(1–x)K0.5Na0.5NbO3-xBi(Mg0.5Ti0.5)O3无铅弛豫铁电陶瓷的介电、铁电和高储能行为

杜金花; 李雍; 孙宁宁; 赵烨; 郝喜红

doi:10.7498/aps.69.20200213

摘要

利用传统固相法制备了(1–x)K_0.5Na_0.5NbO₃-xBi(Mg_0.5Ti_0.5)O₃ (简写: (1–x)KNN-xBMT, x = 0.05, 0.10, 0.15, 0.20)无铅弛豫铁电陶瓷, 并对其相结构、微观形貌、介电特性与储能行为进行了系统的研究. 研究结果表明, 随着BMT含量的增加, (1–x)KNN-xBMT陶瓷由正常铁电体逐渐转变为弛豫铁电体, 表现出强烈的弥散相变特征, 其最大极化强度P_max随之逐渐降低. 当x = 0.15时, 陶瓷具有最大的击穿电场, 为275 kV·cm^–1. 采用间接方式对(1–x)KNN-xBMT陶瓷的储能性能进行计算, 发现当BMT的含量为x = 0.15时, 可获得最佳的储能性能: 当场强为275 kV·cm^–1时, 可释放储能密度W_rec为2.25 J·cm^–3, 储能效率η高达84%. 鉴于实际应用的需求, 对各组分陶瓷进行直接测试, 结果表明随掺杂量的增加, 储能密度W_dis呈现先增大后减小的变化趋势, 当x = 0.15时, 储能密度为1.54 J·cm^–3, 放电时间仅为88 ns. 另外, 该材料在1—50 Hz范围内具有良好的频率稳定性, 在25—125 ℃范围内具有良好的温度稳定性, 储能密度的变化量低于8%. 该研究表明KNN-BMT陶瓷在环境友好高储能密度电容器领域具有广阔的应用前景.

关键词:

Abstract

Lead-free dielectric ceramics with high energy-storage density and efficiency are ideal energy materials for sustainable development of the enery resource. In this paper, (1–x)K_0.5Na_0.5NbO₃–xBi(Mg_0.5Ti_0.5)O₃ ((1–x)KNN-xBMT, x = 0.05, 0.10, 0.15, 0.20) lead-free relaxor ferroelectric ceramics are prepared by the traditional solid-state method. The effects of BMT on the phase structure, microstructure, dielectric properties and energy storage behavior of KNN based ceramics are studied. With the increase of BMT content, the crystal structures of (1–x)KNN-xBMT ceramics gradually change from orthorhombic to pseudo-cubic phase, and transform into cubic phase finally. The addition of BMT can suppress grain growth of the ceramics, resulting in the average grain size decreasing from 850 to 195 nm when x increases from 0.05 to 0.20. Dielectric properties exhibit that the Curie temperature decreases with BMT content increasing, and dielectric peak at Curie temperature is broadened due to the addition of BMT. In addition, ferroelectric properties demonstrate that the addition of BMT reduces the remnant polarization (P_r) and coercive field (E_c) of the ceramics. The results indicate that (1–x)KNN-xBMT ceramics transform from ferroelectric to relaxor ferroelectric phase. Based on the calculation of hysteresis loop, the best energy storage performance is obtained at x = 0.15, of which the recoverable energy storage density (W_rec) and the energy storage efficiency (η) are 2.25 J·cm^–3 and 84% at its dielectric breakdown strength of 275 kV·cm^–1. Meanwhile, the ceramic with x = 0.15 exhibits good stability in a frequency range of 1–50 Hz, with an energy density variation of less than 5%, and temperature stability in a range of 25–125 ℃ with change of less than 8%. Moreover, based on direct measurement, the energy storage density (W_dis) of the ceramic with x = 0.15 is 1.54 J·cm^–3, and the discharge time is only 88 ns. The research shows that (1–x)KNN-xBMT ceramics have a wide application prospect in the field of environmentally friendly capacitors with high energy storage density.

Keywords:

作者及机构信息

1.
内蒙古科技大学, 内蒙古自治区铁电新能源材料与器件重点实验室, 包头　014010

2.
内蒙古科技大学工业技术研究院, 包头　014010

3.
内蒙古科技大学化学与化工学院, 包头　014010

通信作者: 郝喜红, xhhao@imust.cn

基金项目: 国家级-国家自然科学基金(51702169)

Authors and contacts

1.
Inner Mongolia Key Laboratory of Ferroelectric-related New Energy Materials and Devices, Inner Mongolia University of Science and Technology, Baotou 014010, China

2.
Industrial Technology Research Institute, Inner Mongolia University of Science and Technology, Baotou 014010, China

3.
School of Chemistry and Chemical Engineering, Inner Mongolia University of Science and Technology, Baotou 014010, China

Corresponding author: Hao Xi-Hong, xhhao@imust.cn

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 通过组分掺杂减小晶粒尺寸获得铌酸钾钠陶瓷高储能密度的示意图

Fig. 1. Schematic diagram showing the increase of W_rec through decreasing the grain size by doping BMT in KNN ceramics.

下载: 全尺寸图片幻灯片

图 2 直接测试系统的电路示意图

Fig. 2. Circuit diagram of direct test system.

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图 3 (1–x)KNN-xBMT 陶瓷的XRD图

Fig. 3. XRD patterns of (1–x)KNN-xBMT ceramics.

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图 4 (1–x)KNN-xBMT 陶瓷的表面形貌SEM图, 插图为含有平均粒径的粒径分布图　(a) x = 0.05; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20

Fig. 4. SEM images of the (1–x)KNN-xBMT ceramics with their grain size distribution and average grain size inserted: (a) x = 0.05; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20.

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图 5 (a) (1 – x)KNN-xBMT陶瓷在–150 ℃至300 ℃以及KNN陶瓷在25 ℃至500 ℃的介电常数随温度的变化; (b) ln(1/ε_r–1/ε_m) 随ln(T–T_m)的变化

Fig. 5. (a) Dielectric constant as a function of temperature in a temperature range of –150 ℃ to 300 ℃ for (1 – x)KNN-xBMT ceramics and 25 ℃ to 500 ℃ for pure KNN ceramics; (b) plots of ln(1/ε_r–1/ε_m) versus ln(T–T_m) of the (1–x)KNN-xBMT ceramics.

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图 6 (1–x)KNN-xBMT 陶瓷在60 kV·cm^–1电场下P-E曲线和电流回线(I-E)　(a) x = 0; (b) x = 0.05; (c) x = 0.10; (d) x = 0.15; (e) x = 0.20

Fig. 6. P-E loop and I-E curves under 60 kV·cm^–1 electric field of the (1–x)KNN-xBMT ceramics: (a) x = 0; (b) x = 0.05; (c) x = 0.10; (d) x = 0.15; (e) x = 0.20.

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图 7 (1–x)KNN-xBMT陶瓷在击穿电场下的(a) P-E图以及(b)储能密度和储能效率; (1–x)KNN-xBMT陶瓷在185 kV·cm^-1电场下的(c) P-E图以及(d)储能密度和储能效率

Fig. 7. (a) P-E loops, (b) W_rec and η of (1–x)KNN-xBMT ceramics at the maximum applied electric fields; (c) P-E loops, (d) W_rec and η of (1–x)KNN-xBMT ceramics under 200 kV·cm^–1 electric fields.

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图 8 0.85KNN-0.15BMT陶瓷在不同电场下的(a) P-E图以及(b)储能密度和储能效率; 在不同频率下的(c) P-E图和(d)储能密度和储能效率; 在不同温度下的(e) P-E图和(f)储能密度和储能效率

Fig. 8. (a) P-E loops and (b) W_rec and η under different electric fields, (c) P-E loops and (d) W_rec and η at different frequencies, (e) P-E loops and (f) W_rec and η at different temperatures of 0.85KNN-0.15BMT ceramics.

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图 9 (1–x)KNN-xBMT陶瓷在最大击穿电场下直接测试的(a)放电电流随时间的变化, (b)放电储能密度和放电速率t₉₀以及(c) W_dis和W_rec比较图; 0.85KNN-0.15BMT陶瓷在不同电场下直接测试的(d)放电电流随时间的变化, (e) 放电储能密度W_dis以及(f) W_dis和W_rec比较图

Fig. 9. (a) Pulsed discharge current curves, (b) discharge energy density W_dis and discharge time t₉₀, and (c) comparative figures of W_dis and W_rec under breakdown electric field of the (1–x)KNN-xBMT ceramics; (d) pulsed discharge current curves, (e) discharge energy density W_dis, and (f) the comparative figures of W_dis and W_rec under different electric fields of the 0.85KNN-0.15BMT ceramic

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表 1 0.85 KNN-0.15 BMT陶瓷与其他部分无铅陶瓷储能性能的比较

Table 1. Comparison of energy storage properties of 0.85 KNN-0.15 BMT ceramics and other lead-free ceramics.

Material systerm	W_rec/J·cm^–3	η/%	BDS /kV·cm^–1	W_dis/J·cm^–3	t₉₀/ns	Reference
0.88BT-0.12BMT	1.81	88	224	—	—	[20]
0.85BT-0.15BY	0.50	—	100	—	—	[22]
0.61BF-0.33BT-0.06BMN	1.56	75	125	—	—	[24]
0.7BNT-0.3ST + 0.05MnO₂	0.96	74.6	95	—	—	[25]
0.8KNN-0.2SSN	2.02	81.4	295	—	—	[31]
0.85KNN-0.15ST	4.03	52	400	—	—	[32]
0.85KNN-0.15BMT	2.25	84	275	1.54	88	This work

下载: 导出CSV

[1]	Dang Z M, Yuan J K, Zha J W, Zhou T, Li S T, Hu G H 2012 Prog. Mater. Sci. 57 660 Google Scholar
[2]	Yao K, Chen S T, Rahimabady M, Mirshekarloo M S, Yu S H, Tay F E H, Sritharan T, Lu L 2011 IEEE Trans. Ultrason. Ferroelectr. Freq. Control 58 1968 Google Scholar
[3]	Cao Y, Irwin P C, Younsi K 2004 IEEE Trans. Dielectr. Electr. Insul. 11 797 Google Scholar
[4]	Park M H, Kim H J, Kim Y J, Moon T, Kim K D, Hwang C S 2014 Adv. Energy Mater. 4 1400610 Google Scholar
[5]	Chu B J, Zhou X, Ren K L, Neese B, Lin M R, Wang Q, Bauer F, Zhang Q M 2006 Science 313 334 Google Scholar
[6]	Khanchaitit P, Han K, Gadinski M R, Li Q, Wang Q 2013 Nat. Commun. 26 1 Google Scholar
[7]	Li Q, Chen L, Gadinski M R, Zhang S, Zhang G, Li H, Haque A, Chen L, Jackson T, Wang Q 2015 Nature 523 576 Google Scholar
[8]	Xu B, Íñiguez J, Bellaiche L 2017 Nat. Commun. 8 15682 Google Scholar
[9]	Wang D W, Fan Z M, Zhou D, Khesro A, Murakami S, Feteira A, Zhao Q L, Tan X L, Reaney L M 2018 J. Mater. Chem. A 6 4133 Google Scholar
[10]	Wu J Y, Mahajan A, Riekehr L, Zhang H F, Yang B, Meng N, Zhang Z, Yan H X 2018 Nano Energy 50 723 Google Scholar
[11]	Parizi S S, Mellinger A, Caruntu G 2014 ACS Appl. Mater. Interfaces 6 17506 Google Scholar
[12]	Liu X H, Li Y, Hao X H 2019 J. Mater. Chem. A 7 11858 Google Scholar
[13]	Shen B Z, Li Y, Hao X H 2019 ACS Appl. Mater. Interfaces 11 34117 Google Scholar
[14]	Chen L M, Sun N N, Li Y, Zhang Q W, Zhang L W, Hao X H 2018 J. Am. Ceram. Soc. 101 2313 Google Scholar
[15]	Palneedi H, Peddigari M, Hwang G T, Jeong D Y, Ryu J 2018 Adv. Funct. Mater. 28 1803665 Google Scholar
[16]	He C J, An Y, Deng C G, Gu X R, Wang J M, Wu T, Liu Y W, Lu Y G 2019 Mod. Phys. Lett. B 33 1950323 Google Scholar
[17]	Yao Y, Li Y, Sun N N, Du J H, Li X W, Zhang L W, Zhang Q W, Hao X H 2018 Ceram. Int. 44 5961 Google Scholar
[18]	An Y, He C J, Deng C G, Chen Z Y, Chen H B, Wu T, Lu Y G, Gu X R, Wang J M, Liu Y W, Li Z Q 2020 Ceram. Int. 46 4664 Google Scholar
[19]	Sun N N, Li Y, Zhang Q W, Hao X H 2018 J. Mater. Chem. C 6 10693 Google Scholar
[20]	Hu Q Y, Jin L, Wang T, Li C C, Xing Z, Wei X Y 2015 J. Alloys Compd. 640 416 Google Scholar
[21]	Wang T, Jin L, Li C C, Hu Q Y, Wei X Y 2015 J. Am. Ceram. Soc. 98 559 Google Scholar
[22]	Shen Z B, Wang X H, LuoB C, Li L T 2015 J. Mater. Chem. A 3 18146 Google Scholar
[23]	Zhou M X, Liang R H, Zhou Z Y, Dong X L 2018 J. Mater. Chem. A 6 17896 Google Scholar
[24]	Zheng D G, Zuo R Z, Zhang D S, Li Y 2015 J. Am. Ceram. Soc. 98 2692 Google Scholar
[25]	Cao W P, Li W L, Dai X F, Zhang T D, Sheng J, Hou Y F, Fei W D 2016 J. Eur. Ceram. Soc. 36 593 Google Scholar
[26]	Tian Y, Jin L, Hu Q Y, Yu K, Zhuang Y Y, Viola G, Abrahams I, Xu Z, Wei X, Yan H X 2019 J. Mater. Chem. A 7 834 Google Scholar
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[28]	Zhao L, Liu Q, Gao J, Zhang S J, Li J F 2017 Adv. Mater. 29 1701824 Google Scholar
[29]	Qiao X S, Zhang X S, Wu D, Chao X L, Yang Z P 2018 J. Adv. Dielectr. 8 1830006 Google Scholar
[30]	Shao T Q, Du H L, Ma H, Qu S B, Wang J, Wang J F, Wei X Y, Xu Z 2017 J. Mater. Chem. A 5 554 Google Scholar
[31]	Qu B Y, Du H L, Yang Z T 2016 J. Mater. Chem. C 4 1795 Google Scholar
[32]	Yang Z T, Du H L, Qu S B, Hou Y D, Ma H, Wang J F, Wang J, Wei X Y, Xu Z 2016 J. Mater. Chem. A 4 13778 Google Scholar
[33]	Yang Z T, Gao F, Du H L, Jin L, Yan L L, Hu Q Y, Yu Y, Qu S B, Wei X Y, Xu Z, Wang Y J 2019 Nano Energy 58 768 Google Scholar
[34]	Kosec M, Bobnar V, Hrovat M, Bernard J, Malic B, Holc J 2004 J. Mater. Res. 19 1849 Google Scholar
[35]	Malic B, Koruza J, Hrescak J, Bernard J, Wang K, Fisher J, Bencan A 2015 Materials 8 8117 Google Scholar
[36]	Hao X H, Wang Y, Zhang L, Zhang L W 2013 Appl. Phys. Lett. 102 163903 Google Scholar
[37]	杜红亮, 杨泽田, 高峰, 靳立, 程花蕾, 屈少波 2018 无机材料学报 33 1046 Google Scholar Du H L, Yang Z T, Gao F, Jin L, Cheng H L, Qu S B 2018 J. Inorg. Mater. 33 1046 Google Scholar
[38]	Chen L M, Hao X H, Zhang Q W, An S L 2016 J. Mater. Sci.- Mater Electron. 27 4534 Google Scholar
[39]	Chen X F, Zhang H L, Cao F, Wang G S 2009 J. Appl. Phys. 106 034105 Google Scholar
[40]	Zhang H, Chen X, Cao F, Wang G, Dong X, Hu Z, Du T 2010 J. Am. Ceram. Soc. 93 4015 Google Scholar
[41]	Ahn C W, Amarsanaa G, Won S S, Chae S A, Lee D S, Kim I W 2015 ACS Appl. Mater. Interfaces 7 26381 Google Scholar
[42]	Zhang Q M, Li C, Liu H W, Tang Q 2015 J. Am. Ceram. Soc. 98 366 Google Scholar
[43]	Xu R, Xu Z, Feng Y J, He H L, Tian J J, Huang D 2016 J. Am. Ceram. Soc. 99 2984 Google Scholar
[44]	李华梅, 李东杰, 陈学锋, 曹菲, 董显林 2008 物理学报 57 7298 Google Scholar Li H M, Li D J, Chen X F, Cao F, Dong X L 2008 Acta Phys. Sin. 57 7298 Google Scholar
[45]	Xu R, Xu Z, Feng Y J, Wei X Y, Tian J J, Huang D 2016 J. Appl. Phys. 119 224103 Google Scholar
[46]	Zhu M K, Liu L Y, Hou Y D, Wang H, Yan H 2007 J. Am. Ceram. Soc. 90 120 Google Scholar
[47]	Qu B Y, Du H L, Yang Z T, Liu Q H 2017 J. Am. Ceram. Soc. 100 1517 Google Scholar
[48]	Deng C G, He C J, Chen Z Y, Chen H B, Mao R, Liu Y W, Zhu K J, Gao H F, Ding Y 2019 J. Appl. Phys. 126 085702 Google Scholar
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(1–x)K_0.5Na_0.5NbO₃-xBi(Mg_0.5Ti_0.5)O₃无铅弛豫铁电陶瓷的介电、铁电和高储能行为

Dielectric, ferroelectric and high energy storage behavior of (1–x)K_0.5Na_0.5NbO₃–xBi(Mg_0.5Ti_0.5)O₃ lead free relaxor ferroelectric ceramics

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1.
内蒙古科技大学, 内蒙古自治区铁电新能源材料与器件重点实验室, 包头　014010

2.
内蒙古科技大学工业技术研究院, 包头　014010

3.
内蒙古科技大学化学与化工学院, 包头　014010

通信作者: 郝喜红, xhhao@imust.cn

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Corresponding author: Hao Xi-Hong, xhhao@imust.cn

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