Enhancement in the magnetoelectric and energy storage properties of core-shell-like CoFe2O4−BaTiO3 multiferroic nanocomposite

doi:10.1016/j.jallcom.2021.160875

Journal of Alloys and Compounds

Volume 883, 25 November 2021, 160875

https://doi.org/10.1016/j.jallcom.2021.160875 Get rights and content

Highlights

•
Abnormal relaxor-like behavior is observed in the prepared composite.
•
Core-shell-like morphology reduced leakage current and improved interfacial coupling.
•
Enhanced energy storage efficiency and magnetoelectric coefficient are obtained.

Abstract

Herein we report the development of a core-shell-like $Co {Fe}_{2} O_{4} - BaTi O_{3}$ multiferroic nanocomposite (1:1 wt ratio) for their enhanced magnetoelectric coupling and energy storage density by the wet chemical route. Rietveld refinement analysis of the XRD pattern verified the formation of cubic spinel ( $Co {Fe}_{2} O_{4}$ ) and tetragonal perovskite ( $BaTi O_{3}$ ) structures. Whereas the SEM and EDX analysis confirmed the formation of core-shell-like morphology in the composite. The temperature dependence of dielectric permittivity showed two distinct peaks corresponding to the constituent phases´ structural phase transitions. However, the frequency dependence of low-temperature peak revealed an abnormal relaxor-type behavior, which is elucidated due to intrinsic structural defects that might cause alteration in the octahedron arrangement in $BaTi O_{3}$ . Impedance spectroscopy analysis was utilized to calculate the activation energy (E_a) of respective phases, which was found to be>1 eV that confirms the dominance of doubly ionized oxygen vacancies in governing the thermally stimulated conduction process. It was found that the prepared composite exhibited high dielectric permittivity (~2700) and moderate values of saturation magnetization (20 emu/g) and polarization (6.2 μC/cm²) along with low remnant polarization (3 μC/cm²) at room temperature. Moreover, we also observed enhanced energy storage efficiency (67%) and magnetoelectric coefficient (0.18 V/cm Oe), which are explained due to strong interfacial coupling and reduced leakage current, making this composition promising for multifunctional device applications.

Graphical Abstract

Relaxor-like ferroelectric behavior is observed in the core-shell-like multiferroic nanocomposite, which exhibits enhanced ME coupling and energy storage efficiency and is promising for multifunctional device applications.

Introduction

A family of materials that exhibit the ferromagnetic and ferroelectric behavior simultaneously is known as multiferroic materials. These materials have received considerable attention in the last decades due to their unique magnetoelectric (ME) effect and promising applications such as memory storage, sensors, spintronics, and energy storage devices [1], [2], [3]. Usually, the single-phase multiferroics are relatively rare and reveal a weak ME effect below or near room temperature, due to which their utilization in the applied applications is limited [4]. However, to improve the ME coupling for functional applications, multiferroic composites consisting of the magnetic and ferroelectric phases have been developed [5]. Their respective corresponding magnetic and electric field modifies the magnetic and electrical properties of an overall composite. The ME coupling effect in multiferroic composites depends highly on the properties of participating phases, interfaces, size, and connectivity between the individual phases [6]. Different production routes have been investigated to prepare these multiferroic systems, which conserves the constituent phases' fundamental features and improves the ME coupling coefficient of prepared composites [7], [8], [9], [10]. However, many inherent preparation problems such as atomic diffusion and unwanted chemical reactions among the constituent phases can affect the interface, altering its chemical and structural characteristics and lowering the coupling [11]. To suppress these problems, core-shell nanostructures consisting of ferromagnetic and ferroelectric materials have been reported as one of the possible ways to improve the ME coupling because of the availability of a large interfacial area for probable coupling among the magnetic and ferroelectric properties [12], [13].

Among the most prevalent ferroelectric material in core-shell structured multiferroic composites are barium titanate ( $BaTi O_{3}$ ) because of its better chemical stability, high spontaneous polarization (19 μC/cm²), high dielectric permittivity (~10³), low dielectric tangent loss (~0.01), and high resistivity (~10⁹ Ωcm) at room temperature [14], [15]. So far, different core-shell-like multiferroic nanostructures have been synthesized such as ${Fe}_{3} O_{4} - BaTi O_{3}$ , $Co {Fe}_{2} O_{4} - BaTi O_{3}$ , $α {Fe}_{2} O_{3} - BaTi O_{3}$ , ${Ni}_{0.5} {Zn}_{0.5} {Fe}_{2} O_{4} - BaTi O_{3}$ , ${Co}_{1 - x} {Ni}_{x} {Fe}_{2} O_{4} - BaTi O_{3}$ , $Mg {Fe}_{2} O_{4} - BaTi O_{3}$ etc. [16], [17], [18], [19], [20], [21]. From these investigations, it has been found that the core-shell morphology, geometry of core size, interfacial interactions between the core and shell, and the structural compatibility among the ferromagnetic (spinel ferrites) and ferroelectric (perovskite) materials play an essential role in improving the multiferroic properties in these nanocomposites. However, in the above-mentioned multiferroic composites, cobalt ferrite ( $Co {Fe}_{2} O_{4}$ ) is considered to be a key magnetic phase due to its high values of saturation magnetization (~80 emu/g), magnetocrystalline anisotropy (~10⁵ J/m³), and coercive field (~0.5 T), and most importantly $Co {Fe}_{2} O_{4}$ shows the enhanced value of magnetostrictive coefficient [22]. Hence, to achieve a high ME coefficient, the magnetic phase in the composites should have large saturation magnetization values and remnant magnetization. Since the most studied multiferroic nanocomposite is $Co {Fe}_{2} O_{4} - BaTi O_{3}$ made of the magnetostrictive $(Co {Fe}_{2} O_{4})$ core and the piezoelectric $(BaTi O_{3})$ shell [23]. The highest ME effect was achieved for $(0.5) Co {Fe}_{2} O_{4} - (0.5) BaTi O_{3}$ composition in the core-shell $Co {Fe}_{2} O_{4} - BaTi O_{3}$ composites [24]. Whereas Chaudhuri et al. [25] found a significant enhancement in the magnetic, dielectric, and magnetoelectric properties of core-shell $Co {Fe}_{2} O_{4} :BaTi O_{3}$ nanocomposites than that of mixed structure sample. Duong et al. [26] reported that core-shell structured $Co {Fe}_{2} O_{4} - BaTi O_{3}$ composites with $Co {Fe}_{2} O_{4}$ in core showed the highest ME coefficient value in comparison to the similar type of composites with $BaTi O_{3}$ in core and layered structures. Gao et al. [27] obtained a considerable improvement in the magnetic, ferroelectric, and magnetoelectric properties of $Co {Fe}_{2} O_{4} - BaTi O_{3}$ core-shell structured composite with decreasing the core size. These results were explained in terms of overall enhancement in the interfacial coupling effect due to decreased core size. Moreover, a lot of work has already been reported on the ME properties of $Co {Fe}_{2} O_{4} - BaTi O_{3}$ core-shell nanocomposites, and the reported values of ME coefficient are typically ranging from 0.1 mV/cm Oe to 58 mV/cm Oe [28], [29], [30], [31]. However, these obtained values of ME coefficient are less than the theoretically predicted ME values for these composites [32], which is explained by the formation of some charge leakage paths by the magnetostrictive phase that makes it difficult for the ferroelectric phase to polarize fully. Therefore, to achieve high values of ME coefficient, the prepared core-shell composites should be in the form of nanoparticles where every particle has its magnetic core entirely enclosed by a ferroelectric shell to prevent charge leakage problems. However, to avoid losing the core-shell structure in the pelletized sample, comparatively low sintering temperature was employed, resulting in low density and lack good ferroelectric properties [33].

Recently, few research groups have explored the prospective of multiferroic materials in energy storage applications due to their moderate energy storage density and energy storage efficiencies [34], [35]. The ferroelectric relaxor materials are considered favorable materials for getting high energy storage density because of their high polarization and low remnant polarization [36]. Therefore, the relaxor type multiferroic composites might be preferred for improving the energy storage density in these materials. It has been reported that abnormal relaxor-like behavior was observed in the $(x) BaTi O_{3} - (1 - x) Co {Fe}_{2} O_{4}$ composites, which might be related to the intrinsic defects and compositional variation in these composites with a different relaxing degree [37]. So, the purpose of this study was to explore the magnetic, ferroelectric, and magnetoelectric properties along with temperature-dependent (303–773 K) dielectric properties for the prepared relaxor type $(0.5) Co {Fe}_{2} O_{4} - (0.5) BaTi O_{3}$ nanocomposite, which has not been reported before to the best of our knowledge. Here, we also presented simple, cost-effective wet chemical routes to obtain core-shell-like multiferroic nanocomposite, which exhibits an enhanced value of ME coefficient (0.18 V/cm.Oe) and energy storage efficiency (67%) in comparison to the reported values, making these nanocomposites interesting for multifunctional device applications.

Section snippets

Experimental

$Co {Fe}_{2} O_{4} - BaTi O_{3}$ core-shell nanocomposite (1:1 wt ratio) was synthesized by a two-step method using a wet-chemical route. Firstly, pure cobalt ferrite ( $Co {Fe}_{2} O_{4}$ ) was prepared by the co-precipitation method in which the stoichiometric amounts of iron nitrate [Fe(NO₃)₃·9H₂O, Sigma-Aldrich] and cobalt nitrate [Co(NO₃)₂·6H₂O, Sigma-Aldrich] were mixed in 150 ml of deionized water and then stirred to get a homogenous solution. Here, the concentration of metal ions was 2 M. The mixed solution was heated

Results and discussion

Fig. 1 shows the X-ray diffraction (XRD) pattern for the prepared $(0.5) Co {Fe}_{2} O_{4} + (0.5) BaTi O_{3}$ composite sintered at 1000 °C for 2 h. One can see that sharp and well-defined peaks are observed, confirming the presence of cubic spinel structure for ferrite ( $Co {Fe}_{2} O_{4})$ phase and tetragonal perovskite structure for ferroelectric ( $BaTi O_{3})$ phase. Here, the absence of any other distinctive peak indicates no intermediate phase developed at the interface between the constituent phases. Moreover, the structural

Conclusions

In summary, $(0.5) Co {Fe}_{2} O_{4} + (0.5) BaTi O_{3}$ multiferroic nanocomposite have been successfully synthesized by a combination of co-precipitation and sol-gel method. The phase purity and the coexistence of spinel $Co {Fe}_{2} O_{4}$ and perovskite $BaTi O_{3}$ phases have been confirmed by the Rietveld refinement analysis of the XRD pattern. SEM and EDX analysis have confirmed the core-shell-like morphology of the composite. Dielectric measurements exhibited ferroelectric and ferrimagnetic behavior at low and high

CRediT authorship contribution statement

M. Atif: Conceptualization, Supervision, Writing - review & editing. S. Ahmed: Data curation, Investigation, Writing - original draft. Atta Ur Rehman: Formal analysis, Validation. S. Bashir: Investigation. N. Iqbal: Resources. Z. Ali: Writing - review & editing. W. Khalid: Software, Validation. M. Nadeem: Conceptualization, Resources.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgment

Authors appreciate the financial support provided by the Higher Education Commission (HEC), Pakistan, via research grants No. 5232/Federal/NRPU/R&D/HEC/2016 and TDF-044/2017.

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^☆: Dedicated to Prof. Dr. Reiko Sato Turtelli (1943–2020) for her contributions in the field of magnetic materials.

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Enhancement in the magnetoelectric and energy storage properties of core-shell-like CoFe2O4−BaTiO3 multiferroic nanocomposite☆

Highlights

Abstract

Graphical Abstract

Introduction

Section snippets

Experimental

Results and discussion

Conclusions

CRediT authorship contribution statement

Declaration of Competing Interest

Acknowledgment

Compos. Part A: Appl. Sci. Manuf.

J. Magn. Magn. Mater.

Compos. Part B: Eng.

J. Magn. Magn. Mater.

Ceram. Int.

J. Magn. Magn. Mater.

J. Magn. Magn. Mater.

Ceram. Int.

J. Magn. Magn. Mater.

J. Magn. Magn. Mater.

Ceram. Int.

Scr. Mater.

J. Alloy. Compd.

Ceram. Int.

J. Phys. Chem. Solids

Ceram. Int.

Chem. Phys. Lett.

Mater. Chem. Phys.

Compos. Part B: Eng.

Mater. Sci. Eng.: B

Prog. Solid State Chem.

Ceram. Int.

Multiferroic and magnetoelectric materials

Nature

Electric polarization reversal and memory in a multiferroic material induced by magnetic fields

Nature

Fenómenos magnetoeléctricos en sistemas monobásicos y composites

Bol. Soc. Esp. Ceram. Vidr.

Magnetoelectric coupling effects in multiferroic complex oxide composite structures

Adv. Mater.

Hysteretic magnetoelectric behavior of CoFe2O4–BaTiO3 composites prepared by reductive sintering and reoxidation

J. Mater. Chem. C.

Magnetic, dielectric and magnetoelectric propertiesin (1-x)Pb(Zr0.52Ti0.48)O3+ (x)CoFe2O4 composites

J. Mater. Sci.: Mater. Electron.

Enhancement in the magnetoelectric and energy storage properties of core-shell-like ${CoFe}_{2} O_{4} - BaTi O_{3}$ multiferroic nanocomposite☆

Hysteretic magnetoelectric behavior of CoFe₂O₄–BaTiO₃ composites prepared by reductive sintering and reoxidation

Magnetic, dielectric and magnetoelectric propertiesin (1-x)Pb(Zr_0.52Ti_0.48)O₃+ (x)CoFe₂O₄ composites