Effects of sintering temperature on microstructure, initial permeability and electric behaviour of Ni-Mn-Zn ferrites

https://doi.org/10.1016/j.matchemphys.2021.125250Get rights and content

Highlights

  • Ni-Mn-Zn ferrites with dense and fined grained microstructure are obtained at relatively lower sintering temperature.

  • Mössbauer spectra confirmed only sextets in low Mn-substitution (x ≤ 0.2) while x ≥ 0.3 exhibits sextets and doublet.

  • Room temperature dc resistivity values observed in the range 108–107 are found to be appreciably higher.

  • Dielectric measurements suggest the better stoichiometry and homogeneity for all the sintered compositions.

  • Improvement in the initial permeability is observed upon Mn substitution in Ni-Zn ferrites.

Abstract

The effects of sintering temperature on microstructure, initial permeability, and electrical behaviour of Ni0.5-xMnxZn0.5Fe2O4 (0.0 < x < 0.5) prepared using the precursor combustion method have been investigated. X-ray diffraction analysis confirmed the single phase cubic spinel structure of Ni0.5-xMnxZn0.5Fe2O4 (0.0 < x < 0.4) compositions sintered at 1100 °C. The Mn2+ substituent preferentially occupies tetrahedral sites as indicated by the Rietveld analysis and the increase in the IR absorption frequency of ν1 band with increasing Mn substitution. The SEM measurements have revealed homogeneous microstructures of the ferrites with narrow grain size distribution in the range 0.93μm–1.86 μm. Mössbauer spectra exhibit a superposition of two Zeeman sextets for the compositions x ≤ 0.2, a superposition of two Zeeman sextets, and a paramagnetic doublet for the compositions, x = 0.3 and 0.4, and one sextet and single quadrupole doublet for a composition, x = 0.5. The activation energy in the range 0.258 eV–0.612 eV suggests a polaron hopping type conduction mechanism in all the sintered ferrites. The dielectric constant in the range 0.057–55.21 and lower dielectric loss (10−2) imply better stoichiometry and homogeneity. The initial permeability increases at lower Mn substitution (x = 0.2) and exhibits a decrease as the Mn substitution increases. The dc resistivity, dielectric constant, and initial permeability values suggest the suitability of these ferrites for high frequency device applications.

Introduction

Soft magnetic ferrites have been subjected to detailed investigation for their electromagnetic properties which find use in technological applications such as transformer core, multilayered chip inductors (MLCIs), information storage systems, electronic communication, computer circuitry, microwave filters, etc. [[1], [2], [3], [4], [5]]. The electromagnetic properties of spinel ferrites are much better and more practicable over pure metal due to their high electrical resistivity, excellent magnetic permeability and, availability of simple and easy preparation routes, which lowers the processing cost. Furthermore, the spinel class ferrites exhibit high corrosion resistance and excellent thermal stability. Among, the spinel ferrite system, the Ni-Zn ferrites, and Mn-Zn ferrites have been investigated extensively for their electric, dielectric, magnetization as well as permeability properties which are important in specific applications [[6], [7], [8], [9]]. The Mn-Zn ferrites with low electrical resistivity and high magnetic permeability are useful for low frequency applications [[10], [11], [12]] while, the Ni-Zn ferrites with high resistivity and relatively low permeability are suitable for high frequency applications [[13], [14], [15]]. However, for the best performance in high frequency applications, ferrites with high permeability as well as high resistivity are indispensable. This has initiated a lot of research work on various mixed Ni-Mn-Zn ferrite compositions to synthesize materials with better permeability and resistivity characteristics [[16], [17], [18], [19], [20]]. It is a well known fact that the electromagnetic properties of spinel ferrites are controlled by the particle/grain size, microstructure, heat treatment (during synthesis), and cation distribution-rearrangements (during sintering) among the tetrahedral [A] and octahedral [B] interstices in the cubic lattice. These characteristics ultimately depend on the synthesis technique employed and hence there has been a lot of focus on the development of the novel synthetic routes to improve upon the electromagnetic characteristics. Various synthetic approaches adopted by the different researchers include, citrate precursor method [16], co-precipitation [[17], [18], [19]], sol-gel [20,21], combustion [21], precursor combustion method [22,23] etc. The precursor combustion method which utilizes hydrazinated carboxylate precursors has been employed for the synthesis of various materials including spinel ferrites [[21], [22], [23]] due to the autocatalytic decomposition and self-propagating combustion of these precursors. Moreover, the mixed metal oxides are formed at relatively lower temperatures. To the best of our knowledge, the structural and electromagnetic properties of mixed Ni0.5-xMnxZn0.5Fe2O4 (0.0 < x < 0.5) ferrites at lower sintering temperature from 1100 °C to 1250 °C with an interval of 50 °C is not reported so far. Here, we are reporting the effects of sintering temperature on the microstructure, electric, and initial permeability of Ni0.5-xMnxZn0.5Fe2O4 (0.0 < x < 0.5) ferrites processed using the fumarato hydrazinate precursor combustion method.

Section snippets

Synthesis of Ni0.5-xMnxZn0.5Fe2O4 (0.0 < x < 0.5)

The manganese substituted nickel zinc ferrites, Ni0.5-xMnxZn0.5Fe2O4 (0.0 < x < 0.5) ferrites were prepared using the fumarato hydrazinate precursor combustion method. All the reagents used in the synthesis were analytical grade. In a typical synthesis, the yellow coloured precipitate of nickel manganese zinc ferrous fumarato hydrazinate complex was obtained by adding an aqueous solution of mixed metal chlorides to an aqueous solution of sodium fumarate-hydrazine hydrate mixture under the N2

X-ray diffraction measurements

The XRD patterns of Ni0.5-xMnxZn0.5Fe2O4 (0.0 < x < 0.5) ferrites sintered at the 1100 oC and 1250 oC are represented in Fig. 1a and 1b, respectively, while the XRD patterns of ferrites sintered at the 1150 oC and 1200 oC are given in Fig. S1(a-b). The XRD patterns indicate the formation of cubic spinel structure [17] except for a composition x = 0.5 sintered at 1100 °C and 1150 °C. For composition x = 0.5, small impurity peaks observed at 2θ = 24.4°, 33.1°, 36.4° and 54.1° were indexed to the

Conclusions

Ni-Mn-Zn ferrite compositions processed using the precursor combustion method are found to exhibit improved electrical and initial permeability behaviour. Monophasic mixed Ni-Mn-Zn ferrites can be obtained at the lower sintering temperature of 1100 °C. Mn substitution is found to increase the lattice parameter Ni-Zn ferrites as revealed by the XRD measurement. The EDS measurement has confirmed very low zinc losses in all the sintered compositions. The room temperature dc resistivity of the

CRediT authorship contribution statement

U.B. Gawas: Conceptualization, Software, Validation, Investigation, Writing – original draft. V.M.S. Verenkar: Conceptualization, Methodology, Resources, Writing – review & editing, Supervision, Project administration. V.T. Vader: Data curation. Anil Jain: Software, Investigation. Sher Singh Meena: Software, Investigation, Writing – review & editing.

Declaration of competing interest

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

Acknowledgment

One of the authors, UBG would like to thank the Directorate of Higher Education, Government of Goa for financial assistance wide Grant No. 9/328/2026-17/SPSE-PP/DHE/3607. We would like to thank DST, New Delhi for financial support through Nano Mission Project, No. SR/NM/NS/-86/2009 and also under FIST. Also, we would like to acknowledge, Mr. V. D. Khedekar, Principal Technical Officer, and Mr. Girish Prabhu, Senior Technical Officer, CSIR-National Institute of Oceanography, Dona Paula-Goa for

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