Ultrahigh strain in textured BCZT-based lead-free ceramics with CuO sintering agent

doi:10.1016/j.jmst.2022.02.002

Abstract

Abstract:

Textured BaTiO₃ (BT)-based lead-free ceramics have gained significant attention due to their high piezoelectric coefficient (d) and very large field induced strain (S). However, costly nano-size raw materials, excessively high sintering temperature and low Curie temperature (T_c) hinder their device applications. In this work, highly [001]_c-oriented (Ba_0.95Ca_0.05)(Zr_0.04Ti_0.96)O₃ ceramics with x mol% CuO (x = 0.25, 0.5, 1.0, 2.5) denoted as BCZT-x were synthesized by templated grain growth using micro-sized raw powders. The introduction of CuO sintering agent lowered the sintering temperature by 125 °C to 1450 °C, and the BCZT-1.0 achieved a high texture degree of ∼99%. In addition, the CuO-based liquid phases eliminated boundaries between BT templates and BCZT matrix powders. Such liquid-phase sintering reduced sintering stresses, decreased the average grain size of BCZT-1.0 from 16 μm down to 13 μm, and increased the dielectric dispersion coefficient γ to 1.63. The almost smoothed out T_O-T anomaly in the temperature dependence of dielectric permittivity and comparably high T_c (> 102 °C) lead to better temperature stability. The narrower grain orientation distribution with full width at half maximum (FWHM) of ∼5.9° and smaller domains with the size of 0.1-0.5 μm in width and 3-8 μm in length were obtained, a high field induced maximum strain S_max of 0.38% and low H_s of 5.2% have been achieved in BCZT-1.0 textured ceramics together with a high and homogeneous piezoelectric stress coefficient d₃₃ ∼780 pC/N and very large d₃₃* ∼2950 pm/V.

Key words: Lead-free, BCZT, Textured ceramics, Piezoelectric, Strain hysteresis

Yingchun Liu, Hongjun Zhang, Wenming Shi, Qian Wang, Guicheng jiang, Bin Yang, Wenwu Cao, Jiubin Tan. Ultrahigh strain in textured BCZT-based lead-free ceramics with CuO sintering agent[J]. J. Mater. Sci. Technol., 2022, 117: 207-214.

Figures/Tables 7

Fig. 1. (a) XRD patterns of randomly oriented BCZT-R and BT templated BCZT ceramics with various CuO contents (BCZT-x, x = 0.25, 0.5, 1.0 and 2.5), showing different texture fractions f00l. The peaks are indexed using pseudocubic Miller indices; (b) main (002)c peaks of BCZT between 44° and 46°; (c) changes of texture fraction f00l of BCZT-x with sintering temperature.

Fig. 2. SEM images of (a) randomly oriented BCZT-R; (b-e) textured BCZT-x ceramics with various CuO contents (x = 0.25, 0.5, 1.0 and 2.5); (f) average grain sizes of BCZT-x ceramics.

Fig. 3. Texture evolution of BCZT-1.0 with the sintering temperature: (a) 1300 °C, (b) 1350 °C, (c) 1400 °C, (d) 1450 °C, experiencing no soaking stage.

Fig. 4. (a) Temperature dependence of the dielectric constant εr measured at 1 kHz; (b) plots of ln(1/εr- 1/εm) vs. ln(T - Tm) for BCZT-R and BCZT-x ceramics.

Fig. 5. (a) Unipolar S-E curves measured at 20 kV/cm; (b) effective piezoelectric coefficient d33* and strain hysteresis Hs; (c) piezoelectric coefficient d33 and the electromechanical coupling coefficient kt, as a function of CuO content; (d) P-E hysteresis loops measured at 20 kV/cm, for BCZT-R and BCZT-x ceramics.

Fig. 6. (a) Electric field induced unipolar strain S of textured BCZT-1.0 and other well-known Pb-based piezoelectric ceramics, including textured PMN-PZT ceramic, commercial PZT-5H and PZT-4. (b) Piezoelectric coefficient d33 as a function of strain hysteresis Hs for modified BT-based ceramics [[58], [59], [60], [61], [62], [63], [64], [65], [66], [67], [68], [69], [70], [71], [72], [73], [74], [75], [76], [77], [78], [79], [80], [81], [82], [83]]. Both high piezoelectric coefficient and low strain hysteresis at 20 kV/cm was observed in the textured BCZT-1.0 ceramic (this work).

Fig. 7. (a) EBSD map (inverse pole figures, IPFz) and its corresponding (001)c (inverse) pole figures; and (b) grain orientation distributions obtained by fitting (001)c pole figure data to the March-Dollase function of the textured BCZT-1.0 ceramic. PFM amplitude and phase images for unpoled (c) randomly oriented BCZT-R ceramic and (d) textured BCZT-1.0 ceramic.

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