Influence of (Bi0.5Na0.5)0.7Sr0.3TiO3 doping on structure and electrical properties of [0.93NaNbO3-0.07Bi(Mg0.5Sn0.5)O3] ceramics

GUO Yunfeng; WANG Junxian; WANG Zexing; LI Jiamao; CHEN Liming

doi:10.7498/aps.74.20240833

Abstract

Sodium niobate-based dielectric energy storage materials, as key components in capacitors, have the advantages such as low relative density, lead-free, low cost, and excellent energy storage density, and can meet the important requirements of electronic components for miniaturization, harmlessness, integration and light weight. Therefore, they have received extensive attention from the scientific community in recent years. In this work, by introducing both Bi(Mg_0.5Sn_0.5)O₃ and (Bi_0.5Na_0.5)_0.7Sr_0.3TiO₃ components into NaNbO₃ ceramics, a conventional solid-phase sintering method is used to prepare (1–x)[0.93NaNbO₃-0.07Bi(Mg_0.5Sn_0.5)O₃]-x(Bi_0.5Na_0.5)_0.7Sr_0.3TiO₃ (Abbreviated as (1–x)(NN-BMS)-xBNST, 0 ≤ x ≤ 0.3) relaxation ferroelectric ceramics, and the ceramics are characterized by using X-ray diffraction, scanning electron microscopy, UV spectroscopy and Raman spectroscopy so as to study the effects of (Bi_0.5Na_0.5)_0.7Sr_0.3TiO₃ doping on the physical phase composition, microstructure, and electrical properties of NaNbO₃ ceramics, such as dielectric and energy storage. The (1–x)(NN-BMS)-xBNST ceramics exhibit a single perovskite structure, with cell volume a first increasing and then decreasing. The coexistence of Pbma and Pnma phases (1–x)(NN-BMS)-xBNST ceramics exhibits a dense microstructure and clear grain boundaries at an optimal sintering temperature. The average grain size first increases to 4.73 μm, then decreases to 2.17 μm, and finally increases to 3.06 μm. A smaller grain size and a larger bandgap width are beneficial for improving the breakdown strength. The 0.75(NN-BMS)-0.25BNST ceramic shows the excellent dielectric temperature stability (25–160 ℃, Δε/ε_{25 ℃} ≤ ±15%) and dielectric frequency stability, which can meet the EIAZ8U standard and hence work in a special environment (high temperature and high frequency). Meanwhile, 0.75(NN-BMS)-0.25BNST ceramic exhibits excellent energy storage performance at high field strength (390 kV/cm): recoverable energy density W_rec = 2.73 J/cm³, energy storage efficiency η = 82.6%, and high temperature stability in a temperature range of 20–100 ℃. The research results indicate that 0.75(NN-BMS)-0.25BNST ceramics have broad prospects of applications in lead-free dielectric energy storage capacitors.

Keywords:

Authors and contacts

Advanced Ceramics Research Center, School of Materials Science and Engineering, Anhui University of Technology, Ma’anshan 243032, China

Corresponding author: LI Jiamao, lijiamao@ahut.edu.cn

Funds: Project supported by the Natural Science Foundation of the Anhui Higher Education Institutions of China (Grant No. KJ2019A0054).

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References

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[2]	Yang F, Pan Z B, Ling Z Q, Hu D, Ding J, Li P, Liu J J, Zhai J W 2021 J. Eur. Ceram. Soc. 41 2548
[3]	Li S, Nie H C, Wang G S, Xu C H, Liu N T, Zhou M X, Cao F, Dong X L 2019 J. Mater. Chem. C 7 1551 Google Scholar
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Cited By

图 1 (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷实物样品图

Figure 1. Physical photo of (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics.

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图 2 (a) (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷在最佳烧结温度下的XRD图; (b) (100)衍射峰峰位放大图; (c) (110)衍射峰峰位放大图; (d) (200)衍射峰峰位放大图

Figure 2. (a) XRD patterns of (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics at optimal sintering temperature; (b) enlarged image of (100) diffraction peak; (c) enlarged image of (110) diffraction peak; (d) enlarged image of (200) diffraction peak

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图 3 (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷的XRD图谱的Rietveld精修结果　(a) x = 0; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20; (e) x = 0.25; (f) x = 0.30

Figure 3. Rietveld refinement results of XRD patterns of (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics: (a) x = 0; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20; (e) x = 0.25; (f) x = 0.30.

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图 4 (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷在最佳烧结温度下的SEM图　(a) x = 0; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20; (e) x = 0.25; (f) x = 0.30. (g) (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷的平均晶粒尺寸

Figure 4. SEM images of (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics at optimal sintering temperature: (a) x = 0; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20; (e) x = 0.25; (f) x = 0.30. (g) Average grain size of (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics.

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图 5 (a) 0.75(NN-BMS)-0.25BNST陶瓷的EDS能谱图, 插图为SEM图; (b)—(i) EDS元素面扫描图

Figure 5. (a) EDS spectrum of 0.75(NN-BMS)-0.25BNST ceramic, the illustration shows SEM image; (b)–(i) EDS element surface scanning image.

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图 6 (a) 0.75(NN-BMS)-0.25BNST陶瓷的紫外吸收光谱; (b) 相应的Tauc plot图

Figure 6. (a) UV absorption spectra of 0.75(NN-BMS)-0.25BNST ceramic; (b) corresponding Tauc plot.

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图 7 (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷的拉曼光谱图

Figure 7. Raman spectroscopy of (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics.

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图 8 (1–x)(NN-BMS)–xBNST (0 ≤ x ≤ 0.30)陶瓷的介电温谱图　(a) x = 0; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20; (e) x = 0.25; (f) x = 0.30. (g) 0.75(NN-BMS)-0.25BNST陶瓷在不同频率下与温度相关的介电常数变化率

Figure 8. Dielectric temperature spectra of (1–x)(NN-BMS)–xBNST (0 ≤ x ≤ 0.30) ceramics: (a) x = 0; (b) x = 0.10; (c) x = 0.15; (d) x = 0.20; (e) x = 0.25; (f) x = 0.30. (g) Temperature dependent dielectric constant change rate of 0.75(NN-BMS)-0.25BNST ceramic at different frequencies.

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图 9 (1–x)(NN-BMS)–xBNST (0 ≤ x ≤ 0.30)陶瓷的介电频谱图

Figure 9. Dielectric frequency spectra of (1–x)(NN-BMS)–xBNST (0 ≤ x ≤ 0.30) ceramics.

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图 10 (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷　(a) 不同组分下的单极P-E环; (b) 不同组分下的 P_max, P_r 及 ΔP; (c) 不同组分下的电场强度; (d) 不同组分下的储能性能

Figure 10. (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics: (a) Unipolar P-E circuits under different components; (b) P_max, P_r and ΔP under different components; (c) electric field strength under different components; (d) energy storage properties under different components.

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图 11 0.75(NN-BMS)-0.25BNST陶瓷　(a) 不同场强下的P-E环; (b) 不同场强下的P_max, P_r及ΔP; (c) 电场和储能性能的关系

Figure 11. 0.75(NN-BMS)-0.25BNST ceramic: (a) P-E circuits under different field strengths; (b) P_max, P_r and ΔP under different field strengths; (c) relationship between electric field and energy storage performance.

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图 12 0.75(NN-BMS)-0.25BNST陶瓷　(a) 不同温度下的P-E环; (b) 不同温度下的W_rec和η

Figure 12. 0.75(NN-BMS)-0.25BNST ceramic: (a) P-E circuits at different temperatures; (b) W_rec and η at different temperatures.

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表 1 (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30)陶瓷的Rietveld精修结构参数

Table 1. Rietveld refined structural parameters of (1–x)(NN-BMS)-xBNST (0 ≤ x ≤ 0.30) ceramics.

x	Phase	Volume fraction/%	Lattice parameters/Å			V/Å³	R_wp/%	R_p/%	χ²
x	Phase	Volume fraction/%	a	b	c	V/Å³	R_wp/%	R_p/%	χ²
0	Pnma	99.84	7.82(8)	7.82(8)	7.82(8)	479.73(5)	7.64	5.65	7.42
0	Pbma	0.16	5.56(8)	15.74(7)	5.54(7)	486.44(1)	7.64	5.65	7.42
0.10	Pnma	67.2	7.82(3)	7.82(9)	7.83(4)	479.87(3)	5.47	4.18	3.71
0.10	Pbma	32.8	5.54(5)	15.60(9)	5.52(1)	478.00(0)	5.47	4.18	3.71
0.15	Pnma	63.3	7.82(3)	7.82(9)	7.83(5)	479.89(9)	5.59	4.43	3.85
0.15	Pbma	36.7	5.55(0)	15.62(9)	5.52(9)	479.66(5)	5.59	4.43	3.85
0.20	Pnma	53.1	7.82(0)	7.82(6)	7.83(5)	479.59(3)	5.04	3.82	2.89
0.20	Pbma	46.9	5.54(5)	15.63(5)	5.53(9)	480.26(4)	5.04	3.82	2.89
0.25	Pnma	57.1	7.82(1)	7.82(8)	7.83(5)	479.77(9)	5.39	4.21	3.27
0.25	Pbma	42.9	5.42(1)	15.66(4)	5.53(2)	480.28(9)	5.39	4.21	3.27
0.30	Pnma	65.65	7.82(1)	7.82(7)	7.83(5)	479.70(5)	5.04	3.92	2.41
0.30	Pbma	34.35	5.53(8)	15.60(1)	5.52(4)	477.28(3)	5.04	3.92	2.41

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[1]	杨敏铮, 江建勇, 沈洋 2021 硅酸盐学报 49 1249 Google Scholar Yang M Z, Jiang J Y, Shen Y 2021 J. Chin. Ceram. Soc. 49 1249 Google Scholar
[2]	Yang F, Pan Z B, Ling Z Q, Hu D, Ding J, Li P, Liu J J, Zhai J W 2021 J. Eur. Ceram. Soc. 41 2548
[3]	Li S, Nie H C, Wang G S, Xu C H, Liu N T, Zhou M X, Cao F, Dong X L 2019 J. Mater. Chem. C 7 1551 Google Scholar
[4]	Zou K L, Dan Y, Xu H J, Zhang Q F, Lu Y M, Huang H T, He Y B 2019 Mater. Res. Bull. 113 190 Google Scholar
[5]	沈忠慧, 江彦达, 李宝文, 张鑫 2020 物理学报 69 217706 Google Scholar Shen Z H, Jiang Y D, Li B W, Zhang X 2020 Acta Phys. Sin. 69 217706 Google Scholar
[6]	Zhou M X, Liang R H, Zhou Z Y, Yan S G, Dong X L 2018 ACS Sustain. Chem. Eng. 6 12755 Google Scholar
[7]	Zhang S, Xia R, Shrout T R 2007 J. Electroceram. 19 251 Google Scholar
[8]	Shrout T R, Zhang S J 2007 J. Electroceram. 19 113 Google Scholar
[9]	张天富, 司洋洋, 黎意杰, 陈祖煌 2023 物理学报 72 097704 Google Scholar Zhang T F, Si Y Y, Li Y J, Chen Z H 2023 Acta Phys. Sin. 72 097704 Google Scholar
[10]	Yu Z L, Liu Y F, Shen M Y, Qian H, Li F F, Lü Y N 2017 Ceram. Int. 43 7653 Google Scholar
[11]	Yao F Z, Yuan Q, Wang Q, Wang H 2020 Nanoscale 12 17165 Google Scholar
[12]	Li D X, Zeng X J, Li Z P, Shen Z Y, Hao H, Luo W Q, Wang X C, Song F S, Wang Z M, Li Y M 2021 J. Adv. Ceram. 10 675 Google Scholar
[13]	Yang Z T, Du H L, Jin L, Poelman D 2021 J. Mater. Chem. A 9 18026.Google Scholar
[14]	郑明, 杨健, 张怡笑, 关朋飞, 程奥, 范贺良 2023 物理学报 72 177801 Google Scholar Zheng M, Yang J, Zhang Y X, Guan P F, Cheng A, Fan H L 2023 Acta Phys. Sin. 72 177801 Google Scholar
[15]	Liang C, Wang C Y, Zhao H Y, Cao W J, Li F, Wang C C 2023 J. Alloys Compd. 961 170962 Google Scholar
[16]	Ye J M, Wang G S, Chen X F, Dong X L 2021 J. Materiomics 7 339
[17]	Chen J, Qi H, Zuo R Z 2020 ACS Appl. Mater. Inter. 12 32871 Google Scholar
[18]	Wada T, Tsuji K, Saito T, Matsuo Y 2003 Jpn. J. Appl. Phys. 42 6110 Google Scholar
[19]	Qi H, Zuo R Z 2019 J. Mater. Chem. A. 7 3971 Google Scholar
[20]	Pang F H, Chen X L, Sun C C, Shi J P, Li X, Chen H Y, Dong X Y, Zhou H F 2020 ACS Sustain. Chem. Eng. 8 14985 Google Scholar
[21]	Xu Z Q, Liu Z, Dai K, Lu T, Lü Z Q, Hu Z G, Liu Y, Wang G S 2022 J. Mater. Chem. A. 10 13907 Google Scholar
[22]	郭云凤, 王俊贤, 王泽星, 李家茂, 刘畅 2024 化学学报 82 511 Google Scholar Guo Y F, Wang J X, Wang Z X, Li J M, Liu C 2024 Acta Chim. Sinica. 82 511 Google Scholar
[23]	Pang F H, Chen X L, Shi J P, Sun C C, Chen H Y, Dong X Y, Zhou H F 2021 ACS Sustain. Chem. Eng. 9 4863 Google Scholar
[24]	Shannon R D 1979 Acta Cryst. A 32 751
[25]	Zhang S Y, Li W H, Zhang Y S, Tang X G, Jiang Y P, Guo X B 2023 Results Phys. 44 106194 Google Scholar
[26]	Chen H Y, Wang X, Dong X Y, Pan Y, Wang J M, Deng L, Dong Q P, Zhang H L, Zhou H F, Chen X L 2022 ACS Appl. Mater. Inter. 14 25609 Google Scholar
[27]	Dong X Y, Li X, Chen X L, Tan Z, Wu J G, Zhu J G, Zhou H F 2022 Nano Energy 101 107577 Google Scholar
[28]	Chen X L, Li X, Sun J, Sun C C, Shi J P, Pang F H, Zhou H F 2020 Ceram. Int. 46 2764 Google Scholar
[29]	Han K, Luo N N, Chen Z P, Ma L, Chen X L, Feng Q, Hu C Z, Zhou H F, Wei Y Z, Toyohisa F 2020 J. Eur. Ceram. Soc. 40 3562 Google Scholar
[30]	Yan F, Bai H R, Shi Y J, Ge G L, Zhou X F, Lin J F, Shen B, Zhai J W 2021 Chem. Eng. J. 425 130669 Google Scholar
[31]	Shi J P, Chen X L, Li X, Sun J, Sun C C, Pang F H, Zhou H F 2020 J. Mater. Chem. C 8 3784 Google Scholar
[32]	Cao W J, Lin R J, Chen P F, Li F, Ge B H, Song D S, Zhang J, Cheng Z X, Wang C C 2022 ACS Appl. Mater. Inter. 14 54051 Google Scholar
[33]	Sun N N, Li Y, Zhang Q W, Hao X H 2018 J. Mater. Chem. C. 6 10693 Google Scholar
[34]	Shen Y H, Wu L K, Zhao J H, Liu J J, Tang L M, Chen X Q, Li H H, Su Z, Zhang Y, Zhai J W, Pan Z B 2022 Chem. Eng. J. 439 135762 Google Scholar
[35]	Nie X R, He Y, Shi Q Q, Liang Y Q, Wei L L, Liang P F, Chao X L, Hu G X, Yang Z P 2023 J. Adv. Dielect. 13 2242005 Google Scholar
[36]	杜金花, 李雍, 孙宁宁, 赵烨, 郝喜红 2020 物理学报 69 127703 Google Scholar Du J H, Li Y, Sun N N, Zhao Y, Hao X H 2020 Acta Phys. Sin. 69 127703 Google Scholar
[37]	Wei K, Duan J H, Zhou X F, Li G S, Zhang D, Li H 2023 ACS Appl. Mater. Inter. 15 48354 Google Scholar

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Vol. 74, Issue 1 - 2025-01-05

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Influence of (Bi_0.5Na_0.5)_0.7Sr_0.3TiO₃ doping on structure and electrical properties of [0.93NaNbO₃-0.07Bi(Mg_0.5Sn_0.5)O₃] ceramics

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Corresponding author: LI Jiamao, lijiamao@ahut.edu.cn

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