Journal Home > Volume 10 , Issue 1

Lead-free Na0.5Bi0.5TiO3 (NBT) ceramics were prepared via a conventional oxide-mixed sintering route and their electrical transport properties were investigated. Direct current (DC, σDC) and alternating current (AC, σAC) electrical conductivity values, polarization current (first measurements) and depolarization current, current-voltage (I-U) characteristics (first measurements), and the Seebeck coefficient (α) were determined under various conditions. The mechanism of depolarization and the electrical conductivity phenomena observed for the investigated samples were found to be typical. For low voltages, the I-U characteristics were in good agreement with Ohm’s law; for higher voltages, the observed dependences were I-U2, I-U4, and then I-U6. The low-frequency σAC followed the formula σACs (ω is the angular frequency and s is the frequency exponent). The exponent s was equal to 0.18-0.77 and 0.73-0.99 in the low- and high-frequency regions, respectively, and decreased with temperature increasing. It was shown that conduction mechanisms involved the hopping of charge carriers at low temperatures, small polarons at intermediate temperatures, and oxygen vacancies at high temperatures. Based on AC conductivity data, the density of states at the Fermi-level, and the minimum hopping length were estimated. Electrical conduction was found to undergo p-n-p transitions with increasing temperature. These transitions occurred at depolarization temperature Td, 280 ℃, and temperature of the maximum of electric permittivity Tm is as typical of NBT materials.


menu
Abstract
Full text
Outline
About this article

Electrical transport in lead-free Na0.5Bi0.5TiO3 ceramics

Show Author's information J. SUCHANICZaK. KLUCZEWSKA-CHMIELARZa( )D. SITKObG. JAGŁOa
Institute of Technology, Pedagogical University, ul. Podchorazych 2, 30-084 Krakow, Poland
Institute of Physics, Pedagogical University, ul. Podchorazych 2, 30-084 Krakow, Poland

Abstract

Lead-free Na0.5Bi0.5TiO3 (NBT) ceramics were prepared via a conventional oxide-mixed sintering route and their electrical transport properties were investigated. Direct current (DC, σDC) and alternating current (AC, σAC) electrical conductivity values, polarization current (first measurements) and depolarization current, current-voltage (I-U) characteristics (first measurements), and the Seebeck coefficient (α) were determined under various conditions. The mechanism of depolarization and the electrical conductivity phenomena observed for the investigated samples were found to be typical. For low voltages, the I-U characteristics were in good agreement with Ohm’s law; for higher voltages, the observed dependences were I-U2, I-U4, and then I-U6. The low-frequency σAC followed the formula σACs (ω is the angular frequency and s is the frequency exponent). The exponent s was equal to 0.18-0.77 and 0.73-0.99 in the low- and high-frequency regions, respectively, and decreased with temperature increasing. It was shown that conduction mechanisms involved the hopping of charge carriers at low temperatures, small polarons at intermediate temperatures, and oxygen vacancies at high temperatures. Based on AC conductivity data, the density of states at the Fermi-level, and the minimum hopping length were estimated. Electrical conduction was found to undergo p-n-p transitions with increasing temperature. These transitions occurred at depolarization temperature Td, 280 ℃, and temperature of the maximum of electric permittivity Tm is as typical of NBT materials.

Keywords: electrical properties, Na0.5Bi0.5TiO3 (NBT) ceramics, Seebeck coefficient, impedance spectroscopy

References(55)

[1]
HX Fu, RE Cohen. Polarization rotation mechanism for ultrahigh electromechanical response in single-crystal piezoelectrics. Nature 2000, 403: 281-283.
[2]
MH Lee, DJ Kim, JS Park, et al. High-performance lead-free piezoceramics with high curie temperatures. Adv Mater 2015, 27: 6976-6982.
[3]
J Suchanicz, K Kluczewska, P Czaja, et al. The influence of electric poling on structural, thermal, dielectric and ferroelectric properties of Na0.5Bi0.5TiO3 ceramics. Ceram Int 2017, 43: 17194-17201.
[4]
LJ Liu, Z Yang, MX Wu, et al. Dielectric properties of (NaBi(1-x)Kx)0.5Ti(1-x)NbxO3 ceramics fabricated by mechanical alloying. J Alloys Compd 2010, 507: 196-200.
[5]
J Suchanicz, K Kluczewska, P Czaja, et al. Influence of sintering conditions on structural, thermal, electric and ferroelectric properties of Na0.5Bi0.5TiO3 ceramics. Phase Transit 2018, 91: 26-37.
[6]
H Lidjici, B Lagoun, M Berrahal, et al. XRD, Raman and electrical studies on the (1-x)(Na0.5Bi0.5)TiO3-xBaTiO3 lead free ceramics. J Alloys Compd 2015, 618: 643-648.
[7]
J Suchanicz, JP Mercurio, K Konieczny. Electric properties of (Na0.5Bi0.5)0.86Ba0.14TiO3 single crystal. Ferroelectrics 2002, 268: 357-362.
[8]
Y Hiruma, R Aoyagi, H Nagata, et al. Ferroelectric and piezoelectric properties of K0.5Bi0.5TiO3 ceramics. Jpn J Appl Phys 2005, 44: 5040-5044.
[9]
J Suchanicz, A Kania, P Czaja, et al. Structural, thermal, dielectric and ferroelectric properties of K0.5Bi0.5TiO3 ceramics. J Eur Ceram Soc 2018, 38: 567-574.
[10]
L Liu, M Knapp, H Ehrenberg, et al. The phase diagram of K0.5Bi0.5TiO3-Na0.5Bi0.5TiO3. J Appl Cryst 2016, 49: 574-584.
[11]
J Suchanicz, I Faszczowy, D Sitko, et al. Structural, thermal, dielectric and ferroelectric properties of Na0.5K0.5NbO3 and Na0.5K0.5NbO3+0.5mol%MnO2 ceramics. Phase Transit 2014, 87: 992-1001.
[12]
D Hu, ZB Pan, X Zhang, et al. Greatly enhanced discharge energy density and efficiency of novel relaxation ferroelectric BNT-BKT-based ceramics. J Mater Chem C 2020, 8: 591-601.
[13]
D Hu, ZB Pan, ZY He, et al. Significantly improved recoverable energy density and ultrafast discharge rate of Na0.5Bi0.5TiO3-based ceramics. Ceram Int 2020, 46: 15364-15371.
[14]
J Ding, ZB Pan, PX Chen, et al. Enhanced energy storage capability of (1-x)Na0.5Bi0.5TiO3-xSr0.7Bi0.2TiO3 free-lead relaxor ferroelectric thin films. Ceram Int 2020, 46: 14816-14821.
[15]
GO Jones, PA Thomas. Investigation of the structure and phase transitions in the novel A-site substituted distorted perovskite compound Na0.5Bi0.5TiO3. Acta Crystallogr Sect B 2002, 58: 168-178.
[16]
J Kusz, J Suchanicz, H Böhm, et al. High temperature X-ray single crystal study of Na0.5Bi0.5TiO3. Phase Transit 1999, 70: 223-229.
[17]
J Suchanicz, J Kusz, H Böhm, et al. Structural and electric properties of (Na0.5Bi0.5)0.88Ba0.12TiO3. J Mater Sci 2007, 42: 7827-7831.
[18]
GO Jones, PA Thomas. The tetragonal phase of Na0.5Bi0.5TiO3—A new variant of the perovskite structure. Acta Cryst B 2000, 56(Pt 3): 426-430.
[19]
J Suchanicz. Elastic constants of Na0.5Bi0.5TiO3 single crystal. J Mat Sci 2002, 37: 489-491.
[20]
J Suchanicz, U Lewczuk, K Konieczny. Effect of Ba doping on the structural, dielectric and ferroelectric properties of Na0.5Bi0.5TiO3 ceramics. Ferroelectrics 2016, 497: 85-91.
[21]
G Trolliard, V Dorcet. Reinvestigation of phase transitions in Na0.5Bi0.5TiO3 by TEM. Part II: Second order orthorhombic to tetragonal phase transition. Chem Mater 2008, 20: 5074-5082.
[22]
SB Vakhrushev, VA Isupov, BE Kvyatkovsky, et al. Phase transitions and soft modes in sodium bismuth titanate. Ferroelectrics 1985, 63: 153-160.
[23]
BK Barick, KK Mishra, AK Arora, et al. Impedance and Raman spectroscopic studies of Na0.5Bi0.5TiO3. J Phys D: Appl Phys 2011, 44: 355402.
[24]
J East, DC Sinclair. Characterization of (Bi1/2Na1/2)TiO3 using electric modulus spectroscopy. J Mater Sci Lett 1997, 16: 422-435.
[25]
BVB Saradhi, K Srinivas, G Prasad, SV Suryanarayana, T Bhimasankaram. Impedance spectroscopic studies in ferroelectric Na0.5Bi0.5TiO3. Mat Sci Eng B 2003, 98: 10-16.
[26]
M Karpierz, J Suchanicz, K Konieczny, et al. Effects of PbTiO3 doping on electric properties of Na0.5Bi0.5TiO3 ceramics. Phase Transit 2017, 90: 65-71.
[27]
J Petzelt, D Nuzhnyy, V Bovtun, et al. Peculiar Bi-ion dynamics in Na0.5Bi0.5TiO3 from terahertz and microwave dielectric spectroscopy. Phase Transiti 2014, 87: 953-965.
[28]
BN Rao, R Ranjan. Electric-field-driven monoclinic-to-rhombohedral transformation in Na0.5Bi0.5TiO3. Phys Rev B 2012, 86: 134103.
[29]
DE Jain Ruth, B Sundarakannan. Structural and Raman spectroscopic studies of poled lead-free piezoelectric sodium bismuth titanate ceramics. Ceram Int 2016, 42: 4475-4478.
[30]
[31]
JF Scott, CA Araujo, BM Melnick, et al. Quantitative measurement of space-charge effects in lead zirconate-titanate memories. J Appl Phys 1991, 70: 382-388.
[32]
K Kluczewska, D Sitko, J Suchanicz, et al. Isothermal depolarization currents of Na0.5Bi0.5TiO3 ceramics. Phase Transit 2018, 91: 1060-1066.
[33]
AA Grekov, NA Korchagina, ED Rogach, et al. Slow relaxation processes in SbSI crystals. Ferroelectrics 1982, 45: 71-75.
[34]
HH Wieder. Retarded polarization phenomena in BaTiO3 crystals. J Appl Phys 1956, 27: 413-416.
[35]
KC Kao, W Hwang. Electrical Transport in Solids. Oxford (UK): Pergamon Press, 1981.
[36]
CC Wang, CM Lei, GJ Wang, et al. Oxygen-vacancy-related dielectric relaxations in SrTiO3 at high temperatures. J Appl Phys 2013, 113: 094103.
[37]
R Selvamani, G Singh, VS Tiwari, et al. Oxygen vacancy related relaxation and conduction behavior in (1-x) NBT-xBiCrO3 solid solution. Phys Stat Sol (a) 2012, 209: 118-125.
[38]
LH Li, M Li, HR Zhang, et al. Controlling mixed conductivity in Na1/2Bi1/2TiO3 using A-site non-stoichiometry and Nb-donor doping. J Mater Chem C 2016, 4: 5779-5786.
[39]
AK Joncher. Dielectric Relaxation in Solids. London (UK): Chelsea Dielectric Press Ltd, 1983.
[40]
TA Cox. Transition Metal Oxides. Oxford (UK): Oxford University Press, 1992.
[41]
IG Austin, NF Mott. Polarons in crystalline and non-crystalline materials. Adv Phys 1969, 18: 41-102.
[42]
H Botter, VV Bryksin. Hopping Conduction in Solids. Berlin (Germany): Akademie Verlag, 1985.
[43]
GD Sharma, M Roy, MS Roy. Charge conduction mechanism and photovoltaic properties of 1,2-diazoamino diphenyl ethane (DDE) based Schottky device. Mater Sci Eng: B 2003, 104: 15-25.
[44]
R Salam. Trapping parameters of electronic defectes states in indium tin oxide from AC conductivity. Phys Stat Sol (a) 1990, 117: 535-540.
[45]
S Saha, SB Krupanidhi. Dielectric response in pulsed laser ablated (Ba,Sr)TiO3 thin films. J Appl Phys 2000, 87: 849-854.
[46]
A Rose. Space-charge-limited currents in solids. Phys Rev 1955, 97: 1538.
[47]
MA Lampert. Simplified theory of space-charge-limited currents in an insulator with traps. Phys Rev 1956, 103: 1648.
[48]
RM Huey, RM Taylor. Anomalous discharges in ferroelectrics. J Appl Phys 1963, 34: 1557-1560.
[49]
YA Grushevski, AI Sleptsov. Electronic polarization in SbSI near electrodes. Izv VUZ FIZ 1969, 12: 1546-1549.
[50]
VI Burgienko. ELectron traps in silver chloride crystals. Izv VUZ FIZ 1965, 8: 64-66.
[51]
RG Breckenridge, WR Hosler. Electrical properties of titanium dioxide semiconductors. Phys Rev 1953, 91: 793-802.
[52]
PB Macedo, CT Moynihan, R Bose. Role of ionic diffusion in polarization in vitreous ionic conductors. Phys Chem Glasses 1972, 13: 171-179.
[53]
CA Angell. Dynamic processes in ionic glasses. Chem Rev 1990, 90: 523-542.
[54]
M Li, MJ Pietrowski, RA De Souza, et al. A family of oxide ion conductors based on the ferroelectric perovskite Na0.5Bi0.5TiO3. Nat Mater 2014, 13: 31-35.
[55]
D Schütz, M Deluca, W Krauss, et al. Lone-pair-induced covalency as the cause of temperature- and field-induced instabilities in bismuth sodium titanate. Adv Funct Mater 2012, 22: 2285-2294.
Publication history
Copyright
Rights and permissions

Publication history

Received: 26 May 2020
Revised: 22 September 2020
Accepted: 15 October 2020
Published: 18 January 2021
Issue date: February 2021

Copyright

© The Author(s) 2020

Rights and permissions

This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

Return