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Traditional transparent materials, including glasses and polymers, are chemically unstable and mechanically weak. Single crystals of some inorganic materials are also optically transparent, which are more stable than glasses and polymers. The fabrication of crystals, however, is relatively slow. Fortunately, transparent ceramics emerge as a promising candidate. Transparent ferroelectric ceramic is a kind of transparent ceramic with electro-optic effect, which also has excellent characteristics of conventional ceramics with excellent mechanical properties, resistance to high temperature, resistance against corrosion, and high hardness. Lead based transparent ferroelectric ceramic dominates this field for many years due to its superior electro-optic effect. Owing to the high toxicity of lead oxide, however, its development is significantly hampered. Therefore, it is greatly urgent to develop the lead-free transparent ferroelectric ceramics with excellent properties to replace the traditional lead based ceramics. In this paper, (K0.5Na0.5)0.94–3xLi0.06LaxNb0.95Ta0.05O3 (KNLTN-Lax; x = 0, 0.01, 0.015, 0.02) lead-free transparent ferroelectric materials are fabricated by the conventional solid state reaction method and ordinary sintering process. The dependence of microstructure, phase structure, optical transmittance and electrical properties of the ceramic on composition are systemically investigated. The transparent ferroelectric ceramic with relaxor-behavior is obtained at x = 0.02. The optical transmittance of the ceramic near infrared region is as high as 60%. Meanwhile, the electrical properties of the ceramic at x = 0.01 still maintains a relatively high level (d33 = 110 pC/N, kp = 0.267). In addition, the Curie temperature for each of all the samples is higher than 400 ℃. These results suggest that this material might be a novel and promising lead-free material that could be used in a large variety of electro-optical devices.
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Keywords:
- potassium sodium niobate /
- lead-free transparent ferroelectric ceramics /
- optical transmittance /
- electrical properties
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图 1 KNLTN-Lax陶瓷的XRD图谱
Figure 1. XRD patterns of KNLTN-Lax ceramics.
图 2 KNLTN-Lax陶瓷的SEM图
Figure 2. SEM images of KNLTN-Lax ceramics.
图 3 KNLTN-Lax陶瓷的密度和相对密度
Figure 3. Density and relative density of KNLTN-Lax ceramics.
图 4 KNLTN-Lax陶瓷的透过率
Figure 4. Optical transmittance of KNLTN-Lax ceramics.
图 5 KNLTN-Lax陶瓷的数码照片
Figure 5. Digital pictures of KNLTN-Lax ceramics.
图 6 室温下KNLTN-Lax陶瓷的电滞回线
Figure 6. P-E hysteresis loops of KNLTN-Lax ceramics in room temperature.
图 7 KNLTN-Lax陶瓷的介电常数在不同测试频率下随温度的变化
Figure 7. Temperature dependence of dielectric constant for KNLTN-Lax ceramics measured at different frequency.
图 8 10 kHz下KNLTN-Lax陶瓷的介电常数倒数与温度的关系
Figure 8. Inverse dielectric constant (1/εr) as a function of temperature at 10 kHz for KNLTN-Lax ceramics.
图 9 KNLTN-Lax陶瓷的log(1/ε–1/εm)与log(T–Tm)的关系
Figure 9. Plot of log(1/ε–1/εm) as a function of log(T–Tm) for KNLTN-Lax ceramics.
图 10 KNLTN-Lax陶瓷的压电常数、机电耦合系数随x的变化
Figure 10. The d33 and kp of KNLTN-Lax ceramics as a function of x.
表 1 KNLTN-Lax陶瓷的晶胞参数
Table 1. Lattice parameters of KNLTN-Lax ceramics.
KNLTN-Lax a/Å 标准差 b/Å 标准差 c/Å 标准差 x = 0 4.00134 0.00327 3.92609 0.00424 3.96078 0.02185 x = 0.01 3.96785 0.00707 3.96785 0.00707 3.89268 0.07532 x = 0.015 3.96225 0.00393 3.96225 0.00393 3.96067 0.04487 x = 0.02 3.96368 0.00229 3.96368 0.00229 4.01192 0.02727 
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表 2 KNLTN-Lax陶瓷在10 kHz下的Tcw, Tm, ΔTm和γ的数值
Table 2. The parameters Tcw, Tm, ΔTm and γ for the ceramics at 10 kHz.
x 0 0.01 0.015 0.02 Tcw 433 443 440 437 Tm 427 421 408 403 ΔTm 6 22 32 34 γ 1.424 1.624 1.714 1.918
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[1] 兰国政 2008 化学工程与装备 1 46
Google Scholar
Lan G Z 2008 Chem. Eng. Equip. 1 46
Google Scholar
[2] 许煜寰 1978 铁电与压电材料 (北京: 科学出版社) 第207页
Xu Y H 1978 Ferroelectric and Piezoelectric Materials (Beijing: Science Press) p207 (in Chinese)
[3] Xiao Z H, Yu S J, Li Y M, Ruan S C, Kong L B, Huang Q, Huang Z G, Zhou K, Su H B, Yao Z J, Que W X, Liu Y, Zhang T S, Wang J, Liu P, Shen D Y, Allix M, Zhang J, Tang D Y 2020 Mater. Sci. Eng., R. 139 100518
Google Scholar
[4] Zhu Q Q, Yang P F, Wang Z Y, Hu P C 2020 J. Eur. Ceram. Soc. 40 2426
Google Scholar
[5] Peng B, Shi Q W, Huang W X, Wang S S, Qi J Q, Lu T C 2018 Ceram. Int. 44 13674
Google Scholar
[6] Terakado N, Yoshimine T, Kozawa R, Takahashi Y, Fujiwara T 2020 RSC Adv. 10 22352
Google Scholar
[7] Haertling G H 1987 Ferroelectrics 75 25
Google Scholar
[8] Feng Z H, Lin L, Wang Z Z, Zheng Z Q 2017 Opt. Commun. 399 40
Google Scholar
[9] Chen Y J, Sun D Z, Zhu Y Y, Zeng X, Ling L, Qiu P S, He X Y 2020 Ceram. Int. 46 6738
Google Scholar
[10] Zeng X, Xu C X, Xu L 2019 J. Lumin. 213 61
Google Scholar
[11] Zhang H, Wang H, Gu H G, Zong X, Tu B T, Xu P Y, Wang B, Wang W M, Liu S Y, Fu Z Y 2018 J. Eur. Ceram. Soc. 38 4057
Google Scholar
[12] Wu X, Lu S B, Kwok K W 2017 J. Alloys Compd. 695 3573
Google Scholar
[13] Lin C, Wang H J, Ma J Z, Deng B Y, Wu X, Lin T F, Zheng X H, Yu X 2020 J. Alloys Compd. 826 154249
Google Scholar
[14] Yu S, Carloni D, Wu Y 2020 J. Am. Ceram. Soc. 103 4159
Google Scholar
[15] Zhang M, Yang H B, Li D, Lin Y 2020 J. Alloys Compd. 829 154565
Google Scholar
[16] Liu Y, Chu R Q, Xu Z J, Zhang Y J, Chen Q, Li G R 2011 Mater. Sci. Eng., B 176 1463
Google Scholar
[17] Yang D, Yang Z Y, Zhang X S, Wei L L, Chao X L, Yang Z P 2017 J. Alloys Compd. 716 21
Google Scholar
[18] 李艳艳 2010 硕士学位论文 (南昌: 南昌航空大学)
Li Y Y 2010 M.S. Thesis (Nanchang: Nanchang Hangkong University) (in Chinese)
[19] Jian L, Wayman C M 1995 Acta Mater. 43 3893
Google Scholar
[20] Guo Y P, Kakimoto K, Ohsato H 2004 Appl. Phys. Lett. 85 4121
Google Scholar
[21] Zhang P, Zhao Y G 2015 Mater. Lett. 161 620
Google Scholar
[22] 杨振宇 2016 硕士学位论文 (西安: 陕西师范大学)
Yang Z Y 2016 M.S. Thesis (Xi'an: Shaanxi Normal University) (in Chinese)
[23] 耿志明 2015 硕士学位论文 (常州: 常州大学)
Geng Z M 2015 M. S. Thesis (Changzhou: Changzhou University) (in Chinese)
[24] Thomas N W 1990 J. Phys. Chem. Solids 51 1419
Google Scholar
[25] 郝继功 2010 硕士学位论文 (聊城: 聊城大学)
Hao J G 2010 M.S. Thesis (Liaocheng: Liaocheng University) (in Chinese)
[26] 刘涛 2007 博士学位论文 (上海: 中国科学院上海硅酸盐研究所)
Liu T 2007 Ph. D. Dissertation (Shanghai: Shanghai Institute of Ceramics, Chinese Academy of Sciences) (in Chinese)
[27] Uchino K, Nomura S 1982 Ferroelectr. Lett. Sect. 44 55
Google Scholar
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