Materials Today: Proceedings
Effect of Sn on the energy storage performance and electric conduction mechanisms of BCZT ceramic
Introduction
Barium titanate (BaTiO3 or BT)- based materials have been intensively studied for their interesting electrical properties for instance low dielectric loss, high dielectric constant, and ferroelectric behavior. The ferroelectric materials derived from BT have been used for an immense range of applications in electronic devices, functioning as pulse generating devices, multilayer ceramic capacitors, actuators, infrared detectors, voltage tunable devices in microwave electronics, and charge storage devices [1], [2].
Doping of ferroelectric can be used as an effective strategy to tune several functional properties. It has been found that doping BT with different dopants could extremely contribute to the enhancement of the piezoelectric and dielectric properties. For instance it has been reported that doping of BT with Ca2+ and Zr4+ (BaTiO3-CaTiO3-BaZrO3 solid solutions) lead to dramatically enhanced piezoelectric properties (d33 ∼ 620pC/N) with relatively low Curie temperature (TC ∼ 93 °C) for xBa(Zr0.2Ti0.8)O3–(1-x)(Ba0.7Ca0.3)TiO3 (x = 0.5) (BCZT) composition [3].
It should be pointed out that the electrical properties of ceramics fabricated by the solid-state method, are sensitive to the sintering conditions [4], [5], [6]. Moreover, high sintering temperature generally contributes to the formation of impurity phases and a large value of the dielectric loss, which is considered as imperfection in the majority of electronic applications [4]. On the other hand, BCZT ceramics synthesized by wet chemical techniques for instance sol–gel method depicted an excellent electrical performance compared to the ceramics prepared by the solid-state method due to the good stoichiometric composition of the resultant phase, nanoparticle sizes control, reduction in the processing temperatures and the chemical purity [7].
Many research groups have reported the beneficial effect of Sn4+ on enhancing the dielectric properties, the diffuse phase transition, the electrocaloric and energy storage properties of BCZT ceramics [8]. Also it is worth to mention that the ferroelectric–paraelectric (FE– PE) phase could be shifted towards room temperature as Sn4+ ion dopant content increases in BCZT [9], [10], [11], [12], [13], [14], [15]. Mondal et al have reported that the lattice distortion created by the relative difference in the radius of Ca2+ and Ba2+ ions in Ba1-xCaxZr0.1Ti0.9O3 (BCZT) system resulted in the enhancement in the grain boundary resistivity of the Ca doped BZT [16].
In this study, we investigate the effect of Sn substitution on the energy storage performance, and conduction mechanism of (Ba0.85Ca0.15) (Zr0.1-x Snx Ti0.9)O3(x = 0, 0.02, 0.04, and 0.06) ceramics.
Section snippets
Experimental section
(Ba0.85 Ca0.15) (Zr0.1-x Snx Ti0.9) O3 (x = 0, 0.02, 0.04, and 0.06) ceramics were prepared by employing the sol–gel method as we reported previously [8], [17]. The resulting powders were calcined at 1000 °C for 4 h. Then, the pellets pressed at 2.5 ton /cm2 were sintered at 1350 °C for 2 h.
The complex impedance of the sintered ceramics was measured in the frequency range from 20 Hz to 1 MHz and the temperature ranging from 25 °C to 450 °C by using a precision HP 4284A LCR Meter. The function
Energy storage performance
Energy storage referring to the capture of energy generated at one time and consumed at a later time. In the case of nonlinear dielectrics, the energy storage performances such as total energy density (Wtot), recoverable energy density (Wrec), and energy storage efficiency (ɳ) could be determined using the following equations:
* * 100 (3)where Pmax, Pr, E, Wtot, Wrec, Wloss, and ɳ described as maximum polarization, remnant polarization, applied
Complex impedance spectroscopy
The electrical properties of the Sn doped BCZT ceramics have been investigated using complex impedance spectroscopy (CIS). It is a commonly used method to analyze the electrical properties of the polycrystalline materials. The measurement of the resistance and capacistance as a fuction of frequency and temperature allows to differentiate between the grains and grain boundaries distributions. Data can be presented through electrical impedance Z*, electric modulus M*, and dielectric permittivity
The Nyquist diagram
Fig. 9(a-d) represents the Nyquist plots for the (Ba0.85Ca0.15)(Zr0.1-xSnxTi0.9)O3 ceramics for several temperature from the 300 °C to 400 °C range. It is clearly seen that all the samples show two semi-circles in the Nyquist plot which suggest that the polarization response in our system is due to the grain and grain boundary contributions. We also noticed that the heights of the semi-circles for both grain and grain boundary become smaller with increasing temperature. For both semi-circles,
AC conductivity analysis
Fig. 10 (a-d) depicts the electrical conductivity vs. frequency at different temperatures for (Ba0.85Ca0.15)(Ti0.9Zr0.1-xSnx)O3 ceramics. The nature of the variation of σ with temperature indicates that the character of the dispersion phenomenon of conductivity appears both in the low as well as in the high-frequency region. At higher temperatures, the low-frequency conductivity may be approximated to the dc conductivity (σdc), and the high-frequency region corresponds to the ac conductivity (σ
Conclusions
Lead-free (Ba0.85 Ca0.15) (Zr0.1-xSnxTi0.9) O3 (x = 0,0.02, 0.04 and 0.06) ceramics were prepared by sol–gel method , the effect of Sn on the energy storage performance and conduction mechanisms was studied systematically.
The highest recoverable energy density and efficiency were found for x = 0.02 of Sn (BCZT:Sn 2) composition (Wrec = 19 mJ/cm3 at 12 kV/cm and ɳ of 81.65%).
The prominent effect of Sn substitution on the electric properties of the ceramics was revealed. In particular, the net
CRediT authorship contribution statement
S. Belkhadir: Investigation, Writing - original draft, Visualization. S. Khardazi: Investigation. D. Mezzane: Conceptualization, Validation, Resources, Supervision. M. Amjoud: Conceptualization, Validation, Resources, Supervision. O. Shapovalova: Formal analysis, Resources. V. Laguta: Investigation. I. Raevski: Investigation. K. Pushkarova: Formal analysis, Resources. I. Lukyanchuk: Formal analysis, Resources. M. El Marssi: Formal analysis, Resources.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
The authors gratefully acknowledge the financial support of CNRST Priority Program PPR 15/2015 and the European H2020-MSCA-RISE-2017-ENGIMA action. IR acknowledges a support from the Ministry of Science and Higher Education of the Russian Federation [State task in the field of scientific activity, scientific project No. 0852-2020-0032 (BAS0110/20-3-08IF)].
References (38)
- et al.
Sintering temperature-induced electrical properties of (Ba0.90Ca0.10)(Ti0.85Zr0.15)O3 lead-free ceramics
Mater. Res. Bull.
(2012) - et al.
Effect of dwell time during sintering on piezoelectric properties of (Ba0.85Ca0.15)(Ti0.90Zr0.10)O3 lead-free ceramics
J. Alloys Compd.
(2011) - et al.
Structural, electrical and piezoelectric properties of nanocrystalline tin-substituted barium titanate ceramics
J. Alloys Compd.
(2011) - et al.
Multiscale study of ferroelectric – relaxor crossover in BaSn x Ti 1–x O 3 ceramics
J. Eur. Ceram. Soc.
(2014) - et al.
Effect of Ca2+ substitution on impedance and electrical conduction mechanism of Ba1- xCaxZr0.1Ti0.9O3 (0.00 ≤ x ≤ 0.20) ceramics
Phys. B Phys. Condens. Matter
(2017) - et al.
Impedance spectroscopy analysis of the diffuse phase transition in lead-free (Ba0.85Ca0.15)(Zr0.1Ti0.9)O3 ceramic elaborated by sol-gel method
Superlattices Microstruct.
(2019) - et al.
A.C. impedance analysis of the effect of dopant concentration on electrical properties of calcium modified BaSnO3
J. Alloys Compd.
(2005) - et al.
Enhancement of dielectric characteristics in donor doped Aurivillius SrBi2Ta2O9ferroelectric ceramics
J. Eur. Ceram. Soc.
(2007) - et al.
Barium zirconate-titanate / barium calcium-titanate ceramics via sol – gel process : novel high-energy-density capacitors
J. Phys Appl. Phys.
(2011) - et al.
Structure, dielectric, ferroelectric, and energy density properties of (1–x) BZT – x BCT ceramic capacitors for energy storage applications
J. Mater. Sci.
(2013)
Large piezoelectric effect in Pb-free ceramics
Phys. Rev. Lett.
Synthesis and characterization of pseudo-ternary Pb(Fe1/2Nb1/2)O3-PbZrO3-PbTiO3 ferroelectric ceramics via a B-site oxide mixing route
J. Mater. Sci.
Synthesis, structure, dielectric, piezoelectric, and energy storage performance of (Ba0.85Ca0.15)(Ti0.9Zr0.1)O3 ceramics prepared by different methods
J. Mater. Sci. Mater. Electron.
Structural, dielectric and electrocaloric properties of (Ba0.85Ca0.15) (Ti0.9Zr0.1−xSnx)O3 ceramics elaborated by sol–gel method
J. Mater. Sci. Mater. Electron.
Enhanced electrocaloric effect in lead-free BaTi 1–x Sn x O 3 ceramics near room temperature
Appl Phys Lett
Tunability and relaxor properties of ferroelectric barium stannate titanate ceramics
Appl. Phys. Lett.
Microstructure, dielectric properties and diffuse phase transition of barium stannate titanate ceramics
J. Mater. Sci. Mater. Electron.
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2022, Journal of Solid State ChemistryCitation Excerpt :At high temperature (120 °C), Hanani et al. [46] have found a Wtot and Wrec of 16.5 and 14 mJ/cm3 respectively, with an efficiency of 80% in BCZT ceramic. Later, Belkhadir et al. [47] reported an efficiency of 81.65% associated with Wtot and Wrec of 23.2 and 19 mJ/cm3 at 140 °C under a low electric field of 12 kV/cm, in BCZST ceramics prepared by sol-gel method. Fig. 8 displays the evolution of the pyroelectric coefficient as a function of temperature for BSTSn ceramic under a heating rate of 30 °C/min.