Large electrostrictive coefficients of BaTiO<sub>3</sub>-based lead-free ceramics

Chen Xiao-Ming; Li Guo-Rong

doi:10.7498/aps.71.20220451

Abstract

AbstractMicro-displacement actuators have important applications in aerospace, semiconductor, industry and other fields. Now most of the lead-based piezoelectric ceramics are used in the market. In consideration of environmental protection and legal restriction, it is urgent to develop lead-free ceramic materials with excellent electrostrictive properties. As a kind of ABO₃-type ferroelectrics, (Ba,Ca)(Ti,Zr)O₃ lead-free ceramics have attracted a lot of attention because of their high piezoelectricity. In this work, (Ba_0.85Ca_0.15)(Ti_0.9Zr_0.1)O₃ (BCTZ) ceramics with high electrostrictive coefficient are prepared by the solid-state method. The effects of sintering temperature on the structures and electrical properties of BCTZ ceramics are studied. The results show that the sintering temperature can help to improve density and grain growth of BCTZ ceramic.There are no impurity phases in the BCTZ ceramic systems, and all samples show ABO₃-type perovskite structures. At room temperature, the crystal structure of BCTZ ceramic forms coexistence of orthogonal (O)-tetragonal (T) phase. The dielectric peak of BCTZ ceramic is widened, and the Curie temperature reaches a maximum value of 110 ℃ when T_s = 1300 ℃. With the increase of sintering temperature, the dielectric peak of BCTZ ceramic gradually becomes narrowed, and the Curie temperature of ceramic moves toward low temperature.As the sintering temperature is 1300 ℃, the grain size of BCTZ ceramic is 1 μm, the large electrostrictive coefficient Q₃₃ (5.84 × 10^–2 m⁴/C²) can be obtained, which is about twice that of traditional PZT ceramic. This may be attributed to combination of the surface effect caused by grain size of BCTZ ceramic with the strong ionic nature of A-O chemical bond. In addition, although BCTZ ceramic has an O-T phase boundary near room temperature, the electrostrictive coefficient Q₃₃ of ceramic has good temperature stability in a range of 25–100 ℃. It shows that the crystal phase and temperature have no effect on the electrostrictive coefficient of BCTZ lead-free ceramic. It provides a new idea for designing the high electrostrictive properties of lead-free piezoelectric ceramics with potential applications.

Keywords:

Authors and contacts

1.
School of Materials and Energy Engineering, Guizhou Institute of Technology, Guiyang 550003, China
2.
Key Laboratory of Inorganic Functional Materials and Devices, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

Corresponding author: Chen Xiao-Ming, chen-xm123@163.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 52162015), the Natural Science Foundation of Guizhou Province, China (Grant No. [2020]1Y204), the Opening Project of Key Laboratory of Inorganic Functional Materials and Devices, Chinese Academy of Sciences (Grant No. KLIFMD202201), and the Fund of Guizhou Institute of Technology, China (Grant Nos. XJGC20190920, GZLGXM-21).

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References

[1]	Panda P K 2009 J. Mater. Sci. 44 5049 Google Scholar
[2]	Takenaka T, Nagata H 2005 J. Eur. Ceram. Soc. 25 2693 Google Scholar
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[19]	Li F, Jin L, Guo R 2014 Appl. Phys. Lett. 105 232903 Google Scholar
[20]	Jin L, Huo R, Guo R, Li F, Wang D, Tian Y, Hu Q, Wei X, He Z, Yan Y, Liu G 2016 ACS Appl. Mater. Interfaces 8 31109 Google Scholar
[21]	Xiao F, Ma W, Sun Q, Huan Z, Li J, Tang C 2013 J. Mater. Sci. - Mater. Electron. 24 2653 Google Scholar
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[23]	Okazaki K, Nagata K 1973 J. Am. Ceram. Soc. 56 82 Google Scholar
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[29]	Mastelaro V R, Favarim H R, Mesquita A, Michalowicz A, Moscovici J, Eiras J A 2015 Acta Mater. 84 164 Google Scholar
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图 1 (a) 烧结于不同温度下BCTZ陶瓷晶相结构; (b), (c) 相应烧结温度下BCTZ陶瓷在衍射角为44°—46°和65°—67°范围下的衍射峰

Figure 1. (a) X-ray diffraction patterns of the BCTZ ceramics sintered at different temperatures; (b), (c) the expanded XRD patterns of BCTZ ceramics sintered at different temperatures in the range of 44°–46° and 65°–67°

DownLoad: Full-Size Img PowerPoint

图 2 BCTZ陶瓷分别烧于(a) 1300 ℃, (b) 1350 ℃, (c) 1400 ℃, (d) 1450 ℃, (e) 1475 ℃, (f) 1500 ℃/ 2 h下的表面形貌

Figure 2. SEM images of BCTZ ceramics sintered at (a) 1300 ℃, (b) 1350 ℃, (c) 1400 ℃, (d) 1450 ℃, (e) 1475 ℃, (f) 1500 ℃ for 2 h.

DownLoad: Full-Size Img PowerPoint

图 3 在不同烧结温度下BCTZL陶瓷铁电性能

Figure 3. ferroelectric properties of BCTZL ceramics as a function of sintering temperature.

DownLoad: Full-Size Img PowerPoint

图 4 不同烧结温度下BCTZ陶瓷的介温曲线　(a) T_s = 1300 ℃; (b) T_s = 1350 ℃; (c) T_s = 1400 ℃; (d) T_s = 1450 ℃; (e) T_s = 1475 ℃; (f) T_s = 1500 ℃

Figure 4. Temperature dependence of dielectric properties for BCTZ ceramics: (a) T_s = 1300 ℃; (b) T_s = 1350 ℃; (c) T_s = 1400 ℃; (d) T_s = 1450 ℃; (e) T_s = 1475 ℃; (f) T_s = 1500 ℃.

DownLoad: Full-Size Img PowerPoint

图 5 不同烧结温度下BCTZ 陶瓷的双电致应变

Figure 5. Bipolar electric field-induced strain for BCTZ ceramics at different sintering temperatures.

DownLoad: Full-Size Img PowerPoint

图 6 不同烧结温度下BCTZ 陶瓷的S-P曲线:　(a) T_s = 1300 ℃; (b) T_s = 1350 ℃; (c) T_s = 1400 ℃; (d) T_s = 1450 ℃; (e) T_s = 1475 ℃; (f) T_s = 1500 ℃

Figure 6. Strain versus polarization curves for BCTZ ceramics sintered at different temperatures: (a) T_s = 1300 ℃; (b) T_s = 1350 ℃; (c) T_s = 1400 ℃; (d) T_s = 1450 ℃; (e) T_s = 1475 ℃; (f) T_s = 1500 ℃.

DownLoad: Full-Size Img PowerPoint

图 7 不同测量温度下BCTZ 陶瓷的S-P曲线　(a) T_s = 1300 ℃; (b) T_s = 1475 ℃

Figure 7. Strain versus polarization curves for BCTZ ceramics measured at different temperatures: (a) T_s = 1300 ℃; (b) T_s = 1475 ℃.

DownLoad: Full-Size Img PowerPoint

图 8 一些陶瓷体系的Q₃₃与$\displaystyle\sum q^2/{\bar{z}}_{33}^{*2}$的联系

Figure 8. Q₃₃ of ceramics as functions of $\displaystyle\sum q^2/{\bar{z}}_{33}^{*2}$.

DownLoad: Full-Size Img PowerPoint

表 1 不同烧结温度下BCTZ 陶瓷电致伸缩系数Q₃₃

Table 1. Q₃₃ as a function of sintering temperature for BCTZ ceramics.

T_s/℃ Q₃₃/
(10^–2 m⁴·C^–2) R-square ε_r Average grain size/μm

1300 5.84 0.9772 1621 1
1350 3.51 0.9728 2870 2
1400 4.09 0.98768 2836 6
1450 4.27 0.98677 2781 12
1475 4.34 0.98067 2904 —
1500 4.47 0.98348 2776 14

DownLoad: CSV

表 2 不同测量温度下BCTZ 陶瓷电致伸缩系数Q₃₃ (T_s = 1300 ℃; 1475 ℃)

Table 2. Q₃₃ as a function of temperature for BCTZ ceramics (T_s = 1300 ℃; 1475 ℃).

T/℃ T_s = 1300 ℃
Q₃₃/(10^–2 m⁴·C^–2) T_s = 1475 ℃
Q₃₃/(10^–2 m⁴·C^–2)

25 5.84 4.34
50 6.39 4.62
70 6.61 4.78
85 6.76 4.68
100 6.83 4.29

DownLoad: CSV

map

[1]	Panda P K 2009 J. Mater. Sci. 44 5049 Google Scholar
[2]	Takenaka T, Nagata H 2005 J. Eur. Ceram. Soc. 25 2693 Google Scholar
[3]	Wada S, Nitta M, Kumada N, Tanaka D, Furukawa M, Ohno S, Moriyoshi C, Kuroiwa Y 2008 Jpn. J. Appl. Phys. 47 7678 Google Scholar
[4]	Huang Y, Zhao C, Wu B, Wu J 2020 ACS Appl. Mater. Interfaces 12 23885 Google Scholar
[5]	Habib M, Lqbal M J, Lee M H, Kim D, Akram F, Gul M, Zeb A, Rehman I U, Kim M H, Song T K 2022 Mater. Res. Bull. 146 111571 Google Scholar
[6]	Liu Z G, Tang Z H, Hu S C, Yao D J, Sun F, Chen D Y, Guo X B, Liu Q X, Jiang Y P, Tang X G 2020 J. Mater. Chem. C 8 13405 Google Scholar
[7]	Jaita P, Jarupoom P 2021 J. Asian Ceram. Societies 9 975 Google Scholar
[8]	Duraisamy D, Venkatesan G N 2020 Sens. Actuators, A 315 112307 Google Scholar
[9]	Wu W J, Ma J, Wang N N, Shi C Y, Chen K, Zhu Y L, Chen M, Wu B 2020 J. Alloys Compd. 814 152240 Google Scholar
[10]	Ni H M, Luo L H, Li W P, Zhu Y J, Luo H S 2011 J. Alloys Compd. 509 3958 Google Scholar
[11]	Cao W P, Sheng J, Liu Z, Gao C, Wang Z H, Wang J, Chang J, Wang Z, Li W L 2020 Mod. Phys. Lett. B 34 2050100 Google Scholar
[12]	Varade P, Pandey A H, Gupta S M, Venkataramani N, Kulkarni A R 2020 Appl. Phys. Lett. 117 212901 Google Scholar
[13]	Chen K, Ma J, Wu J, Wang X Y, Miao F, Huang Y, Shi C Y, Wu W J, Wu B 2020 J. Mater. Sci.-Mater. Electron. 31 12292 Google Scholar
[14]	Tsai C C, Liao W H, Chu S Y, Hong C S, Yu M C, Wei Z Y, Lin Y Y 2021 Ceram. Int. 47 7207 Google Scholar
[15]	Wang P, Li Y X, Lu Y Q 2011 J. Eur. Ceram. Soc. 31 2005 Google Scholar
[16]	Liu W, Ren X 2009 Phys. Rev. Lett. 103 257602 Google Scholar
[17]	Chen X, Zeng J, Kim D, Zheng L, Lou Q, Hong Park C, Li G 2019 Mater. Chem. Phys. 231 173 Google Scholar
[18]	Dai Z H, Xie J L, Chen Z B, Zhou S, Liu J J, Liu W G, Xi Z Z, Ren X B 2021 Chem. Eng. J. 410 128341 Google Scholar
[19]	Li F, Jin L, Guo R 2014 Appl. Phys. Lett. 105 232903 Google Scholar
[20]	Jin L, Huo R, Guo R, Li F, Wang D, Tian Y, Hu Q, Wei X, He Z, Yan Y, Liu G 2016 ACS Appl. Mater. Interfaces 8 31109 Google Scholar
[21]	Xiao F, Ma W, Sun Q, Huan Z, Li J, Tang C 2013 J. Mater. Sci. - Mater. Electron. 24 2653 Google Scholar
[22]	Chen X, Ruan X, Zhao K, He X, Zeng J, Li Y, Zheng L, Park C H, Li G 2015 J. Alloys Compd. 632 103 Google Scholar
[23]	Okazaki K, Nagata K 1973 J. Am. Ceram. Soc. 56 82 Google Scholar
[24]	陈小明, 王明焱, 唐木智明, 李国荣 2021 70 197701 Google Scholar Chen X M, Wang M Y, Karaki T, Li G R 2021 Acta Phys. Sin. 70 197701 Google Scholar
[25]	Yu Z, Ang C, Guo R, Bhalla A S 2007 Mater. Lett. 61 326 Google Scholar
[26]	Yu Z, Ang C, Guo R, Bhalla A S 2002 J. Appl. Phys. 92 2655 Google Scholar
[27]	Sciau P, Calvarin G, Ravez J 1999 Solid State Commun. 113 77 Google Scholar
[28]	Tang X G, Wang J, Wang X X, Chan H L W 2004 Solid State Commun. 131 163 Google Scholar
[29]	Mastelaro V R, Favarim H R, Mesquita A, Michalowicz A, Moscovici J, Eiras J A 2015 Acta Mater. 84 164 Google Scholar
[30]	Känzig W 1955 Phys. Rev. 98 549 Google Scholar
[31]	Cross L E 1996 Mater. Chem. Phys. 43 108 Google Scholar
[32]	Zhang S T, Kounga A B, Aulbach E, Ehrenberg H, Rödel J 2007 Appl. Phys. Lett. 91 112906 Google Scholar
[33]	Guo Y, Gu M, Luo H, Liu Y, Withers R L 2011 Phys. Rev. B 83 054118 Google Scholar
[34]	Yan K, Ren X 2014 J. Phys. D:Appl. Phys. 47 015309 Google Scholar
[35]	Li F, Jin L, Xu Z, Zhang S 2014 Appl. Phys. Rev. 1 011103 Google Scholar
[36]	Zuo R Z, Qi H, Fu J, Li J F, Shi M, Xu Y D 2016 Appl. Phys. Lett. 108 232904 Google Scholar
[37]	Haertling G H 1987 Ferroelectrics 75 25 Google Scholar
[38]	Weaver P M, Cain M G, Stewart M 2010 Appl. Phys. Lett. 96 142905 Google Scholar
[39]	Zhang S T, Kounga A B, Jo W, Jamin C, Seifert K, Granzow T, Rödel J, Damjanovic D 2009 Adv. Mater. 21 4716 Google Scholar
[40]	Bobnar V, Malič B, Holc J, Kosec M, Steinhausen R, Beige H 2005 J. Appl. Phys. 98 024113 Google Scholar
[41]	Li F, Jin L, Guo R P 2014 Appl. Phys. Lett. 105 232903
[42]	Zuo R, Qi H, Fu J, Li J, Shi M, Xu Y 2016 Appl. Phys. Lett. 108 232904
[43]	Ghosez P, Gonze X, Lambin P, Michenaud J P 1995 Phys. Rev. B 51 6765 Google Scholar
[44]	Ghosez P, Michenaud J P, Gonze X 1998 Phys. Rev. B 58 6224 Google Scholar
[45]	Haertling G H, Land C E 1971 J. Am. Ceram. Soc. 54 1 Google Scholar

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Large electrostrictive coefficients of BaTiO₃-based lead-free ceramics

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Corresponding author: Chen Xiao-Ming, chen-xm123@163.com

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T_s/℃	Q₃₃/ (10^–2 m⁴·C^–2)	R-square	ε_r	Average grain size/μm
1300	5.84	0.9772	1621	1
1350	3.51	0.9728	2870	2
1400	4.09	0.98768	2836	6
1450	4.27	0.98677	2781	12
1475	4.34	0.98067	2904	—
1500	4.47	0.98348	2776	14

T/℃	T_s = 1300 ℃ Q₃₃/(10^–2 m⁴·C^–2)	T_s = 1475 ℃ Q₃₃/(10^–2 m⁴·C^–2)
25	5.84	4.34
50	6.39	4.62
70	6.61	4.78
85	6.76	4.68
100	6.83	4.29

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Article

留言板

Large electrostrictive coefficients of BaTiO3-based lead-free ceramics

Abstract

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Corresponding author: Chen Xiao-Ming, chen-xm123@163.com

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Large electrostrictive coefficients of BaTiO₃-based lead-free ceramics