- Email: [email protected]
2)O3 modification
Journal Pre-proof Ultralow dielectric loss of BiScO3 -PbTiO3 ceramics by Bi(Mn1/2 Zr1/2 )O3 modification Yang Yu, Jikun Yang, Jingen Wu, Xiangyu Gao, Lang Bian, Xiaotian Li, Xudong Xin, Zhonghui Yu, Wanping Chen, Shuxiang Dong
PII:
S0955-2219(20)30095-9
DOI:
https://doi.org/10.1016/j.jeurceramsoc.2020.02.015
Reference:
JECS 13062
To appear in:
Journal of the European Ceramic Society
Please cite this article as: Yu Y, Yang J, Wu J, Gao X, Bian L, Li X, Xin X, Yu Z, Chen W, Dong S, Ultralow dielectric loss of BiScO3 -PbTiO3 ceramics by Bi(Mn1/2 Zr1/2 )O3 modification, Journal of the European Ceramic Society (2020), doi: https://doi.org/10.1016/j.jeurceramsoc.2020.02.015
This is a PDF file of an article that has undergone enhancements after acceptance, such as the addition of a cover page and metadata, and formatting for readability, but it is not yet the definitive version of record. This version will undergo additional copyediting, typesetting and review before it is published in its final form, but we are providing this version to give early visibility of the article. 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. © 2020 Published by Elsevier.
Ultralow dielectric loss of BiScO3-PbTiO3 ceramics by Bi(Mn1/2Zr1/2)O3 modification
Yang Yu1,2, Jikun Yang2, Jingen Wu2 , Xiangyu Gao 2, Lang Bian 2, Xiaotian Li 3 , Xudong Xin2 , Zhonghui Yu2, Wanping Chen 1,*, Shuxiang Dong 2, * 1
School of Physics and Technology, Wuhan University, Wuhan, Hubei, 430072, China 2 Department of Materials Science and Engineering, College of Engineering,
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Peking University, Beijing, 100871, China 3 Department of materials science and engineering, school of power and mechanical engineering, Wuhan University, Wuhan, Hubei, 430072, China *Corresponding authors E-mail addresses: [email protected] (W. Chen), [email protected] (S. Dong).
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Abstract
BiScO3-PbTiO3 ceramics are attractive for high-temperature piezoelectric applications while their high dielectric loss has to be substantially reduced. In this
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paper, a ternary perovskite system of xBi(Mn1/2Zr1/2)O3-(1-x-y)BiScO3-yPbTiO3 (abbreviated as xBMZ-BS-yPT) with x = 0.02, 0.04 and y = 0.62 - 0.67 were
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fabricated by conventional solid-phase method, and their ceramics were systematically studied with regards to phase structure, microstructure, dielectric and
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piezoelectric properties. X-ray diffraction results indicate a gradual change from rhombohedral to tetragonal phase with increasing PT composition. Morphotropic phase boundary (MPB) is revealed for the system with x = 0.02，y = 0.64, at which ultralow dielectric loss factor (0.58%), almost unchanged Curie temperature (449 oC), high electromechanical properties (d33 = 360 pC/N, kp = 0.53), and stable strain output below 200 oC are observed. With such excellent piezoelectric properties and high-temperature stability, BMZ modified BS-PT ceramics are promising candidates 1
for power electromechanical devices, especially operating in high-temperature environments.
Keywords ： Ultralow dielectric loss factor (tanδ); Piezoelectric ceramics; BiScO3-PbTiO3; High-temperature application; Temperature stability.
1．Introduction Nowadays, there is an increasing technological demand for sensors and transducers
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operating at rather high temperatures (T > 200 oC), such as those applied in oil/gas
drilling and aerospace explorations industries.1-7 Traditional lead-based piezoelectric ceramics have been widely applied in various industrial devices at room temperature
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or relatively low temperatures. Especially, Pb(Zr,Ti)O3-based ceramics have highly competitive properties, such as good piezoelectric and electromechanical properties near the MPB composition.8-13 However, it is very difficult for PZT-based ceramics to
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be used above 200 oC, because their Curie temperature is below 350 ℃ and they may
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start to depolarize above 200 oC. Bismuth layer structured ceramics, such as Na0.5Bi4.5Ti3.975Co0.025O15 (Tc ~ 670 oC),14 CaBi2Nb2O9 (Tc ~ 930 oC),15 usually possess very high Curie temperature. However, their applications are limited due to
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relatively lower piezoelectric constant (d33 ≦ 40 pC/N).14-17 Recently, the discovery of perovskite compound Bi(Me)O3-PbTiO3 systems (Me =
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Sc, In, Yb, Y, etc) has attracted more and more research interest for high temperature piezoelectric applications. It is reported that 0.36BiScO3-0.64PbTiO3 ceramics in
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MPB composition simultaneously have large piezoelectric constant (d33 = 450 pC/N) and high Curie temperature Tc around 450 oC, which is about 100 oC higher than that of commercial PZT piezoelectric ceramics.18-20 The ceramic series exhibit great potential for high temperature applications. However, the high dielectric loss factor (tanδ > 3%) and low mechanical quality factor (Qm < 30) of BS-PT-based ceramics will cause serious heat generation and energy dissipation and further restrict their applications as power electronic devices operating at resonance frequency.21-25 To 2
decrease tanδ or increase Qm, previous works have reported some methods such as MnO2 doping and introduction of Pb(Mn1/3Sb1/3)O3 or Pb(Mn1/3Nb1/3)O3.26-30 Unfortunately, the dielectric loss factor of these modified ceramics is still at a relatively high level (tanδ > 1%), and what is worse, the piezoelectric performance (d33 < 300 pC/N) deteriorates seriously.31 In this paper, for the first time, we report that the introduction of Bi(Mn1/2Zr1/2)O3 (BMZ) end member into BS-PT ceramics can greatly reduce dielectric loss factor, while piezoelectric coefficient and Curie temperature are still maintained at relatively
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high values. BMZ of different concentrations were introduced in BS-PT ceramics, and the effects of PT concentration on the phase, microstructure, dielectric, ferroelectric and piezoelectric properties were also investigated in detail. Ultralow dielectric loss
factor (tanδ = 0.58%), large piezoelectric constant (d33 = 360 pC/N), high planar
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electromechanical coupling coefficient (kp = 0.53) and high Tc (Tc = 449 oC) were
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2. Experimental procedure
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obtained at 0.02Bi(Mn1/2Zr1/2)O3-0.34BiScO3-0.64PbTiO3 MPB composition.
Series of xBi(Mn1/2Zr1/2)O3-(1-x-y)BiScO3-yPbTiO3 ceramics (abbreviated as xBMZ-BS-yPT), with x = 0.02, 0.04 and y = 0.62 - 0.67, were prepared by the
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conventional mixed oxide process method. The starting raw materials, including PbO (99.9%), Bi2O3 (99%), Sc2O3 (99.99%), MnO2 (97.5%), TiO2 (99%) and ZrO2 (99%),
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were weighted according to the stoichiometric proportion with 2% PbO excess to compensate the evaporation of lead during the high-temperature sintering reaction.
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They were wet milled in polyethylene jar with agate balls for 8 h in ethanol. The milled powder was dried at 100 oC and calcined at 850 oC for 3 h in air. The calcined powder was then ball-milled for 24 h. Dried powder was sieved and pressed into pellets (Ф 14 × 1.2 mm3) using PVA as a binder at a pressure of 10 MPa followed by cold iso-static pressing (CIP) under pressure of 200 MPa for 10 min. After burning off PVA, the green compacts were embedded in the calcined powder of the same composition and sintered in a covered crucible at 1000 - 1040 oC for 2 h. 3
The crystalline structures of the sintered pellets were determined by X-ray diffraction (XRD) technology with Cu-Ka1 radiation (D/Max 2500, Rigaku, Tokyo, Japan). The fracture surface microstructure of the sintered pellets was observed by scanning electron microscopy (SEM, S-4800, Hitachi, Tokyo, Japan). The density of the ceramics was measured using a density tester according to Archimedes method. The sintered pellets were polished down to 0.8 mm, and were coated by electrodes with a post-fire silver paste at 650 °C for 0.5 h. For electrical measurements, the ceramics were poled in 140 oC silicone oil bath under a DC electric field of 40 kV/cm
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for 20 min. The poled specimens were aged in air for 24 h before any electrical measurement. The piezoelectric constant d33 was measured using a quasistatic d33 meter (ZJ-3D, Institute of Acoustics, Beijing, China). The dielectric constant and loss factor (tanδ) were measured in the temperature range from room temperature to 500 o
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C at the frequency of 1 kHz by utilizing an impedance analyzer (4294A, Agilent
Technologies). The electromechanical coupling factor kp and the mechanical quality
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factor Qm were calculated according to formulae (1) - (2) by using the resonance and anti-resonance technique (using an impedance analyzer 4294A, Agilent Technologies).
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The room temperature P-E hysteresis loops of samples were measured at a frequency of 1 Hz using a ferroelectric testing system (TF Analyzer 2000, aixACCT Systems
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GmbH, Germany).
1
2
fr
0 . 398
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Qm
0 . 579
fa fr
kp
(1)
2
fa 2 f r RC
T
( fa fr ) 2
2
(2)
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Here, fr and fa are the resonance and anti-resonance frequencies, respectively, R is the resonant impedance, and CT is the electric capacitance at 1 kHz.
3. Results and discussion
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Fig. 1 XRD patterns of (a) 0.02Bi(Mn1/2Zr1/2)O3-(0.98-y)BiScO3-yPbTiO3, with y = 0.62, 0.63, 0.64, 0.65, 0.66, 0.67, (b) Enlarged view of XRD patterns at 2θ = 31 - 33o, (c) 0.04Bi(Mn1/2Zr1/2)O3-(0.96-y)BiScO3-yPbTiO3, with
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y = 0.62, 0.63, 0.64, 0.65, 0.66, 0.67, (d) Enlarged view of XRD patterns at 2θ = 31 - 33o, (e) and (f) the calculated
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lattice parameters and c/a ratios obtained from these patterns.
Fig. 1 (a) and (b) display the room temperature X-ray diffraction spectra of 0.02Bi(Mn1/2Zr1/2)O3-(0.98-y)BiScO3-yPbTiO3 (y = 0.62, 0.63, 0.64, 0.65, 0.66, 0.67)
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ceramics sintered at 1040 oC with various PT contents. There are no traces of pyrochlore phase or impurities in the XRD patterns of any specimens, indicating that
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the BMZ members with BS-PT solid solution formed a stable single-phase perovskite structure. Meanwhile, the coexistence of rhombohedral (R) and tetragonal (T) phases is detectable. The effect of the PT content on the phase composition of ceramics is studied. It can be seen that the phase structure of the ceramic with y = 0.62 is rhombohedral (R) phase. While in the XRD pattern of the ceramic with y = 0.67, the splitting of (110)T and (101)T peak is markedly observed, indicating that the phase structure of BMZ-BSPT ceramic has changed into tetragonal (T) phase.32 With the 5
decrease of PT content from 0.67 to 0.62, the crystalline phase of ceramics gradually changes from tetragonal to rhombohedral. Thus, it is clear that the morphotropic phase boundary (MPB) exists in the range of y = 0.63 - 0.65. Piezoelectric ceramics near the MPB region will present the highest d33. The similar situation occurs in 0.04Bi(Mn1/2Zr1/2)O3-(0.96-y)BiScO3-yPbTiO3 ceramics from Fig. 1 (c) and (d). With the increase of PT content from 0.62 to 0.67, (100) single peak near 2θ = 31o - 33o degree splits into two peaks of (101) and (110), which reveals that the crystalline phase of ceramics changes from rhombohedral to tetragonal. It is clear that the
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morphotropic phase boundary (MPB) near the range of y = 0.63 - 0.65 is obtained. Tetragonality (which is reflected in the c/a ratio) is an important structural
parameter of the perovskite lattice that determines the spontaneous polarization of piezoelectric ceramics. Fig. 1 (e) and (f) show the calculated tetragonality values of
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0.02BMZ-BSPT and 0.04BMZ-BSPT ceramics as a function of PT content. It can be
seen that the increase of PT content leads to tetragonality strengthening, as a result of
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PT being tetragonal phase.
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Fig. 2 SEM images of the fracture surfaces from (a)-(f) 0.02BMZ-(0.98-y)BS-yPT (y = 0.62 - 0.67) ceramics and (g) - (l) 0.04BMZ-(0.96-y)BS-yPT (y = 0.62 - 0.67) ceramics.
Fig. 2 shows the fresh fracture surfaces of 0.02BMZ-(0.98-y)BS-yPT and
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0.04BMZ-(0.96-y)BS-yPT (y = 0.62 - 0.67) ceramics samples sintered at 1040 oC for 2 h. The ceramics samples are high density, with few holes, tight grains and distinct
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grain boundaries. The fracture modes of both are mainly intergranular fracture, which indicate that the mechanical strength of grain was stronger than the grain boundary, and fine crystallization was obtained. In order to explore the grain size distribution quantitatively, the linear intercept method was used to statistically analyze the grain size, and the results are given in the insets of Fig. 2. The average grain size of 0.02BMZ-0.34BS-0.64PT sample is around 4.97-7.37 μm, and 0.04BMZ-0.32BS-0.64PT sample possess a large grain size of 8
approximately 9.1-11.3 μm. The average grain size increases with the increased BMZ doping amount. Similar phenomena are also observed in previous Mn-doped or PMS-doped BS-PT-based systems.[29,33-36] Similar to previous reported results, oxygen vacancies are generated because of Ti substitution by multi-valence Mn element (Mn2+ or Mn3+), which promotes mass transport and further assists grain growth during sintering process.[29, 36] TABLE 1. Room temperature piezoelectric and dielectric properties of BMZ-BS-PT ceramics.
d33 (pC/N)
kp
0.02BMZ-0.36BS-0.62PT
Cm
240
0.51
0.02BMZ-0.35BS-0.63PT
Cm/P4mm
310
0.52
0.02BMZ-0.34BS-0.64PT
Cm/P4mm
360
0.53
0.02BMZ-0.33BS-0.65PT
P4mm
280
0.43
0.02BMZ-0.32BS-0.66PT
P4mm
210
0.02BMZ-0.31BS-0.67PT
P4mm
200
0.04BMZ-0.34BS-0.62PT
Cm
0.04BMZ-0.33BS-0.63PT
Cm/P4mm
0.04BMZ-0.32BS-0.64PT
Cm/P4mm
0.04BMZ-0.31BS-0.65PT
Qm
Tc (oC)
ρ (g/cm3)
0.34%
676
102
434
7.68
0.54%
1048
97
445
7.64
0.58%
1464
61
449
7.59
0.49%
1276
171
455
7.62
0.47%
976
178
464
7.59
0.35
0.40%
813
250
472
7.57
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0.38
0.47
0.36%
655
174
406
7.58
270
0.48
0.50%
839
163
424
7.50
281
0.51
0.52%
1333
155
430
7.55
P4mm
230
0.43
0.43%
1172
271
438
7.57
P4mm
190
0.38
0.35%
1012
414
445
7.58
P4mm
161
0.35
0.32%
836
535
456
7.58
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0.04BMZ-0.29BS-0.67PT
εr
220
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0.04BMZ-0.30BS-0.66PT
tan δ (1kHz)
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Space group
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Material
Table 1 summarizes the piezoelectric and dielectric properties of BMZ-BS-PT
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ceramics. It’s found that the values of d33, kp and εr for 0.02BMZ-BS-PT ceramics are very sensitive to the phase structure, which are determined by PT contents. These
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three values reach their maximum at the PT content of 0.64. This results further demonstrate that the MPB content of 0.02BMZ-BS-PT ceramics occurs at the PT content of 0.64. The excellent dielectric and piezoelectric properties are attributed to the coupling between two equivalent energy states, i.e., the rhombohedral and tetragonal phases, which promotes optimum domain reorientation during the poling. Dielectric loss factor (tanδ) of 0.02BMZ-BS-PT ceramics is below 0.58%, which is much less than that (tanδ = 3%) of pure BS-PT ceramics, indicating that the 9
introduction of BMZ to BS-PT can effectively restrain dielectric loss. Compared with the Qm of pure ceramics (around 20), it can be seen from the calculated results presented in Table 1 that Qm (61 - 250) values of 0.02BMZ-BS-PT ceramics have been improved a lot. According to previous researched reports, Mn ions can exist as multivalent states in perovskite phase, such as Mn2+, Mn3+, and Mn4+, especially, Mn2+ and Mn3+ states could coexist and replace the B4+ ions in ABO3-type perovskites. Therefore, this substitution may lead to acceptor characteristic and form oxygen vacancies to maintain the electrical neutrality. The oxygen vacancy can cause pinning
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effect and inhibit domain wall movement, so that tanδ is decreased and Qm is improved. The optimum values of planar electromechanical coupling coefficient (kp), dielectric constant (εr), piezoelectric constant (d33), Curie temperature (Tc) and dielectric loss factor (tan δ) at the MPB content are 0.53, 1464, 360 pC/N, 449 oC and
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0.58%, respectively.
When the BMZ content increased from 2 mol% to 4 mol%, d33, εr, Tc and kp are
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relatively reduced. But dielectric loss factor tan δ and Mechanical quality factor Qm show better values. The MPB composition of 0.04BMZ-BS-PT ceramics occurs at the
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PT content of 0.64. The dielectric loss factor is further reduced while Qm is significantly improved. This phenomenon can be apparently attributed to the
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generation of more oxygen vacancies with BMZ content increase. This also reveals that the BMZ is more effective composition of Mn doping29, 31 to decrease dielectric loss of BSPT ceramics and transform the material from soft-type ceramics to
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hard-type ones. The excellent values of planar electromechanical coupling coefficient (kp), dielectric constant (εr), piezoelectric constant (d33), Curie temperature (Tc),
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mechanical quality factor (Qm) and dielectric loss factor (tan δ) at the 0.64 content are measured to be 0.51, 1333, 281 pC/N, 430 oC, 155 and 0.52%, respectively.
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Fig. 3 Temperature-dependent dielectric constant εr and dielectric loss factor tanδ of (a) and (b) 0.02BMZ-BS-PT ceramics and (c) and (d) 0.04BMZ-BS-PT ceramics.
To demonstrate the stable performance of this novel material under high
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temperature, the temperature dependence of the dielectric constant and dielectric loss of 0.02BMZ-(0.98-y)BS-yPT and 0.04BMZ-(0.96-y)BS-yPT ceramic samples sintered
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at 1040 oC were tested at 1 kHz frequency as shown in Fig. 3. The temperature Tm corresponded to the maximum value of the dielectric constant is considered to be the
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Curie temperature Tc. For all ceramics, Curie temperature increase with the increase of PT content, as shown in Fig. 3 (a and b), which are ascribed to the high phase transition temperature of PbTiO3 (490 oC) member. For the 0.02BMZ-0.34BS-0.64PT ceramic samples, Curie temperature Tc is 449 oC, which is almost consistent with pure 0.36BS-0.64PT Curie temperature (Tc = 450 oC).18 Therefore, the deterioration of Curie temperature caused by introducing BMZ into BS-PT ceramics is much smaller than Mn and PMS, which is beneficial for ceramics to work at high temperature.18 11
The dielectric loss factor (tanδ) drops dramatically at room temperature as the BMZ content increase. The dielectric loss factor of all ceramics are less than 0.58%, especially, the dielectric loss factor of 0.04BMZ-0.39BS-0.67PT even reaches down to 0.35%. Clearly, in comparison with pure BS-PT or soft BS-PT-based ceramics with high loss factor (approximately 3%),18 the BMZ modification is a very effective way
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to reduce dielectric loss factor.
Fig. 4 Effect of thermal depoling on d33 values of (a) 0.02BMZ-BS-PT and (b) 0.04BMZ-BS-PT with different PT
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contents.
For high temperature application, the temperature stability of piezoelectric ceramics
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is one of the most important qualities. To verify the high-temperature stability of BMZ-BSPT, the polarized plate samples are annealed at different temperatures for one hour and their piezoelectric constant d33 was measured again at room temperature.
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Fig. 4 shows the measured piezoelectric constant d33 of 2% - 4% mol BMZ doped ceramics from room temperature (RT) up to 450 oC. It is clearly seen that at the initial
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stage (temperature T is below 250 ℃), d33 values appear to be almost unchanged as T rises. However, when T increases to depolarization temperature Td or it is close to the
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Curie temperature Tc, d33 values fall rapidly. The temperature at which d33 values decline rapidly is estimated as the depolarization temperature (Td). The depolarization temperatures of 0.02 BMZ and 0.04 BMZ doped ceramics are about 325 oC. The high Td should be attributed to the large coercive field (approximate 20 kV/cm) and high Curie temperature (approximate 450 oC), which are far higher than that of PZT ceramics (10 kV/cm and 350 oC). The high Tc means that a large thermodynamic movement energy is needed to destroy the ferroelectricity. It should be noted that 12
these values are about 150 oC higher than that of soft type PZT ceramics, and
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BMZ-BS-PT ceramics show their great potential for high-temperature application.
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Fig. 5 Piezoelectric constant d33 and dielectric loss factor (tan δ) of 0.02BMZ-0.34BS-0.64 PT ceramics in comparison with reported BS-PT based ceramics.
In order to evaluate the excellent performances of this novel material, we made a
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statistical study as illustrated in Fig. 5, including d33 and tan δ values of our samples 8, 12, 29, 31, 36
The 0.02BMZ -
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and other ceramics reported in previous literatures.7,
0.34BS - 0.64PT ceramic simultaneously exhibits both high d33 (360 pC/N) and the lowest tan δ (0.58%) that are never reported in modified BS-PT ceramic series. The
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comprehensive properties of this material are better than most of BS-PT based ceramics. Thus, this ceramic is potential for piezoelectric materials and devices
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employed in high temperature environments.
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Fig. 6 Room temperature P - E loops of (a) 0.02BMZ-BS-PT and (b) 0.04BMZ-BS-PT ceramics with different PT contents, (c) and (d) Pr and Ec of 0.02BMZ-BS-PT and 0.04BMZ-BS-PT ceramics with differing PT contents.
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Fig. 6 shows the polarization-electric field (P - E) hysteresis loops of the BMZ-BS-PT ceramics. These polarization loops were measured at frequency of 1Hz
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under an electric field of 60 kV/cm. They are symmetric and no obvious conductive problem observed. The remnant polarization Pr of 0.02BMZ-BS-PT ceramic samples increases with PT content, and reaches maximum value at y = 0.64 composition
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(MPB), then decreases with further increased PT content. Similar results also occur in 0.04BMZ-BS-PT ceramic series. The values of remnant polarization and coercive
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electric field of the 0.02BMZ-BS-PT series and 0.04BMZ-BS-PT series range from 4.8 - 18 μC/cm2 and 16.4 - 21.8 kV/cm, 5.1 - 17.5 μC/cm2 and 18.5 - 24 kV/cm, respectively.
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Fig. 7 Unipolar strain-electric field (S-E) curves at room temperature of (a) 0.02BMZ-BS-PT and (b) 0.04BMZ-BS-PT ceramics with different PT contents.
Fig. 7 shows the electric field induced unipolar strain curves of BMZ-BS-PT ceramics under the same driving electric field of 60 kV/cm. Generally, the strain
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caused by electric field are contributed by external and internal parts. The extrinsic
part is provided by the movement of domain walls and phase boundaries, while the
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internal part is supplied by the lattice distortion caused by inverse piezoelectric effect. The domain movement and switching process under an electric field can be partly
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reversible and partly irreversible. Furthermore, the domain switching could induce complex nonlinear and hysteretic behavior under high driving electric field.
37-39
It’s
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found that the strain of 0.02BMZ-BS-PT ceramics increase and then decrease through the transformation of rhombohedral to tetragonal, and reaches the maximum value at the MPB (0.64), which is approximately 0.24%. This can be attributed to the
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enhanced domain wall movement and polarizability in the MPB region where large numbers of thermodynamically stable polarization directions of the tetragonal phase
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(6 possible directions) and rhombohedral phase (8 possible directions) exist.22, 33 The same trend also exists in 0.04 BMZ doped ceramics, and the maximum value of unipolar strain is 0.21%, which is slightly lower than 0.02 BMZ doped ceramics. This may be related to the decrease of piezoelectric properties due to the increase of BMZ content.
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Fig. 8 (a). Unipolar strain curves of the 0.02BMZ-0.34BS-0.64PT ceramics measured at different temperatures, (b)
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the temperature-dependent d33* calculated from the obtained unipolar loop.
For precisely piezoelectric actuations, stable displacement output in a wide
temperature range is one of the most critical properties.12, 24, 40 As shown in Fig. 8(a), the unipolar strain curves of poled 0.02BMZ-0.34BS-0.64PT ceramics under the
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applied electric field of 10 kV/cm at various temperatures were measured. It is obvious seen that the field induced-strain keeps almost unchanged (less than 8%) in
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the temperature range of 50 to 200 oC, indicatings a reliable temperature stability of actuation performance. Above 200 ℃，the strain increase with the increase of
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environment temperatures, and it even reaches to 0.068% at 290 oC, which is about 1.5 time more than that at room temperature. The enhanced strain at higher temperature is attributed to the reason that the domain walls were activated by
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sufficient thermal energy and became more easily rotated by external electric field. Fig. 8(b) shows the measured large-signal piezoelectric coefficient d33* (Smax/Emax) as
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a function of temperature, which is obtained from the measured unipolar strains versus electric field curves. The good temperature stability below 200 ℃ guarantees
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the stable displacement output of the 0.02BMZ-0.34BS-0.64PT ceramic.
4. Conclusion
In summary, the phase structure, microstructure, piezoelectric, dielectric and ferroelectric properties of BMZ-BS-PT ceramics prepared by traditional solid-state reaction method were studied. The MPB composition of 0.02BMZ-BS-PT ceramics occurs near the PT content of 0.64. It is found that the introduction of BMZ reduces 16
the dielectric loss to about 0.58%, which is the lowest value ever reported in modified BSPT ceramics. Simultaneously, the planer electromechanical coupling coefficient (kp), dielectric constant (εr), piezoelectric constant (d33), Curie temperature (Tc), mechanical quality factor (Qm) and dielectric loss factor (tanδ) at the MPB content are measured to be 0.53, 1464, 360 pC/N, 449 oC, 61 and 0.58%, respectively. The strain outputs of 0.02BMZ-BS-PT ceramics are demonstrated to be stable below 200 oC (less than 8%). Comparing with other BS-PT based ceramics, these results indicate that the BMZ-BS-PT ceramics with lowest dielectric loss and high piezoelectric
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performance are very competitive piezoelectric materials for high temperature power electromechanical device applications.
Declaration of interests
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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.
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Acknowledgments
The authors gratefully acknowledge the support of the National Natural Science
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References
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Foundation of China (Grant No. 51772005 and 51705373).
1. S. J. Zhang, X. N. Jiang, M. Lapsley, P. Moses, T. R. Shrout, Piezoelectric accelerometers for ultrahigh
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temperature application, Appl. Phys. Lett., 96 (1) (2010) 013506. 2. J. G. Wu, H. D. Shi, T. L. Zhao, Y. Yu, and S. X. Dong, High-Temperature BiScO3-PbTiO3 Piezoelectric Vibration Energy Harvester, Adv. Funct. Mater., 26 (39) (2016) 7186-94. 3. J. G. Chen, J. R. Cheng, S. X. Dong, Review on high temperature piezoelectric ceramics and actuators based on BiScO3–PbTiO3 solid solutions, J. Adv. Dielectr., 4 (1) (2014) 1430002. 4. F. Li, D. B. Lin, Z. B. Chen, Z. X. Cheng, J. L. Wang, C. C. Li, Z. Xu, Q. W. Huang, X. Z. Liao, L. Q. Chen, T. R. Shrout, S. J. Zhang, Ultrahigh piezoelectricity in ferroelectric ceramics by design, Nat. Mater. 17 (4) (2018) 349-354. 5. S. Chen, X. L. Dong, C. L, Mao, F. Cao, Thermal stability of (1-x)BiScO3-xPbTiO(3) piezoelectric ceramics for high-temperature sensor applications, J. Am. Ceram. Soc., 89 (10) (2006) 3270-3272. 17
6. X. N. Jiang, K. Kim, S. J. Zhang, J. Johnson, and G. Salazar, High-Temperature Piezoelectric Sensing, Sensors, 14 (1) (2014) 144-169. 7. H. Y. Zhao, Y. D. Hou, X. L. Yu, M. P. Zheng, M. K. Zhu, Construction of high Tc BiScO3-BiFeO3-PbTiO3 and its enhanced piezoelectric properties by sintering in oxygen atmosphere, J. Appl. Phys., 124 (19) (2018) 194103. 8. H. Jia, X. K. Hu, J. G. Chen, Temperature-dependent piezoelectric strain and resonance performance of Fe2O3-modified BiScO3-PbTiO3-Pb(Nb1/3Mn2/3)O3 ceramics, J. Eur. Ceram. Soc., 39 (2019) 2348-2353. 9. J. K. Yang, Z. M. Li, X. D. Xin, X. Y. Gao, X. T. Yuan, Z. H. Wang, Z. H. Yu, X. H. Wang, J. Zhou, S. X. Dong, Dedigning electriomechanical metamaterial with full nanzero pieozelectric coefficients, Sci. Adv., 5 (2019) 1782. 10. M. A. Qaiser, X. Z. Ma, R. T. Ma, W. J. Ali, X. J. Xu, G. L. Yuan, and L. Chen, High‐temperature multilayer actuators based on CuO added BiScO3-PbTiO3 piezoceramics and Ag electrodes, J. Am. Ceram. Soc., 102, (9) (2019) 5424-5431. 11. Y. Saito, H. Takao, T. Tani, T. Nonoyama, K. Takatori, T. Homma, T. Nagaya M. Nakamura, Lead-free piezoceramics, Nature, 432 (2004) 84–87.
ro of
12. Z. Liu, C. L. Zhao, J. F. Li, K. Wang, J. G. Wu, Large strain and temperature-insensitive piezoelectric effect in high-temperature piezoelectric ceramics, J. Mater. Chem. C, 6 (2018) 456-463.
13. R. Guo, L. E. Cross, S. E. Park, B. Noheda, D. E. Cox, G. Shirane, Origin of the High Piezoelectric Response in PbZr1-xTixO3, Phys. Rev. Lett., 84 (23) (2008) 5423-5426.
14. T. L. Zhao, Z. L. Guo, and C. M. Wang, The Effects of Na/K Ratio on the Electrical Properties of Sodium‐
-p
Potassium Bismuth Titanate Na0.5Bi4.5Ti4O15-K0.5Bi4.5Ti4O15, J. Am. Ceram. Soc., 95 (3) 2012 1062-1067. 15. Z. H. Peng, Q. Chen, Y. D. Wang, D. Q. Xin, D. Q. Xiao, and J. G. Zhu, Mater. Lett., 2013, 15, 14-16.
16. J. Chen, J. Yuan, S. M. Bao, Y. J. Wu, G. Liu, Q. Chen, D. Q. Xiao, J. G. Zhu, Effects of (Li, Ce, Y)
re
co-substitution on the properties of CaBi2Nb2O9 high temperature piezoceramics, Ceram. Int., 43 (6) (2017) 5002-5006.
17. X. D. Zhang, H. X. Yan, and R. M. J. Reece, Effect of A Site Substitution on the Properties of CaBi2Nb2O9
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Ferroelectric Ceramics, J. Am. Ceram. Soc., 91 (9) (2008) 2928-2932.
18. R. E. Eitel, C. A. Randall, T. R. Shrout, S. E. Park, Preparation and Characterization of High Temperature Perovskite Ferroelectrics in the Solid-Solution (1-x)BiScO3–xPbTiO3, Jpn. J. Appl. Phys., 41 (2002) 2099-2104. 19. C. A. Randall, R. E. Eitel, B. Jones, T. R. Shrout, D. I. Woodward, I. M. Reaney, Investigation of a high Tc
na
piezoelectric system: (1−x)Bi(Mg1/2Ti1/2)O3-(x)PbTiO3, J. Appl. Phys., 95 (7) (2004) 3633-3639. 20. R. E. Eitel, C. A. Randall, T. R. Shrout, P. W. Rehring, W. Hackenberger, S. E. Park, New High Temperature Morphotropic Phase Boundary Piezoelectrics Based on Bi(Me)O3-PbTiO3 Ceramics, Jpn. J. Appl. Phys., 40 (2001)
ur
5999-6002.
21. S. S. Zhang, Y. Yu, J. G. Wu, X. Y. Gao, C. Huang, and S. X. Dong, Enhanced piezoelectric performance of BiScO3-PbTiO3 ceramics modified by 0.03Pb(Sb1/2Nb1/2)O3, J. Alloy. Compd., 731 (15) (2018) 1140-1145.
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22. J. G. Chen, T. L. Zhao, J. R. Cheng, S. X. Dong, Enhanced piezoelectric performance of (0.98-x) Bi(Sc3/4In1/4)O3-xPbTiO3-0.02Pb(Zn1/3Nb2/3)O3 ternary high temperature piezoelectric ceramics, J. Appl. Phys., 113 (14) (2013) 144102. 23. T. L. Zhao, J. G. Chen, C. M. Wang, Y. Yu, S. X. Dong, Ferroelectric, piezoelectric, and dielectric properties of BiScO3-PbTiO3-Pb(Cd1/3Nb2/3)O3 ternary high temperature piezoelectric ceramics, J. Appl. Phys., 114 (2) (2013) 027014. 24. T. L. Zhao, A. A. Bokov, J. G. Wu, H. L. Wang, C. M. Wang, Y. Yu, C. L. Wang, K. Y. Zeng, Z. G. Ye, S. X. Dong, Giant Piezoelectricity of Ternary Perovskite Ceramics at High Temperatures, Adv. Funct. Mater., 29 (2019) 1807920. 25. Z. H. Yao, H. X. Liu , Y. Liu, Z. Li, X. B. Cheng, M. H. Cao, and H. Hao, Morphotropic phase boundary in 18
Pb(Sc1/2Nb1/2)O3-BiScO3-PbTiO3 high temperature piezoelectrics, Mater. Lett., 62 (29) (2008) 4449-4451. 26. M. D. Drahus, P. Jakes, E. Erdem, S. Schaab, J. Chen, M. Ozerov, S. Zvyagin, R.-A. Eichel, Manganese-doped (1 − x)BiScO3–xPbTiO3 high-temperature ferroelectrics: Defect structure and mechanism of enhanced electric resistivity, Phys. Rev. B, 84 (2011) 064113. 27. S. J. Zhang, E. F. Alberta, R. E. Eitel, C. A. Randall, T. R. Shrout, Elastic, Piezoelectric, and Dielectric Characterization of Modified BiScO3-PbTiO3 Ceramics, IEEE T. Ultrason. Ferr., 52 (11) (2005) 2131-2139. 28. B. Kowalski, A. Sayir, A. Sehirlioglu, Aliovalent Mn Ti and GaTi substitution in hightemperature piezoelectric (x)Bi(Zn0.5Zr0.5)O3 - (y)BiScO3-(100 - x - y)PbTiO3, J. Mater. Sci. 51 (2016) 6761-6769. 29. B. L. Deng, Q. Wei, C. He, Z. J. Wang, X. M. Yang, X. F. Long, Effect of Pb(Mn1/3Sb2/3)O3 addition on the electrical properties of BiScO3-PbTiO3 piezoelectric ceramics, J. Alloy. Compd., 790 (2019) 397-404. 30. J.
Ryu ,
S.
Priya,
C.
Sakaki,
K.
Uchino,
High
power
piezoelectric
characteristics
of
BiScO3-PbTiO3-Pb(Mn1/3Nb2/3)O3, Jpn. J. Appl. Phys. 41 (2002) 6040-6044. 31. Z. Liu, B. Wu, and J. G. Wu, Reduced dielectric loss and high piezoelectric constant in Ce and Mn co-doped
ro of
BiScO3-PbCexTi1-xO3-Bi(Zn0.5Ti0.5)O3 ceramics, Ceram. Int., 44 (14) (2018) 16483-16488.
32. Z. H. Dai, J. L. Xie, W. G. Liu, S. B. Ge, M. X. Fang, D. B. Lin, L. X. Pang, H. F. Ji, S. Zhou, X. B. Ren, High piezoelectricity of BiScO3-PbTiO3 ceramics prepared by two step sintering, Mater. Lett., 241 (2019) 55-59.
33. X. Luo, J. T. Zeng, X. Shi, L. Y. Zheng, K. Y. Zhao, Z. Y. Man, G. R. Li, Dielectric, ferroelectric and
piezoelectric properties of MnO2-doped Pb(Yb1/2Nb1/2)O3-Pb(Zr,Ti)O3 ceramics, Ceram. Int., 44 (7) (2018)
-p
8456-8460.
34. J. G. Chen, Z. Q. Hu, H. D. Shi, M. Y. Li, S. X. Dong, High-power piezoelectric characteristics of manganese-modified BiScO3-PbTiO3 high-temperature piezoelectric ceramics, J. Phys. D Appl. Phys., 45 (46)
re
(2012) 465303.
35. J. G. Chen, G. X. Jin, C. M. Wang, J. R. Cheng, Reduced Dielectric Loss and Strain Hysteresis in Fe and Mn Comodified High-Temperature BiScO3-PbTiO3 Ceramics, J. Am. Ceram. Soc., 97 (12) (2014) 3890-3896.
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36. J. G. Wu, Y. Yu, X. T. Li, X. Y. Gao, and S. X. Dong, Investigation on Resonant Vibration Performances of Fe-Doped BiScO3-PbTiO3 Ceramics in High-Temperature Environment, J. Am. Ceram. Soc., 98 (10) (2015) 3145 3152.
37. T. L. Zhao, C. L. Fei, X. Y. Dai, J. J. Song, S. X. Dong, Structure and enhanced piezoelectric performance of
na
BiScO3-PbTiO3-Pb(Ni1/3Nb2/3)O3 ternary high temperature piezoelectric ceramics, J. Alloy. Compd., 806 (2019) 11-18.
38. G. Viola, T. Saunders, X. Wei, K. B. Chong, H. Luo, M. J. Reece, H. Yan, Contribution of piezoelectric effect,
ur
electrostriction and ferroelectric/ferroelastic switching to strain-electric field response of dielectrics, J. Adv. Dielec., 3 (1) (2013) 1350007.
39. Y. Tan, G. Viola, V. Koval, C. Yu, A. Mahajan, J. Zhang, H. Zhang, X. Zhou, N.V. Tarakina, H. Yan,On the
Jo
origin of grain size effects in Ba(Ti0.96Sn0.04)O3 perovskite ceramics, J. Eur. Ceram. Soc., 39 (6) (2019) 2064-2075. 40. N. N. Luo, Q. Li, Z. G. Xia, and X. C. Chu, Phase Diagram, Temperature Stability, and Electrical Properties of (0.85−x)Pb(Mg1/3Nb2/3)O3-0.10Pb(Fe1/2Nb1/2)O3-0.05PbZrO3-xPbTiO3 System, J. Am. Ceram. Soc., 95 (10) (2012) 3246-3253.
19
PII:
S0955-2219(20)30095-9
DOI:
https://doi.org/10.1016/j.jeurceramsoc.2020.02.015
Reference:
JECS 13062
To appear in:
Journal of the European Ceramic Society
Please cite this article as: Yu Y, Yang J, Wu J, Gao X, Bian L, Li X, Xin X, Yu Z, Chen W, Dong S, Ultralow dielectric loss of BiScO3 -PbTiO3 ceramics by Bi(Mn1/2 Zr1/2 )O3 modification, Journal of the European Ceramic Society (2020), doi: https://doi.org/10.1016/j.jeurceramsoc.2020.02.015
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Ultralow dielectric loss of BiScO3-PbTiO3 ceramics by Bi(Mn1/2Zr1/2)O3 modification
Yang Yu1,2, Jikun Yang2, Jingen Wu2 , Xiangyu Gao 2, Lang Bian 2, Xiaotian Li 3 , Xudong Xin2 , Zhonghui Yu2, Wanping Chen 1,*, Shuxiang Dong 2, * 1
School of Physics and Technology, Wuhan University, Wuhan, Hubei, 430072, China 2 Department of Materials Science and Engineering, College of Engineering,
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Peking University, Beijing, 100871, China 3 Department of materials science and engineering, school of power and mechanical engineering, Wuhan University, Wuhan, Hubei, 430072, China *Corresponding authors E-mail addresses: [email protected] (W. Chen), [email protected] (S. Dong).
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Abstract
BiScO3-PbTiO3 ceramics are attractive for high-temperature piezoelectric applications while their high dielectric loss has to be substantially reduced. In this
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paper, a ternary perovskite system of xBi(Mn1/2Zr1/2)O3-(1-x-y)BiScO3-yPbTiO3 (abbreviated as xBMZ-BS-yPT) with x = 0.02, 0.04 and y = 0.62 - 0.67 were
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fabricated by conventional solid-phase method, and their ceramics were systematically studied with regards to phase structure, microstructure, dielectric and
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piezoelectric properties. X-ray diffraction results indicate a gradual change from rhombohedral to tetragonal phase with increasing PT composition. Morphotropic phase boundary (MPB) is revealed for the system with x = 0.02，y = 0.64, at which ultralow dielectric loss factor (0.58%), almost unchanged Curie temperature (449 oC), high electromechanical properties (d33 = 360 pC/N, kp = 0.53), and stable strain output below 200 oC are observed. With such excellent piezoelectric properties and high-temperature stability, BMZ modified BS-PT ceramics are promising candidates 1
for power electromechanical devices, especially operating in high-temperature environments.
Keywords ： Ultralow dielectric loss factor (tanδ); Piezoelectric ceramics; BiScO3-PbTiO3; High-temperature application; Temperature stability.
1．Introduction Nowadays, there is an increasing technological demand for sensors and transducers
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operating at rather high temperatures (T > 200 oC), such as those applied in oil/gas
drilling and aerospace explorations industries.1-7 Traditional lead-based piezoelectric ceramics have been widely applied in various industrial devices at room temperature
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or relatively low temperatures. Especially, Pb(Zr,Ti)O3-based ceramics have highly competitive properties, such as good piezoelectric and electromechanical properties near the MPB composition.8-13 However, it is very difficult for PZT-based ceramics to
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be used above 200 oC, because their Curie temperature is below 350 ℃ and they may
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start to depolarize above 200 oC. Bismuth layer structured ceramics, such as Na0.5Bi4.5Ti3.975Co0.025O15 (Tc ~ 670 oC),14 CaBi2Nb2O9 (Tc ~ 930 oC),15 usually possess very high Curie temperature. However, their applications are limited due to
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relatively lower piezoelectric constant (d33 ≦ 40 pC/N).14-17 Recently, the discovery of perovskite compound Bi(Me)O3-PbTiO3 systems (Me =
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Sc, In, Yb, Y, etc) has attracted more and more research interest for high temperature piezoelectric applications. It is reported that 0.36BiScO3-0.64PbTiO3 ceramics in
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MPB composition simultaneously have large piezoelectric constant (d33 = 450 pC/N) and high Curie temperature Tc around 450 oC, which is about 100 oC higher than that of commercial PZT piezoelectric ceramics.18-20 The ceramic series exhibit great potential for high temperature applications. However, the high dielectric loss factor (tanδ > 3%) and low mechanical quality factor (Qm < 30) of BS-PT-based ceramics will cause serious heat generation and energy dissipation and further restrict their applications as power electronic devices operating at resonance frequency.21-25 To 2
decrease tanδ or increase Qm, previous works have reported some methods such as MnO2 doping and introduction of Pb(Mn1/3Sb1/3)O3 or Pb(Mn1/3Nb1/3)O3.26-30 Unfortunately, the dielectric loss factor of these modified ceramics is still at a relatively high level (tanδ > 1%), and what is worse, the piezoelectric performance (d33 < 300 pC/N) deteriorates seriously.31 In this paper, for the first time, we report that the introduction of Bi(Mn1/2Zr1/2)O3 (BMZ) end member into BS-PT ceramics can greatly reduce dielectric loss factor, while piezoelectric coefficient and Curie temperature are still maintained at relatively
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high values. BMZ of different concentrations were introduced in BS-PT ceramics, and the effects of PT concentration on the phase, microstructure, dielectric, ferroelectric and piezoelectric properties were also investigated in detail. Ultralow dielectric loss
factor (tanδ = 0.58%), large piezoelectric constant (d33 = 360 pC/N), high planar
-p
electromechanical coupling coefficient (kp = 0.53) and high Tc (Tc = 449 oC) were
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2. Experimental procedure
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obtained at 0.02Bi(Mn1/2Zr1/2)O3-0.34BiScO3-0.64PbTiO3 MPB composition.
Series of xBi(Mn1/2Zr1/2)O3-(1-x-y)BiScO3-yPbTiO3 ceramics (abbreviated as xBMZ-BS-yPT), with x = 0.02, 0.04 and y = 0.62 - 0.67, were prepared by the
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conventional mixed oxide process method. The starting raw materials, including PbO (99.9%), Bi2O3 (99%), Sc2O3 (99.99%), MnO2 (97.5%), TiO2 (99%) and ZrO2 (99%),
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were weighted according to the stoichiometric proportion with 2% PbO excess to compensate the evaporation of lead during the high-temperature sintering reaction.
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They were wet milled in polyethylene jar with agate balls for 8 h in ethanol. The milled powder was dried at 100 oC and calcined at 850 oC for 3 h in air. The calcined powder was then ball-milled for 24 h. Dried powder was sieved and pressed into pellets (Ф 14 × 1.2 mm3) using PVA as a binder at a pressure of 10 MPa followed by cold iso-static pressing (CIP) under pressure of 200 MPa for 10 min. After burning off PVA, the green compacts were embedded in the calcined powder of the same composition and sintered in a covered crucible at 1000 - 1040 oC for 2 h. 3
The crystalline structures of the sintered pellets were determined by X-ray diffraction (XRD) technology with Cu-Ka1 radiation (D/Max 2500, Rigaku, Tokyo, Japan). The fracture surface microstructure of the sintered pellets was observed by scanning electron microscopy (SEM, S-4800, Hitachi, Tokyo, Japan). The density of the ceramics was measured using a density tester according to Archimedes method. The sintered pellets were polished down to 0.8 mm, and were coated by electrodes with a post-fire silver paste at 650 °C for 0.5 h. For electrical measurements, the ceramics were poled in 140 oC silicone oil bath under a DC electric field of 40 kV/cm
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for 20 min. The poled specimens were aged in air for 24 h before any electrical measurement. The piezoelectric constant d33 was measured using a quasistatic d33 meter (ZJ-3D, Institute of Acoustics, Beijing, China). The dielectric constant and loss factor (tanδ) were measured in the temperature range from room temperature to 500 o
-p
C at the frequency of 1 kHz by utilizing an impedance analyzer (4294A, Agilent
Technologies). The electromechanical coupling factor kp and the mechanical quality
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factor Qm were calculated according to formulae (1) - (2) by using the resonance and anti-resonance technique (using an impedance analyzer 4294A, Agilent Technologies).
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The room temperature P-E hysteresis loops of samples were measured at a frequency of 1 Hz using a ferroelectric testing system (TF Analyzer 2000, aixACCT Systems
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GmbH, Germany).
1
2
fr
0 . 398
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Qm
0 . 579
fa fr
kp
(1)
2
fa 2 f r RC
T
( fa fr ) 2
2
(2)
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Here, fr and fa are the resonance and anti-resonance frequencies, respectively, R is the resonant impedance, and CT is the electric capacitance at 1 kHz.
3. Results and discussion
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Fig. 1 XRD patterns of (a) 0.02Bi(Mn1/2Zr1/2)O3-(0.98-y)BiScO3-yPbTiO3, with y = 0.62, 0.63, 0.64, 0.65, 0.66, 0.67, (b) Enlarged view of XRD patterns at 2θ = 31 - 33o, (c) 0.04Bi(Mn1/2Zr1/2)O3-(0.96-y)BiScO3-yPbTiO3, with
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y = 0.62, 0.63, 0.64, 0.65, 0.66, 0.67, (d) Enlarged view of XRD patterns at 2θ = 31 - 33o, (e) and (f) the calculated
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lattice parameters and c/a ratios obtained from these patterns.
Fig. 1 (a) and (b) display the room temperature X-ray diffraction spectra of 0.02Bi(Mn1/2Zr1/2)O3-(0.98-y)BiScO3-yPbTiO3 (y = 0.62, 0.63, 0.64, 0.65, 0.66, 0.67)
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ceramics sintered at 1040 oC with various PT contents. There are no traces of pyrochlore phase or impurities in the XRD patterns of any specimens, indicating that
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the BMZ members with BS-PT solid solution formed a stable single-phase perovskite structure. Meanwhile, the coexistence of rhombohedral (R) and tetragonal (T) phases is detectable. The effect of the PT content on the phase composition of ceramics is studied. It can be seen that the phase structure of the ceramic with y = 0.62 is rhombohedral (R) phase. While in the XRD pattern of the ceramic with y = 0.67, the splitting of (110)T and (101)T peak is markedly observed, indicating that the phase structure of BMZ-BSPT ceramic has changed into tetragonal (T) phase.32 With the 5
decrease of PT content from 0.67 to 0.62, the crystalline phase of ceramics gradually changes from tetragonal to rhombohedral. Thus, it is clear that the morphotropic phase boundary (MPB) exists in the range of y = 0.63 - 0.65. Piezoelectric ceramics near the MPB region will present the highest d33. The similar situation occurs in 0.04Bi(Mn1/2Zr1/2)O3-(0.96-y)BiScO3-yPbTiO3 ceramics from Fig. 1 (c) and (d). With the increase of PT content from 0.62 to 0.67, (100) single peak near 2θ = 31o - 33o degree splits into two peaks of (101) and (110), which reveals that the crystalline phase of ceramics changes from rhombohedral to tetragonal. It is clear that the
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morphotropic phase boundary (MPB) near the range of y = 0.63 - 0.65 is obtained. Tetragonality (which is reflected in the c/a ratio) is an important structural
parameter of the perovskite lattice that determines the spontaneous polarization of piezoelectric ceramics. Fig. 1 (e) and (f) show the calculated tetragonality values of
-p
0.02BMZ-BSPT and 0.04BMZ-BSPT ceramics as a function of PT content. It can be
seen that the increase of PT content leads to tetragonality strengthening, as a result of
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PT being tetragonal phase.
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7
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Fig. 2 SEM images of the fracture surfaces from (a)-(f) 0.02BMZ-(0.98-y)BS-yPT (y = 0.62 - 0.67) ceramics and (g) - (l) 0.04BMZ-(0.96-y)BS-yPT (y = 0.62 - 0.67) ceramics.
Fig. 2 shows the fresh fracture surfaces of 0.02BMZ-(0.98-y)BS-yPT and
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0.04BMZ-(0.96-y)BS-yPT (y = 0.62 - 0.67) ceramics samples sintered at 1040 oC for 2 h. The ceramics samples are high density, with few holes, tight grains and distinct
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grain boundaries. The fracture modes of both are mainly intergranular fracture, which indicate that the mechanical strength of grain was stronger than the grain boundary, and fine crystallization was obtained. In order to explore the grain size distribution quantitatively, the linear intercept method was used to statistically analyze the grain size, and the results are given in the insets of Fig. 2. The average grain size of 0.02BMZ-0.34BS-0.64PT sample is around 4.97-7.37 μm, and 0.04BMZ-0.32BS-0.64PT sample possess a large grain size of 8
approximately 9.1-11.3 μm. The average grain size increases with the increased BMZ doping amount. Similar phenomena are also observed in previous Mn-doped or PMS-doped BS-PT-based systems.[29,33-36] Similar to previous reported results, oxygen vacancies are generated because of Ti substitution by multi-valence Mn element (Mn2+ or Mn3+), which promotes mass transport and further assists grain growth during sintering process.[29, 36] TABLE 1. Room temperature piezoelectric and dielectric properties of BMZ-BS-PT ceramics.
d33 (pC/N)
kp
0.02BMZ-0.36BS-0.62PT
Cm
240
0.51
0.02BMZ-0.35BS-0.63PT
Cm/P4mm
310
0.52
0.02BMZ-0.34BS-0.64PT
Cm/P4mm
360
0.53
0.02BMZ-0.33BS-0.65PT
P4mm
280
0.43
0.02BMZ-0.32BS-0.66PT
P4mm
210
0.02BMZ-0.31BS-0.67PT
P4mm
200
0.04BMZ-0.34BS-0.62PT
Cm
0.04BMZ-0.33BS-0.63PT
Cm/P4mm
0.04BMZ-0.32BS-0.64PT
Cm/P4mm
0.04BMZ-0.31BS-0.65PT
Qm
Tc (oC)
ρ (g/cm3)
0.34%
676
102
434
7.68
0.54%
1048
97
445
7.64
0.58%
1464
61
449
7.59
0.49%
1276
171
455
7.62
0.47%
976
178
464
7.59
0.35
0.40%
813
250
472
7.57
re
0.38
0.47
0.36%
655
174
406
7.58
270
0.48
0.50%
839
163
424
7.50
281
0.51
0.52%
1333
155
430
7.55
P4mm
230
0.43
0.43%
1172
271
438
7.57
P4mm
190
0.38
0.35%
1012
414
445
7.58
P4mm
161
0.35
0.32%
836
535
456
7.58
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0.04BMZ-0.29BS-0.67PT
εr
220
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0.04BMZ-0.30BS-0.66PT
tan δ (1kHz)
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Space group
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Material
Table 1 summarizes the piezoelectric and dielectric properties of BMZ-BS-PT
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ceramics. It’s found that the values of d33, kp and εr for 0.02BMZ-BS-PT ceramics are very sensitive to the phase structure, which are determined by PT contents. These
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three values reach their maximum at the PT content of 0.64. This results further demonstrate that the MPB content of 0.02BMZ-BS-PT ceramics occurs at the PT content of 0.64. The excellent dielectric and piezoelectric properties are attributed to the coupling between two equivalent energy states, i.e., the rhombohedral and tetragonal phases, which promotes optimum domain reorientation during the poling. Dielectric loss factor (tanδ) of 0.02BMZ-BS-PT ceramics is below 0.58%, which is much less than that (tanδ = 3%) of pure BS-PT ceramics, indicating that the 9
introduction of BMZ to BS-PT can effectively restrain dielectric loss. Compared with the Qm of pure ceramics (around 20), it can be seen from the calculated results presented in Table 1 that Qm (61 - 250) values of 0.02BMZ-BS-PT ceramics have been improved a lot. According to previous researched reports, Mn ions can exist as multivalent states in perovskite phase, such as Mn2+, Mn3+, and Mn4+, especially, Mn2+ and Mn3+ states could coexist and replace the B4+ ions in ABO3-type perovskites. Therefore, this substitution may lead to acceptor characteristic and form oxygen vacancies to maintain the electrical neutrality. The oxygen vacancy can cause pinning
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effect and inhibit domain wall movement, so that tanδ is decreased and Qm is improved. The optimum values of planar electromechanical coupling coefficient (kp), dielectric constant (εr), piezoelectric constant (d33), Curie temperature (Tc) and dielectric loss factor (tan δ) at the MPB content are 0.53, 1464, 360 pC/N, 449 oC and
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0.58%, respectively.
When the BMZ content increased from 2 mol% to 4 mol%, d33, εr, Tc and kp are
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relatively reduced. But dielectric loss factor tan δ and Mechanical quality factor Qm show better values. The MPB composition of 0.04BMZ-BS-PT ceramics occurs at the
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PT content of 0.64. The dielectric loss factor is further reduced while Qm is significantly improved. This phenomenon can be apparently attributed to the
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generation of more oxygen vacancies with BMZ content increase. This also reveals that the BMZ is more effective composition of Mn doping29, 31 to decrease dielectric loss of BSPT ceramics and transform the material from soft-type ceramics to
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hard-type ones. The excellent values of planar electromechanical coupling coefficient (kp), dielectric constant (εr), piezoelectric constant (d33), Curie temperature (Tc),
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mechanical quality factor (Qm) and dielectric loss factor (tan δ) at the 0.64 content are measured to be 0.51, 1333, 281 pC/N, 430 oC, 155 and 0.52%, respectively.
10
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Fig. 3 Temperature-dependent dielectric constant εr and dielectric loss factor tanδ of (a) and (b) 0.02BMZ-BS-PT ceramics and (c) and (d) 0.04BMZ-BS-PT ceramics.
To demonstrate the stable performance of this novel material under high
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temperature, the temperature dependence of the dielectric constant and dielectric loss of 0.02BMZ-(0.98-y)BS-yPT and 0.04BMZ-(0.96-y)BS-yPT ceramic samples sintered
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at 1040 oC were tested at 1 kHz frequency as shown in Fig. 3. The temperature Tm corresponded to the maximum value of the dielectric constant is considered to be the
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Curie temperature Tc. For all ceramics, Curie temperature increase with the increase of PT content, as shown in Fig. 3 (a and b), which are ascribed to the high phase transition temperature of PbTiO3 (490 oC) member. For the 0.02BMZ-0.34BS-0.64PT ceramic samples, Curie temperature Tc is 449 oC, which is almost consistent with pure 0.36BS-0.64PT Curie temperature (Tc = 450 oC).18 Therefore, the deterioration of Curie temperature caused by introducing BMZ into BS-PT ceramics is much smaller than Mn and PMS, which is beneficial for ceramics to work at high temperature.18 11
The dielectric loss factor (tanδ) drops dramatically at room temperature as the BMZ content increase. The dielectric loss factor of all ceramics are less than 0.58%, especially, the dielectric loss factor of 0.04BMZ-0.39BS-0.67PT even reaches down to 0.35%. Clearly, in comparison with pure BS-PT or soft BS-PT-based ceramics with high loss factor (approximately 3%),18 the BMZ modification is a very effective way
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to reduce dielectric loss factor.
Fig. 4 Effect of thermal depoling on d33 values of (a) 0.02BMZ-BS-PT and (b) 0.04BMZ-BS-PT with different PT
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contents.
For high temperature application, the temperature stability of piezoelectric ceramics
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is one of the most important qualities. To verify the high-temperature stability of BMZ-BSPT, the polarized plate samples are annealed at different temperatures for one hour and their piezoelectric constant d33 was measured again at room temperature.
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Fig. 4 shows the measured piezoelectric constant d33 of 2% - 4% mol BMZ doped ceramics from room temperature (RT) up to 450 oC. It is clearly seen that at the initial
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stage (temperature T is below 250 ℃), d33 values appear to be almost unchanged as T rises. However, when T increases to depolarization temperature Td or it is close to the
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Curie temperature Tc, d33 values fall rapidly. The temperature at which d33 values decline rapidly is estimated as the depolarization temperature (Td). The depolarization temperatures of 0.02 BMZ and 0.04 BMZ doped ceramics are about 325 oC. The high Td should be attributed to the large coercive field (approximate 20 kV/cm) and high Curie temperature (approximate 450 oC), which are far higher than that of PZT ceramics (10 kV/cm and 350 oC). The high Tc means that a large thermodynamic movement energy is needed to destroy the ferroelectricity. It should be noted that 12
these values are about 150 oC higher than that of soft type PZT ceramics, and
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BMZ-BS-PT ceramics show their great potential for high-temperature application.
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Fig. 5 Piezoelectric constant d33 and dielectric loss factor (tan δ) of 0.02BMZ-0.34BS-0.64 PT ceramics in comparison with reported BS-PT based ceramics.
In order to evaluate the excellent performances of this novel material, we made a
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statistical study as illustrated in Fig. 5, including d33 and tan δ values of our samples 8, 12, 29, 31, 36
The 0.02BMZ -
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and other ceramics reported in previous literatures.7,
0.34BS - 0.64PT ceramic simultaneously exhibits both high d33 (360 pC/N) and the lowest tan δ (0.58%) that are never reported in modified BS-PT ceramic series. The
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comprehensive properties of this material are better than most of BS-PT based ceramics. Thus, this ceramic is potential for piezoelectric materials and devices
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employed in high temperature environments.
13
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Fig. 6 Room temperature P - E loops of (a) 0.02BMZ-BS-PT and (b) 0.04BMZ-BS-PT ceramics with different PT contents, (c) and (d) Pr and Ec of 0.02BMZ-BS-PT and 0.04BMZ-BS-PT ceramics with differing PT contents.
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Fig. 6 shows the polarization-electric field (P - E) hysteresis loops of the BMZ-BS-PT ceramics. These polarization loops were measured at frequency of 1Hz
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under an electric field of 60 kV/cm. They are symmetric and no obvious conductive problem observed. The remnant polarization Pr of 0.02BMZ-BS-PT ceramic samples increases with PT content, and reaches maximum value at y = 0.64 composition
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(MPB), then decreases with further increased PT content. Similar results also occur in 0.04BMZ-BS-PT ceramic series. The values of remnant polarization and coercive
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electric field of the 0.02BMZ-BS-PT series and 0.04BMZ-BS-PT series range from 4.8 - 18 μC/cm2 and 16.4 - 21.8 kV/cm, 5.1 - 17.5 μC/cm2 and 18.5 - 24 kV/cm, respectively.
14
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Fig. 7 Unipolar strain-electric field (S-E) curves at room temperature of (a) 0.02BMZ-BS-PT and (b) 0.04BMZ-BS-PT ceramics with different PT contents.
Fig. 7 shows the electric field induced unipolar strain curves of BMZ-BS-PT ceramics under the same driving electric field of 60 kV/cm. Generally, the strain
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caused by electric field are contributed by external and internal parts. The extrinsic
part is provided by the movement of domain walls and phase boundaries, while the
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internal part is supplied by the lattice distortion caused by inverse piezoelectric effect. The domain movement and switching process under an electric field can be partly
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reversible and partly irreversible. Furthermore, the domain switching could induce complex nonlinear and hysteretic behavior under high driving electric field.
37-39
It’s
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found that the strain of 0.02BMZ-BS-PT ceramics increase and then decrease through the transformation of rhombohedral to tetragonal, and reaches the maximum value at the MPB (0.64), which is approximately 0.24%. This can be attributed to the
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enhanced domain wall movement and polarizability in the MPB region where large numbers of thermodynamically stable polarization directions of the tetragonal phase
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(6 possible directions) and rhombohedral phase (8 possible directions) exist.22, 33 The same trend also exists in 0.04 BMZ doped ceramics, and the maximum value of unipolar strain is 0.21%, which is slightly lower than 0.02 BMZ doped ceramics. This may be related to the decrease of piezoelectric properties due to the increase of BMZ content.
15
Fig. 8 (a). Unipolar strain curves of the 0.02BMZ-0.34BS-0.64PT ceramics measured at different temperatures, (b)
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the temperature-dependent d33* calculated from the obtained unipolar loop.
For precisely piezoelectric actuations, stable displacement output in a wide
temperature range is one of the most critical properties.12, 24, 40 As shown in Fig. 8(a), the unipolar strain curves of poled 0.02BMZ-0.34BS-0.64PT ceramics under the
-p
applied electric field of 10 kV/cm at various temperatures were measured. It is obvious seen that the field induced-strain keeps almost unchanged (less than 8%) in
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the temperature range of 50 to 200 oC, indicatings a reliable temperature stability of actuation performance. Above 200 ℃，the strain increase with the increase of
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environment temperatures, and it even reaches to 0.068% at 290 oC, which is about 1.5 time more than that at room temperature. The enhanced strain at higher temperature is attributed to the reason that the domain walls were activated by
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sufficient thermal energy and became more easily rotated by external electric field. Fig. 8(b) shows the measured large-signal piezoelectric coefficient d33* (Smax/Emax) as
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a function of temperature, which is obtained from the measured unipolar strains versus electric field curves. The good temperature stability below 200 ℃ guarantees
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the stable displacement output of the 0.02BMZ-0.34BS-0.64PT ceramic.
4. Conclusion
In summary, the phase structure, microstructure, piezoelectric, dielectric and ferroelectric properties of BMZ-BS-PT ceramics prepared by traditional solid-state reaction method were studied. The MPB composition of 0.02BMZ-BS-PT ceramics occurs near the PT content of 0.64. It is found that the introduction of BMZ reduces 16
the dielectric loss to about 0.58%, which is the lowest value ever reported in modified BSPT ceramics. Simultaneously, the planer electromechanical coupling coefficient (kp), dielectric constant (εr), piezoelectric constant (d33), Curie temperature (Tc), mechanical quality factor (Qm) and dielectric loss factor (tanδ) at the MPB content are measured to be 0.53, 1464, 360 pC/N, 449 oC, 61 and 0.58%, respectively. The strain outputs of 0.02BMZ-BS-PT ceramics are demonstrated to be stable below 200 oC (less than 8%). Comparing with other BS-PT based ceramics, these results indicate that the BMZ-BS-PT ceramics with lowest dielectric loss and high piezoelectric
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performance are very competitive piezoelectric materials for high temperature power electromechanical device applications.
Declaration of interests
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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.
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Acknowledgments
The authors gratefully acknowledge the support of the National Natural Science
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References
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Foundation of China (Grant No. 51772005 and 51705373).
1. S. J. Zhang, X. N. Jiang, M. Lapsley, P. Moses, T. R. Shrout, Piezoelectric accelerometers for ultrahigh
Jo
temperature application, Appl. Phys. Lett., 96 (1) (2010) 013506. 2. J. G. Wu, H. D. Shi, T. L. Zhao, Y. Yu, and S. X. Dong, High-Temperature BiScO3-PbTiO3 Piezoelectric Vibration Energy Harvester, Adv. Funct. Mater., 26 (39) (2016) 7186-94. 3. J. G. Chen, J. R. Cheng, S. X. Dong, Review on high temperature piezoelectric ceramics and actuators based on BiScO3–PbTiO3 solid solutions, J. Adv. Dielectr., 4 (1) (2014) 1430002. 4. F. Li, D. B. Lin, Z. B. Chen, Z. X. Cheng, J. L. Wang, C. C. Li, Z. Xu, Q. W. Huang, X. Z. Liao, L. Q. Chen, T. R. Shrout, S. J. Zhang, Ultrahigh piezoelectricity in ferroelectric ceramics by design, Nat. Mater. 17 (4) (2018) 349-354. 5. S. Chen, X. L. Dong, C. L, Mao, F. Cao, Thermal stability of (1-x)BiScO3-xPbTiO(3) piezoelectric ceramics for high-temperature sensor applications, J. Am. Ceram. Soc., 89 (10) (2006) 3270-3272. 17
6. X. N. Jiang, K. Kim, S. J. Zhang, J. Johnson, and G. Salazar, High-Temperature Piezoelectric Sensing, Sensors, 14 (1) (2014) 144-169. 7. H. Y. Zhao, Y. D. Hou, X. L. Yu, M. P. Zheng, M. K. Zhu, Construction of high Tc BiScO3-BiFeO3-PbTiO3 and its enhanced piezoelectric properties by sintering in oxygen atmosphere, J. Appl. Phys., 124 (19) (2018) 194103. 8. H. Jia, X. K. Hu, J. G. Chen, Temperature-dependent piezoelectric strain and resonance performance of Fe2O3-modified BiScO3-PbTiO3-Pb(Nb1/3Mn2/3)O3 ceramics, J. Eur. Ceram. Soc., 39 (2019) 2348-2353. 9. J. K. Yang, Z. M. Li, X. D. Xin, X. Y. Gao, X. T. Yuan, Z. H. Wang, Z. H. Yu, X. H. Wang, J. Zhou, S. X. Dong, Dedigning electriomechanical metamaterial with full nanzero pieozelectric coefficients, Sci. Adv., 5 (2019) 1782. 10. M. A. Qaiser, X. Z. Ma, R. T. Ma, W. J. Ali, X. J. Xu, G. L. Yuan, and L. Chen, High‐temperature multilayer actuators based on CuO added BiScO3-PbTiO3 piezoceramics and Ag electrodes, J. Am. Ceram. Soc., 102, (9) (2019) 5424-5431. 11. Y. Saito, H. Takao, T. Tani, T. Nonoyama, K. Takatori, T. Homma, T. Nagaya M. Nakamura, Lead-free piezoceramics, Nature, 432 (2004) 84–87.
ro of
12. Z. Liu, C. L. Zhao, J. F. Li, K. Wang, J. G. Wu, Large strain and temperature-insensitive piezoelectric effect in high-temperature piezoelectric ceramics, J. Mater. Chem. C, 6 (2018) 456-463.
13. R. Guo, L. E. Cross, S. E. Park, B. Noheda, D. E. Cox, G. Shirane, Origin of the High Piezoelectric Response in PbZr1-xTixO3, Phys. Rev. Lett., 84 (23) (2008) 5423-5426.
14. T. L. Zhao, Z. L. Guo, and C. M. Wang, The Effects of Na/K Ratio on the Electrical Properties of Sodium‐
-p
Potassium Bismuth Titanate Na0.5Bi4.5Ti4O15-K0.5Bi4.5Ti4O15, J. Am. Ceram. Soc., 95 (3) 2012 1062-1067. 15. Z. H. Peng, Q. Chen, Y. D. Wang, D. Q. Xin, D. Q. Xiao, and J. G. Zhu, Mater. Lett., 2013, 15, 14-16.
16. J. Chen, J. Yuan, S. M. Bao, Y. J. Wu, G. Liu, Q. Chen, D. Q. Xiao, J. G. Zhu, Effects of (Li, Ce, Y)
re
co-substitution on the properties of CaBi2Nb2O9 high temperature piezoceramics, Ceram. Int., 43 (6) (2017) 5002-5006.
17. X. D. Zhang, H. X. Yan, and R. M. J. Reece, Effect of A Site Substitution on the Properties of CaBi2Nb2O9
lP
Ferroelectric Ceramics, J. Am. Ceram. Soc., 91 (9) (2008) 2928-2932.
18. R. E. Eitel, C. A. Randall, T. R. Shrout, S. E. Park, Preparation and Characterization of High Temperature Perovskite Ferroelectrics in the Solid-Solution (1-x)BiScO3–xPbTiO3, Jpn. J. Appl. Phys., 41 (2002) 2099-2104. 19. C. A. Randall, R. E. Eitel, B. Jones, T. R. Shrout, D. I. Woodward, I. M. Reaney, Investigation of a high Tc
na
piezoelectric system: (1−x)Bi(Mg1/2Ti1/2)O3-(x)PbTiO3, J. Appl. Phys., 95 (7) (2004) 3633-3639. 20. R. E. Eitel, C. A. Randall, T. R. Shrout, P. W. Rehring, W. Hackenberger, S. E. Park, New High Temperature Morphotropic Phase Boundary Piezoelectrics Based on Bi(Me)O3-PbTiO3 Ceramics, Jpn. J. Appl. Phys., 40 (2001)
ur
5999-6002.
21. S. S. Zhang, Y. Yu, J. G. Wu, X. Y. Gao, C. Huang, and S. X. Dong, Enhanced piezoelectric performance of BiScO3-PbTiO3 ceramics modified by 0.03Pb(Sb1/2Nb1/2)O3, J. Alloy. Compd., 731 (15) (2018) 1140-1145.
Jo
22. J. G. Chen, T. L. Zhao, J. R. Cheng, S. X. Dong, Enhanced piezoelectric performance of (0.98-x) Bi(Sc3/4In1/4)O3-xPbTiO3-0.02Pb(Zn1/3Nb2/3)O3 ternary high temperature piezoelectric ceramics, J. Appl. Phys., 113 (14) (2013) 144102. 23. T. L. Zhao, J. G. Chen, C. M. Wang, Y. Yu, S. X. Dong, Ferroelectric, piezoelectric, and dielectric properties of BiScO3-PbTiO3-Pb(Cd1/3Nb2/3)O3 ternary high temperature piezoelectric ceramics, J. Appl. Phys., 114 (2) (2013) 027014. 24. T. L. Zhao, A. A. Bokov, J. G. Wu, H. L. Wang, C. M. Wang, Y. Yu, C. L. Wang, K. Y. Zeng, Z. G. Ye, S. X. Dong, Giant Piezoelectricity of Ternary Perovskite Ceramics at High Temperatures, Adv. Funct. Mater., 29 (2019) 1807920. 25. Z. H. Yao, H. X. Liu , Y. Liu, Z. Li, X. B. Cheng, M. H. Cao, and H. Hao, Morphotropic phase boundary in 18
Pb(Sc1/2Nb1/2)O3-BiScO3-PbTiO3 high temperature piezoelectrics, Mater. Lett., 62 (29) (2008) 4449-4451. 26. M. D. Drahus, P. Jakes, E. Erdem, S. Schaab, J. Chen, M. Ozerov, S. Zvyagin, R.-A. Eichel, Manganese-doped (1 − x)BiScO3–xPbTiO3 high-temperature ferroelectrics: Defect structure and mechanism of enhanced electric resistivity, Phys. Rev. B, 84 (2011) 064113. 27. S. J. Zhang, E. F. Alberta, R. E. Eitel, C. A. Randall, T. R. Shrout, Elastic, Piezoelectric, and Dielectric Characterization of Modified BiScO3-PbTiO3 Ceramics, IEEE T. Ultrason. Ferr., 52 (11) (2005) 2131-2139. 28. B. Kowalski, A. Sayir, A. Sehirlioglu, Aliovalent Mn Ti and GaTi substitution in hightemperature piezoelectric (x)Bi(Zn0.5Zr0.5)O3 - (y)BiScO3-(100 - x - y)PbTiO3, J. Mater. Sci. 51 (2016) 6761-6769. 29. B. L. Deng, Q. Wei, C. He, Z. J. Wang, X. M. Yang, X. F. Long, Effect of Pb(Mn1/3Sb2/3)O3 addition on the electrical properties of BiScO3-PbTiO3 piezoelectric ceramics, J. Alloy. Compd., 790 (2019) 397-404. 30. J.
Ryu ,
S.
Priya,
C.
Sakaki,
K.
Uchino,
High
power
piezoelectric
characteristics
of
BiScO3-PbTiO3-Pb(Mn1/3Nb2/3)O3, Jpn. J. Appl. Phys. 41 (2002) 6040-6044. 31. Z. Liu, B. Wu, and J. G. Wu, Reduced dielectric loss and high piezoelectric constant in Ce and Mn co-doped
ro of
BiScO3-PbCexTi1-xO3-Bi(Zn0.5Ti0.5)O3 ceramics, Ceram. Int., 44 (14) (2018) 16483-16488.
32. Z. H. Dai, J. L. Xie, W. G. Liu, S. B. Ge, M. X. Fang, D. B. Lin, L. X. Pang, H. F. Ji, S. Zhou, X. B. Ren, High piezoelectricity of BiScO3-PbTiO3 ceramics prepared by two step sintering, Mater. Lett., 241 (2019) 55-59.
33. X. Luo, J. T. Zeng, X. Shi, L. Y. Zheng, K. Y. Zhao, Z. Y. Man, G. R. Li, Dielectric, ferroelectric and
piezoelectric properties of MnO2-doped Pb(Yb1/2Nb1/2)O3-Pb(Zr,Ti)O3 ceramics, Ceram. Int., 44 (7) (2018)
-p
8456-8460.
34. J. G. Chen, Z. Q. Hu, H. D. Shi, M. Y. Li, S. X. Dong, High-power piezoelectric characteristics of manganese-modified BiScO3-PbTiO3 high-temperature piezoelectric ceramics, J. Phys. D Appl. Phys., 45 (46)
re
(2012) 465303.
35. J. G. Chen, G. X. Jin, C. M. Wang, J. R. Cheng, Reduced Dielectric Loss and Strain Hysteresis in Fe and Mn Comodified High-Temperature BiScO3-PbTiO3 Ceramics, J. Am. Ceram. Soc., 97 (12) (2014) 3890-3896.
lP
36. J. G. Wu, Y. Yu, X. T. Li, X. Y. Gao, and S. X. Dong, Investigation on Resonant Vibration Performances of Fe-Doped BiScO3-PbTiO3 Ceramics in High-Temperature Environment, J. Am. Ceram. Soc., 98 (10) (2015) 3145 3152.
37. T. L. Zhao, C. L. Fei, X. Y. Dai, J. J. Song, S. X. Dong, Structure and enhanced piezoelectric performance of
na
BiScO3-PbTiO3-Pb(Ni1/3Nb2/3)O3 ternary high temperature piezoelectric ceramics, J. Alloy. Compd., 806 (2019) 11-18.
38. G. Viola, T. Saunders, X. Wei, K. B. Chong, H. Luo, M. J. Reece, H. Yan, Contribution of piezoelectric effect,
ur
electrostriction and ferroelectric/ferroelastic switching to strain-electric field response of dielectrics, J. Adv. Dielec., 3 (1) (2013) 1350007.
39. Y. Tan, G. Viola, V. Koval, C. Yu, A. Mahajan, J. Zhang, H. Zhang, X. Zhou, N.V. Tarakina, H. Yan,On the
Jo
origin of grain size effects in Ba(Ti0.96Sn0.04)O3 perovskite ceramics, J. Eur. Ceram. Soc., 39 (6) (2019) 2064-2075. 40. N. N. Luo, Q. Li, Z. G. Xia, and X. C. Chu, Phase Diagram, Temperature Stability, and Electrical Properties of (0.85−x)Pb(Mg1/3Nb2/3)O3-0.10Pb(Fe1/2Nb1/2)O3-0.05PbZrO3-xPbTiO3 System, J. Am. Ceram. Soc., 95 (10) (2012) 3246-3253.
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