Dye removal from aqueous solution using low cost … JRF, School of Civil Engineering, SASTRA...
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INTERNATIONAL JOURNAL OF ENVIRONMENTAL SCIENCES Volume 1, No 7, 2011
© 2011 Velmurugan.P et al., licensee IPA- Open access - Distributed under Creative Commons Attribution License 2.0
Research article ISSN 0976 – 4402
Received on March 2011 Published on April 2011 1499
Dye removal from aqueous solution using low cost adsorbent Velmurugan
.P
1, Rathina kumar.V
2, Dhinakaran.G
3
1- JRF, School of Civil Engineering, SASTRA University, Tamil Nadu, India
2- Assistant Professor, School of Civil Engineering, SASTRA University, Tamil Nadu, India
3- Professor, School of Civil Engineering, SASTRA University, Tamil nadu-613 401, India
doi:10.6088/ijessi.00107020009
ABSTRACT
The use of cheap and eco-friendly adsorbents studied as an alternative substitution of
activated carbon for removal of dyes from wastewater. Adsorbents prepared from orange peel,
which is a domestic waste, successfully used to remove the methylene blue from an aqueous
solution in a batch wise column. This study investigates the potential use of orange peel,
pretreated with nominal treatment method, for removal of methylene blue from simulated
wastewater. Treated orange peel used to adsorb methylene blue at varying dye concentration,
adsorbent dosage, pH and contact time. Similar experiments conducted with some other low-
cost adsorbent such as banana peel, neem leaves and commercially available powdered
activated carbon (PAC). The adsorption capacity of orange peels decreased in the order of
methyl orange (MO) > methylene blue (MB) > Rhodamine B (RB) > Congo red (CR) >
methyl violet (MV) > amido black 10B (AB). Removal efficiency of all the adsorbents is
quite effective, but orange peel found to be very effective compared to other low cost
adsorbent within the short period. The sorption data were then correlated with the freundlich
and the langmuir adsorption isotherm models. In both isotherms exhibited a maximum K
value in which indicates that the orange peel has greater affinity for methylene blue. The
maximum color removal efficiencies of orange peel at dosage of 1.0g for time duration of 45
min found to be 99% of the dye from an aqueous solution of 12.32 ppm. From the study it is
understood that pH, contact time and adsorbent dosage plays a vital role in removal of dye.
Keywords: Adsorbent, Methylene blue, pH, Orange peel, Neem leaves, Banana peel.
1 Introduction
Dyes are chemicals, which on binding with a material will give color to them. Dyes are ionic,
aromatic organic compounds with structures including aryl rings, which have delocalized
electron systems. The color of dye provided by the presence of a chromophore group. A
chromophore is a radical configuration consisting of conjugated double bonds containing
delocalized electrons. The Chromogen, which is the aromatic structure normally containing
benzene, naphthalene or anthracene rings, is part of a chromogen-chromophore structure
along with an auxochrome. The presence of ionising groups known as auxochromes results in
a much stronger alteration of the maximum absorption of the compound and provides a
bonding affinity. Colored dye wastewater arises as a direct result of the production of the dye
and because of its use in the textile and other industries. There are more than 100,000
commercially available dyes with over 7 x 105
of dyes produced annually worldwide [1-2].
Dyes are widely used in industries such as textile, rubber, paper, plastic, cosmetic etc. Among
these various industries, textile ranks first in usage of dyes for coloration of fiber. The
convectional biological treatment process is not very effective in treating a dyes wastewater,
due to low biodegradation of dyes. It is usually treated by either physical or chemical
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Velmurugan. P, Rathina kumar. V, Dhinakaran. G
International Journal of Environmental Sciences Volume 1 No.7, 2011
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processes. However, these processes were very expensive and could not be effectively used
to treat the wide range of dyes waste [Grag et al, 2003].
The adsorption process is one of the effective methods for removal dyes from the waste
effluent. The process of adsorption has an edge over the other methods due to its sludge free
clean operation and completely removed dyes, even from the diluted solution. Activated
carbon (powdered or granular) is the most widely used adsorbents because it has excellent
adsorption efficiency for the organic compound. Nevertheless, commercially available
activated carbon is very expensive. Furthermore, regeneration using solution produced small
additional effluent while regeneration by refractory technique results in a 10-15% loss of
adsorbents and its uptake capacity [Shaobin Wang et al, 2005]. The sorption data have been
correlated with adsorption isotherm to determine the efficiency of adsorption process.
Numerous researchers worked earlier on variety of adsorpents as mentioned below. Wool
Fiber and Cotton Fiber [Rasheed Khan et al, 2005], Banana pith [Namasivayam et al,
1993a,1993b], Biogas residual slurry [Namasivayam et al, 1992a], Carbonized coir pith
[Namasivayam et al, 2001a], Coir pith [Namasivayam et al, 2001b,2002], Chitosan [Juang et
al, 1996], Hardwood [Asfour et al, 1985], Mahogany sawdust, rice husk [Namasivayam et
al,1992b], Parthenium hysterophorus [Rajeshwarisivaraj et al, 2002], Neem (Azadirachta
Indica) husk [Alau et al, 2010], Rice husk [Singh et al, 2001], Rice husk [Guo et al, 2003],
Silk cotton hull, coconut tree sawdust [Kadirvelu et al, 2003], Gypsum [Muhammad Rauf et
al, 2009], Tuberose Sticks [Ahsan habib et al, 2006], Tamarind Fruit Shell[Papita Saha 2010].
2 Experimental Investigations
2.1 Preparation of the Adsorbent
Adsorbents like Orange Peel, Neem leaves and Banana peel collected from the local areas of
Thanjavur District. The peels and leaves collected and dried at low temperature (<105˚C) for
48 hrs to remove moisture content. After drying process, peels were ground to fine powder
and sieved through 600 µ size. The adsorbents used in the present research work prepared
under Nominal Treatment only.
2.2 Dye solution preparation
The characteristics of the Methylene blue used for the present work is given in Table 1. An
accurately weighed quantity of the dye dissolved in double distilled water to prepared stock
solution (1000 ppm). Solution used in the experiment for the desired concentration obtained
by successive dilutions. Dye concentration was determined by using absorbance values
measured before and after the treatment, at 650 nm with Shimadzu UV Visible Spectrometer
(Model : UV mini 1240). Experiments were carried out at initial pH value is 6.5 and was
controlled by addition of sodium hydroxide or hydrochloric acid, physical characteristics of
various adsorbents given in Table 2.
Table 1: Properties of Methylene Blue
Chemical formula C14H18N3SCl
Molecular weight 319.85 g/mol
Melting point 100 – 110 C
Type of dye Basic blue
Boiling point Decomposes
max 665 mm
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Table 2: Physical Properties of Adsorbents
2.3 Calibration of Methylene Blue
The synthetic dye sample calibrated in order to find out various optical densities at various
concentrations. The calibrated results are very effective to identify the respective color
removal capacities of various adsorbents Figure1 showing the graphical representation of
Calibration of Methylene Blue.
Figure 1: Calibration of Methylene Blue.
No. Parameter Value
Orange Peel Neem
Leaves
Banana
Peel
Activeted
Carbon
01. Moisture Content (%) 38.50 11.10 7.70 30.00
02. Ash Content (%) 17.80 4.30 5.60 30.00
03. Volatile Content (%) 43.70 84.60 86.70 40.00
04. Specific Gravity 3.22 2.85 3.13 1.83
05. Fineness Modulus 3.24 3.128 3.02 2.17
06. Particle size (mm) 0.150 0.186 0.200 0.002
07. Void ratio 0.75 0.75 0.36 0.50
08. Particle Density (g/cc) 1.44 0.56 0.92 1.90
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2.4 Effect of time on various adsorbents
In each adsorption experiment, 20 ml of dye solution of known concentration and pH was
added to 0.1g of adsorbents in 250 ml round bottom flask at room temperature and the
mixture was stirred on a rotary orbital shaker at 150 rpm. The sample withdrawn from the
shaker at the pre determined time intervals for 10 minutes each. At the end of 10 min, the
agitated sample taken from the shaker and tested for its optical density using the UV-Visible
Spectrophotometer. The corresponding Optical Density interpolated with the initial
calibration values in order to find out color removal efficiency of the adsorbent. From the
Comparative results, it is clearly known that, the effect of duration plays a very important
role in adsorption process of color removal. All the adsorbents are quite effective, but Orange
peel found to be very effective next to activated Carbon. The color removal efficiencies of the
adsorbents have a break through at 60 minutes duration, in which there is no further color
removal takes place. Orange Peel found to be very effective with color removing efficiency
of 96%. The results of present study are compared with results of Papita Saha 2010, who has
done experiments with Tamarind shell. It is inferred from the comparison that, upto the
duration of 40 min, orange peel showed lesser efficiency and after 40 min it shows higher
efficiency than the Tamarind shell. The comparative results of efficiency of various adsorbent
with respect to time given in Figure 2. However, activated carbon performs well when
compared to all these low cost adsorbents.
Figure 2: Comparative results of various adsorbents on to Effect of Time
2.5 Effect of adsorbent dosage on various adsorbents
20 ml of the stock solution of 1000 ppm taken and with varied amount (0.2, 0.4, 0.6, 0.8, 1 g)
of adsorbent fed into the 250ml round bottom flask and kept for agitation at 150 rpm using
rotary orbital shakers for the regular interval of 45 minutes. At the end, the agitated sample
taken from the shaker and tested for its optical density using the UV-Visible
Spectrophotometer. The corresponding Optical Density interpolated with the initial
calibration values in order to find out color removal efficiency of the adsorbent. From the
Comparative results, it is clearly understood that the Effect of Adsorbent Dosage is also plays
a very vital role in adsorption process for color removal. Among the three adsorbents, Orange
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peel found to be very effective next to Activated Carbon. Therefore, from the two parameters
such as Effect of Time and Effect of Adsorbent dosage, Orange peel found to be an excellent
adsorbent compared to Neem leaves and Banana Peel. The maximum color removal
efficiencies of Orange peel, Neem leaves and Banana Peel at dosage of 1 g for a time
duration of 45 minutes is found to be 98.76, 97.77 and 97.93 respectively Figure 3 Showing
the graphical representation of comparative results various adsorbent with respect to
adsorbent dosage.
Figure 3: Comparative results of various Adsorbents on to Effect of Adsorbent Dosage
2.6 Effect of pH on Orange Peel for Color Removal
In Order to find the effect of pH, series of experiments conducted at various pH values from
2-4 and 8-10 in acidic and alkaline conditions respectively. However, the initial pH of the
stock solution prepared was 6.50 at 1000 ppm. The value of pH controlled by addition of
sodium hydroxide or hydrochloric acid. For the present research, the stock solution of 20 ml
taken and 0.1 g of adsorbent fed into round bottom flask and kept for rotary orbital shaker at
150 rpm. The sample withdrawn from the shaker at the pre determined time intervals for 10
minutes each. At the end of each 10 minutes the agitated sample is taken from the shaker and
tested for its optical density using the UV-Visible Spectrophotometer.
Effect of pH under acidic condition imparts a new color (greenish yellow) in which the
respective optical density found to be more than 4.00, because of some acidic elements
already present in the orange peel. Again some sample was analyzed at the pH of 4, the value
of the optical density is slightly above the calibration value of the Methylene blue. Hence
color removal under acidic condition using orange peel as an adsorbent found to be
insignificant, where as for alkaline condition it is significant. Effect of pH and different
dosage of adsorbent under alkaline conditions are depicted in Figures 4 and 5.
Dye removal from aqueous solution using low cost adsorbent
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Figure 4: Effect of pH under alkaline conditions at regular time interval.
Figure 5: Effect of pH under alkaline conditions at various adsorbent dosages
2.7 Column Study using Orange peel
The column tests carried out in a micro-glass column with inside diameter of 12.5 mm,
length 750 mm with a capacity of 50 ml. By using column study burette found to be very
economical and there is no external driven force applied to the system. Series of burettes
operated in a parallel way and filled with 10 ml of adsorbent and 40 ml of adsorbate. A thin
layer of very fine particles of sand of diameter of 0.7 mm with the depth of 50 mm placed at
the bottom in order to remove the foreign and dust particles. Figure 6 shows experimental
setup of column study.
Particle size plays a foremost role in adsorption process especially in the column studies and
the particle size of the adsorbent is 0.6 mm. The effluent of the first column considered as the
influent of the second column with time interval of 60 minutes each. The results are shown in
Figure 7.
The effluent from the each burette was taken and measured for its optical density. In order to
correct for any adsorption of color by the container, control experiments carried out without
adsorbents. It was found that there was no adsorption by the container walls. Similarly same
test were carried out by using the filling material and was found that no adsorption took place,
and the entire column tests conducted at room temperature only.
Dye removal from aqueous solution using low cost adsorbent
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Figure 6: Series of column tests conducted using burettes
Figure 7: Efficiency of color removal using orange peel as adsorbent
3 RESULTS AND DISCUSSIONS
The study of isotherm data is important to find out the adsorption capacity of various
adsorbents. In order to investigate the adsorption isotherm, two equilibrium isotherms were
analyzed: Langmuir and Freundlich isotherms are used for fitting the experimental data in
adsorption studies to understand the extent and degree of favorability of adsorption.
3.1 Freundlich Isotherm
The equilibrium adsorption isotherms are of fundamental importance in the design of
adsorption systems. The equilibrium adsorption data could be satisfactory by the Freudlich
isotherm
x/m = K.C 1/n
where x is the amount adsorbed per mass of adsorbent (m), Co is the initial concentration of
the solution (ppm), C is the equilibrium concentration (ppm), and K and n are Freudlich
Dye removal from aqueous solution using low cost adsorbent
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constants. The constant K, partition coefficient in equilibrium is positively related to the
extent of degree of adsorption, while then constant „n‟ provides a rough estimation of the
intensity of adsorption. A linear form of the Freundlich expression will yield the constants K
and n hence:
log x/m = log K+1/n log C
The analysis and design of adsorption separation process require the relevant adsorption
equilibrium, which is the most important piece of information in understanding the
adsorption process. The adsorption isotherms are equilibrium equation and apply to
condition resulting after the adsorbate-containing phase has seen in contact with the
adsorbent of sufficient time to reach equilibrium [Tan et al, 2010]. The adsorption capacity of
any adsorbent may be determined by the used of an adsorption isotherm. Knowledge of
adsorption capacity of an adsorbent material such as lignite enables the designer to develop
treatment systems for particular adsorbate/adsorbent systems [Allen et al, 1989].
Freudlich constants were determined from the graphs plotted for log (X/M) in ordinate and
log Ce in abscissa. Table 3 shows the Orange peel has the maximum K value followed by
Banana Peel and Neem leaves. The higher value of K (0.775mg/g) indicates that Orange Peel
have greater affinity for methylene blue compared with other adsorbents. The adsorption
intention „n‟ is found to 1.50, 0.612 and 1.273 for Orange peel, Neem leaves and Banana peel
respectively. It is observed that all the adsorbents do not satisfy the condition of
heterogeneity, i.e., 1<n<10. Only Orange Peel and Banana Peel satisfy those conditions.
Table 3: Freudlich Isotherm constants for Adsorbents
Sl.No Name of the
Adsorbent
Value of „n” K (mg/g) R2
1. Orange Peel 1.50 0.775 0.6210
2. Neem leaves 0.612 -0.327 0.8373
3. Banana Peel 1.273 0.635 0.6716
4. Activated Carbon 0.952 -0.7276 0.8975
3.2 Langmuir Isotherm
The Langmuir model was developed based on the assumption of the formation of a
monolayer of the absorbate species onto the surface of the adsorbent. It has also been
assumed that the surface sites are completely energetically homogeneous. But in the true
sense, the adsorbent surface is energetically homogeneous. The study of the Langmuir
isotherm is essential in assessing the adsorption efficiency of the adsorbent. This study is
also useful in optimizing the operating conditions for effective adsorption. In the respect, the
Langmuir isotherm is important, though the restrictions and the limitations of this model have
been well recognized.
The Langmuir and the arranged Langmuir equations are given below,
q = (Xmk C) / (1+kC)
Ce/Qe = 1/k.Xm + Ce/Xm
Where q is the amount of dye adsorbed per unit weight of the adsorbent, C is the
Concentration of dye remaining in solution at equilibrium, Xm is the amount of dye adsorbed
Dye removal from aqueous solution using low cost adsorbent
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per unit weight of adsorbent in forming a complete monolayer on the surface and k is the
constant related to the energy. By plotting Ce versus Ce/Qe, a curve is obtained which is
linear at low equilibrium concentrations, followed by a curvature and with an asymptotic
tendency to saturation corresponding to a monolayer covering.
Table 4: Langmuir Constants for various adsorbents
Sl.No Name of the
Adsorbent
a (l/mg) K (l/g) R2
1. Orange Peel 0.00502 10,000 0.08368
2. Neem leaves -0.00903 -3,333.33 0.5529
3. Banana Peel 0.00411 10,000 0.0769
4. Activated Carbon -0.00370 -33,333.33 0.0402
From the Table 4 , the higher value of K (10,000) indicates that the amount of methylene
blue per unit weight of adsorbent seem to significantly higher than Neem leaves, in which
both orange peel and Banana peel have same values. Neem leaves is found to very non-linear,
this will normally occur after dye particles fill the available monolayer in the adsorbents.
This non-linearity may also be due to any primary expansion of adsorbent while will give
way to a secondary or tertiary expansion which can occur at much reduced rates. From the
results the higher value of K from Orange peel is found to be very effective followed by
Banana peel and Neem leaves, which confirmes the result obtained from the Freudlich
Isotherm that Orange peel has the maximum K value followed by Banana peel and Neem
leaves. The plots showing results between log(X/M) and log (Ce) is given in Figure 8 for
Freundlich Isotherm and between Ce/Qe and Ce is given in Figure 9 for Langmuir Isotherm.
Figure 8: Freudlich Isotherm using Orange Peel
Dye removal from aqueous solution using low cost adsorbent
Velmurugan. P, Rathina kumar. V, Dhinakaran. G
International Journal of Environmental Sciences Volume 1 No.7, 2011
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Figure 9: Langmuir Isotherm using Orange Peel
4 Conclusions
From the results of the present study, it is concluded that, the adsorption process is a very
effective process for the decolorization of textile wastewater, as we can reach 97%
decolorization in few minutes. There is a need to enhance the adsorption process effectively
by varying parameters so as to bring down the values to permissible limits for wastewater
before discharging it to the water environment. The removal of color from aqueous solutions
and wastewaters using activated carbon and three low cost sorbent materials orange peel,
neem leaves and banana peel was studied by studying the effect of time, adsorbent dosage
and pH. A separate column study was conducted in which, flow was due to gravity. Two
types of isotherms were investigated, namely the Langmuir and Freundlich isotherms.
The adsorption studies revealed that the optimum time adsorption of Orange Peel, Neem
leaves and Banana peel was found to be 60 minutes and adsorbent dosage was 1 g for all the
three adsorbents. The isotherm analysis revealed that orange peel prepared under nominal
treatment was found to be very effective than the Neem leaves and Banana Peel. Adsorption
was an effective process for decolorization of textile wastewaters. Although activated carbon
was the most effective sorbent, other low cost sorbents could be used for color removal. The
final choice of the sorbent is a matter of economics. Batch studies and column studies
confirm that these low cost materials can be used as a substitute for high cost adsorbent.
Dye removal from aqueous solution using low cost adsorbent
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