Journal of Hazardous Materials 175 (2010) 1106–1112

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Journal of Hazardous Materials

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Short communication

Removal of petroleum hydrocarbons from aqueous solution using sugarcane

bagasse as adsorbent
Poliana C. Brandão, Túlio C. Souza, Cíntia A. Ferreira, Carla E. Hori, Lucienne L. Romanielo ∗
Federal University of Uberlândia, Av. João Naves de Ávila, 2160, Bloco K, Campus Santa Mônica, CEP: 38400-902 Uberlândia, MG, Brazil

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

Article history: In the present work, the adsorption ability of sugarcane bagasse to remove oil by-products from aqueous
Received 22 March 2009 solution was evaluated. The objective was treating the contaminated wastewater while enriching the
Received in revised form 16 October 2009 bagasse for its later use as fuel in boilers. Adsorption experiments were carried out in an agitated reactor
Accepted 16 October 2009
at room temperature to obtain kinetic curves and adsorption isotherms of gasoline and n-heptane on
Available online 24 October 2009
sugarcane bagasse. The results showed the great potential of bagasse as an adsorbent, since it was able to
adsorb up to 99% of gasoline and 90% of n-heptane in solutions containing about 5% of these contaminants.
Keywords:
In the adsorption kinetics of gasoline, the equilibrium was reached after just 5 min. This result shows that
Adsorption isotherm
Petroleum Hydrocarbons removal
the adsorption is very favorable. Langmuir, Freundlich, Temkin and D-R models did not describe well the
Bioadsorbents adsorption behavior obtained for these systems.
Sugarcane bagasse © 2009 Elsevier B.V. All rights reserved.

1. Introduction Table 1 presents a brief literature review of sugarcane bagasse

During the last few decades, the scientific community has been
engaged to develop processes that avoid the release of pollutants
into bodies of water. Oil and its derivatives are some of the prod-
ucts with high polluting potentials, because besides being stable to
light and to heat, they are also very difficult to undergo biodegrada-
tion [1]. They decrease the contact area between water surface and
atmospheric air preventing oxygen transfer from occurring, besides
causing esthetical problems. Among the processes employed to
remove these pollutants, adsorption has drawn great attention,
especially processes which use low-cost adsorbing materials, such
as biomass [2,3]. The highly hydrophobic characteristic of biomass
combined with its high porosity, develop a capillary force towards
the adsorption of oils. Vegetal tissues, with large surface area and
big pores, tend to adsorb organic contaminants through physi-
cal and chemical mechanisms, in a similar way to charcoal [4–7].
Among the type of biomasses employed as adsorbents are sea
plants, cotton fibers, saw dust, corncob, coconut fibers, and sugar-
cane bagasse [2,8]. These materials can be used as a support for new
adsorbents as well as being used “in-nature”, representing thus a
great reduction in costs [9–11]. Several researchers, while studying
adsorption of oil by-products using different types of biomass, have
observed the promising character of these materials as adsorbents
[12].
∗ Corresponding author. Tel.: +55 34 3239 4292; fax: +55 34 3239 4188.
E-mail address: lucienne@ufu.br (L.L. Romanielo).
uses as adsorbent. It is interesting to notice that most of references
used modified sugarcane bagasse. Although it can be seen that mod-
ified bagasse is very efficient to adsorb a variety of compounds, the
pre-treatment can add important costs to the process. Therefore, in
this study, the capacity of “in-nature” sugarcane bagasse to remove
gasoline and n-heptane from aqueous solutions was evaluated.
Since Brazilian gasoline has a large amount of oxygenates com-
pounds, especially due to the addition of 25% of ethanol (the average
composition of the commercial Brazilian gasoline used in this work
is presented in Table 2), the treatment of gasoline contaminated
water can be particularly expensive. The adsorption experiments
were carried out in a glass agitated reactor at room temperature to
obtain the kinetic curves and the adsorption isotherms. Langmuir,
Freundlich, Temkin and D-R isotherms were used to correlate the
experimental data.
2. Experimental
2.1. Adsorbent characterization
Before the use in the adsorption experiments, sugarcane bagasse
was washed in tap water and then in distilled water to try to
avoid possible contaminants. After this, the bagasse was dried at
60 ◦ C and then grinded until achieving particle sizes smaller than
2 mm. After this stage, the physical and chemical characterization
of the adsorbent was carried out. The moisture content, ash con-
tent, volatile matter and fixed carbon were determined according to
Standard Methods. Surface area was determined using BET surface

0304-3894/$ – see front matter © 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.jhazmat.2009.10.060
 P.C. Brandão et al. / Journal of Hazardous Materials 175 (2010) 1106–1112 1107

Table 2
Nomenclature Commercial Brazilian gasoline composition.

Type of components Percentage

P adsorbate/adsorbent ratio (mL/g)
Aromatics 13.72 ± 1.30%
qcal adsorbed amount calculated in the equilibrium by
Isoparaffins 18.24 ± 2.05%
the model (mL/g) Naphthenes 10.93 ± 0.95%
qe experimental adsorbed amount in the equilibrium Olefins 19.50 ± 1.40%
(mL/g) Paraffins 9.90 ± 0.71%
Ceq concentration of adsorbate in equilibrium (mL/mL) Oxygenates (major ethanol) 25.21 ± 0.54%

qmax maximum capacity of adsorption (mL/g)
b Henry’s constant (g/mL)
K dimensionless parameter of Freundlich isotherm
A parameter of Temkin isotherm (mL/g)
B parameter of Temkin isotherm (mL/g)
ε Dubinin potential (mol/kJ)2
n parameter related to the solid heterogeneity in Fre-
undlich isotherm
Np number of experimental points
analyzer (Quantsorb Jr – QuantaChrome). In order to improve the
characterization, FTIR analysis was performed too. The sugarcane
bagasse, with diameter less then 0.297 mm, was mixed with KBr
powder and compressed to form a pellet. The FTIR spectra have
been recorded using a Bruker Equinox 55 with a spectral range
from 4000 cm−1 to 400 cm−1 . An MIR, GLOBAR generator cooled
with air was used. The detection was carried out with a DLATGS
detector with a KBr window. The spectral resolution was about
4 cm−1 .
2.2. Kinetic curves and adsorption isotherms
To simulate the wastewater contaminated by oil by-products,
commercial gasoline with 25% of ethanol was dispersed in water.
The adsorbent dose (10 g) and the stirring speed (400 rpm), were
chosen using the results obtained during preliminary tests. Each
experimental point was measured at least three times or until
the difference on the measured concentration was less than 10%.
Although the pH of the solution is an important variable in adsorp-
tion of ions, it is not so important in the adsorption of species
such as the hydrocarbons used in this work. Therefore, pH, was
not controlled. For all tests it did not varied significantly from
the initial value (pH 4.5). In order to verify if there was consider-
able hydrocarbons evaporation or sorption on the glassware during
the adsorption experiments, three “blank” runs were conducted.
In these tests, 250 mL of solution with different concentrations of
gasoline in water were placed in 600 mL beakers. The beakers were
sealed and then, subjected to agitation for 60 min. In the end of
each experiment, the samples were filtered under vacuum using
Values reported by Ré-Poppi et al. [19].
a number 2, Buchner funnel, sealed. The two phases were split
through decantation and the volumes were measured in a num-
ber two test tube. The results showed a difference of 2% between
the initial and final volumes of gasoline. The difference is proba-
bly due to evaporation, which is a very reasonable experimental
error.
The adsorption isotherms were obtained using a glass agi-
tated reactor at room temperature. 250 mL of water and 10 g of
sugarcane bagasse were placed in 600 mL beakers. After this, a
certain amount of contaminant was added to each beaker. The
beakers were sealed and then, subjected to agitation. Two adsor-
bate/adsorbent ratios were used to obtain the kinetic curves
of gasoline adsorption on sugarcane bagasse: 3.75 mL/g and
5.00 mL/g. For each of these ratios, the concentration of pollu-
tant in the water solution was measured after contact times of:
5 min, 15 min, 30 min, 45 min, 60 min and 90 min. In the end of
each experiment, the samples were filtered under vacuum using
a number 2, Buchner funnel, sealed. In some amounts of contam-
inant added, the filtrate presented two phases. In these cases, the
phases were split through decantation and the contaminant was
quantified through direct determination of volume in a number
two test tube. With this procedure, it was possible to deter-
mine by difference the amount of contaminant adsorbed on the
bagasse.
The equilibrium is considered achieved when the adsorbed
amount does not change with time of agitation. In this work,
the equilibrium was achieved for all ratios of pollutant/adsorbent
within 60 min. The ratios used in this study are presented in
Tables 3 and 4, for gasoline/bagasse and n-heptane/bagasse, respec-
tively.
2.3. Correlation of experimental results
The experimental results obtained were used in the thermody-
namic modeling of the adsorption process. A non-linear regression
of the results was carried out using the software program STATIS-
TICA. Version 5.1. The weighted least squares method was used as
a minimization criterion. For all of the models, the relative mean

Table 1
Literature references about use of sugarcane bagasse as an adsorbent.

Adsorbent Adsorbate pH Adsorption capacity (mg/g) Ref.

Treated sugarcane bagasse Pb(II) 5 227.7 [15]

Mercerized sugarcane bagasse Cu(II)Cd(II)Pb(II) 5.4 7.0 6.0 153.9 250 500 [7]
Mercerized sugarcane bagasse Ca(II) Mg(II) 5.5–10 5.5–9.0 46.4–54.1 23.5–42.6 [20]
Modified sugarcane bagasse Sulphate ions 10 38,400 [21]
Activated carbon prepared from sugarcane bagasse Phenol – 24.68 [22]
Activated carbons prepared from sugarcane bagasse pith Reactive dye 1 3.92 [3]
Chemically modified sugarcane bagasse Cu(II)Cd(II)Pb(II) 5.5–66.5–7.55–6 139 313 313 [23]
Activated carbons prepared from biomass Phenol 3–8 140 [8]
Sugarcane bagasse pith Cr(VI) 2 13.4 [24]
Sugarcane bagasse pith Cd(II) 6 6.75 [25]
Sugarcane bagasse pith Ni(II) 6.5 26.3 [26]
Sugarcane bagasse pith Cr(VI) 2 5.75 [27]
Modified sugarcane bagasse Cr(VI) 3 103 [28]
Bagasse fly ash DDD, DDE 7 0.00769 [16]
1108 P.C. Brandão et al. / Journal of Hazardous Materials 175 (2010) 1106–1112

Table 3
Gasoline/bagasse ratios used in adsorption experiments.

Contaminant/ Initial volume of Contaminant/water Concentration of contaminant

bagasse ratio, P (mL/g) contaminant, Vinitial (mL) ratios (mL/mL) in the effluent (%)

1.50 15.0 0.06 5.66

2.00 20.0 0.08 7.41
2.50 25.0 0.10 9.09
3.30 33.0 0.13 11.66
3.75 37.5 0.15 13.04
5.00 50.0 0.20 16.67
6.00 60.0 0.24 19.35
7.50 75.0 0.30 23.08
9.00 90.0 0.36 26.47
10.00 100.0 0.40 28.57
15.00 150.0 0.60 37.50
20.00 200.0 0.80 44.44
25.00 250.0 1.00 50.00

Table 4
n-Heptano/bagasse ratios used in adsorption experiments.

Contaminant/ Initial volume of Contaminant/water Concentration of contaminant

bagasse ratio, P (mL/g) contaminant, Vinitial (mL) ratios (mL/mL) in the effluent (%)

1.50 15.0 0.06 5.66

2.50 25.0 0.10 9.09
3.75 37.5 0.15 13.04
5.00 50.0 0.20 16.67
6.00 60.0 0.24 19.35
7.50 75.0 0.30 23.08

deviation (DMR) (%) was calculated, according to Eq. (1): 2.4. Evaluation of superior calorific value
n  
qcal − qe  /qe In order to verify if the hydrocarbon remained in the bagasse
i=1 i i i
DMR = (1) after the adsorption process, experiments tests to evaluate the
Np
superior calorific value were performed before adsorption and 1
where qcal and qe are amounts adsorbed in the equilibrium calcu- week after adsorption. The sugarcane bagasse containing gaso-
lated by the model and measured experimentally respectively, and line was retrieved after an adsorption experiment conducted with
Np is the number of experimental points used. 250 mL of water, 50 mL of gasoline and 10 g of bagasse. The tests
The models tested were Langmuir (Eq. (2)), Freundlich (Eq. were conducted according Brazilian rules (ABNT NBR 8633/84).
(3)), Temkin (Eq. (4)) and Dubinin–Radushkevich (D-R, Eq. (5))
isotherms since they are the models most often mentioned in the 3. Results and discussion
literature to describe adsorption processes in liquid phase. In Eqs.
(2)–(5) Ceq is the concentration of adsorbate in equilibrium (mL/mL) The characterization of “in-nature” sugarcane bagasse is pre-
and qeq is the adsorbed amount per gram of adsorbent (mL/g) in the sented in Table 5. The values of moisture content and ash content
equilibrium. are in agreement with that reported in literature [15], as well as,
the values found for volatile matter and fixed carbon, reported
qmax bCeq
qeq = (2) by Brazilian Industry of Ethanol. However, the value of surface
1 + bCeq
area is different from those reported in the literature [15–17].
1/n This is probably due to the fact that the sugarcane bagasse used
qeq = KCeq (3) in this work was “in-nature” rather than pretreated or activated
materials which, of course, presented higher values for the surface
qeq = A + B ln(Ceq ) (4)
area.
Fig. 1 shows the FTIR spectrum from untreated sugar cane
qeq = qmax exp(−kε) (5)
bagasse. The result is in agreement with that reported in the lit-
In the Langmuir isotherm (Eq. (2)), qmax is a parameter related to
the maximum capacity of adsorption and b is the Henry’s constant, Table 5
parameter related to the force between adsorbate and adsorbent. Physical and chemical characterization of the
The parameter K of the Freundlich isotherm (Eq. (3)) is associated adsorbent.
to the adsorption capacity and the parameter n is related to the Contents Results
solid heterogeneity. The Temkin isotherm (Eq. (4)) assumes that
Moisture (%) 8.1 ± 0.1
the fall in the heat of adsorption is linear rather than logarithmic,
Ashes (%) 1.3 ± 0.1
as implied in the Freundlich equation. A and B are Temkin constants. Volatile matter (%) 88.6 ± 1.7
In Eq. (5), D-R isotherm, ε(RT ln(1 + 1/Ceq )) is the Polanyi potential, Fixed carbona (%) 1.9
qmax (mL/g) is the adsorption capacity, and k (mol2 /kJ2 ) is a constant Surface area 40 m2 /g
related to the adsorption energy when it is transferred to the surface a
Fixed carbon (%) = 100 − moisture (%) −
of the solid from infinity in the solution. volatile matter (%) − ashes (%).
 P.C. Brandão et al. / Journal of Hazardous Materials 175 (2010) 1106–1112
Fig. 1. FTIR spectra of “in-nature” sugarcane bagasse.
Table 6
Superior calorific value of sugarcane bagasse.
Type of bagasse Superior calorific
value (kJ/g)
“in-nature” 29.14
1 week after adsorption 33.98
erature for sugarcane bagasse untreated [18]. The strong signal
at 3400 cm−1 is typical from cellulose and the reasonable defined
shoulder at 3250 cm−1 is related to hemi-cellulose. The medium
signal, between 1500 cm−1 and 1750 cm−1 , is due to the carboxylic
groups, present in lignin and hemi-cellulose. This is consistent with
the nature of Brazilian sugarcane bagasse that is composed by 49.1%
of cellulose, 20.3% of lignin, 27.8% of hemi-cellulose and 1.6% of
ashes.
In order to verify if the hydrocarbons adsorbed remained in
the solid, measurements of superior calorific values of the sug-
arcane bagasse were conducted before and 1 week after the
adsorption. The results are presented in Table 6. It can be notice
that there was an improvement of the superior calorific value
of bagasse by the adsorption of gasoline. Therefore, even after
a week following the adsorption, there was still gasoline left in
Fig. 2. Final volume of solute in water after the adsorption of gasoline on sugarcane
bagasse at room temperature as a function of contact time.
1109
Fig. 3. Adsorbed amount of gasoline on sugarcane bagasse at room temperature
versus time.
the sugarcane bagasse enough to improve its superior calorific
value.
Fig. 2 shows the influence of contact times between the phases
on the final amount of gasoline left in the liquid phase. Fig. 3
presents the kinetic curves of adsorption expressed in terms of
adsorbed gasoline per gram of bagasse. The kinetic curves are
slightly changed by the initial ratio of gasoline/bagasse. For the
ratio P = 3.75 mL/g, the equilibrium was reached after 60 min and
85% of the initial gasoline was adsorbed during the first 5 min.
Therefore, there was a very small variation on the adsorbed
volume between 5 min and 60 min, around 3 mL. For the ratio
P = 5 mL/g, an average value of 8.5 mL of gasoline was detected
in the solution between the times of 3 min and 60 min. This
corresponds to an adsorption percentage of 83% and a capacity
of adsorption of 4.15 mL/g. Therefore, it can be concluded that
the adsorption kinetics of gasoline on sugarcane bagasse is very
fast.
Fig. 4 shows the percentage of pollutant adsorbed (Pads ) on
sugarcane bagasse, at room temperature, versus the initial con-
centration of pollutant in aqueous solution. It can be observed
that sugarcane bagasse is able to adsorb up to 99% of gasoline
and 90% of n-heptane in aqueous solutions containing around of
5% of these contaminants. For higher concentrations, that could
Fig. 4. Percentage of pollutant adsorbed as a function of initial concentration of
pollutant in aqueous solution.
1110 P.C. Brandão et al. / Journal of Hazardous Materials 175 (2010) 1106–1112

Fig. 5. Adsorption isotherm of gasoline on sugarcane bagasse at room temperature.

occur due to an accidental spilling of these products, sugarcane
bagasse was able to adsorb up to 48% of gasoline and 30% of n-
heptane in aqueous solution with 50% e 23% of these pollutants,
respectively.
The adsorption isotherms of gasoline on sugarcane bagasse
at room temperature are presented in Fig. 5. Experimental data
are presented along with the results of the correlation obtained
through the isotherms of Langmuir, Freundlich, Temkin and D-R.
The shape of the isotherm is an example of a common behavior in
physic adsorption with strong interaction forces between adsor-
bate and adsorbent, observed in solids with a wide range of pore
sizes distribution. The first points are characteristic of a concave
favorable isotherm such as a Langmuir isotherm. This kind of shape
is named class L [13]. For this class of isotherm, large amounts can
be adsorbed at low concentrations of solute. This was observed by
the high percentage of adsorbed gasoline in this region. According
to Giles et al. [13], there are few sub-groups of this class of isotherm
(named by the authors as sub-groups 1, 2, 3, 4 and mx). One of them
fits the observed behavior, the class L, sub-group 3. The inflection
in the isotherm is due to the formation of a monolayer. From this
point, the adsorption continues in multi-layers and the intensity of
the interaction forces between adsorbate and adsorbent are much
lower. This can be confirmed by smaller inclination of the curve
Fig. 6. Adsorption isotherm of n-heptane on sugarcane bagasse at room tempera-
ture.
and the smaller percentages of adsorbed gasoline in the final range.
Similar adsorption isotherm behavior using sugarcane bagasse was
already reported in the literature during the adsorption of Pb(II)
ions [15].
Fig. 6 presents the adsorption isotherms of n-heptane on sugar-
cane bagasse at room temperature (experimental data and fitting of
the isotherms of Langmuir and Freundlich). The general shape of the
experimental n-heptane adsorption isotherm obtained in this work
is not very common. In fact, the maximum point observed is very
atypical. For that reason, this experimental point was repeated five
times, with a maximum difference between the points less than 7%.
Looking for similar results in the literature, we could find only two
references. One of them is presented by apud Gregg and Sing [14],
which reported this kind of behavior and classified it as class L, sub-
group mx, according to their classification of liquid isotherms. The
first points are characteristic of concave favorable isotherms with
high percentages of adsorbed n-heptane (as all class L isotherms).
After the monolayer formation, the adsorption takes place in multi-
layers. At higher contaminant concentrations, there is a decrease
on the amount adsorbed. One hypothesis to explain this behavior
is the possibility that the solute molecules themselves may be clus-
tered into micelles at higher pollutant concentrations making the

Table 7
Parameters of the isotherms tested in this work, with respective correlation coefficients (R2 ) and mean relative devia-
tions (MRD).

Isotherm System

Water/gasoline Water/heptane

qmax (mL/g) 8.3604 2.7771

b (mL/mL) 60.7344 266.4997
Langmuir
R2 0.85358 0.58995
MRD (%) 25.3 19.06

K 14.9450 3.4663
1/n 0.3431 0.1250
Freundlich
R2 0.96176 0.51071
MRD (%) 12.6 20.3

qmax (mL/g) 10.99164 3.0595

k (mol2 /kJ2 ) 0.2658 0.0051
Dubinin–Radushkevich (D-R)
R2 0.9603 0.4805
MRD (%) 21.1 16.7

A (mL/g) 10.60758 3.28293

B (mL/g) 1.45493 0.20404
Temkin
R2 0.88587 0.4241
MRD (%) 30.1 19.98
 P.C. Brandão et al. / Journal of Hazardous Materials 175 (2010) 1106–1112
adsorption process more difficult in some of the adsorbent pores by
size exclusion. This probably happens because n-heptane is more
hydrophobic than the Brazilian commercial gasoline, which has 25%
of ethanol in its composition. The presence of ethanol increases
a lot the solubility of hydrocarbons in water. For example, the
activity coefficient of heptane in water in infinite dilution (i∞ ) eval-
uated by UNIFAC model is 33535.04, however this value, i∞ , in a
mixture with 25% of ethanol in water decreases to 112.88, show-
ing the increases of solubility of heptane in a water solution with
ethanol.
All the isotherms fitted well the experimental data of gaso-
line adsorption when the contaminant concentration present in
the aqueous solution was low, until the beginning of the mono-
layer formation. However, for concentrations higher than 0.04 mL
of gasoline/mL of solution the errors observed between the experi-
mental and correlated data increased. This behavior was already
expected for the Langmuir model since it limits the adsorbed
amount to the formation of the monolayer. For this reason it
does not represent well the adsorption on solids with a wide
pore size distribution, which often present multilayer adsorp-
tion, such as class L, sub-groups 2, 3, 4 and mx, from the Giles
et al. classification [13]. The Freundlich isotherm presented the
best performance in the description of the gasoline adsorption
compared to others isotherms tested. This can be attributed
to the fact that the Freundlich isotherm considers the hetero-
geneity of the solid and does not limit the amount adsorbed
to the monolayer. Nevertheless, the performance is not satis-
factory for the whole concentration range. For higher pollutant
concentrations, D-R and Temkin isotherms present better per-
formances than Langmuir and worse than Freundlich. The same
discussion made for gasoline can be applied to n-heptane. How-
ever, for n-heptane, the fit for all isotherms tested was very
poor, which can be confirmed by the small correlation coefficient
obtained.
Table 7 presents the values of the parameters obtained by the fit
of the experimental data with the correspondent correlation coeffi-
cient (R2 ) and the mean relative deviations (MRD), for all isotherms
used: Langmuir, Freundlich, D-R and Temkin. The values of adsorp-
tion capacity around 7 g/g for gasoline and 2 g/g for heptane show
that sugarcane bagasse has a great potential to remove hydro-
carbons from aqueous solutions. The results also show that the
presence of ethanol in gasoline improves the adsorption capacity
of the sugarcane bagasse.
4. Conclusions
Based on the results shown it can be concluded that the
kinetics of adsorption of gasoline in aqueous solution using sug-
arcane bagasse, at room temperature, is very fast. The shape of
the isotherm for the gasoline adsorption in aqueous solution is
characteristic of favorable type in multilayer adsorption: class L,
sub-group 3, according the classification of liquid isotherms pro-
posed by Giles et al. [13]. Also the adsorption of n-heptane is very
favorable at low concentrations of this pollutant in aqueous solu-
tions. However, for higher concentrations of n-heptane, the amount
adsorbed decreases. This atypical behavior fits the class L, sub-
group mx of the Giles et al. classification. The Langmuir, Freundlich,
Temkin and D-R isotherm models do not present a good perfor-
mance in the fitting of the experimental data, especially for high
concentrations of pollutant. However, all models can be used for
low concentrations. Fortunately, this is the region with the more
usual concentration in the industrial water disposal effluents. The
results also indicate that the use of the sugarcane bagasse as adsor-
bent of non-polar substances such as gasoline and n-heptane is very
favorable.
1111
Acknowledgments
The authors thank CNPq for the financial support and to
MEC/SESu for the scholarship of Túlio C. Souza, student of the PET
program.
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