Enhanced electromechanical performance of Si-modified lead-free BiFeO3-BaTiO3 ceramics for high-temperature piezoelectric applications

Hussein Alrobei; Muhammad Habib; Shoaib Ali; Rizwan Ahmed Malik; Muhammad Javid Iqbal; Qamar Iqbal; Fadl A. Essa; Z.M. Omara

doi:10.1371/journal.pone.0318768

Abstract

Environmental pollution generated by industrial wastes are deteriorating land, water, and marine life, which raises major concerns about climate change. Since environmentally friendly piezoelectric materials can generate clean energy by applying mechanical forces, they are seen as viable agents for industrial applications. In recent research work, the Si-modified 0.70Bi_1.03FeO₃-0.30BaTiO₃ (BF30BT) environmentally friendly piezoceramics were synthesized using a solid-state method followed by a thermal quenching process. The crystalline structure, microstructure, and electromechanical characteristics were explored as a function of Si for both dopants (BC; before calcination) and additives (AC; after calcination). The result of pure BF30BT ceramic reveals a dominant rhombohedral phase exhibiting a d₃₃ of 251 pC/N with a higher T_C of 560 °C. The Si-doping gradually transformed the predominant rhombohedral phase to the rhombohedral-tetragonal mixed phase asymmetry as a result a good balance was achieved among d₃₃ (209 pC/N), Q_m (32.6), and k_p (0.32%) with a high T_C (465 °C). A giant-induced electric field bipolar strain of 0.39% corresponding to a large-signal piezoelectric coefficient d₃₃^* ≈ 750 pm/V was perceived in Si-doped BF30BT ceramic. The defect dipoles by acceptor doping play an essential role in the enhancement of piezoelectricity. The defect dipole aligns in the spontaneous polarization and also offers restoring force for domain switching leading to high asymmetric electrostrain. This study provides a good design benchmark for a new generation of eco-friendly large-strain actuator piezoceramics.

Figures

Citation: Alrobei H, Habib M, Ali S, Malik RA, Iqbal MJ, Iqbal Q, et al. (2025) Enhanced electromechanical performance of Si-modified lead-free BiFeO₃-BaTiO₃ ceramics for high-temperature piezoelectric applications. PLoS ONE 20(3): e0318768. https://doi.org/10.1371/journal.pone.0318768

Editor: Azim Uddin, Zhejiang University, CHINA

Received: August 31, 2024; Accepted: January 22, 2025; Published: March 7, 2025

Copyright: © 2025 Alrobei et al. This is an open access article distributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

Data Availability: All relevant data are within the paper and its Supporting Information files.

Funding: This project is sponsored by Prince Sattam Bin Abdulaziz University (PSAU) as part of funding for its SDG Roadmap Research Funding programme project number PSAU-2023-SDG-2023/SDG/114.

Competing interests: The authors have declared that no competing interests exist.

1. Introduction

The concept of piezoelectric materials is the interconversion of mechanical stress and electrical voltage [1]. Piezoelectric ceramics are now widely used in electromechanical devices owing to their rapid response. The potential applications of high electrostrain piezoceramic materials are presented schematically in Fig 1. In general, piezoelectric materials can be categorized into two types such as lead-based and lead-free piezoceramics. Lead-based (Pb Zr_1-xTi_x O₃, PZT) piezoelectric materials dominate the commercial market due to their superior piezoelectric performance and easily modifiable electric characteristics with simple fabrication. However, the high amount of lead (more than 60%) in the solid solution is a massive concern for the environment and human health. Therefore, significant attention has been devoted to materials, such as (Bi_0.5Na_0.5)TiO₃ (BNT), (K_0.5Na_0.5)NbO₃ (KNN), BaTiO₃ BiFeO₃ materials [2–4]. BNT-based materials reflect superior strain performance (0.4% – 0.7%) among these lead-free piezoelectric materials [5,6]. Unfortunately, the BNT piezoelectric ceramics possess high strain hysteresis (70%), low depolarization temperature ( < 120 °C), and a high electric field (80-100 kV/cm) is required for large electrostrain [7].

Download:

Fig 1. The potential applications of ultrahigh electrostrain piezoceramic materials and their preferred devices.

https://doi.org/10.1371/journal.pone.0318768.g001

Now for real applications high strain under the low electric field is a significant challenge. Saito achieved a high piezoelectric constant(d₃₃*) of 750 pm/V in textured ceramics under an ultralow electric field of 20 kV/cm [8]. However, the texturing process is complicated and expensive for mass production. Furthermore, a significant recoverable electro-strain 0.75% with d₃₃^* of 3700 pm/V has been reported in the Fe³⁺-acceptor-doped BaTiO₃ single crystals, utilizing the defect dipoles [9]. However, many parameters are required during the synthesis of a single crystal and also the large strain hysteresis (80%) of this work restricts their use for practical applications. Additionally, the BaTiO₃ shows lower T_C and limits its use for high-temperature applications. Recently, the solid solution of BiFeO₃-BaTiO₃ (BF-BT) ceramics have gained papularity due to their good piezoelectric performance and high T_C ≥ 450 °C [10]. However, the high leakage current and secondary phase formation in the BiFeO₃-based material restrict its potential properties.

Many approaches have been adopted for the enhancement of electromechanical performance such as phase boundary engineering and local structure inhomogeneity or polar nano regions [11]. Defect dipole engineering is a novel material design strategy for high electrostrain performance. Recently ultrahigh electric field-induced strain of over 1% has been achieved in the acceptor-doped KNN-based [12,13]. Therefore, in this work, a new composition of acceptor doping is designed according to the chemical formula 0.7Bi_1.03FeO₃-0.3BaTi_1-xSi_xO₃, where the Si²⁺ substitution on Ti⁴⁺ induces oxygen vacancy. This oxygen vacancy creates a defect dipole with A-site or B-site cation vacancy and the one-way round trip to this defect dipole under the bipolar applied field induces high asymmetric strain. The electromechanical properties of the lead-free piezoelectric BF-BT system are schematically studied as given in the schematic diagram of Fig 2.

Download:

Fig 2. The functional properties of lead-free piezoelectric BiFeO₃-BaTiO₃ ceramic and desired parameters.

https://doi.org/10.1371/journal.pone.0318768.g002

2. Experimental procedure

2.1. Raw materials

The raw powders of the oxides and carbonates, such as Bi₂O₃ (99.99%, Sigma Aldrich), Si₂O₃ (99.99%, Alfa Aesar), Fe₂O₃ (≥ 99.99%, Sigma Aldrich), BaCO₃ (≥ 99.99%, Sigma Aldrich) and TiO₂ (≥ 99.95%, Sigma Aldrich) were used.

2.2. Material synthesis

A typical solid-state reaction technique was used to fabricate lead-free 0.70Bi_1.03FeO₃-0.30BaTi_1-xSi_xO₃ ceramics with x = 0.00, 0.005(BC), 0.01(BC), 0.01(AC), where BC and AC show the addition of Si₂O₃ mol% powder before and after calcination, respectively. The 3mol% Bi₂O₃ excess powder was added for their compensation at high temperatures. The initial reagents were thoroughly mixed and ball-milled for 24 h in ethanol. Then, this slurry was dried at 120°C for 6 h and then calcined at 700 °C for 2 h at a heating rate of 10 °C/min. The calcined powder was re-milled for 6 hours to achieve chemical homogeneity. The 5 wt % polyvinyl alcohol (PVA) was added with calcinated powder and dried at 120 °C for at least 6 h. The dried powder was hand-grind by using a mortar and pestle. These crushed powders were passed from 100 µm mash and then, pressed into disk-shaped pellets with a ~10 mm diameter. To prevent Bi₂O₃ from volatilizing during the sintering process, pellets were buried in the same structural powder. Initially, the binder (PVA) was removed at 300°C for 1 h and then all samples were sintered for 3 h at a temperature of 980-1000 °C. All ceramics were immediately quenched in water to avoid the unstable temperature range and suppress non-ferroelectric secondary phases. The samples were polished to a thickness of 400 μm and silver paste was coated on both sides of the pellets and dried at 100 °C.

2.3 Characterization

X-ray diffraction (XRD, Bruker, D8 Advance) was used to examine the crystalline structures of the sintered samples. An impedance analyzer (HP4194A, Agilent) connected with a computer-programmed furnace system was used to find out the dielectric properties. The ceramics were poled in the silicone oil bath under 50 kV/cm for 30 min and their d₃₃ values were measured by using the d₃₃-meter (IACAS, ZJ-6B). A ferroelectric measuring device (aixACCT System GmbH 1000, Germany) used an electric field of 50 kV/cm to measure the ferroelectric and piezoelectric properties. The resonance-antiresonance measurements were made using an Agilent 4294A precision impedance analyzer to calculate mechanical quality factor (Q_m) and planar electromechanical coupling coefficient (k_p) (Hewlett-Packard, Palo Alto, CA).

3. Results and discussion

Fig 3(a) shows the XRD patterns for BF30BT sintered ceramics at ambient temperature in the 2θ range of 10° − 80° with x = 0.00(BC), 0.005(BC), 0.01(BC), 0.01(AC). All compositions demonstrate a single perovskite structure, indicating the formation of a stable solid solution. This indicates that the Si³⁺ ion has completely diffused in the BF30BT lattice and has led to a stable solid solution with a pure phase structure. In the rhombohedral (R) unit cell, the direction of polarization is (111), and for the tetragonal (T), it is either (100) or (200). The splitting of the (200) and (111) peaks allows the identification of the T and R phases [14,15]. Therefore, the magnified view of the (111) and (200) diffraction peaks are shown in Fig 3(b). A slight shift of the peak toward the lower angle is due to the larger ionic radius of Si³⁺ than the Ti⁴⁺ ion. The doublet (111)/(11) peaks and a single (200) peak for undoped BF30BT indicating the predominance of R symmetry. However, after Si-doping the (11) and (111) peaks gradually merged, suggesting the R+T mixed phase symmetry. On the other hand, for 0.01(AC) a distinct splitting can be observed near 39° suggesting that Si₂O₃ addition before calcination is more effective as compared to after calcination Si-doping. The MPB between the R and T phases was also previously reported for the BF-BT ceramics [16,17].

Download:

Fig 3. (a) The X-ray diffraction patterns in the suggested range of 2θ = 10° − 60°, (b) magnified view for (111) peak at 2θ = 38° − 40° and (200) peak at 2θ = 38° − 40°, and (c, d) XRD Rietveld refinements patterns of x = 0.00(BC), 0.01(BC) samples for Si-modified BF30BT solid solutions.

https://doi.org/10.1371/journal.pone.0318768.g003

To analyze the exact crystal structure Rietveld refinement was performed for BF30BT and 0.01(BC) samples as shown in Fig 3(c, d). In the previous investigation of BF-BT solid solution the R3c and P4mm mixed-phase model have been applied. Therefore, in this work, a biphasic model (R3c and P4mm) was used during the refinement method which shows the best goodness of fit (χ²) values. The rhombohedral lattice constant a_R = 4.0100 Å was deduced from the hexagonal unit cell indirectly. The tetragonal lattice constant a_T = 3.9956 Å and c_T = 4.0171 Å, with tetragonality c_T/a_T = 1.005 was found for pure BF30BT ceramic. By Si-doping with x = 0.01, a_R = 4.0117 Å, a_T = 3.9894 Å, c_T = 4.0222 Å, and c_T/a_T = 1.012 were found. This large lattice distortion plays a significant role in the enhancement of piezoelectricity [18]. Therefore, the coexistence of R and T phases with the largest lattice distortion in BF30BTSi ceramic leads to a high piezoelectric response.

Fig 4(a-d) depicts the the ferroelectric polarization-electric field (P−E) hysteresis loops of the BF30BT ceramic with various Si³⁺ concentrations under the 55 kV/cm applied electric field at 10 Hz. Each loop is well-saturated and symmetrical, with sharp loop corners. The pure sample exhibits a hard P−E hysteresis loop, confirming the ferroelectric nature of BF30BT ceramics, and is associated with domain-wall pinning [19] resulting from the defects. The addition of Si has a considerable impact on the contour of the P−E loops and the polarization response of the BFBT system. At 0.00 ≤ x ≤ 0.005(BC), typical ferroelectric polarization hysteresis loops were identified as x increased, demonstrating that adequate Si concentrations can increase domain-wall pinning and improve ferroelectric characteristics. When the applied electric field is removed, the ferroelectric phase’s long-range order maintains its polarization. Therefore, the pure BF30BT ceramic displayed the remnant polarization (P_r) of 16.75 μC/cm² and saturation polarization (P_s) of 22.7 μC/cm². The introduction of small amount of Si in to BF30BT ceramics slightly increased ferroelectric response and showed the highest P_r of 21.9 μC/cm² and P_S of 29.3 μC/cm² for x = 0.01(AC) near MBP composition.

Download:

Fig 4. (a-d) Ferroelectric polarization (P − E) hysteresis loops for Si-doped BF30BT ceramics.

https://doi.org/10.1371/journal.pone.0318768.g004

In order to investiage the effect of aceeptor doping on the defect chemistry and origin of high piezoelectric performance the bipolar piezoelectric strain-electric field (S−E) curves were measured under the 50 kV/cm as shown in Fig 5(a,b). Actually, the acceptor doping are induces for charge balance and form defect dipoles [20]. Recently, asymmetric S−E loops with a large strain were achieved in the lead-free ceramics by creating defect dipole [21,22]. For the sample Si-doping before calcination the maximum electrostrain (S_max) value of 0.39% is achtived at 50 kV/cm for the 0.5(BC) as shown in Fig 5c. The activation energy of hopping (about 1 eV) is substantially larger than the activation energy of domain barriers (roughly 0.1 eV) [4]. The one way trip of this defect dipole unfer the bipolar electric field produces asymmetric S−E hysteresis loop [12]. Fig 5(d) illustrates the computed d₃₃* values as a function of the Si concentration. A highest of 750 pm/V was achieved for x = 0.01(BC) composition which exceeds to reported lead-free ceramics and many lead-free BF-BT ceramics and equivalent to KNN-textured materials as shown Fig 5(e). More detailed is given in Table 1 for comparasion the piezoelectric strain response under the applied electric field and its working temperature range.

Download:

Table 1. Summary of applied field (E_a), Curie temperature (T_C) and dynamic piezoelectric constant (d₃₃^*) and comparasion with other piezoelectric ceramics.

https://doi.org/10.1371/journal.pone.0318768.t001

Download:

Fig 5. (a, b) Butterfly bipolar strain-electric field (S − E) curves recorded under an applied electric field of 50 kV/cm, (c) maximum strain (S_max), and (d) d₃₃, d₃₃^* of BF30BT ceramic as a function of Si^3 + concentration. (e) Nd-doped BF30BT [23], BF40BT-BiM_2/3Nb_1/3O₃ (BF40BT-BMN)[57], Sm-doped BF30BT (BSmF30BT) [24], Nb-doped BF33BT (BF33BTNb) [1], BF35BT [58], Zr-doped BF33BT (BF33BZrT) [14], BFBT-BiScO₃ [28], Zr-doped BF36BT [30], LiNbO₃-BF33BT (BF33BT-LN) [31], Ba-site Sm-doped BF33BT (BF33BSmT) [59], Bi-site BF33BT (BSmF33BT) [60], PZT and KNN-textured [8].

https://doi.org/10.1371/journal.pone.0318768.g005

This significant increase in bipolar strain may be ascribed to the phase transition from ferroelectrics to relaxor ferroelectrics and defect-dipole. The negative strain (S_neg) indicates the non-180° reorientation of domains, and positive strain is the sum of intrinsic piezoelectric lattice strain and extrinsic reversible domain switching strain [47]. A dramatic decrease occurred in the |−S_neg| ≈ 0.18% of the pure BF30BT to 0.01% for Si-doped ceramic at x = 0.03(AC). This low S_neg value shows a decrease in hard ferroelectric behavior with Si-acceptor doping. The higher piezoelectric strain performance for the optimum composition may be attributed to the dominating relaxor phase, dominance of extrinsic contribution from the reversible electric field-induced phase shit and defect-dipole induced asymmetric strain [2,3,48]. Nevertheless, the bipolar S−E curves change into sprout-shaped curves and the S_neg value decreases to 0.01 percent at x = 0.03(AC). With Si-doping the drop in S_neg values provides evidence for the relaxor ferroelectric effect. Therefore, the Si-addition before calcination is a more effective way to the improvement of electromechanical performance as compared to the after calcination. In the current study, slight asymmetry in the polarization hysteresis loops were also observed, although less pronounced than the strain hysteresis loops. This difference may arise because the electrostrain and the polarization hysteresis loops were recorded under different frequencies. Its further indicates that asymmetric behavior is more pronounced at lower frequencies. This behavior also hints towards the presence of defect structures in the investigated compositions. These defect structures reconfigure more slowly under the applied field as compared to domain polarization reversal. This phenomenon is in good agreement with previously reported work [49].

Fig 6(a-c) displays the frequency dependence impedance |Z| and phase angle (θ) of poled samples. According to the impedance spectra, the samples exhibit a resonance frequency of around (290–304) kHz. Fig 6(d) illustrates the mechanical quality factor Q_m and electromechanical coupling factor k_p calculated from their corresponding spectra. At resonance and anti-resonance frequencies, the impedance curves exhibit abrupt variations. These characteristics are consistent with observations for other hard piezoelectric ceramics [50]. The phase angle shift for the BF30BT ceramics was low, about 30.5°, but rose with increasing Si content to approach 50.7° for x = 0.005(BC)-0.01(BC). The higher θ value suggested that the substitution of Si³⁺ ions for Ti⁴⁺ ions resulted in a perfect poling state, which improved dielectric performance. The optimal poling condition is reached when θ approaches 90° in the frequency range between the resonance and anti-resonance frequencies. With increasing frequency, a perfect piezoelectric material exhibits a phase angle change from −90° to 90° during resonance and anti-resonance [50].

Download:

Fig 6. (a-c) Frequency characteristics of | Z | and θ of x = 0.005(BC), 0.01(BC), 0.01(AC), and (d) piezoelectric properties of Q_m and K_p as a function of Si concentration for BF30BT ceramics.

https://doi.org/10.1371/journal.pone.0318768.g006

As the concentration of Si increased from 0.00 to 0.005(BC) wt%, the values of k_p increased dramatically from 0.295 to 0.325 then decreased to 0.27 at x = 0.01(AC) as can be seen in Fig 6(d). It can be explained that as Si₂O₃ is doped at x = 0.01(AC), the grain size decreases, the domain wall is pinched or clamped by more grain boundaries, and the domain is difficult to reverse by electric field, resulting in low k_p value. As x increases from 0.005(BC) to 0.01(BC), it can be seen that the k_p increases from 0.29 percent to 0.32 percent. For x = 0.01(BC), yields the highest k_p = 0.32% ascribing to the phase structure MPB [51]. For x = 0.005(BC), yields the highest Q_m (32.6) and a higher Q_m suggests suppression of domain wall motion. Because the acceptor doping creates oxygen vacancy or defect dipoles that can occupy energetically favored lattice locations. These anisotropic centers induce an internal bias field and pinning or clamping of the domain wall motion that leads to high Q_m values [52–54]. The piezoelectric strain performance under the applied field and T_C of this work were compared with other piezoelectric ceramics in Table 1. A large d₃₃^* ≈ 750 pm/V under the 50 kV/cm with a high T_C ≈ 450 °C of this work, are fascinating results for high-temperature device applications.

Fig 7, the temperature-dependent dielectric constant (ε_r) for Si-doped BF30BT ceramics at 10 kHz and 100 kHz in the temperature range of 25°–600 °C. The pure BF30BT ceramic illustrates typical ferroelectric behavior and exhibits a very sharp peak with T_C ≈ 560 °C [Fig 7(a)]. The Si-doping in BF30BT ceramics induces an additional dielectric peak near 350-450 °C as shown in Fig 7(b, c). This anomaly is related to the compositional heterogeneity or defect charges migration at high temperatures [5]. Both anomalies are seen on the dielectric constant curves, one at depolarization temperature (T_d), and the other at the dielectric maximum temperature (T_max). The Si fusion lowers T_d to ambient temperature but does not affect T_max. In addition, the dielectric constant peak at T_max is reduced and flattened in ceramics with a larger Si content. Similar dielectric anomalies are seen in Mn-doped BF-BT ceramics [55]. However, the wide/broad transition peak can be observed for 0.01(AC) suggesting the relaxor ferroelectrics behavior [Fig 7(d)]. The weak peaks can be attributed to oxygen tilting or the presence of defects in these ceramics. With the addition of Si content, the maximum dielectric constant declines fast and the T_m peaks become exceedingly broad. Furthermore, the T_d peaks slowly disappear as the Si content increases, indicating that T_d has been relocated below room temperature. As disorder arises, the material’s structure becomes inhomogeneous, resulting in a better range of local conditions for the dipoles. This leads to a larger temperature range for dipole alignment, obscuring the dielectric constant peak. In classical ferroelectrics, peaks in the real component of the dielectric constant are sharp and do not move to higher temperatures as frequency increases because ferroelectric phase transition is well-defined and nearly frequency-independent. However, if the T_d peaks gradually disappear as the Si content increases, it means that T_d has been shifted below room temperature. The decrease in T_d caused by Si modification confirms the compositionally induced ferroelectric-relaxor transition. This behavior is typical of a relaxor, in which the peak broadens and changes due to the presence of high local disorder and weak dynamics in polar nanoregions.

Download:

Fig 7. (a-d) Temperature-dependent dielectric constant (ε_r) from room temperature to 600 °C, (e) tanδ from room temperature to 200 °C, and (f) room temperature tanδ for Si-doped BF30BT ceramics.

https://doi.org/10.1371/journal.pone.0318768.g007

As shown in Fig 7(e) for all compositions the dielectric losses gradually decrease up to ≈ 100 °C and then substantially increase at the higher temperature. It also showed that the small amount of Si₂O₃ additive had little effect on the dielectric loss of BF30BT ceramics, making it appropriate for high-power applications. The room temperature dielectric losses of the pure BF30BT ceramic dramatically decrease from 0.065 to 0.043 for x = 0.01(BC) and again raised to tanδ ≈ 0.095 for x = 0.01(AC) as shown in Fig 7(f). Tan losses are minor at 100 °C, but increase sharply at high temperatures, indicating an increase in DC conductivity. When the Si concentration of the BFBT was increased to x = 0.01(AC), the dielectric permittivity widened and the T_C fell down. The T_C is moved toward the lower temperature through the relation as T_C ≈ (K_L − K_S)/B, where K_L is the long-range electrostatic force constant, K_S is the short-range harmonic force constant and B is the inharmonic coefficient [15]. The Si doping in BFBT ceramics causes local structure heterogeneity, which suppresses long-range ferroelectric order, as a result of which a chemically induced phase change from the regular ferroelectric phase to the relaxor phase occurs. Normally, hard ferroelectric ceramics exhibited small dielectric losses as compared to their counterpart of soft-ferroelectric ceramics [56]. Hence, the dielectric properties further support that Si-addition before calcination induces a hard ferroelectric effect while after calcination it creates a soft ferroelectric effect. Furthermore, this increase in tanδ at high temperatures is mainly associated with long-range space charge conduction [33].

4. Conclusion

The existing investigation involved the fabrication of lead-free Si-modified 0.7Bi_1.03FeO₃-0.3BaTiO₃ piezoelectric ceramics by a conventional solid-state method, followed by thermal quenching. The XRD investigation reveals a structural phase transition caused by composition, going from a predominately rhombohedral to a mixed rhombohedral and tetragonal symmetry. The dielectric, ferroelectric and electric-strain properties of these doped BF30BT-based ceramics were studied. The current investigation shows the comparative study of Si addition before, and after calcination, where the Si-acceptor doping induces hard-ferroelectric behavior that improves the electromechanical performance. A large strain and dynamic piezoelectric coefficient d₃₃ * ~ 750 pm/V were achieved simultaneously in a single critical composition at x = 0.01(BC). A new step forward in piezoelectric material exploration and actuation has been made possible by the outstanding electromechanical properties of lead-free ceramics. The currently investigated ceramics show significant progress in lead-free piezoelectric actuators and sensors for high-temperature applications.

Supporting information

S1 File.

S1 Fig. This is the schematic figure. The potential applications of ultrahigh electrostrain piezoceramic materials and their preferred devices. S2 Fig. This is the schematic figure. The functional properties of lead-free piezoelectric BiFeO3-BaTiO3 ceramic and desired parameters. S3 Fig. Data set for Fig. 3 (a) The X-ray diffraction patterns in the suggested range of 2θ = 10° − 60°, (b) magnified view for (111) peak at 2θ = 38° − 40° and (200) peak at 2θ = 38° − 40°, and (c, d) XRD Rietveld refinements patterns of x = 0.00(BC), 0.01(BC) samples for Si-modified BF30BT solid solutions. S4 Fig. Data set for Fig. 4 (a-d) Ferroelectric polarization (P−E) hysteresis loops for Si-doped BF30BT ceramics. S5 Fig. Data set for Fig. 5 (a, b) Butterfly bipolar strain-electric field (S−E) curves recorded under an applied electric field of 50 kV/cm, (c) maximum strain (S_max), and (d) d₃₃, d₃₃^* of BF30BT ceramic as a function of Si³⁺ concentration. (e) Nd-doped BF30BT [23], BF40BT-BiM_2/3Nb_1/3O₃ (BF40BT-BMN)[57], Sm-doped BF30BT (BSmF30BT) [24], Nb-doped BF33BT (BF33BTNb) [1], BF35BT [58], Zr-doped BF33BT (BF33BZrT) [14], BFBT-BiScO₃ [28], Zr-doped BF36BT [30], LiNbO3-BF33BT (BF33BT-LN) [31], Ba-site Sm-doped BF33BT (BF33BSmT) [59], Bi-site BF33BT (BSmF33BT) [60], PZT and KNN-textured [8]. S6 Fig. Data set for Fig 6(a-c) Frequency characteristics of | Z | and θ of x = 0.005(BC), 0.01(BC), 0.01(AC), and (d) piezoelectric properties of Q_m and K_p as a function of Si concentration for BF30BT ceramics. S7 Fig. Data set for Fig. 7 Fig. 7: (a-d) Temperature-dependent dielectric constant (ε_r) from room temperature to 600 °C, (e) tanδ from room temperature to 200 °C, and (f) room temperature tanδ for Si-doped BF30BT ceramics.

https://doi.org/10.1371/journal.pone.0318768.s001

(XLSX)

References

1. Iqbal Q, Habib M, Alzaid M, Ahmad P, Khan MT. Synergistic approach for enhancement of piezoelectricity in the lead-free BiFeO₃-BaTiO₃ ceramics. J Alloy Compd. 2023;947169414.
- View Article
- Google Scholar
2. Lv X, Wang X, Ma Y, Zhang X-x, Wu J. Temperature stability of perovskite-structured lead-free piezoceramics: Evaluation methods, improvement strategies, and future perspectives. Materials Science and Engineering: R: Reports. 2024;159:100793.
- View Article
- Google Scholar
3. Hao J, Li W, Zhai J, Chen H. Progress in high-strain perovskite piezoelectric ceramics. Mater Sci Eng R Rep. 2019;135:1–57.
- View Article
- Google Scholar
4. Zhou X, Xue G, Luo H, Bowen C, Zhang D. Phase structure and properties of sodium bismuth titanate lead-free piezoelectric ceramics. Prog Mater Sci. 2021;122(1):100836.
- View Article
- Google Scholar
5. Habib M, Munir M, Khan S, Song T, Kim M-H. Evaluation of high strain response in lead-free BNBTFS-xNb ceramics by structure and ferroelectric characterizations. J Phys Chem Solids. 2020;138:109230.
- View Article
- Google Scholar
6. Liu X, Tan X. Giant Strains in Non-Textured (Bi_1/2Na_1/2)TiO₃ -Based Lead-Free Ceramics. Adv Mater. 2016;28(3):574–8. pmid:26596685
- View Article
- PubMed/NCBI
- Google Scholar
7. Rödel J, Webber KG, Dittmer R, Jo W, Kimura M, Damjanciv D. Transferring lead-free piezoelectric ceramics into application. J Eur Ceram Soc. 2015;35:1659–81.
- View Article
- Google Scholar
8. Saito Y, Takao H, Tani T, Nonoyama T, Takatori K, Homma T, et al. Lead-free piezoceramics. Nature. 2004;432(7013):84–7. pmid:15516921
- View Article
- PubMed/NCBI
- Google Scholar
9. Ren X. Large electric-field-induced strain in ferroelectric crystals by point-defect-mediated reversible domain switching. Nat Mater. 2004;3(2):91–4. pmid:14716304
- View Article
- PubMed/NCBI
- Google Scholar
10. Lee MH, Kim DJ, Choi HI, Kim MH, Song TK. Low sintering temperature for lead-free BiFeO₃-BaTiO₃ ceramics with high piezoelectric performance. J Am Ceram Soc. 2018;102:2666–74.
- View Article
- Google Scholar
11. Zheng T, Wu H, Yuan Y, Lv X, Li Q, Men T, et al. The structural origin of enhanced piezoelectric performance and stability in lead free ceramics. Energy Environ Sci. 2017;10:528–37.
- View Article
- Google Scholar
12. Huangfu G, Zeng K, Wang B, Wang J, Fu Z, Xu F, et al. Giant electric field-induced strain in lead-free piezoceramics. Science. 2022;378(6624):1125–30. pmid:36480626
- View Article
- PubMed/NCBI
- Google Scholar
13. Wang B, Huangfu G, Wang J, Li H, Guo Y. Defect dipole‐induced fatigue strain recoverability in lead‐free piezoelectric ceramics. Adv Funct Materials. 2023;33(45):2306416.
- View Article
- Google Scholar
14. Habib M, Iqbal MJ, Lee MH, Kim DJ, Akram F, Gul M, et al. Piezoelectric performance of Zr-modified lead-free BiFeO₃-BaTiO₃ ceramics. Mater Res Bull. 2022;146:111571.
- View Article
- Google Scholar
15. Habib M, Lee MH, Kim DJ, Akram F, Choi HI, Kim M-H, et al. Phase diagram for Bi-site La-doped BiFeO₃BaTiO₃ lead-free piezoelectric ceramics. J Materiomics. 2021;7(1):40–50.
- View Article
- Google Scholar
16. Wang Z, Huangfu G, Xiao H, Guo Y. Excellent thermal stability and enhanced piezoelectric performance of Bi(Ni_2/3Nb_1/3)O₃‐modified BiFeO₃–BaTiO₃ ceramics. J Am Ceram Soc. 2021;105(1):317–26.
- View Article
- Google Scholar
17. Khan SA, Ahmed T, Park HW, Habib M, Song TK, Wang C, et al. Effects of B- and A/B-sites Codoping on lattice distortion and defect concentration for high electromechanical response of lead-free piezoelectrics. Acta Materialia. 2024;278:120262.
- View Article
- Google Scholar
18. Habib M, Lee MH, Kim DJ, Choi HI, Kim M-H, Kim W-J, et al. Phase evolution and origin of the high piezoelectric properties in lead-free BiFeO₃–BaTiO₃ ceramics. Ceram Int. 2020;46(14):22239–52.
- View Article
- Google Scholar
19. Ahart M, Somayazulu M, Cohen RE, Ganesh P, Dera P, Mao H, et al. Origin of morphotropic phase boundaries in ferroelectrics. Nature. 2008;451(7178):545–8. pmid:18235495
- View Article
- PubMed/NCBI
- Google Scholar
20. Feng Y, Wu J, Chi Q, Li W, Yu Y, Fei W. Defects and aliovalent doping engineering in electroceramics. Chem Rev. 2020;120(3):1710–87. pmid:31899631
- View Article
- PubMed/NCBI
- Google Scholar
21. Wang B, Huangfu G, Zheng Z, Guo Y. Giant electric field‐induced strain with high temperature‐stability in textured KNN‐based piezoceramics for actuator applications. Adv Funct Mater. 2023;33:2214643.
- View Article
- Google Scholar
22. Lai L, Li B, Tian S, Zhao Z, Zhang S. Giant electrostrain in lead‐free textured piezoceramics by defect dipole design. Adv Mater. 2023;35(23):2300519.
- View Article
- Google Scholar
23. Wang D, Khesro A, Murakami S, Feteira A, Zhao Q, et al. Temperature dependent, large electromechanical strain in Nd-doped BiFeO₃-BaTiO₃ lead-free ceramics. J Eur Ceram Soc. 2017;37(1):1857–60.
- View Article
- Google Scholar
24. Ma Z, Li G, Sun B, He L, Gao W, Sun Q, et al. Enhanced electric-field-induced strain in 0.7Bi_(1−x)Sm_xFeO₃–0.3BaTiO₃ lead-free ceramics. J Mater Sci. 2020;55(19):8134–44.
- View Article
- Google Scholar
25. Xun B, Song A, Yu J, Yin Y, Li J-F, Zhang B-P. Lead-free BiFeO₃-BaTiO₃ ceramics with high curie temperature: fine compositional tuning across the phase boundary for high piezoelectric charge and strain coefficients. ACS Appl Mater Interfaces. 2021;13(3):4192–202. pmid:33438390
- View Article
- PubMed/NCBI
- Google Scholar
26. Wang D, Fan Z, Li W, Zhou D, Feteira A, Wang G, et al. High energy storage density and large strain in Bi(Zn_2/3Nb_1/3)O₃-doped BiFeO₃–BaTiO₃ ceramics. ACS Appl Energy Mater. 2018;1(8):4403–12.
- View Article
- Google Scholar
27. Habib M, Lee M, Akram F, Kim M-H, Kim W-J. Temperature-insensitive piezoelectric properties of lead-free BiFeO₃–BaTiO₃ ceramics with high Curie temperature. J Alloys Compd. 2020;851:156788.
- View Article
- Google Scholar
28. Murakami S, Ahmed NTAF, Wang D, Feteira A, Sinclair DC, Raney IM. Optimising dopants and properties in BiMeO₃ (Me= Al, Ga, Sc, Y, Mg_2/3Nb_1/3, Zn_2/3Nb_1/3, Zn_1/2Ti_1/2) lead-free BaTiO₃-BiFeO₃ based ceramics for actuator applications. J Eur Ceram Socety. 2018;38:4220–31.
- View Article
- Google Scholar
29. Lee MH, Kim DJ, Choi HI, Kim M-H, Song TK, Kim W-J. Thermal quenching effects on the ferroelectric and piezoelectric properties of BiFeO₃-BaTiO₃ ceramics. ACS App Electron Mater. 2019;1:1772–80.
- View Article
- Google Scholar
30. Fu D, Ning Z, Hu D, Cheng J, Wang F. Large and temperature-insensitive piezoelectric strain in xBiFeO₃-(1-x)Ba(Zr_0.05Ti_0.95)O₃ lead-free piezoelectric ceramics. J Mater Sci. 2019;54:1153–61.
- View Article
- Google Scholar
31. Malik RA, Hussain A, Song TK, Kim W-J, Ahmed R, Sung YS, et al. Enhanced electromechanical properties of (1-x)BiFeO₃-BaTiO₃-xLiNbO₃ ceramics by quenching process. Ceram Int. 2017;43(5):198–203.
- View Article
- Google Scholar
32. Murakami S, Wang D, Mostaed A, Khesro A, Feteira A, Sinclair DC, et al. High strain (0.4%) Bi(Mg_2/3Nb_1/3)O₃‐BaTiO₃‐BiFeO₃ lead-free piezoelectric ceramics and multilayers. J Am Ceram Soc. 2018;101:5428–42.
- View Article
- Google Scholar
33. Habib M, Tang L, Xue G, Zhou X, Zhang D. Improvement in piezoelectric performance of the lead-free BiFeO₃-BaTiO₃ ceramics by synergistic approach. J Mater Sci Technol. 2023;160:55–65.
- View Article
- Google Scholar
34. Ryu G-H, Hussain A, Lee M-H, Malik R, Song T. Lead-free high performance Bi(Zn_0.5Ti_0.5)O₃-modified BiFeO₃-BaTiO₃ piezoceramics. J Eur Ceram Soc. 2018;34:4414–21.
- View Article
- Google Scholar
35. Chen J, Daniels JE, Jian J, Cheng Z, Cheng J, Wang J, et al. Origin of large electric-field-induced strain in pseudo-cubic BiFeO₃–BaTiO₃ ceramics. Acta Materialia. 2020;197:1–9.
- View Article
- Google Scholar
36. Liu X, Zhai J, Shen B. Novel bismuth ferrite-based lead-free incipient piezoceramics with high electromechanical response. J Mater Chem C. 2019;7(17):5122–30.
- View Article
- Google Scholar
37. Wang K, Yao F, Jo W, Gobeljic D, Shvartsman VV, Lupascu DC, et al. Temperature‐Insensitive (K,Na)NbO₃‐Based Lead‐Free Piezoactuator Ceramics. Adv Funct Materials. 2013;23(33):4079–86.
- View Article
- Google Scholar
38. Lv X, Wu J, Xiao D, Zhu J, Zhang J, Zhang X. modifying temperature stability of (K,Na)NbO₃ ceramics through phase boundary. Adv Elect Materials. 2018;4(9):1800205.
- View Article
- Google Scholar
39. Zhang M-H, Wang K, Zhou J-S, Zhou J-J, Chu X, Lv X, et al. Thermally stable piezoelectric properties of (K,Na)NbO₃-based lead-free perovskite with rhombohedral-tetragonal coexisting phase. Acta Materialia. 2017;122344–51.
- View Article
- Google Scholar
40. Zhang M-H, Wang K, Du Y-J, Dai G, Sun W, Li G, et al. High and Temperature-Insensitive Piezoelectric Strain in Alkali Niobate Lead-free Perovskite. J Am Chem Soc. 2017;139(10):3889–95. pmid:28233999
- View Article
- PubMed/NCBI
- Google Scholar
41. Zhou J-S, Wang K, Yao F-Z, Zheng T, Wu J, Xiao D, et al. Multi-scale thermal stability of niobate-based lead-free piezoceramics with large piezoelectricity. J Mater Chem C. 2015;3(34):8780–7.
- View Article
- Google Scholar
42. Chen K, Ma J, Shi C, Wu W, Wu B. Enhanced temperature stability in high piezoelectric performance of (K, Na)NbO₃-based lead-free ceramics trough co-doped antimony and tantalum. J Alloys Compd. 2021;852:156865.
- View Article
- Google Scholar
43. Shi C, Ma J, Wu J, Wang X, Miao F, Huang Y, et al. Coexistence of excellent piezoelectric performance and high Curie temperature in KNN-based lead-free piezoelectric ceramics. J Alloys Compd. 2020;846:156245.
- View Article
- Google Scholar
44. Liu Q, Zhang Y, Gao J, Zhou Z, Wang H, et al. High-performance lead-free piezoelectrics with local structural heterogeneity. Energy Environ Sci. 2018;11:3531–9.
- View Article
- Google Scholar
45. Chen M, Yao X, Zhang L. Grain size dependence of dielectric and field-induced strain properties of chemical prepared (Pb, La)(Zr, Sn, Ti)O₃ antiferroelectric ceramics. Ceram Int. n.d.;28:201–7.
- View Article
- Google Scholar
46. Pathak A, Prakash C, Chatterjee R. Shape memory effect in PZST system at exact morphotropic phase boundary. Physica B: Condensed Matter. 2009;404(20):3457–61.
- View Article
- Google Scholar
47. Qi H, Zuo R, Fu J, Dou M. Thermally stable electrostrains of morphotropic 0.875NaNbO₃-0.1BaTiO₃-0.025CaZrO₃ lead-free piezoelectric ceramics. Appl Phys Lett. 2017;110(11):112903.
- View Article
- Google Scholar
48. Zhao Z, Lv Y, Dai Y, Zhang S. Ultrahigh electro-strain in acceptor-doped KNN lead-free piezoelectric ceramics via defect engineering. Acta Materialia. 2020;200:35–41.
- View Article
- Google Scholar
49. Li W, Zhou C, Wang J, Yuan C, Xu J, Li Q, et al. Giant electro-strain nearly 1% in BiFeO₃-based lead-free piezoelectric ceramics through coupling morphotropic phase boundary with defect engineering. Mater Today Chem. 2022;26:101237.
- View Article
- Google Scholar
50. Hong C-H, Kim H-P, Choi B-Y, Han H-S, Son JS, Ahn CW, et al. Lead-free piezoceramics–Where to move on?. J Materiomics. 2016;2(1):1–24.
- View Article
- Google Scholar
51. Damjanovic D. Contributions to the piezoelectric effect in ferroelectric single crystals and ceramics. J Am Ceram Soc. 2005;88:2663–76.
- View Article
- Google Scholar
52. Cheng Y, Fan W, Chen H, Xie L, Xing J, Tan Z, et al. Hardening Effect in Lead-Free KNN-Based Piezoelectric Ceramics with CuO Doping. ACS Appl Mater Interfaces. 2022;14(50):55803–11. pmid:36482677
- View Article
- PubMed/NCBI
- Google Scholar
53. Waqar M, Wu H, Chen J, Yao K, Wang J. Evolution from lead-based to lead-free piezoelectrics: engineering of lattices, domains, boundaries, and defects leading to giant response. Adv Mater. 2022;34(25):e2106845. pmid:34799944
- View Article
- PubMed/NCBI
- Google Scholar
54. Liu YX, Qu W, Thong HC, Zhang Y, Zhang Y, Yao FZ, et al. Isolated‐Oxygen‐vacancy hardening in lead‐free piezoelectrics. Adv Mater. 2022;34(29):e2202558. pmid:35593489
- View Article
- PubMed/NCBI
- Google Scholar
55. Calisir I, Hall DA. Chemical heterogeneity and approaches to its control in BiFeO3–BaTiO3 lead-free ferroelectrics. J Mater Chem C. 2018;6(1):134–46.
- View Article
- Google Scholar
56. Chou X, Zhai J, Jiang H, Yao X. Dielectric properties and relaxor behavior of rare-earth (La, Sm, Eu, Dy, Y) substituted barium zirconium titanate ceramics. J Appl Phys. 2007;102:084106.
- View Article
- Google Scholar
57. Li C, Xue H, Zheng T, Wu J. An exploration for new strategy: Achieving both excellent temperature stability and good electrostrain in BiFeO₃–BaTiO₃-based relaxor ferroelectrics by domain engineering. Mater Today Phys. 2022;27:100747.
- View Article
- Google Scholar
58. Zheng T, Wu J. Perovskite BiFeO₃–BaTiO₃ ferroelectrics: engineering properties by domain evolution and thermal depolarization modification. Adv Electron Mater. 2020;6:2000079.
- View Article
- Google Scholar
59. Habib M, Zhou X, Tang L, Xue G, Rahman A, Akram F, et al. Enhancement of Piezoelectricity by Novel Poling Method of the Rare‐Earth Modified BiFeO₃–BaTiO₃ Lead‐Free Ceramics. Adv Elect Mater. 2023;9(5):2201210.
- View Article
- Google Scholar
60. Habib M, Akram F, Ahmad P, Kebaili I, Rahman A, Din IU, et al. Ultrahigh piezoelectric strain in lead-free BiFeO₃-BaTiO₃ ceramics at elevated temperature. J Alloys Compd. 2022;919:165744.
- View Article
- Google Scholar

[ref1] 1. Iqbal Q, Habib M, Alzaid M, Ahmad P, Khan MT. Synergistic approach for enhancement of piezoelectricity in the lead-free BiFeO₃-BaTiO₃ ceramics. J Alloy Compd. 2023;947169414.
View Article
Google Scholar

[2] View Article

[3] Google Scholar

[ref2] 2. Lv X, Wang X, Ma Y, Zhang X-x, Wu J. Temperature stability of perovskite-structured lead-free piezoceramics: Evaluation methods, improvement strategies, and future perspectives. Materials Science and Engineering: R: Reports. 2024;159:100793.
View Article
Google Scholar

[5] View Article

[6] Google Scholar

[ref3] 3. Hao J, Li W, Zhai J, Chen H. Progress in high-strain perovskite piezoelectric ceramics. Mater Sci Eng R Rep. 2019;135:1–57.
View Article
Google Scholar

[8] View Article

[9] Google Scholar

[ref4] 4. Zhou X, Xue G, Luo H, Bowen C, Zhang D. Phase structure and properties of sodium bismuth titanate lead-free piezoelectric ceramics. Prog Mater Sci. 2021;122(1):100836.
View Article
Google Scholar

[11] View Article

[12] Google Scholar

[ref5] 5. Habib M, Munir M, Khan S, Song T, Kim M-H. Evaluation of high strain response in lead-free BNBTFS-xNb ceramics by structure and ferroelectric characterizations. J Phys Chem Solids. 2020;138:109230.
View Article
Google Scholar

[14] View Article

[15] Google Scholar

[ref6] 6. Liu X, Tan X. Giant Strains in Non-Textured (Bi_1/2Na_1/2)TiO₃ -Based Lead-Free Ceramics. Adv Mater. 2016;28(3):574–8. pmid:26596685
View Article
PubMed/NCBI
Google Scholar

[17] View Article

[18] PubMed/NCBI

[19] Google Scholar

[ref7] 7. Rödel J, Webber KG, Dittmer R, Jo W, Kimura M, Damjanciv D. Transferring lead-free piezoelectric ceramics into application. J Eur Ceram Soc. 2015;35:1659–81.
View Article
Google Scholar

[21] View Article

[22] Google Scholar

[ref8] 8. Saito Y, Takao H, Tani T, Nonoyama T, Takatori K, Homma T, et al. Lead-free piezoceramics. Nature. 2004;432(7013):84–7. pmid:15516921
View Article
PubMed/NCBI
Google Scholar

[24] View Article

[25] PubMed/NCBI

[26] Google Scholar

[ref9] 9. Ren X. Large electric-field-induced strain in ferroelectric crystals by point-defect-mediated reversible domain switching. Nat Mater. 2004;3(2):91–4. pmid:14716304
View Article
PubMed/NCBI
Google Scholar

[28] View Article

[29] PubMed/NCBI

[30] Google Scholar

[ref10] 10. Lee MH, Kim DJ, Choi HI, Kim MH, Song TK. Low sintering temperature for lead-free BiFeO₃-BaTiO₃ ceramics with high piezoelectric performance. J Am Ceram Soc. 2018;102:2666–74.
View Article
Google Scholar

[32] View Article

[33] Google Scholar

[ref11] 11. Zheng T, Wu H, Yuan Y, Lv X, Li Q, Men T, et al. The structural origin of enhanced piezoelectric performance and stability in lead free ceramics. Energy Environ Sci. 2017;10:528–37.
View Article
Google Scholar

[35] View Article

[36] Google Scholar

[ref12] 12. Huangfu G, Zeng K, Wang B, Wang J, Fu Z, Xu F, et al. Giant electric field-induced strain in lead-free piezoceramics. Science. 2022;378(6624):1125–30. pmid:36480626
View Article
PubMed/NCBI
Google Scholar

[38] View Article

[39] PubMed/NCBI

[40] Google Scholar

[ref13] 13. Wang B, Huangfu G, Wang J, Li H, Guo Y. Defect dipole‐induced fatigue strain recoverability in lead‐free piezoelectric ceramics. Adv Funct Materials. 2023;33(45):2306416.
View Article
Google Scholar

[42] View Article

[43] Google Scholar

[ref14] 14. Habib M, Iqbal MJ, Lee MH, Kim DJ, Akram F, Gul M, et al. Piezoelectric performance of Zr-modified lead-free BiFeO₃-BaTiO₃ ceramics. Mater Res Bull. 2022;146:111571.
View Article
Google Scholar

[45] View Article

[46] Google Scholar

[ref15] 15. Habib M, Lee MH, Kim DJ, Akram F, Choi HI, Kim M-H, et al. Phase diagram for Bi-site La-doped BiFeO₃BaTiO₃ lead-free piezoelectric ceramics. J Materiomics. 2021;7(1):40–50.
View Article
Google Scholar

[48] View Article

[49] Google Scholar

[ref16] 16. Wang Z, Huangfu G, Xiao H, Guo Y. Excellent thermal stability and enhanced piezoelectric performance of Bi(Ni_2/3Nb_1/3)O₃‐modified BiFeO₃–BaTiO₃ ceramics. J Am Ceram Soc. 2021;105(1):317–26.
View Article
Google Scholar

[51] View Article

[52] Google Scholar

[ref17] 17. Khan SA, Ahmed T, Park HW, Habib M, Song TK, Wang C, et al. Effects of B- and A/B-sites Codoping on lattice distortion and defect concentration for high electromechanical response of lead-free piezoelectrics. Acta Materialia. 2024;278:120262.
View Article
Google Scholar

[54] View Article

[55] Google Scholar

[ref18] 18. Habib M, Lee MH, Kim DJ, Choi HI, Kim M-H, Kim W-J, et al. Phase evolution and origin of the high piezoelectric properties in lead-free BiFeO₃–BaTiO₃ ceramics. Ceram Int. 2020;46(14):22239–52.
View Article
Google Scholar

[57] View Article

[58] Google Scholar

[ref19] 19. Ahart M, Somayazulu M, Cohen RE, Ganesh P, Dera P, Mao H, et al. Origin of morphotropic phase boundaries in ferroelectrics. Nature. 2008;451(7178):545–8. pmid:18235495
View Article
PubMed/NCBI
Google Scholar

[60] View Article

[61] PubMed/NCBI

[62] Google Scholar

[ref20] 20. Feng Y, Wu J, Chi Q, Li W, Yu Y, Fei W. Defects and aliovalent doping engineering in electroceramics. Chem Rev. 2020;120(3):1710–87. pmid:31899631
View Article
PubMed/NCBI
Google Scholar

[64] View Article

[65] PubMed/NCBI

[66] Google Scholar

[ref21] 21. Wang B, Huangfu G, Zheng Z, Guo Y. Giant electric field‐induced strain with high temperature‐stability in textured KNN‐based piezoceramics for actuator applications. Adv Funct Mater. 2023;33:2214643.
View Article
Google Scholar

[68] View Article

[69] Google Scholar

[ref22] 22. Lai L, Li B, Tian S, Zhao Z, Zhang S. Giant electrostrain in lead‐free textured piezoceramics by defect dipole design. Adv Mater. 2023;35(23):2300519.
View Article
Google Scholar

[71] View Article

[72] Google Scholar

[ref23] 23. Wang D, Khesro A, Murakami S, Feteira A, Zhao Q, et al. Temperature dependent, large electromechanical strain in Nd-doped BiFeO₃-BaTiO₃ lead-free ceramics. J Eur Ceram Soc. 2017;37(1):1857–60.
View Article
Google Scholar

[74] View Article

[75] Google Scholar

[ref24] 24. Ma Z, Li G, Sun B, He L, Gao W, Sun Q, et al. Enhanced electric-field-induced strain in 0.7Bi_(1−x)Sm_xFeO₃–0.3BaTiO₃ lead-free ceramics. J Mater Sci. 2020;55(19):8134–44.
View Article
Google Scholar

[77] View Article

[78] Google Scholar

[ref25] 25. Xun B, Song A, Yu J, Yin Y, Li J-F, Zhang B-P. Lead-free BiFeO₃-BaTiO₃ ceramics with high curie temperature: fine compositional tuning across the phase boundary for high piezoelectric charge and strain coefficients. ACS Appl Mater Interfaces. 2021;13(3):4192–202. pmid:33438390
View Article
PubMed/NCBI
Google Scholar

[80] View Article

[81] PubMed/NCBI

[82] Google Scholar

[ref26] 26. Wang D, Fan Z, Li W, Zhou D, Feteira A, Wang G, et al. High energy storage density and large strain in Bi(Zn_2/3Nb_1/3)O₃-doped BiFeO₃–BaTiO₃ ceramics. ACS Appl Energy Mater. 2018;1(8):4403–12.
View Article
Google Scholar

[84] View Article

[85] Google Scholar

[ref27] 27. Habib M, Lee M, Akram F, Kim M-H, Kim W-J. Temperature-insensitive piezoelectric properties of lead-free BiFeO₃–BaTiO₃ ceramics with high Curie temperature. J Alloys Compd. 2020;851:156788.
View Article
Google Scholar

[87] View Article

[88] Google Scholar

[ref28] 28. Murakami S, Ahmed NTAF, Wang D, Feteira A, Sinclair DC, Raney IM. Optimising dopants and properties in BiMeO₃ (Me= Al, Ga, Sc, Y, Mg_2/3Nb_1/3, Zn_2/3Nb_1/3, Zn_1/2Ti_1/2) lead-free BaTiO₃-BiFeO₃ based ceramics for actuator applications. J Eur Ceram Socety. 2018;38:4220–31.
View Article
Google Scholar

[90] View Article

[91] Google Scholar

[ref29] 29. Lee MH, Kim DJ, Choi HI, Kim M-H, Song TK, Kim W-J. Thermal quenching effects on the ferroelectric and piezoelectric properties of BiFeO₃-BaTiO₃ ceramics. ACS App Electron Mater. 2019;1:1772–80.
View Article
Google Scholar

[93] View Article

[94] Google Scholar

[ref30] 30. Fu D, Ning Z, Hu D, Cheng J, Wang F. Large and temperature-insensitive piezoelectric strain in xBiFeO₃-(1-x)Ba(Zr_0.05Ti_0.95)O₃ lead-free piezoelectric ceramics. J Mater Sci. 2019;54:1153–61.
View Article
Google Scholar

[96] View Article

[97] Google Scholar

[ref31] 31. Malik RA, Hussain A, Song TK, Kim W-J, Ahmed R, Sung YS, et al. Enhanced electromechanical properties of (1-x)BiFeO₃-BaTiO₃-xLiNbO₃ ceramics by quenching process. Ceram Int. 2017;43(5):198–203.
View Article
Google Scholar

[99] View Article

[100] Google Scholar

[ref32] 32. Murakami S, Wang D, Mostaed A, Khesro A, Feteira A, Sinclair DC, et al. High strain (0.4%) Bi(Mg_2/3Nb_1/3)O₃‐BaTiO₃‐BiFeO₃ lead-free piezoelectric ceramics and multilayers. J Am Ceram Soc. 2018;101:5428–42.
View Article
Google Scholar

[102] View Article

[103] Google Scholar

[ref33] 33. Habib M, Tang L, Xue G, Zhou X, Zhang D. Improvement in piezoelectric performance of the lead-free BiFeO₃-BaTiO₃ ceramics by synergistic approach. J Mater Sci Technol. 2023;160:55–65.
View Article
Google Scholar

[105] View Article

[106] Google Scholar

[ref34] 34. Ryu G-H, Hussain A, Lee M-H, Malik R, Song T. Lead-free high performance Bi(Zn_0.5Ti_0.5)O₃-modified BiFeO₃-BaTiO₃ piezoceramics. J Eur Ceram Soc. 2018;34:4414–21.
View Article
Google Scholar

[108] View Article

[109] Google Scholar

[ref35] 35. Chen J, Daniels JE, Jian J, Cheng Z, Cheng J, Wang J, et al. Origin of large electric-field-induced strain in pseudo-cubic BiFeO₃–BaTiO₃ ceramics. Acta Materialia. 2020;197:1–9.
View Article
Google Scholar

[111] View Article

[112] Google Scholar

[ref36] 36. Liu X, Zhai J, Shen B. Novel bismuth ferrite-based lead-free incipient piezoceramics with high electromechanical response. J Mater Chem C. 2019;7(17):5122–30.
View Article
Google Scholar

[114] View Article

[115] Google Scholar

[ref37] 37. Wang K, Yao F, Jo W, Gobeljic D, Shvartsman VV, Lupascu DC, et al. Temperature‐Insensitive (K,Na)NbO₃‐Based Lead‐Free Piezoactuator Ceramics. Adv Funct Materials. 2013;23(33):4079–86.
View Article
Google Scholar

[117] View Article

[118] Google Scholar

[ref38] 38. Lv X, Wu J, Xiao D, Zhu J, Zhang J, Zhang X. modifying temperature stability of (K,Na)NbO₃ ceramics through phase boundary. Adv Elect Materials. 2018;4(9):1800205.
View Article
Google Scholar

[120] View Article

[121] Google Scholar

[ref39] 39. Zhang M-H, Wang K, Zhou J-S, Zhou J-J, Chu X, Lv X, et al. Thermally stable piezoelectric properties of (K,Na)NbO₃-based lead-free perovskite with rhombohedral-tetragonal coexisting phase. Acta Materialia. 2017;122344–51.
View Article
Google Scholar

[123] View Article

[124] Google Scholar

[ref40] 40. Zhang M-H, Wang K, Du Y-J, Dai G, Sun W, Li G, et al. High and Temperature-Insensitive Piezoelectric Strain in Alkali Niobate Lead-free Perovskite. J Am Chem Soc. 2017;139(10):3889–95. pmid:28233999
View Article
PubMed/NCBI
Google Scholar

[126] View Article

[127] PubMed/NCBI

[128] Google Scholar

[ref41] 41. Zhou J-S, Wang K, Yao F-Z, Zheng T, Wu J, Xiao D, et al. Multi-scale thermal stability of niobate-based lead-free piezoceramics with large piezoelectricity. J Mater Chem C. 2015;3(34):8780–7.
View Article
Google Scholar

[130] View Article

[131] Google Scholar

[ref42] 42. Chen K, Ma J, Shi C, Wu W, Wu B. Enhanced temperature stability in high piezoelectric performance of (K, Na)NbO₃-based lead-free ceramics trough co-doped antimony and tantalum. J Alloys Compd. 2021;852:156865.
View Article
Google Scholar

[133] View Article

[134] Google Scholar

[ref43] 43. Shi C, Ma J, Wu J, Wang X, Miao F, Huang Y, et al. Coexistence of excellent piezoelectric performance and high Curie temperature in KNN-based lead-free piezoelectric ceramics. J Alloys Compd. 2020;846:156245.
View Article
Google Scholar

[136] View Article

[137] Google Scholar

[ref44] 44. Liu Q, Zhang Y, Gao J, Zhou Z, Wang H, et al. High-performance lead-free piezoelectrics with local structural heterogeneity. Energy Environ Sci. 2018;11:3531–9.
View Article
Google Scholar

[139] View Article

[140] Google Scholar

[ref45] 45. Chen M, Yao X, Zhang L. Grain size dependence of dielectric and field-induced strain properties of chemical prepared (Pb, La)(Zr, Sn, Ti)O₃ antiferroelectric ceramics. Ceram Int. n.d.;28:201–7.
View Article
Google Scholar

[142] View Article

[143] Google Scholar

[ref46] 46. Pathak A, Prakash C, Chatterjee R. Shape memory effect in PZST system at exact morphotropic phase boundary. Physica B: Condensed Matter. 2009;404(20):3457–61.
View Article
Google Scholar

[145] View Article

[146] Google Scholar

[ref47] 47. Qi H, Zuo R, Fu J, Dou M. Thermally stable electrostrains of morphotropic 0.875NaNbO₃-0.1BaTiO₃-0.025CaZrO₃ lead-free piezoelectric ceramics. Appl Phys Lett. 2017;110(11):112903.
View Article
Google Scholar

[148] View Article

[149] Google Scholar

[ref48] 48. Zhao Z, Lv Y, Dai Y, Zhang S. Ultrahigh electro-strain in acceptor-doped KNN lead-free piezoelectric ceramics via defect engineering. Acta Materialia. 2020;200:35–41.
View Article
Google Scholar

[151] View Article

[152] Google Scholar

[ref49] 49. Li W, Zhou C, Wang J, Yuan C, Xu J, Li Q, et al. Giant electro-strain nearly 1% in BiFeO₃-based lead-free piezoelectric ceramics through coupling morphotropic phase boundary with defect engineering. Mater Today Chem. 2022;26:101237.
View Article
Google Scholar

[154] View Article

[155] Google Scholar

[ref50] 50. Hong C-H, Kim H-P, Choi B-Y, Han H-S, Son JS, Ahn CW, et al. Lead-free piezoceramics–Where to move on?. J Materiomics. 2016;2(1):1–24.
View Article
Google Scholar

[157] View Article

[158] Google Scholar

[ref51] 51. Damjanovic D. Contributions to the piezoelectric effect in ferroelectric single crystals and ceramics. J Am Ceram Soc. 2005;88:2663–76.
View Article
Google Scholar

[160] View Article

[161] Google Scholar

[ref52] 52. Cheng Y, Fan W, Chen H, Xie L, Xing J, Tan Z, et al. Hardening Effect in Lead-Free KNN-Based Piezoelectric Ceramics with CuO Doping. ACS Appl Mater Interfaces. 2022;14(50):55803–11. pmid:36482677
View Article
PubMed/NCBI
Google Scholar

[163] View Article

[164] PubMed/NCBI

[165] Google Scholar

[ref53] 53. Waqar M, Wu H, Chen J, Yao K, Wang J. Evolution from lead-based to lead-free piezoelectrics: engineering of lattices, domains, boundaries, and defects leading to giant response. Adv Mater. 2022;34(25):e2106845. pmid:34799944
View Article
PubMed/NCBI
Google Scholar

[167] View Article

[168] PubMed/NCBI

[169] Google Scholar

[ref54] 54. Liu YX, Qu W, Thong HC, Zhang Y, Zhang Y, Yao FZ, et al. Isolated‐Oxygen‐vacancy hardening in lead‐free piezoelectrics. Adv Mater. 2022;34(29):e2202558. pmid:35593489
View Article
PubMed/NCBI
Google Scholar

[171] View Article

[172] PubMed/NCBI

[173] Google Scholar

[ref55] 55. Calisir I, Hall DA. Chemical heterogeneity and approaches to its control in BiFeO3–BaTiO3 lead-free ferroelectrics. J Mater Chem C. 2018;6(1):134–46.
View Article
Google Scholar

[175] View Article

[176] Google Scholar

[ref56] 56. Chou X, Zhai J, Jiang H, Yao X. Dielectric properties and relaxor behavior of rare-earth (La, Sm, Eu, Dy, Y) substituted barium zirconium titanate ceramics. J Appl Phys. 2007;102:084106.
View Article
Google Scholar

[178] View Article

[179] Google Scholar

[ref57] 57. Li C, Xue H, Zheng T, Wu J. An exploration for new strategy: Achieving both excellent temperature stability and good electrostrain in BiFeO₃–BaTiO₃-based relaxor ferroelectrics by domain engineering. Mater Today Phys. 2022;27:100747.
View Article
Google Scholar

[181] View Article

[182] Google Scholar

[ref58] 58. Zheng T, Wu J. Perovskite BiFeO₃–BaTiO₃ ferroelectrics: engineering properties by domain evolution and thermal depolarization modification. Adv Electron Mater. 2020;6:2000079.
View Article
Google Scholar

[184] View Article

[185] Google Scholar

[ref59] 59. Habib M, Zhou X, Tang L, Xue G, Rahman A, Akram F, et al. Enhancement of Piezoelectricity by Novel Poling Method of the Rare‐Earth Modified BiFeO₃–BaTiO₃ Lead‐Free Ceramics. Adv Elect Mater. 2023;9(5):2201210.
View Article
Google Scholar

[187] View Article

[188] Google Scholar

[ref60] 60. Habib M, Akram F, Ahmad P, Kebaili I, Rahman A, Din IU, et al. Ultrahigh piezoelectric strain in lead-free BiFeO₃-BaTiO₃ ceramics at elevated temperature. J Alloys Compd. 2022;919:165744.
View Article
Google Scholar

[190] View Article

[191] Google Scholar

Abstract

Figures

1. Introduction

2. Experimental procedure

2.1. Raw materials

2.2. Material synthesis

2.3 Characterization

3. Results and discussion

4. Conclusion

Supporting information

S1 File.

References

Cookie Preference Center

Customize Your Cookie Preference