Crystallographic texture engineering through templated grain growth (TGG) has gained prominence as a highly effective strategy for optimizing the electromechanical performance of lead-free piezoelectric ceramics, offering a pathway toward sustainable alternatives to lead-based systems like lead zirconate titanate (PZT). By achieving high degrees of texture, with Lotgering factors (LFs) often exceeding 90%, these systems have demonstrated piezoelectric properties that rival or even surpass their lead-based counterparts. Despite these advancements, the field lacks a comprehensive understanding of how specific template parameters influence the texture quality and functional properties across different material systems. This review provides an in-depth analysis of the influence of the template morphology, composition, and crystallographic orientation on the texturing of key lead-free systems, including BaTiO₃ (BT), (K_0.5Na_0.5)NbO₃ (KNN), and Bi_0.5Na_0.5TiO₃ (BNT). Furthermore, it explores how the template selection affects the induced crystallographic direction, and how this impacts the material’s phase structure and domain configurations, ultimately influencing the piezoelectric and dielectric properties. By consolidating the existing knowledge and identifying current challenges, this work highlights key strategies for optimizing the texture and electromechanical performance in lead-free ceramics, providing essential insights for future research aimed at advancing high-performance, environmentally friendly piezoelectric materials for applications such as sensors, actuators, and energy-harvesting devices.

Durable, high‐performance, and environmentally friendly lead‐free piezoceramics are essential for next‐generation sustainable energy transducers and electromechanical systems. However, piezoceramics are mechanically weak, which negatively impacts their working conditions and durability. A solution to improve their mechanical durability without sacrificing piezoelectric performance remains elusive. Here, we design a bioinspired brick‐and‐mortar Bi _0.5 Na _0.5 TiO ₃ (BNT) ceramics with BNT bricks and silica mortar. This deliberate microstructure design yields a 2.8‐fold, from 104 to 294 MPa, increase in strength and 2‐fold, from 0.9 to 1.8 MPa·m ^0.5 , increase in fracture toughness compared with conventional BNT without sacrificing piezoelectric performance. These improvements translate into a 110‐fold increase in ferroelectric fatigue lifetime and a 37% higher voltage output and slower degradation as energy transducers. These gains originate from anisotropic residual stress fields, revealed by Raman and XRD, which delay crack initiation events. Given its microstructural origin, this strategy is broadly applicable to other systems where both functional and structural performance are critical.

Molten salt synthesis (MSS) is a versatile route for fabricating anisotropic microcrystals used to prepare textured ceramics, but its widespread use is constrained by excessive salt consumption and the accumulation of massive waste streams. Here, we introduce a circular MSS strategy that eliminates these inefficiencies by enabling recycling of both salt and precursors. Using the two-step synthesis of BaTiO3 platelike templates as a model, we demonstrate direct recovery and reuse of the NaCl/KCl from the first-step MSS of Bi4Ti3O12 templates, together with a new chemical pathway for reclaiming bismuth from the by-products of the second-step MSS of BaTiO3 platelike templates. The recycled inputs yield BaTiO3 templates that are structurally and morphologically identical to those produced from fresh reagents, while cutting waste generation by closing the materials loop. This work establishes MSS as a sustainable, closed-loop process, advancing a circular economy framework that couples high-quality anisotropic microcrystal synthesis with drastic waste minimization.

Compounds and solid solutions of bismuth ferrite (BiFeO₃)—barium titanate (BaTiO₃) system are of great scientific and engineering interest as multiferroic and potential high-temperature lead-free piezoelectric materials. In the present paper, the results of research on the synthesis and characterisation of 0.67Bi₁.₀₂FeO₃–0.33BaTiO₃ (67BFBT) ceramics in terms of crystal structure and dielectric and piezoelectric properties are reported. It was found that the produced 67BFBT ceramics were characterised by a tetragonal crystal structure described by the P4mm space group, an average crystallite size <D> ≈ 80 nm, and an average strain <ε> = 0.01%. Broad-band dielectric spectroscopy (BBDS) was employed to characterise the dielectric response of polycrystalline ceramics. The frequency range from ν = 10⁻¹ Hz to ν = 10⁵ Hz was used to characterise the influence of the electric field strength on dielectric response of the ceramic sample at room temperature. The dielectric spectra were checked for consistency with the Kramers–Kronig test, and the high quality of the measurements were confirmed. The electric equivalent circuit method was used to fit the dielectric spectra within the frequency range that corresponded to the occurrence of the resonant spectra of the radial mode for thin disk sample, i.e., from ν = 10⁵ Hz to ν = 10⁷ Hz and the temperature range from T = −20 °C to T = 50 °C. The electric equivalent circuit [R_sCPE₁([L₁R₁C₁]C₀)] was used, and good fitting quality was reached. The relevant calculations were performed, and it was found that the piezoelectric charge coefficient exhibited a value of d₃₁ = 35 pC/N and the planar coupling factor was k_p = 31% at room temperature. Analysis of impedance spectra performed in terms of circumferential magnetic field made it possible to establish an influence of magnetic field on piezoelectric parameters of 67BFBT multiferroic ceramics. Additionally, the “magnetic” tunability of the modulus of the complex dielectric permittivity makes 67BFBT a sensing material with vast potential.