Influence of A-site non-stoichiometry on electromechanical properties of Sr(Hf0.5Zr0.5)O3-modified Bi0.5(Na0.8K0.2)0.5TiO3 piezoelectric ceramics
Source abstract
Abstract
Effect of Na non-stoichiometry in Sr(Hf0.5Zr0.5)O3-modified Bi0.5(Na(0.8+x)K0.2)0.5TiO3 ceramics was examined in the range of − 0.04 ≤ x ≤ 0.04. The effect of Na non-stoichiometry on microstructure, ferroelectric, piezoelectric, dielectric properties and high-temperature impedance was explored. Compared to the stoichiometric compositions, Na excess and deficiency exhibit the same effect as observed for the acceptor and donor doping, respectively. All non-stoichiometric and stoichiometric compositions exhibit a pure ABO3 perovskite phase with pseudocubic symmetry. The deficiency of Na in ceramics decreases the grain size and drives the system towards ergodic relaxor as evident by pinched ferroelectric loop and the negligible negative strain along with an increase in maximum strain (Sm). The corresponding normalized strain (Sm/Emax.) increased from 275 to 800 pm/V when Na content decreased from x = + 0.04 to − 0.04. In contrast, excess Na exhibits the converse effect and drives the system towards ferroelectricity. Composition with deficient Na also exhibits lower dielectric loss and increase in resistivity by an order of magnitude compared to excess Na as observed from the high-temperature dielectric and impedance measurements. The results of this study demonstrate that Na non-stoichiometry significantly affects the electric properties of the studied system and thus can be effectively modulated to achieve improved electromechanical properties for materials having actuator-based applications.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Ferroelectric and Piezoelectric Materials · Multiferroics and related materials · Microwave Dielectric Ceramics Synthesis
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (80)
Show source-provided references
1. Aksel E, Jakes P, Erdem E, Smyth DM, Ozarowski A, van Tol J, Jones JL, Eichel RA (2011) Processing of manganese-doped [Bi0.5Na0.5]TiO3 ferroelectrics: reduction and oxidation reactions during calcination and sintering. J Am Ceram Soc 94:1363–136710.1111/j.1551-2916.2010.04249.x ↗
2. Ehmke M, Glaum J, Jo W, Granzow T, Rödel J (2011) Stabilization of the Fatigue-Resistant Phase by CuO Addition in (Bi1/2Na1/2)TiO3–BaTiO3. J Am Ceram Soc 94:2473–247810.1111/j.1551-2916.2010.04379.x ↗
3. Glaum J, Simons H, Acosta M, Hoffman M (2013) Tailoring the piezoelectric and relaxor properties of (Bi1/2Na1/2)TiO3–BaTiO3 via zirconium doping. J Am Ceram Soc 96:2881–288610.1111/jace.12405 ↗
4. Gupta SK, McQuade R, Gibbons B, Mardilovich P, Cann DP (2020) Electric field-induced strain in Sr(Hf0.5Zr0.5)O3-modified Bi0.5(Na0.8K0.2)0.5TiO3 piezoelectric ceramics. J Appl Phys 127:07410410.1063/1.5132536 ↗
5. Han H-S, Jo W, Rödel J, Hong I-K, Tai W-P, Lee J-S (2012) Coexistence of ergodicity and nonergodicity in LaFeO3-modified Bi1/2(Na0.78K0.22)1/2TiO3 relaxors. J Phys Condens Matter 24:36590110.1088/0953-8984/24/36/365901 ↗
6. Jo W, Dittmer R, Acosta M, Zang J, Groh C, Sapper E, Wang K, Rödel J (2012) Giant electric-field-induced strains in lead-free ceramics for actuator applications–status and perspective. J Electroceram 29:71–9310.1007/s10832-012-9742-3 ↗
7. Jo W, Erdem E, Eichel R-A, Glaum J, Granzow T, Damjanovic D, Rödel J (2010) Effect of Nb-donor and Fe-acceptor dopants in (Bi1/2Na1/2)TiO3–BaTiO3–(K0.5Na0.5)NbO3 lead-free piezoceramics. J Appl Phys 108:01411010.1063/1.3437645 ↗
8. Kumar N, Ansell TY, Cann DP (2014) Role of point defects in bipolar fatigue behavior of Bi(Mg1/2Ti1/2)O3 modified (Bi1/2K1/2)TiO3-(Bi1/2Na1/2)TiO3 relaxor ceramics. J Appl Phys 115:15410410.1063/1.4871671 ↗
9. Patterson EA, Cann DP (2012) Bipolar piezoelectric fatigue of Bi(Zn0.5Ti0.5)O3-(Bi0.5K0.5) TiO3-(Bi0.5Na0.5)TiO3 Pb-free ceramics. Appl Phys Lett 101:04290510.1063/1.4738770 ↗
10. Jo W, Schaab S, Sapper E, Schmitt LA, Kleebe H-J, Bell AJ, Rödel J (2011) On the phase identity and its thermal evolution of lead free (Bi1/2Na1/2)TiO3-6 mol% BaTiO3. J Appl Phys 110:07410610.1063/1.3645054 ↗
11. Zhang S-T, Kounga AB, Aulbach E, Granzow T, Jo W, Kleebe H-J, Rödel J (2008) Lead-free piezoceramics with giant strain in the system Bi0.5Na0.5TiO3–BaTiO3–K0.5Na0.5NbO3. I. Structure and room temperature properties. J Appl Phys 103:03410810.1063/1.2838476 ↗
12. Dittmer R, Gobeljic D, Jo W, Shvartsman VV, Lupascu DC, Jones JL, Rödel J (2014) Ergodicity reflected in macroscopic and microscopic field-dependent behavior of BNT-based relaxors. J Appl Phys 115:08411110.1063/1.4867157 ↗
13. Li F, Yang K, Liu X, Zou J, Zhai J, Shen B, Li P, Shen J, Liu B, Chen P (2017) Temperature induced high charge–discharge performances in lead-free Bi0.5Na0.5TiO3-based ergodic relaxor ferroelectric ceramics. Scripta Mater 141:15–1910.1016/j.scriptamat.2017.07.010 ↗
14. Liu X, Zhao Y, Shi J, Du H, Xu X, Lu H, Che J, Li X (2019) Improvement of dielectric and ferroelectric properties in bismuth sodium titanate based relaxors through Bi non-stoichiometry. J Alloy Compd 799:231–23810.1016/j.jallcom.2019.05.321 ↗
15. Prasertpalichat S, Schmidt W, Cann DP (2016) Effects of A-site nonstoichiometry on oxide ion conduction 0.94Bi0.5Na0.5TiO3–0.06BaTiO3 in ceramics. J Adv Dielectr 6:165001210.1142/S2010135X16500120 ↗
16. Ni F, Luo L, Li W, Chen H (2012) A-site vacancy-induced giant strain and the electrical properties in non-stoichiometric ceramics Bi0.5+x(Na1−yKy)0.5−3xTiO3. J Phys D Appl Phys 45:41510310.1088/0022-3727/45/41/415103 ↗
17. Randall CA, Markgraf S, Bhalla A, Baba-Kishi K (1989) Incommensurate structures in highly ordered complex perovskites Pb(Co1/2W1/2)O3 and Pb(Sc1/2Ta1/2)O3. Phys Rev B 40:41310.1103/PhysRevB.40.413 ↗
18. Zhou Q, Zhou C, Yang H, Yuan C, Li W (2010) Dielectric properties and depolarization temperature of Bi0.5(Na, K)0.5TiO3–BiFeO3 lead-free ceramics. Phys B 405:613–61810.1016/j.physb.2009.09.075 ↗
19. Guo Y, Gu M, Luo H (2011) Antiferroelectric phase and pyroelectric response in (Nay, Biz)Ti1−xO3(1–x)− xBaTiO3 ceramics. J Am Ceram Soc 94:1350–135310.1111/j.1551-2916.2011.04509.x ↗
20. Guo Y, Gu M, Luo H, Liu Y, Withers RL (2011) Composition-induced antiferroelectric phase and giant strain in lead-free (Nay, Biz)Ti1−xO3(1–x)− xBaTiO3 ceramics. Phys Rev B 83:05411810.1103/PhysRevB.83.054118 ↗
21. Hiruma Y, Nagata H, Takenaka T (2009) Thermal depoling process and piezoelectric properties of bismuth sodium titanate ceramics. J Appl Phys 105:08411210.1063/1.3115409 ↗
22. Zuo R, Su S, Wu Y, Fu J, Wang M, Li L (2008) Influence of A-site nonstoichiometry on sintering, microstructure and electrical properties of (Bi0.5Na0.5)TiO3 ceramics. Mater Chem Phys 110:311–31510.1016/j.matchemphys.2008.02.007 ↗
23. Sung Y, Kim J, Cho J, Song T, Kim M, Park T (2011) Effects of Bi nonstoichiometry in ceramics (Bi0.5+xNa)TiO3. Appl Phys Lett 98:01290210.1063/1.3525370 ↗
24. Spreitzer M, Valant M, Suvorov D (2007) Sodium deficiency in Na0.5Bi0.5TiO3. J Mater Chem 17:185–19210.1039/B609606A ↗
25. Sung Y, Kim J, Cho J, Song T, Kim M, Chong H, Park T, Do D, Kim S (2010) Effects of Na nonstoichiometry in (Bi0.5Na0.5+x)TiO3 ceramics. Appl Phys Lett 96:02290110.1063/1.3275704 ↗
26. Li M, Pietrowski MJ, De Souza RA, Zhang H, Reaney IM, Cook SN, Kilner JA, Sinclair DC (2014) A family of oxide ion conductors based on the ferroelectric perovskite Na0.5Bi0.5TiO3. Nat Mater 13:31–3510.1038/nmat3782 ↗
27. Li L, Li M, Zhang H, Reaney IM, Sinclair DC (2016) Controlling mixed conductivity in Na1/2Bi1/2TiO3 using A-site non-stoichiometry and Nb-donor doping. J Mater Chem C 4:5779–578610.1039/C6TC01719C ↗
28. Li M, Zhang H, Cook SN, Li L, Kilner JA, Reaney IM, Sinclair DC (2015) Dramatic influence of A-site nonstoichiometry on the electrical conductivity and conduction mechanisms in the perovskite oxide Na0.5Bi0.5TiO3. Chem Mater 27:629–63410.1021/cm504475k ↗
29. Wu Y, Wang X, Zhong C, Li L (2011) Effect of Na/K excess on the electrical properties of Na0.5Bi0.5TiO3–K0.5Bi0.5TiO3 thin films prepared by sol–gel processing. Thin Solid Films 519:4798–480310.1016/j.tsf.2011.01.077 ↗
30. Lee K-M, Jang HM, Park W-J (1997) Mechanism of 1: 1 nonstoichiometric short-range ordering in La-doped Pb(Mg1/3Nb2/3)O3 relaxor ferroelectrics. J Mater Res 12:1603–161310.1557/JMR.1997.0220 ↗
31. Lei N, Zhu M, Yang P, Wang L, Wang L, Hou Y, Yan H (2011) Effect of lattice occupation behavior of Li+ cations on microstructure and electrical properties of (Bi1/2Na1/2)TiO3-based lead-free piezoceramics. J Appl Phys 109:05410210.1063/1.3555598 ↗
32. Chen J, Tang Z, Tian R, Bai Y, Zhao S, Zhang H (2016) Domain switching contribution to the ferroelectric, fatigue and piezoelectric properties of lead-free (Na0.85K0.15)0.5TiO3 films. RSC Adv 6:33834–3384210.1039/C6RA04262G ↗
33. Takahashi S (1982) Effects of impurity doping in lead zirconate-titanate ceramics. Ferroelectrics 41:143–15610.1080/00150198208210617 ↗
34. Jo W, Granzow T, Aulbach E, Rödel J, Damjanovic D (2009) Origin of the large strain response in (K0.5Na0.5)NbO3-modified (Bi0.5Na0.5)TiO3–BaTiO3 lead-free piezoceramics. J Appl Phys 105:09410210.1063/1.3121203 ↗
35. ASTM B962–17, Standard Test Methods for Density of Compacted or Sintered Powder Metallurgy (PM) Products Using Archimedes’ Principle, ASTM International, West Conshohocken, PA, 2017.
36. Bai W, Chen D, Huang Y, Zheng P, Zhong J, Ding M, Yuan Y, Shen B, Zhai J, Ji Z (2016) Temperature-insensitive large strain response with a low hysteresis behavior in BNT-based ceramics. Ceram Int 42:7669–768010.1016/j.ceramint.2016.01.181 ↗
37. Bai W, Li P, Li L, Zhang J, Shen B, Zhai J (2015) Structure evolution and large strain response in BNT–BT lead-free piezoceramics modified with Bi (Ni0.5Ti0.5)O3. J Alloy Compd 649:772–78110.1016/j.jallcom.2015.07.178 ↗
38. Jones G, Kreisel J, Thomas P (2002) A structural study of the (Na1− xKx)0.5Bi0.5TiO3 perovskite series as a function of substitution (x) and temperature. Powder Diffr 17:301–31910.1154/1.1505047 ↗
39. Seifert KT, Jo W, Rödel J (2010) Temperature-insensitive large strain of (Bi1/2Na1/2)TiO3–(Bi1/2K1/2)TiO3–(K0.5Na0.5)NbO3 lead-free piezoceramics. J Am Ceram Soc 93:1392–139610.1111/j.1551-2916.2009.03573.x ↗
40. Daniels JE, Jo W, Rödel J, Honkimäki V, Jones JL (2010) Electric-field-induced phase-change behavior in (Bi0.5Na0.5)TiO3–BaTiO3–(K0.5Na0.5)NbO3: A combinatorial investigation. Acta Mater 58:2103–211110.1016/j.actamat.2009.11.052 ↗
41. Daniels JE, Jo W, Rödel J, Jones JL (2009) Electric-field-induced phase transformation at a lead-free morphotropic phase boundary: Case study in a 93% (Bi0.5Na0.5)TiO3–7% BaTiO3 piezoelectric ceramic. Appl Phys Lett 95:03290410.1063/1.3182679 ↗
42. Qiao X-s, Chen X-m, Lian H-l, Zhou J-p, Liu P (2016) Dielectric, ferroelectric, piezoelectric properties and impedance analysis of nonstoichiometric (Bi0.5Na0.5)0.94+ xBa0.06TiO3 ceramics. J Eur Ceram Soc 36:3995–400110.1016/j.jeurceramsoc.2016.06.032 ↗
43. Qiao XS, Chen XM, Lian HL, Chen WT, Zhou JP, Liu P (2016) Microstructure and electrical properties of nonstoichiometric 0.94(Na0.5Bi0.5+x)TiO3–0.06BaTiO3 lead-free ceramics. J Am Ceram Soc 99:198–20510.1111/jace.13941 ↗
44. Qiu Y-z, Chen X-m, Lian H-l, Ma J-p, Ouyang W-q (2017) Structure and electrical behavior of unpoled and poled 0.97(Bi0.5Na0.5)0.94Ba0.06TiO3-0.03BiAlO3 ceramics. Mater Chem Phys 202:197–20310.1016/j.matchemphys.2017.09.038 ↗
45. Wang T, Chen X-m, Qiu Y-z, Lian H-l, Chen W-t (2017) Microstructure and electrical properties of (1–x)[0.8 Bi0.5Na0.5TiO3-0.2 Bi0.5K0.5TiO3]-xBiCoO3 lead-free ceramics. Mater Chem Phys 186:407–41410.1016/j.matchemphys.2016.11.012 ↗
46. Zhu M, Liu L, Hou Y, Wang H, Yan H (2007) Microstructure and electrical properties of MnO-doped (Na0.5Bi0.5)0.92Ba0.08TiO3 lead-free piezoceramics. J Am Ceram Soc 90:120–12410.1111/j.1551-2916.2006.01349.x ↗
47. Chen X, Ma H, Pan W, Pang M, Liu P, Zhou J (2012) Microstructure, dielectric and ferroelectric properties of (NaxBi0.5)0.94Ba0.06TiO3 lead-free ferroelectric ceramics: effect of Na nonstoichiometry. Mater Chem Phys 132:368–37410.1016/j.matchemphys.2011.11.039 ↗
48. Verma R, Rout S (2019) Frequency-dependent ferro-antiferro phase transition and internal bias field influenced piezoelectric response of donor and acceptor doped bismuth sodium titanate ceramics. J Appl Phys 126:09410310.1063/1.5111505 ↗
49. Fisher JG, Kang S-JL (2009) Microstructural changes in (K0.5Na0.5)NbO3 ceramics sintered in various atmospheres. J Eur Ceram Soc 29:2581–258810.1016/j.jeurceramsoc.2009.02.006 ↗
50. Jung Y-I, Choi S-Y, Kang S-JL (2006) Effect of oxygen partial pressure on grain boundary structure and grain growth behavior in BaTiO3. Acta Mater 54:2849–285510.1016/j.actamat.2006.02.025 ↗
51. Chung S-Y, Yoon DY, Kang S-JL (2002) Effects of donor concentration and oxygen partial pressure on interface morphology and grain growth behavior in SrTiO3. Acta Mater 50:3361–337110.1016/S1359-6454(02)00139-8 ↗
52. Lee B-K, Chung S-Y, Kang S-JL (2000) Grain boundary faceting and abnormal grain growth in BaTiO3. Acta Mater 48:1575–158010.1016/S1359-6454(99)00434-6 ↗
53. Dawber M, Scott J (2000) A model for fatigue in ferroelectric perovskite thin films. Appl Phys Lett 76:1060–106210.1063/1.125938 ↗
54. He L, Vanderbilt D (2003) First-principles study of oxygen-vacancy pinning of domain walls in PbTiO3. Physical Review B 68:13410310.1103/PhysRevB.68.134103 ↗
55. Scott J, Dawber M (2000) Oxygen-vacancy ordering as a fatigue mechanism in perovskite ferroelectrics. Appl Phys Lett 76:3801–380310.1063/1.126786 ↗
56. Erhart P, Eichel R-A, Träskelin P, Albe K (2007) Association of oxygen vacancies with impurity metal ions in lead titanate. Physical Review B 76:17411610.1103/PhysRevB.76.174116 ↗
57. Zhang Z, Wu P, Lu L, Shu C (2008) Defect and electronic structures of acceptor substituted lead titanate. Appl Phys Lett 92:11290910.1063/1.2898212 ↗
58. Shrout TR, Zhang SJ (2007) Lead-free piezoelectric ceramics: Alternatives for PZT? J Electroceram 19:113–12610.1007/s10832-007-9047-0 ↗
59. Zhang S, Lim JB, Lee HJ, Shrout TR (2009) Characterization of hard piezoelectric lead-free ceramics. IEEE Trans Ultrason Ferroelectr Freq Control 56:1523–152710.1109/TUFFC.2009.1215 ↗
60. Noguchi Y, Miwa I, Goshima Y, Miyayama M (2000) Defect control for large remanent polarization in bismuth titanate ferroelectrics–doping effect of higher-valent cations–. Jpn J Appl Phys 39:L125910.1143/JJAP.39.L1259 ↗
61. Bidault O, Husson E, Morell A (1997) Effects of lead vacancies on the spontaneous relaxor to ferroelectric phase transition in Pb[(Mg1/3Nb2/3)0.9Ti0.1]O3. J Appl Phys 82:5674–567910.1063/1.366430 ↗
62. Chu F, Reaney I, Setter N (1995) Spontaneous (zero-field) relaxor–to–ferroelectric-phase transition in disordered Pb(Sc1/2Nb1/2)O3. J Appl Phys 77:1671–167610.1063/1.358856 ↗
63. Hao J, Bai W, Li W, Zhai J (2012) Correlation Between the Microstructure and Electrical Properties in High-Performance (Ba0.85Ca0.15)(Zr0.1Ti0.9)O3 Lead-Free Piezoelectric Ceramics. J Am Ceram Soc 95:1998–200610.1111/j.1551-2916.2012.05146.x ↗
64. Bai W, Li H, Xi J, Zhang J, Shen B, Zhai J (2016) Effect of different templates and texture on structure evolution and strain behavior of< 001>-textured lead-free piezoelectric BNT-based ceramics. J Alloy Compd 656:13–2310.1016/j.jallcom.2015.09.209 ↗
65. Hussain A, Ahn CW, Lee JS, Ullah A, Kim IW (2010) Large electric-field-induced strain in Zr-modified lead-free Bi0.5(Na0.78K0.22)0.5TiO3 piezoelectric ceramics. Sens Actuators, A 158:84–8910.1016/j.sna.2009.12.027 ↗
66. Hussain A, Ahn CW, Ullah A, Lee JS, Kim IW (2012) Dielectric, ferroelectric and field-induced strain behavior of K0.5Na0.5NbO3-modified Bi0.5(Na0.78K0.22)0.5TiO3 lead-free ceramics. Ceram Int 38:4143–414910.1016/j.ceramint.2012.01.074 ↗
67. Dorcet V, Trolliard G, Boullay P (2008) Reinvestigation of phase transitions in Na0.5Bi0.5TiO3 by TEM. Part I: First order rhombohedral to orthorhombic phase transition. Chem Mater 20:5061–507310.1021/cm8004634 ↗
68. Carreaud J, Bogicevic C, Dkhil B, Kiat J (2008) Dielectric evidences of core-shell-like effects in nanosized relaxor PbMg1/3Nb2/3O3. Appl Phys Lett 92:24290210.1063/1.2945884 ↗
69. Papet P, Dougherty JP, Shrout TR (1990) Particle and grain size effects on the dielectric behavior of the relaxor ferroelectric Pb(Mg1/3Nb2/3)O3. J Mater Res 5:2902–290910.1557/JMR.1990.2902 ↗
70. Randall CA, Hilton A, Barber D, Shrout T (1993) Extrinsic contributions to the grain size dependence of relaxor ferroelectric Pb(Mg1/3Nb2/3)O3:PbTiO3 ceramics. J Mater Res 8:880–88410.1557/JMR.1993.0880 ↗
71. Gentner J, Gerthsen P, Schmidt N, Send R (1978) Dielectric losses in ferroelectric ceramics produced by domain-wall motion. J Appl Phys 49:4485–448910.1063/1.325453 ↗
72. Härdtl K (1982) Electrical and mechanical losses in ferroelectric ceramics. Ceram Int 8:121–12710.1016/0272-8842(82)90001-3 ↗
73. Mishra A, Khatua DK, De A, Majumdar B, Frömling T, Ranjan R (2019) Structural mechanism behind piezoelectric enhancement in off-stoichiometric Na0.5Bi0.5TiO3 based lead-free piezoceramics. Acta Mater 164:761–77510.1016/j.actamat.2018.11.015 ↗
74. Xu Q, Chen M, Chen W, Liu H-X, Kim B-H, Ahn B-K (2008) Effect of CoO additive on structure and electrical properties of (Na0.5Bi0.5)0.93Ba0.07TiO3 ceramics prepared by the citrate method. Acta Mater 56:642–65010.1016/j.actamat.2007.10.014 ↗
75. Badapanda T, Sahoo S, Nayak P Dielectric, Ferroelectric and Piezoelectric study of BNT-BT solid solutions around the MPB region. In: IOP Conference Series: Materials Science and Engineering, 2017. vol 1. IOP Publishing, p 01203210.1088/1757-899X/178/1/012032 ↗
76. Guo Y, Fan H, Shi J (2015) Origin of the large strain response in tenary SrTi0.8Zr0.2O3 modified Bi0.5Na0.5TiO3–Bi0.5K0.5TiO3 lead-free piezoceramics. J Mater Sci 50:403–411. https://doi.org/10.1007/s10853-014-8599-z10.1007/s10853-014-8599-z ↗
77. Guo Y, Liu Y, Withers RL, Brink F, Chen H (2010) Large electric field-induced strain and antiferroelectric behavior in (1–x)(Na0.5Bi0.5)TiO3-xBaTiO3 ceramics. Chem Mater 23:219–22810.1021/cm102719k ↗
78. Xu Q, Huang D-P, Chen M, Chen W, Liu H-X, Kim B-H (2009) Effect of bismuth excess on ferroelectric and piezoelectric properties of a (Na0.5Bi0.5)TiO3–BaTiO3 composition near the morphotropic phase boundary. J Alloy Compd 471:310–31610.1016/j.jallcom.2008.03.078 ↗
79. Sinclair DC (1995) Characterisation of electro-materials using ac impedance spectroscopy. Boletín de la Sociedad Española de Cerámica y Vidrio 34:55–65
80. West AR, Sinclair DC, Hirose N (1997) Characterization of electrical materials, especially ferroelectrics, by impedance spectroscopy. J Electroceram 1:65–7110.1023/A:1009950415758 ↗