Jing-Feng Li - Lead-Free Piezoelectric Materials

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Piezoelectric materials are used in a large variety of applications including actuators, sensors, electromechanical motors, and sonar systems. In the future, the applications will be extended to energy harvesting systems for distributed low‐power systems. The global market for piezoelectric devices is estimated to be valued at US$ 25.1 billion in 2019 and projected to expand at a compounded annual growth rate of 6.2% through the next five years [1]. One of the most widely used piezoelectric ceramic materials is the solid solution of lead zirconate (PbZrO 3) and lead titanate (PbTiO 3), commonly known as PZT, with general formula PbZr 1−xTi xO 3[2]. As mentioned in Chapter 1, although BaTiO 3was discovered before lead zirconate titanate (PZT), the latter soon dominated the market for piezoelectric applications because of its comprehensively excellent piezoelectric properties and high Curie temperature as well as the flexibility for compositional modification to adjust to specific applications.

The outstanding properties of PZT originate from the nature of end‐number compounds and the phase structure evolution in their solid solutions. Both PbZrO 3and PbTiO 3have perovskite structure with Pb ions at the same A‐site. PbZrO 3is antiferroelectric, but PbTiO 3is ferroelectric [3]. Solid solutions are formed between them in a full range, but there exists a steep boundary where a transition occurs between the rhombohedral Zr‐rich phase and the tetragonal Ti‐rich phase, as shown in Figure 2.1. It should be noted that the tetragonal PbTiO 3has a high transition temperature to cubic phase, which endow high Curie temperature to PZT. The phase boundary separating two phases in a solid solution system is called morphotropic phase boundary (MPB), where piezoelectric coefficients, dielectric constant, and electromechanical coupling factor are greatly enhanced [4]. The “phase boundary” is also considered as a composition where the two phases are believed to coexist, which renders the materials more responsive to extra stimuli. It should be noticed that the MPB is nearly temperature independent, which is why the properties of PZT ceramics have excellent temperature stability. More in‐depth studies had been conducted regarding the nature of the MPB using advanced structural characterization techniques, leading to several modified versions of the PZT phase diagram. One representative work suggested that the MPB is a narrow region where monoclinic phases exist in between the tetragonal and rhombohedral phases [5, 6]. It seems that the hierarchical structures ubiquitously present in ferroelectric materials makes the phase diagram studies more complicated than non‐ferroelectric materials [7]. Nevertheless, a similar concept of MPB is useful and highly desirable for the development of lead‐free piezoelectric materials.