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IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308
__________________________________________________________________________________________
Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 623
STRUCTURE, MICROSTRUCTURE AND DIELECTRIC STUDY OF
(Ba0.6Sr0.4)(Zr0.6Ti0.4)O3-Nb2O5-Fe2O3-RE (RE=La2O3,Gd2O3) CERAMICS
Chandrashekar M Tavade1
, Nagabasawanna G2
, R.L.Raibagkar3
Abstract
The influence of La and Gd doped on the microstructure and dielectric properties, including the phase structure, temperature
dependence of permittivity, (Ba0.6Sr0.4)(Zr0.6Ti0.4)O3–Nb2O5–Fe2O3(BSZT40NF) materials have been investigated by X-ray diffraction,
SEM, and LCR analyzer, respectively. Experimental results revealed that incorporation of proper content of La and Gd basically
soluted in the lattice of BSZT40NF and can control the grain growth, reduce the dielectric loss of the BSZT40NF materials. The
development of microstructure promoted by the additives can result in the improvement of the dielectric constant.
Keywords: Perovskite, BT, BSZT, Rare earth ion, SEM, dielectric properties.
----------------------------------------------------------------------***---------------------------------------------------------------------
1. INTRODUCTION
Barium titanate (BT) is the most widely used perovskite
structured ceramic compound which finds large number of
electronics applications among all perovskite structured
ceramics [1]. Doping process is undertaken for certain
properties of ceramics and dopant plays an important role in
modifying the ceramics behavior such as multilayer ceramics
capacitor, data storage media, high capacity memory cells and
thermistors etc. BT-based ferroelectric exhibiting high
dielectric nonlinearity has become one of the promising
materials to realize the potential applications for tunable
ceramic capacitors and tunable microwave devices [2, 3].
Barium strontium titanate (BST) is another vital material
which has significant performance in the microwave
frequency range, because of its large dielectric constant (εr)
and high dielectric tunability at room temperature has been
frequently used in the tunable filters [4]. Barium zirconate
titanate (BZT), as an important member of the BaTiO3-based
ferroelectric materials family, has received extensive attention
due to its eminent dielectric performance. BZT ceramics
present high voltage resistance characteristics because Zr4+
is
chemically more stable than Ti4+
[5-8]. Barium strontium
zirconate titanate (BSZT) has the advantages of both additives
Sr and Zr [9].
Dielectric materials with high tunability, low dielectric loss,
and moderate dielectric constant are desired for tunable
microwave applications. Many researchers [10–12] have
reported that better dielectric properties of BaTiO3-based
ferroelectric ceramics have been obtained by substitution of
some rare earth ions. Among them rare earth and transition
elements all most important kind of dopant, the
microstructural and dielectric properties of BSZT had been
reported [13].The effects of rare earth oxides on the dielectric
properties and reliability have been discussed in several recent
papers, [14, 15] whereas little research has been carried out
focusing on La2O3-doped BSZTNF. The microstructural and
dielectric properties of BSZTNF system have not been
reported to our knowledge. The Nb2O5 is a donor dopant,
which resulted in the lattice distortion and increased the
tetragonality, and Fe2O3 is an acceptor dopant, which led to
the high density of oxygen vacancy and promoted crystal grain
growth of BSZT ceramics. In this paper, we report the
influence of the rare earth elements such as La2O3, Gd2O3 on
the microstructure and dielectric properties of BSZTNF
materials.
2. EXPERIMENTAL
Ceramics samples were prepared by conventional solid slate
reaction method from the weighed amount of BaCO3, SrCO3,
ZrO2, TiO2, Nb2O5, Fe2O3, La2O3, and Gd2O3 (all hi media,
India purity 99.99%. The starting material were ground for 4
hours and calcined at 1000°C for 12 hours, they were further
ground for 2hours, and subjected for pre-sintering at 1000°C.
This product obtained was again ground for 2hours and
pressed into circular shaped disk pellet (diameter 10mm and
thickness 1-2mm) using 5% PVA as a binding agent. Pellets
were sintered at 1000°C for 8 hours for good electrical contact
a silver paste is applied on both the sides of pellets.
The room temperature X-ray diffractograms of synthesized
samples were recorded by using X-ray diffractometer. (
Phillips, X’perts-PRO, PAN analytical ) with Cu-Kα radiation
( λ = 1.54056Ǻ) with a step size of 0.02° and scanning rate of
2°/min., micrographs was taken from SEM (JSM / 8048 / SM,
JEOL, Japan and the grain size was determined by the linear
intercept technique and dielectric properties were measured by
LCR meter.
IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308
__________________________________________________________________________________________
Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 624
3. RESULTS AND DISCUSSION
The tolerance factor for the modified samples was calculated
with the ionic radius of A-site cation Ba2+
= 1.35 , Sr2+
=
1.13 , B-site cation Zr4+
= 0.79 Ti4+
= 0.88 Fe3+
=
0.64 , Nb5+
=0.70 , La3+ =
1.04 , Gd3+
= 0.94 and anion
O2-
= 1.4 , respectively, by Goldschmidt equation [16].
Fig 1: XRD pattern for BSZT40NFL and BSZT40NFG
The XRD patterns shown in figure 1 reveals that, all indexed
peaks corresponds to perovskite phase indicating single phase
of the compound. By the addition of rare earth ions (La and
Gd) shifts the phase transition temperature to lower values and
as a consequence, rhombohedral, orthorhombic and tetragonal
phases co-exists at room temperature in La and Gd doped
BSZT40NF materials. Cell volume, x-ray density and the
particle size was calculated and given in the Table 1.
Table-1 Crystallographic data of BSZT40NF-RE ceramics
Sample code
Lattice parameter (Ǻ) Cell
volume(Ǻ)3
Particle size
(nm)
X-ray density (ρ)
(gm/cm3
)A c c/a
BSZT40NFL 4.133 4.146 ≈1.00 70.84 2.31 22.04
BSZT40NFG 4.129 4.12 5 ≈1.00 70.34 2.60 24.24
From table 1, it is observed that the c/a ratio for the
BSZT40NFL, BSZT40NFG is almost equal to 1.00 which
leads to cubic phase transition [17].
Fig 2: Scanning electron micrographs of BSZT40NFL and BSZT40NFG
Figure 2 depicts the micrographs of the samples. By the
addition of La and Gd to BSZT40NF the grain size is of about
0.81nm and shows no appreciable difference in grain size in
the synthesized ceramic compounds. From figure 2, it is also
observed that BSZT40NFG show a small needle shape phase
located on grain boundaries. Such defect would affect the
transport phenomenon and thereby modifying the resistivity of
the material [18]
20 25 30 35 40 45 50 55 60 65 70
1000
2000
3000
4000
5000
6000
7000
8000
(100)
(220)
(211)
(200)
(111)
(110)
Intensity(Counts)
2 (degree)
BSZT40NFL(d)
20 25 30 35 40 45 50 55 60 65 70
1000
2000
3000
4000
5000
6000
7000
8000
9000
(220)
(211)
(200)
(111)
(110)
Intensity(Counts)
2 (degree)
BSZT40NFG(e)
IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308
__________________________________________________________________________________________
Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 625
Fig 3: Frequency dependence of dielectric constant for BSZT40NFL and BSZT40NFG
The frequency dependence of dielectric constant behaviour at
different temperatures for BSZT40NFL and BSZT40NFG are
shown in Fig.3. The dielectric properties are measured at
different temperatures (300
C, 500
C, 750
C and 1000
C)
respectively. Small frequency dispersion is observed for the
temperature 750
C and 1000
C. A strong dispersion is found at
the temperature 300
C and 500
C for the BSZT40NFL and
BSZT40NFG ceramics, respectively. The temperature Tm,
corresponding to the maximum value of the dielectric
constant, is shifted to higher temperature and the maximum
value of the dielectric constant is decreased with increasing
frequencies. This shows that samples have similar regularity in
the frequency dispersion. This phenomenon demonstrates
typical ferroelectric relaxor behavior.
4. CONCLUSIONS
BSZT40NFL and BSZT40NFG ceramics are fabricated via the
conventional solid-state reaction method. Rare-earth ions with
various ionic radii enter the unit cell to substitute for A-site
Ba2+
ions maintaining the perovskite structure of solid
solution. The rare-earth substituted ions are effective to inhibit
the grain growth. The grain size of ceramics is almost same
for both the samples and found to be 0.81nm.The typical
ferroelectric relaxor behavior is induced for rare-earth ion (La
and Gd) substituted BSZT40NF ceramics. The effect of La2O3
and Gd2O3 content on the microstructure and dielectric
properties has been investigated on ceramics in the ternary
system (Ba0.6Sr0.4)(Zr0.6Ti0.4)O3–Nb2O5–Fe2O3. The addition of
La and Gd induced that BSZT40NF ceramics has cubic
structures and that the solubility of Nb2O5 and Fe2O3 in BSZT
with 0.99 wt%, 1.465 wt% La and Gd is below 5.66 wt%. The
dielectric properties of BSZT ceramics with La and Gd
additions are strongly dependent on the densification and the
microstructure.
ACKNOWLEDGEMENTS
I would like to thank to the Principal and Management of
Rural Engineering College Bhalki for giving me an
opportunity to carry out research work in the Department of
Material science, Gulbarga University Gulbarga.
REFERENCES
[1]. B.Jaffe, W.Cook, H.Jaffe, Academic Press, London,
3120(1971)
[2]. P. Sciau, G. Calvarin, and J. Ravez, Solid State Commun.
113, 755 (2000)
[3]. W. Chang, J. S. Horwitz, A. C. Cater, J. M. Pond, S. W.
Kirchoefer, C. M. Gilmore, and D. B. Chrisey, Appl. Phys.
Lett. 74, 1033 (1999)
[4]. Y.Zhi, A.Chen, P.M. Vilarinho, P.Q.Mantas, and
J.L.Baptista, J. Eur. Ceram.Soc., vol.18, pp.1613- 1619
(1998).
[5]. J. W. Zhai, X. Yao, L. Y. Zhang, and B. Shen, Appl. Phys.
Lett. 84, 3136 (2006)
[6]. J. W. Zhai, D. Hu, X. Yao, Z. K. Xu, and H. Chen, J. Eur.
Ceram. Soc. 26, 1917 (2006).
[7]. Y. Zhi, A. Chen, R. Guo, and A. S. Bhalla, Appl. Phys.
Lett. 81, 1285 (2002)
[8]. T. Maiti, R. Guo, and A. S. Bhalla, Appl. Phys. Lett. 89,
122909 (2006)
[9]. Chandrashekhar M Tavade, Raghavendra Sagar,
Shivanand Madolappa, and R. L. Raibagkar.WJ S T, 1(8): 12-
14 (2011).
[10]. H. I. Hsiang and G. P. Lai, Mater. Sci. Eng., B B123, 69
(2005)
[11]. D. Y. Lu, M. Toda, and M. Sugano, J. Am. Ceram. Soc.
89, 3112 (2006)
[12]. X. H. Wang, W. Z. Lu, J. Liu, Y. L. Zhou, and D. X.
Zhou, J. Eur. Ceram. Soc. 26, 1981 (2006)
4 5 5 6 6
1200
1600
2000
2400
2800'
log f
BSZT40NFL T30 BSZT40NFL T50
BSZT40NFL T75 BSZT40NFL T100
(d)
4 5 5 6 6
250
500
750
1000
1250
'
log f
BSZT40NFG T30 BSZT40NFG T50
BSZT40NFG T75 BSZT40NFG T100
(e)
IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308
__________________________________________________________________________________________
Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 626
[13]. C. M. Tawade, Shivanand Madolappa, Nagbasavanna
Sharanappa, and R. L Raibagkar. IJRET,Vol.02 Issue: 08,
(2013)
[14]. C. H. Kim, K. J. Park, and Y. J. Yoon, J. Eur.Ceram.
Soc., 28 [6] 1213–9 (2008)
[15]. Yang Gong-An J. Am. Ceram. Soc., 92 [8] 1891–1894
(2009)
[16]. V.M.Goldschmidt,”Skr.Akad.oslo.”K12 117(1926)
[17]. In Chyuan, Shen li fu,J. Mat. Sci., 25 4699-4703 (1990)
[18]. Z.Ru-Bing, Y.Chun-Sheng, D.Gui-Pu, F.Jie , Mater.
Res.Bull., 40 1490-1496 (2005)

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Structure, microstructure and dielectric study of (ba0.6 sr0.4)(zr0.6ti0.4)o3 nb2o5-fe2o3-re (re=la2o3,gd2o3) ceramics

  • 1. IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308 __________________________________________________________________________________________ Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 623 STRUCTURE, MICROSTRUCTURE AND DIELECTRIC STUDY OF (Ba0.6Sr0.4)(Zr0.6Ti0.4)O3-Nb2O5-Fe2O3-RE (RE=La2O3,Gd2O3) CERAMICS Chandrashekar M Tavade1 , Nagabasawanna G2 , R.L.Raibagkar3 Abstract The influence of La and Gd doped on the microstructure and dielectric properties, including the phase structure, temperature dependence of permittivity, (Ba0.6Sr0.4)(Zr0.6Ti0.4)O3–Nb2O5–Fe2O3(BSZT40NF) materials have been investigated by X-ray diffraction, SEM, and LCR analyzer, respectively. Experimental results revealed that incorporation of proper content of La and Gd basically soluted in the lattice of BSZT40NF and can control the grain growth, reduce the dielectric loss of the BSZT40NF materials. The development of microstructure promoted by the additives can result in the improvement of the dielectric constant. Keywords: Perovskite, BT, BSZT, Rare earth ion, SEM, dielectric properties. ----------------------------------------------------------------------***--------------------------------------------------------------------- 1. INTRODUCTION Barium titanate (BT) is the most widely used perovskite structured ceramic compound which finds large number of electronics applications among all perovskite structured ceramics [1]. Doping process is undertaken for certain properties of ceramics and dopant plays an important role in modifying the ceramics behavior such as multilayer ceramics capacitor, data storage media, high capacity memory cells and thermistors etc. BT-based ferroelectric exhibiting high dielectric nonlinearity has become one of the promising materials to realize the potential applications for tunable ceramic capacitors and tunable microwave devices [2, 3]. Barium strontium titanate (BST) is another vital material which has significant performance in the microwave frequency range, because of its large dielectric constant (εr) and high dielectric tunability at room temperature has been frequently used in the tunable filters [4]. Barium zirconate titanate (BZT), as an important member of the BaTiO3-based ferroelectric materials family, has received extensive attention due to its eminent dielectric performance. BZT ceramics present high voltage resistance characteristics because Zr4+ is chemically more stable than Ti4+ [5-8]. Barium strontium zirconate titanate (BSZT) has the advantages of both additives Sr and Zr [9]. Dielectric materials with high tunability, low dielectric loss, and moderate dielectric constant are desired for tunable microwave applications. Many researchers [10–12] have reported that better dielectric properties of BaTiO3-based ferroelectric ceramics have been obtained by substitution of some rare earth ions. Among them rare earth and transition elements all most important kind of dopant, the microstructural and dielectric properties of BSZT had been reported [13].The effects of rare earth oxides on the dielectric properties and reliability have been discussed in several recent papers, [14, 15] whereas little research has been carried out focusing on La2O3-doped BSZTNF. The microstructural and dielectric properties of BSZTNF system have not been reported to our knowledge. The Nb2O5 is a donor dopant, which resulted in the lattice distortion and increased the tetragonality, and Fe2O3 is an acceptor dopant, which led to the high density of oxygen vacancy and promoted crystal grain growth of BSZT ceramics. In this paper, we report the influence of the rare earth elements such as La2O3, Gd2O3 on the microstructure and dielectric properties of BSZTNF materials. 2. EXPERIMENTAL Ceramics samples were prepared by conventional solid slate reaction method from the weighed amount of BaCO3, SrCO3, ZrO2, TiO2, Nb2O5, Fe2O3, La2O3, and Gd2O3 (all hi media, India purity 99.99%. The starting material were ground for 4 hours and calcined at 1000°C for 12 hours, they were further ground for 2hours, and subjected for pre-sintering at 1000°C. This product obtained was again ground for 2hours and pressed into circular shaped disk pellet (diameter 10mm and thickness 1-2mm) using 5% PVA as a binding agent. Pellets were sintered at 1000°C for 8 hours for good electrical contact a silver paste is applied on both the sides of pellets. The room temperature X-ray diffractograms of synthesized samples were recorded by using X-ray diffractometer. ( Phillips, X’perts-PRO, PAN analytical ) with Cu-Kα radiation ( λ = 1.54056Ǻ) with a step size of 0.02° and scanning rate of 2°/min., micrographs was taken from SEM (JSM / 8048 / SM, JEOL, Japan and the grain size was determined by the linear intercept technique and dielectric properties were measured by LCR meter.
  • 2. IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308 __________________________________________________________________________________________ Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 624 3. RESULTS AND DISCUSSION The tolerance factor for the modified samples was calculated with the ionic radius of A-site cation Ba2+ = 1.35 , Sr2+ = 1.13 , B-site cation Zr4+ = 0.79 Ti4+ = 0.88 Fe3+ = 0.64 , Nb5+ =0.70 , La3+ = 1.04 , Gd3+ = 0.94 and anion O2- = 1.4 , respectively, by Goldschmidt equation [16]. Fig 1: XRD pattern for BSZT40NFL and BSZT40NFG The XRD patterns shown in figure 1 reveals that, all indexed peaks corresponds to perovskite phase indicating single phase of the compound. By the addition of rare earth ions (La and Gd) shifts the phase transition temperature to lower values and as a consequence, rhombohedral, orthorhombic and tetragonal phases co-exists at room temperature in La and Gd doped BSZT40NF materials. Cell volume, x-ray density and the particle size was calculated and given in the Table 1. Table-1 Crystallographic data of BSZT40NF-RE ceramics Sample code Lattice parameter (Ǻ) Cell volume(Ǻ)3 Particle size (nm) X-ray density (ρ) (gm/cm3 )A c c/a BSZT40NFL 4.133 4.146 ≈1.00 70.84 2.31 22.04 BSZT40NFG 4.129 4.12 5 ≈1.00 70.34 2.60 24.24 From table 1, it is observed that the c/a ratio for the BSZT40NFL, BSZT40NFG is almost equal to 1.00 which leads to cubic phase transition [17]. Fig 2: Scanning electron micrographs of BSZT40NFL and BSZT40NFG Figure 2 depicts the micrographs of the samples. By the addition of La and Gd to BSZT40NF the grain size is of about 0.81nm and shows no appreciable difference in grain size in the synthesized ceramic compounds. From figure 2, it is also observed that BSZT40NFG show a small needle shape phase located on grain boundaries. Such defect would affect the transport phenomenon and thereby modifying the resistivity of the material [18] 20 25 30 35 40 45 50 55 60 65 70 1000 2000 3000 4000 5000 6000 7000 8000 (100) (220) (211) (200) (111) (110) Intensity(Counts) 2 (degree) BSZT40NFL(d) 20 25 30 35 40 45 50 55 60 65 70 1000 2000 3000 4000 5000 6000 7000 8000 9000 (220) (211) (200) (111) (110) Intensity(Counts) 2 (degree) BSZT40NFG(e)
  • 3. IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308 __________________________________________________________________________________________ Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 625 Fig 3: Frequency dependence of dielectric constant for BSZT40NFL and BSZT40NFG The frequency dependence of dielectric constant behaviour at different temperatures for BSZT40NFL and BSZT40NFG are shown in Fig.3. The dielectric properties are measured at different temperatures (300 C, 500 C, 750 C and 1000 C) respectively. Small frequency dispersion is observed for the temperature 750 C and 1000 C. A strong dispersion is found at the temperature 300 C and 500 C for the BSZT40NFL and BSZT40NFG ceramics, respectively. The temperature Tm, corresponding to the maximum value of the dielectric constant, is shifted to higher temperature and the maximum value of the dielectric constant is decreased with increasing frequencies. This shows that samples have similar regularity in the frequency dispersion. This phenomenon demonstrates typical ferroelectric relaxor behavior. 4. CONCLUSIONS BSZT40NFL and BSZT40NFG ceramics are fabricated via the conventional solid-state reaction method. Rare-earth ions with various ionic radii enter the unit cell to substitute for A-site Ba2+ ions maintaining the perovskite structure of solid solution. The rare-earth substituted ions are effective to inhibit the grain growth. The grain size of ceramics is almost same for both the samples and found to be 0.81nm.The typical ferroelectric relaxor behavior is induced for rare-earth ion (La and Gd) substituted BSZT40NF ceramics. The effect of La2O3 and Gd2O3 content on the microstructure and dielectric properties has been investigated on ceramics in the ternary system (Ba0.6Sr0.4)(Zr0.6Ti0.4)O3–Nb2O5–Fe2O3. The addition of La and Gd induced that BSZT40NF ceramics has cubic structures and that the solubility of Nb2O5 and Fe2O3 in BSZT with 0.99 wt%, 1.465 wt% La and Gd is below 5.66 wt%. The dielectric properties of BSZT ceramics with La and Gd additions are strongly dependent on the densification and the microstructure. ACKNOWLEDGEMENTS I would like to thank to the Principal and Management of Rural Engineering College Bhalki for giving me an opportunity to carry out research work in the Department of Material science, Gulbarga University Gulbarga. REFERENCES [1]. B.Jaffe, W.Cook, H.Jaffe, Academic Press, London, 3120(1971) [2]. P. Sciau, G. Calvarin, and J. Ravez, Solid State Commun. 113, 755 (2000) [3]. W. Chang, J. S. Horwitz, A. C. Cater, J. M. Pond, S. W. Kirchoefer, C. M. Gilmore, and D. B. Chrisey, Appl. Phys. Lett. 74, 1033 (1999) [4]. Y.Zhi, A.Chen, P.M. Vilarinho, P.Q.Mantas, and J.L.Baptista, J. Eur. Ceram.Soc., vol.18, pp.1613- 1619 (1998). [5]. J. W. Zhai, X. Yao, L. Y. Zhang, and B. Shen, Appl. Phys. Lett. 84, 3136 (2006) [6]. J. W. Zhai, D. Hu, X. Yao, Z. K. Xu, and H. Chen, J. Eur. Ceram. Soc. 26, 1917 (2006). [7]. Y. Zhi, A. Chen, R. Guo, and A. S. Bhalla, Appl. Phys. Lett. 81, 1285 (2002) [8]. T. Maiti, R. Guo, and A. S. Bhalla, Appl. Phys. Lett. 89, 122909 (2006) [9]. Chandrashekhar M Tavade, Raghavendra Sagar, Shivanand Madolappa, and R. L. Raibagkar.WJ S T, 1(8): 12- 14 (2011). [10]. H. I. Hsiang and G. P. Lai, Mater. Sci. Eng., B B123, 69 (2005) [11]. D. Y. Lu, M. Toda, and M. Sugano, J. Am. Ceram. Soc. 89, 3112 (2006) [12]. X. H. Wang, W. Z. Lu, J. Liu, Y. L. Zhou, and D. X. Zhou, J. Eur. Ceram. Soc. 26, 1981 (2006) 4 5 5 6 6 1200 1600 2000 2400 2800' log f BSZT40NFL T30 BSZT40NFL T50 BSZT40NFL T75 BSZT40NFL T100 (d) 4 5 5 6 6 250 500 750 1000 1250 ' log f BSZT40NFG T30 BSZT40NFG T50 BSZT40NFG T75 BSZT40NFG T100 (e)
  • 4. IJRET: International Journal of Research in Engineering and Technology eISSN: 2319-1163 | pISSN: 2321-7308 __________________________________________________________________________________________ Volume: 03 Special Issue: 03 | May-2014 | NERIET-2014, Available @ http://www.ijret.org 626 [13]. C. M. Tawade, Shivanand Madolappa, Nagbasavanna Sharanappa, and R. L Raibagkar. IJRET,Vol.02 Issue: 08, (2013) [14]. C. H. Kim, K. J. Park, and Y. J. Yoon, J. Eur.Ceram. Soc., 28 [6] 1213–9 (2008) [15]. Yang Gong-An J. Am. Ceram. Soc., 92 [8] 1891–1894 (2009) [16]. V.M.Goldschmidt,”Skr.Akad.oslo.”K12 117(1926) [17]. In Chyuan, Shen li fu,J. Mat. Sci., 25 4699-4703 (1990) [18]. Z.Ru-Bing, Y.Chun-Sheng, D.Gui-Pu, F.Jie , Mater. Res.Bull., 40 1490-1496 (2005)