Tailoring depolarization temperature by phase transition causing properties evolution in Bi0.5(Na1-xKx)0.5TiO3 ceramics

doi:10.1016/j.jmst.2021.09.066

Abstract

Abstract:

(Bi_0.5Na_0.5)TiO₃-based materials have attracted widespread attention due to large electro-strain, large remnant polarization (P_r) and high Curie temperature (T_C), but the existence of inherent depolarization temperature (T_d) limits the temperature stability and application temperature range. In this work, we find that K/Na ratio can regulate T_d (from 90 °C to 246 °C) of the ceramics, which confirms that the increase of K substitution can effectively improve the temperature stability of the material. The phase structure and electrical properties of Bi_0.5(Na_1-_xK_x)_0.5TiO₃ (BNKTx) ceramics can be well modulated by changing K/Na. In addition, BNKTx system exhibits excellent piezoelectric response at morphotropic phase boundary (MPB) of 20% BKT content (d₃₃=180 pC/N), where rhombohedral (R3c) phase and tetragonal (P4bm) phase coexist in MPB. With K further substitution, BNKTx ceramics transform into tetragonal phase, and the domain size grows due to the structural transition from short-range-correlated P4bm to long-range-correlated P4mm. The deferment of T_d is also tightly related to the increase of P4mm/P4bm ratio. This work can provide an effective way to tailor depolarization temperature and electrical properties of BNT-based ceramics.

Key words: Depolarization temperature, (Bi_0.5Na_0.5)TiO₃, Piezoelectric ceramics, Piezoelectric constant, Temperature stability

Diyan Yang, Jihui Han, Jie Yin, Haoyue Xue, Jiagang Wu. Tailoring depolarization temperature by phase transition causing properties evolution in Bi_0.5(Na_1-_xK_x)_0.5TiO₃ ceramics[J]. J. Mater. Sci. Technol., 2022, 114: 111-119.

Figures/Tables 9

Fig. 1. FE-SEM images of surface macrographs of BNKTx ceramics with different K contents: (a) x = 0.18, (b) x = 0.35, (c) x = 0.50, and (d) x = 0.80. (e) XRD patterns of unpoled BNKTx samples with different x contents, and their enlarged XRD patterns. (f-i) Grain size distributions from SEM images (f, g, h, i are derived from a, b, c and d, respectively).

Fig. 2. (a) The normalized d33 (measurement at in-situ environment) of poled BNKTx ceramics as a function of temperature. Variations of (b) d33, as well as (c) εr and tanδ values of BNKTx ceramics with different K contents.

Fig. 3. (a-e) Rietveld refinement of XRD results for the poled BNKTx samples (x = 0.2, 0.35, 0.5, 0.65, and 0.8), (f) variation of weight fraction of P4mm/R3c/P4bm phases with K doping.

Fig. 4. Composition-dependent vertical PFM images for the unpoled samples with (a, c, e) x=0.2 and (b, d, f) x=0.8 at the ambient temperature. The same scanning area of images (a-d) is 2μm×2μm. A negative DC voltage (30 V) was first applied to the tip during the scanning of a 4μm×4μm area. Then, a positive DC voltage with different values (5, 10, 15 and 20 V), depending on the scanning areas, was applied. (e, f) The PFM images for the poled x=0.2 sample (e) and x=0.8 sample (f), respectively. (g, h) Domain size distributions from PFM images (g and h are derived from a and b, respectively).

Fig. 5. Temperature dependence of poled dielectric constants and loss tangents of BNKTx ceramics: (a) x = 0.20, (b) x = 0.35, (c) x = 0.5, (d) x = 0.65, (e) x = 0.80, (f) x = 1.

Fig. 6. (a-c) Temperature-dependent polarization versus electric field (P-E) loops for BNKTx (x = 0.35, 0.80, 1.0). (d-f) Temperature-dependent Pr and EC derived from P-E loops.

Fig. 7. (a-c) Temperature-dependent bipolar electro-strain versus electric field (S-E) loops for BNKTx ceramics (x = 0.35, 0.80, 1.0). (d-f) And temperature-dependent Smax (maximum electro-strain) and Sneg (negative electro-strain) derived from temperature-dependent S-E loops.

Fig. 8. (a-c) Temperature-dependent unipolar electro-strain versus electric field (S-E) loops for BNKTx ceramics (x = 0.35, 0.80, 1.0). (d-f) And temperature-dependent S derived from temperature-dependent S-E loops.

Fig. 9. (a-c) Temperature-dependent polarization current versus electric field (J-E) loops for BNKTx ceramics (x = 0.2, 0.35, 0.8).

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Tailoring depolarization temperature by phase transition causing properties evolution in Bi_0.5(Na_1-_xK_x)_0.5TiO₃ ceramics

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