Dielectric properties of unfilled tetragonal tungsten bronze Ba₄PrFe_0.5Nb_9.5O₃₀ ceramics

Abstract

In order to found new dielectrics ceramics in tungsten bronze structure, unfilled tungsten bronze (TB) ceramics with nominal formula Ba₄PrFe_0.5Nb_9.5O₃₀ were prepared by the solid state reaction method. The microstructure and dielectric properties were studied using powder X-ray diffraction, field emission scanning electron microscope, and variable temperature dielectric test system. The results show that the ceramics have a single phase and belong to the space group of P4bm with the cell of a = b = 12.4839(3) Å, c = 3.9409(5) Å, V = 614.192(2) ų. The frequency dependent dielectrics properties show that the ceramics have a Debye-like relaxation at room temperature, while the temperature dependent dielectrics properties indicate that the ceramics are a relaxor and the relaxation is due to the nanopolars and oxygen vacancies. The ceramics have a potential application in electronic ceramics as temperature-stable multilayer ceramic capacitors.

Keywords

unfilled tetragonal tungsten bronze / dielectric properties / ceramic

References

[1] Cohen RE. Relaxors Go Critical[J]. Nature, 2006, 441: 941-942.

[2] Anem S, Rao KS, Rao KH. Investigation of Lanthanum Substitution in Lead-free BNBT Ceramics for Transducer Applications[J]. Ceram. Int., 2016, 42: 15319-15326.

[3] Hu CZ, Hou LJ, Fang L, et al. Preparation and Dielectric Properties of Unfilled Tungsten Bronze Ferroelectrics Ba₄RETiNb₉O₃₀[J]. J. Alloy. Compd., 2013, 581: 547-552.

[4] Li WB, Zhou D, He B, et al. Structure and Dielectric Properties of Nd(Zn_1/2Ti_1/2)O₃-BaTiO₃ Ceramics for Energy Storage Applications[J]. J. Alloy. Compd., 2016, 685: 418-422.

[5] Qiao XS, Chen XM, Lian HL, et al. Dielectric, Ferroelectric, Piezoelectric Properties and Impedance Analysis of Nonstoichiometric (Bi_0.5Na_0.5)_(0.94+x)B_a0.06TiO₃ Ceramics[J]. J. Eur. Ceram. Soc., 2016, 36: 3995-4001.

[6] Yang P, Yang B, Hao SL, et al. Variation of Electrical Properties with Structural Vacancies in Ferroelectric Niobates (Sr_0.53Ba_0.47)_(2.5-0.5x)Na_xN-b₅O₁₅ Ceramics[J]. J. Alloy. Compd., 2016, 685: 175-185.

[7] Gao TT, Chen W, Zhu XN, et al. Dielectric and Ferroelectric Characteristics of Ba₄Pr₂Fe₂Nb₈O₃₀ Tungsten Bronze Ceramics[J]. Mater. Chem. Phys., 2016, 181: 47-53.

[8] Liu LL, Hou ZP, Quan XJ. Effect of Li⁺ Ion Occupancy on Microstructure and Dielectric Characteristics in KSr₂Nb₅O₁₅ Tungsten Bronze Ceramics[J]. Mater. Sci. Eng. B, 2016, 211: 1-6.

[9] Hu CZ, Sun Z, Zhu QH, et al. Dielectric and Ferroelectric Properties of Unfilled Tungsten Bronze KBa₃RNb₁₀O₃₀ Ceramics[J]. J. Mater. Sci. Mater. Electron., 2015, 26: 515-520.

[10] Simon A, Ravez J. Solid-state Chemistry and Non-linear Properties of Tetragonal Tungsten Bronzes Materials[J]. Comptes Rendus Chim., 2006, 9: 1268-1276.

[11] Rotaru A, Miller AJ, Arnold DC, et al. Towards Novel Multiferroic and Magnetoelectric Materials: Dipole Stability in Tetragonal Tungsten Bronzes[J]. Phil. Trans. R. Soc. A, 2014, 372: 20120451.

[12] Bijumon PV, Kohli V, Parkash O, et al. Dielectric Properties of Ba₅M-Ti₃A₇O₃₀ [M = Ce, Pr, Nd, Sm, Gd, Dy and Bi; A = Nb, Ta] Ceramics[J]. Mater. Sci. Eng. B, 2004, 113: 13-18.

[13] Shannigrahi SR, Choudhary RN, Kumar PA, et al. Phase Transition in Ba₅RTi₃Nb₇O₃₀ (R = Dy, Sm) Ferroelectric Ceramics[J]. J. Phys. Chem. Solids, 1998, 59: 737-742.

[14] Chen XM, Sun YH, Zheng XH. High Permittivity and Low Loss Dielectric Ceramics in the BaO-La₂O₃-TiO₂-Ta₂O₅ System[J]. J. Eur. Ceram. Soc., 2003, 23: 1571-1575.

[15] Stennett MC, Miles GC, Sharman J, et al. A New Family of Ferroelectric Tetragonal Tungsten Bronze Phases Ba₂MTi₂X₃O₁₅[J]. J. Eur. Ceram. Soc., 2005, 25: 2471-2475.

[16] Zhang J, Wang G, Gao F, et al. Influence of Sr/Ba Ratio on the Dielectric, Ferroelectric and Pyroelectric Properties of Strontium Barium Niobate Ceramics[J]. Ceram. Int., 2013, 39: 1971-1976.

[17] Huang CJ, Li K, Liu XQ, et al. Effects of A1/A2-Sites Occupancy upon Ferroelectric Transition in (Sr_xBa_1−x)Nb₂O₆ Tungsten Bronze Ceramics[J]. J. Am. Ceram. Soc., 2014, 97: 507-512.

[18] Elissalde C, Ravez J. Relaxation Mechanisms in Sr_0.3Ba_0.7Nb₂O₆[J]. J. Mater. Chem., 2000, 10: 681-683.

[19] Pandey CS, Schreuer J, Burianek M, et al. Relaxor Behavior of Ca_x-Ba_1-xNb₂O₆(0.18 ≤ x ≤ 0.35) Tuned by Ca/Ba Ratio and Investigated by Resonant Ultrasound Spectroscopy[J]. Phys. Rev.B, 2013, 87: 094.

[20] Pandey CS, Schreuer J, Burianek M, et al. Relaxor Behavior of Ferroelectric Ca_0.22Sr_0.12Ba_0.66Nb₂O₆[J]. Appl. Phys. Lett., 2013, 102: 022903.

[21] Wakiya N, Wang JK, Saiki A, et al. Synthesis and Dielectric Properties of Ba_1-xR_2x/3Nb₂O₆ (R: rare earth) With Tetragonal Tungsten Bronze Structure[J]. J. Eur. Ceram. Soc., 1999, 19: 1071-1075.

[22] Gardner J, Morrison FD. A-site Size Effect in a Family of Unfilled Ferroelectric Tetragonal Tungsten Bronzes: Ba₄R_0.67Nb₁₀O₃₀ (R = La, Nd, Sm, Gd, Dy and Y)[J]. Dal. Trans., 2014, 43: 11687-11695.

[23] Chen W, Yang WZ, Liu XQ, et al. Structural, Dielectric and Magnetic Properties of Ba₃SrLn₂Fe₂Nb₈O₃₀ (Ln = La, Nd, Sm) Filled Tungsten Bronze Ceramics[J]. J. Alloy. Compd., 2016, 675: 311-316.

[24] Ma HQ, Lin K, Liu LJ, et al. Structure and Electrical Properties of Tetragonal Tungsten Bronze Ba₂CeFeNb₄O₁₅[J]. Rsc Adv., 2015, 5: 76957-76962.

[25] Josse M, Heijboer P, Albino M, et al. Original Crystal-Chemical Behaviors in (Ba,Sr)₂Ln(Fe,Nb,Ta)₅O₁₅ Tetragonal Tungsten Bronze: Anion-Driven Properties Evidenced by Cationic Substitutions[J]. Crys. Growth Design, 2014, 14: 5428-5435.

[26] Albino M, Veber P, Pechev S, et al. Growth and Characterization of Ba₂LnFeNb₄O₁₅ (Ln = Pr, Nd, Sm, Eu) Relaxor Single Crystals[J]. Crys. Growth Design, 2014, 14: 500-512.

[27] Josse M, Bidault O, Roulland F, et al. The Ba₂LnFeNb₄O₁₅ “Tetragonal Tungsten Bronze”: Towards RT Composite Multiferroics[J]. Solid State Sci., 2009, 11: 1118-1123.

[28] Hu CZ, Sun Z, Zhu QH, et al. Relaxor Behavior and Ferroelectric Properties of a New Ba₄SmFe_0.5Nb_9.5O₃₀ Tungsten Bronze Ceramic[J]. Ceram. Int., 2016, 42: 14999-15004.

[29] Coelho A. Coelho Software[CP]. Brisbane, Australia, 2007

[30] SHANNON RD. Revised Effective Ionic Radii and Systematic Studies of Interatomie Distances in Halides and Chaleogenides[J]. Acta Cryst., 1976, 32: 751-767.

[31] Bokov AA, Ye ZG. Dielectric Relaxation in Relaxor Ferroelectrics[J]. J. Adv. Dielectrics, 2012, 2: 1241010.

[32] Ravez J, Simon A. Some Solid State Chemistry Aspects of Lead-free Relaxor Ferroelectrics[J]. J. Solid State Chem., 2001, 162: 260-265.

[33] Li K, Zhu XL, Liu XQ, et al. Relaxor Ferroelectric Characteristics of Ba₅LaTi₃Nb₇O₃₀ Tungsten Bronze Ceramics[J]. Appl. Phys. Lett., 2012, 100: 012902.

[34] Gong G, Zerihun G, Fang Y, et al. Relaxor Behavior and Large Room-temperature Polarization of Ferroelectric Sr₄CaBiTi₃Nb₇O₃₀ Ceramics[J]. J. Am. Ceram. Soc., 2015, 98: 109-113.

[35] Ang C, Yu Z, Cross LE. Oxygen-vacancy-related Low-frequency Dielectric Relaxation and Electrical Conduction in Bi:SrTiO₃[J]. Phys. Rev. B, 2000, 62: 228-236.

[36] Padhee R, Das PR, Parida BN, et al. Dielectric and Electrical Properties of a Tungsten Bronze Tantalate Ceramic[J]. Curr. Appl. Phys., 2013, 13: 1014-1020.