Abstract Good thermal stability in lead-free BaTiO3 ceramics is important for their applications above room temperature. In this study, thermal stable piezoelectricity in lead-free (Ba,Ca)(Ti,Zr)O3 ceramics was enhanced by tailoring their phase transition behaviors. Comparison between (1-x)Ba(Ti0.8Zr0.2)O3-x(Ba0.65Ca0.35)TiO3 and (1-y)Ba(Ti0.8Zr0.2)O3-y(Ba0.95Ca0.05)TiO3 revealed that latter system at y = 0.80 had much better thermal stable piezoelectric coefficient than the former at x = 0.45. Both systems crystalized in tetragonal to orthorhombic phase boundary at room temperature. The phase transition temperature and degree of diffusion were adjusted by Ca and Zr ions contents and demonstrated great influence on temperature dependent dielectric permittivity, hysteresis loops, and in-situ domain structures. The improved thermal stability of (1-y)Ba(Ti0.8Zr0.2)O3-y(Ba0.95Ca0.05)TiO3 prepared at y = 0.80 was linked to its higher paraelectric to ferroelectric phase transition temperature (Tm = 115.7 °C) and less degree of diffusion (degree of diffusion constant γ = 1.35). By comparison, (1-x)Ba(Ti0.8Zr0.2)O3-x(Ba0.65Ca0.35)TiO3 prepared at x = 0.45 revealed Tm = 81.3 °C and γ = 1.65. Overall, these findings look promising for future stimulation of phase transition behaviors and design of piezoelectric materials with good thermal stabilities.

中文翻译：

---

通过调整相变行为提高无铅 (Ba,Ca)(Ti,Zr)O3 系统中压电的热稳定性

摘要 无铅 BaTiO3 陶瓷良好的热稳定性对其在室温以上的应用很重要。在这项研究中，无铅 (Ba,Ca)(Ti,Zr)O3 陶瓷的热稳定压电性能通过调整其相变行为得到增强。(1-x)Ba(Ti0.8Zr0.2)O3-x(Ba0.65Ca0.35)TiO3与(1-y)Ba(Ti0.8Zr0.2)O3-y(Ba0.95Ca0.05)对比TiO3 表明后一种系统在 y = 0.80 时比前者在 x = 0.45 时具有更好的热稳定压电系数。两种系统在室温下均以四方至正交相界结晶。相变温度和扩散程度由 Ca 和 Zr 离子含量调节，并且对温度相关的介电常数、磁滞回线和原位域结构有很大影响。在 y = 0.80 下制备的 (1-y)Ba(Ti0.8Zr0.2)O3-y(Ba0.95Ca0.05)TiO3 改善的热稳定性与其较高的顺电到铁电相变温度 (Tm = 115.7 ° C) 和较小的扩散程度（扩散程度常数 γ = 1.35）。相比之下，在 x = 0.45 制备的 (1-x)Ba(Ti0.8Zr0.2)O3-x(Ba0.65Ca0.35)TiO3 显示 Tm = 81.3 °C 和 γ = 1.65。总的来说，这些发现对于未来相变行为的刺激和具有良好热稳定性的压电材料的设计看起来很有希望。45 显示 Tm = 81.3 °C 和 γ = 1.65。总的来说，这些发现对于未来相变行为的刺激和具有良好热稳定性的压电材料的设计看起来很有希望。45 显示 Tm = 81.3 °C 和 γ = 1.65。总的来说，这些发现对于未来相变行为的刺激和具有良好热稳定性的压电材料的设计看起来很有希望。