
By fitting the experimental data to the corresponding plots of log(qe – qt) versus t, t/qt versus t
and qt versus t1/2, the corresponding values of k1, k2, ki, qe, C and the regression coefficient (R2)
were calculated (see Table 2). As shown in this table, the pseudo-second-order model provided a
good value for R2, thereby indicating that the adsorption of ARS onto AMNS followed pseudo-
second-order kinetics. In addition, the value of qe arising from the application of the
pseudo-second-order model was calculated as 74.24 mg/g, which was close to the experimental
value of 74.20 mg/g. This result suggests that chemical adsorption was the rate-controlling step.
The value of C arising from the intra-particle diffusion model was not zero (68.8 mg/g), indicating
that intra-particle diffusion might not be the controlling step in the process (Gupta and
Bhattacharyya 2006).

Adsorption thermodynamics

The values of the thermodynamic parameters such as the Gibbs’ free energy (∆G0), the standard
enthalpy change (∆H0) and the standard entropy change (∆S0) were also examined in order to
provide a better understanding of the effect of temperature on the process. The magnitude of ∆G0
was obtained from equation (11), viz.:

∆G 0 = − RT ln K c (11)

TABLE 2. Kinetic Model Parameters for the

Adsorption of ARS onto AMNS
Parameters Magnitude

Pseudo-first-order
k1 (min1) 0.02303
qe (mg/g) 1.556
R2 0.9304

Pseudo-second-order
k2 [mg/(g min)] 0.0940
qe (mg/g) 74.24
R2 0.9999

Intra-particle diffusiona
ki [mg/(g min1/2)] 1.152
C (mg/g) 68.9
qe (mg/g) 74.36
R2 0.9041
a
Parameters calculated from the linear portion of the
plot of qt versus t1/2.
Adsorption of Alizarin Red S onto Nano-sized Silica Modified with γ-Aminopropyltriethoxysilane 299

TABLE 3. Thermodynamic Parameters for the Adsorption of ARS onto AMNS

∆G0 (kJ/mol) at ∆H0 ∆S0
(kJ/mol) [J/(mol K)]
288 K 293 K 298 K 303 K 308 K

–6.68 –5.23 –3.78 –2.34 –0.89 –90.05 –289.34

where Kc is the equilibrium constant, T is the absolute temperature (K), R is the universal gas
constant [8.314 J/(mol K)] and Kc is equal to the ratio of qe to ce, viz.:

qe
Kc = (12)
ce

The value of ∆G0 may also be determined using equation (13):

∆G 0 = ∆H 0 − T∆S0 (13)

Thus, calculating ∆G0 at various temperatures by the use of equations (11) and (12) would allow
the values of ∆H0 and ∆S0 to be obtained (Table 3). The values of ∆H0 and ∆S0 were 90.0 kJ/mol
and 289 J/(mol K), respectively, indicating the adsorption of ARS onto AMNS was exothermic
and that the randomness at the solid/solution interface was thereby reduced (Purkait et al. 2007).
At room temperature, ∆G0 was found to be negative, thereby indicating that the adsorption of ARS
onto AMNS was spontaneous. However, the value of |∆H0| was not much higher than that of
|T∆S0|, showing that the adsorption process was easily affected by temperature. This result
supports the possible recoveries of ARS and AMNS by changing the temperature of the system.

CONCLUSIONS

The adsorption of ARS from aqueous solution onto AMNS has been systematically investigated.
It was found that the adsorption was highly dependent on the various operational parameters
employed, such as the pH value, the adsorbent dosage, the initial ARS concentration, the contact
time and the temperature. The best initial pH value for the ARS solution was ca. 2.2. The
percentage removal of ARS increased with increasing contact time as well as increasing AMNS
dosage. The percentage removal of ARS attained a value of 89% after 2 min contact time and 97%
after 5 min contact time. Although the removal of ARS increased with increasing AMNS dosage,
the equilibrium adsorption capacity of AMNS for ARS decreased. The removal of ARS was
greater than 98% when the initial ARS concentration was in the range 250–1000 mg/
. Increasing
temperature was found to be disadvantageous towards the removal of ARS. The adsorption
process was better described by the Langmuir isotherm model, while the kinetics of the process
were well modelled by the pseudo-second-order rate expression. Thermodynamic analysis
supported the view that the adsorption was spontaneous and exothermic at room temperature. The
results of this investigation support the view that AMNS may be employed as an adsorbent
material for the removal of ARS from aqueous solutions. This should be useful in the design of an
adsorption approach towards the removal of ARS on an industrial basis.
300 Deliang Li et al./Adsorption Science & Technology Vol. 29 No. 3 2011

ACKNOWLEDGEMENTS

The authors are grateful to the Ministry of Science and Technology of P. R. China (Project of
“973’’ plan, Grant No. 2007CB607606) for financial support.

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