Linear-like NaNbO3-based Lead-free Relaxor Antiferroelectric Ceramics with Excellent Energy-storage and Charge-discharge Properties

doi:10.15541/jim20230486

Abstract

Abstract:

Antiferroelectric (AFE) materials exhibit great potential in the application of high-performance dielectric energy storage capacitors due to their electric field-induced AFE-ferroelectric (FE) phase transition. However, the large hysteresis of field-induced phase transition makes it difficult to simultaneously achieve high energy-storage density (W_rec) and efficiency (η) for AFEs. This work improved the energy-storage performance of NaNbO₃-based lead-free AFE ceramics by introducing the third group Bi(Mg_0.5Ti_0.5)O₃ into 0.76NaNbO₃-0.24(Bi_0.5Na_0.5) TiO₃ to regulate its relaxation characteristics. Novel lead-free AFE ceramics, (0.76-x)NaNbO₃-0.24(Bi_0.5Na_0.5)TiO₃-xBi(Mg_0.5Ti_0.5)O₃, were prepared by a traditional solid-state reaction method. Their phase structure and microstructure as well as dielectric, energy-storage, and charge-discharge characteristics were studied. The results indicated that introduction of Bi(Mg_0.5Ti_0.5)O₃ obviously enhanced the dielectric relaxor behavior of the matrix without changing its AFE R-phase structure, which led to the significantly reduced polarization hysteresis. Especially, a linear-like polarization-field hysteresis loop with extremely-low hysteresis was obtained in the composition of x=0.050. At the same time, microstructure of the ceramic was effectively optimized, its dielectric constant decreased, and its breakdown strength had significant enhanced. As a result, a high W_rec=3.5 J/cm³ and a high η=93% were simultaneously achieved under a moderate electric field of 30 kV/mm in the x=0.050 ceramic. Moreover, the x=0.050 ceramic also exhibited excellent charge-discharge characteristics with a high-power density P_D=131(1±1%) MW/cm³, a high discharge energy density W_D=1.66(1±6%) J/cm³ and a fast discharge rate t_0.9<290 ns at 20 kV/mm. The charge-discharge properties maintained good stability within a wide temperature range of 25-125 ℃. These results indicate that 0.71NaNbO₃-0.24(Bi_0.5Na_0.5)TiO₃-0.050Bi(Mg_0.5Ti_0.5)O₃ ceramics can be expected to be applied in high-power energy-storage capacitors.

Key words: lead-free ceramic, antiferroelectric, relaxor behavior, energy-storage property, charge-discharge characteristic

CLC Number:

TQ174

SHI Ruijian, LEI Junwei, ZHANG Yi, XIE Aiwen, ZUO Ruzhong. Linear-like NaNbO₃-based Lead-free Relaxor Antiferroelectric Ceramics with Excellent Energy-storage and Charge-discharge Properties[J]. Journal of Inorganic Materials, 2024, 39(4): 423-431.

Figures/Tables 10

Fig. 1 XRD patterns of (0.76-x)NN-0.24BNT-xBMT ceramics with different composition at room temperature

Fig. 2 Rietveld refinement results of XRD patterns for (0.76-x)NN-0.24BNT-xBMT ceramics with different compositions (a) x=0; (b) x=0.025; (c) x=0.050; (d) x=0.075

Table 1 Refined structural parameters of full spectrum fitting for (0.76-x)NN-0.24BNT-xBMT ceramics

x	Space group	Lattice parameters	V/nm³	R_wp/%	R_p/%	χ²
0	Pnma	a=0.77920 nm, b=0.77852 nm, c=2.33854 nm, α=β=γ=90^o	1.418608	5.35	3.70	3.62
0.025	Pnma	a=0.77965 nm, b=0.77897 nm, c=2.34045 nm, α=β=γ=90^o	1.421413	5.20	3.62	3.59
0.050	Pnma	a=0.77899 nm, b=0.77995 nm, c=2.33913 nm, α=β=γ=90^o	1.421193	6.27	4.05	4.17
0.075	Pnma	a=0.78060 nm, b=0.78000 nm, c=2.34481 nm, α=β=γ=90^o	1.427666	4.99	3.56	2.96

Fig. 3 Evolution of lattice constant ratios for (0.76-x)NN-0.24BNT-xBMT ceramics with composition

Fig. 4 Grains morphologies of thermally etched surfaces of (0.76-x)NN-0.24BNT-xBMT ceramics and corresponding grain distributions

Fig. 5 Temperature dependent curves of εr and tanδ of (0.76-x)NN- 0.24BNT-xBMT ceramics

Fig. 6 Weibull distributions of (0.76-x)NN-0.24BNT-xBMT ceramics breakdown resistance (a) and variation of EB with composition (b)

Fig. 7 Energy-storage properties of (0.76-x)NN-0.24BNT-xBMT ceramics (a, b) P-E hysteresis loops (a) and energy-storage performance (b) of different compositions measured at 20 kV/mm; (c, d) P-E hysteresis loops (c) and energy-storage performance (d) of the x=0.050 ceramic measured under different electric fields

Fig. 8 Electric field-dependent charge-discharge characteristics of (0.76-x)NN-0.24BNT-xBMT (x=0.050) ceramics (a, b) Overdamped discharging current curves (a) and WD versus time curves (b) of the x=0.050 ceramic under different electric fields; (c, d) Underdamped discharging curves (c) and variation of PD, WD, and t0.9 (d) of the x=0.050 ceramics

Fig. 9 Temperature-dependent charge-discharge characteristics of (0.76-x)NN-0.24BNT-xBMT (x=0.050) ceramics (a, b) Overdamped discharging current curves (a) and WD versus time curves (b) of the x=0.050 ceramic under different electric fields; (c, d) Underdamped discharging curves (c) and variation of PD, WD, and t0.9 (d) of the x=0.050 ceramics

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Linear-like NaNbO₃-based Lead-free Relaxor Antiferroelectric Ceramics with Excellent Energy-storage and Charge-discharge Properties

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