The field of lead-free piezoceramics, which aims to replace lead zirconate titanate (PZT) and related perovskite materials, has been vibrant for almost 15 years. Once the science in this field attained a certain stage of maturity, materials with properties better than PZT have appeared, and the first products are about to reach the marketplace. This article describes the three most promising lead-free piezoceramics currently under discussion to replace PZT. Each has a pronounced property profile geared for specific applications. Guidelines for directions for fundamental future research on as well as technology transfer to industry of lead-free piezoceramics are provided.

/pdf/lead-free-piezoceramics-status-and-perspectives-25zjhc5zto.pdf

Lead-free piezoceramics: Status and perspectives

A lead-free multiferroic ceramic of BiFe0.96Sc0.04O3–BaTiO3 is a type of ABO3 perovskite structure, belonging to the R3c space group, but exhibiting poor insulation and weak multiferroicity. In this work, the critical roles of Mn-ions in tailoring the electrical and magnetic properties of BiFeO3-based materials are revealed: the introduction of MnO2 into BiFe0.96Sc0.04O3–BaTiO3 induces a dramatic improvement in insulation, piezoelectricity and multiferroicity. New compositions of BiFe0.96Sc0.04O3–BaTiO3 + x mol% MnO2 were synthesized by a conventional solid-state reaction method. All the ceramics possess a perovskite structure, and a morphotropic phase boundary (MPB) of rhombohedral and monoclinic phases is formed at x = 0.5–1.0. The formation of and is noticeably suppressed and the resistivity of the ceramics is increased by ∼100 times after the addition of 0.5–1.0 mol% MnO2, which make the ceramic polarizable and thus give strong ferroelectricity and considerable piezoelectricity. The ceramics with the MPB composition exhibit high electrical insulation (R = 1.2–1.7 × 1010 Ω cm), good piezoelectricity (d33 = 123–143 pC N−1, kp = 0.34–0.35), strong ferroelectricity (Pr = 13.1–17.6 μC cm−2), high Curie temperature (590–596 °C) and excellent temperature stability of piezoelectric and ferroelectric properties. These improvements are greatly associated with the contribution of Mn ions in the ceramics. Surprisingly, sharply enhanced ferromagnetism with Mr = 0.4946 emu g−1 and Ms = 1.0298 emu g−1 is obtained in the ceramic with x = 7.0, almost one thousand times larger than that of an un-doped ceramic. The origin of unusual ferromagnetism is associated with significant changes in magnetic ordering caused by Mn doping. The high magnetoelectric effect (α33 = 429.6 mV cm−1 Oe−1) is obtained after the addition of 2.0 mol% Mn ions. Our study suggests that the present ceramics may have potential applications in advanced memory devices as promising lead-free high temperature piezoelectric and multiferroic materials.

Critical roles of Mn-ions in enhancing the insulation, piezoelectricity and multiferroicity of BiFeO3-based lead-free high temperature ceramics

Lead-free and high-temperature 0.71BiFeO3-0.29BaTiO3 ceramics with Mn modification (BF-BT-x %Mn) were fabricated by conventional solid-state reaction method, and the high temperature dielectric, ferroelectric and piezoelectric properties were investigated. All compositions exhibited pseudo-cubic phases. Mn modification improved the electrical properties of BF-BT solid solutions at both room and high temperature. The Curie temperature T
 C, depolarization temperature T
 d, dielectric constant e
 r, dielectric loss tanδ, piezoelectric constant d
 33, electromechanical coupling factor k
 p, remnant polarization P
 r of BF-BT-1.2 %Mn ceramics were 506, 500 °C, 556, 0.04, 169 pC N−1, 0.373, 31.4 μC cm−2, respectively. The e
 r, tanδ, and k
 p of BF-BT-1.2 %Mn ceramics were stable with the increase of temperature until 500 °C. The coercive field E
 c of BF-BT-1.2 %Mn ceramics was nearly 30 kV cm−1 at 200 °C, which was much larger than those of PZT, BS-PT,BNT and KNN ceramics. The high field strain coefficient d*33 reached as large as 525 pm V−1 at 200 °C. These results showed that the BF-BT-x %Mn ceramics were promising candidate for high temperature piezoelectric applications.

High temperature dielectric, ferroelectric and piezoelectric properties of Mn-modified BiFeO3-BaTiO3 lead-free ceramics

Enhanced thermal stability of lead-free high temperature 0.75BiFeO3–0.25BaTiO3 ceramics with excess Bi content

Less temperature-dependent high dielectric and energy-storage properties of eco-friendly BiFeO3–BaTiO3-based ceramics

Effect of Zr4+ substitution on thermal stability and electrical properties of high temperature BiFe0.99Al0.01O3–BaTi1−xZrxO3 ceramics

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Effect of Zr4+ substitution on thermal stability and electrical properties of high temperature BiFe0.99Al0.01O3–BaTi1−xZrxO3 ceramics