xiuli chen , xu li, huanfu zhou, jie sun, xiaoxia li, xiao yan ... · recently, chen et al. [19]...

Journal of Advanced Ceramics 2019, 8(3): 427–437 ISSN 2226-4108 https://doi.org/10.1007/s40145-019-0326-4 CN 10-1154/TQ

Research Article

www.springer.com/journal/40145

Phase evolution, microstructure, electric properties of

(Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics

Xiuli CHEN*, Xu LI, Huanfu ZHOU, Jie SUN, Xiaoxia LI, Xiao YAN, Congcong SUN, Junpeng SHI

Collaborative Innovation Center for Exploration of Hidden Nonferrous Metal Deposits and Development of New Materials in Guangxi, Key Laboratory of Nonferrous Materials and New Processing Technology, Ministry of

Education, School of Materials Science and Engineering, Guilin University of Technology, Guilin 541004, China

Received: December 28, 2018; Revised: March 8, 2019; Accepted: March 22, 2019 © The Author(s) 2019.

Abstract: (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 (abbreviated as BBNTBS, 0.02 ≤ x ≤ 0.12) ceramics were fabricated via a traditional solid state reaction method. The phase transition of BBNTBS from tetragonal to pseudo cubic is demonstrated by XRD and Raman spectra. The BBNTBS (x = 0.1) ceramics have decent properties with a high εr (~2250), small Δε/ε25°C values of ±15% over a wide temperature range from –58 to 171 ℃, and low tanδ ≤ 0.02 from 10 to 200 ℃. The basic mechanisms of conduction and relaxation processes in the high temperature region were thermal activation, and oxygen vacancies might be the ionic charge transport carriers. Meanwhile, BBNTBS (x = 0.1) exhibited decent energy storage density (Jd = 0.58 J/cm3) and excellent thermal stability (the variation of Jd is less than 3% in the temperature range of 25–120 ℃), which could be a potential candidate for high energy density capacitors. Keywords: structure; thermal stability; energy storage

1 Introduction

With the rapid development of microelectronics, dielectric capacitors with high dielectric constant and good thermal stability have attracted much attention [1]. In general, most dielectric capacitors are lead-based relaxor compositions [2,3]. However, lead is a harmful element, which seriously endangers the human’s health and the surrounding environment [4]. Hence, it is an inevitable trend to develop lead-free materials to replace lead-based materials.

As one of the lead-free materials, BaTiO3 (BT) has * Corresponding author. E-mail: [email protected]

been extensively studied and applied in capacitors for many years due to its decent dielectric properties [5–8]. However, pure BT has three phase transition points at a certain temperature [9], corresponding to three unusually large dielectric constants, which seriously restricts its further application in industry. As we know, the doping of equivalent or heterovalent ions has been demonstrated as an effective strategy to regulate the dielectric properties [10–12]. Among them, BaTiO3-based solutions have been extensively investigated. For example, BaTiO3–Bi(Mg2/3Nb1/3)O3 [13] exhibited a high relative permittivity (~6800). Binary solid solution based on (Bi0.5Na0.5)TiO3–BaTiO3 was a candidate in high- temperature energy-storage application [14–17]. BaTiO3–BiYO3 ceramics could meet the X9R criterion

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[18]. The above materials have obtained good dielectric properties in a wide temperature range.

Recently, Chen et al. [19] reported that the amphoteric behavior of Bi ion doped BT could improve the thermal stability of ceramics. An amphoteric behavior similar to Bi ions has been reported in rare earth element doped BT and Bi0.5Na0.5TiO3 ceramics [20–23]. Furthermore, as an effective dopant, SnO2 could enhance the dielectric temperature stability of BT ceramics [24,25]. In our previous works, (Ba1–xBi0.5xSr0.5x) (Ti1–xBi0.5xSn0.5x)O3 solid solutions were successfully prepared and could meet the X9R criterion [26]. Therefore, it could be expected that (Ba1–xBi0.67xNa0.33x) (Ti1–xBi0.33xSn0.67x)O3 (BBNTBS) may exhibit decent dielectric properties. Meanwhile, the phase evolution, microstructure, and electric properties of BBNTBS ceramics were also systematically studied.

2 Experimental procedure

BBNTBS (0.02 ≤ x ≤ 0.12) ceramics were prepared by a conventional solid phase reaction method and detailed experimental processes were described in the Electronic Supplementary Material (ESM). The samples were sintered at 1160–1260 ℃ for 2 h in the air. The tests were described in the ESM.

3 Results and discussion

In order to confirm the phase structure of (Ba1–xBi0.67x- Na0.33x)(Ti1–xBi0.33xSn0.67x)O3 (BBNTBS, 0.02 ≤ x ≤ 0.12) ceramics, room temperature (RT) XRD patterns of BBNTBS ceramics were measured and the results are shown in Fig. 1(a). It can be seen that the systems form a homogenous solid solution within the concerned composition range. The magnification XRD patterns in near 45° (phase transition area) are presented in Fig. 1(b). It can be clearly seen that (002)/(200) diffraction peaks exist in near 45° as x ≤ 0.04, which is consistent with the characteristics of tetragonal [19]. With further increasing x, the merging of (200)T and (002)T peaks into a single (200)P-C peak was observed, which indicates that the phase transformed to pseudo-cubic [13]. Hence, the phase transition point can be determined near x = 0.04. Furthermore, the single peak gradually shifts to a lower degree with further increasing x. This may be ascribed to the truth

that the ionic radius difference between Na+ (1.39 Å, CN = 12), Bi3+ (1.32 Å, CN = 12), and Ba2+ (1.61 Å, CN = 12) are small (13.6%, 14%) in the A-site. But Bi3+ (1.03 Å, CN = 6) and Sn4+ (0.69 Å, CN = 6) are larger (70.2%, 14%) than Ti4+ (0.605 Å, CN = 6) in the B-site based on an ideal perovskite ABO3 structure, leading to lattice expansion [27]. Meanwhile, in order to determine the relative content of the phase for BBNTBS (x = 0.1) ceramics and identify the occupation of Bi ions, a Rietveld refinement using GSAS software with the cubic and tetragonal BaTiO3 structures as the original models was done and the result is presented in Fig. 2. Similar methods have been reported in previous literature [4,28]. Final refined structural parameters of BBNTBS (x = 0.1) are listed in Table 1. The reliability factors for BBNTBS (x = 0.1), Rwp , Rp, and χ2 values are 6.47%, 4.59%, and 5.00, respectively. Based on the above analysis, it has been confirmed that one part of Bi+ ions occupied A-site and the other occupied B-site, which was consistent with the design of the original formulation.

Fig. 1 (a) XRD patterns of (Ba1–xBi0.67xNa0.33x) (Ti1–xBi0.33xSn0.67x)O3 (0.02 ≤ x ≤ 0.12) and (b) the enlarged region 44°−46° of BBKTBS ceramics.

Fig. 2 Rietveld refinement for (Ba1–xBi0.67xK0.33x) (Ti1–xBi0.33xSn0.67x)O3 (x = 0.1) ceramics at room temperature.

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Table 1 Final refined structural parameters of BBNTBS (x = 0.1)

Phase fraction Atoms(Wyck.) Occupancy x y z Biso (Å2)

95.2% Pm3m

Ba(1a) 0.9 0 0 0 0.006

Bi(1a) 0.067 0 0 0 0.01

Na(1a) 0.033 0 0 0 0.01

Ti(1b) 0.9 0.5 0.5 0.5 0.01

Bi(1b) 0.033 0.5 0.5 0.5 0.01

Sn(1b) 0.067 0.5 0.5 0.5 0.01

O1 1 0 0.5 0.5 0.01

4.8% P4mm

Ba(1a) 0.9 0 0 0 0.01

Bi(1a) 0.067 0 0 0 0.01

Na(1a) 0.033 0 0 0 0.01

Ti(1b) 0.9 0.5 0.5 0.5 0.02

Bi(1b) 0.033 0.5 0.5 0.5 0.01

Sn(1b) 0.067 0.5 0.5 0.5 0.01

O1 0.25 0.52 0.52 −0.03 4.1

O2 1 0 0.5 0.48 4.4

In order to further verify the phase transition process of BBNTBS ceramics, the Raman spectra in the

frequency range of 80–1000 cm–1 at RT of BBNTBS ceramic samples are carried out and their deconvolution using Gaussian functions are presented in Fig. 3. It can be seen that all Raman bands of BBNTBS ceramics are relatively wide, which is believed to be due to the disorder in the sub lattice of BBNTBS, resulting from several overlapping Raman peaks [29]. In low- and mid-wavenumber range, Raman spectra for BBNTBS (0.02 ≤ x ≤ 0.04) are characterized by interference dip at ~180 cm–1 and a sharp E(TO) “silent” mode at ~305 cm–1, which is consistent with the spectra of the tetragonal BT phase [30,31]. With further increasing x, the interference dip at 180 cm–1 vanishes but two new modes a and c appear in ~110 and ~180 cm–1 respectively (as shown in Fig. 3(c)), indicating the emergence of a pseudo-cubic phase [32]. Meanwhile, the emergence of modes a and c may be related to A−O vibrations, which indicates that the nano region of test samples has enrichment of Ba2+ and Bi3+ cations [33]. The vibration in the high wavenumber range may be related to the oxygen octahedron. The above analysis is also consistent with the XRD analysis.

Fig. 3 (a) Room temperature Raman spectra, (b) fitting spectra, and (c) variations of the peak frequency of modes in the Raman spectra in the band at 100–200 cm−1 of (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 (0.02 ≤ x ≤ 0.12) ceramics.

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Representative SEM images of BBNTBS ceramics are presented in Figs. 4(a)–4(e). Meanwhile, the bulk density of these samples is also shown in Fig. 4(f). The average grain sizes of ceramics enlarged from 0.59 to 2.22 µm with increasing x from 0.02 to 0.1, which suggests that the substitution of a few ions can facilitate the grain growth of BT ceramics. The increase of average grain size may be attributed to the

lattice expansion arising from the radius mismatch on the A-site and B-site [34], which is consistent with the XRD analysis.

Figures 5(a) and (b) demonstrate the temperature dependences of the relative permittivity (εr) and dielectric loss (tanδ) for BBNTBS (0.04 ≤ x ≤ 0.12) ceramics measured at the various frequencies, respectively. As x = 0.1, the ceramic presents decent

Fig. 4 SEM micrographs of (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics sintered at their optimized temperatures: (a) x = 0.02, 1260 ℃, (b) x = 0.04, 1240 ℃, (c) x = 0.06, 1220 ℃, (d) x = 0.08, 1200 ℃, and (e) x = 0.1, 1180 ℃. Insert shows the grain size distribution of (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics. (f) The bulk density of BBNTBS ceramics as a function of x.

Fig. 5 (a) Relative permittivity and (b) dielectric loss as a function of temperature of (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics measured at 1, 10, and 100 kHz. (c) Plots of ln(1/ε–1/εm) versus ln(T–Tm) at 1 kHz for BBNTBS ceramics.

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dielectric performance with εr ≈ 2250, tanδ < 2% in the temperature range of 20–200 ℃, and Δε/ε25°C ≤ ±15% in the temperature range of –58–171 ℃, as shown in Fig. 6. The above results show that (Ba0.9Bi0.067Na0.033) (Ti0.9Bi0.033Sn0.067) O3 ceramics may meet the criterion in MLCC of X8R. According to ferroelectric domain dynamics [35], two dielectric peaks, corresponding to the ferroelectric−ferroelectric (TFE) and ferroelectric paraelectric phase transition (TC), could be observed in all samples, which may be related to the special structure of the grain. In addition, it can be also seen that the first characteristic peak shifted to a lower temperature and another peak became more flat with increasing x, which may be due to chemical disturbance caused by differences in the radius and valence of different cations (i.e., the replacement of (Bi3+, Na+) for Ba2+ and (Bi3+, Sn4+) for Ti4+ would destroy the long-range driving dipolar and promote the formation of local polar region) [13]. And the cation disorder on the A-site and B-site may cause relaxor behavior in ceramics. To further describe the relaxor nature of the systems, a modified Curie–Weiss law is expressed as follows:

m

m

( )1 1 T TC

γ

ε ε−

− =

where εm is the maximum dielectric constant, C is the Curie constant, and γ is the indicator of the diffuseness degree. The value of γ can vary between 1 and 2. It can be seen from Fig. 5(c) that the value of γ increases from 1.35 to 1.5 with increasing of x, indicating that the relaxor nature of the samples increases.

To ascertain the conduction mechanism of BBNTBS

ceramics at different temperatures, impedance spect-roscopy was adopted and fitted using 2RQC (Q is constant phase element) equivalent circuit, where the 2RQC components are grain and grain boundary, respectively. It can be seen that two superimposed semicircles are presented in Figs. 7(a)–7(f), which are thought to have two dielectric relaxations. One arc is associated with the grain response in the high frequency band, and the other is related to the grain boundary response [36]. With increasing temperature, the radius of semicircles decreased (i.e., impedance decreased), which indicates that the conductivity of the ceramic increased. In the meantime, the values of grain (Rg) and grain boundary resistance (Rgb) for BBNTBS

ceramics at various temperatures are listed in Table 2. The resistance of the ceramics decreases with increasing temperature, suggesting the semiconductor behaviors of the systems. Furthermore, the centers of arcs fell below the real impedance Z' axis, indicating that the relaxation process is non-Debye type in ceramics, which may be due to the grain size, grain boundaries, and distribution of atomic defects, etc. [37].

Figure 8 shows the functional diagram of impedance imaginary part Z"(f) for BBNTBS ceramics at various temperatures. It can be seen that the relaxation peak of Z" shows a gradual shift toward high frequency with increasing measurement temperature, which indicates the electron relaxation occurs in the system [38]. The relaxation time as a function of absolute temperature was shown in the insets in Figs. 8(a)–8(d). The relaxation time can be estimated via the following formula:

Fig. 6 Temperature dependence of (a) thermal stability (Δε/ε25℃) and (b) dielectric loss for (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics measured at 10 kHz, and (c) thermal stability (Δε/ε25°C) and (d) dielectric loss for (Ba0.9Bi0.067Na0.033)(Ti0.9Bi0.033Sn0.067)O3 ceramics as a function of the measured temperature from –110 to 200 ℃.

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Table 2 Comparison between the grain (Rg) and grain boundary (Rgb) resistance of (Ba1–xBi0.67xNa0.33x) (Ti1–xBi0.33xSn0.67x)O3 ceramics Sample Temperature (℃) Rg (Ω) Rgb (Ω) Sample Temperature (℃) Rg (Ω) Rgb (Ω)

x=0.02

460 20.41 922.80

x=0.06

520 19.02 306.2

480 14.81 521.50 540 16.79 182.7

500 10.76 305.60 560 14.4 111.3

520 8.34 179.80

x=0.08

460 1982 3776

540 6.89 103.10 480 484.2 2262

560 6.61 59.93 500 161.7 1419

x=0.04

460 51.46 2136.00 520 88.01 898.4

480 27.9 1198.00 540 78.16 553.5

500 13.87 707.30 560 10.42 168.9

520 8.69 439.10

x=0.1

460 28889 248180

540 7.80 302.00 480 2038 19624

560 7.29 173.90 500 445.5 10637

x=0.06

460 60.71 1794.00 520 244 6133

480 38.55 941.40 540 121.9 3627

500 25.26 521.60 560 117.8 2168

Fig. 7 Nyquist plots of impedance and equivalent circuit for (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics at selected temperatures.

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Fig. 8 Frequency dependence of imaginary part of impedance (Z″) for (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics at selected temperatures. Insert shows the Arrhenius plot for relaxation time. The dotted line is a linear fit to Eq. (1).

max

1τω

=

where ωmax (= 2πfmax) is the angular frequency corresponding to the frequency of Z" maximum. The relaxation activation energies of samples are calculated by the following law:

( )0 a Bexp /E k Tτ τ= (1)

where τ0 is the constant, kB is the Boltzmann constant, and Ea is the relaxation activation energy. Ea can be estimated and their values are 1.96, 1.9, 1.96, 1.63, 1.61, and 1.49 eV, respectively (as shown in the inset of Fig. 8). These values are large, which may be the result of the ionic conductivity of the ceramic [39].

The frequency dependence of AC conductivity (σac) for BBNTBS ceramics is shown in Fig. 9. With increasing the frequency, σac gradually increases, which indicates the existence of moving charge carriers. In addition, the curves tend to flatten in the low frequency

band, indicating a DC conductivity (σdc) behavior. σac of ceramics could be calculated via the universal Jonscher’s law:

ac dcnAσ σ ω= +

where ω is angular frequency, and n (0 ≤ n ≤ 1) values are two temperature-dependent adjustment constants. Meanwhile, the temperature change of σdc follows Arrhenius law:

dc 0 dc Bexp( / )E k Tσ σ= − (2)

where σ0 is the constant, and Edc is the activation energy. The Edc can be calculated by Eq. (2) and these values are 1.34, 1.23, 1.39, 1.26, 1.5, 1.37 eV, respectively, as shown in the inset of Fig. 9. It can be seen that Edc is smaller than Erel. This phenomenon may be that Edc is caused by the generation of carriers and long-distance migrations, but the Erel is caused by the jump of the carrier in the adjacent lattice and the migration of carrier [40].

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Fig. 9 Frequency dependence of AC conductivity for (Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 ceramics at different temperature. Insert shows the Arrhenius plot of the DC conductivity. The squares are the experimental points and the dotted line is a linear fit to Eq. (2).

The energy storage behavior of BBNTBS ceramics

was investigated by the P–E hysteresis loops, as shown in Fig. 10(a). The discharge energy storage density (Jd)

could be given by the following equation: b

d 0d

EJ E P= ∫

The energy storage efficiency (η ) follows the law:

d

c100%J

Jη = ×

where P, E, Eb, and Jc are the polarization, electric field, dielectric breakdown electric field, and charge energy storage density, respectively.

The P–E hysteresis loops for BBNTBS (x =

0.06–0.12) ceramics measured at the critical electric field are shown in Fig. 10(b). It can be seen that the remnant polarization (Pr) decreases (i.e., the P–E loop becomes slimmer) with increasing x. Meanwhile, ΔP (Pmax–Pr) and Eb (breakdown strength) are two important parameters for energy storage materials [41], which determine the energy density and working electric field of the materials, as shown in Fig. 10(c). Figure 10(d) presents Jd and η of the ceramics. It can be seen that the largest Jd is 0.58 J/cm3 (pure BaTiO3 is 0.4 J/cm3), which can be obtained in the sample of x = 0.1. In addition, to assess the potential applications of the BBNTBS (x = 0.1) ceramic in energy storage devices, its thermal stability was also studied. Figure 10(e)

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Fig. 10 (a) Schematic diagram of energy storage parameters calculation; (b) P–E hysteresis loops measured at 10 Hz of BBNTBS ceramics under the critical electric field; (c) variation of ΔP and Eb; (d) Jd and η as a function of x; (e) P–E loops of the BBNTBS ceramics measured at a temperature range of 25–120 ℃ at 10 Hz and at 80 kV/cm; (f) Jd and η at 80 kV/cm as functions of temperature from 25 to 120 ℃.

presents the P–E loops of the BBNTBS (x = 0.1) ceramic from 25 to 120 ℃ at 80 kV/cm. The Jd and η values are displayed in Fig. 10(f). It can be seen that the thermal fluctuation is less than 3% in the temperature range of 25−120 ℃, which indicated that the BBNTBS ceramics could be an excellent candidate for potential high energy density capacitors.

4 Conclusions

(Ba1–xBi0.67xNa0.33x)(Ti1–xBi0.33xSn0.67x)O3 lead-free solid solutions ceramics have been smoothly synthesized via the traditional solid phase reaction method. The phase evolution, microstructure, and electric properties of

BBNTBS (0.02 ≤ x ≤ 0.12) ceramics have been systematically analyzed. The phase transition of BBNTBS from tetragonal to pseudo cubic was demonstrated by XRD and Raman spectra. When x = 0.1, the ceramic exhibited decent dielectric properties with large εr (~2250), low tanδ < 2% (10−200 ℃), and good thermal stability Δε/ε25°C (≤ ±15%) from –58 to 171 ℃. Meanwhile, energy storage density reached 0.58 J/cm3 for x = 0.1, which could be an excellent candidate for potential high energy density capacitors.

Acknowledgements

This work was supported by National Natural Science

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Foundation of China (Nos. 11664008 and 61761015), and Natural Science Foundation of Guangxi (Nos. 2018GXNSFFA050001, 2017GXNSFDA198027, and 2017GXNSFFA198011).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s40145-019-0326-4.

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