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Synthesis and Properties of Fe3O4 Nanoparticles by Co-precipitation Method


to Removal Procion Dye

Article  in  International Journal of Environmental Science and Development · June 2013


DOI: 10.7763/IJESD.2013.V4.366

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International Journal of Environmental Science and Development, Vol. 4, No. 3, June 2013

Synthesis and Properties of Fe3O4 Nanoparticles by


Co-precipitation Method to Removal Procion Dye
Poedji Loekitowati Hariani, Muhammad Faizal, Ridwan, Marsi, and Dedi Setiabudidaya

in recent years. Many of papers have been published


Abstract—Fe3O4 (magnetite) nanoparticles were synthesized demonstrating that magnetic Fe3O4 can be used for
by chemical co-precipitation method. The structure, wastewater purification, such as to adsorb arsenite, arsenate,
morphology and magnetic properties of as-prepared were crom, cadmium, nickel [9],[10]. Fe3O4 also can be used to
characterized by X Ray Diffraction (XRD), Scanning Electron
Microscope-Energy Dispersive X Ray Spectrometry
alkalinity and hardness removal, desalination, decolorisation
(SEM-EDS), Transmission Electron Microscope (TEM) and of pulp mill effluent and removal of natural organic
Vibrating Sample Magnetometer (VSM). The result of XRD compounds [3]. After adsorption, Fe3O4 can be separated
characterization was indicated Fe3O4 as the product. SEM and from the medium by a simple magnetic process. Thus, an
TEM image of the Fe3O4 showed nanoparticles Fe3O4 have the efficient, economic, scalable, and non toxic. Synthesis of
mean diameter 5-20 nm. The EDS spectra showed strong peaks Fe3O4 nanoparticles is highly preferred for potential
of Fe and O. Magnetic characteristic of Fe3O4 nanoparticles was
indicated super paramagnetic properties. The saturation
application and fundamental research [11],[12].
magnetic was 89.46 emu g-1. Therefore, the nanoparticles Fe3O4 In current study, Fe3O4 will be used to adsorb dye.
is suitable to remove dye in the water by a simple magnetic Removal of dyes from wastewater is a major environmental
separation process. The optimum adsorption occurred at initial problem because dyes are visible even at low concentration.
concentration of procion dye 100 mg L-1, pH solution 6, dosage The existence of highly colored waste is not only
of Fe3O4 0.8 g L-1 and contact time 30 minutes under room aesthetically disturbance, but it also impedes light
temperature with color removal 24.40 % and adsorption
capacity was 30.503 mg g-1.
penetration, thus up setting biological process within a stream,
some dyes also being toxic or carcinogenic [13]. It is
Index Terms—Fe3O4 nanoparticles, co-precipitation, estimated that 10-50 % of the dye is lost in the effluent [14].
adsorption, dye Therefore, the treatment of effluent containing such a dye is a
interest due to its harmful impacts on receiving waters [15].
The objective of this study were to synthesis Fe3O4 by
I. INTRODUCTION co-precipitation methods and assess the ability of Fe3O4 to
The magnetic nanoparticles have many uses such as remove procion dye. The procion dye including azo dyes
magnetic drug target, magnetic resonance imaging forclinical which have -N=N- bond. Additionally procion dyes have two
diagnosis, recording material and catalyst, environment, etc of aromatic group and one atom sodium. These dye are used
[1]-[3]. Iron oxides nanoparticles play a major role in many in the textile industrial for dyeing process. Various
areas of chemistry, physics and materials science. Fe3O4 techniques for removing dyes from effluents have been
(magnetite) is one of the magnetic nanoparticles. There are developed, including electrochemical treatment,
many various ways to prepare Fe3O4 nanoparticles, which sonochemical treatment, photo catalytic oxidation and
have been reported in other papers, such as energy milling [3], adsorption. Adsorption method is a promising and attractive
reducing [4], ultrasonic assisted impregnation [5], and using alternative for treatment of azo containing effluents if
Tridax procumbens leaf extract [6]. Co-precipitation method adsorbents used are inexpensive and readily available [12],
is a method of synthesis of Fe3O4 which is easy to do with the [14], [15].
success rate from 96 to 99.9% [7]. In this method, ferrous and
ferric ions at the ratio of 1 to 2 in alkaline medium. Chemical
co-precipitation can produced fine, stoichiometry particles of II. MATERIAL AND METHODS
single and multi component metal oxides [8]. A. Materials
The application of magnetic technology to solve
All the reagents used for the synthesis Fe3O4 were
environmental problems has received considerable attention
analytical grade and used without further purification. Ferric
chloride [FeCl3], ferrous chloride [FeCl2], sodium hydroxide
Manuscript received February 5, 2013; revised March 28, 2013. This [NaOH] were purchased from Merck, Germany.
work was supported in part by the Competitive Research Sriwijaya
University for financial support No 0366/UN9.4.2.1/LK/2011). B. Synthesis Fe3O4
Poedji Loekitowati Hariani and Muhammad Faizal are with the
Chemistry Department, University of Sriwijaya, Palembang, Indonesia Synthesis of Fe3O4 magnetics nanoparticles were prepared
(email: pujilukitowati@yahoo.com; faizal_ga@yahoo.com). by co-precipitation of ferric and ferrous salts under the
Ridwan is with the National Nuclear Energy Agency, Tangerang Selatan presence of N2 gas. 16.25 FeCl3 and 6.35 g of FeCl2 were
15314, Indonesia (email: ridwan@batan.go.id)
Marsi is with Agrotechnology Department, University of Sriwijaya, dissolve into 200 mL of deoxygenated distilled water. After
Palembang 30139, Indonesia (email: mbasihin1960@yahoo.com). stirring for 60 minutes, chemical precipitation was achieved
Dedi Setiabudidaya is with the Physics Department, University of at 300C under vigorous stirring by adding of 2 M NaOH
Sriwijaya, Palembang 30139, Indonesia (email:
setiabudidaya@hotmail.com). solution under presence of N2 gas. The reaction system keep

DOI: 10.7763/IJESD.2013.V4.366 336


International Journal of Environmental Science and Development, Vol. 4, No. 3, June 2013

at 700C for 5 h and pH solution ± 12. Completed precipitation


of Fe3O4 expected at pH between 8 and 14 [16]. After the
system was cooled to room temperature, the precipitates were 90
separated by a permanent magnet and washed with 80
deoxygenated distilled water until pH neutral. Finally Fe3O4 70
washed with acetone and dried in oven at 60-700C. The

Intensity
60
relevant chemical reaction can be expressed as follows eq.1: 50
40
Fe2+ + 2Fe3+ + 8OH-→Fe3O4 + 4H2O (1) 30
20
C. Characterizations of Materials. 10
The crystal structure of the products was characterized by 0
X-ray Diffraction (XRD) Shimadzu XD-610. The patterns 0 10 20 30 40 50 60 70 80 90
with the Cu Kα radiation (λ = 1,54051 Å) were recorded in 2 θ (degree)
the region of 2θ range 10 to 800. The morphology of the Fig. 1. XRD pattern for Fe3O4
Fe3O4 materials were examined by Scanning Electron
Microscope-Energy Dispersive X Ray Spectrometry In order to investigate the morphology of obtained
(SEM-EDS) JEOL-JSM-6510 LV. Transmission Electron materials by SEM and TEM images. Fig. 2. shown SEM
Microscope (TEM) JEOL JEM 1400 was used for image of Fe3O4, in the picture appears that Fe3O4 particles
characterizing the size of nanoparticles. The magnetic composed of small particle. Fig. 3. shown the TEM image of
properties of the Fe3O4 materials measurement by Vibrating Fe3O4, from which we can know that the diameter size 5-20
Sample Magnetometers (VSM) Lakeshore 74004 at room nm. Fe3O4 synthesized by co-precipitation with different
temperature. Uv-Vis Spectrometry by Shimadzu 2550 used reagen (FeCl3.6H2O, FeCl2.4H2O, propylene glycol and
to measurement procion dye concentration. ammonium hydroxide) indicated the mean size of particles
was 8 nm [18]. The control of the monodisperse size is very
D. Adsorption Experiment. important because the properties of nano crystal strongly
The studies of procion dye adsorption were performed by depend upon the dimension of nanoparticles [16].
batch adsorption method. The adsorption experiments were
conducted by varying initial concentration of procion dye
from 25 to 150 mg L-1, pH solution was adjusted over the
range pH 5-9 using HCl and NaOH 1 M, dosage of Fe3O4
from 0,5; 0,6; 0,7; 0,8; 0,9 and 1 g L-1 and contact time at 15,
30, 45, 60 and 75 minutes. Adsorption experiments were
carried out with a thermostatic shaker at 120 rpm.
Adsorption data analysis. The concentration retained in
color removal color (η,%) and adsorption capacity for Fe3O4,
qe (mg g-1), was determined by analyzing procion dye before
and after the treatment and calculated by using the eq.2. and
eq.3

% (2) Fig. 2.SEM images of Fe3O4

(3)

where C0 and Ce are initial and equilibrium dye concentration


in the solution (mg L-1), m is the adsorbent dosage (mg), and
V is the volume of the solution (mL).

III. RESULT AND DISCUSSION


A. Characteristic of the Fe3O4.
Fig. 1. shown XRD patterns of the Fe3O4. Six
characteristic peaks at 30,2050, 35,5150, 43,3250, 53,7110, Fig. 3. TEM images of Fe3O4
57,2150 and 62,9450 were corresponding to the (220), (311),
(400), (422), (511) and (440) crystal planes of a pure Fe3O4 Characterization of Fe3O4 using EDS in Fig. 4. The EDS
with a spinal structure (JCPDS file PDF no.65-3107) [17]. spectra showed the strong peaks of Fe and O. The
The peaks indicating that Fe3O4 with a spinal structure and no composition components of Fe3O4 formed by co-precipitation
characteristic peak of impurities are detected in the XRD synthesis Fe was 73.36% and O was 21.02%. These results
pattern. demonstrate the purity of the synthesis results.

337
International Journal of Environmental Science and Development, Vol. 4, No. 3, June 2013

resulted from electrostatic attraction [21]. The color removal


of procion dye at pH 6 which is 24.40 %, no thighly different
from th pH 5 shown in Fig. 7. Thus, in the adsorption process
used at pH 6 because it closer to neutral pH solution.
C
o
u
n 31
t
s 29

Color removal (%)


27
25
23
21
19
Energy (Kev) 17
15
0 25 50 75 100 125 150 175

Initial concentration procion dye (mg/L)


Fig. 4. EDS images of Fe3O4
Fig. 6. Effect initial concentration of procion dye

100
Momen Magnet (emu/gr)

80 30

Color removal (%)


60 25
40
20
20
15
0
10
-1 -20 0 1
-40 5
-60 0
-80 4 5 6 7 8 9 10

-100
pH solution
Fig. 7. Effect pH solution procion dye
Field (tesla)
Fig. 5. Saturation Magnetization of Fe3O4 Fig. 8 shows effect of dosage Fe3O4 and contact time to
adsorb procion dye. The corresponding result showed that an
Fig. 5 shows the magnetization curve of Fe3O4 obtained by increased in adsorbent dosage could increase adsorption
VSM at 250C. The saturation magnetization of Fe3O4 capacity. With increasing adsorbent dosage, more surface
nanoparticles was 89.46 emu g-1. The magnetization of Fe3O4 area was available for adsorption due to the increase in active
is not far from the actual magnetization of the Fe3O4 is 92 site on the surface Fe3O4 and thus making easier penetration
emu g-1 [19]. The excellent magnetic responsivity was of adsorbate to adsorption. The dosage Fe3O4 to adsorb
necessary for magnetic separation from dye-containing procion dye at a fixed of 0.8 g L-1.
effluents in the future.
B. Optimum Condition Adsorption 30
Color removal (%)

The effect of initial concentration of procion dye on the 25


adsorption properties shows in Fig. 6. The increase of color
20
removal has positive comparison with the increase of initial
15
concentration of procion dye. It was clear that the adsorption
process dependent on initial procion dye concentration. The 10
large number of vacant surface sites were available for 5
adsorption during initial stage. Initial concentration of 0
procion dye on the adsorption process is then used at a 0.4 0.5 0.6 0.7 0.8 0.9 1 1.1
concentration of 100 mg L-1
The pH of dye solution plays an important role in the Dosage Fe3O4 (g L-1)
whole adsorption process and particularly on the color Fig. 8. Effect dosage Fe3O4
removal. The most color removal was 25.19 % at pH
solution 5. The dye with two sulfonic groups ionized easily Effect contact time, color removal also increased with
even in acidic media and became a soluble anion dye. Anion increasing contact time shown in Fig. 9. The equilibrium time
dye and neutral solutions were easily adsorbed to Fe3O4 with at 30 minutes and after equilibrium time the color removal
positive surface charge [20]. All the adsorption was highly was stable. In the optimum condition adsorption has color
pH dependent. The optimal pH for the removal of Cr(VI), removal was 24.40 % . This condition color removal is
Cu(II) and Ni(II) were 2.5, 6.5 and 8.5 by maghemite optimum so that extra time does not increase the color
nanoparticles. Under the optimal pH , their uptakes mainly removal.

338
International Journal of Environmental Science and Development, Vol. 4, No. 3, June 2013

[9] J. T. Mayo, et al., “The Effect of Nano Crystalline Magnetite Size on


Arsenic Removal,” Journal of Science and Technology Materials, vol.
30 8, pp. 71-75, 2008
25 [10] F. Rosada, M. Otero, A. Moran, and A. I. Garcia, “Adsorption of
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Heavy Metals onto Sewage Sludge-Derived Materials,” Bioresour


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0366/UN9.4.2.1/LK/2011).

REFERENCE
Poedji Loekitowati Hariani was born in Madiun,
[1] U. Hafeli, W. Schutt, J. Teller, and M. Zborowski, Scientific and Indonesia, on August 27, 1968. In 1992 graduated with
Clinical Applications of Magnetic Microspheres, Plenum, New York, a scholar science in Chemistry Department, Gadjah
pp. 324-326, 1997. Mada University, Indonesia. In 1997 graduated from
[2] V. S. Zaitsev, D. S. Filimonov, I. A. Presnyakov, R. J. Gambino, and B. master of scince, field of environmental chemistry at
Chu, “Physical and Chemical Properties of Magnetite and Magnetite the Institute of Technology Bandung, Indonesia. At this
Polymer Nanoparticles and Their Colloidal Dispersions,” Journal time, she is study doctoral in the field of environmental
Colloid Interface Sci., vol. 212, pp. 49-57, 1999 scince at Sriwijaya University, Indonesia. She works
[3] B. A. Bolto, “Magnetic Particle Technology for Wastewater has a lecturer in the Chemistry Department, Faculty of
Treatment,” Waste Management, vol. 10, pp. 11-21, 1990 Mathematics and Science, Sriwijaya University, Palembang, Indonesia.
[4] A. B. Fuertes and P. Tartaj, “A Facile Route for the Preparation of Research carried out for this focus wastewater treatment.
Superparamagnetic Porous Carbon,” Chem. Mater, vol. 18, pp.
1675-1679, 2008.
[5] T. Yang, S. H. Zhu, D. Zhang, and S. H. Xu, “Synthesis and properties Muhammad Faizal was born in Palembang Indonesia
of magnetic Fe3O4-Activated Carbon Nanocomposite Particles for Dye on May 14, 1958. Currently he is working as a lecturer
Removal,” Mater. Lett., vol. 62, pp. 645-647, 2008. in the Department of Chemical Engineering, Faculty of
[6] M. Senthil and C. Ramesh, “Biogenic Syhthesis of Fe3O4 Engineering and at Graduate School Program (master
Nanoparticles using Tridax Procumbens leaf Extract and Its and doctor program) University of Sriwijaya. He has
Antibacterial Activity on Pseudomonas Aeruginosa,” Journal of completed formal education engineering degree in the
Nanomaterials and Biostructures, vol. 7, no. 3, pp. 1655-1660, 2012. Department of Chemical Engineering Faculty of
[7] S. Liong, “A Multifunctional Approach to Development, Fabrications Engineering, Sriwijaya University in 1983. She has
and Characterizations of Fe3O4 Composite,” Georgia Institut of completed a master's program in ENSCT-INPT
Technology, North Ave, Atlanta, Georgia, pp. 213-217, 2005. Toulouse France in 1988, and a doctoral program in the same university in
[8] S. E. Kentish and G. W. Stevens, “Innovation in Separations 1991. He is currently also active in the field of environment and energy
Technology for the Recycling and Re-use of Liquid Waste Streams,” J. researchs.
Chem. Eng., vol. 84, pp. 149-159, 2001.

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International Journal of Environmental Science and Development, Vol. 4, No. 3, June 2013

Ridwan was born in Prabumulih City, Indonesia, on 28 Dedi Setiabudidaya was born in Bandung, West Java
Juny 1959. Doctor of Science on Solid State Physics in 1960. His bachelor degree in Physics was from
from Kyoto University. At this time, Ridwan is a Bandung Institute of Technology, Indonesia in 1984.
professor in the field physics material and work at He obtained his M.Sc degree in Exploration
National Nuclear Energy Agency, Tangerang Selatan Geophysics from Department of Earth Sciences, the
15314, Indonesia. Currently, Prof. Dr. Ridwan is a University of Leeds, UK in 1987 and his PhD from
member of Indo-Asean Magnetic Material. Department of Earth Sciences (now Department of
Earth, Ocean and Ecological Sciences, School of
Environmental Sciences), the University of Liverpool,
UK in 1992. He has worked as a lecturer at Sriwijaya University, Indonesia
Marsi was born at Petanggan, East OKU, South since 1986.
Sumatra, Indonesia on July 14th, 1960. He was
graduated from Bogor Agricultural University,
Indonesia for his Bachelor Degree in field of Soil
Science in 1983. He got his Master Degree in 1989
and Ph.D Degree in 1992 both from University of
Kentucky, USA, in field of soil chemistry. He has
worked as a lecturer at Soil Science Department,
Faculty of Agriculture, Sriwijaya University since 1985. He is interested in
soil chemistry of swampy land for his focus research since one-third of South
Sumatera area was covered by swampy land. Currently, Dr. Marsi is a
member of Indonesian Soil Science Society.

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