<i>B</i>位空位补偿型钐掺杂PZT(54/46)陶瓷中的缺陷分析及其对压电性能的影响

杨静; 冯少蓉; 张涛; 牛旭平; 王荣; 李敏; 于润升; 曹兴忠; 王宝义

doi:10.7498/aps.73.20231872

摘要

用固相反应法制备了B位空位补偿型钐掺杂非准同型相界组分PZT(54/46)陶瓷. 通过正电子湮没寿命谱(PALS)和符合多普勒展宽能谱(CDBS)对陶瓷中的缺陷结构进行综合表征, 结合常规表征手段如X射线衍射(XRD), 电子扫描显微镜(SEM), 介电、铁电和压电性能测量, 研究缺陷对陶瓷压电性能的影响. XRD结果显示所有陶瓷均为纯钙钛矿相, 掺杂诱导了菱方-四方(R-T)相变, 准同型相界位于Sm掺杂量x = 0.01$- $0.02. 电学测量结果反映: 介电、铁电和压电性能均先增强后减弱, MPB附近两个样品都有优异的介电和铁电性能, 但其压电性能差别很大. x = 0.01给出最优压电性能d₃₃ = 572 pC/N, 较未掺杂样品增强了一倍. PALS结果表明掺杂使陶瓷中缺陷类型发生变化, x ≤ 0.01, 样品中同时含有A位空位与B位空位; x ≥ 0.02, 样品中以A位相关缺陷为主, B位空位浓度很低. CDBS结果进一步证实x = 0.01和0.02中B位空位浓度分别是该体系中最高和最低的. 由以上结果推断出: x = 0.01获得的最优压电性能与其中较高浓度的B位空位有关, B位空位可稀释A位空位浓度, 降低氧空位浓度, 从而降低A位空位与氧空位形成缺陷偶极子的几率, 促进畴壁运动, 使压电性能增强.

关键词:

Abstract

Rare earth dopping, especially samarium (Sm) dopping is considered as an effective way to obtain high piezoelectricity by increasing local structure heterogeneity in Pb-containing ABO₃ perovskite ceramics. Defects play an significant role in determining piezoelectric properties in aliovalent ion doping systems. In order to obtain an insight into the effect of defects, especially B-site vacancies on piezoelectricity, Sm-doped PZT(54/46) ceramics compensated by B-site vacancies are fabricated by conventional solid state reaction method. The influence of defects on piezoelectric properties is studied by positron annihilation lifetime spectroscopy (PALS), coincidence Doppler broadening spectroscopy (CDBS), and conventional methods such as X-ray diffraction (XRD), scanning electron microscope (SEM), electrical performance testing on dielectricity, ferroelectricity and pizoelectricity. The XRD results show that all ceramics crystallize in a pure perovskite phase, Sm³⁺ doping causes a transformation from the rhombohedral to tetragonal phase and the morphotropic phase boundary (MPB) lies near Sm³⁺ doping content x = 0.01–0.02. Electrical performance testing results indicate that with the increase of x, all of the dielectricity, ferroelectricity and pizoelectricity first increase and then decrease, the sample with x = 0.01 and 0.02 exhibit similar excellent dielectricity and ferroelectricity, while their pizoelectricity differs greatly, the optimal piezoelectric coefficient d₃₃ = 572 pC/N (nearly double that of undoped sample) is obtained in the sample with x = 0.01. The PALS results show that Sm doping leads the defect types to change from the coexistence of A-site and B-site vacancies for x ≤ 0.01 to mainly A-site related defects for x ≥ 0.02. The CDBS results further verify that the concentration of B-site vacancies is highest for x = 0.01 and lowest for x = 0.02. It is inferred that the high pizoelectricity for x = 0.01 is related to its high concentration of B-site vacancies, which can dilute the number of A-site vacancies and oxygen vacancies, reducing the chance of forming defect dipoles between an A-site vacancy and an oxygen vacancy, facilitating domain wall motion, and enhancing piezoelectricity. This study indicates that B-site vacancies can enhance piezoelectricity to some extent, which will provide some guidance for defect engineering.

Keywords:

作者及机构信息

1.
西安科技大学理学院, 西安　710600

2.
西安科技大学材料科学与工程学院, 西安　710600

3.
中国科学院高能物理研究所, 北京　100049

通信作者: 杨静, yangjing10@xust.edu.cn ; 张涛, tzhang@xust.edu.cn ;

基金项目: 国家自然科学基金(批准号: 12075189, 11605133, 12004300, 11974275)、中国博士后科学基金(批准号: 2018M643813XB)和陕西省联合基金重点项目(批准号: 2021JML-05)资助的课题.

Authors and contacts

1.
College of Science, Xi’an University of Science and Technology, Xi’an 710600, China

2.
College of Materials Science and Engineering, Xi’an University of Science and Technology, Xi’an 710600, China

3.
Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Yang Jing, yangjing10@xust.edu.cn ; Zhang Tao, tzhang@xust.edu.cn ;

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 12075189, 11605133, 12004300, 11974275), the China Postdoctoral Science Foundation (Grant No. 2018M643813XB), and the Key Joint Funds of Shaanxi Province, China (Grant No. 2021JML-05).

文章全文

参考文献

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施引文献

图 1 xSm-PZT(54/46)陶瓷的XRD结果　(a) 20°—70°全谱图; (b) 42°—46°的慢扫谱图

Fig. 1. XRD patterns of xSm-PZT(54/46) ceramics: (a) 2θ = 20°—70°; (b) selected region of 2θ = 42°—46°.

下载: 全尺寸图片幻灯片

图 2 0.02 Sm-PZT(54/46)陶瓷的SEM图像

Fig. 2. SEM images of 0.02 Sm-PZT (54/46) ceramics.

下载: 全尺寸图片幻灯片

图 3 xSm-PZT(54/46)的介电频谱　(a) 介电常数; (b) 介电损耗

Fig. 3. Dielectric spectrum of xSm-PZT(54/46): (a) Permittivity; (b) loss tangent.

下载: 全尺寸图片幻灯片

图 4 xSm-PZT(54/46)陶瓷的铁电性能　(a) P-E电滞回线; (b) J-E曲线

Fig. 4. Ferroelectric properties of xSm-PZT(54/46): (a) P-E hysteresis loops; (b) J-E curves.

下载: 全尺寸图片幻灯片

图 5 xSm-PZT(54/46)陶瓷的压电性能

Fig. 5. Piezoelectric properties of the xSm-PZT(54/46) ceramics.

下载: 全尺寸图片幻灯片

图 6 xSm-PZT(54/46)陶瓷的CBDS商谱结果(以未掺杂PZT为参比)　(a) 全谱图; (b) O 2p峰放大图

Fig. 6. CDBS ratio curves of xSm-PZT(54/46) ceramics, using undoped PZT as the reference: (a) Full curves; (b) enlarged O 2p peak curves.

下载: 全尺寸图片幻灯片

表 1 xSm-PZT(54/46)陶瓷的铁电性能指标

Table 1. Ferroelectric parameters of xSm-PZT(54/46) ceramics

样品	矫顽场E_c/(kV·cm^–1)	最大极化值P_m/(µC·cm^–2)	剩余极化2P_r/(µC·cm^–2)
0.000 Sm-PZT(54/46)	6.50543	22.9362	17.8235
0.005 Sm-PZT(54/46)	9.07716	28.9513	41.7151
0.010 Sm-PZT(54/46)	11.96854	29.7117	43.8174
0.020 Sm-PZT(54/46)	16.22384	30.0491	45.7736
0.030 Sm-PZT(54/46)	19.54932	26.0871	40.9861
0.040 Sm-PZT(54/46)	12.44085	21.0489	28.7527

下载: 导出CSV

表 2 xSm-PZT(54/46)陶瓷PALS解谱结果(τ₁固定为160 ps)

Table 2. Decomposed PALS results of xSm-PZT(54/46) ceramics (with τ₁ fixed to 160 ps).

Sample	τ₁/ps	I₁/%	τ₂/ps	I₂/%	τ₃/ps	I₃/%	Fit’s variance
0.000 Sm-PZT(54/46)	160	41.01 ± 0.24	272.5 ± 1.1	58.02 ± 0.24	1386 ± 58	0.97 ± 0.05	1.0526
0.005 Sm-PZT(54/46)	160	33.69 ± 0.64	275.9 ± 1.4	65.37 ± 0.64	1531 ± 33	0.94 ± 0.03	1.0155
0.010 Sm-PZT(54/46)	160	31.61 ± 0.20	276.3 ± 0.4	67.45 ± 0.20	1477 ± 34	0.94 ± 0.02	0.9946
0.020 Sm-PZT(54/46)	160	23.01 ± 0.65	293.0 ± 1.5	75.97 ± 0.65	1531 ± 39	1.01 ± 0.04	1.0727
0.030 Sm-PZT(54/46)	160	24.25 ± 0.53	289.9 ± 1.2	74.87 ± 0.53	1457 ± 81	0.88 ± 0.06	0.9906
0.040 Sm-PZT(54/46)	160	31.33 ± 0.42	286.3 ± 1.3	67.57 ± 0.42	1402 ± 34	1.09 ± 0.04	1.0466

下载: 导出CSV

表 3 xSm-PZT(54/46)陶瓷归一化PALS解谱结果

Table 3. Normalized parameters of decomposed PALS results of xSm-PZT(54/46) ceramics.

Sample	τ₁/ps	I₁/%	τ₂/ps	I₂/%	Fit’s variance
0.000 Sm-PZT(54/46)	160	41.41 ± 0.24	272.5 ± 1.1	58.59 ± 0.24	1.047
0.005 Sm-PZT(54/46)	160	34.01 ± 0.64	275.9 ± 1.4	65.99 ± 0.64	1.0155
0.010 Sm-PZT(54/46)	160	31.91 ± 0.20	276.3 ± 0.4	68.09 ± 0.20	0.9954
0.020 Sm-PZT(54/46)	160	23.25 ± 0.65	293.0 ± 1.5	76.75 ± 0.65	1.0683
0.030 Sm-PZT(54/46)	160	24.47 ± 0.53	289.9 ± 1.2	75.53 ± 0.53	0.9928
0.040 Sm-PZT(54/46)	160	31.68 ± 0.42	286.3 ± 1.3	68.32 ± 0.42	1.0511

下载: 导出CSV

[1]	Jaffe B, Roth R S, Marzullo S 1954 J. Appl. Phys. 25 809 Google Scholar
[2]	Yan Y, Li Z, Jin L, Du H, Zhang M, Zhang D, Hao Y 2021 ACS Appl. Mater. Interfaces 13 38517 Google Scholar
[3]	Li F, Lin D, Chen Z, Cheng Z, Wang J, Li C, Xu Z, Huang Q, Liao X, Chen L, Shrout T R, Zhang S 2018 Nat. Mater. 17 349 Google Scholar
[4]	Fang Z, Tian X, Zheng F, Jiang X, Ye W, Qin Y, Wang X, Zhang Y 2022 Ceram. Int. 48 7550 Google Scholar
[5]	Guo Q, Li F, Xia F, Gao X, Wang P, Hao H, Sun H, Liu H, Zhang S 2019 ACS Appl. Mater. Interfaces 11 43359 Google Scholar
[6]	Seshadri S B, Nolan M M, Tutuncu G, Forrester J S, Sapper E, Esteves G, Granzow T, Thomas P A, Nino J C, Rojac T, Jones J L 2018 Sci. Rep. 8 4120 Google Scholar
[7]	Gao B, Yao Z, Lai D, Guo Q, Pan W, Hao H, Cao M, Liu H 2020 J. Alloys Compd. 836 155474 Google Scholar
[8]	Yan P, Qin Y, Xu Z, Han F, Wang Y, Wen Z, Zhang Y, Zhang S 2021 ACS Appl. Mater. Interfaces 13 54210 Google Scholar
[9]	Guo Q, Hou L, Li F, Xia F, Wang P, Hao H, Sun H, Liu H, Zhang S 2019 J. Am. Ceram. Soc. 102 7428 Google Scholar
[10]	Qin Y, Yan P, Han F, Zhang Y, Lü Z, Zhou C 2022 J. Alloys Compd. 891 161959 Google Scholar
[11]	Li C, Xu B, Lin D, Zhang S, Bellaiche L, Shrout T R, Li F 2020 Phys. Rev. B 101 140102 Google Scholar
[12]	Peng G, Zheng D, Cheng C, Zhang J, Zhang H 2017 J Alloys Compd. 693 1250 Google Scholar
[13]	Cheng C, Zheng D Y, Peng G G, Hu S M, Zhang H, Zhang J 2016 J. Mater. Sci. 28 1624 Google Scholar
[14]	Kim T Y, Jang H M 2000 Appl. Phys. Lett. 77 3824 Google Scholar
[15]	Garcia-Zaldivar O, Pelaiz-Barranco A, Guerra J D S, Mendoza M E, Calderon-Pinar F, Hall D A 2011 Physica B 406 1622 Google Scholar
[16]	Pandey A H, Gupta S M 2020 Mater. Sci. Eng., B 253 114495 Google Scholar
[17]	Damjanovic D 2005 J. Am. Ceram. Soc. 88 2663 Google Scholar
[18]	Li Z, Thong H C, Zhang Y F, Xu Z, Zhou Z, Liu Y X, Cheng Y Y S, Wang S H, Zhao C, Chen F, Bi K, Han B, Wang K 2021 Adv. Funct. Mater. 31 2005012 Google Scholar
[19]	Keeble D J, Singh S, Mackie R A, Morozov M, McGuire S, Damjanovic D 2007 Phys. Rev. B 76 144109 Google Scholar
[20]	Asoka-Kumar P, Alatalo M, Ghosh V J, Kruseman A C, Nielsen B, Lynn K G 1996 Phys. Rev. Lett. 77 2097 Google Scholar
[21]	熊涛, 高传波, 陈祥磊, 周先意, 翁惠民, 曹方宇, 叶邦角, 韩荣典, 杜淮江 2009 物理学报 58 6946 Google Scholar Xiong T, Gao C B, Chen X L, Zhou X Y, Weng H M, Cao F Y, Ye B J, Han R D, Du H J 2009 Acta Phys. Sin. 58 6946 Google Scholar
[22]	Qin M, Gao F, Cizek J, Yang S, Fan X, Zhao L, Xu J, Dong G, Reece M, Yan H 2019 Acta Mater. 164 76 Google Scholar
[23]	Chakrabarti M, Bhowmick D, Sarkar A, Chattopadhyay S, Dechoudhury S, Sanyal D, Chakrabarti A 2005 J. Mater. Sci. 40 5265 Google Scholar
[24]	Čížek J, Melikhova O, Procházka I, Kuriplach J, Kužel R, Brauer G, Anwand W, Konstantinova T E, Danilenko I A 2010 Phys. Rev. B 81 024116 Google Scholar
[25]	Li K, Sun E, Zhang Y, Song Z, Qi X, Sun Y, Li J, Yang B, Liu J, Cao W 2021 J. Mater. Chem. C 9 2426 Google Scholar
[26]	Bellaiche L, Íñiguez J, Cockayne E, Burton B P 2007 Phys. Rev. B 75 014111 Google Scholar
[27]	Zhu W, Fujii I, Ren W, Trolier-McKinstry S 2012 J. Am. Ceram. Soc. 95 2906 Google Scholar

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B位空位补偿型钐掺杂PZT(54/46)陶瓷中的缺陷分析及其对压电性能的影响

Analysis of defects in B-vacancy compensated Sm-doped PZT(54/46) ceramics and their influences on piezoelectric properties

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1.
西安科技大学理学院, 西安　710600

2.
西安科技大学材料科学与工程学院, 西安　710600

3.
中国科学院高能物理研究所, 北京　100049

通信作者: 杨静, yangjing10@xust.edu.cn ; 张涛, tzhang@xust.edu.cn ;

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1.
College of Science, Xi’an University of Science and Technology, Xi’an 710600, China

2.
College of Materials Science and Engineering, Xi’an University of Science and Technology, Xi’an 710600, China

3.
Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Yang Jing, yangjing10@xust.edu.cn ; Zhang Tao, tzhang@xust.edu.cn ;

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B位空位补偿型钐掺杂PZT(54/46)陶瓷中的缺陷分析及其对压电性能的影响

Analysis of defects in B-vacancy compensated Sm-doped PZT(54/46) ceramics and their influences on piezoelectric properties

摘要

Abstract

作者及机构信息

1. 西安科技大学理学院, 西安 710600 2. 西安科技大学材料科学与工程学院, 西安 710600 3. 中国科学院高能物理研究所, 北京 100049

通信作者: 杨静, yangjing10@xust.edu.cn ; 张涛, tzhang@xust.edu.cn ;

Authors and contacts

1. College of Science, Xi’an University of Science and Technology, Xi’an 710600, China 2. College of Materials Science and Engineering, Xi’an University of Science and Technology, Xi’an 710600, China 3. Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Yang Jing, yangjing10@xust.edu.cn ; Zhang Tao, tzhang@xust.edu.cn ;

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1.
西安科技大学理学院, 西安　710600

2.
西安科技大学材料科学与工程学院, 西安　710600

3.
中国科学院高能物理研究所, 北京　100049

1.
College of Science, Xi’an University of Science and Technology, Xi’an 710600, China

2.
College of Materials Science and Engineering, Xi’an University of Science and Technology, Xi’an 710600, China

3.
Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China