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 Yun-Feng; Wang Jun-Xian; Wang Ze-Xing; Li Jia-Mao; Chen Li-Ming

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, 0.00 ≤ 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°C ≤ ±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:
sodium niobate /

relaxor ferroelectric /

lead-free energy storage ceramics /

energy storage properties
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图 1 (1–x)(NN-BMS)–xBNST (0.00 ≤ x ≤ 0.30)陶瓷实物样品图

Figure 1. Physical photo of (1–x) (NN-BMS)–xBNST (0.00 ≤ x ≤ 0.30) ceramics.

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图 2 (a) (1–x)(NN-BMS)–xBNST (0.00 ≤ 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 (0.00 ≤ 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 (0.00 ≤ x ≤ 0.30)陶瓷的XRD图谱的Rietveld精修结果　(a) x = 0.00; (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 (0.00 ≤ x ≤ 0.30) ceramics: (a) x = 0.00; (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 (0.00 ≤ x ≤ 0.3)陶瓷在最佳烧结温度下的SEM图　(a) x = 0.00; (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 (0.00 ≤ x ≤ 0.30)陶瓷的平均晶粒尺寸

Figure 4. SEM images of (1–x)(NN-BMS)–xBNST (0.00 ≤ x ≤ 0.30) ceramics at optimal sintering temperature: (a) x = 0.00; (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 (0.00 ≤ 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)Ó(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 (0.00 ≤ x ≤ 0.30)陶瓷的拉曼光谱图

Figure 7. Raman spectroscopy of (1–x)(NN-BMS)–xBNST (0.00 ≤ x ≤ 0.30) ceramics.

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图 8 (1–x)(NN-BMS)–xBNST (0.00 ≤ x ≤ 0.3)陶瓷的介电温谱图　(a) x = 0.00; (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 (0.00 ≤ x ≤ 0.30) ceramics: (a) x = 0.00; (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 (0.00 ≤ x ≤ 0.30)陶瓷的介电频谱图

Figure 9. Dielectric frequency spectra of (1–x)(NN-BMS)–xBNST (0.00 ≤ x ≤ 0.30) ceramics.

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图 10 (1–x)(NN-BMS)–xBNST (0.00 ≤ 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 (0.00 ≤ 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 (0.00 ≤ 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 (0.00 ≤ 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
0.00	Pnma	99.84	7.82(8)	7.82(8)	7.82(8)	479.73(5)	7.64	5.65	7.42
0.00	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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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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