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Journal of Advanced Ceramics  2014, Vol. 3 Issue (1): 17-30    doi: 10.1007/s40145-014-0089-x
Research Article     
Effect of sintering temperature on microstructure and electrical properties of Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions
Laboratory of Applied Mineral Chemistry, Department of Chemistry, Faculty of Sciences, University Tunis ElManar, Campus 2092, Tunis, Tunisia
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In this study, we investigated the effect of sintering temperature on densification, grain size, conductivity and dielectric properties of Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 ceramics, prepared by hydrothermal method. Pellets were sintered at different temperatures. Density increased with sintering temperature, reaching up to 96% at 800 ℃. A grain growth was observed with increasing sintering temperature. Impedance spectroscopy analyses of the sintered samples at various temperatures were performed. Increase in dielectric constant and in Curie temperature with sintering was discussed. Electrical conductivity and activation energy were calculated and attributed to the microstructural factors.

Key wordsceramics      sintering      light scattering      dielectric properties     
Received: 13 September 2013      Published: 10 June 2014
Corresponding Authors: Hana NACEUR   
Cite this article:

Hana NACEUR,Adel MEGRICHE,Mohamed EL MAAOUI. Effect of sintering temperature on microstructure and electrical properties of Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions. Journal of Advanced Ceramics, 2014, 3(1): 17-30.

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Fig. 1 Sintered density percentage as function of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 2 Sintered density percentage as function of sintering duration at 840 ℃ for Na0.5Bi2.5Nb2O9 ceramic.
Fig. 3 Densification factor as function of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 4 Thickness shrinkage percentage as function of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 5 Diameter shrinkage percentage as function of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 6 Mean grain size as function of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 7 Logarithm of average grain versus reciprocal of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 8 Activation energy of grain growth as function of composition.
Fig. 9 Dielectric constant as function of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 10 Curie temperature as function of sintering temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 11 Electrical conductivity as function of temperature at different sintering temperatures for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
Fig. 12 Arrhenius plots of electrical conductivities as function of temperature for Sr1-x(Na0.5Bi0.5)xBi2Nb2O9 solid solutions.
[1]   Wang PE, Chaki TK. Sintering behaviour and mechanical properties of hydroxyapatite and dicalcium phosphate. J Mater Sci: Mater M 1993, 4: 150–158.
[2]   G?k?e A, Findik F. Mechanical and physical properties of sintered aluminum powders. Journal of Achievements in Materials and Manufacturing Engineering 2008, 30: 157–164.
[3]   Mohan CRK, Bajpai PK. Effect of sintering optimization on the electrical properties of bulk BaxSr1-xTiO3 ceramics. Physica B 2008, 403: 2173–2188.
[4]   Hallmann L, Ulmer P, Reusser E, et al. Effect of dopants and sintering temperature on microstructure and low temperature degradation of dental Y-TZP-zirconia. J Eur Ceram Soc 2012, 32: 4091–4104.
[5]   Shaw NJ. Densification and coarsening during solid state sintering of ceramics: A review of the models III. Coarsening. Int J Powder Metall 1989, 21: 25–29.
[6]   Coondoo I, Jha AK, Agarwal SK. Enhancement of dielectric characteristics in donor doped Aurivillius SrBi2Ta2O9 ferroelectric ceramics. J Eur Ceram Soc 2007, 27: 253–260.
[7]   Kajewski D, Ujma Z, Szot K, et al. Dielectric properties and phase transition in SrBi2Nb2O9–SrBi2Ta2O9 solid solution. Ceram Int 2009, 35: 2351–2355.
[8]   Wu W, Liang S, Wang X, et al. Synthesis, structures and photocatalytic activities of microcrystalline ABi2Nb2O9 (A = Sr, Ba) powders. J Solid State Chem 2011, 184: 81–88.
[9]   Panda AB, Tarafdar A, Pramanik P. Synthesis, characterization and properties of nano-sized SrBi2Ta2O9 ceramics prepared by chemical routes. J Eur Ceram Soc 2004, 24: 3043–3048.
[10]   Dhak D, Dhak P, Pramanik P. Influence of substitution on dielectric and impedance spectroscopy of Sr1-xBi2+yNb2O9 ferroelectric ceramics synthesized by chemical route. Appl Surf Sci 2008, 254: 3078–3092.
[11]   Prasanta D, Debasis D, Kausikisankar P, et al. Studies of structural and electrical properties of Ca1−xBi2+yNb2O9 [0.0 ≤ x ≤ 0.4; 0.000 ≤ y ≤ 0.266] ferroelectric ceramics prepared by organic precursor decomposition method. Solid State Sci 2008, 10: 1936–1946.
[12]   Júnior NLA, Sim?es AZ, Cavalheiro AA, et al. Structural and microstructural characterization of SrBi2 (Ta0.5Nb0.48W0.02)2O9 powders. J Alloys Compd 2008, 454: 61–65.
[13]   Gaikwad SP, Dhage SR, Potdar HS, et al. Co-precipitation method for the preparation of nanocrystalline ferroelectric SrBi2Nb2O9 ceramics. J Electroceram 2005, 14: 83–87.
[14]   Gaikwad SP, Potdar HS, Samuel V, et al. Co-precipitation method for the preparation of fine ferroelectric BaBi2Nb2O9. Ceram Int 2005, 31: 379–381.
[15]   Radha R, Gupta UN, Samuel V, et al. A co-precipitation technique to prepare BiNbO4 powders. Ceram Int 2008, 34: 1565–1567.
[16]   Kato K, Zheng C, Finder JM, et al. Sol–gel route to ferroelectric layer-structured perovskite SrBi2Ta2O9 and SrBi2Nb2O9 thin films. J Am Ceram Soc 1998, 81: 1869–1875.
[17]   Nelis D, Van Werde K, Mondelaers D, et al. Aqueous solution–gel synthesis of strontium bismuth niobate (SrBi2Nb2O9). J Sol–Gel Sci Technol 2003, 26: 1125–1129.
[18]   Zanetti SM, Santiago EI, Bulh?es LOS, et al. Preparation of characterization of nanosized SrBi2Nb2O9 powder by the combustion synthesis. Mater Lett 2003, 57: 2812–2816.
[19]   Lu C-H, Chen Y-C. Sintering and decomposition of ferroelectric layered perovskites: Strontium bismuth tantalate ceramics. J Eur Ceram Soc 1999, 19: 2909–2915.
[20]   Chen D, Liu Y, Li Y, et al. Low-temperature sintering of M-type barium ferrite with BaCu(B2O5) additive. J Magn Magn Mater 2012, 324: 449–452.
[21]   Liu H, Li Q, Ma J, et al. Effects of Bi3+ content and grain size on electrical properties of SrBi2Ta2O9 ceramic. Mater Lett 2012, 76: 21–24.
[22]   Iqbal Y, Jamal A, Ullah R, et al. Effect of fluxing additive on sintering temperature, microstructure and properties of BaTiO3. Bull Mater Sci 2012, 35: 387–394.
[23]   Zhang P, Hua Y, Xia W, et al. Effect of H3BO3 on the low temperature sintering and microwave dielectric properties of Li2ZnTi3O8 ceramics. J Alloys Compd 2012, 534: 9–12.
[24]   Zhang G, Liu S, Yu Y, et al. Microstructure and electrical properties of (Pb0.87Ba0.1La0.02) (Zr0.68Sn0.24Ti0.08)O3 anti-ferroelectric ceramics fabricated by the hot-press sintering method. J Eur Ceram Soc 2013, 33: 113–121.
[25]   Nygren M, Shen Z. On the preparation of bio-, nano- and structural ceramics and composites by spark plasma sintering. Solid State Sci 2003, 5: 125–131.
[26]   Li J-F, Wang K, Zhang B-P, et al. Ferroelectric and piezoelectric properties of fine-grained Na0.5K0.5NbO3 lead-free piezoelectric ceramics prepared by spark plasma sintering. J Am Ceram Soc 2006, 89: 706–709.
[27]   Polotai A, Breece K, Dickey E, et al. A novel approach to sintering nanocrystalline barium titanate ceramics. J Am Ceram Soc 2005, 88: 3008–3012.
[28]   Wang X-H, Deng X-Y, Bai H-L, et al. Two-step sintering of ceramics with constant grain-size, II: BaTiO3 and Ni–Cu–Zn ferrite. J Am Ceram Soc 2006, 89: 438–443.
[29]   Fang J, Wang X, Tian Z, et al. Two-step sintering: An approach to broaden the sintering temperature range of alkaline niobate-based lead-free piezoceramics. J Am Ceram Soc 2010, 93: 3552–3555.
[30]   Senthil V, Badapanda T, Bose AC, et al. Impedance and electrical modulus study of microwave- sintered SrBi2Ta2O9 ceramic. ISRN Ceramics 2012, 2012: 943734.
[31]   Lu SW, Lee BI, Wang ZL, et al. Hydrothermal synthesis and structural characterization of BaTiO3 nanocrystals. J Cryst Growth 2000, 219: 269–276.
[32]   Dias A, Buono VTL, Ciminelli VST, et al. Hydrothermal synthesis and sintering of electroceramics. J Eur Ceram Soc 1999, 19: 1027–1030.
[33]   Li L, Gong Y-Q, Gong L-J, et al. Low-temperature hydro/solvothermal synthesis of Ta-modified K0.5Na0.5NbO3 powders and piezoelectric properties of corresponding ceramics. Mater Design 2012, 33: 362–366.
[34]   Hotta Y, Duran C, Sato K, et al. Densification and grain growth in BaTiO3 ceramics fabricated from nanopowders synthesized by ball-milling assisted hydrothermal reaction. J Eur Ceram Soc 2008, 28: 599–604.
[35]   Venkataraman BH, Varma KBR. Impedance and dielectric studies of ferroelectric SrBi2Nb2O9 ceramics. J Phys Chem Solids 2003, 64: 2105–2112.
[36]   Pookmanee P, Rujijanagul G, Ananta S, et al. Effect of sintering temperature on microstructure of hydrothermally prepared bismuth sodium titanate ceramics. J Eur Ceram Soc 2004, 24: 517–520.
[37]   Naceur H, Megriche A, Maaoui ME. Structural distortion and dielectric properties of Sr1−x(Na0.5Bi0.5)xBi2Nb2O9 (x = 0.0, 0.2, 0.5, 0.8 and 1.0). J Alloys Compd 2013, 46: 145–150.
[38]   Aoyagi R, Takeda H, Okamura S, et al. Synthesis and electrical properties of sodium bismuth niobate Na0.5Bi2.5Nb2O9. Mater Res Bull 2003, 38: 25–32.
[39]   Einstein A. Eine neue Bestimmung der Moleküldimensionen. Annalen der Physik 1906, 324: 289–306.
[40]   Garcia DE, Klein AN, Hotza D. Advanced ceramics with dense and fine-grained microstructures through fast firing. Rev Adv Mater Sci 2012, 30: 273–281.
[41]   Wang Q, Wang Q, Zhang X, et al. The effect of sintering temperature on the structure and degradability of strontium-doped calcium polyphosphate bioceramic. Ceram-Silikaty 2010, 54: 97–102.
[42]   Krishnan K, Sahay SS, Singh S, et al. Modeling the accelerated cyclic annealing kinetics. J Appl Phys 2006, 100: 093505.
[43]   Hungría T, Galy J, Castro A. Spark plasma sintering as a useful technique to the nanostructuration of piezo-ferroelectric materials. Adv Eng Mater 2009, 11: 615–631.
[44]   Hu M, Luo C, Tian H, et al. Phase evolution, crystal structure and dielectric behavior of (1-x)Nd(Zn0.5Ti0.5)O3+xBi(Zn0.5Ti0.5)O3 compound ceramics. J Alloys Compd 2011, 509: 2993–2999.
[45]   Skidmore TA, Milne SJ. Phase development during mixed-oxide processing of a [Na0.5K0.5NbO3]1-x– [LiTaO3]x powder. J Mater Res 2007, 22: 2265–2272.
[46]   Rivas-Vázquez LP, Rendón-Angeles JC, Rodríguez-Galicia JL, et al. Preparation of calcium doped LaCrO3 fine powders by hydrothermal method and its sintering. J Eur Ceram Soc 2006, 26: 81–88.
[47]   Mandoki NT, Courtois C, Champagne P, et al. Hydrothermal synthesis of doped PZT powders: Sintering and ceramic properties. Mater Lett 2004, 58: 2489–2493.
[48]   Yahya N, Masoud RAH, Daud H, et al. Synthesis of Al3Fe5O12 cubic structure by extremely low sintering temperature of sol gel technique. Am J Engg & Applied Sci 2009, 2: 76–79.
[49]   Cahn JW. The impurity-drag effect in grain boundary motion. Acta Metall 1962, 10: 789–798.
[50]   Shannon RD. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Cryst 1976, A32: 751–767.
[51]   Floro JA, Thompson CV, Carel R, et al. Competition between strain and interface energy during epitaxial grain growth in Ag films on Ni(001). J Mater Res 1994, 9: 2411–2424.
[52]   Shirsath SE, Kadam RH, Gaikwad AS, et al. Effect of sintering temperature and the particle size on the structural and magnetic properties of nanocrystalline Li0.5Fe2.5O4. J Magn Magn Mater 2011, 323: 3104–3108.
[53]   Cortés J, Valencia E. Phenomenological equations of the kinetics of heterogeneous adsorption with interaction between adsorbed molecules. Phys Rev B 1995, 51: 2621–2623.
[54]   Budworth DW. The selection of grain-growth control additives for the sintering of ceramic. Mineral Mag 1970, 37: 833–838.
[55]   Coble RL. Sintering crystalline solids. I. Intermediate and final state diffusion models. J Appl Phys 1961, 32: 787–792.
[56]   Dosdale T, Brook RJ. Comparison of diffusion data and of activation energies. J Am Ceram Soc 1983, 66: 392–395.
[57]   Fang T-T, Shiue J-T, Shiau F-S. On the evaluation of the activation energy of sintering. Mater Chem Phys 2003, 80: 108–113.
[58]   Jardiel T, Caballero AC, Villegas M. Sintering kinetic of Bi4Ti3O12 based ceramics. Bol Soc Esp Ceram 2006, 45: 202–206.
[59]   Kan Y, Wang P, Li Y, et al. Low-temperature sintering of Bi4Ti3O12 derived from co-precipitation method. Mater Lett 2002, 56: 910–914.
[60]   Wu A, Vilarinho PM, Salvado IMM, et al. Sol–gel preparation of lead zirconate titanate powders and ceramics: Effect of alkoxide stabilizers and lead precursors. J Am Ceram Soc 2000, 83: 1379–1385.
[61]   Shaikh PA, Kolekar YD. Study of microstructural, electrical and dielectric properties of perovskite (0.7) PMN–(0.3) PT ferroelectric at different sintering temperatures. J Anal Appl Pyrol 2012, 93: 41–46.
[62]   Prasad KVR, Raju AR, Varma KBR. Grain size effects on the dielectric properties of ferroelectric Bi2VO5.5 ceramics. J Mater Sci 1994, 29: 2691–2696.
[63]   Cheng ZX, Wang XL, Dou SX, et al. Ferroelectric properties of Bi3.25Sm0.75V0.02T2.98O12 thin film at elevated temperature. Appl Phys Lett 2007, 90: 222902.
[64]   Yan LC, Hassan J, Hashim M, et al. Effect of sintering temperatures on the microstructure and dielectric properties of SrTiO3. World Appl Sci J 2011, 15: 1614–1618.
[65]   Shannon RD. Dielectric polarizabilities of ions in oxides and fluorides. J Appl Phys 1993, 73: 348–366.
[66]   Su H, Zhang H, Tang X, et al. High-permeability and high-Curie temperature NiCuZn ferrite. J Magn Magn Mater 2004, 283: 157–163.
[67]   Chen XM, Ma HY, Ding W, et al. Microstructure, dielectric, and piezoelectric properties of Pb0.92Ba0.08Nb2O6–0.25 wt% TiO2 ceramics: Effect of sintering temperature. J Am Ceram Soc 2011, 94: 3364–3372.
[68]   Mishra P, Sonia, Kumar P. Effect of sintering temperature on dielectric, piezoelectric and ferroelectric properties of BZT–BCT 50/50 ceramics. J Alloys Compd 2012, 545: 210–215.
[69]   Bhuiyan MA, Hoque SM, Choudhury S. Effect of sintering temperature on microstructure and magnetic properties of NiFe2O4 prepared from nano size powder of NiO and Fe2O3. Journal of Bangladesh Academy of Sciences 2010, 34: 189–195.
[70]   Zhang Q, Zhang Y, Wang X, et al. Influence of sintering temperature on energy storage properties of BaTiO3–(Sr1-1.5xBix)TiO3 ceramics. Ceram Int 2012, 38: 4765–4770.
[71]   Wada N, Tanaka H, Hamaji Y, et al. Microstructures and dielectric properties of fine-grained BaTiO3 ceramics. Jpn J Appl Phys 1996, 35: 5141–5144.
[72]   Chen T-C, Thio C-L, Desu SB. Impedance spectroscopy of SrBi2Ta2O9 and SrBi2Nb2O9 ceramics correlation with fatigue behavior. J Mater Res 1997, 12: 2628–2637.
[73]   Shrivastava V, Jha AK, Mendiratta RG. Structural and electrical studies in La-substituted SrBi2Nb2O9 ferroelectric ceramics. Physica B 2006, 371: 337–342.
[74]   Forbess MJ, Seraji S, Wu Y, et al. Dielectric properties of layered perovskite SrxA1-xBi2Nb2O9 ferroelectrics (with A = La, Ca and x = 0, 0.1). Appl Phys Lett 2000, 76: 2934–2936.
[75]   He LX, Yoo HI. Effects of B-site ion (M) substitution on the ionic conductivity of (Li3xLa2/3-x)1+y/2(MyTi1-y)O3 (M = Al, Cr). Electrochim Acta 2003, 48: 1357–1366.
[76]   Kuang X, Allix MMB, Claridge JB, et al. Crystal structure, microwave dielectric properties and AC conductivity of B-cation deficient hexagonal perovskites La5MxTi4-xO15 (x = 0.5, 1; M = Zn, Mg, Ga, Al). J Mater Chem 2006, 16: 1038–1045.
[77]   Kr?ger FA. The chemistry of imperfect crystals. J Appl Cryst 1975, 8: 497–498.
[78]   Parkash OM, Mandal KD, Christopher CC, et al. Electrical behaviour of lanthanum- and cobalt-doped strontium stannate. Bull Mater Sci 1994, 17: 253–257.
[79]   Kant R, Singh K, Pandey OP. Microstructural and electrical behavior of Bi4V2-xCuxO11-δ (0≤x≤0.4). Ceram Int 2009, 35: 221–227.
[80]   Wang XP, Fang QF. Mechanical and dielectric relaxation studies on the mechanism of oxygen ion diffusion in La2Mo2O9. Phys Rev B 2002, 65: 064304.
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