Graphical Abstract
![](https://wqketang.oss-cn-beijing.aliyuncs.com/zip-unzip/zip-07389c6c-0d8b-4feb-9265-34aaef963b71/jmat-9-3-464/files/jmat-9-3-464-FE1.jpg?Expires=1725757078&OSSAccessKeyId=STS.NT5eViCkqzTYdbfdqxMkjpyyq&Signature=joE5tKEM1AO3yrmfAPZ2L7JbLzs%3D&security-token=CAISywJ1q6Ft5B2yfSjIr5eALuzdrrRQzZayZkTXgHEtQeRGn7zSkzz2IHtKenhsBOsbtfk1mG5W5%2FgZlqJ9SptIAEfJa9d99MzUP%2FpFltCT1fau5Jko1beHewHKeTOZsebWZ%2BLmNqC%2FHt6md1HDkAJq3LL%2Bbk%2FMdle5MJqP%2B%2FUFB5ZtKWveVzddA8pMLQZPsdITMWCrVcygKRn3mGHdfiEK00he8TouufTinpHMskGA1Aell7Mvyt6vcsT%2BXa5FJ4xiVtq55utye5fa3TRYgxowr%2Fwo0v0YpGya5YzHXwcPskvdKZbo78UqLQlla6w%2BGqFJqvPxr%2Fp8t%2Fx5fWJKAezhVgs8cVM8JOjIqKOscIsiJsO71SmqFV55c8Fdm%2BgUooJVgIMhTnduUfAPJAGOxzJitP%2BUVGGphr60TEnBL4rB5MUctfzRp75SXVPUTzDnGoABjuNLcf76FQN6p3t%2BSlCg%2FxR5C72RIk78k%2BUi44L9ZBmFT6F8GV7aXA52D1Ps56knKF6PAnhRivwyTxgsolycBfvccb3t5jGJ24SgY0aYosAECutxAo7sJhSwlwZvGwGDZJsop1vGiZ8eN1MbtZeRRuMeaZ2I%2BQo%2BnVP6Cf%2F0pDsgAA%3D%3D)
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Morphotropic phase boundary (MPB) plays a key role in tuning piezoelectric responses of ferroelectric ceramics. Here, Bi0·5Na0·5TiO3 modified BiFeO3–BaTiO3 ternary solid solutions of 0.7BiFeO3-(0.3-x)BaTiO3-xBi0.5Na0·5TiO3 (referred to as BF-BT-xBNT, 0.00 ≤ x ≤ 0.04) were prepared for lead-free piezoelectrics. All the ceramics exhibit an MPB with coexisting rhombohedral (R) and tetragonal (T) phases, and the R/T phase ratio decreases upon increasing x. The increment of BNT promotes the grain growth, lowers the leakage current and Curie temperature (TC), and gradually drives the ferroelectric to relaxor transition. Because of the MPB with appropriate R/T phase ratio, increased grain size and density, and decreased leakage current, the well-balanced performance between d33 = 206 pC/N and TC = 488 ℃ is obtained in x = 0.01 case. In addition, the further enhanced in-situ d33 = 286–347 pC/N is obtained in BF-BT-xBNT ceramics along with the improved depolarization temperature Td from 280 to 312 ℃, showing a potential application for lead-free piezoceramics at high temperature.
Sterianou I, Sinclair D, Reaney I, Comyn T, Bell A. Investigation of high Curie temperature (1−x)BiSc1−yFeyO3–xPbTiO3 piezoelectric ceramics. J Appl Phys 2009;106:084107.
Chen J, Cheng J, Dong S. Review on high temperature piezoelectric ceramics and actuators based on BiScO3-PbTiO3 solid solutions. J Adv Dielectr 2014;4:1430002.
Li S, Zhao Z, Liu M, Liu X, Huang W, Sun S, Jiang Y, Liu Y, Zhang J, Zhang Z. Remarkably enhanced photocatalytic performance of Au/AgNbO3 heterostructures by coupling piezotronic with plasmonic effects. Nano Energy 2022;95:107031.
Chen Y, Zhu J, Xiao D, Qin B, Jiang Y. Bismuth-modified BiScO3–PbTiO3 piezoelectric ceramics with high Curie temperature. Mater Lett 2008;62:3567–9.
Hao X, Zhai J, Kong LB, Xu Z. A comprehensive review on the progress of lead zirconate-based antiferroelectric materials. Prog Mater Sci 2014;63:1–57.
Ma C, Zhou W, Chen G, Cheng J, Zhai Z, Tan W, Wang X, Wang X. Compositional dependent electric-field-induced photoluminescence modulation in Eu3+-doped (1-x)Na0.5Bi0·5TiO3-xCaTiO3 (x=0.07, 0.1) piezoelectric ceramics. J Lumin 2020:228.
Rödel J, Webber KG, Dittmer R, Jo W, Kimura M, Damjanovic D. Transferring lead-free piezoelectric ceramics into application. J Eur Ceram Soc 2015;35:1659–81.
Shrout TR, Zhang SJ. Lead-free piezoelectric ceramics: alternatives for PZT? J Electroceram 2007;19:113–26.
Li P, Fu Z, Wang F, Huan Y, Zhou Z, Zhai J, Shen B, Zhang S. High piezoelectricity and stable output in BaHfO3 and (Bi0.5Na0.5)ZrO3 modified (K0.5Na0.5)(Nb0.96Sb0.04)O3 textured ceramics. Acta Mater 2020;199:542–50.
Wang J, Neaton JB, Zheng H, Nagarajan V, Ogale SB, Liu B, Viehland D, Vaithyanathan V, Schlom DG, Waghmare UV, Spaldin NA, Rabe KM, Wuttig M, Ramesh R. Epitaxial BiFeO3 multiferroic thin film heterostructures. Science 2003;299:1719–22.
Neaton JB, Ederer C, Waghmare UV, Spaldin NA, Rabe KM. First-principles study of spontaneous polarization in multiferroic BiFeO3. Phys Rev B 2005;71:014113.
Nong YQ, Cheng S, Zhang BP, Zhao JT, Zhou CR, Rao GH, et al. Phase structure, electrical and luminescent properties of Eu-modified 0.93Bi0.5Na0.5TiO3-0.07BaTiO3 multifunctional ceramics. Ceram Int 2022;48:17481–8.
Liu W, Ren X. Large piezoelectric effect in Pb-free ceramics. Phys Rev Lett 2009;103:257602.
Wu J, Fan Z, Xiao D, Zhu J, Wang J. Multiferroic bismuth ferrite-based materials for multifunctional applications: ceramic bulks, thin films and nanostructures. Prog Mater Sci 2016;84:335–402.
Wei Y, Wang X, Zhu J, Wang X, Jia J, Damjanovic D. Dielectric, ferroelectric, and piezoelectric properties of BiFeO3–BaTiO3 ceramics. J Am Ceram Soc 2013;96.
Lee MH, Kim DJ, Choi HI, Kim M-H, Song TK, Kim W-J, Do D. Thermal quenching effects on the ferroelectric and piezoelectric properties of BiFeO3–BaTiO3 ceramics. ACS Appl Electron Mater 2019;1:1772–80.
Cheng S, Zhang B-P, Wang L-J, Yang T, Yuan C-L, Zhou C-R, Rao G-H, Yin Y. Enhanced piezoelectric and ferroelectric properties of tetragonal BiFeO3–BaTiO3 ceramics via tailoring sintering temperature and dwell time. J Mater Sci Mater Electron 2021;32:24496–506.
Cheng S, Zhang BP, Zhao L, Wang KK. Enhanced insulating and piezoelectric properties of BiFeO3-BaTiO3-Bi0.5Na0.5TiO3 ceramics with high Curie temperature. J Am Ceram Soc 2019;102:7355–65.
Emery S, Cheng C-J, Kan D, Rueckert F, Alpay S, Nagarajan V, Takeuchi I, Wells B. Phase coexistence near a morphotropic phase boundary in Sm-doped BiFeO3 films. Appl Phys Lett 2010;97:152902.
Lu Y-S, Dai JQ. Enhanced electrical properties of (Zn, Mn)-modified BiFeO3–BaTiO3 lead-free ceramics prepared via sol–gel method and two-step sintering. J Alloys Compd 2022:899.
Wei JF, Pu YP, Mao YQ, Wang JF. Effects of BNT addition on the microstructure and PTC properties of La-doped BaTiO3-based PTCR ceramics. Ferroelectrics 2010;403:91–6.
Fan QL, Zhou CR, Li QL, Xu JW, Yuan CL, Chen GH. Temperature stability of sodium-doped BiFeO3-BaTiO3 piezoelectric ceramics. J Mater Sci Mater Electron 2015;26:9336–41.
Zhang H, Liu W, Wu P, Hai X, Guo M, Xi X, Gao J, Wang X, Guo F, Xu X. Novel behaviors of multiferroic properties in Na-Doped BiFeO3 nanoparticles. Nanoscale 2014;6:10831–8.
Tamilselvan A, Balakumar S, Sakar M, Nayek C, Murugavel P, Kumar KS. Role of oxygen vacancy and Fe–O–Fe bond angle in compositional, magnetic, and dielectric relaxation on Eu-substituted BiFeO3 nanoparticles. Dalton Trans 2014;43:5731–8.
Soltani T, Lee BK. Improving heterogeneous photo-Fenton catalytic degradation of toluene under visible light irradiation through Ba-doping in BiFeO3 nanoparticles. J Mol Catal Chem 2016;425:199–207.
Wen X, Chen Z, Liu E, Lin X, Chen C. Effect of Ba and Mn doping on microstructure and multiferroic properties of BiFeO3 ceramics. J Alloys Compd 2016;678:511–7.
Miriyala N, Prashanthi K, Thundat T. Oxygen vacancy dominant strong visible photoluminescence from BiFeO3 nanotubes. Phys Status Solidi Rapid Res Lett 2013;7:668–71.
Kozakov A, Kochur A, Googlev K, Nikolsky A, Raevski I, Smotrakov V, Yeremkin V. X-ray photoelectron study of the valence state of iron in iron-containing single-crystal (BiFeO3, PbFe1/2Nb1/2O3), and ceramic (BaFe1/2Nb1/2O3) multiferroics. J Electron Spectrosc Relat Phenom 2011;184:16–23.
Xu D, Zhao W, Cao W, Li W, Fei W. Electrical properties of Li and Nb modified BiFeO3 ceramics with reduced leakage current. Ceram Int 2021;47:4217–25.
Cheng S, Zhang B-P, Zhao L, Wang K-K. Enhanced insulating and piezoelectric properties of 0.7BiFeO3–0.3BaTiO3 lead-free ceramics by optimizing calcination temperature: analysis of Bi3+ volatilization and phase structures. J Mater Chem C 2018;6:3982–9.
Gou XL, Bai YL, Zhao SF. K0.5Na0.5NbO3Bi4-xPrxTi3O12 relaxation ferroelectric capacitor with piezoelectric unit inserted into Bi4Ti3O12 matrix. J Alloys Compd 2021;869:7.
Wang T, Zhang HM, Huang YY, Chen JM, Gong WP. Improved energy storage density and efficiency in BaTiO3-BiFeO3- based relaxor-ferroelectric ceramics. J Alloys Compd 2022;920:10.
Xun B, Song A, Yu J, Yin Y, Li JF, Zhang BP. 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;13:4192–202.
Behera C, Choudhary RNP, Das PR. Structural and electrical properties of La-modified BiFeO3-BaTiO3 composites. J Mater Sci Mater Electron 2014;25:2086–95.
Tong K, Zhou CR, Li QN, Wang J, Yang L, Xu JW, Chen GH, Yuan CL, Rao GH. Enhanced piezoelectric response and high-temperature sensitivity by site-selected doping of BiFeO3-BaTiO3 ceramics. J Eur Ceram Soc 2018;38:1356–66.
Habib M, Lee MH, Akram F, Choi HI, Kim M-H, Kim W-J, Song TK. Phase diagram for Bi-site La-doped BiFeO3-BaTiO3 lead-free piezoelectric ceramics. J Materiomics 2021;7:40–50.
Habib M, Akram F, Ahmad P, Kebaili I, Rahman A, Din IU, Iqbal MJ, Zeb A, Khandaker MU, Karoui A, Kim M-H, Song TK. Ultrahigh piezoelectric strain in lead-free BiFeO3-BaTiO3 ceramics at elevated temperature. J Alloys Compd 2022:919.
Habib M, Iqbal MJ, Lee MH, Kim DJ, Akram F, Gul M, Zeb A, Rehman IU, Kim M-H, Song TK. Piezoelectric performance of Zr-modified lead-free BiFeO3-BaTiO3 ceramics. Mater Res Bull 2022:146.
Lv X, Zhang X-X, Wu J. Nano-domains in lead-free piezoceramics: a review. J Mater Chem 2020;8:10026–73.
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