Equilibrium synthesis and magnetic properties of BaFe12O19/NiFe2O4 nanocomposite prepared by co precipitation method

C. Thirupathy; S. Cathrin Lims; S. John Sundaram; Ahmed Hossam Mahmoud; K. Kaviyarasu

doi:10.1016/j.jksus.2019.12.019

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Original article

32 (

); 1612-1618

doi:

10.1016/j.jksus.2019.12.019

Equilibrium synthesis and magnetic properties of BaFe₁₂O₁₉/NiFe₂O₄ nanocomposite prepared by co precipitation method

C. Thirupathy^{^a}, S. Cathrin Lims^{^a}, S. John Sundaram^{^a,⁎}, Ahmed Hossam Mahmoud^{^b}, K. Kaviyarasu^{^c,^d}

a Department of Physics, Sacred Heart College (Autonomous), Tirupattur - 635601, Tirupattur District, Tamil Nadu, India

b Department of Zoology, College of Science, King Saud University, Riyadh, Saudi Arabia

c UNESCO-UNISA Africa Chair in Nanosciences/Nanotechnology Laboratories, College of Graduate Studies, University of South Africa (UNISA), Muckleneuk Ridge, PO Box 392, Pretoria, South Africa

d Nanosciences African Network (NANOAFNET), Materials Research Group (MRG), iThemba LABS-National Research Foundation (NRF), 1 Old Faure Road, 7129, PO Box 722, Somerset West, Western Cape Province, South Africa

⁎Corresponding author. johnsundaram@shctpt.edu (S. John Sundaram)

Received: 2019-9-30, Accepted: 2019-12-17, Published: 2019-03-01

Disclaimer:
This article was originally published by Elsevier and was migrated to Scientific Scholar after the change of Publisher.

Peer review under responsibility of King Saud University.

Abstract

The hard and soft magnetic nanocomposites (BaFe₁₂O₁₉/NiFe₂O₄) at the ratio 1:1 were prepared by simple mixing and heat treatment. XRD peak indicates the formation of good crystalline quality of the prepared sample. The FTIR spectra reveals the bands for metal oxygen stretching which ranges from 584 cm⁻¹ to 540 cm⁻¹ forms the tetrahedral shape in nature. However, the hexaferrite site ranges from 580 cm⁻¹ to 440 cm⁻¹ and this bands assign to Ba-O and Fe-O bonds respectively. Furthermore, the UV–visible range, the observed absorption peak indicates that the prepared sample color is congo red, the characteristic absorption peaks at ∼739 nm for BaFe₁₂O₁₉, 698 nm for NiFe₂O₄ and 780 nm for BaFe₁₂O₁₉/NiFe₂O₄. Overall, the ferrite powder seems agglomerated, but the microstructure shows its respective structure. The particle size of BaFe₁₂O₁₉ (hexagonal) is 150 nm, again the particle size of NiFe₂O₄ (cubic) is 89 nm apparently. Finally, the structure of composite (BaFe₁₂O₁₉/NiFe₂O₄₎ material seems to achieve intermediate and its particle size is 120 nm correspondingly.

Keywords

Magnetic properties

Electron microscopy

Ferrite materials

UV–vis absorbance spectroscopy

XRD phase transition

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1 Introduction

Ferrites have numerous industrial applications with excellent electric and magnetic properties (Zhidong et al., 2006), which shows promising properties in radar absorption, microwave absorption, magneto optic or perpendicular recording media, magnetic device, transformers and spintronics (Remya et al., 2016). Therefore, the magnetic nanocomposites have obvious advantage over nonmagnetic materials, these nanocomposite materials consist of hard and soft magnetic phase (Prakash et al., 2016). Which make them suitable for many different applications which include permanent magnet too (Kadi and Mohamed, 2014). The magnetic fillers of ferrite materials are spinal ferrite and hexaferrite it shows a loss nearer to dipole relaxation and ferromagnetic resonance (Couture et al., 2017). In addition, spinal ferrites can be used in EMR absorption upto 3 GHz frequency range, but hexagonal ferrite use up to the frequency range of (2–18 GHz) because of uniaxial anisotropic property (Sun et al., 2017). Hexaferrites are sub classified in different categories M,U,W,X,Y and Z with general formula like BaFe₁₂O₁₉; Ba₄Me₂Fe₃₆O₆₀; BaMe₂Fe₁₆O₂₂; Ba₂Me₂Fe₂₈O₄₆; BaMe₂Fe₁₂O₂₂ and Ba₂Me₂Fe₂O₄₁. Where Me- divalent cation of first transition series like Ni, Co, Zn and Mg. Among different system these combing hexagonal ferrite with spinal/inverse spinal ferrite have obtained noticeable attention by researcher (Bashir et al., 2019a). In order to get high crystalline mono-domain particle barium hexaferrite and nickel ferrite different synthesis techniques were adapted they are sol–gel (Bashir et al., 2019b), co-precipitation (Williams et al., 2018), solvothermal method (Tyagi et al., 2018), organic acid precursor method (Ali et al., 2017) etc., In this work the present investigation deals with barium and nickel ferrite nanocomposite followed by co-precipitation method. Due to this method is low cost and easytechnique to mass production compared with other applications (Kennedy et al., 2016). Therefore, the established nanocomposites were characterized by X-ray diffraction (XRD) pattern will reveal the crystalline nature of nanocomposites. FTIR spectrum shows the presence of functional group and vibrational bands at the surface of BaFe12O19 /NiFe2O4 nanocomposite. Finally, scanning electron microscopy (SEM) shows the morphology growth of the samples with EDAX will explain to confirm the elemental composition which is present in the compound. Lastly, VSM will show the magnetic property of the entire samples were reported in detail.

2 Experimental procedure

2.1

2.1 Synthesis of BaFe₁₂O₁₉/NiFe₂O₄ and BaFe₁₂O₁₉ /NiFe₂O₄ nanocomposites

In the present investigation barium nitrate(Ba(No₃)₂), ferric nitrate monohydrate (FeH₁₈N₃O₁₈)₁₂; nickel nitrate (Ni(No₃)₂) and ammonia solution is used for synthesizing BaFe₁₂O₁₉/NiFe₂O₄ and BaFe₁₂O₁₉/NiFe₂O₄nanocomposite by co-precipitation method.1% of barium nitrate and 12% of ferric nitrate monohydrate of molecular weight is taken (I). The, 1% nickel nitrate and 2% of ferric nitrate monohydrate of molecular weight taken (II) separately. Add the two mixture separately in a 50 ml of water, let these mixtures stir for 2 h continuously until the compound’s mixtures and dissolves completely. In that condition, after 2 h ammonia solution was added drop by drop until the precipitate forms then allowed to stir for an hour, finally, the brown precipitate deposits at the bottom and the crystal-clear liquid will deposits on the brown precipitate. Then the solution is completely washed with water and ethanol for several times, the washed nanoparticles were kept in hot air oven for 24 h at 120 °C. The dried, brown rocky like nanomaterial forms. By using the mortar, the brown rocky material was grained well. The grinded particles were put into a silicon crucible kept in a muffled furnace for 2 h up to 800 °C. Therefore, the prepared BaFe₁₂O₁₉and NiFe₂O₄nanoparticles has been done by mixing the hard and soft ferrite in weight ratio of 1:1then the sample was grained and heated for 100 °C respectively.

3 Results and discussion

3.1

3.1 X-ray powder diffraction (XRD)

The XRD pattern of barium hexaferrite (BaFe₁₂O₁₉) and nickel ferrite (NiFe₂O₄) nanopowders were calcinated under 800 °C for 2 h as shown in Fig. 1.The hard and soft magnetic nanocomposites (BaFe₁₂O₁₉/NiFe₂O₄)at the ratio 1:1 were prepared by simple mixing and heat treatment. The well-defined sharp peak indicates the formation of good crystalline quality of the prepared sample. The peaks in BaFe₁₂O₁₉ corresponds to hexagonal structure (a = b ≠ c) according to the (JCPDS file number 84–0757) and NiFe₂O₄ corresponds to cubic structure (a = b = c) according to (JCPDS file number 86–2267). All these diffraction peaks for BaFe₁₂O₁₉ (♣) and NiFe₂O₄ (♦) and no other impurity peaks has been observed even after simple mixing heat treatment. Therefore, the XRDpeak positions of those composites BaFe₁₂O₁₉/NiFe₂O₄ has both hard and soft magnetic ferrite phase and this confirms the presence of both BaFe₁₂O₁₉ and NiFe₂O₄ exist in nature (Kaviyarasu et al., 2012). The average grain size of powder sample was estimated from full width at half maximum (FWHM) by using Debye Scherer formula to determine the crystallite size, dislocation, lattice strain and inter planner distance were listed in Table 1.

XRD pattern of (a) BaFe12O19; (b) NiFe2O4 and (c) BaFe12O19/NiFe2O4.

Table 1 Powder XRD pattern of (a) BaFe₁₂O₁₉, (b) NiFe₂O₄ and (c) BaFe₁₂O₁₉/NiFe₂O_4.

Sample	BaFe₁₂O₁₉	NiFe₂O₄	BaFe₁₂O₁₉/NiFe₂O₄
Crystallite size	41 nm	40 nm	31 nm
Dislocation $(δ) = \frac{1}{L 2}$	0.493 × 10¹⁵	0.625 × 10¹⁵	1.040 × 10¹⁵
Lattice train(∑) = $\frac{β C O S θ}{4}$	0.9371 × 10⁻³	0.9935 × 10⁻³	1.0891 × 10⁻³
Inter planner distance $(d)$	0.952 × 10¹⁰	0.921 × 10¹⁰	2.0033 × 10¹⁰

3.2

3.2 Fourier transform infra-red spectroscopy (FTIR)

The FTIR spectra were recorded in mid-range 400 cm⁻¹ to 4000 cm⁻¹for barium hexaferrite (BaFe₁₂O₁₉) and nickel ferrite (NiFe₂O₄) and the composite of BaFe₁₂O₁₉/NiFe₂O₄ with the ratio 1:1 as shown in the Fig. 2. The FTIR spectra reveals the bands for metal oxygen stretching which ranges from 584 cm⁻¹ to 540 cm⁻¹ forms the tetrahedral shape. The hexaferrite site ranges from 580 cm⁻¹ to 440 cm⁻¹ and this bands assign to Ba-O and Fe-O bonds. The other bands likeCo₂-, –OH peaks are completely vanished under calcination at 800 °C for 2 h.

FTIR spectrum of BaFe12O19; NiFe2O4 andBaFe12O19/NiFe2O4.

3.3

3.3 UV–visible spectrometer

The optical properties are closely related to the atomic structure, electronic bond patterns. The optical properties of nano composites were analyzed from wavelength ranges from 200 to 2500 nm as shown in Fig. 3(a).At UV–visible range the observed absorption peak indicates that the prepared sample color is congo red, the characteristic absorption peaks at ∼739 nm for BaFe₁₂O₁₉; 698 nm for NiFe₂O₄ and 780 nm for BaFe₁₂O₁₉/NiFe₂O₄ (MobeenAmanulla et al., 2018). Therefore, the energy gap can be obtained from Tauc plot, αhγ = A(hγ − Eg)^m; where, α – is the absorption co-efficient; hγ - is photon energy; E_g - is the optical energy band gap; A – is a constant; M – is the characteristics of transition. At near infrared range transmittance occurred so the material can be used in radar absorption or microwave absorption applications (Kaviyarasu et al., 2017). The energy gap can be obtained from Tauc plot as shown in Fig. 3(b, c). The Tauc plots were plotted for direct and indirect transition and the band gap were listed in the Table2.

(a) UV–visible spectrum of BaFe12O19, NiFe2O4,BaFe12O19/NiFe2O4nanocomposites, (b) Tauc plot forindirect transition, (c) direct transition.

Table 2 Tauc plot of BaFe₁₂O₁₉;NiFe₂O₄ and BaFe₁₂O₁₉/NiFe₂O₄nanocomposites for (a) direct transition, (b) indirect transition.

Sample	Direct bandgap energy (eV)	Indirect bandgap energy (eV)
BaFe₁₂O₁₉	1.72	1.41
NiFe₂O₄	1.40	1.16
BaFe₁₂O₁₉/NiFe₂O₄	1.57	1.05

3.4

3.4 Scanning electron microscope& EDAX

The scanning electron microscopic image BaFe₁₂O₁₉, NiFe₂O₄ferrite nanoparticles as well as hard and soft magnetic phase mixed (BaFe₁₂O₁₉/NiFe₂O₄) in the ratio of 1:1 as shown in the Figs. 4–6 , the image says that the ferrites and composites are not well dispersed because of its un favorable condition (Kaviyarasu et al., 2013). Ferrite powder seems agglomerated but the micro structure shows its respective structure (Sazelee et al., 2018). The particle size of BaFe₁₂O₁₉ (hexagonal) is 150 nm as shown in Fig. 4(a-g), the particle size of NiFe₂O₄(cubic) is 89 nm as shown in Fig. 5(a-g) and the structure of composite (BaFe₁₂O₁₉/NiFe₂O₄₎ material seems to achieve intermediate and its particle size of is 120 nm Fig. 6(a-g). From the image the elongated shape says that the composition is insufficient to the formation of nanoparticles (Salwa et al., 2014). The spherical particles will also disappear by increasing its temperature (Jesudoss et al., 2017). The data which is generated by energy dispersive X-ray microanalysis has some peaks corresponds to different elements that are present in the sample and each element has a specific peak of unique energy, all comprehensively documented (Ming and Liang Gao, 2012). The EDAX spectra of BaFe₁₂O₁₉; NiFe₂O₄ and BaFe₁₂O₁₉/NiFe₂O₄ as shown in Fig. 6, the peak corresponding to the elements BA, Ni, Fe and O were observed in ferrite nano particles and the peaks of the elements Ba, Ni, Fe and O were observed in composite (Virk et al., 2011). The observed percentage of Ba, Ni, Fe and O match with the amount of respective precursor without any characteristic peak (Gurbuz et al., 2012). The atomic percentage and weight percentage were also listed.

(a-g). SEM with EDAX image for BaFe12O19 nanocomposites.

(a-g). SEM with EDAX image forNiFe2O4 nanocomposites.

(a-g). SEM with EDAX image forBaFe12O19/NiFe2O4nanocomposites.

3.5

3.5 Vibrating sample magnetometer (VSM)

The magnetic properties were studied using vibrating sample magnetometer at room temperature and various magnetic properties were listed using the curve below in the Table 3 (Sivakumara et al., 2012). Hysteresis loop are important in the construction of several electrical devices as shown in Fig. 7(a-d).

Table 3 VSM image of BaFe₁₂O_19, NiFe₂O₄ and BaFe₁₂O₁₉/NiFe₂O₄nanocomposites.

S. No	Properties	BaFe₁₂O₁₉	NiFe₂O₄	Ba₂Ni₂Fe₁₂O₂₂
1	Coercivity (Hci)	6246.3 G	190.93 G	824.04 G
2	Saturation Magnetization (Ms)	0.41713 emu	0.21146 emu	0.38348 emu
3	Retentivity (Mr)	0.19876 emu	48.071E⁻³ emu	0.12533 emu

(a) VSM image of different nanocomposites; (b) BaFe12O19; (c) NiFe2O4; (d) BaFe12O19/NiFe2O4 nanostructures.

4 Conclusion

In summary, the structure of nanocomposites BaFe₁₂O₁₉/NiFe₂O₄seems to achieve intermediate and its particle size of is 120 nm. From the XRD peak positions have confirmed the presence of both BaFe₁₂O₁₉ and NiFe₂O₄ exist in the composites. The FTIR spectra reveals the bands for metal oxygen stretching which ranges from 584 cm⁻¹ to 540 cm⁻¹ and the other bands like Co₂–, –OH peaks were completely vanished under calcination at 800 °C for 2 h. SEM image were elongated shapes that the composition is insufficient to the formation of nanoparticles. Therefore, the spherical particles have disappeared by increasing the temperature.

Acknowledgment

The authors extend their appreciation to The Researchers supporting project number (RSP-2019/108) King Saud University, Riyadh, Saudi Arabia.

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Introduction

Experimental procedure

Synthesis of BaFe12O19/NiFe2O4 and BaFe12O19 /NiFe2O4 nanocomposites

Results and discussion

X-ray powder diffraction (XRD)
Fourier transform infra-red spectroscopy (FTIR)
UV–visible spectrometer
Scanning electron microscope& EDAX
Vibrating sample magnetometer (VSM)

Conclusion

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[1] Ali K., Bahadur A., Jabbar A., Iqbal S., Imran Bashir M., Synthesis Structural, . Dielectric and Magnetic properties of CuFe₂O₄/MnO₂ Nanocomposites. J. Magn. Magn. Mater.. 2017;434:30-36.
[Google Scholar]

[2] Bashir A.K.H., Furqan C.M., Bharuth-Ram K., Kaviyarasu K., Tchokonte M.B.T., Maaza M., . Structural, optical and Mossbauer investigation on the biosynthesized α-Fe₂O₃: study on different precursors. Physica E. 2019;111:152-157.
[Google Scholar]

[3] Bashir A.K.H., Razanamahandry L.C., Nwanya A.C., Kaviyarasu K., Saban W., Mohamed H.E.A., Nwtampe S.C., Ezema F.I., Maaza M., . Biosynthesis of NiO nanoparticles for photodegradation of free cyanide solutions under ultraviolet light. J. Phys. Chem. Solids. 2019;134:133-140.
[Google Scholar]

[4] Couture P., Williams G.V.M., Kennedy J., Leveneur J., Murmu P.P., Chong S.V., Rubanov S., . Nanocrystalline multiferroic BiFeO₃ thin films made by room temperature sputtering and thermal annealing, and formation of an iron oxide-induced exchange bias. J. Alloy. Compd.. 2017;695:3061-3068.
[Google Scholar]

[5] Gurbuz A., Omar N., Ozdemir I., CahitKaronglanli A., Celik E., . Structural, Thermal and Magnetic properties of Nerium- ferrite powders substituted with Mn, Cu or Co and X (X= Sr and Ni) prepared by the Sol-Gel method. Mater. Technol.. 2012;46(3):305-310.
[Google Scholar]

[6] Jesudoss S.K., Judith Vijaya J., IyyappaRajan P., Kaviyarasu K., Sivachidambaram M., John Kennedy L., Al-Lohedan Hamad A., Jothiramalingam R., Munusamy Murugan A., . High performance multifunctional green Co₃O₄ spinel nanoparticles: photodegradation of textile dye effluents, catalytic hydrogenation of nitro-aromatics and antibacterial potential. Photochem. Photobiol. Sci.. 2017;16:766-778.
[Google Scholar]

[7] Kadi M.W., Mohamed R.M., . Synthesis and optimization of cubic NiFe₂O₄ nanoparticles with enhanced saturation magnetization. Ceram. Int.. 2014;40:227-232.
[Google Scholar]

[8] Kaviyarasu K., Raja A., Devarajan P.A., . Structural elucidation and spectral characterizations of Co₃O₄ nanoflakes. Spectrochim. Acta Part A Mol. Biomol. Spectrosc.. 2013;114:586-591.
[Google Scholar]

[9] Kaviyarasu K., Devarajan P.A., Xavier S.J., Thomas S.A., Selvakumar S., . One pot synthesis and characterization of cesium doped SnO₂ nanocrystals via a hydrothermal process. J. Mater. Sci. Technol.. 2012;28:15-20.
[Google Scholar]

[10] Kaviyarasu K., Murmu P.P., Kennedy J., Thema F.T., Letsholathebe D., Kotsedi L., Maaza M., . Structural, optical and magnetic investigation of Gd implanted CeO₂ nanocrystals. Nucl. Instrum. Methods Phys. Res., Sect. B. 2017;409:147-152.
[Google Scholar]

[11] Kennedy J., Murmu P.P., Leveneur J., Markwitz A., Futter J., . Controlling preferred orientation and electrical conductivity of zinc oxide thin films by post growth annealing treatment. Appl. Surf. Sci.. 2016;367:52-58.
[Google Scholar]

[12] Ming Liu X., Liang Gao W., . Preparation and Magnetic Properties of NiFe₂O₄ Nanoparticles by Modified Pechini Method, Journal. Mater. Manuf. Processes. 2012;27:905-909.
[Google Scholar]

[13] MobeenAmanulla A., Jasmine Shahina S.K., Sundaram R., Maria Magdalane C., Kaviyarasu K., Letsholathebe D., Mohamed S.B., Kennedy J., Maaza M., . Antibacterial magnetic, optical and humidity sensor studies of β-CoMoO₄-Co₃O₄ nanocomposites and its synthesis and characterization. J. Photochem. Photobiol., B. 2018;183:233-241.
[Google Scholar]

[14] Prakash T., Williams Grant V.M., Kennedy J., Rubanov S., . Formation of magnetic nanoparticles by low energy dual implantation of Ni and Fe into SiO₂. J. Alloy. Compd.. 2016;667:255-261.
[Google Scholar]

[15] Remya K.P., Prabhu D., Amirthapandian S., Viswanathan C., Ponpandian N., . Exchange spring magnetic behavior in BaFe₁₂O₁₉/Fe₃O nanocomposites. J. Magn. Magn. Mater.. 2016;406:233-238.
[Google Scholar]

[16] Salwa A.M., Abdel Hameed M., Ibrahim M., Nehal A., . Utilization of iron oxide bearing pellets waste for preparing hard and soft ferromagnetic glass ceramics. J. Adv. Ceram.. 2014;3(4):259-268.
[Google Scholar]

[17] Sazelee N.A., Idris N.H., Md Din M.F., Mustafa N.S., Ali N., Yahya M.S., Halim Yap F.A., Sulaiman N.N., Ismail M., . Synthesis of BaFe₁₂O₁₉ by solid state method and its effect on hydrogen storage properties of MgH₂. Int. J. Hydrogen Energy. 2018;43:20853-20860.
[Google Scholar]

[18] Sivakumara P., Ramesh R., Ramanand A., Ponnusamy S., Muthamizhchelvan C., . Preparation and properties of nickel ferrite (NiFe₂O₄) nanoparticles via sol-gel auto-combustion method. Mater. Res. Bull.. 2012;46:2204-2207.
[Google Scholar]

[19] Sun L., Zhang Z., Wang L., Ju E., Cao Y., . Zhang, Structural, dielectric and magnetic properties of NiFe₂O prepared via sol-gel auto-combustion method. J. Magn. Magn. Mater.. 2017;421:65-70.
[Google Scholar]

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