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Phase transitions, relaxor behavior, and electrical properties in (1-x)(Bi0.5Na0.5)Ti03-x(K0.5Na0.5)NbO3 lead-free piezoceramics

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Abstract

Phase structures and electrical properties of lead-free piezoelectric (1—x)(Bi0.5Na0.5)TiO3-x (K0.5Na0.5)NbO3 (BNT-XKNN) ceramics with 0.08 ≤ x ≤ 0.19 were systematically investigated. Results showed that a phase transition from a tetragonal to a pseudocubic phase occurred in this system, as KNN content increases. The addition of KNN shifted both the depolarization temperature Td and rhombohedral-tetragonal phase transition temperature TR-T to lower temperatures and tended to enhance the relaxor behavior of the ceramics, which was well explained by the microdomain-macrodomain transition theory with calculating criterion K. At x = 0.10-0.11, Td reached room temperature (RT), which accordingly induced an enhancement of the unipolar strain that peaks at a value of 0.22% was obtained. Furthermore, as the compositions (x = 0.12-0.15) have Td below RT, samples exhibited high electrostrictive response with large electrostrictive coefficient Q33 (0.017-0.019 m4/C2) and good thermostability comparable with that of traditional Pb-based electro stridors.

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References

  1. T. Takenaka and H. Nagata: Current status and prospects of lead-free piezoelectric ceramics. J. Eur. Ceram. Soc. 25, 2693 (2005).

    Article  CAS  Google Scholar 

  2. J. Rödel, W. Jo, K.T.P. Seifert, E.M. Anton, T. Granzow, and D. Damjanovic: Perspective on the development of lead-free piezoceramics. J. Am. Ceram. Soc. 92, 1153 (2009).

    Article  CAS  Google Scholar 

  3. A. Sasaki, T. Chiba, Y. Mamiya, and E. Otsuki: Dielectric and piezoelectric properties of (Bi0.5Na0.5)TiO3-(Bi0.5K0.5)TiO3 systems. Jpn. J. Appl. Phys. 38, 5564 (1999).

    Article  CAS  Google Scholar 

  4. L.Y. Liu, M.K. Zhu, Y.D. Hou, H. Yan, and R.P. Liu: Abnormal piezoelectric and dielectric behavior of 0.92Na0.5Bi0.5TiO3-0.08BaTiO3 induced by La doping. J. Mater. Res. 22, 1188 (2007).

    Article  CAS  Google Scholar 

  5. A.B. Kounga, S.T. Zhang, W. Jo, T. Granzow, and J. Rödel: Morphotropic phase boundary in (1-x)Bi0.5Na0.5TiO3-xK0.5Na0.5NbO3 lead-free piezoceramics. Appl. Phys. Lett. 92, 222902 (2008).

    Article  CAS  Google Scholar 

  6. Y. Hiruma, K. Yoshii, H. Nagata, and T. Takenaka: Phase transition temperature and electrical properties of (Bi1/2Na1/2)TiO3-Bi1/2A1/2) TiO3 (A = Li and K) lead-free ferroelectric ceramics. J. Appl. Phys. 103, 084121–084127 (2008).

    Article  CAS  Google Scholar 

  7. J. Shieh, K.C. Wu, and C.S. Chen: Switching characteristics of MPB compositions of (Bi0.5Na0.5)TiO3-BaTiO3-(Bi0.5K0.5)TiO3 lead-free ferroelectric ceramics. Acta Mater. 55, 3081–3087 (2007).

    Article  CAS  Google Scholar 

  8. S. Zhang, T.R. Shrout, H. Nagata, Y. Hiruma, and T. Takenaka: Piezoelectric properties in (K0.5Bi0.5)TiO3-(Na0.5Bi0.5)TiO3-BaTiO3 lead-free ceramics. IEEE Trans. Ultrason. Ferroelectr. Freq. Control 54, 910 (2007).

    Article  Google Scholar 

  9. T.R. Shrout and S.J. Zhang: Lead-free piezoelectric ceramics: Alternatives for PZT? J. Electroceram. 19, 111 (2007).

    Article  CAS  Google Scholar 

  10. Y. Hiruma, H. Nagata, and T. Takenaka: Phase diagrams and electrical properties of (Bi1/2Na1/2)TiO3-based solid solutions. J. Appl. Phys. 104, 124106 (2008).

    Article  CAS  Google Scholar 

  11. S-H. Lee, C-B. Yoon, S-M. Lee, H-E. Kim, and K-W. Lee: Piezoelectric properties of lead-free (Na0.5Bi0.5)TiO3-(Na0.5K0.5) NbO3-BaTiO3 ceramics. J. Mater. Res. 23, 115 (2008).

    Article  CAS  Google Scholar 

  12. K. Wang, A. Hussain, W. Jo, and J. Rödel: Temperature-dependent properties of (Bi1/2Na1/2)TiO3-(Bi1/2K1/2)TiO3-SrTiO3 lead-free piezoceramics. J. Am. Ceram. Soc. 95, 2241 (2012).

    Article  CAS  Google Scholar 

  13. Y.P. Guo, M.Y. Gu, H.S. Luo, Y. Liu, and R.L. Withers: Composition-induced antiferroelectric phase and giant strain in lead-free (Nay, Biz)Ti1_x03(1_x)-xBaTiO3 ceramics. Phys. Rev. B 83, 054118 (2011).

    Article  CAS  Google Scholar 

  14. Y. Hiruma, H. Nagata, and T. Takenaka: Detection of morphotropic phase boundary of (Bi1/2Na1/2)TiO3-Ba(Al1/2Sb1/2)O3 solid-solution ceramics. Appl. Phys. Lett. 95, 052903 (2009).

    Article  CAS  Google Scholar 

  15. S-T. Zhang, A.B. Kounga, E. Aulbach, H. Ehrenberg, and J. Rödel: Giant strain in lead-free piezoceramics. Appl. Phys. Lett. 91, 112906 (2007).

    Article  CAS  Google Scholar 

  16. K.T.P. Seifert, W. Jo, and J. Rödel: Temperature-insensitive large strain of (Bi1/2Na1/2)TiO3-(Bi1/2K1/2)TiO3-(K0.5Na0.5)NbO3 lead-free piezoceramics. J. Am. Ceram Soc. 93, 1392 (2010).

    CAS  Google Scholar 

  17. F.F. Wang, M. Xu, Y.X. Tang, T. Wang, W.Z. Shi, and C.M. Leung: Large strain response in the ternary Bi0.5Na0.5TiO3-BaTiO3-SrTiO3 solid solutions. J. Am. Ceram. Soc. 95, 1955 (2012).

    Article  CAS  Google Scholar 

  18. P. Jarupoom, E. Patterson, B. Gibbons, G. Rujijanagul, R. Yimnirun, and D. Cann: Lead-free ternary perovskite compounds with large electromechanical strains. Appl. Phys. Lett. 99, 152901 (2011).

    Article  CAS  Google Scholar 

  19. A. Ullah, C.W. Ahn, A. Hussain, S.Y. Lee, and I.W. Kim: Phase transition, electrical properties, and temperature-insensitive large strain in BiA1O3-modiried Bi0.5(Na0.75K0.25)0.5TiO3 lead-free piezoelectric ceramics. J. Am. Ceram Soc. 94, 3915 (2011).

    Article  CAS  Google Scholar 

  20. W. Jo, T. Granzow, E. Aulbach, J. Rödel, and D. Damjanovic: Origin of the large strain response in (K0.5Na0.5)NbO3-modiried (Bi0.5Na0.5)TiO3-BaTiO3 lead-free piezoceramics. J. Appl. Phys. 105, 094102 (2009).

    Article  CAS  Google Scholar 

  21. W. Jo, S. Schaab, E. Sapper, L.A. Schmitt, H-J. Kleebe, A.J. Bell, and J. Rödel: On the phase identity and its thermal evolution of lead free (Bi1/2Na1/2)TiO3-6 mol% BaTiO3. J. Appl. Phys. 110, 074106 (2011).

    Article  CAS  Google Scholar 

  22. V. Bobnar, B. Malic, J. Hole, M. Kosec, R. Steinhausen, and H. Beige: Electrostrictive effect in lead-free relaxor K0.5Na0.5NbO3-SrTiO3 ceramic system. J. Appl. Phys. 98, 024113 (2005).

    Article  CAS  Google Scholar 

  23. C. Ang and Z. Yu: High, purely electrostrictive strain in lead-free dielectrics. Adv. Mater. 18, 103 (2006).

    Article  CAS  Google Scholar 

  24. S.T. Zhang, A.B. Kounga, W. Jo, C. Jamin, K. Seifert, T. Granzow, J. Rödel, and D. Damjanovic: High-strain lead-free antiferroelectric electrostrictors. Adv. Mater. 21, 4716 (2009).

    Article  CAS  Google Scholar 

  25. S.T. Zhang, F. Yan, B. Yang, and W. Cao: Phase diagram and electrostrictive properties of Bi0.5Nag0.5TiO3-BaTiO3-K0.5Na0.5NbO3 ceramics. Appl. Phys. Lett. 97, 122901 (2010).

    Article  CAS  Google Scholar 

  26. V.D. Ngoc, T.H-S. Han, C-H. Yoo, J-S. Lee, W. Jo, and J. Rödel: Lead-free electrostrictive bismuth perovskite ceramics with thermally stable field-induced strains. Mater. Lett. 65, 2607 (2011).

    Article  CAS  Google Scholar 

  27. J.M. Li, F.F. Wang, X.M. Qin, M. Xu, and W.Z. Shi: Large electrostrictive strain in lead-free Bi0.5Na0.5TiO3-BaTiO3-KNbO3 ceramics. Appl. Phys. A 104, 117 (2011).

    Article  CAS  Google Scholar 

  28. G.H. Haertling: Ferroelectric ceramics: History and technology. J. Am. Ceram. Soc. 82, 797 (1999).

    Article  CAS  Google Scholar 

  29. G.O. Jones, J. Kreisel, and P.A. Thomas: A structural study of the (Na1_xKx)0.5Bi0.5TiO3 perovskite series as a function of substitution and temperature. Powder Diffr. 17, 301 (2002).

    Article  CAS  Google Scholar 

  30. K. Ito, K. Tezuka, and Y. Hinatsu: Preparation, magnetic susceptibility, and specific heat on interlanthanide perovskites ABO3 (A = La-Nd, B = Dy-Lu). J. Solid State Chem. 157, 173 (2001).

    Article  CAS  Google Scholar 

  31. W-C. Lee, C-Y. Huang, L-K. Tsao, and Y-C. Wu: Chemical composition and tolerance factor at the morphotropic phase boundary in (Bi0.5Na0.5)TiO3-based piezoelectric ceramics. J. Eur. Ceram. Soc. 29, 1443 (2009).

    Article  CAS  Google Scholar 

  32. E. Sapper, S. Schaab, W. Jo, T. Granzow, and J. Rödel: Influence of electric fields on the depolarization temperature of Mn-doped (1-x)(Bi1/2Na1/2)Ti03-xBaTiO3. J. Appl. Phys. 111, 014105 (2012).

    Article  CAS  Google Scholar 

  33. Y. Hiruma, H. Nagata, and T. Takenaka: Thermal depoling process and piezoelectric properties of bismuth sodium titanate ceramics. J. Appl. Phys. 105, 084112 (2009).

    Article  CAS  Google Scholar 

  34. E.M. Anton, W. Jo, D. Damjanovic, and J. Rödel: Determination of depolarization temperature of (Bii/2Na1/2)TiO3-based lead-free piezoceramics. J. Appl. Phys. 110, 094108 (2011).

    Article  CAS  Google Scholar 

  35. X. Tan, E. Aulbach, W. Jo, T. Granzow, J. Kling, M. Marsilius, H.J. Kleebe, and J. Rödel: Effect of uniaxial stress on ferroelectric behavior of (Bi1/2Na1/2)TiO3-based lead-free piezoelectric ceramics. J. Appl. Phys. 106, 044107 (2009).

    Article  CAS  Google Scholar 

  36. R. Dittmer, W. Jo, D. Damjanovic, and J. Rödel: Lead-free high-temperature dielectrics with wide operational range. J. Appl. Phys. 109,034107(2011).

  37. M. Hinterstein, M. Knapp, M. Hölzel, W. Jo, A. Cervellino, and H. Ehrenberg: Field-induced phase transition in Bi1/2Na1/2TiO3-based lead-free piezoelectric ceramics. J. Appl. Crystallogr. 43, 1314 (2010).

    Article  CAS  Google Scholar 

  38. K.G. Webber, Y. Zhang, W. Jo, J.E. Daniels, and J. Rödel: High temperature stress-induced “double loop-like” phase transitions in Bi-based perovskites. J. Appl. Phys. 108, 014101 (2010).

    Article  CAS  Google Scholar 

  39. P. Laoratanakul, R. Yimnirun, and S. Wongsaenmai: Phase formation and dielectric properties of bismuth sodium titanate potassium sodium niobate ceramics. Curr. Appl. Phys. 11, S161 (2011).

    Article  Google Scholar 

  40. E.A. Patterson, D.P. Cann, J. Pokorny, and I.M. Reaney: Electromechanical strain in Bi(Zn1/2Ti1/2)O3-(Bi1/2Na1/2)TiO3-(Bi1/2K1/2) TiO3 solid solutions. J. Appl. Phys. 111, 094105 (2012).

    Article  CAS  Google Scholar 

  41. R.Z. Zuo, X.S. Fang, and C. Ye: Phase structures and electrical properties of new lead-free (Na0.5K0.5)NbO3-(Bi0.5Na0.5)TiO3 ceramics. Appl. Phys. Lett. 90, 092904 (2007).

    Article  CAS  Google Scholar 

  42. K. Uchino and S. Nomura: Critical exponents of the dielectric constants in diffused phase transition crystals. Ferroelectr. Lett. Sect. 44, 55 (1982).

    Article  CAS  Google Scholar 

  43. D.J. Zhang and X. Yao: Dynamics on microdomain-macrodomain transition of relaxor ferroelectrics. Acta Phys. Chim. Sin. 20, 712 (2004).

    Article  Google Scholar 

  44. F. Gao, L.L. Liu, B. Xu, G.X. Hu, X. Cao, R.Z. Hong, and C.S. Tian: Texture development and dielectric relaxor behavior of 0.80Na0.5Bi0.5TiO3-0.20K0.5Bi0.5TiO3 ceramics templated by plate-like NaNbO3 particles. J. Eur. Ceram. Soc. 31, 2987 (2011).

    Article  CAS  Google Scholar 

  45. Y. Hirum, H. Nagata, and T. Takenaka: Formation of morphotropic phase boundary and electrical properties of (Bi1/2Na1/2TiO3-Ba (Al1/2Nb1/2)O3 solid solution ceramics. Jpn. J. Appl. Phys. 48, 09KC08 (2009).

    Google Scholar 

  46. J. Petzelt, S. Kamba, J. Fabry, D. Noujni, V. Porokhonskyy, A. Pashkin, I. Franke, K. Roleder, J. Suchanicz, R. Klein, and G.E. Kugel: Infrared, Raman and high-frequency dielectric spectroscopy and the phase transition in Na1/2Bi1/2TiO1/2. J. Phys. Condens. Matter 16, 2719 (2004).

    Article  CAS  Google Scholar 

  47. S.T. Zhang, A.B. Kounga, E. Aulbach, and Y. Deng: Temperature-dependent electrical properties of 0.94Bi0.5Na0.5TiO3-0.06BaTiO3 ceramics. J. Am. Ceram. Soc. 91, 3950 (2008).

    Article  CAS  Google Scholar 

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Acknowledgment

The authors would like to acknowledge the support from the National Natural Science Foundation of China under Grant No. 50932007 and Shanghai Municipal Natural Science Foundation under Grant No. 12ZR1434600.

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Correspondence to Jiwei Zhai.

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Hao, J., Bai, W., Li, W. et al. Phase transitions, relaxor behavior, and electrical properties in (1-x)(Bi0.5Na0.5)Ti03-x(K0.5Na0.5)NbO3 lead-free piezoceramics. Journal of Materials Research 27, 2943–2955 (2012). https://doi.org/10.1557/jmr.2012.328

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