Accepted Manuscript

Temperature-dependent phase transition: Structural and magnetic properties of

Ba0.5Sr0.5Fe12O19-CoFe2O4 nanocomposites

V. Harikrishnan, R. Ezhil Vizhi

PII: S0022-3697(17)32047-4
DOI: https://doi.org/10.1016/j.jpcs.2018.12.004
Reference: PCS 8820

To appear in: Journal of Physics and Chemistry of Solids

Received Date: 30 October 2017

Revised Date: 2 December 2018
Accepted Date: 3 December 2018

Please cite this article as: V. Harikrishnan, R. Ezhil Vizhi, Temperature-dependent phase transition:
Structural and magnetic properties of Ba0.5Sr0.5Fe12O19-CoFe2O4 nanocomposites, Journal of
Physics and Chemistry of Solids (2019), doi: https://doi.org/10.1016/j.jpcs.2018.12.004.

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Temperature-dependent phase transition: Structural and magnetic properties of

Ba0.5Sr0.5Fe12O19-CoFe2O4 nanocomposites

V. Harikrishnan and R. Ezhil Vizhi*

Materials Research Laboratory

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Department of Physics
School of Advanced Sciences, Vellore Institute of Technology, Vellore-632014, India

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* revizhi@gmail.com, rezhilvizhi@vit.ac.in

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Abstract

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Ba0.5Sr0.5Fe12O19(hard)-CoFe2O4(soft) nanocomposite ferrites synthesized using the citrate-
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gel combustion method was subjected to different annealing temperatures (Ta) (700°C,

800°C, 900°C, and 1000°C), and the resultant structural and magnetic properties were
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investigated. The microstructural characterization of nanocomposites via X-ray diffraction

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(XRD), Raman, and transmission electron microscopy (TEM) analysis at first revealed the
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dominance of soft phases annealed at 700°C and then showed the presence of hard phases at

900°C. Lattice vibrational analysis again showed a clear distinction between the bands
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corresponding to Ta at 700°C and 900°C. An increase in saturation magnetization (MS) and

coercivity (HC) was observed upon increasing the Ta. A good combination of MS (56.9 emu/g)
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and HC (3.3 kOe) was obtained at Ta = 900°C. In addition, high-temperature magnetic studies
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confirmed the dominance of soft phase with Curie temperatures of 592°C and 480°C for the

samples annealed at 700°C and 900°C, respectively. Combining these facts, a detailed

mechanism involving the domination of spinel plates and hexagonal layers was drawn. The

magneto crystalline anisotropy was evaluated and showed a maximum for Ta at 900°C. The

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extent of exchange coupling between the hard and soft phases was further analyzed by

switching field distribution curves and is discussed in detail.

Keywords: nanocomposite, X-ray techniques, sintering, structural, magnetic materials

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1. Introduction

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Rare earth-based permanent magnets (PM) play an essential role in a variety of technological

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applications, viz., magnetic recording devices, sensors and generators, PM, magnetic data

storage materials, as well as components in electrical devices such as those operating at radio

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frequency [1]. However, their increasing cost and depleting reserves have forced researchers
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to focus on suitable alternatives [2]. In the past few decades, researchers have focused on
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nanocomposite magnets which have the combined effects of hard and soft phases in a single

material, thus showing superior magnetic properties when compared with that of single-phase
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magnets [3–6]. In this context, hexaferrites have gained enormous importance in the PM
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industry because of their low price and reasonably good magnetic properties. It is well known

that they possess strong uniaxial anisotropy with the easy axis along the c direction [7].
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Similarly, spinel ferrites are also technologically attractive candidates in terms of their

potential applications in electrical components, as well as memory and microwave devices

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owing to their ability to operate at higher frequencies with minimal eddy current losses [8].
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Barium hexaferrite is one of the most important commercial hard magnetic materials

representing the class of hexagonal M-type ferrites. It has a large magnetocrystalline

anisotropy, high saturation magnetization and coercivity, and high electrical resistivity, and

the corrosion resistance of these materials make them useful as components in high frequency

devices, PM, high-density recording media, and microwave devices. On the contrary,

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CoFe2O4 belongs to the spinel ferrites category with a high Curie temperature of 520°C and

also shows relatively large magnetic hysteresis, which distinguishes it from the rest of the

spinel ferrites [9,10]. Magnetic materials with high saturation magnetization MS and high

coercivity HC are found to be useful in many applications. It should be noted that most

conventional magnetic materials possess either high MS or low HC and vice versa. In this

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context, exchange coupled composites possess high HC and MS at the same point. They

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usually possess both hard and soft magnetic phases having good exchange coupling between

them. Another important strategy which can be used in tuning the magnetic properties of

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these exchange spring magnets is by varying the weight ratios [11]. However, it is very

important to understand that annealing temperature-dependent phase transition changes also

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play a major role in exchange coupling between the hard and soft phases. It should be noted
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that Ba0.5Sr0.5Fe12O19 gives good HC. Kanagesan et al. reported Ba0.5Sr0.5Fe12O19 with a high
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HC of 5 kOe and a considerable MS of 58 emu/g [12–14]. Hence, the reason for choosing

Ba0.5Sr0.5Fe12O19 forms an important strategy to improve the BHmax of the nanocomposite

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with the combination of CoFe2O4. This combination of Ba0.5Sr0.5Fe12O19 and CoFe2O4 in the
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form of nanocomposite magnets has a potential to obtain higher BHmax when compared with

other combinations such as BaFe12O19-ZnFe2O4 and SrFe12O19-MgFe2O4. Such magnetic

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nanocomposites comprising Ba0.5Sr0.5Fe12O19 and CoFe2O4 will pave the way for its
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suitability for PM applications. One active strategy to produce PM is to process them in the
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form of (Ba,Sr) Fe12O19-CoFe2O4 nanocomposite magnets. There have been many reports on

the synthesis and properties (Ba,Sr) Fe12O19-CoFe2O4 [15,16], but very few reports are

available on the effect of the annealing temperature (Ta)-dependent phase as well as variation

of Curie temperature TC in these types of nanocomposites.

It should be noted that the Ta involved in the fabrication of nanocomposite magnets

decisively plays a major role in determining the phase formation of these magnets. In

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particular, higher Ta leads to excess grain growth, which is disadvantageous in realizing the

concept of exchange-coupled nanocomposite magnets [17]. For instance, Tyagi et al. [18]

obtained a saturation magnetization (MS) and coercivity (HC) of 48 emu/g and 2.6 kOe at

900°C, respectively, and the HC value decreased when the Ta was increased to 1000°C for

SrFe11Zn0.5Ni0.5O19. More recently, Xia et al. [19] reported a higher MS of 70 emu/g but a

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lower HC of 2.3 kOe for SrFe12O19-CoFe2O4 nanocomposites annealed at 900°C. To realize

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the full potential of nanocomposite magnets, a systematic study is therefore required to

understand the phase evolution of both hard and soft magnetic phases in these ferrite systems.

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One of the most extensively used methods for synthesizing nanocomposite magnets is the

physical method. This method involves the processing two compounds separately by means

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of any wet chemical synthesis and then subjecting the powders for milling at a particular
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weight ratio. It has to be noted that, in order to obtain good exchange coupling between the
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phases in nanocomposite magnets, the chemical method can be used [20–22]. A varying

concentration of both hard and soft ferrites in (Ba0.5Sr0.5Fe12O19)1-x(CoFe2O4)x

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nanocomposites was recently investigated by our group, in which the individual roles of both
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ferrites in achieving useful magnetic properties with good exchange coupling have been

discussed in detail [23]. As a continuation of that discussion, in this work we analyze the
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evolution of the structural and magnetic properties of hexaferrites (P63/mmc) and spinel
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ferrites (Fd3m) in Ba0.5Sr0.5Fe12O19-CoFe2O4 nanocomposites during the process of

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increasing the Ta from 700°C to 1000°C. As far as the synthesis is concerned, we have

adopted the one-step citrate gel combustion method in order to obtain strongly exchange-

coupled nanocomposite magnets [24]. In nanocomposite magnets comprising

Ba0.5Sr0.5Fe12O19 and CoFe2O4, it is critical to analyze the phase formation at every Ta and

also the substitution effect occurring in the S and S* blocks of hexaferrites which leads to the

formation of dual phases comprising the hexaferrites and spinels [25].2. Experimental

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2.1 Chemicals

Sr(NO3)2, Ba(NO3)2, Fe(NO3)3⋅9H2O, Co(NO3)2⋅6H2O, ammonium solution, and citric acid

were acquired from Merck Co. (Germany) and were used as received without further

treatment.

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2.2 Synthesis of Ba0.5Sr0.5Fe12O19-CoFe2O4 nanocomposite magnets at different Ta

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First, an aqueous solution of 0.5M Sr(NO3)2, 0.5M Ba(NO3)2, and 14M Fe(NO3)2⋅9H2O was

prepared in de-ionized water, and simultaneously 2M Co(NO3)2⋅6H2O was added to the

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homogenous solution according to the stoichiometric calculations. The molar ratio of metal

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nitrates to citric acid was kept at 1:2. The pH of the resultant solution was maintained at 7 by
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addition of ammonia solution. The homogenous solution was subjected to heating at 80°C for

2 h. As a result, a greenish gel was formed which was subjected to combustion by placing the
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beaker containing the gel in a preheated furnace maintained at 200°C for 1 h. The resultant

fluffy mass was crushed and subjected to calcination at 500°C for 5 h. The resultant fine
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powders were again subjected to annealing at four Ta values—700°C, 800°C, 900°C, and

1000°C—for 2 h. The X-ray diffraction (XRD) patterns of the samples were recorded on a
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Bruker D8 advance powder diffractometer using Cu-Kα (1.5406 Ǻ) radiation. Both field

emission scanning electron microscope (FE-SEM) and high-resolution transmission electron

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microscope (HR-TEM) were used to investigate the morphology of

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Ba0.5Sr0.5Fe12O19/CoFe2O4 nanocomposites. Their magnetic properties of at room temperature

(RT) were obtained using a Lakeshore 7407 magnetometer with a maximum applied field of

20 kOe.3. Results and discussion

3.1 Structural and morphological analysis

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The results of XRD patterns of Ba0.5Sr0.5Fe12O19-CoFe2O4 samples treated at different Ta

levels (700°C, 800°C, 900°C, and 1000oC) are displayed in Fig. 1. The patterns

corresponding to Ba0.5Sr0.5Fe12O19 were indexed with JCPDS 51-1879 and those

corresponding to CoFe2O4 were indexed with JCPDS 22-1086. The crystallite sizes of the

samples are depicted in the same figure, and they show an increasing trend with Ta. The

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Ba0.5Sr0.5Fe12O19 crystallizes in the P63/mmc space group, whereas CoFe2O4 crystallizes in

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the Fd3m space group. The sample annealed at 700°C displayed the characteristic peaks of

spinel phase assigned to CoFe2O4. It is noteworthy that the intensity of (3 1 1) reflection was

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dominating when compared with the other reflections of hard phase. Meanwhile, for 900°C,

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two important characteristic peaks of M-type hexaferrite, (1 1 4) and (1 0 7), are more
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dominant as the intensity of the spinel phase is diminished. Additional Bragg reflections

corresponding to α-Fe2O3 as a consequence of the excess amount of Fe3+ ions present during
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the synthesis process can be observed in the XRD patterns [26]. The lattice parameters do not

show much difference (shown in Table 1), and hence no solid solutions have been formed.
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Moreover, with increasing Ta, the diffraction peaks of hexaferrites became stronger when
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compared with those of the spinel ferrites. However, the formation of CoFe2O4 at lower Ta

arises due to the spinel ferrite block present in the hexaferrite unit. Meanwhile, for higher Ta,
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the other blocks consisting of hexagonal layers also come into play. Crystallite, depicted in
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Fig. 1, has been evaluated using the Scherrer formula, and it is tabulated for different phases
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in Table 2. The increase in crystallite size with the increase in annealing temperature Ta is

observed in the present case. It cannot be predicted that the phase transition domination from

spinel to hexaferrites has any correlation with increase in crystallite size of the

nanocomposite. The growth of crystallites depends on the variation of the annealing

temperature and the same has been illustrated using FE-SEM analysis. The difference in the

grain growth of BSFO and CFO has been ascribed to the grain boundary migration, which

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usually occurs via a long-range diffusion for a two-phase system with a mutual limited

solubility [3].

Raman spectra have been widely used to study the crystal lattice vibrations. In the case of

hexagonal ferrites, there are 42 Raman active modes whereas for spinel ferrites there are 5

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Raman active modes [27,28]. In the present work, a large difference has been found in the

Raman spectra for 700°C Ta and 900°C Ta (Fig. 2). The strong peaks observed in the case of

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700°C Ta were indexed for spinel ferrites; however, a weak band (A1g) representing the

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hexagonal ferrite was seen that was probably caused by the initial formation of the hexaferrite

phase as evidenced from the XRD pattern. On the contrary, for 900°C Ta the strong peaks

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were indexed to the various sublattices of Fe3+ ions. However, a weak band representing the
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spinel ferrites was seen at 190 cm-1 showing the T1g mode. The rest of the four sublattices

were found to be indexed with the standard data. In the case of 900 Ta, the dominance of both
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spinel and hexagonal blocks was confirmed from the Raman spectra. It should be noted that
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the assignments are analyzed through the intensity variations obtained from the XRD
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patterns. For Ta at 700°C, there was domination of the spinel phase, and hence T1g(1), T1g(2),

T1g(3), and Eg modes of CoFe2O4 were assigned, whereas for 900°C Ta higher domination of
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hexaferrites was found from the XRD pattern. As a result, the Raman spectra for 900°C Ta

are wholly based on the hexaferrite assignment. An increase in intensity at 300 cm-1 may
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show the higher domination of spinel ferrites than hexaferrites. All the wavenumbers for
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900°C Ta were analyzed for hard phase with only one peak representing the spinels. Fourier

transform infrared (FTIR) spectroscopy was used to analyze the stretching (symmetric and

anti-symmetric) deformations of the inter-bond angles. The wavenumber representing 2000-

400 cm-1 is depicted in Fig. 3. The ferrite bands occur because of the tetrahedral and

octahedral complex vibrations. For all samples, the ferrite bands were visible, representing

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the tetrahedral and octahedral vibrations. The different Ta did not show much variation in the

FTIR bands; however, at 800°C Ta, a split in the band was visible that was not seen in the

case of 700°C Ta.

Fig. 4(a)-(d) show the FE-SEM micrographs of samples with Ta of 700°C, 800°C, 900°C, and

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1000°C and show the presence of irregular platelets with grain sizes smaller for 700°C when

compared with those of other Ta. The Energy Dispersive X-Ray Analysis (EDAX) patterns

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are depicted in Fig. 5(a) and (b) which show the presence of all the elements and are

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comparable with those of experimental values. Table 3 shows the concentration of all

elements, which are found to be in accordance with experimental values.

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Fig. 6(a) and (b) show the HR-TEM, TEM micrographs, and Selected Area Electron
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Diffraction (SAED) patterns of 700°C and 900°C Ta. The lattice fringe spacing of 700°C Ta
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displayed a uniform set of planes (1 1 1), whereas for 900°C Ta two different sets of planes

are observed: 0.241 nm, which is consistent with the (2 2 2) reflection of CoFe2O4, and 0.179
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nm for the (4 2 2) reflection of Ba0.5Sr0.5Fe12O19. The TEM micrograph of 700°C Ta reveals

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the presence of irregular platelets with sizes ranging from 40 to 70 nm, whereas the 900°C Ta

approximately shows hexagonal platelets with a diameter of 50 nm. The SAED patterns of
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700°C and 900°C Ta confirm the presence of completed rings demonstrating the crystalline
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nature of the nanocomposites. The SAED patterns are indexed for the presence of spinel
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ferrites and hexagonal ferrites.

3.2 Magnetic property characterization

The RT hysteresis of 700°C, 800°C, 900°C, and 1000°C Ta are depicted in Fig. 7(a). The

sample treated at 700°C Ta exhibits soft magnetic behavior with an HC of 1.3 kOe and an MS

of 50.2 emu/g. Such a low value of HC may be attributed to the presence of Co2+ ions in the S

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and S* blocks of hexaferrites. When the Ta was increased to 900°C, the HC values reached a

maximum of 3.3 kOe while an MS of 56 emu/g was obtained, showing the dominance of hard

phases. Another characteristic feature of the hard and soft ferrites is their difference in Curie

temperatures (TC). It is well known that in strongly exchange-coupled nanocomposite

magnets, there is only one TC which is independent of the individual magnetic phases.

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Consequently, the TC of nanocomposites would always be higher than the volume average of

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the TC of individual phases [29]. Moreover, good exchange coupling between the two phases

also plays a major role in maneuvering the TC of the nanocomposites. In the present case, the

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700°C Ta sample exhibited a TC of 592°C, where the spinel phase is dominant; meanwhile,

the 900°C Ta exhibited a TC of 480°C, where the hard phase is dominant over other

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reflections. This result is in accordance with the fact that the TC of nanocomposites is always

higher than the volume average of the TC of individual phases involved in it. The exchange
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bias between different phases is affected by the creation of oxygen vacancies [32]. It should

be noted that as the annealing temperature is increased, the intensity of oxygen vacancies also
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increases. This considerably decreases the super exchange interaction in the lattice structure.
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As a result, the coercivity is considerably decreased. Moreover, the concentration of oxygen

ions in nanocomposite magnets is higher; hence, at higher annealing temperatures, there is

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always a possibility of oxygen vacancies. One effective strategy that can be used to lower the
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oxygen vacancies is to employ spark plasma sintering where low sintering time is required in
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order to achieve densified particles. Table 4 shows the different magnetic parameters

obtained from the hysteresis such as MS, HC, squareness ratio, K1, and BHmax. At 700°C, the

coercivity was found to be 1.3 kOe and the hysteresis was found to be conventional. This

shows that there was dominance of spinel ferrites at low annealing temperatures. However, at

higher annealing temperatures, the coercivity increased to 3.3 kOe. An increased coercivity

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would have been achieved, but oxygen vacancies hampered the exchange coupling between

the hard and soft ferrites.

Furthermore, in order to analyze the exchange coupling between the two phases, switching

field distribution curves were used, as depicted in Fig. 8(a) and (b). Moreover, smooth

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demagnetization curves show that there was good exchange coupling between the hexaferrite

and spinel phases. The switching field distribution curve shows that for 700°C Ta a peak

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appeared at higher fields whereas for higher Ta the peak shifted to lower fields. In the case of

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700°C Ta, a smooth narrow curve was seen showing the presence of a dominant single phase

of spinel ferrites, whereas for higher Ta the peak broadened. In the case of 800°C and 1000°C

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Ta, a split in the peak was observed, showing less exchange coupling between the soft and
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hard phases. On the contrary, for 900°C, the peak was found intermediate between 800°C and

1000°C Ta without any split, showing good exchange coupling between the soft and hard
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phases. It has to be noted that 900°C Ta showed good exchange coupling when compared
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with other Ta, which forms an important parameter for PM applications. Fig. 8(c) shows the
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variation in MS and HC with Ta. However, the value of HC increases with the increase in Ta,

which may be attributed to the increase in grain size and is not related with the composite
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system. Magnetic crystalline anisotropy was evaluated using the law of approach to

saturation [30].
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= 1− − + , (1)

where MS is the saturation magnetization and is the field-induced spontaneous

magnetization occurring in the magnetic domains. The material constant A arises due to the

sample in homogeneities and B represents the magnetocrystalline anisotropy contribution.

The magnetization data obtained in the field range of 15-20 kOe were plotted against 1/H2 at

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first, and straight lines were obtained. The slopes of the lines were used to determine the

anisotropy field from the relation [31]

= (2)

The first anisotropy constant was evaluated by the relation

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= (3)

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The variation in magnetocrystalline anisotropy with Ta is shown in Fig. 8(d). A large

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improvement in magnetic crystalline anisotropy was found for 800–1000°C Ta when

compared with that at 700°C Ta. This may be attributed to the increase in MS value with the

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increase in Ta.

The structure of single-phase M-type hexaferrites are explained in terms of four blocks,
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namely, an S block consisting of two spinel units (2MFe2O4) and an R block consisting of
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Ba2+ or Sr2+, Fe3+, and O2- ions forming (Ba,Sr)Fe6O11 as presented in Fig 9. The third and
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fourth blocks are named S* and R*, respectively [25]. It can be presumed that for 700°C Ta,

the Co2+ ions occupied the spinel sites (S and S*) of hexaferrites, thus forming 2(CoFe2O4),
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resulting in irregular platelets as well as rods. When the Ta is increased to 900°C, phase

formation of hexaferrites comes into play, in which R and R* blocks fully dominate, thus
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forming hexagonal platelets depicted from the TEM micrographs. Moreover, the change in
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morphology is in full accordance with the HC values of 700°C and 900°C Ta. The variation in

the case of TC can be explained by the formation of hexagonal and spinel platelets. At first,

the TC for 700°C Ta was found to be 592°C, which clearly shows the domination of spinel

ferrites, and thereafter at 900°C Ta it was found to be 480°C, which showed the domination

of hexaferrites. A detailed list of magnetic properties is compared with those found in the

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literature (Table 5). At higher annealing temperatures, a low coercivity is reported in most

studies in the literature. Meng et al. [3] reported that they had obtained a single-phase-like

magnetic hysteresis with no steps.

4. Conclusion

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Ba0.5Sr0.5Fe12O19/CoFe2O4 nanocomposites synthesized using the one-step citrate-gel

combustion method were subjected to annealing at four Ta values (700°C, 800°C, 900°C, and

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1000°C). The results indicated differences in the structural and magnetic properties of

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samples at 700°C and 900°C Ta. XRD and Raman analysis confirmed the phase

transformation from spinel to hexagonal symmetry. HR-TEM micrograph analysis showed

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the presence of dual phases with two different orientations representing hexagonal and spinel
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ferrites. In addition, a good combination of MS (56.9 emu/g) and HC (3.3 kOe) was obtained
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for the sample thermally treated at 900°C Ta, and TC was found to be 480°C. Furthermore, a

look into the step-by-step process of formation of spinels inside the hexagonal symmetry was
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analyzed using schematics, and it was concluded that the Co2+ ions got substituted in the S
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and S* blocks of hexagonal ferrites at low temperatures, thus dominating the spinel phase at

700°C Ta. Meanwhile, at higher Ta the R and R* blocks of hexagonal ferrites along with the S
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and S* blocks resulted in the formation of dual phases. The results are quite encouraging and
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indicate the potential of these materials to replace rare earth-based PMs. However, the
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present technique needs to be improved in the sintering process where spark plasma sintering

can be applied.

Acknowledgements

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The authors are thankful to the management Vellore Institute of Technology, Vellore, for
continuous support. One of the authors, HK, acknowledges the Research Associateship
offered by Vellore Institute of Technology, Vellore.

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Table. 1 Lattice parameters of spinel ferrites and hexagonal ferrites in Ba0.5Sr0.5Fe12O19-
CoFe2O4 composites.

Annealing temperature of Lattice parameter of Lattice parameter of

Ba0.5Sr0.5Fe12O19- CoFe2O4 CoFe2O4 Ba0.5Sr0.5Fe12O19
a(Å) a (Å) c (Å)
700oC 8.36 5.90 22.92

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800oC 8.37 5.89 23.08
900oC 8.38 5.90 22.92

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1000oC 8.36 5.89 23.08

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Table 2. Represents the crystallite size of samples for different Ta

Ta Crystallite size Crystallite size

corresponding to corresponding to
(311) (114)
700oC 30 -
800oC 23 43
900oC 21 46
1000oC 23 55

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Table. 3 Representing the concentration of different elements for 700oC and 900oC Ta.

700oC Ta 900oC Ta
Element Weight% Atomic% Weight% Atomic
%
OK 6.42 20.08 8.86 26.48

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Fe K 78.41 70.26 73.81 63.20
Co K 7.78 6.60 8.34 6.77

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Sr L 1.76 1.01 2.10 1.15
Ba L 5.64 2.05 6.88 2.40

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Totals 100.00 100.00

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Table .4 Magnetic parameters of Ba0.5Sr0.5Fe12O19/CoFe2O4 obtained at different Ta.

Ta of Ba0.5Sr0.5Fe12O19 Ms MR Hc R= K1 (erg/cm3) BHmax

/CoFe2O4 (emu/g) (emu/g) (kOe) MR/MS ˟106 kj/m3

700oC 50.2 23.9 1.3 0.47 0.87 1.46

800oC 56.5 29.7 3.2 0.52 1.23 2.54
900oC 56.9 30.7 3.3 0.53 1.25 2.59
1000oC

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55.1 29.2 3.3 0.52 1.21 2.54

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Method of Composition Annealing Magnetic Reference
Preparation temperature Properties
MS HC
emu/g kOe
Chemical Co- ZnFe2O4/SrFe12O19 1100oC 34 2.2 [33]
precipitation
Co-precipitation SrFe12O19/NiFe2O4 800oC 57 1.7 [34]
method 1000oC 63 2.6
900oC

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Chemical Co- SrFe12O19/NiFe2O4 48 2.6 [35]
precipitation 1200oC 59 1.2
method
Sol-gel spinning SrFe12O19/ 600oC 30 0.1 [3]

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technique Ni0.8Zn0.2Fe2O4 800oC 48 0.8
(Composite Fibres)
900oC 63 2.6

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1000oC 67 4.0
1100oC 63 2.6
One pot sol-gel (Mn0.2Ni0.4Zn0.4Fe2O4) 800oC 56 3.2 [36]

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synthesis (OP) 0.5 (BaFe12O19)0.5
Physical mixing
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(PM) 53 2.4
Sol gel process BaFe12O19/ 700oC 31 0 [37]
Ni0.8Zn0.2Fe2O4 800oC 60 1.3
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900oC 53 1.3
1000oC 57 1.2
1100oC 63 1.6
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1200oC 62 0.8
Sol Gel Auto Ni0.7Zn0.3Fe2O4 / 400oC 17 1.2 [38]
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Combustion SrFe12O19 500oC 36 2.1

600oC 51 2.5
800oC 50 0.8
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One step sol-gel Ba0.5Sr0.5Fe12O19/ 700oC 50 1.3 Present

auto combustion CoFe2O4 800oC 56 3.2 Work
method 900oC 56 3.3
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1000oC 55 3.3
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Table 5. Comparison of magnetic properties with that of the literature

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Fig. 1 Typical X-ray diffraction patterns at different Ta showing the evolution of

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Ba0.5Sr0.5Fe12O19/CoFe2O4
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Fig. 2 Raman spectra shows a wide difference between the 700oC Ta and 900oC Ta
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Fig 3. FTIR spectrum of Ba0.5Sr0.5Fe12O19/CoFe2O4 obtained at different Ta.

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Fig 4. (a) - (d) FE-SEM micrographs of 700oC, 800oC, 900oC & 1000oC Ta.
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Fig. 5 (a) & (b) EDAX pattern of 700oC Ta and 900oC Ta
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Fig 6 (a) & (b) HR-TEM, TEM and SAED patterns of 700oC and 900oC Ta showing the
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lattice fringes. SAED patterns of both Ta shows completed rings with high degree of
crystallinity.
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Fig 7 (a) Room temperature hysteresis of Ba0.5Sr0.5Fe12O19/CoFe2O4 obtained at different Ta.
(b) Temperature dependence of magnetization of Ba0.5Sr0.5Fe12O19/CoFe2O4 for 700oC &

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900oC Ta showing decrease in TC with the increase in Ta.
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Fig. 8 (a) & (b) shows the demagnetization curve and also the switching field distribution
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curves while (c) shows the variation of MS and HC with varying Ta and (d) shows the M vs
(1/H2) while (e) shows the variation of magnetocrystalline anisotropy with Ta
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Fig 9. Schematics showing morphology changes in the transformation from irregular platelets to
hexagonal platelets

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Highlights

• Ba0.5Sr0.5Fe12O19-CoFe2O4 magnetic nanocomposites were studied at annealing

temperatures (Ta) of 700°C, 800°C, 900°C, and 1000°C.

• Curie temperature (TC) was evaluated for selected samples.

• The TC for 700°C Ta showed the dominance of spinel ferrites.

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• Schematics showing the formation of dual phases have been drawn.

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Original Article Statement

Herewith I assure you that, submitted manuscript is the authors' original work and has not
been published nor has it been submitted simultaneously elsewhere. All authors have checked
the manuscript and have agreed to the submission and it will not be submitted elsewhere
before a decision is made by this journal.

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