Application of Modified Bagasse as a Biosorbent for Reactive Dyes Removal from Industrial Wastewater

doi:10.4236/jwarp.2013.57A003

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Journal of Water Resource and Protection, 2013, 5, 10-17

http://dx.doi.org/10.4236/jwarp.2013.57A003 Published Online July 2013 (http://www.scirp.org/journal/jwarp)

Application of Modified Bagasse as a Biosorbent for

Reactive Dyes Removal from Industrial Wastewater

Abd El-Aziz A. Said1*, Aref A. M. Aly1, Mohamed M. Abd El-Wahab1, Soliman A. Soliman1,

Aly A. Abd El-Hafez1, V. Helmey2, Mohamed N. Goda1

1Chemistry Department, Faculty of Science, Assiut University, Assiut, Egypt

2 Mechanical Engineering Department, Faculty of Engineering, Assiut University, Assiut, Egypt

Email: *[email protected]

Received April 15, 2013; revised May 18, 2013; accepted June 25, 2013

cense, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

ABSTRACT

Propionic acid modified bagasse was used for the removal of reactive yellow 2 and reactive blue 4. The effects of pH,

contact time, initial dye concentrations, adsorbent particle size and adsorbent dose on the adsorption of the two dyes

were investigated. Additionally, the desorption process and intra-particle diffusion were studied. Acidic pH values were

favorable for adsorption of both dyes. The equilibrium adsorption data were best fitted with the Freundlich isotherm for

reactive yellow 2 and the Langmiur isotherm for reactive blue 4. The values of their corresponding constants were de-

termined. The kinetic for dye adsorption is well described by a pseudo-first order kinetic model for the reactive yellow

2 and by pseudo-second order for the reactive blue 4. The investigation revealed that the hydroxyl groups of bagasse

and the carboxylic group of propionic acid play a great role in the removal of both reactive dyes.

Keywords: Modified Bagasse; Reactive Yellow 2; Reactive Blue 4; Adsorption; Kinetics

1. Introduction

Dyes are widely used in many industries such as textile,

plastic, paper, food and cosmetic for coloring their prod-

ucts. These dyes are water pollutants and cause environ-

mental hazards. In addition, many dyes are difficult to be

biodegradable and tend to persist in the environment cre-

ating serious water quality and public health problems.

So, a conventional biological treatment process is not

very effective in treating dyes wastewater. There are

various methods for removing dyes including coagula-

tion and flocculation [1], oxidation or ozonation [2] and

membrane separation [3]. However, these processes are

very expensive and cannot be effectively used to treat the

wide range of dyes waste. Alternative methods include

adsorption on natural biosorbents which are becoming

now of high interest for removal of dyes from waste ef-

fluents. In this way several studies have used natural ma-

terials locally available, renewable and of low costs [4-6].

Among these sorbents are banana, bagasse, coir pith,

palm-fruit bunch, apple-pomace, wheat straw, rice husk,

pine sawdust, peanut hull, coffee husk, maize cob, or-

ange peel, sugar cane dust and luffa fiber [7-9].

Recently, sugarcane bagasse was used as potential low-

cost adsorbent for removal of many dyes from wastewater

[10-14].

Reactive dyes are generally used for colouring cotton

and other cellulosic material, but are also applied to a

small extent on wool and nylon. In the present study re-

moval of reactive yellow 2 and reactive blue 4 from

aqueous solutions using bagasse pre-treated with propi-

onic acid was investigated. Several parameters have been

studied such as pH, contact time, biomass dosage, and

particle size and desorption process. The equilibrium

sorption capacity and the kinetic adsorption of both dyes

on the modified bagasse were studied. The selection of

bagasse for this study was based on low cost raw mate-

rial and environmental impact.

2. Materials and Methods

Reactive yellow 2 and reactive blue 4 dyes were pur-

chased from Sigma-Aldrish Chemical Co. The chemical

structures of the two dyes are presented in Figure 1.

2.1. Preparation of Adsorbent

Sugar cane bagasse modified with propionic acid was

previously described [13].

*Corresponding author.

A. E.-A. A. SAID ET AL. 11

(a)

(b)

Figure 1. Chemical structures of reactive yellow 2(a) and

reactive blue 4(b).

2.2. Preparation of Aqueous Dye Solution

Stock solutions of the two dyes were prepared by dis-

solving accurately a weighed amount of each dye in dis-

tilled water (1000 mg/L) and diluting these solutions

prior to performing the adsorption experiments.

2.3. Adsorption Experiment

In each adsorption experiment 50 mL of dye solution of

known concentration and pH was added to known weight

of adsorbent in 100 mL airtight volumetric flasks at room

temperature (27˚C ± 1˚C) and the mixture was stirred on

a rotary orbital Shaker at 150 rpm. The dye solution was

filtered from bagasse and determined spectrophotometri-

cally by recording the absorbance changes at maximum

absorption (405 nm for reactive yellow 2 and 595 nm for

reactive blue 4) using Thermofischer Scientific, aqua

mate, Evolution 166 Uv-visible spectrophotometer. All

pH measurements were carried out with a pH-meter

model number JENWAY 3450. The initial pH values

were adjusted with 0.1 M HCl or NaOH to form series of

pH’s. Effect of adsorbent dosage was studied with dif-

ferent adsorbent doses and 50 ml of the dye solution at

equilibrium time. For the desorption studies the adsorb-

ent used for the adsorption of the dye solution was thor-

oughly washed with distilled water to remove unad-

sorbed dye and desorption process was conducted at a

range of pH values. The amount of dye adsorbed onto the

bagasse, qe (mg/g) was calculated as the following equa-

tion:



eie

CVWqC (1)

where Ci and Ce are the initial and equilibrium time solu-

tion concentration of the dye (mg/L) , respectively, V the

volume of the solution (L) and W the dry weight of the

sorbent (g).

2.4. Kinetic Studies

To assess the applicability of the adsorption process it is

necessary to determine the kinetic parameters, using the

batch technique. A series of volumetric flasks containing

100 mL capacity, containing 50 mL dye solutions of

known concentrations at the appropriate pH and were

agitated by mechanical shaker at room temperature. After

a definite time interval, the solutions were filtered and

the filtrates thus obtained were then analyzed spectro-

photometrically. All the experiments were duplicated and

only the mean values are reported. The maximum devia-

tion observed was less than ±5%.

2.5. Thermal Studies

Thermogravimetric analysis TGA and differential ther-

mal analysis DTA techniques of original and treated with

propionic acid (5 wt%) were carried out using a Shima-

dzu Thermal Analyzer model (TG 60 H). Curves of TGA

and DTA were recorded upon heating up to 600˚C at

10˚C·min −1 and flow of air of 30 mL·min−1.

3. Results and Discussion

3.1. Characteristics of Dyes

Table 1 summarizes some important characteristics of

reactive yellow 2 and reactive blue 4 dyes.

3.2. Thermal Analysis

Figure 2(a) shows that the decomposition of untreated

bagasse proceeds in five stages. The first region of (36˚C -

124˚C) which accompanied with 5.3% weight loss with an

endothermic peak minimized at 77˚C is attributed to the

physically adsorbed water. The second stage of (125˚C -

208˚C) which accompanied with 8.1% weight loss is due

to the dehydration water. The major weight loss (53.2%)

takes place within (209˚C - 358˚C) range which exhibit

exothermic peak maximized at 316˚C. This peak is cor-

responded to the decomposition of cellulose and hemi-

celluloses in bagasse [14]. The fourth stage of (359˚C -

459˚C) and with exothermic peak maximized at 426˚C

and the fifth region of (462˚C - 600˚C) which accompa-

nied with 4% weight loss with exothermic peak maxi-

mized at 480˚C are attributed to the decomposition of

lignin component of bagasse [14]. The TGA and DTA

curves of treated bagasse with 5 wt% propionic acid was

carried out and presented in Figure 2(b) and the data are

cited in Table 2, it shows that the thermal decomposition

of treated bagses proceeds in similar behaviour of un-

treated bagasse i.e., takes place in five stages. It is clear

from the DTA curve and the data depicted in Table 2 that

the addition of propionic acid retards the third decompo-

A. E.-A. A. SAID ET AL.

JWARP

Table 1. Characteristics of the used reactive dyes.

No. of functional groups available for interaction

Dye λmax (nm) C(wt%)

No. of ionizable

groups −SO −C=O −NH −Cl −NH2

Reactive yellow 2 404 34.5 3 9 1 2 3 -

Reactive blue 4 595 35 2 6 2 2 2 1

Table 2. Data for thermal decomposition of untreated and treated bagasse.

Temperature range (˚C) and weight loss (%)

Adsorbent 1st stage 2nd stage 3rd stage 4th stage 5th stage

Total weight loss

(%)

36 - 124 125 - 208 209 - 358 359 - 459 462 - 600

Original bagasse 5.3 8.1 53.2 21.1 4.0

91.7

36 - 123 124 - 231 232 - 357 358 - 439 440 - 600

Treated bagasse 3.7 11.5 54.7 24.1 2.6

96.6

sition step while enhances the fourth and fifth decompo-

sition stages. This reflects that the presence of propionic

acid strongly affected the structure of bagasse, i.e., a good

interaction between bagasse and propionic acid. So, the

results of thermal analysis indicated that propionic acid

should affect the physico-chemical properties of bagasse.

3.3. Effect of pH

The pH of the dye solution has a great influence on the

adsorption of the dye on the biosorbent presumably due

to the effect on the surface properties of the adsorbent

and ionization or dissociation of the dye molecules. Fig-

ure 3 represents the effect of pH on the removal of both

dyes. The highest dye removal efficiency was observed

at pH = 1.9 and pH = 2.1 for reactive yellow 2 and reac-

tive blue 4, respectively.

These acidic pH values might correspond to the rate of

dissociation of the sulphonic acid groups located on the

dyes. Furthermore, it is assumed that under acidic condi-

tions the hydroxyl groups of bagasse and the carboxylic

group of propionic acid are protonated i.e., 2



50100 150 200 250 300 350 400 450 500 550 600

100

and

–COOH2+. Thus a significant electrostatic interaction

may occur between the positively charged sites of the

adsorbent and the negatively charged part of the two re-

active dyes (sulphonate groups) [15]. The lower adsorp-

tion of both dyes at alkaline pH values may be due to the

presence of excess OH− ions competing with the dye

anions for the adsorption sites.

100

3.4. Effect of Agitation Time and Initial Dye

Concentration

The relation between removal of both dyes and the contact

time was studied and the results are shown in Figure 4. It

appears that removal of both dyes was rapid in the initial

stages and then steadily increases with increasing time.

Temper ature (oC)

Weight loss (%)

(a)

(b)

TExo

Endo

Figure 2. TGA and DTA curves of (a) untreated bagasse and

(b) bagasse treated with 5 wt% propionic acid.

The rapid removal at the initial contact time may be as-

cribed to the availability of high positive charges on the

bagasse surface for adsorption of the anionic reactive dyes.

The subsequent slow adsorption of the two dyes is pre-

sumably correlated with the electrostatic repulsion be-

tween the adsorbed species onto the bagasse surface and

the negative charge adsorbate species existing in the so-

lution besides the slow pore diffusion of the dye into the

bulk of the adsorbent [16]. Figure 5 shows the influence

of the initial concentration of both dye solutions on the

A. E.-A. A. SAID ET AL. 13

Figure 3. Effect of pH on dye removal, (1 g of 1 mm particle

size).

Figure 4. Effect of agitation time on dye removal.

0100 200 300

100

120

140

160

180

200

400 500

Reactive blue 4

Reactive yellow 2

Adsorption capacity (mg/g)

Dye concentration (mg/L)

Figure 5. Effect of initial dye concentration on dye removal.

adsorption dynamics by bagasse treated with propionic

acid. Upon raising the initial dye concentration of the

reactive yellow 2 from 50 to 500 mg/L the adsorbent

capacity increased from 12.5 to 180 mg/g whereas for

reactive blue 4 the capacity increases from 20 to 200

mg/g when the initial dye concentration increased from

25 to 500 mg/L.

3.5. Effect of Sorbent Particle Size

The effect of particle size on the adsorption of the two

dyes onto the modified bagasse was studied (Figure 6),

using a fixed sorbent dose (25 mg/50 ml). Different par-

ticle sizes range i.e., 0.25, 0.5, 0.71 and 1 mm were

adopted. The results reveal that the percentage removal

of the dyes increases with the decrease in bagasse parti-

cle size. Clearly a decrease in particle size would in-

crease the surface area and consequently an increase in

dye adsorption onto the bagasse surface occurs. Various

factors are responsible for the low adsorption capacity of

the dyes on the sorbent large particles. Among them are

the diffusional path length or mass transfer resistance,

contact time and blockage sections of the particles (not

utilized for adsorption) [17].

3.6. Effect of Sorbent Dosage

The effect of adsorbent mass on the adsorption of the two

dyes was investigated on treated bagasse of 1 mm parti-

cle size at initial dye concentration of 500 mg/L. Figure

7 depicts the expected pattern for both dyes where the

percent removal of each dye increases as the adsorbent

dosage increases. This may be attributed to the increase

in surface area of bagasse and availability of adsorption

sites for the two reactive dyes. However, the adsorption

density, the amount adsorbed by unit mass, decreases.

This may be due to unsaturation of adsorption sites or

Figure 6. Effect of sorbent particle size on dye removal.

A. E.-A. A. SAID ET AL.

Figure 7. Effect of bagasse dosage on dye removal.

due to some sort of particle interaction such as aggrega-

tion which will decrease the total surface area of adsorb-

ent and consequently an increase in the diffusion path

length [18]. It is clear from the obtained results that the

removal of reactive blue 4 is more pronounced relative to

that of reactive yellow 2 upon increasing of the bagasse

weight above 1 gm.

3.7. Adsorption Isotherms

The adsorption isotherms are important to optimize the

design of an adsorption system to remove the dye. The

parameters obtained from the different isotherms provide

important information about the adsorption mechanisms

and surface properties. The most widely accepted surface

adsorption models are those of Freundlich and Langmuir.

3.7.1. Freundlic h Isotherm

Freundlich isotherm is expressed as.

eFe

qKC (2)

where qe (mg/g) is the amount of dye adsorbed at equi-

librium, Ce (mg/L) is the equilibrium liquid-phase con-

centration of the dye and KF is a constant related to the

bonding energy and adsorption capacity. 1/n indicates the

adsorption intensity of dye onto the adsorbent and the type

of isotherm to be irreversible (1/n = 0), favorable (0 < 1/n

< 1) and unfavorable (1/n < 1).

Equation (2) can be arranged to a linear form:



1log e

1.5 1.6 1.7 1.8 1.9 2.0 2.12.2 2.3

0.0

0.2

0.4

0.6

0.8

1.0

1.2

og qe

log C

log log

qK (3)

To study the applicability of the Freundlich equation

for dye absorption onto bagasse a linear plot of log qe

versus log Ce is plotted and presented in Figure 8 and the

calculated parameters for Freundlich linear equation are

shown in Table 3. The reactive yellow 2 adsorption by

Figure 8. Freundlich isotherm for the sorption of reactive

yellow 2 at pH 1.9.

Table 3. Langmiur and Freundlic h isotherm parameters for

reactive yellow 2 and reactive blue 4 on modified bagasse.

Freundlich

Dye

R2 KF 1/n

Reactive yellow 20.9916 0.0045 1.5439

Reactive blue 4- - -

Langmuir

Dye

R2 Qm(mg/g) a(L/mg)

Reactive yellow 2- - -

Reactive blue 40.9956 13.2 0.052

modified bagasse fitted the Freundlich model well with R2

= 0.9916. The linear plot suggests the applicability of the

Freundlich equation. The 1/n is lower than 1.0, indicating

that reactive yellow 2 is favorably adsorbed by the pre-

treated bagasse. On the other hand the linear plot of the

Freundlich equation is not valid for reactive blue 4.

3.7.2. Langmiur Isotherm

The Langmiur equation is expressed as follows:



eme e

qaQC aC (4)

where qe and Ce are defined as in Freundlich equation, Qm

is the maximum adsorption capacity and a is the Langmiur

constant. Its linear form is expressed as:



eeme m

CqaQ CQ (5)

The Qm and a values can be obtained from the slope

(1/Qm) and the intercept (1/a Qm) of the linear plot Ce/qe

versus Ce. Figure 8 illustrates the linear form of Langmuir

isotherm of the reactive blue 4 and the calculated pa-

A. E.-A. A. SAID ET AL. 15

rameters are included in Table 3. It is clear from Figure 9

that the adsorption of the reactive blue 4 fits very well the

Langmuir equation with R2 = 0.9956 while the data do not

fit with the Freundlich equation .

0 10203040

0.6

0.7

0.8

0.9

1.0

3.8. Adsorption Kinetics

log (qe-qt)

time (min)

0 1020304050607080

0.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

4.0

In order to investigate the adsorption process of the reac-

tive dyes by pretreated bagasse, pseudo-first order (Equa-

tion (6)) and pseudo-second order (Equation (7)) kinetic

models were used.



12.303

qktlog log

qq (6)

And

h tq



140 160

tq (7)

where qe is the amount of dye sorbed at equilibrium (mg/

g), qt is the amount of dye sorbed at time t (mg/g), k1 is the

rate constant of the pseudo-first order sorption (min−1), h

2e is the initial adsorption rate (mg/g·min) and k2 is

the rate constant of pseudo-second order kinetics (mg/g

min). Fi gure 10 shows that the pseudo first order equation

fits well for the adsorption of reactive yellow 2 whereas

the pseudo-second order equation is not valid. Moreover,

the correlation coefficient R2 and K1 were calculated from

the intercept and slope respectively and presented in Ta-

ble 4. The linear plot of t/qt versus t for reactive blue 4

shows a good linear relationship, Figure 11. On the other

hand the applicability of the pseudo-first order equation

on the adsorption of reactive blue 4 was found not appli-

cable. The correlation coefficient R2 and K2 were calcu-

lated from the intercept and the slope respectively and

recorded in Table 4.

From Table 4, the correlation coefficients for the first

and second order kinetic models are greater than 0.99

which led to believe that the first and second order equa-

020 40 60 80100120

Ce/qe (g/L)

Ce (mg/L)

Figure 9. Linear f orm o f th e Langmuir is oth erm for re a ctive

blue 4 at pH 2.1.

Figure 10. Pseudo-first order plot for the desorption of re-

active yellow 2 at pH 1.9.

t (min g/mg)

time (min)

Figure 11. Pseudo-second order plot for adsorption of reac-

tive blue 4 at pH 2.1.

Table 4. Comparison of the first and second order adsorp-

tion rate constants and the correlation coefficients.

Pseudo-first order Pseudo-second

order

Dye

R2 K

1 (min−1) R2 K2

(g·mg−1·min−1)

Reactive

yellow 2

0.9945

0.0248

Reactive blue

4 - - 0.9950 0.0106

tions provided good correlations for the biosorption of

reactive yellow 2 and reactive blue 4 respectively, on

modified bagasse.

3.9. Intra-Particle Diffusion

The intra-particle diffusion model was applied to test the

A. E.-A. A. SAID ET AL.

possibility of intra-particle diffusion of reactive yellow 2

and reactive blue 4 into pre-treated bagasse. The adsorp-

tion process involves a transport of solute from the

aqueous phase to the surface of the solid particles with a

subsequent diffusion of the dye molecules into the inte-

rior pores which is a slow process and is therefore, a rate

determining step. The particle diffusion model is ex-

pressed by the following equation [19]:

qKt C

246810

(8)

where C (mg/g) is the intercept and Kd is the intra-parti-

cle diffusion rate constant (mg/g·min−1/2). Two intersect-

ing linear plots are obtained for both dyes indicating dif-

fusion of the dye molecules into macro- and micropores

of bagasse. If the mechanism of adsorption follows on

intra-particle diffusion process, the plot of qt versus t1/2

should be straight line and pass through origin. Figure

12 shows that there are two separate regions that repre-

sent the steps involved during the process of adsorption.

The initial straight line is due to the bulk diffusion while

the second straight line corresponds to the intra-particle

diffusion for both dyes. The plots were not best-fit

straight lines passing through the origin. This phenome-

non indicates that there is a boundary layer resistance.

One of the possible reasons for the deviation of the

straight line from the origin is that there is a difference in

the rate of mass transfer in the initial and final stages of

dye adsorption. The results of the experiment suggest

that the intra-particle diffusion is not the only step con-

trolling adsorption of the two dyes [20].

3.10. Desorption and Reuse

A further goal of any adsorbent used is reuse potential.

So, before the investigation of reuse, the adsorption ex-

periments were carried out to find the optimum pH-de-

sorption conditions. Figure 13 shows the effect of pH

values on the desorption process of the two dyes. It

shows that the two dyes are stable at lower pHs whereas

increasing pH higher than 10 results in a rapid desorption

of both dyes from bagasse surface. It is thus to be con-

cluded that the two reactive dyes are stable in the pH

range 3 - 10 for reactive yellow 2 and 6 - 10 for reactive

blue 4 while they may be completely recovered from the

treated bagasse surface at pH = 12 and higher. It is of

interest to mention here that these results are in agree-

ment with the results presented in Figure 2 which show

that the remarkable dye removal of both dyes on modi-

fied bagasse was at lower pH values.

4. Conclusion

Modified bagasse by propionic acid is an effective bio-

sorbent for the removal of both reactive yellow 2 and

reactive blue 4 dyes from wastewater. The maximum

R eactive blue 4

t (mg/g)

t1/2

R eactive yellow 2

Figure 12. Intra-particle diffusion model for reactive yellow

2 at pH 1.9 and reactive blue 4 at pH 2.1.

24681012

100 Reactve blue 4

Reactive yellow 2

D esorption %

Figure 13. Effect of pH on the desorption process of the two

dyes.

removal was observed at pH = 1.9 and pH = 2.1 for reac-

tive yellow 2 and reactive blue 4, respectively. Moreover,

the decrease of particle size of adsorbent was accompa-

nied with a pronounced removal of both dyes. The equi-

librium adsorption was best fitted with the Frundlich

isotherm for reactive yellow 2 and with the Langmuir

isotherm for reactive blue 4. Adsorption kinetics revealed

A. E.-A. A. SAID ET AL.

that reactive yellow 2 is well described by a pseudo-first

order whereas reactive blue 4 fits good for pseudo-second

order. Modified bagasse can be reused by desorption of

both dyes in the pH = 12 and higher. The hydroxyl and

carboxylic groups from bagasse and propionic acid re-

spectively enhance the removal of both reactive dyes.

5. Acknowledgements

The authors would like to thank the financial supports

from the Science and Technology for Development Fund,

STDF, Ministry of Higher Education, Egypt.

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