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• A valid strategy to improve the piezoelectricity of Bi4Ti3O12-based systems is proposed by tailoring oxygen vacancy defects.
• Excellent piezoelectricity (d33) 32.1 pC/N and Curie temperature (Tc) 659 ℃ are gotten in the Bi4Ti3O12-based ceramics.
• Bi4Ti3O12-based ceramics is featured with excellent piezoelectric stability and low conductivity (~10−7 Ω−1 cm−1 at 500 ℃).
Bismuth titanate (Bi4Ti3O12, BIT) piezoelectric materials have attracted increasing attention due to their high-temperature applications. However, it is quite challenging to simultaneously achieve outstanding piezoelectric properties and high Curie temperature in BIT-based systems. In this study, oxygen vacancy defects tailoring strategy was utilized to solve this problem, excellent piezoelectric coefficient (32.1 pC/N), and ultrahigh Curie temperature (659 ℃) are gotten in Bi4Ti3-x(Mn1/3Nb2/3)xO12 (BTMN) ceramics, which are among the top values in the BIT-based ceramics. More importantly, the (Mn1/3Nb2/3)(4+δ)+ complex-ion modified Bi4Ti3O12-based ceramics are characterized with excellent piezoelectric stability up to 500 ℃ (d33 > 30.0 pC/N at 500 ℃)) and significantly reduced conductivity (only ~ 10−7 Ω−1 cm−1 at 500 ℃). Moreover, enhanced ferroelectricity and good dielectric stability were also obtained. The better comprehensive properties can be ascribed to two aspects. First, the concentration of oxygen vacancy defects is obviously reduced, and their distribution is effectively controlled in BITMN ceramics. Second, the introduction of (Mn1/3Nb2/3)(4+δ)+ complex-ion gives rise to the antiphase boundaries and massive ferroelectric domain walls. This works not only reveal the high potential of BITMN ceramics for high-temperature piezoelectric applications but also deepen the understanding of the structure-properties relationship in BIT-based materials.
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