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Researchers are studying how to replace PZT materials to protect the environment. Continuous research is ongoing to construct different lead-free materials for environmentally friendly applications. This article considers research conducted by Kuanar, B, and others. 

Image source: BossCo77/Shutterstock.com

Scientists have been focusing on high dielectric constant capacitors, buzzers, sensors, ultrasonic motors, actuators, piezoelectric sonar, ultrasonic transducers, medical diagnostic transducers, ferroelectric thin film memories, multilayer capacitors, ferroelectrics Random Access Memory (FERAM) and very fast. Due to the presence of lead, the piezoelectric ceramic PZT used in functional devices is toxic. 

At present, researchers turn to lead-free piezoelectric ceramics, namely titanate-based perovskite materials (BaTiO3, Na0.5Bi0.5TiO3, K0.5Bi0.5TiO3 and BaZr0.08Ti0.92O3) and their solid solutions.

The main disadvantage of natural piezoelectric materials is the truncated piezoelectricity. Lead oxide is a PZT component and is highly toxic in behavior. Due to its volatility at high temperatures, toxicity can be enhanced. 

Between two different lead-free systems: (i) Perovskite materials are bismuth sodium titanate (BNT), barium titanate oxide (BaTiO3), potassium niobate (KNbO3), sodium titanate oxide (NaTiO3) ) Wait. (ii) Materials such as non-perovskite bismuth layer structure and tungsten bronze have become suitable materials to replace lead-based ceramics.

However, the main bottlenecks include low Curie temperature (TC) and high coercivity, which makes it difficult for ceramics to undergo polarization state transitions and has significant conductivity and dielectric loss.

Due to the large remanent polarization (Pr∼38 μC/cm2), sodium bismuth titanate (Ba0.5Na0.5TiO3; BNT) is considered to be the right candidate for lead-free piezoelectric ceramics at room temperature. BNT has a complex perovskite structure and rhombohedral phase. If the transition temperature is 200 °C, it will transform into the antiferroelectric phase. The Curie temperature (Tc) of this material is approximately 320 °C.

Due to the above-mentioned advantages of BNT, the author mainly focuses on the phase transition, electrical and dielectric behavior changes of BNT, its solid solution with other perovskite structures, and at stations A and/or B.

Figure 1 shows the sample stoichiometry followed by the various research teams. Among the various powder preparation methods available, the most common is to adopt the mixed oxide route, in which the appropriate stoichiometric ratio of the desired oxide is used. In order to achieve the required chemical and optical uniformity, ball milling is essential. Grinding time is based on powder characteristics and ranges from 2 to 16 hours.

Figure 1. Sample preparation and characterization steps: (a) solid-state route, (b) spontaneous combustion route, and (c) sol-gel route. Image credit: Kuanar et al., 2021

Usually, the mixture is ground with zirconia or alumina balls with non-flammable liquids (such as trichloroethylene) or distilled water. The ground powder is then dried and calcined (800°C–900°C) for 2 to 3 hours.

In the calcination process, volatile components such as moisture are separated, and then the desired phase is formed. Organic vehicles usually include binder (ethyl cellulose), plasticizer (polyethylene glycol), dispersant (butoxy ethoxy ethyl acetate) and solvent (α-terpineol).

After the calcination process, polyvinyl alcohol (PVA) is used as a binder to compact the granulated powder particles. The pellets are then sintered at a temperature varying between 1050°C and 1200°C. For the electrode, the sintered particles are coated with silver paste, and for the orientation, the ferroelectric domains and electrical properties in the ceramic are measured by applying a strong DC field.

Use automatic LCR meter bridge for dielectric measurement (dielectric loss and permittivity). The Sawyer-Tower circuit is used to perform ferromagnetic hysteresis measurements. The piezoelectric constant tester is used to measure the piezoelectric coefficient d33. Researchers use Raman, FTIR, PL and UV to study other properties of materials for various industrial applications.

The ferroelectric oxide with the general formula ABO3 is considered to be a perovskite structure, such as Bi0.5Na0.5TiO3 (BNT), BaTiO3 (BT), KNbO3, NaTiO3, NaTaO3, etc., which are well-known lead-free piezoelectric materials. According to the requirements of its simple structure, the physical properties of this structure can be easily adjusted by using several equivalent and heterovalent substitutions at the A site or B site of the ABO3 structure.

It has been observed that BNT-based compositions modified with BaTiO3, BiKTiO3, NaNbO3, BiFeO3, La2O3, Sc2O3, BaCO3, etc., show improved performance and are easily polarized.

The substitution of Zr in the B site enhances the relative ion displacement and electrical properties through the expansion of the perovskite lattice. It can also be seen that the substitution of Zr suppresses the desired conduction of electrons in the oxidation states of Ti4 and Ti3.

Adding Gd to the Bi site will cause distortion, and it is an amphoteric dopant. Therefore, it is possible to use this material as a photovoltaic cell.

Bismuth Magnesium Titanate (Bi (Mg0.5Ti0.5) O3) [BMT] is a rhombohedral ferroelectric perovskite, similar to bismuth sodium titanate (Bi0.5Na0.5) TiO3 [BNT] ceramics. In order to improve the ferroelectric and piezoelectric properties, the researchers studied the effect of magnesium dopants as additives. It has been concluded that the rhombohedral structure is maintained to x = 0.04 mole fraction and becomes a cubic phase at higher mole fractions.

A new group of compounds (Bi0.5Na0.5) TiO3-(Bi0.5(1 x) Na0.5) TiO3-0.75x was used to study the piezoelectric and thermal depolarization properties of bismuth sodium titanate ceramics. The ratio of assumed and measured density exceeds 97%. As Bi increases or Na decreases in BNT, the resistivity increases.

Researchers studied another interesting BNT-based ceramic (1-x) NBT-xBT. The intermediate coexistence of the structural phase transition and the homomorphic phase boundary (MPB) using XRD and Raman spectroscopy has been reported. All ferroelectric and dielectric properties are listed in Table 1.

Table 1. Features of NBT-BT system. Source: Kuanar et al., 2021

The influence of a small amount (2.0 wt.%) of Ba2 ions on the substitution of A and B positions in BNT was studied. As the frequency increases, the dielectric constant drops rapidly. The dielectric loss decreases as the frequency increases.

(1-x) Bi0.5Na0.5TiO3-xSr0.85Bi0.1TiO3 ceramic at 1260 °C and most importantly, the PE circuit is hysteresis-free, which shows that it is a material suitable for high-precision actuator applications.

When x is close to 0.06-0.08, the presence of MPB is shown in Figure 2, reflecting the binary system phase (1-x) Bi1/2Na1/2TiO3-x BaTiO3 (BNT-BT). Based on the piezoelectric enhancement properties, the presence of MPB becomes apparent in the composition.

Figure 2. The isotropic phase boundary in BNT-BT. Image credit: Kuanar et al., 2021

Researchers have further studied the dielectric and ferroelectric properties of BNT-BT-xBZT (0≤x(BZT)≤0.10). They synthesized ceramics through traditional solid-state reaction methods.

They also confirmed that the rhombohedral and tetragonal phases of all samples coexist, and that the tetragonal phase increases with the increase in the amount of BZT. Table 2 lists the dielectric constant (εr), dielectric loss (tanδ), phase transition temperature (TFA), residual polarization (ps) and coercive field (Ec) values.

Table 2. Characteristics of the BNT-BT-xBZT system. Source: Kuanar et al., 2021

The effect of BiFeO3 on the electrical and electrochemical properties and structure (microstructure) of the BNT-BKTx-BFy ternary system is shown in Table 3. The doped BF diffuses into the BNT-BKT lattice to form a solid solution, but the reduction of tetragonal and rhombohedral distortion has a great impact on performance, so it is a good piezoelectric material.

Table 3. Characteristics of the BNT-BKTx-BFy system. Source: Kuanar et al., 2021

The researchers also studied the same phase boundary in the BNT-BKT-BT system, as shown in Figure 3. As the amount of BKT and BT increases, the dielectric constant values ​​of all compositions increase. The ternary mixture, that is, 0.865 BNT–0.035 BT–0.100 BKT isomorphic composition shows a high electromechanical coupling factor (kp = 0.26 and kt = 0.57) piezoelectric constant (d33 = 133 pC/N), which confirms a good pressure Electrical performance, as shown in table 4.

Figure 3. The directional phase boundary of the BNT-BKT-BT system. Image credit: Kuanar et al., 2021

Table 4. Characteristics of BNT-BKT-BT content. Source: Kuanar et al., 2021

The influence of NiNb2O6 content on the dielectric properties and structure of the BT-BNT system was observed. The results show that the doping of NiNb2O6 can inhibit grain growth. Initially, the dielectric constant increases and then decreases at low temperatures. The Curie temperature increases slightly with the doping concentration.

For samples doped with 1.5 mol.% NiNb2O6, they showed excellent dielectric properties at room temperature, with a dielectric constant value of 1652, and dielectric loss values ​​found in different documents, as described in Table 5.

Table 5. Some characteristics of BNT-based solid solution systems. Source: Kuanar et al., 2021

Lead-free ferroelectric ceramic oxides have been widely used in modern technology due to their high dielectric constant, piezoelectric coefficient, large remanent polarization, low coercivity and high Curie temperature, and can replace the widely used lead Based ceramics, because they have a pollution-free ecological environment. -Friendly nature. However, these ferroelectric oxides have serious polarization problems.

Due to its high coercivity and high conductivity, PZT is ahead of BNT in industrial applications. For this reason, the researchers intend to develop new lead-free ferroelectric oxides with characteristics suitable for multifunctional applications in a wide range of temperature and frequency.

A new type of application of this material is a photostrictive actuator, which is the combined result of the photovoltaic effect and the piezoelectric effect. One of the applications of piezoelectric composites is piezoelectric transducers. These ceramic-polymer composite materials have a wide range of applications in the fields of hydrophones, sensors and medical ultrasound.

Researchers have been studying many dopants in bismuth sodium titanate ceramics to solve industrial needs, and it is expected that smart and very smart materials will be developed in the future for a wide range of applications.

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