Advances in Environmental Biology Hamid Reza Moazzen,

Advances in Environmental Biology, 8(17) September 2014, Pages: 1140-1147
AENSI Journals
Advances in Environmental Biology
ISSN-1995-0756
EISSN-1998-1066
Journal home page: http://www.aensiweb.com/AEB/
Kinetic and Isotherm study of Sudan Black B removal
1Hamid
Reza Moazzen, 2Mohammad Ali Moazzen, 3Ali Faghihi-Zarandi and 4Eghbal Sekhavati
1
Department of Chemistry, Islamic Azad University, Firozabad Branch, Firozabad, Iran.
Department of Chemistry, Islamic Azad University, Firozabad Branch, Firozabad, Iran.
3
Department of Occupational Health, School of Public Health, Kerman University of Medical Sciences, Kerman, Iran.
4
Larestan School of medical Sciences, Larestan, Iran
2
ARTICLE INFO
Article history:
Received 25 September 2014
Received in revised form
26 October 2014
Accepted 25 November 2014
Available online 29 December 2014
Keywords:
Adsorption; Sudan Black B (SBB);
Cadmium hydroxide nano particle
loaded on activated carbon (Cd(OH)2NP-AC); Kinetic and Thermodynamics
of adsorption
ABSTRACT
Cadmium hydroxide nano particle loaded on activated carbon (Cd(OH)2 -NP-AC)
efficiently used for the removal ofSudan Black B. in batch studies the optimum values
of variable was set as: pH1.0, 0.03g cd(OH) 2-NP-AC at contacttime of 30 etc. this
adsorbent useful for removal of Sudan b l a c k B f o r a t least 20 mg of adsorbent.
Afteroptimizationof variable, the experimental equilibrium data was analyzed by
different conventional models such as Langmuir, Freundlich, Tempkin and Dubinin–
Radushkevich and based on the adsorbent correlation coefficient and error analysis the
suitability of Langmuir model for interpretation of equilibrium data with high
adsorption capacity. The adsorption of Sudan Black B was endothermic and feasible in
nature. The removal data versus time was analyzed by different kinetic models and it
was found that low quantity of adsorbent (<0.03 g) is suitable for removal of large
amount of Sudan Black B in short time (<30 min) the adsorption process following
pseudo second order kinetics and involvement of particle diffusion mechanism.
© 2014 AENSI Publisher All rights reserved.
To Cite This Article: Hamid Reza Moazzen, Ali Moazzen, Ali Faghihi-Zarandi and Eghbal Sekhavati., Kinetic and Isotherm study of
Sudan Black B removal. Adv. Environ. Biol., 8(17), 1140-1147, 2014
INTRODUCTION
Generally, dyes applied in industries like textile, paints, pulp and paper, carpet and printing. There is
growing interest and demands in textiles industry for application of synthetic organic dyes for coloring textile
fibers such as cotton and polyester. These dyes and organic pollutant containing waste water lead to generation
and creation of certain health hazards and environmental pollution. Dye effluents are aesthetic pollutants, while
their colors via hider light penetration in the receiving water bodies, disturb the biological processes. On the
other hand, dye containing waste water may possess chemicals exhibit toxic effects toward microbial
populations and can be toxic and/or carcinogenic to mammalian animal [1]. EPA imposed threshold limit on the
concentrations of discharged pollutant arrived from aqueous effluents of dyestuff manufacturing and textile
industries [2]. Sudan Black B (C26 H24 N4 O) (Fig.1) is a nonfluorescent, relatively thermostablelysochrome (fatsoluble dye) diazo dye used for staining of neutral triglycerides and lipids on frozen sections and some
lipoproteins on paraffin sections and used for Sudan staining.
Fig. 1: structure of Sudan Black B.
Sudan Black B is applicable for staining all material in addition to liquid Sudan Black B used for fingerprint
enhancement and recognition of fats contaminated with oil and grease. In differentiating hematological
disorders Sudan black will stain myeloblasts but not lymphoblasts [3,x]. Among different branch of dyes such as
Corresponding Author: Eghbal Sekhavati, Larestan School of medical Sciences, Larestan, Iran
E-mail: [email protected]
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Advances in Environmental Biology, 8(17) September 2014, Pages: 1140-1147
anionic, cationic, non-ionic and zwitterionic Cationic dyes are more toxic than anionic dyes [5,6]. Various and
extensive procedure efficiency applied for dye removal and elimination the discharged effluents to decrease
their ecosystem environment impact. These methods includeadsorption onto inorganic or organic matrices,
decolourization by photo-catalysis or photo-oxidation processes, microbiological decomposition, chemical
oxidation, ozonation and coagulation [7]. Adsorption as widely used procedure generally lead to quantitative
removal of dyes with lesser hazards. The biggest limitation for adsorption application the high cost of available
adsorbents for commercial application. This limitation and disadvantage can be overcome using regenerable and
high surface area atom to be able for quaint inexpensive [8]. Adsorption is superior to all other dye removal
techniques in view ofefficiency, capacity and large scale applicability, regeneration and recycling potential of
adsorbents. Some commercial and traditional systems are based on using activated carbon dyes wastewater [913]. However, the high cost of activated carbon and high removal times restricts its comprehensive and
universal application. There is more focus on development and designing new adsorbents with high surface
atom and areas to be able for quantitative dye removal in short time with high adsorption capacity. These entire
requirements will be benefited by decreasing and synthesis of nanomaterials and nanoparticles. In this paper, the
adsorption of SBB from aqueous solutions onto Cd(OH)2-NP-AC adsorbent has reported. Equilibrium
adsorption isotherms were measured and the experimental data were analyzed to commonly used models
including Langmuir, Freundlich, Tempkin and Dubinin- Radushkevich Isotherm equations.
Experimental:
Instruments and Reagents:
Sudan Black B (SBB) (United States, Sigma-Aldrich) stock solution was prepared by dissolving require
amount of their solid material in double distilled water. The test solutions daily were prepared by diluting their
stock solution to the desired concentrations. The concentration ofSudan Black B (SBB) was determined at 596605 nm respectively. The pH measurements were done using pH/Ion meter model-682 (Metrohm, Switzerland,
swiss) and absorption studies were carried out using Jusco UV-Visible spectrophotometer model V-570.
Batch Adsorption Experiments:
Concentration of Sudan Black B (SBB) in was estimated accurately using the calibration curve obtained at
the same condition concentrations. The dye adsorption capacities of adsorbent were determined at the time
intervals in the range of 0-30 min at room temperatures (10–60 ◦C) after 30 min. The effect of initial pH on
adsorptions was examined 20 mg L−1 in the pH range of 1-6 (adjusted by the addition of HCl or KOH). The
actual value of adsorbed dye to each step and finally equilibrium can be calculated based on well known
following equation:
qe = (x0 − C e) V/W
(1)
where C0and Ce are the initial and equilibrium dye concentrations in solution, respectively (mgL −1 ), V the
volume of the solution (l) and W is the mass (g) of the adsorbent used.
Preparation of Cd(OH) 2-NP-AC:
The Cadmium hydroxide nanoparticles was loaded on activated carbon (Cd(OH)2 -NP) as follow: 100mL of
0.01 mol L - 1 Cd(CH 3COO) 2sulution was added to the 2 mol L- 1ammonia solution and the mixture was stirred
until appearance of a white by 2 g was initially observed, which subsequently dissolved back into solution upon
the further addition of the NH 3 solution. The above solution was uniformly mixed with the activated carbon in
ultrasonic bath and the mixture was maintained at pH of ca.12 at room temperature for 5 days. This
phenomenon lead toresulting in the direct growth of the Cd(OH) 2-NP-AC in the solution. Following
neutralization, the adsorbent was dried under air and used for further characterization.
RESULTS AND DISCUSSION
Characterization of the Cd(OH) 2 -NP-AC:
The optical properties and ability of Cd (OH)2-NP-AC for UV-Vis absorption (Fig.2) show distinct and
distinguished peak.
The band gap of Cd(OH)2-NP was calculated from plotting (αhν)2vshν (Fig. 2) was found to be about 3.35
eV is larger than the direct band gap of bulk Cd(OH) 2 that was 3.2 xV[14]. The Cd(OH)2-NP-AC identity was
recognized by powder XRD patterns (Fig. 3).
The five broad peaks observed in the diffractogram around 29.45º, 34.55º, 48.85º, 57.85º and 60.53º belong
to the planes (100), (011), (012), (003) and (200) which show hexagonal structure of lattice structure of
Cd(OH)2-NW [15]. The match of obtained diffraction pattern with hexagonal Cd(OH)2 (JCPDF No. 73-0969)
show the formation of Cd(OH) 2-NPs. Field emission scanning electron microscopy (FE-SEM) image of the
Cd(OH)2-NP-AC (Fig. 4) show formation of large quantity of Cd(OH) 2 nanowires with micrometer lengths and
diameters of 80 ±10 nm.
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Fig. 3: X-ray diffraction (XRD) pattern of the Cd(OH)2 nanowires.
Fig. 4: Typical FE-SEM image of the Cd(OH)2 nanowires grown on a glass.
The SBB removal percentage on Cd(OH)2-NP-AC was studied at different adsorbent amount in the range of
0.04 g at 20 mg/L SBB concentration, pH (1) and (25±1ºC) at 30 min. As it is observed (Fig.5) by raising the
amount of adsorbent till 0.6 g/L due to increase in the number of vacant site and diffusion (driving force of
adsorption) the rate of SBB transfer to adsorbent surface significantly increase.
Fig. 5: Effect of amount of ( Cd (OH)2 -NW-AC) on the removal of SBB.
Effect of Contact Time:
The effect of contact time on the removal percentage of SBB at 20 mg/L at various stirring time in the range
of 0-30 min investigated. The available adsorption results reveal show that initial fast sorption rate becomes
slower at higher time and reach to equilibrium at 30 min (Fig. 6).
At initial step of removal process due to huge number of vacant site the diffusion driving force of transport
lead to increase in the mass transfer. Therefore, it is much easier for the adsorbate to reach the adsorption site
and after a lapse of time, the number of active sites becomes less and the adsorbent becomes crowded inside the
particles [16, 17]. For the initial concentrations of 20 mg/L, the equilibrium was achieved within 30 min,
respectively [18].
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Fig. 6: Effect of contact time on the removal of SBB onto (Cd(OH)2 -NW-AC).
Effect of Ph:
The pH of the solution affects the surface charge of the adsorbents as well as the degree of ionization of the
materials present in the solution. The hydrogen ion and hydroxyl ions are adsorbed quite strongly. Therefore, the
dye as ionic species adsorption of other ions is affected by the pH of the solution. The change of pH affects the
adsorptive process via influencing the dissociation of functional groups and the active sites of adsorbent, which
leads to shift in reaction kinetics and equilibrium characteristics of the absorption process (Fig. 7).
Fig. 7: Effect of pH on the removal of SBB by Cd (OH)2 -NW-AC. Contact time: 30 min; adsorbent dosage:
0.04 x in 50 ml ; dye concentration: 20 mg L-1 Room temperature.
It is expected observation that the surface adsorbs anions at lower pH due to abundance of H+ ions and
intend for the captions adsorption at higher pH due to the deposition of OH− ions.
Consequently, the dye molecule has high positive charge density at a lower pH . Therefore, for pH 0 <7, due
to electrostatic repulsion between the positively adsorbent and the positive charged dye molecule, the removal
percentage significantly decreased. This illustrates why adsorptionincreases with rising pH . 0 By decreasing the
pH of0 the test solution, the number of negativelycharged adsorbent sites decreases and positively charged sites
increases that did not favored the adsorption of positively charged dye captions due to electrostatic repulsion
[19, 20].
Effect of initial SBB concentration:
Concentrations ranging from 10-20 mg/L of SBB were investigated with fixed amounts of adsorbent at
room temperatures. The SBB extent of adsorption increases with rising its initial concentration, so that by
increase in concentration of the adsorbate exhibits a prominent increase in its. Maximum and quantitative
removal percentage of dye molecule occurs up to initial concentration of 20mg/L at the same conditions that
may be attributed to the saturation of all vacant site of adsorbent.
Effect of ionic strength:
For almost all the treatment strategies, the effect of typical wastewater contaminants on decolorization
efficiencies is very important [21]. Generally, presence certain additives and ionic strength adjuster such as
soluble salts can either accelerate or retard dye adsorption processes. Usually sodium chloride used as stimulator
in dyeing processes by affecting the electrostatic interaction of opposite charges in adsorbents and the dye
molecules, and an increase higher salt concentration lead to reducing the amount removal percentage on the
other hand, salts via increasing the fraction of dissociation of the dye molecules facilitate their removal percent.
The attraction interaction is responsible for adsorption of acid dyes by such adsorbents. So, the ionic strength
may be another important factor in the adsorption of certain dyes onto chitosan [22-26]. The influence of ionic
strength at various concentration of NaCl investigate by conducting a set of similar and it was found that by
increasing the sodium chloride concentration till 0.25 mol/L removal percentage increase.
Kinetic parameters of adsorption:
The kinetic parameters (helpful for determination of the rate controlling and mass transfer step) give
important information for selection application of on efficient low cost with high adsorption capacity adsorbent.
To uptake some information the influence of contact time on the adsorption process was investigated and the
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time dependency removal data was fitted by different conventional models such as pseudo-first-order, pseudosecond-order [15], Elovich [16] and intraparticle diffusion [17] models. The judgment for examination of model
suitability is based on agreement between experimental and the model-predicted adsorption capacity values and
the correlation coefficients (R2 , values close or equal to 1 and the relatively higher value shows the
applicability of the model).
Pseudo-first-order equationThe adsorption kinetic data were described by the Lagergren pseudo-first-order
model [27] is commonly expresses in linear form as follows:
Log (qe − qt ) = log (qe) −k1 t / 2.303
(2)
Generally by Plotting the log (qe −q t) versus t (linear relationship) k1 and q e can be evaluated from the
slope and intercept of the respective line respectively. If the intercept is not dose to q e means then the reaction is
not likely to be first-order reaction even the obtained lineand plot has high correlation coefficient [28,29].
However, this model is applicable for fitting and interpretation of adsorption data and phenomena at initial
stages (rapid adsorption) but cannot be applied for the entire adsorption process. Additionally, the calculated q e
value significantly for from experimental qe values (Table 1) which indicates un-suitability of first-order
reaction for fixing experimental data.
Pseuxo-second-order equation Due to insufficiently of first order kinetic model for explanation of
adsorption over whole data it is necessary that experimental data be fitted by Pseudo-second-order model [30]
that in linear expresses as follows:
(t/qt ) =1/ (k2 qe) +t/q
(3)
It was seen that the plots of t/q t versus t give a straight line that show its suitability and applicability for
fitting and interpretation of experimental data. The k2 and equilibrium adsorption capacity (q e) values was
evaluated from the intercept and slope of this line and respective value is presented in Table 1. The values of R 2
and close of experimental and theoretical q e indicate applicability of this model in comparison to other models
for explanation of adsorption process.
Table 1: The Elovich constants obtained from the slope and the intercept of the straight line.
Elovich kinetic equation:
The Elovich equation [30] as another rate equation based on the adsorption capacity in linear form is as
follows:
qt = 1/β ln (αβ) + 1/β ln(t)
(4)
Plot of qt versus in (t) should yield a linear relationship if the Elovich is applicable with a slope of (1/β) and
an intercept of (1/β) ln (αβ). The Elovich constants obtained from the slope and theintercept of the straight line
reported in Table 1. The correlation coefficients R2 are higher than 0.911 show suitability of model for
evaluation of adsorption process.
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The intraparticle diffusion model:
Generally, most of adsorption process follows intraparticle diffusion [31] other kinetic model in addition to
study the rate-limiting step for SBB adsorption onto Cd(OH)2 -NW-AC. This model is based on well known
following equation:
qt = K diff t1/2+ C
(5)
The values of K diff and C (Table 1) were calculated from the slope and intercept of the plot of q t versus t
1/2
. C value is related to the thickness of the boundary layer and K diff is the intraparticle Diffusion rate constant
(1/2 mg/g min). These models give two lines and rate constant (K diff ) directly evaluated from the slope of
the second regression line, while the first one represent surface adsorption (start of adsorption) and the second
show intraparticle diffusion.
Adsorption equilibrium study:
The experimental adsorption equilibrium data provides some insight into the adsorption mechanism, the
surface properties and affinity of the adsorbent for adsorbate [32-34]. A constant agitation speed of 350 rpm,
0.03g of adsorbent at room temperature (25 C) o was maintained for adsorption experiments. Equilibrium data
was fitted by Langmuir, Freundlich and Tempkin isotherms Langmuir equation [34] is represented in the linear
form as:
Ce/q e=1/k QL m +Ce/Q m
(6)
The value of Q m, k L and the correlation coefficient for this model calculated from the slope and intercept
of line obtained by plotting C /q vs. C and their values are presented in Table 2. Thehigh correlation coefficients
of this model show its applicability for interpretation of experimental equilibrium data. It seems that SBB first
layer adsorb on the surface of adsorbent via attraction force and further layer of adsorbent molecule is
impossible due to electrostatic repulsive force. The linear form of Freundlich isotherm is expressed as [35]:
log qe = log KF +1/n log C e
(7)
The values of K and 1/n is determined from the intercept and slope of linear plot of log q versus log C e,
respectively The value of n varies with the heterogeneity of adsorbent for favorable adsorption process the value
of n should be less than 10 and higher than unity [36]. The linear form of Tempkin isotherm [37, 38] is
presented as follows:
qe = B1 ln KT + B1 ln Ce
Where B11 = R T/b, T is the absolute temperature in Kelvin, R the universal gas Constant (8.314 J K -1 mol
-1
), Values of B1 and KT were calculated from the Plot of qe against in Ce (Table 2).
Fitting the experimental data in three isotherm models and considering the higher values of correlation
coefficients (R2> 0.99) show that Langmuir isotherm model is the best model to explain the SBB adsorption
over Cd (OH) 2-NW-AC.
Table 2: Values of B1 and KT were calculated from the Plot of qe against in Ce.
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Conclusions:
An adsorption experiment of SBB under different experimental conditions in bath mode has been conducted
and the influence of variables such as amount of adsorbent, SBB concentration, contact time and pH of the
solution on its removal percentage has been investigated. Higher dyeremoval was found within 30 min of the
start of every experiment that under the optimum experimental pH of 1-6. The proposed adsorption system
hasThe removal process follow Langmuir model with maximum adsorption capacity of 66.67 mg/g.
The rate of SBB from bulk to the adsorbent surface follow pseudo second order kinetic model with
involvement of inter particle diffusion model.
1) Using small amount of Cd (OH)2 -NW-AC, the high amount (0.03 g) and removal percentage (higher of
95%) SBB significantly can be removal in short time (30 min).
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