Crystallization kinetics and magnetic properties of Fe63.5Co10Si13.5B9Cu1Nb3 nanocrystalline powder cores

https://doi.org/10.1016/j.jnoncrysol.2011.09.008Get rights and content

Abstract

Amorphous ribbons of the alloy Fe63.5Co10Si13.5B9Cu1Nb3 were prepared by the standard single copper wheel melt spinning technique in air and their crystallization kinetics was analyzed by non-isothermal differential scanning calorimetry (DSC) measurements. The crystallization activation energies (Ex, Ea1 and Ea2) of amorphous ribbons calculated from Kissinger model were 448, 385 and 396 kJ/mol for the first and the second crystallizations, respectively. The Avrami exponent n was calculated from the Johnson–Mehl–Avrami (JMA) equation and was used to identify the crystallization mechanism for the amorphous ribbons. The ribbons were milled into different sized flakes, which were molded subsequently to cores using 3 wt.% epoxy as a binder. The effective permeability of the cores showed high frequency stability and increased with the size of the flakes. For the cores made from small sized flakes (− 75 μm), the quality factor was increased at high frequencies, which was attributed to the reduction in the eddy current loss.

Highlights

► The crystallization activation energies were calculated. ► The mechanism for the crystallite growth was discussed. ► The effective permeability and quality factor of the cores were studied.

Introduction

The magnetic properties of Fe-based nanocrystalline alloys have been extensively studied since Yoshizawa et al. [1] reported the excellent soft magnetic behaviors of these nanocrystalline alloys. In particular, it was found that adding small amounts of Cu and Nb to the Fe–Si–B amorphous alloys can significantly improve their soft magnetic properties after partial devitrification through isothermal annealing [2]. The alloy elements Cu and Nb play an important role in the formation of nanostructure in the Fe–Si–B–Cu–Nb alloys. Cu segregates at the initial stage of crystallization to form Cu-rich clusters that facilitate nucleation of α-Fe (Si) grains. Rejection of insoluble and slow diffusing Nb atoms to the grain interfaces hinders the grain growth, which leads to a decrease in crystallization kinetics and reduction in grain size [2], [3], [4]. The excellent soft magnetic properties are attributed to the ultrafine structure composed of α-Fe (Si) nanocrystallites in a residual amorphous matrix [5]. In such a structure, the positive magnetostriction of the amorphous phase can be compensated by the negative magnetostriction of the nanocrystalline α-Fe (Si) phase. Furthermore, since the size of nanocrystallites (~ 10–15 nm) is smaller than the ferromagnetic exchange interaction length (about 35 nm for FeSiBCuNb amorphous/nanocomposite system), ferromagnetic exchange coupling between the nanocrystalline α-Fe (Si) grains and amorphous matrix evens out of the magnetocrystalline anisotropy [6]. As a result, ultrasoft magnetic properties with high saturation, very high permeability, low frequency losses, low coercivity and near zero magnetostriction are obtained [7], [8].

In recent years, many studies have been made on the fabrication of Fe-based nanocrystalline and amorphous alloy powder cores [9], [10], [11]. Most of these studies have been centered on applying the melt spinning and in-rotating-water quenching techniques to produce soft magnetic materials which are mostly in the form of ribbons or wires. Ribbons and wires are satisfactory forms for a range of applications such as sensors and pulse generators, but are not suitable for applications where large or complex shaped components are required. The ball milling technique combines the possibility of phase formation with a product material which is in powdered form, and therefore is suitable for compaction and densification in a variety of shapes. The soft magnetic properties of nanocrystalline alloys are significantly changed during the fabrication process of consolidated cores. These changes include crystallization heat treatment, fragmentation of the crystallized ribbons by milling, ball milling, compacting and stress relief annealing, during which processes the magnetic properties such as permeability and core loss will be changed. The soft magnetic behavior is directly related to the size and shape of fragmented particles and the size of grains within the particles [12], [13]. The crystallization kinetics is very important for the nanocrystalline/amorphous matrix structure materials, as it provides the ability to tailor the microstructure. The amount of the nanocrystalline phase formed within the matrix can be controlled to achieve the desired magnetic performance. The aim of this paper is to investigate the effects of substitution of small amounts of Fe with Co in Fe63.5Co10Si13.5B9Cu1Nb3 alloy on the crystallization kinetics and to study the effect of permeability and quality factor of the nanocrystalline alloy powder cores.

Section snippets

Experimental

The master alloy ingot with a nominal composition of Fe63.5Co10Si13.5B9Cu1Nb3 was prepared by arc-melting of high purity metals in a high-purity argon atmosphere. The ingot was re-melted at least three times to ensure the homogeneity. The amorphous ribbon was subsequently produced by the standard single copper wheel melt spinning technique in air. The crystallization kinetics of the as-spun sample was investigated using the technique of differential scanning calorimetry (DSC: Thermal Analysis

Results

The room-temperature powder XRD patterns of Fe63.5Co10Si13.5B9Cu1Nb3 alloy are presented in Fig. 1. For the rapidly quenched ribbon (Fig. 1a), the diffraction pattern exhibits only one broad band centered at around 2θ = 45° and no diffraction peaks of crystalline phases were detected, indicating that the quenched ribbon was fully amorphous. The ribbon annealed at 500 °C remained amorphous but began to crystallize at 550 °C (Fig. 1b and c). The ribbons annealed at 550 °C and 600 °C exhibited a

Discussion

The average grain size of α-Fe (Co, Si) phase (D) was determined from the XRD patterns using the Scherrer relationship [16]:D=0.9λσcosθwhere λ is the X-ray wavelength (λ = 1.54056 Å), 2θ is the angle of the dominant Bragg maximum and the σ (rad) is the full-width at the half-maximum of the diffraction peak. The average grain sizes determined were 19 nm, 25 nm for samples annealed at 550 °C and 600 °C, respectively. It is useful to point out that the average grain sizes were larger than that of the

Conclusions

Crystallization kinetics of the Finemet-type amorphous alloy Fe63.5Co10Si13.5B9Cu1Nb3 has been studied. The average grain sizes of the crystalline phase in the alloy were 19 nm, 25 nm after annealing at 550 °C and 600 °C, respectively, for 1 h in a vacuum furnace. The activation energies (Ex, Ea1 and Ea2) for the growth of crystalline phase were 448, 385 and 396 kJ/mol for the first and the second crystallizations, respectively. The value of the Avrami exponent n estimated was 1.74, indicating that

Acknowledgments

This work was supported by the Hubei Province Key Laboratory of Systems Science in Metallurgical Process under Grant No. C201020, the Hubei Provincial Department of Education under Grant No. D20111103 and the National Natural Science Foundation of China under Grant nos. , .

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