Enhancement of Piezoelectric Properties in CaBi4Ti4O15-based Ceramics through Bi3+ Self-doping Strategy

doi:10.15541/jim20240537

Abstract

Abstract:

High-temperature piezoelectric vibration sensors are the preferred choice for structural health monitoring in harsh environments such as high temperatures and complex vibrations. Bismuth layer-structured CaBi₄Ti₄O₁₅ (CBT) high-temperature piezoelectric ceramics, with high Curie temperature (T_C), are the key components for piezoelectric vibration sensors operating at temperatures exceeding 500 ℃. However, their low piezoelectric coefficient (d₃₃) greatly limits their high-temperature applications. In this work, a novel Bi³⁺ self-doping strategy was employed to enhance the piezoelectric performance of CBT ceramics. The enhancement is attributed to an increase in the number of grain boundaries, providing more sites for space charge accumulation and promoting formation of space charge polarization. Furthermore, given that space charge polarization predominantly occurs at low frequencies, dielectric temperature spectra at different frequencies were used to elucidate the mechanism by which space charge polarization enhances piezoelectric properties of CBT ceramics. Excellent overall performance was achieved for the CBT-based high-temperature piezoelectric ceramics. Among them, T_C reached 778 ℃, d₃₃ increased by more than 30%, reaching 20.1 pC/N, and the electrical resistivity improved by one order of magnitude (reaching 6.33×10⁶ Ω·cm at 500 ℃). These advancements provide a key functional material with excellent performance for practical applications of piezoelectric vibration sensors at 500 ℃ and above.

Key words: high-temperature piezoelectric ceramic, bismuth layer structure, self-doping, space charge polarization, oxygen vacancy

CLC Number:

O482

ZHOU Yangyang, ZHANG Yanyan, YU Ziyi, FU Zhengqian, XU Fangfang, LIANG Ruihong, ZHOU Zhiyong. Enhancement of Piezoelectric Properties in CaBi₄Ti₄O₁₅-based Ceramics through Bi³⁺ Self-doping Strategy[J]. Journal of Inorganic Materials, 2025, 40(6): 719-728.

Figures/Tables 8

Fig. 1 (a-e) Surface SEM images of CBT-xBi ceramics after thermal etching; (f) XRD patterns of CBT-xBi ceramics and corresponding localized enlarged patterns (a) x=0; (b) x=0.02; (c) x=0.04; (d) x=0.06; (e) x=0.08

Fig. 2 Dielectric properties of CBT-xBi ceramics (a-c) Dielectric constant as a function of temperature at different frequencies after polarization: (a) x=0, (b) x=0.04 and (c) x=0.06; (d-f) Dielectric constant as a function of temperature at 100 Hz before and after polarization: (d) x=0, (e) x=0.04 and (f) x=0.06

Fig. 3 XPS core-level spectra of CBT-xBi ceramics (a) O1s; (b) Bi4f; (c) Bi4d3/2 and Ti2p

Table 1 Results of CBT-xBi ceramics O1s XPS peak fitting analysis

x	S₁ (Oxygen vacancy area)	S₂ (Lattice oxygen area)	S (Total area, S₁+S₂)	S₁/S₂	S₁/S
0	5581.86	23546.90	29128.76	0.24	0.19
0.04	5635.40	28758.79	34394.19	0.20	0.16
0.06	5078.49	27836.63	32915.12	0.18	0.15
0.06 (Oxygen sintering)	3969.83	24463.16	28432.99	0.16	0.14

Fig. 4 Characterization of CBT-0.06Bi ceramic sintered in a flowing oxygen atmosphere (a) XRD patterns; (b) SEM image of the thermal etching surface; (c) O1s XPS spectrum; (d) Dielectric temperature spectra at 100 Hz before and after polarization

Fig. 5 (a) Dielectric temperature spectra of CBT-xBi ceramics; (b) Temperature dependence of DC resistivity of CBT-xBi ceramics; (c) Effect of heat treatment on the piezoelectric constants of CBT-xBi ceramics (set temperature annealing 2 h); (d) In-situ XRD patterns of CBT-0.06Bi ceramic; (e) Relationship between lattice constants and unit cell volume with temperature; (f) (119) peak position and I(200)/I(020) changed with temperature

Fig. 6 (a) XRD refinement results of CBT-xBi ceramics; (b) Visual crystal structures of CBT-xBi ceramics; (c) Raman scattering spectra in the range of 80-900 cm-1; (d) Wavenumber displacements of B2g, B3g, A1g, and B1g modes

Fig. 7 PFM characterization of CBT-xBi ceramics (a-c) PFM phase images for (a) x=0, (b) x=0.04, and (c) x=0.06; (d-f) PFM amplitude distribution histograms for (d) x=0, (e) x=0.04, and (f) x=0.06; (g) TEM image of CBT-0.06Bi; (h) 5 μm×5 μm PFM phase image of CBT-0.06Bi; (i) Hysteresis loops of CBT-xBi ceramics after polarizing at 180 ℃ and 1 Hz. Colorful figures are available on website

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Enhancement of Piezoelectric Properties in CaBi₄Ti₄O₁₅-based Ceramics through Bi³⁺ Self-doping Strategy

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