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(1-x)K0.5Na0.5NbO3-xBi(Zn2/3Nb1/3)O3 ((1-x)KNN-xBZN, x = 0.010, 0.015, 0.020, 0.025, and 0.030) lead-free ceramics were fabricated via a traditional solid-state method. The crystal structure, microstructure, dielectric, and conductivity behavior of this system were studied. Combined with X-ray diffraction (XRD) patterns, Rietveld refinement, and dielectric spectroscopy, an orthorhombic phase was determined for x = 0.010, an orthorhombic-tetragonal mixed phase was identified for x = 0.015, and a rhombohedral symmetry appears in 0.020 ≤ x ≤ 0.030. Both 0.98KNN-0.02BZN and 0.975KNN-0.025BZN ceramics exhibit stable permittivity and low dielectric loss tangent (tanδ) in wide temperature ranges owing to the combination of rhombohedral-tetragonal step-like feature and the diffuse phase transition from tetragonal to cubic. The activation energies of dielectric relaxation and conductivity behavior at high temperatures initially decrease slightly, then drop sharply, and finally decline slowly, which could be attributed to microstructure morphologies and the concentration of oxygen vacancies.


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Structure evolution, dielectric, and conductivity behavior of (K0.5Na0.5)NbO3-Bi(Zn2/3Nb1/3)O3 ceramics

Show Author's information Tianxiang YANa( )Kaiyuan CHENaChengqi LIaMin LIUbJie WANGcLiang FANGaLaijun LIUa
College of Mechanical and Control Engineering & College of Materials Science and Engineering, Guilin University of Technology, Guilin 541004, China
Institute of Fluid Engineering Equipment, Jiangsu Industrial Technology Research Institute, Jiangsu University, Zhenjiang 212013, China
Key Laboratory for RF Circuits and Systems, Ministry of Education & Key Laboratory of Large Scale Integrated Design, Hangzhou Dianzi University, Hangzhou 310018, China

Abstract

(1-x)K0.5Na0.5NbO3-xBi(Zn2/3Nb1/3)O3 ((1-x)KNN-xBZN, x = 0.010, 0.015, 0.020, 0.025, and 0.030) lead-free ceramics were fabricated via a traditional solid-state method. The crystal structure, microstructure, dielectric, and conductivity behavior of this system were studied. Combined with X-ray diffraction (XRD) patterns, Rietveld refinement, and dielectric spectroscopy, an orthorhombic phase was determined for x = 0.010, an orthorhombic-tetragonal mixed phase was identified for x = 0.015, and a rhombohedral symmetry appears in 0.020 ≤ x ≤ 0.030. Both 0.98KNN-0.02BZN and 0.975KNN-0.025BZN ceramics exhibit stable permittivity and low dielectric loss tangent (tanδ) in wide temperature ranges owing to the combination of rhombohedral-tetragonal step-like feature and the diffuse phase transition from tetragonal to cubic. The activation energies of dielectric relaxation and conductivity behavior at high temperatures initially decrease slightly, then drop sharply, and finally decline slowly, which could be attributed to microstructure morphologies and the concentration of oxygen vacancies.

Keywords:

ceramic, crystal structure, dielectric spectroscopy, oxygen vacancies
Received: 14 November 2020 Revised: 03 March 2021 Accepted: 10 March 2021 Published: 05 August 2021 Issue date: August 2021
References(44)
[1]
Watson J, Castro G. A review of high-temperature electronics technology and applications. J Mater Sci: Mater Electron 2015, 26: 9226-9235.
[2]
Ren PR, He JJ, Yan FX, et al. Temperature-stable dielectric and energy storage properties of (1-x)(0.94Bi0.5Na0.5TiO3- 0.09BiAlO3)-xSrTiO3 ceramics. J Alloys Compd 2019, 807: 151676.
[3]
Chen Z, Li GZ, Sun XJ, et al. La2O3 modified 0.4(Ba0.8Ca0.2)TiO3-0.6Bi(Mg0.5Ti0.5)O3 ceramics for high-temperature capacitor applications. Ceram Int 2015, 41: 11057-11061.
[4]
Hirose S, Usui T, Crossley S, et al. Progress on electrocaloric multilayer ceramic capacitor development. APL Mater 2016, 4: 064105.
[5]
Kishi H, Mizuno Y, Chazono H. Base-metal electrode-multilayer ceramic capacitors: Past, present and future perspectives. Jpn J Appl Phys 2003, 42: 1-15.
[6]
Kobayashi K, Ryu M, Doshida Y, et al. Novel high-temperature antiferroelectric-based dielectric NaNbO3-NaTaO3 solid solutions processed in low oxygen partial pressures. J Am Ceram Soc 2013, 96: 531-537.
[7]
Yan TX, Han FF, Ren SK, et al. Dielectric properties of (K0.5Na0.5)NbO3-(Bi0.5Li0.5)ZrO3 lead-free ceramics as high-temperature ceramic capacitors. Appl Phys A 2018, 124: 338.
[8]
Chen XL, Yan X, Li XX, et al. Excellent temperature stability on relative permittivity, and conductivity behavior of K0.5Na0.5NbO3 based lead free ceramics. J Alloys Compd 2018, 762: 697-705.
[9]
Lin Y, Zhang YJ, Zhan SL, et al. Synergistically ultrahigh energy storage density and efficiency in designed sandwich-structured poly(vinylidene fluoride)-based flexible composite films induced by doping Na0.5Bi0.5TiO3 whiskers. J Mater Chem A 2020, 8: 23427-23435.
[10]
Lin Y, Li D, Zhang M, et al. Excellent energy-storage properties achieved in BaTiO3-based lead-free relaxor ferroelectric ceramics via domain engineering on the nanoscale. ACS Appl Mater Interaces 2019, 11: 36824-36830.
[11]
Li D, Lin Y, Zhang M, et al. Achieved ultrahigh energy storage properties and outstanding charge-discharge performances in (Na0.5Bi0.5)0.7Sr0.3TiO3-based ceramics by introducing a linear additive. Chem Eng J 2020, 392: 123729.
[12]
Ogihara H, Randall CA, Trolier-Mckinstry S. Weakly coupled relaxor behavior of BaTiO3-BiScO3 ceramics. J Am Ceram Soc 2009, 92: 110-118.
[13]
Muhammad R, Iqbal Y, Reaney IM. BaTiO3-Bi(Mg2/3Nb1/3)O3 ceramics for high-temperature capacitor applications. J Am Ceram Soc 2016, 99: 2089-2095.
[14]
Acosta M, Zang JD, Jo W, et al. High-temperature dielectrics in CaZrO3 modified Bi1/2Na1/2TiO3-based lead-free ceramics. J Eur Ceram Soc 2012, 32: 4327-4334.
[15]
Zeb A, Jan SU, Bamiduro F, et al. Temperature-stable dielectric ceramics based on Na0.5Bi0.5TiO3. J Eur Ceram Soc 2018, 38: 1548-1555.
[16]
Du HL, Zhou WC, Luo F, et al. Phase structure, dielectric properties, and relaxor behavior of (K0.5Na0.5)NbO3- (Ba0.5Sr0.5)TiO3 lead-free solid solution for high temperature applications. J Appl Phys 2009, 105: 124104.
[17]
Cheng HL, Zhou WC, Du HL, et al. Enhanced dielectric relaxor properties in (1-x)(K0.5Na0.5)NbO3- x(Ba0.6Sr0.4)0.7Bi0.2TiO3 lead-free ceramic. J Alloys Compd 2013, 579: 192-197.
[18]
Chen XL, Wang YL, Chen J, et al. Dielectric properties and impedance analysis of K0.5Na0.5NbO3-Ba2NaNb5O15 ceramics with good dielectric temperature stability. J Am Ceram Soc 2013, 96: 3489-3493.
[19]
Liu LJ, Knapp M, Ehrenberg H, et al. Average vs. local structure and composition property phase diagram of K0.5Na0.5NbO3-Bi1/2Na1/2TiO3 system. J Eur Ceram Soc 2017, 37: 1387-1399.
[20]
Yan TX, Ren SK, Ma X, et al. Dielectric properties of (Bi0.5K0.5)ZrO3 modified (K0.5Na0.5)NbO3 ceramics as high temperature ceramic capacitors. J Electron Mater 2018, 47: 7106-7113.
[21]
Du HL, Zhou WC, Luo F, et al. High Tm lead-free relaxor ferroelectrics with broad temperature usage range: 0.04BiScO3-0.96(K0.5Na0.5)NbO3. J Appl Phys 2008, 104: 044104.
[22]
Cheng HL, Du HL, Zhou WC, et al. Bi(Zn2/3Nb1/3)O3- (K0.5Na0.5)NbO3 high-temperature lead-free ferroelectric ceramics with low capacitance variation in a broad temperature usage range. J Am Ceram Soc 2013, 96: 833-837.
[23]
Liu ZY, Fan HQ, Li MM. High temperature stable dielectric properties of (K0.5Na0.5)0.985Bi0.015Nb0.99Cu0.01O3 ceramics with core-shell microstructures. J Mater Chem C 2015, 3: 5851-5858.
[24]
Zuo RZ, Fang XS, Ye C. Phase structures and electrical properties of new lead-free (Na0.5K0.5)NbO3-(Bi0.5Na0.5)TiO3 ceramics. Appl Phys Lett 2007, 90: 092904.
[25]
Long CB, Li TY, Fan HQ, et al. Li-substituted K0.5Na0.5NbO3-based piezoelectric ceramics: Crystal structures and the effect of atmosphere on electrical properties. J Alloys Compd 2016, 658: 839-847.
[26]
Wang RP, Itoh M. Phase diagram of (Na0.5K0.5)NbO3- (Bi0.5Na0.5)ZrO3 solid solution. J Adv Dielect 2016, 6: 1650014.
[27]
Hewat AW. Cubic-tetragonal-orthorhombic-rhombohedral ferroelectric transitions in perovskite potassium niobate: Neutron powder profile refinement of the structures. J Phys C: Solid State Phys 1973, 6: 2559-2572.
[28]
Shannon RD. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallogr Sect A 1976, 32: 751-767.
[29]
Du HL, Zhou WC, Zhu DM, et al. Sintering characteristic, microstructure, and dielectric relaxor behavior of (K0.5Na0.5)NbO3-(Bi0.5Na0.5)TiO3 lead-free ceramics. J Am Ceram Soc 2008, 91: 2903-2909.
[30]
Chen XL, Chen J, Ma DD, et al. High relative permittivity, low dielectric loss and good thermal stability of novel (K0.5Na0.5)NbO3-Bi(Zn0.75W0.25)O3 solid solution. Mater Lett 2015, 145: 247-249.
[31]
Liang WF, Wu WJ, Xiao DQ, et al. Construction of new morphotropic phase boundary in 0.94(K0.4-xNa0.6BaxNb1-xZrx)O3-0.06LiSbO3 lead-free piezoelectric ceramics. J Mater Sci 2011, 46: 6871-6876.
[32]
Guo YP, Kakimoto KI, Ohsato H. Dielectric and piezoelectric properties of lead-free (Na0.5K0.5)NbO3-SrTiO3 ceramics. Solid State Commun 2004, 129: 279-284.
[33]
Uchino K, Nomura S. Critical exponents of the dielectric constants in diffused-phase-transition crystals. Ferroelectrics 1982, 44: 55-61.
[34]
Liu LJ, Knapp M, Ehrenberg H, et al. The phase diagram of K0.5Na0.5NbO3-Bi1/2Na1/2TiO3. J Appl Crystallogr 2016, 49: 574-584.
[35]
Liu LJ, Knapp M, Schmitt LA, et al. Structure and dielectric dispersion in cubic-like 0.5K0.5Na0.5NbO3-0.5Na1/2Bi1/2TiO3 ceramic. EPL Europhys Lett 2016, 114: 47011.
[36]
Bokov AA, Ye ZG. Recent progress in relaxor ferroelectrics with perovskite structure. J Mater Sci 2006, 41: 31-52.
[37]
Wu JG, Wang J. Ferroelectric and impedance behavior of La- and Ti-codoped BiFeO3 thin films. J Am Ceram Soc 2010, 93: 2795-2803.
[38]
Wu JG, Xiao DQ, Zhu JG. Potassium-sodium niobate lead-free piezoelectric materials: Past, present, and future of phase boundaries. Chem Rev 2015, 115: 2559-2595.
[39]
Yan TX, Sun XJ, Deng JM, et al. Dielectric and conductivity behavior of Mn-doped K0.5Na0.5NbO3 single crystal. Solid State Commun 2017, 264: 1-5.
[40]
Boukriba M, Sediri F, Gharbi N. Hydrothermal synthesis and electrical properties of NaNbO3. Mater Res Bull 2013, 48: 574-580.
[41]
Liu LJ, Wu MX, Huang YM, et al. Frequency and temperature dependent dielectric and conductivity behavior of 0.95(K0.5Na0.5)NbO3-0.05BaTiO3 ceramic. Mater Chem Phys 2011, 126: 769-772.
[42]
Li TY, Fan HQ, Long CB, et al. Defect dipoles and electrical properties of magnesium B-site substituted sodium potassium niobates. J Alloys Compd 2014, 609: 60-67.
[43]
Abdelkafi Z, Abdelmoula N, Khemakhem H, et al. Dielectric relaxation in BaTi0.85(Fe1/2Nb1/2)0.15O3 perovskite ceramic. J Appl Phys 2006, 100: 114111.
[44]
Liu LJ, Fan HQ, Fang L, et al. Effects of Na/K evaporation on electrical properties and intrinsic defects in Na0.5K0.5NbO3 ceramics. Mater Chem Phys 2009, 117: 138-141.
Publication history
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Publication history

Received: 14 November 2020
Revised: 03 March 2021
Accepted: 10 March 2021
Published: 05 August 2021
Issue date: August 2021

Copyright

© The Author(s) 2021

Acknowledgements

This work was supported by the Natural Science Foundation of Guangxi (Grant Nos. 2019GXNSFBA245069, AA138162, GA245006, and AA294014), the Middle-aged and Young Teachers’ Basic Ability Promotion Project of Guangxi (Grant No. 2019KY0290), the Guilin University of Technology (Grant No. GUTQDJJ20176612037), the High Level Innovation Team and Outstanding Scholar Program of Guangxi Institutes, the Open Research Program of Key Laboratory of RF Circuit and System, Ministry of Education, and the Key Laboratory of Large Scale Integrated Design of Zhejiang.

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