Low temperature sintering and ferromagnetic properties of Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites doped with BaO–ZnO–B2O3–SiO2 glass

Accepted Manuscript Low Temperature Sintering and Ferromagnetic Properties of Li0.43Zn0.27Ti0.13Fe2.17O4 Ferrites Doped with BaO-ZnO-B2O3-SiO2 Glass Dainan Zhang, Xiaoyi Wang, Fang Xu, Jie Li, Tinchuan Zhou, Lijun Jia, Huaiwu Zhang, Yulong Liao PII:

S0925-8388(15)31047-1

DOI:

10.1016/j.jallcom.2015.09.071

Reference:

JALCOM 35346

To appear in:

Journal of Alloys and Compounds

Received Date: 18 June 2015 Revised Date:

29 August 2015

Accepted Date: 8 September 2015

Please cite this article as: D. Zhang, X. Wang, F. Xu, J. Li, T. Zhou, L. Jia, H. Zhang, Y. Liao, Low Temperature Sintering and Ferromagnetic Properties of Li0.43Zn0.27Ti0.13Fe2.17O4 Ferrites Doped with BaO-ZnO-B2O3-SiO2 Glass, Journal of Alloys and Compounds (2015), doi: 10.1016/ j.jallcom.2015.09.071. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

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Low Temperature Sintering and Ferromagnetic Properties of

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Li0.43Zn0.27Ti0.13Fe2.17O4 Ferrites Doped with BaO-ZnO-B2O3-SiO2

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Glass

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Dainan Zhang, a,b Xiaoyi Wang, a Fang Xu,a Jie Li, a Tinchuan Zhou, a Lijun Jia, a Huaiwu

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Zhang, a and Yulong Liao, a∗ a

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b

State Key Laboratory of Electronic Thin Film and Integrated Devices, University of Electronic Science and Technology, Chengdu 610054, China

Department of Electrical and Computer Engineering, University of Delaware, Newark, Delaware 19716, USA Abstract

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In this study, effects of a BaO-ZnO-B2O3-SiO2 (BZBS) glass on the ferromagnetic

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properties of Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites were systematically investigated. Through

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the solid-state reaction process, it was observed that a pure spinel phase was obtained with

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the sintering temperature raging from 880oC to 920oC, indicating the compatibility of

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co-firing with silver. Results revealed that the addition of BZBS glass significantly

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promoted

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Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites. With an optimized

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the saturation induction was increased

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9.3 GHz was dramatically reduced from ~800 to 275 Oe. This study indicates that BZBS

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glass is a promising candidate for low temperature co-fired ceramics (LTCC).

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and

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growth

enhanced

ferromagnetic

properties

of

the

addition of BZBS glass (2.0 wt.%),

from ~100 to 285 mT and the FMR line width at

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grain

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Keywords: Li-Zn-Ti ferrites; BZBS glass; LTCC

∗ Corresponding author: Tel.: +86-28-83201440; Fax: +86-28-83202556 Email address: [email protected] (Y.L.) 1

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Introduction

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Low temperature co-fired ceramics (LTCC) have been widely researched in recent

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years on account of their multi-functionalities and high performances, which are crucial

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for the development of miniaturizing microwave modules and devices.[1-4]

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acknowledged that ceramics co-firing with silver at low temperature (< 950oC) is the key

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process of manufacturing LTCC devices.[5,

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material, Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites, were found have superior ferromagnetic

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properties in our earlier study, such as high saturation induction and relative low

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ferromagnetic resonance linewidth at high frequency. Nevertheless, they need to be

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sintered above 1000oC by traditional methods.[7-10] Apparently, it is hardly to make

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Li-Zn-Ti ferrites co-firing with silver by traditional methods due to the high sintering

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temperature. In general, there are two common sintering agents to reducing the sintering

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temperature, namely adding glass and low melting point oxides (B2O3, Bi2O3 etc.).[11-14] It

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was believed that adding glass is an easier and effective way to realize excellent electrical

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properties together with acceptable densification at the low temperature.[15]

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As one kind of important gyromagnetic

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It is

In this study, , BaO-ZnO-B2O3-SiO2 (BZBS) glass was chosen as the sintering agent

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to reduce the sintering temperature of Li-Zn-Ti ferrites, because the BZBS glass has a

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relatively low melting temperature (575oC).[16] Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites doped with

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0.0 wt.% to 4.0 wt.% BZBS glass were prepared using a low-temperature ceramic

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sintering process (from 880 oC to 920 oC). The addition of BZBS glass is expected to

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facilitate grain growth of the ferrites and form a more compact structure under a relatively

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low temperature (below 950

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Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites were discussed and investigated.

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Experimental Procedure

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o

C). Structural and ferromagnetic properties of the

Li-Zn-Ti ferrites with chemical composition of Li0.43Zn0.27Ti0.13Fe2.17O4 , and BZBS 2

ACCEPTED MANUSCRIPT glass with mass proportion x wt.% (x=0.0, 0.5, 1.0, 2.0 3.0 and 4.0) were synthesized by a

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solid-state reaction method. Firstly, High purity raw materials (Li2CO3, ZnO, TiO2, and

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Fe2O3) were weighed according to the required stoichiometric formulation of

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Li0.43Zn0.27Ti0.13Fe2.17O4. The batched powders were mixed and milled for 4 h using a

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planetary mill with steel balls as milling media and then pre-sintered at 800oC for 2 h. As

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for the synthesis of BZBS glass, 10 wt.% BaCO3, 40 wt.% ZnO, 40 wt.% B2O3 and 10 wt.%

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SiO2 were mixed and milled for 6 h using zirconia balls and then oven-dried at 90oC for

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24 h; after drying and sieving, the powders were then melted in an alumina crucible at

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1300°C for 1 h, followed by quenching to room temperature. Subsequently, the

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pre-sintered ferrite powders were mixed with various amount of BZBS powders and then

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wet-milled for 6 h. The dried mixtures were granulated with 8 wt.% polyvinyl alcohol as a

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binder, sieved through a mesh of 100 µm, and then pressed into toroidal samples (∅18

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mm× 8 mm) at 10 MPa. Finally, samples were sintered in air at 880oC, 900oC, and 920oC

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for 2 h.

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The phase formation was characterized by X-ray diffraction (XRD) using CuKα

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radiation (D/max 2400; Rigaku, Tokyo, Japan), and the scanning speed was 5°/min at a

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step of 0.02°. The microstructure properties of the Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites doped

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with various amount of BZBS glass were observed using a scanning electron microscope

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(SEM; JSM6490LV, JEOL, Tokyo, Japan). The volume densities of the samples were

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measured by the Archimedes method. The saturation induction and coercivity were tested

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by an Iwatsu BH analyzer (SY8232) in an alternating magnetic field of 1600 A/m at 1 kHz.

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As for FMR line width (∆H), the sample should be ground into a single sphere with

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diameter of about 1.0 mm firstly and then was measured in TE106 perturbation method

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cavity at 9.3 GHz.

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Results and Discussion

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ACCEPTED MANUSCRIPT Figure 1 shows x-ray diffraction (XRD) patterns of the Li0.43Zn0.27Ti0.13Fe2.17O4

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ferrites sintered under different temperatures (880oC, 900oC, and 920oC) with various

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proportions of BZBS glass from 0.0 wt.% to 4.0 wt.%. Almost all of the samples exhibit

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characteristic peaks of spinel structure, except a weak impurity peak at around 2θ = 33°

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(possibly α-Fe2O3) could be detected due to Li segregation.[9] It should be noted that as the

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BZBS glass content increased above 0.5 wt.%, the impurity peaks disappeared. The

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corresponding x-ray diffraction peaks can be indexed to (220), (311), (222), (400), (422),

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(511),

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Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites was well preserved during the sintering process after

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BZBS glass was added. The XRD results suggest that spinel phase was successfully

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formed when the sintering temperature ranged from 880oC to 920oC, and BZBS glass is an

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applicable sintering aid for low temperature co-fired Li-Zn-Ti ferrites.

of

spinel

structure,

indicating

the

spinel

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SEM micrographs of the Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites

structure

of

doped with x wt.% (x=0.0,

0.5, 1.0, 2.0 3.0 and 4.0) of BZBS glass are presented in Fig .2 (sintered at 920oC). It can

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be seen that with increasing doping content, the grain size of the Li-Zn-Ti ferrites

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significantly increased from less than 1 µm to almost 7 µm (see Fig .2(a) and Fig .2(d)). It

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could be contributed to a rapid grain growth resulted from the formation of a thin layer of

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glass-rich liquid phase. Meanwhile, intragranular pores can be easily discerned when there

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was not sufficient BZBS glass (Fig .2(b) and Fig .2(c))

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pores when doped with 2.0 wt.% of BZBS glass (Fig .2(d)). When the BZBS glass content

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exceeded 2.0 wt.%, further grain growth is restricted and some small grains could not

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combine with large grains, see Fig .2(e) and Fig .2(f). It is considered that excessive liquid

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phase presented on grain boundaries would bring in an additional resistance for sintering

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and competitive grain growth. It should be noted that grain edges of the samples doped

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with 0.0 wt.% ~ 1.0 wt.% BZBS glass are hackly, nevertheless the grain edges are quite

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smooth when doped with 2.0 wt.% ~ 4.0 wt.%, which could be explained by that the

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hackly edge embossments dissolved in glass liquid during the sintering process. In a word,

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the SEM results reveal that the grain growth of the Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites was

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intensely influenced by addition of BZBS glass. Figure 3 shows the saturation induction (Bs) value of the Li0.43Zn0.27Ti0.13Fe2.17O4

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ferrites with various amounts of BZBS glass sintered under different temperatures. Firstly,

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it was observed that the Bs values for all the samples sintered at different temperature

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(880oC, 900oC, and 920oC) showed a similar tendency. Bs value rapidly increased with the

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adding of BZBS glass and achieved its maximum when the addition amount was 2.0 wt.%.

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Further increasing the BZBS glass had no benefit on the enhancement of Bs value; on the

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contrary, it decreased the Bs value. For the initial Bs increase, it can be explained that a

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moderate amount of BZBS glass promoted the grain growth and the grain size could reach

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about 7µm. Therefore with the proportion of large size grains increased, the degree of

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crystallization was promoted and subsequently the Bs value was enhanced. For the

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thereafter Bs decrease, it can be explained that too much nonmagnetic liquid phase was

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formed and then diluted the Li-Zn-Ti ferrites and finally decreased the Bs value. It can be

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concluded that an optimal amount of BZBS glass could strongly enhanced the Bs value,

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indicating the successful synthesis of Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites at low temperature.

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The coercivity (Hc) of the samples sintered at different temperatures was shown in

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Fig. 4. Hc decreased rapidly and achieved its lowest value (from ~800 to 275A/m) when

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2.0 wt.% of the BZBS glass was added. It was reported that the Hc value is inversely

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proportional to grain size.[17] For this work, it could be confirmed from the SEM results

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that the sample doped with 2.0 wt.% BZBS glass possessed the maximum size of grains

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(Fig .2(d)), and the lowest Hc value (275 A/m) was observed consequently. The sample

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doped with 0.0 wt.% BZBS glass possessed the minimum size of grains (Fig .2(a)) and the 5

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the solid phase reaction could be accelerated and reacted more thoroughly. Subsequently,

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the densification degree of the sample was promoted (Fig .2(d)) and finally leaded to high

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Bs value. Moreover, for the same BZBS glass doping amount, Hc of the samples was

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found decreased with the elevation of sintering temperature from 880 to 920 oC. This

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could be attribute to the bigger grains were formed with the increased sintering

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temperature, which finally decreased the coercive force. It should be focused on the fact

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that Hc increased slightly when excessive amount of BZBS glass was added This could be

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contributed to the fact that too much liquid phase at the grain boundaries, resulting in the

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increased hindrance force.

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Figure 5 shows the remanence square ratio of the Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites. It

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can be seen that the inflection point of each curve is the point where the amount of BZBS

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glass was 2.0 wt.%, and the tendency of remanence square ratio is quite similar to the

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tendency of Bs (Fig .3). In addition, the remanence square ratio increased slowly when the

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sintering temperature increased. It should be noted that the optimal value (about 0.85) was

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quite close to the samples which were sintered at a relatively high temperature (above

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950oC) such as Ref. [18]. What’s more, other ferromagnetic properties presented a similar

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rule in comparison with the high temperature sintering process. However, this study shows

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a novel formula of glass (BZBS) which could realize the low-temperature sintering.

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The densities of the samples doped with various amount of BZBS glass sintered

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under different temperatures are presented in Fig .6. It can be seen that both the sintering

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temperature and the proportion of BZBS glass are influencing factors. As for the former

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factor, the elevated sintering temperature promoted the grain growth and accelerated the

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process of small size grains combining together into larger grains, which decreased

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porosity factor and finally increased the bulk density. As for the latter factor, the densities 6

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wt.%). Nevertheless, when the BZBS glass amount exceeded 2.0 wt.%, the rising trend

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slows down its step or even turns into downtrend. The above phenomenon could be

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explained by that too much BZBS glass with lower density decreased the average density

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of the sample. In short, these results indicate that the BZBS glass can effectively improve

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the densification of the Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites.

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Figure 7 shows the FMR spectra of the Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites doped with

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various amount of BZBS glass sintered at 920oC. It can be seen for almost all the samples,

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Lorentz-Fit lines were more anastomotic than Gauss-Fit lines. At first, without the BZBS

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glass, both the Lorentz-Fit and the Gauss-Fit fitted poorly. When the addition of BZBS

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glass was 2.0 wt.%, not only the Lorentz-Fit line but also the Gauss-Fit line was fitted best

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with experimental data compared with the rest of the samples. The FMR line width (∆H)

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value calculated from the experimental data is presented in Fig. 8. It was observed that the

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∆H value decreased significantly when doped with just 0.5 wt.% BZBS glass (from ~800

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Oe to 388 Oe) and the curve shows a downtrend when the doping content was less than

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2.0 wt.%. In addition, ∆H value reached its minimum (275 Oe) when doped with 2.0 wt.%

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BZBS glass and increased slightly with further increasing doping content. On the basis of

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the formula,

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  ∆    = ∆      + 2.07   + 1.5(4)# 4 in polycrystalline garnets [19, 20], where Ha represents the anisotropy field and P represents

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the

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Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites were composed of relatively large-size grains, resulting in

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low porosity and the P value decreased subsequently, which finally caused the reduction

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of ∆H. However, when the doping content amount exceeded 2.0 wt.%, small grains and

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large grains coexisted (Fig .2(e) and Fig .2(f)), resulting in the increase of anisotropy field.

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porosity.

When

adding

an

appropriate

amount

of

BZBS

glass,

the

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Therefore, the above-mentioned factors finally caused the decrease of ∆H when further

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doping with BZBS glass.

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Conclusion In summary, Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites were successfully synthesized under a

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relatively low temperature (from 880 to 920 oC). The BZBS glass doping content plays a

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vital role in the low temperature co-firing process of the Li-Zn-Ti ferrites. All the samples

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doped with various amount of BZBS glass sintered at different temperatures showed pure

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spinel phase, indicating the successful synthesis of the ferrites. Moreover,

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BZBS glass is the optimal doping amount with which the Li-Zn-Ti ferrites possess

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enhanced ferromagnetic properties such as saturation induction (from ~100 to 285 mT),

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coercivity (from 620 to 255 A/m) and FMR line width (from ~800 to 275 Oe). It can be

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concluded

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Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites via low-temperature co-fired technology.

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Acknowledgments

BZBS

glass

is

a

promising

candidate

for

2.0 wt.%

synthesis

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This work was financially supported by the National Nature Science Foundation of

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China under Grant No. 51502033 and No.61571079, National Basic Research Program of

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China under Grant No. 2012CB933104, 111 Project No. B13042.

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Figure Captions:

254 Figure 1. XRD patterns of samples sintered under different temperatures: (a) 880 oC, (b)

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900 oC, and (c) 920 oC with various BZBS glass content from 0.0 wt.% to 4.0

257

wt.%.

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Figure 2. SEM micrographs of Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites sintered at 920 oC for 2 h

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with BZBS glass addition of (a) 0.0 wt.%, (b) 0.5 wt.%, (c) 1.0 wt.%, (d) 2.0

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wt.%, (e) 3.0 wt.%, and (f) 4.0 wt.%.

263 264 265 266 267

with BZBS glass content from 0.0 wt.% to 4.0 wt.%.

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Figure 3. The saturation induction (Bs) of the samples sintered at 880oC, 900oC and 920oC

Figure 4. The coercivity (Hc) of the samples sintered at different temperatures with BZBS glass content from 0.0 wt.% to 4.0 wt.%.

Figure 5. The remanence square of the samples sintered at 880oC, 900oC and 920oC with BZBS glass content from 0.0 wt.% to 4.0 wt.%.

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Figure 6 . The bulk density of Li-Zn-Ti ferrites samples sintered at different temperatures (880oC, 900 oC and 920oC ) with various BZBS glass addition from 0.0 wt.%

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to 4.0 wt.%.

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Figure 7. FMR spectra with fitted Lorentz and Gauss curves of the Li-Zn-Ti ferrites sintered under 920 oC with (a) 0.0 wt.%, (b) 0.5 wt.%, (c) 1.0 wt.%, (d) 2.0

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wt.%, (e) 3.0 wt.%, and (f) 4.0 wt.% BZBS glass addition.

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Figure 8. FMR line width (∆H) calculated from the experimental data of FMR spectra of

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the Li-Zn-Ti ferrites sintered under 920 oC with various BZBS glass content .

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(c) Figure 1 13

ACCEPTED MANUSCRIPT 285 286 287

291

EP

290

Figure 2

AC C

289

TE D

M AN U

SC

RI PT

288

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RI PT

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295 296

TE D EP

298

Figure 3

AC C

297

15

ACCEPTED MANUSCRIPT 299 300

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RI PT

301

302

TE D EP

304

Figure 4

AC C

303

16

ACCEPTED MANUSCRIPT 305

M AN U

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RI PT

306

307 308

Figure 5

EP AC C

310

TE D

309

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317

Figure 6

EP

316

AC C

315

TE D

M AN U

SC

RI PT

314

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ACCEPTED MANUSCRIPT 318 319

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TE D EP

323

Figure 7

AC C

322

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330 331

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Figure 8

AC C

328

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ACCEPTED MANUSCRIPT 332 Table Captions:

334

Table 1. Influence of the additive content of BZBS glass to the magnetic properties and

335

densities of the Li0.43Zn0.27Ti0.13Fe2.17O4 ferrites sintered at 920 oC

336

RI PT

333

(g/cm3)

(µm)

3.623

0.94

4.145

2.83

309

4.19

3.94

275

4.32

4.20

619.9

175.7

0.7433

765

0.5 wt. %

315.42

268.74

0.812

388

1.0 wt. %

271.36

279.65

0.8427

2.0 wt. %

255.11

284.98

0.8373

3.0 wt. %

261.9

4.0 wt. %

270.75

259.01

0.8065

375

4.356

2.32

251.67

0.7802

399

4.295

2.48

AC C

EP

TE D

338

SC

0.0 wt. %

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Density Grain size

M AN U

BZBS glass Content Hc(A/m) Bs (mT) Br / Bs ∆H(Oe)

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ACCEPTED MANUSCRIPT Research Highlights： ：

AC C

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Low-temperature preparation of Li-Zn-Ti ferrites (below 950oC)
All the samples with BZBS glass addition show a typical spinel structure
Bs increased from ~100 to 285 mT with the ∆H decreased from 800 to 275 Oe