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    Phase Formation, Morphology and Electrical Properties of Lead-Free BNBLT-xBSN Ceramics Synthesized via the Solid-State Combustion Technique
    (2023-01-01)
    Thatawong, Bhoowadol
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    Rittidech, Aurawan
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    Bongkarn, Theerachai
    Lead-free 1-x(Bi<inf>0.47</inf>Na<inf>0.47</inf>Ba<inf>0.06</inf>)<inf>0.95</inf>La<inf>0.05</inf>TiO<inf>3</inf>-xBa(Sn<inf>0.70</inf>Nb<inf>0.24</inf>)O<inf>3</inf> (BNBLT-xBSN) ceramics with x = 0, 0.01, 0.02, 0.03 and 0.04 mol.% were synthesized by the solid-state combustion technique with a calcination temperature of 750 °C for 2 h and a sintering temperature of 1150 °C for 2 h. The effect of BSN substitution on the phase formation, microstructure, dielectric, ferroelectric and energy storage properties of the BNBLT ceramics was investigated. With the substitution of BSN, the coexisting rhombohedral (R) and tetragonal (T) phases transformed into coexisting R and cubic (C) phase, verified by Rietveld refinement. The C phase increased with increased BSN content. The average grain size decreased from 1.14 to 0.89 µm when x increased to 0.03 and then increased to 0.96 µm. The measured density and maximum dielectric constant (ε <inf>m</inf>) tended to increase from 5.44 to 5.87 g/cm<sup>3</sup> and 1800 to 1942 when x increased to 0.03, then decreased to 5.25 g/cm<sup>3</sup> and 1501, respectively. The remanent polarization (P <inf>r</inf>) and coercive field (E <inf>c</inf>) decreased when x increased to 0.03. The 0.97BNBLT-0.03BSN ceramic exhibited the lowest energy loss density (W <inf>loss</inf> ∼ 0.10 J/cm<sup>3</sup>) and the highest energy-storage efficiency (η ∼ 77.3%) measured under an electric field of 70 kV/cm.
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    Effect of Na+ Substitution on the Phase, Microstructure, Electrical and Energy Storage Properties of BSBZNT Ceramics Prepared by the Solid-State Combustion Technique
    (2023-01-01)
    Chongsatan, Wistsarut
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    Didpim, Ratirom
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    Julphunthong, Phongthorn
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    Thatawong, Bhoowadol
    ;
    (Ba<inf>0.704</inf>Sr<inf>0.176</inf>Bi<inf>0.12</inf>)<inf>1-x</inf>Zn<inf>0.08</inf>Nb<inf>0.04</inf>Ti<inf>0.88</inf>O<inf>3</inf>-Na<inf>x</inf> (BSBZNT-xNa) ceramics with x = 0, 0.01, 0.03 and 0.05 mol%, were prepared by the solid-state combustion technique. The samples were calcined and sintered at 950 °C and 1375 °C, respectively, for 2 h. The phase, microstructure, dielectric, ferroelectric and energy storage properties were investigated. The X-ray diffraction patterns of the BSBZNT-xNa powders showed a perovskite phase for all samples. When x increased from 0-0.03, the average particle size increased from 380 to 480 nm, then decreased to 420 nm. All sintered samples showed the coexistence of the orthorhombic and cubic phases. The average grain size was in the range of 2.03 to 1.39 µm. The BSBZNT-0.01Na ceramic exhibited the highest dielectric properties at room temperature (ɛ<inf>r</inf> = 902, tanδ = 0.10), the lowest remanent polarization (P <inf>r</inf> = 0.10 µC/cm<sup>2</sup>), coercive field (E <inf>c</inf> = 0.43 kV/cm), and the highest energy storage efficiency (η ∼ 94.70%) measured under an electric field of 70 kV/cm.
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    PHASE FORMATION AND ELECTRICAL PROPERTIES OF BCLTS CERAMICS SYNTHESIZED VIA THE SOLID-STATE COMBUSTION TECHNIQUE
    (2025-01-01)
    Somsri, Widchaya
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    Charoenthai, Nipaphat
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    Sutthapintu, Aekkasit
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    Noisak, Jitrawan
    ;
    Lead-free Ba<inf>0.93</inf>Ca<inf>0.04</inf>La<inf>0.03</inf>Ti<inf>0.90</inf>Sn<inf>0.10</inf>O<inf>3</inf> (BCLTS) ceramics were fabricated via solid-state combustion technique. The BCLTS powders were calcined in a temperature range of 1075-1175°C for 2h and sintered in a temperature range of 1350-1450°C for 2h. The BCLTS powders exhibited a pure perovskite phase when calcined above 1150°C. All BCLTS ceramic samples displayed a perovskite structure with coexisting cubic and tetragonal phases, with a secondary phase observed only at 1450°C. The growth of grain size was increased with increasing sintering temperature (0.42 to 0.65 μm.). The highest dielectric and ferroelectric properties (ε<inf>r</inf>=3047, tan δ<inf>r</inf> = 0.029, P<inf>max</inf> = 9.52 μC/cm<sup>2</sup>, P<inf>r</inf> = 0.48 μC/cm<sup>2</sup>, E<inf>c</inf>= 1.04 kV/cm) were obtained at the sintering temperature of 1400°C. The altered phase structure in this research, compared to earlier studies, results in distinct outcomes for the dielectric and ferroelectric properties.
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    Effect of the Firing Temperatures on the Phase Evolution and Electrical Properties of 0.85[0.94Bi0.5Na0.5TiO3-0.06BaTiO3]-0.15[Na0.73Bi0.09NbO3] Ceramics Synthesized via the Solid-State Combustion Method
    (2023-01-01)
    Pattanakasem, Wiwat
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    Yotthuan, Surirat
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    Hongsamsibjed, Pakornkiat
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    Suriwong, Tawat
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    Prasertpalichat, Sasipohn
    In this research paper, we describe 0.85[0.94Bi<inf>0.5</inf>Na<inf>0.5</inf>TiO<inf>3</inf>-0.06BaTiO<inf>3</inf>]-0.15[Na<inf>0.73</inf>Bi<inf>0.09</inf>NbO<inf>3</inf>] (BNT-BT-NBN) ceramics fabricated by the solid-state combustion technique. The phase evolution, microstructure, dielectric, ferroelectric and energy storage properties were examined. The BNT-BT-NBN powders and ceramics were calcined and sintered between 650–900 °C and 1100–1175 °C, respectively, for 2 h. All samples showed a typical perovskite structure, as revealed by X-ray diffraction. The Rietveld refinement analysis of the ceramics suggested the samples sintered between 1100 and 1150 °C had coexisting R + T phases, while the R + T+C phases were observed in the ceramics sintered at 1175 °C. The average grain size of the samples increased from 0.52 to 1.39 μm with increased sintering temperature. The density of the ceramics increased from 5.12 to 5.45 g/cm<sup>3</sup> when the sintering temperature increased from 1100 to 1150 °C, and then decreased. Increasing the sintering temperature from 1100 to 1150 °C caused the dielectric constant at T <inf>s</inf> (ε <inf>s</inf>) and the dielectric constant at T <inf>m</inf> (ε <inf>m</inf>) to increase from 1727 to 1945 and 1564 to 1750, respectively, and then ε <inf>s</inf> and ε <inf>m</inf> declined. All BNT-BT-NBN ceramics had good dielectric temperature stability with only a±10% change when the temperature ranged from room temperature to ∼300 °C. The optimum energy-storage properties (W <inf>rec</inf> = 0.62 J/cm<sup>3</sup> and η = 83.2%) were obtained from the BNT-BT-NBN ceramics sintered at 1150 °C for 2 h. This data indicates that BNT-BT-NBN ceramics can be useful as lead-free materials for high density energy-storage capacitors.
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    ELECTRIC AND MAGNETIC PROPERTIES OF Ba0.97Ca0.03Ti0.94Sn0.06O3-Mn0.85Ni0.15Zn0.15Fe2O4 MULTIFERROIC CERAMIC COMPOSITES FABRICATED VIA THE SOLID-STATE COMBUSTION TECHNIQUE
    (2025-01-01)
    Sonchaopria, Nutkamon
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    Meechob, Jirayut
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    Thatawong, Bhoowadol
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    Pinitsoontorn, Supree
    Multiferroic composites with the general formula (1-x)(Ba0.97Ca0.03Ti0.94Sn0.06O3)-x(Mn0.85Ni0.15Zn0.15Fe2O4) (BCTS/MNZF) (x = 0.1, 0.2, 0.3, 0.4, and 0.5) were prepared using the solid-state combustion method. The structure, morphology, dielectric, ferroelectric, magnetic, and magnetoelectric properties were analyzed. The samples were sintered at 1,300ºC for 2 h. The X-ray Diffraction (XRD) patterns revealed tetragonal perovskite, orthorhombic perovskite, and cubic spinel structures corresponding to the BCTS and MNZF phases. Secondary phases (Mn2O3 and SnO) appeared in the sintered samples with x>0.2. Increasing MNZF content enhanced ferrite grain growth in the composites. The dielectric constant showed an overall decreasing trend with increasing MNZF content, with a smaller effect at lower frequencies. At lower frequencies, the dielectric constant declined with increasing frequency before stabilizing around 10 kHz. As ferrite content increased, the density, dielectric constant, and magnetoelectric coefficient (αME) decreased from 5.66 to 5.12 g/cm³, 1388 to 862, and 7.24 to 4.05 mV/cm·Oe, respectively. While the saturation magnetization (Ms) rose substantially from 0.75 to 13.14 emu/g. These findings offer valuable insights into enhancing lead-free multiferroic composite ceramics for targeted applications in magnetoelectric devices.
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    ELECTRICAL AND MAGNETIC PROPERTIES OF MULTIFERROIC Co0.6Zn0.4Fe1.7Mn0.3O4 DOPED 0.99Bi0.47Na0.47Ba0.06TiO3-0.01Ba(Sn0.70Nb0.24)O3 CERAMICS SYNTHESIZED VIA THE SOLID-STATE COMBUSTION TECHNIQUE
    (2025-01-01)
    Luangpangai, Anupong
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    Chuai, Phomphon
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    Rittidech, Aurawan
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    Pinitsoontorn, Supree
    ;
    Jantaratana, Pongsakorn
    Multiferroic (1-x)[0.99Bi<inf>0.47</inf>Na<inf>0.47</inf>Ba<inf>0.06</inf>TiO<inf>3</inf>-<inf>0.01</inf>Ba(Sn<inf>0.70</inf>Nb<inf>0.24</inf>)O<inf>3</inf>]-xCo<inf>0.6Z</inf>n<inf>0.4</inf>Fe<inf>1.7</inf>Mn<inf>0.3</inf>O<inf>4</inf> (abbreviated as BNBT-BSN-xCZFMO) ceramics with x ranging from 0 to 0.20 were fabricated using the solid-state combustion technique. The effect of varying BNBT-BSN: CZFMO ratios on the phase structure, microstructure, electrical and magnetic properties was investigated. X-ray diffraction (XRD) analysis of pure BNBT-BSN showed a perovskite structure with rhombohedral and tetragonal phases. The doped BNBT-BSN-xCZFMO ceramics displayed coexisting rhombohedral, tetragonal, and cubic spinel phases, with the cubic spinel phase increasing when the CZFMO content increased. In addition, the XRD peaks shifted to higher angles as the CZFMO content increased, indicating a decrease in lattice parameters. The dielectric constant decreased with higher CZFMO content and higher frequencies. The pure BNBT-BSN ceramic exhibited a saturated P-E loop with a Pmax of 33.2 µC/cm<sup>2</sup>, Pr of 26.1 µC/cm<sup>2</sup>, and an Ec of 14.5 kV/cm. With increased CZFMO content, non-saturated and bloated P-E loops with lower Pmax, Pr, and Ec were observed, implying a rise in the leakage current. The addition of CZFMO induced ferromagnetic behavior in the ceramics, leading to an increase in Ms and a reduction in Hc as CZFMO content increased. The magnetoelectric coupling coefficient of BNBT-BSN-xCZFMO ceramics continuously increased with higher CZFMO content.
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    PHASE FORMATION AND ELECTRICAL PROPERTIES OF Ba0.91Ca0.09Ti0.916Sn0.084O3-0.1WT%ZnO -0.1WT%MnO2 LEAD-FREE FERROELECTRIC CERAMICS SYNTHESIZED VIA THE SOLID-STATE COMBUSTION METHOD
    (2025-01-01)
    Yimsabai, Sununta
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    Somsri, Widchaya
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    Charoenthai, Nipaphat
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    Suthapintu, Aekasit
    This work investigated the effect of firing temperatures on the phase formation, microstructure, and electrical properties of Ba0.91Ca0.09Ti0.916Sn0.084O3-0.1wt%ZnO-0.1wt%MnO2 (BCTS-ZnMn) lead-free ferroelectric ceramics synthesized via the solid-state combustion method. Glycine was used as fuel to reduce the synthesis temperature. The samples were calcined at temperatures from 1050 to 1250°C (in 50°C increments) for 3 h and sintered from 1250 to 1450°C (in 50°C increments) for 3 h. A pure perovskite phase was found in the powders calcined above 1100°C. The phase structure, microstructure, dielectric and ferroelectric properties of the ceramics were examined. The X-ray diffraction (XRD) analysis for the ceramics revealed the presence of tetragonal (T) and orthorhombic (O) phases in all the ceramics. The average particle size and average grain size increased with increasing firing temperatures. The density, dielectric constant at the Curie temperature (ɛc), Pr and Ps tended to increase with increasing sintering temperatures, up to 1400°C, and then decreased at 1450°C. The ceramic sintered at 1400°C exhibited the highest density (5.89 g/cm3), dielectric response (ɛc = 13324) and good ferroelectric behavior (Pr = 8.67 μC/cm2, Ps = 17.92 μC/cm2 and Ec = 0.99 kV/cm).
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    The role of γ-C2H5NO2 as a new transient liquid phase in cold sintering process of BaTiO3 composites
    (2024-07-01)
    Noisak, Jitrawan
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    Ieamviteevanich, Pimchanok
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    Charoonsuk, Thitirat
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    Pakawanit, Phakkhananan
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    Pinpru, Nattapong
    Dielectric materials, such as barium titanate (BT)-based materials, have excellent dielectric properties but require high temperatures (above 1300 °C) for ceramic fabrication, leading to high costs and energy loss. The cold sintering process (CSP) offers a solution to these issues and is gaining worldwide attention as an innovative fabrication route. In this work, we proposed an alternative organic ferroelectric phase, gamma-glycine (γ-GC), which acts as a transient liquid phase to fabricate high-density composites with barium titanate (BT) at low temperatures through CSP. Our findings show that the density of 15γ-GC/85BT reached 96.7%±1.6% when it was sintered at 120 °C for 6 h under 10 MPa uniaxial pressure. Scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS) mappings of the composite suggested that γ-GC completely underwent the precipitation–dissolution process and, therefore, filled between BT particles. Moreover, X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FTIR) confirmed the preservation of γ-GC without undesired phase transformation. In addition, the ferroelectric and dielectric properties of γ-GC/BT composites have been reported. The high dielectric constant (ε<inf>r</inf>) was 3600, and the low dielectric loss (tanδ) was 1.20 at 200 °C and 100 kHz for the 15γ-GC/85BT composite. The hysteresis loop showed a remanent polarization (P<inf>r</inf>) of 0.55 µC·cm<sup>-2</sup> and a coercive field (E<inf>c</inf>) of 7.25 kV·cm<sup>-1</sup>. Our findings reaffirmed that an organic ferroelectric material (γ-GC) can act as a transient liquid phase in a CSP that can successfully and sustainably fabricate γ-GC/BT composites at low temperatures while delivering outstandingly high performance.
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    Sintering Temperature Effect on Phase Formation, Microstructure and Electrical Properties of Modified KNLNTS Solid Solution Prepared via the Solid-State Combustion Technique
    (2023-01-01)
    Kornphom, Chittakorn
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    Thawong, Pichittra
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    Khiwoon, Suprakorn
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    ;
    Bongkarn, Theerachai
    In this study, the effect of sintering temperature (1000–1100 °C for 2 h) on phase formation, phase transition, microstructure and electrical properties of lead-free piezoelectric (K<inf>0.44</inf>Na<inf>0.52</inf>Li<inf>0.04</inf>)(Nb<inf>0.84</inf>Ta<inf>0.10</inf>Sb<inf>0.06</inf>)O<inf>3</inf> (KNLNTS) solid solution with 0.3 wt%Bi<inf>2</inf>O<inf>3</inf> + 0.4 wt%Fe<inf>2</inf>O<inf>3</inf> + 0.2 wt%CuO additive (abbreviate as modified KNLNTS) was investigated. Modified KNLNTS ceramics were synthesized by the solid-state combustion technique using glycine as fuel. The modified KNLNTS powders were prepared using the calcination condition of 650 °C for 2 h. The XRD pattern of all sintered ceramics exhibited a pure perovskite phase. Using Rietveld refinement to analyze the phase formation showed that the modified KNLNTS ceramics had co-existing phases of orthorhombic and tetragonal in all sintered ceramics and the orthorhombic phase increased when the sintering temperature increased. The average grain size, T<inf>O-T</inf>, T<inf>c</inf>, P<inf>r</inf> and Ec increased with increasing sintering temperature. At the sintering temperature of 1025 °C, the modified KNLNTS ceramic showed the best electrical properties (C<inf>ε</inf> ≈ 6745, S<inf>max</inf> ≈0.274% and d*<inf>33</inf> ≈ 548 pm/V). The good electrical properties of the modified KNLNTS ceramics makes them good candidates for lead-free applications to replace Pb-based ceramics.
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    Optimal Bi₀.₈Ba₀.₂FeO₃ doping in Bi₀.₅(Na₀.₇₇K₀.₂₀Li₀.₀₃)₀.₅TiO₃ multiferroic ceramics synthesized by the solid-state combustion technique
    (2025-12-01)
    Thawong, Pichittra
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    Prasertpalichat, Sasipohn
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    Suriwong, Tawat
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    Pinitsoontorn, Supree
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    Jantaratana, Pongsakorn
    (1-x)Bi<inf>0.5</inf>(Na<inf>0.77</inf>K<inf>0.20</inf>Li<inf>0.03</inf>)<inf>0.5</inf>TiO<inf>3</inf>-xBi<inf>0.8</inf>Ba<inf>0.2</inf>FeO<inf>3</inf> ((1-x)BNKLT-xBBF) ceramics with x = 0-0.4 were synthesized by the solid-state combustion technique. X-ray diffraction (XRD) analysis confirmed a pure perovskite structure with coexisting rhombohedral and tetragonal phases. Rietveld refinement revealed that the unit cell volume increased with increased x due to the substitution of smaller Bi<sup>3+</sup> and Ti<sup>4+</sup> ions by larger Ba<sup>2+</sup> and Fe<sup>3+</sup> ions at the A- and B-sites, respectively. The average grain size and measured density also increased with increasing x, while the resistivity decreased. At room temperature, (1-x)BNKLT-xBBF ceramics with x = 0.2–0.4 exhibited multiferroic behavior, characterized by ferroelectric and ferromagnetic hysteresis loops. The 0.8BNKLT-0.2BBF ceramic exhibited the most favorable properties, including: the highest relative density (95.48%), the highest dielectric constant and low dielectric loss at room temperature (ε<inf>R</inf> = 1746 and tan δ<inf>R</inf> = 0.0296), good ferroelectric properties (P<inf>r</inf>=6.46 µC/cm<sup>2</sup> and E<inf>c</inf>=11.84 kV/cm) and good ferromagnetic properties (M<inf>r</inf>=0.002 emu/g, H<inf>c</inf>=110 Oe and α<inf>E</inf> = 1.092 mV/Oe·cm). These results indicate that 0.8BNKLT-0.2BBF has the potential for applications in lead-free, room temperature multiferroic applications.